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mlatter
nluclear
slcience
i to takahashi
ken-ichiro ota
yasuhiro iwamura
ondensed
m otter
n"uclear
science
proceedings of the 12th international conference on cold fusion
This page is intentionally left blank
ondensed
m after
n uclear
cience
proceedings of the 12th international conference on cold fusion
Yokohama, Japan
Editors
Akito Takahashi
Osaka University, Japan
Ken-ichiro Ota
Yokohama National University, Japan
Yasuhiro Iwamura
Mitsubishi Heavy Industries, Japan
For photocopying of material in this volume, please pay a copying fee through the Copyright Clearance Center,
Inc., 222 Rosewood Drive, Danvers, MA 01923, USA. In this case permission to photocopy is not required from
the publisher.
ISBN 981-256-901-4
The study of Condensed Matter Nuclear Science (CMNS) has continued to advance
through 11 past conferences (ICCF1 at Utah, USA in 1989 to ICCF11 at Marseilles,
France in 2004) and many new compelling scientific findings are becoming known.
The historical 1989 claim of "cold fusion" had renewed hope of a portable clean
nuclear reactor. The subsequent great wave of denial and hostility forced the claim
and further research efforts out of mainstream science. Nevertheless, due to miscon-
ceptions and misinformation, very few people know that several hundred researchers
from around the world have continued this research during the past 16 years. The
efforts by this faint stream of research have now revealed that there exist new kinds
of nuclear effects directly related to the nature of condensed matter. The nuclear
effects in condensed matter are much more than real "cold fusion"; they include
important nuclear effects such as transmutations and resulting release of energy
as significant heat with minimal and safe radiation. Low levels of radiation are
found in at least some reactions, but are usually absorbed within the cell itself so
the system is categorically safe. Through discussions at international conferences
(ICCF1-ICCF11), a majority of researchers agreed that the name "cold fusion"
was misleading. A new name, closer to the exact phenomenon, Condensed Matter
Nuclear Science, is most appropriate.
This emerging field, CMNS, treats nuclear effects in and/or on condensed mat-
ter, targeting its application for portable clean nuclear sources. This is an inter-
and multi-disciplinary academic field, including nuclear physics, condensed matter
physics, surface physics, and chemistry and electrochemistry. CMNS applications
involve many other fields of science and technology (nuclear engineering, mechanical
engineering, electrical engineering, laser science and engineering, material science,
nano-technology, biotechnology, energy politics, etc. To promote the development
of CMNS and establish the academic field of CMNS, the field needs highly efficient,
cooperative efforts of researchers, and related people working in different fields.
International linkage and collaborations are also needed.
The full name of this conference is the 12th International Conference on Con-
densed Matter Nuclear Science. However, we decided to keep the acronym ICCF12
for the Conference, considering our original standpoint and tradition.
The International Society for Condensed Matter Nuclear Science (ISCMNS)
made a start in 2004 to promote the understanding, development and application
of CMNS and has become a main supporting body of the ICCF series conferences
till ICCF11. However, ICCF12 is sponsored by other societies like JCF (Japan-CF
Research Society) and supported also by non-ISCMNS members. ICCF12 will
provide an international scientific forum for direct interaction and stimulation
among many scientists working in the CMNS field and participation and presenta-
tion of newcomers will be welcome.
V
vi
The Conference site and date were: Shin-Yokohama Prince Hotel, Yokohama-
city, Japan on 27 November-2 December 2005.
The following topics were discussed in the conference:
For organizing and preparing ICCF12, the following members of LOC (Local Or-
ganizing Committee) and IAC (International Advisory Committee) have made
contributions.
Sponsors of ICCF12
ISCMNS: International Society for Condensed Matter Nuclear Science.
TEET: Thermal and Electric Energy Technology Foundation.
JCF: Japan CF-Research Society.
All the full papers submitted for Proceedings book were peer-reviewed by the
specialists from Japan. Revised drafts were edited, converted into LaTeX format
and send to the publisher (World Scientific Publishing Co. Pte. Ltd., Singapore).
For some of the presentations at the meeting of ICCF12, authors did not submit
full papers and those papers are not included in the Proceedings book.
Due to trivial mistake, a few papers submitted to ICCFll (Marseilles) Pro-
ceedings could not be included in the Proceedings of ICCFll (published by World
Scientific Co, 2006). These missing papers by Dr. V. Violante group are included
in the present book for compensation.
Editors
Akito Takahashi, Ken-ichiro Ota, and Yasuhiro Iwamura
30 June 2006
CONTENTS
Preface v
1. G E N E R A L
Summary of ICCF-12 26
X. Z. Li
2. EXCESS HEAT A N D He D E T E C T I O N
Production method for violent TCB jet plasma from cavity 163
F. Amini
3. T R A N S M U T A T I O N
5. MATERIAL SCIENCE
6. THEORY
A K I T O TAKAHASfflt
Osaka University, Yamadaoka 2-1, Suita, Osaka 565-0871, Japan
E-mail: akito@sutv.zaq.ne.jp
Recent studies of condensed matter nuclear science (CMNS) including cold fusion
have accumulated some convincing data and theoretical modeling, and we are
about to conclude that (1) deuteron-related clean fusion reactions and (2) cold
and special transmutations may take place in the environment of condensed matter
containing deuterons and protons. This emerging field of CMNS is expected to give
us strong impact on the future of basic sciences for energy-application, fundamental
nuclear science, and condensed matter sciences.
1. Introduction
Condensed matter nuclear science (CMNS) was born as a descendant research field
of Cold Fusion. In March 1989, S. Pons and M. Fleischmann at University of Utah
announced "cold fusion" by D 2 0 / P d electrolysis in test tube. The experimental
system looked very simple. So many people in the world were involved in hur-
ried trials of replication-experiments. In most trials, however, huge excess heat as
claimed by Pons-Fleischmann was not observed. Parallel replication trials for the
Nature paper by S. Jones on weak 2.45 MeV DD neutron emission from D20/Ti
electrolysis cell were not either successful. Very negative mood was seen in almost
all scientific communities in the world. 1
In 1990-1992, some hopeful data on excess heat in D 2 0 / P d cells were reported
from research teams in USA, Japan, and Italy. Although reproducibility was yet
to be attained, great expectation was come back for the clean energy application
based on "new nuclear energy process". In Japan, the New Hydrogen Energy (NHE)
project was implemented in 1994-1998, at Shin-Sapporo Laboratory, where about
20 researchers from major Japanese industries and several foreign scientists worked
together to verify the excess heat effect in Fleischmann-Pons type systems. The
NHE effort was concentrated in D/H absorption data in metal-samples and excess
heat detection. In spite of energetic efforts by the NHE team, they made final
report that excess heat effect was not confirmed. Few positive data on excess
heat from foreign researchers and some positive data on nuclear products from
Japanese University teams were unfortunately not meaningfully evaluated by the
NHE evaluation committee. The NHE project was terminated in 1998.
1
2
Slide 1
p + t + 4.02MeV;50%
Slide 2
Major experiments
(green; after 2001)
Slide 3
l»1 -mi TM>3 W>i JS>5 I Tub 6 » 7 THUS Ware HF " f «•?«» !'"
0/00:00:00 0/09:58:40 0/19:57:21
.000 „ . 17 H
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34,000
COPE = (Pout-Pinet): Pim - (20-0.74):0.74 » 25
32,000
w.
118,000
^ 16,000
14,000
\r*\'
6,000
4,000
2,000
Average P inet -0.74 W ;
llfcliilliHiTt lit <m WyfliWOfc^ t u l i l i f t ' i U i M l 11 iin UK i m i ^ ' Mil liW HI
0,000 f
*: ••- j 4 f ]
5000 10000 15000 20000 25000 30000 35000 40000 45000 50000 55000 00000 S5000 71S24 *
This group is trying superposed stimulation with laser beam and ultrasonic
wave. This is interesting trial. The group has obtained data for 4 He production in
correlation with excess heat generation. An example of data is shown in Fig. 2.
When we irradiate laser on surface of Pd cathode, we can choose laser wavelength in
ultraviolet and EUV region due to the classical Drude formula for frequency depen-
dence of dielectric constant of metal. They used He-Ne laser (632 nm wavelength).
Also they observed increase of excess power of several times of laser input power
(33 mW). On the right-hand side figure of Fig. 2, time-dependent data of relative
resistance ratio of PdDx are drawn. During the laser irradiation and excess power
episode, D/Pd ratio kept more than 0.9. However, continuation of laser irradiation
induced no excess power and decrease of D/Pd ratio (increase of resistance ratio).
This is very interesting data showing relation between excess power and D/Pd ratio
under laser stimulation.
Arata et al.11^15 have made significant contribution to provide clear experimen-
tal data of 4 He production from their own double structure cathode of Pd in heavy
water electrolysis cell and from D-gas-phase absorption system of Pd nano-particles
7
that the effect is real. It was observed that Pd-plate was destroyed into small
powders during the experiment. Stringham 24 has been studying the similar method
with higher frequency (in MHz range) ultrasonic wave.
We have other reports on 4 He production by de Ninno, Isobe, 18 and so on. We
can say that the phenomenon of excess heat with 4 He generation is "qualitatively"
reproducible.
However, conditions for 100% reproducible protocols are yet to be established.
To find quantitatively reproducible conditions, we need investigations on nano-
modification of samples, procedures to keep high D/Pd ratios and dynamic D-flux
through samples and external stimulation methods (electrolysis patterns, laser and
ultra-sonic wave irradiations, and so on).
150
Gradient )'=18.36X
it = 0,99
Differential y = 18.36x
f? = 0.99
100 Gradient Q = 31 ± 13 MeV/atom
4=
Differential 0= 32 ± 13 MeV/atom ! ^-'
50
0 <3^H ^—
0 2 3 4 5 6
Helium increase (ppmV/V)
Major reports 2 " 6 are from Iwamura, Mizuno, Celani, Yamada, Karabut,
Violante, Miley, Mastromatteo, Savvatimova, Passel, Szpak, and so on. Key issues
in experiments are mass-analysis, isotopic-ratio analysis, spectroscopic detection of
particles (including X-rays and gamma-rays), nano-modification of samples, and
external stimulation (or triggering).
Most remarkable and reproducible transmutation experiments have been re-
ported by MHI Iwamura group. 2 5 " 2 9 They are using Pd-complex samples which
have multi-layered structure of about 100 nm surface Pd layer and following four
layers of alternative CaO/Pd composition (see Fig. 4) on 0.1 mm thick Pd sub-
strate plate. They put small amount of test elements (Cs or Sr) on surface. They
set a sample in a chamber filled with 1-atom D2 gas and evacuate the volume
rear sample plate. D-atoms permeate through sample by keeping permeation rate
higher than 1 seem. They have made in situ analyses of surface elements by X-
ray-induced Photoelectron Spectroscopy (XPS) or X-ray Fluorescence Spectroscopy
(XFS). Amazingly, they observed transmutations of 133 Cs -^ 1 4 1 Pr, 88 Sr -^ 96 Mo
for the cases of D-permeation, but did not at all for H-permeation.
i..rT-"-;>T j.
Dflux
Vacuum
up new chamber with incidence of strong SOR X-ray beam to make in situ FXS
analysis of surface elements of Pd-complex under D-permeation. They have repeat-
edly observed transmutation from 133 Cs to 1 4 1 Pr (see Fig. 5). They have made
sample analysis after experiments by Time-of-Flight Secondary Ionization Mass
Spectroscopy (TOF-SIMS) to find that transmuted Pr distributed within about
10 nm depth from surface of Pd-complex sample (see Fig. 6). The data in Fig. 6
give insight that the transmutation reaction should have taken place in near surface
region.
.....a...... 35
™, # ™>36 Cs-U;, Cs-L p1
1
4
Iw—s*
Br ^.4
T
•
;
,if 1m -A
i'
I
i
• •, • • i
1
100- . ^
i ' !-\
' V i
'i*
Cs Lp2
J
50-
Energy (keV)
Takahshi et a/. 32-34 have proposed a deterministic fission theory [Selective Chan-
nel Scission (SCS) model] based on rotating liquid drop model of excited nucleus.
They checked the model successfully for calculating mass and atomic number dis-
tributions of fission products (FP) by 2 3 5 U+n fission process 33 to be compared with
experimental data. Then they applied the model for predicting FP distributions of
lower mass nuclei of A < 200. Mizuno's foreign element data are compared with
Takahashi calculation in Fig. 7.
Theoretically predicted element distribution looks similar to Mizuno experiment.
In the SCS process, isotopic ratios of FP element become very different from natural
abundances. For example, 57 Fe exists with 0.3% in natural iron, but both of FP of
SCS theory and experiments by Mizuno gave similar values of about 10% in FP iron
100
Pd-natural
.MPIF
LB-1
• MIZUNO-EXP
10
1 Sr
t -
0.1
0 5 10 15 20 25 30 35 40 45 50
Atomic number
Figure 7. Foreign atom distribution obtained by Mizuno's D2O electrolysis, compared with the-
oretical prediction of Pd-fission products calculated by SCS theory by Takahashi et al.
12
isotopes. These agreements are quite interesting, and further studies are expected
to verify if the phenomenon is really nuclear fission process for lighter nuclei in
the environment of metal-D systems. Similar results have been reported for Ni-H
systems as discuss below. The SCS theory predicts that fission products for A < 200
nuclei become very much cleaner (less radio-active and very small neutron emission)
due to predominant production of stable isotopes. 3 2 - 3 4
4. Metal—Hydrogen Systems
Observation of anomalous production of foreign elements and excess heat in metal-
ordinary-water/H systems have been claimed 2 " 6 in reports by Piantelli, Ohmori,
Miley, Yamada, Romadanov, Dash, Li, Mizuno, and so on. Key issues of experi-
ments are again calorimetry, mass and isotopic analyses, radiation detection, sample
fabrication, and triggering and stimulation techniques.
Piantelli et al.36'37oi Siena University has been doing a H-gas absorption and
diffusion type experiments using cylindrical Ni samples in chamber with heating
device. They have made claim of large excess heat and gamma-ray emission with
production of foreign elements. Figure 8 shows one of their typical data for obser-
vation of gamma-ray emission.
They set up a standard 137 Cs gamma-ray (661 keV peak) source for calibration.
The observed peak at around 744 keV is a surprise, which they say the gamma-
line from Mn isotope. A theoretical prediction by Takahashi's 4p/TSC-induced
fission35interpret that 52 Mn and 56 Ni as FPs of Ni + 4p fission process can be
sources of 744 keV line.
It is well known that Miley-Patterson 38 reported distributed production of trans-
muted elements and excess heat in their Ni-ordinary-water electrolysis experiments.
Comment by A. T.
400.00
Mn (EC)
Ni-fl-4p-> C +
"Fs(EC)"Mn(ECi"cr(EC) 0.00 1
1 ' 1 ' 1 ' 1 Canal!
0.00 200.00 400.00 600-00 800.00
1
, > t. < i
1
Yield (%)
»NA»
5 10 15 20 25 30 35 40 45 50 <
S
Atomic number
-
1 1 2
Ni + 4p/TSC to fission 3 10 20 30 40 50
calculated by selective
Atomic number
channel fission model
Figure 9. F P elements by SCS versus Miley experiment (G. Miley and J. Patterson J. New
Energy, 1996, 1, p. 5).
58 s8 61 81
* 8.8 MeV -t t- Zn (EC) Cu (EC) -»18.9MeV + • + Zn (EC) Cu (EC)
• 8.8 MeV + v M Ar (EC) MCI (EC) ^15.9 MeV+ + 68 Fe(EC) 68 Mn(3.7x10 8 y)
4!
^11.0 MeV + ! + Ti (EC) ..
37
—17.4 MeV + • + Ar(EC)
!(2) °°Ni (26.2%) + 4p - * " G e (Ex = 19.1 MeV) !7
-,12.0 MeV + Si(EC) + •
- . 16.4 MeV + He + 80Zn (EC) 60Cu (EC) -*17.5MeV +
- t 13.6 MeV + "Be + "TN|I (EC) 56Co (EC) ;
- . 13.0 MeV + 12C + 52Fe (EC) MMn (EC) ' .
48 48
-»12.2 MeV + " 0 + Cr (EC) V (EC)
-»13.5 MeV + + Note:
^ 1 6 . 4 MeV + +
-.16.7 MeV + +
• Average kinetic energy of
-.6.5 MeV + + 26 Sl(EC)AI(10 5 y)
fission product = 9.7 MeV for
Ni-natural
Takahashi;ICCF11
Slide 4
14
« Branching ratio:
Sn(0)/Sp(0)/Sg(0) =
&»s/////////J< r„/r,/rg =
20.577 • „ 3 © . n + aHe 0.5/0.5/0.0000001
19,814- — -*• p +1 • r n = r p = 0.2 MeV
• r g = 0.2 MeV
Qamma transition • r, = r n + r p + r g
.T = WT,=1E-22S
Figure 10. Final state interaction and branching ratios for d-d fusion.
2) Minimum TSC
V A
^
4 4
He He
xr
Figure 11. Illustration of TSC squeezed condensation; (a) TSC formation at t = 0, (b) minimum
size state of condensed TSC, (c) formation of 8 Be* by strong interaction, and (d) break-up of 8 Be*
into two alpha-particles.
Strong F.
Bare Coulomb potential
Figure 12. Shielded Coulomb potential for dde* pseudo-molecule under steady-state assumption;
relation to screening energy and strong interaction range for d-d reaction is illustrated.
17
e* Us(eV) b0 (pm)
(1.1) 36 72 40 20
(2.2) 360 411 4 3.5
(4,4) 4000 1108 0.36 1.3
(8,8) 22154 960 0.065 1.5
(208,1) 7579 7200 0.19 0.20
not happen unless high potential barriers of Coulomb repulsion can be overcome
by particular ways that we should theorize. We have to estimate how Coulomb
repulsion is overcome in the initial state interaction, how intermediate compound
state is and what are branching ratios in the final state interaction. Theoretical
modeling should be self-consistent so as to be quantified.
The theory of EQPET/TSC by Takahashi 50 " 58 is trying to give quantified pre-
dictions. Recently at ICC10, Takahashi proposed TSC of four deuterons and four
electrons in PdDx lattice dynamics forming a transient quasi-molecular state of
orthogonally coupled two D2 molecules and squeezing semiclassically into central
T-site to reach TSC-minimum-size state with about 10 fm diameter as charge neu-
tral pseudo-particle. The TSC-minimum state for 4D/TSC causes self-fusion of 4D
to 4 He + 4 He + 47.6 MeV, or capture reaction (selective transmutation) with host
metal nucleus. This scenario is shown in Fig. 11.
Takahashi treats transiently bosonized states of electron pairs with anti-parallel
spins and quadruplet coupling e*(4,4) by Electronic Quasi-Particle Expansion
Theory (EQPET). 5 1 - 5 5 He treats virtual pseudo-molecule dde* as illustrated in
Fig. 12. He calculated screened potentials for dde* molecules and estimated screen
energies and other potential parameters as given in Table 1.
Nuclear strong force for fusion is estimated based on the concept of optical
potential (see Fig. 13) and effective surface sticking force P E F 5 2 - 5 8 for multi-body
(4D) fusion by TSC.
• U ( r ) = V(r) + ilV(r}
J •4 IV(r) - W „ 8 ( r - r 0 )
-"0
^—iment b\ A T
Fusion rate for collision process
dynamic or transient process-
• 7= OF, |Hint| ¥i>
= (Initial state interaction)
x (Intermediate compound state)
x (Final state interaction)
• Cross-section - T2 p (E')
• p (E'): final state density
- Reaction-rate (ov): (4TCS//I)V72 p (E')
• (Initial) = (El. EM int) (strong int)
• (Final) = BRs to irreversible decays
Slide 5
Practical formulas are given in Fig. 14. Time averaged cluster fusion rates for
the TSC squeezing motion is given in Table 2. He reports some of key issues in
CMNE can be explained by these EQPET/TSC models as shown in Table 3.
Kim 61 ' 62 is studying CMN effects in Bose-Einstein condensation (BEC) process.
He assumes that many deuterons, metal ions like Li + and electrons are confined in
a void cavity in metal lattice and they are behaving as plasma. Superposition of
many-body wave functions by BEC is supposed to play role for strong enhancement
of dd fusion and d-6Li fusion (source of 4 He generation). Deuteron is a boson. To
F l J S i O n T a t e Of D - C l U S t e r |Takahasni:racemRes.Devel.Physics,6(2005) 1
FnD = 0F12>(4'22>Cl'32>-vI'„2>
*Virtual value.
minimize system Coulomb energy of particles in the cavity should, however, lead to
charge neutralization between deuterons and electrons to form D-atoms for dilute
gas (or D2 molecules after collision process for dense gas). Plasma state at room
temperature looks no good idea. And D-atoms are fermions due to odd (non-integer)
spin for electron. Models by Kim and Tsuchiya need further elaboration.
Takahashi's EQPET/TSC models are kind of bosonized condensate models.
However, TSC is bosonized condensate under strong constraint (namely ordering
process in lattice), different from BEC of dilute gas at near zero temperature but
similar to bosonization of fermions (formation of Cooper pair) for super-conductivity
and super-fluid. New aspect as CMNS is "Bosonization in Ordering Process".
X. Z. Li has studied Resonant Tunneling Model. 64 ' 65 Intermediate compound
state of fusion reactions in CM may have, he proposes, excited state with very long
(as 104 s) life time to select resonating decay channel for final state interaction.
During his study he has made nice progress to fit fusion cross sections for DD, DT,
and D 3 He reactions using revised formulas of elementary phase-shift analysis of
scattering matrix and optical potential. This is good progress. However, his model
cannot change the situation of Fig. 10, namely for drastically increase branching
ratio to 4 He channel since longer life time makes the gamma-transition branching
ratio smaller.
Hagelstein has been studying a kind of coherent fusion model to explain neutron-
less 4 He generation and excess heat. His models do not reach the stage of quantified
theory, but are trying to approach to quantification. Recently he is proposing the
phonon-coupled gauge models, assuming 'compact' intermediate state of (n-3He)
to evaluate gauge transform between (d-d) state, (n-3He) state, and irreversible
out-going channel to 4 He. This is an elegant approach. However, there are some
fundamental problems. First, (n-3He) state may not exist with meaningfully large
life time to be prohibited to going out to the n + 3 He + 3.25 MeV channel with very
short life time (on the order of 10~ 22 s) from the intermediate compound state 4 He*
as shown in Fig. 10. He estimates that the transform strength (QM flow) between
states by phonon exchange is on the order of 1 0 - 4 , which is right but is much
smaller than field coupling between strong interactions (see Slide 6, accordingly).
Branching ratio to electromagnetic transition (decay channel to 4 He) cannot be
increased by more than 10~ 4 of those (0.5) for n + 3 He or p + t channels.
Chubb-Chubb 7 1 - 7 4 have proposed a kind of coherent fusion model through the
D-ion-band state in PdDx lattice Bloch potential. They assume that QM waves of
many deuterons inside a well of many-body (more than 10,000 Ds) potential can
link widely and, due to the double Bloch symmetry conditions, Coulomb repulsions
between deuterons eliminate in scale of 1/Nwell for Nwell more than 10,000. They
also assume this coherent condition should change the intermediate compound state
(4He*) of DD interaction to form 4 He-ion-band state with long life time, for which
we can use wave-function form of 4 He. This is another elegant theory. To reach
quantified predictions by this theory, we need to substantiate many things; to prove
definitely the 1/Nwell law, to
a ~ (T-matrix)2
Slide 6
Slide 7
Here key issue will be how reaction rates via weak interactions can be enhanced.
Quantitative predictability is the key.
Brief scenario of Widom's theory is; on the flat surface of metal-hydride, coherent
coupling between many-body electron oscillations and proton oscillations makes
effective electron mass significantly heavy. Mini-atom orbit of H-atom with heavy
electron forms. Electron capture process into proton may be very strongly enhanced
to generate near-zero-momentum neutrons. These very low-energy neutrons will be
absorbed within very short range near surface to induce neutron-induced reactions.
This kind of theory has many fundamental problems as:
We can make such skeptical critics easily for other models also. By making
clear every question, one by one, one can improve m o d e l s 8 4 - 8 9 and approach t o the
target. We need tough efforts of elaborations.
7. C o n c l u s i o n s
References
1. J. R. Huizenga, Cold Fusion, The Scientific Fiasco of the Century (University of
Rochester Press, USA, 1992).
2. Proceedings of ICCF9, Tsinhua University Pub. (2003).
3. Proceedings of ICCF10, World Scientific Pub., to be published, see also internet
version at http://www.lenr-cana.org/
4. Proceedings of ICCFU : World Scientific Pub., to be published, see also internet site
http://www.iscmns.org/
5. Proceedings of ASTI5 Meeting, see internet site http://www.iscmns.org/
6. Proceedings of SIENA2005 Workshop, see ibid.
7. P. Hagelstein, M. McKubre, D. Nagel, T. Chubb, and R. Heckman, New Physical
Effects in Metal Deuterons, Reprot to US-DoE (2003).
8. US-DoE: Report of the Review of Low Energy Nuclear Reactions, December 1, 2003,
see to find paper at http://www.newenergytimes.com/
9. El Boher et al, Proceedings of ICCF11, see Ref. 4.
10. V. Violante et al, Proceedings of SIENA 2005 Workshop, see Ref. 6.
11. Y. Arata et al, II Nuevo Saggitore 20, 66-71 (2004).
12. Y. Arata et al, JJAP 37 (11), L1274 (1998).
13. Y. Arata et al, JJAP 38 (7), L774 (1999).
14. Y. Arata et al, JJAP 39 (7), L4198 (2000).
15. Y. Arata et al, J. High Temp. Soc. Japan 29, 1-40 (2003).
16. M. McKubre et al, Proceedings of ICCF10, see Ref. 3
17. M. McKubre et al, Proceedings of ICCF11, see Ref. 4
18. Y. Isobe et al, JJAP 4 1 , 1546 (2002).
19. L. Case, Catalytic fusion of deuterium into helium-4, Proc. ICCF7, Vancouver (1998).
20. M. McKubre et al, Excess power observations in electrochemical studies of the D / P d
system, Frontiers of Cold Fusion, Proc. ICCF3, Nagoya (1992), see http://www.lenr-
canr.org/ Library.
21. M. McKubre et al, Development of advanced concepts for nuclear processes in
deuterated metals, EPRI-Report (1994), see http://www.lenr-canr.org/ Library.
22. Y. Isobe et al, JJAP 4 1 , 866-870 (2002).
23. R. George, see Ref. 6.
24. R. Stringham, 1.6 MHz sonofusion device, Proc. ICCF11, see Ref. 4.
25. Y. Iwamura et al JJAP 4 1 , 4642 (2002).
26. Y. Iwamura et al, Proc. ICCF10, see Ref. 3.
27. Y. Iwamura et al, Proc. ICCF11, see Ref. 4.
24
X I N G Z. LI
Department of Physics, Tsinghua University, Beijing 100084, China
E-mail: lxz-dmp@tsinghua.edu.cn
The progress of the Condensed Matter Nuclear Science reported during ICCF-12 is
summarized with emphasis on reply to the DOE review in 1989 and in 2004. The 18
reviewers might not be aware of the new achievement in the Advanced Technology
Research Center, Mitsubishi Heavy Industries; hence, their conclusion should have
been more positive toward this research. Arata's DS-reactor and the "heat after
death" experiment should change the conclusion about the "excess heat" and its
prospect. Various fundamental researches have shown the consistent nature in
understanding. A cost effective and comprehensive study is mentioned.
26
27
the three key elements to reproduce his discovery, i.e., the nuclear transmutation
induced by deuterium flux. He found that X-ray photoelectron spectroscopy was
the most suitable in-situ diagnostic tool to monitor the nuclear transmutation. His
supervisor was so judicious to allow him traveling between Yokohama and Kobe in
every week in order to continue his study. Indeed he was so brave to try the high Z
element as a candidate to interact with the low energy deuterium gas; and he was so
patient to wait for weeks in order to observe the nuclear transmutation. When his
methodology was established, he was able to send his sample to France for the SIMS
(time-of-flight) analysis; and send his sample to SPring-8 for microbeam analysis.
Moreover, professor Takahashi of Osaka university was able to use his method to
make sample, and use the Neutron Activation Analysis to verify the product of
the nuclear transmutation (Pr). 5 Now Mitsubishi Heavy Industries is collaborating
with Naval Research Laboratory (NRL) in US in order to use NRL's Trace Element
Analysis Mass Spectroscopy equipments. The Disclose Agreement between MHI and
NRL restricted the information flow before the publication; however, we might still
learn from Drs. Iwamura, Narita, and Yamada's presentations. 6,7 The unidentified
peak was discovered using the microbeam. Possibly, it was lanthanum (La). It was
just the element between Cs and Pr. It might imply that Cs was added a deuteron
first; then, one more deuteron was added to reach the Pr. Moreover, if we look at
the natural abundance of lanthanum, there is only one stable isotope for lanthanum
with a little mixture of long life-time isotope (0.09%, 1.05 x 10 11 years). This is
very similar to the praseodymium which has only one stable isotope as well. Indeed,
terbium (Tb) and thulium (Tm) were discovered in the early Electron Probe Micro-
Analysis experiment also when we tried to identify any new elements in the sample
of palladium hydride. 8 To my surprise, Tb and Tm have only one stable isotope as
well (see Table 1).
La Ce Pr Nd Pm Sm Eu Gd Tb Dy Ho Er Tm Yb Lu
99.91 100 100 100
replied with humor "I am a conventional chemist." However, the most impressive
results are the four peaks in the distribution of nuclear products which appeared in
various experiments in the world (Refs. 10-12). The organizer of ICCF-12 made a
good program to arrange a minicourse presentation by Miley. It should be empha-
sized that both Miley and Iwamura used thin film samples and used super-lattice
complexes in their experiments.
Figure 1. About 140°C as a characteristic temperature was discovered in both Arata's Sauna
bath and an early Chinese correlation experiment where D2 gas was permeating Pd thin wall.
The DOE reviewers in 2004 asked the frequently asked questions in those excess
heat experiments: "The reviewers who did not find the production of excess power
convincing cite a number of issues including: excess power in the short term is not
the same as net energy production over the entire of time of an experiment; all
possible chemical and solid state causes of excess heat have not been investigated
and eliminated as an explanation; and production of power over a period of time is
29
a few percent of the external power applied and hence calibration and systematic
effects could account for the purported net effect."
As a supplement to against those criticisms, we may add one more experiment:
"Heat after Death" work. 15
M. Fleischmann's "Heat after Death" experiment in 1993 provided a compelling
estimate. His electrolytic cell was boiled to dry in 10 min. The vaporization heat
was so large (102.5 kJ) that all uncertainties in the other effects might be ignored
(22.5 kJ for input from electrolysis, 6.7kJ for heat transfer to ambient). The volume
of the palladium cathode was only 0.0392 cm 3 which is about 4.6 x 10~ 3 mol. Hence,
the most conservative estimate would be 18.8 MJ per mol of Pd (i.e. 195 eV per Pd
atom). Even if this amount of energy had have been stored in the palladium due to
some unknown mechanism during the long period of electrolysis, this would have
still be an anomalous "chemical" effect (if it is not a nuclear effect). Would the
reviewers still say "While significant progress has been made in the sophistication
of calorimeters since the review of this subject in 1989, the conclusions reached by
the reviewers today are similar to those found in the 1989 review," if they had paid
attention to this calculation.
resistance ratio and loading ratio was very complicated because there was no good
calibration for the high loading region where the sample was supposed to work, and
because the resistance depended on temperature while the temperature coefficient
depended on loading ratio also. The recommendation is that resistance ratio might
be still a good characteristic if we specified the temperature at which this ratio was
measured.
The careful study on the temperature coefficient of the resistance of the palla-
dium hydride revealed a possible phase transition in the high loading region which
might be just the region of interests for CMNS.
and the Preparata Medal. Professor Takahashi announced that there would be a
Joint Project between Italian and Japanese scientists to explore the possibility of
processing the nuclear waste using the nuclear transmutation induced by deuterium
flux. The first phase would be supported by 13 million Euros and followed by second
phase with 12 million Euros.
9. A Cost-Effective Study
Dr. Thomas O. Passell, the Co-Chairman of the ICCF-4, proposed further his
results in using discharge tube for excess heat detection. 24 He intended to use the
small size gas discharge tube to make a wide-range survey on various materials
for electrodes and gases while keeping the sensitivity and efficiency high enough.
When the government support is still a long way to go, he used his retirement
money to keep the project running. As a retired manager from the Electrical Power
Research Institute, he has been optimistic towards the future of the Condensed
Matter Nuclear Science.
Israel group represents an excellent private company to achieve constant progress
in excess heat with the best international collaboration (Mckubre of SRI, Violante
of INFN). 25 DOE's recommendation, "Emphasis should be placed on calorimetry
with closed systems and total gas recombination, use of alternative calorimetric
methods, use of reasonably well characterized materials, exchange of materials be-
tween groups, and careful estimation of systematic and random errors. Cooperative
experiments are encouraged to resolve some of the claims and counterclaims in
calorimetry", has been fully realized already.
10. Prospects
The situation is changing gradually towards favorable to Condensed Matter Nuclear
Science. The Journal of Fusion Energy, decided to accept the submission from
the Condensed Matter Nuclear Science.26 It has been mainly a hot fusion journal
edited by the former DOE officer (Dr. Steve Dean), and published by the famous
Springer Verlag. Springer Verlag even decided to publish an academic book about
the Condensed Matter Nuclear Science as well. This "New Physical Effects in Metal
Deuterides" would be disseminated eventually, and lead to a clean and sustainable
energy resource for the world.
Acknowledgements
This work is supported by the Natural Science Foundation of China (#10475045),
Ministry of Science and Technology (Division of Fundamental Research), and
Tsinghua University (985-11, Basic Research Funds). I would like address that we
are grateful to Professor A. Takahashi, Dr. Y. Iwamura, Professor K. Ota, and the
local organization committee for a very successful ICCF-12. It was well planned,
well organized and well programmed.
32
References
1. Cold Fusion Research, DOE/S-0073, A report of the energy research advisory board
to the united states department of energy (1989).
2. Peter L. Hagelstein, Michael C.H. McKubre, David J. Nagel, Talbot A. Chubb, and
Randall J. Hekman, New Phys. Eff. Met. Deuterides (2004).
3. U.S. Department of Energy Cold Fusion Review Reviewer Comments, http://www.
newenergytimes.com/DOE/DOE.htm (2004).
4. Y. Iwamura et al., Observation of surface distribution of products by X-ray fluores-
cence spectrometry during D2 gas permeation through Pd complexes, Presentation
ICCF-12, Yokohama, Japan, November 27-December 2 (2005).
5. T. Higashiyama, A. Takahashi et al., Replication of MHI transmutation experiment
by D2 gas permeation through Pd complex, in: P. Hagelstein, S.R. Chubb (eds),
World Scientific (New Jersey, 2006), Proc. ICCF-10, Cambridge, USA, 24-29 August
(2003).
6. S. Narita et al., Discharge experiment using P d / C a o / P d multi-layered cathode, Pre-
sentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005).
7. H. Yamada et al., Producing transmutation element on multi-layered Pd sample
by deuterium permeation, Presentation ICCF-12, Yokohama, Japan, November 27-
December 2 (2005).
8. G.S. Qiao, X.Z. Li et al., Nuclear products in a gas-loading D/Pd and H/Pd system,
Proc. ICCF7, Vancouver, Canada, April 19-24, ENECO, Inc., Salt Lake City, UT
(1998).
9. G.H. Miley, Overview of light water/hydrogen-based low energy nuclear reactions,
Presentation ICCF-12, Yokohama, Japan, November 27-December 2 (2005).
10. T. Mizuno, T. Ohmori and M. Enyo, Change of isotope distribution deposited
on palladium induced by electrochemical reaction, J. New Energy 1(1), 23
(1996).
11. T. Ohmori and M. Enyo, Iron formation in gold and palladium cathodes, J. New
Energy 1(1), 15 (1996).
12. J.O-M. Bockris, Histroy of the discovery of transmutation at texas A & M university,
in: Jean-Paul Biberian (ed.), World Scientific (New Jersey 2006) Proc. ICCF-11,
Marseilles, France, 31 October-5 November (2004), p. 562.
13. Y. Arata and M.J.A.Y.C. Zhang, Development of 'DS-Reactor' as the practical reactor
of cold fusion based on the 'DS-CelF with the 'DS-Cathode', Presentation ICCF-12,
Yokohama, Japan, November 27-December 2 (2005).
14. X.Z. Li, Jian Tian et al., Correlation between abnormal deuterium flux and heat flow
in a D/Pd system, J. Phys. D: Appl. Phys. 36, 3095 (2003).
15. M. Fleischmann and S. Pons, Calorimetry of the Pd-D20 system: from simplicity via
complications to simplicity, Phys. Lett. A 176, 118 (1993).
16. A. Kubato et al., Development and experiments on a flow calorimetry system, in: M.
Okamoto (ed.), Proc ICCF-6, Toya, Japan, 13-18 October (1996), Vol. 1, p. 52.
17. G.H. Miley et al, Quantitative observation of transmutation products occurring in
thin-film coated microspheres during electrolysis, in: M. Okamoto (ed.), Proc ICCF-
6, Toya, Japan, 13-18 October (1996), Vol. 2, p. 629.
18. Y. Iwamura et al., Correlation between behavior of deuterium in palladium and occur-
rence of nuclear reactions observed by simultaneous measurement of excess heat and
nuclear products, in: M. Okamoto (ed.), Proc. ICCF-6, Toya, Japan, 13-18 October
(1996), Vol. 1, p. 274.
19. M.C.H. Mckubre et al., Using resistivity to measure H/Pd and D/Pd loading: method
and significance, Presentation ICCF-12, Yokohama, Japan, November 27-December 2
(2005).
33
G E O R G E H. M I L E Y
Department of Nuclear, Plasma and Radiological Engineering, University of Illinois,
103 S. Goodwin Avenue, Urbana, IL 61801, USA
E-mail: ghmiley@uiuc.edu
P R A J A K T I J. S H R E S T H A
NPL Associates Inc., 912 W. Armory Avenue, Champaign, IL 61821, USA
E-mail: pshresth@uiuc.edu
This paper reviews light water and hydrogen-based low-energy nuclear reactions
(LENRs) including the different methodologies used to study these reactions and
the results obtained. Reports of excess heat production, transmutation reactions,
and nuclear radiation emission are cited. An aim of this review is to present a
summary of the present status of light water LENR research and provide some
insight into where this research is heading.
1. Introduction
This review focuses on the transmutation reactions and excess heat production in ex-
periments using light water electrolysis or hydrogen gas/plasma loading undergoing
low-energy nuclear reactions (LENRs). Although most LENR ("cold fusion") re-
search has focused on heavy water, a considerable number of experiments have used
light water electrolysis or hydrogen gas loading. A few experiments have attempted
to compare the results from light versus heavy water, 1 - 4 but these comparisons
remain inconclusive.
There are a wide variety of cold fusion nuclear reactions. As shown in Fig. 1,
the original Pons-Fleishmann (P-F) reaction involved DD fusion, where unlike in
hot fusion, the reaction channel is "interrupted" through deactivation of the excited
He4 reaction product by energy transfer to the host lattice, ultimately heating the
lattice. Alternately, a number of researchers have reported transmutation reactions
that involve interactions between deuterium (or hydrogen) directly with atoms in
the host lattice, typically heavy metals. This branch of "cold fusion" is commonly
termed LENR, although recently there has been a move to also term P - F type DD
reactions as LENRs as well.
The observation of nuclear reactions between electrolyte and host metal atoms is
quite unexpected due to the very large coulombic barrier involved (much larger than
for D-D reactions). Consequently, one purpose of this review is to bring together
much of the data accumulated on this striking new phenomenon. The readers are
34
35
left to decide for themselves if the data is adequate to establish the case for such
reactions and possibly to formulate new experiments that build on and extend this
data base.
About 40 publications were included in this review (see references herein). This
was intended to be representative but not exhaustive of the field. Researchers
wishing to add information to the data base are invited to contact the authors.
D-D Reactions
% branching
hot fusion "P—F" type
T +p 50 < 0.1
D - D - > He-3+ n 50 < 106
He-4 + gamma < 10 99+
LENRs
p + metal —fc- products or "fission" product array
Figure 1. Comparison of LENR reactions and DD reactions occurring in hot and "cold" ( P - F
type) fusion.
1.1. Methodology
A summary of various methods employed for this study is given in Table 1. A
majority of the researchers cited used electrolysis to study LENR: Pd/Pt, Ni/Pt
were commonly used electrodes. K2CO3 is a popular choice as an electrolyte, a
trend perhaps started by the Mills and Kneizy's early experiments where extremely
large reaction rates were reported. Gas loading is also frequently used while a few
researchers have reported using a glow discharge (GD) plasma.
Electrolysis Total
Electrode
Pt/Pd 14
Pt/Ni 5
Pt/W 3
Pt/Au 4
Pt/Sn 1
Pt/Re 1
Pt/Ti 2
Pt/Ag 1
Pt/Pt 2
Electrolyte
K2CO3 10
H2SO4 3
Na2C03 5
Li2S04 4
KOH 1
Na2S04 5
CS2SO4 1
H20 2
GD plasma 1
Gas loading 5
and Iorio used SEM to study transmutation products. 9 Arapi et al. used TOF-
SIMS for product analysis. 5 Iwamura et al. used XPS extensively in their studies,
although they concentrated on D2 gas experiments (versus H2), so are not included
in this survey per se. 36
2. Results
2.1. Transmutation Products
A quantitative measure of the yield of transmutation products (and isotopic shifts
from natural distribution in key products) in four major atomic groups (6-18, 22-35,
44-54, and 75-85) were obtained by Miley et al.1 Others also have reported sig-
nificant nuclear reaction products and isotopic shifts in light water LENRs. In
some cases of the observed elements were from the lanthanide group, including
Lu, Tb, Pr, Eu, Sm, Gd, Dy, Ho, Nd, and Yb. It is widely accepted that these
rare earth elements are less likely to be found as impurities, strengthening confi-
dence in their results (although most researchers have tried to rule out mistakes
due to impurities versus the common "product" elements such as Fe, Cu, Ag,
Zn, Au, etc via analysis of cell components, electrodes and electrolyte prior to
LENR runs).
37
Isotopic shifts are another key feature often cited against mistaken identifica-
tion of impurities as reaction products. Violante's study showed that the 6 3 Cu/ 6 5 Cu
isotopic ratio shifted.33 In this Ni-hydride film work the most abundant copper iso-
tope was 65 Cu with a shift from natural distribution by f360%. Cirillo and Iorio
found Re, Os, Au, Hf, Tl, Er, and Yb on the surface of the cathode, which was not
present before the reactions. 9 Ohmori et al. reported finding Hg, Kr, Ni, and Fe
with anomalous compositions in Au electrodes during light water electrolysis.29 In
addition Si, Mg with other anomalous compositions were also detected in the precip-
itates separated from the Au electrode after electrolysis at extremely high current
densities. They found significant deviations from natural values. Minor product
elements such as Os, W, and Ru in particular showed large deviation, whereas
elements with larger yields like Pb and Ag rarely showed significant deviations.
Yamada et al. also reported a large increase of Cr, Fe, Cu, and Ag in their
experiment where Pd was loaded with hydrogen gas. 35 Arapi et al. found Be and
Ni in heavy water while in light water LENR they report Li, Ba, and Ni. 5 Dash et al.
reported formation of Au and Ag in both light and heavy water LENR; however,
the concentrations were somewhat higher in the heavy water experiments. 10
Table 2 summarizes the list of elements observed in light water by the number
of times they were reported being produced in their research by different research
groups. Fe and Cu were commonly observed. Rare earth elements were reported
less frequently. Also note that a majority of the transmutated elements reported
have changes in their isotopic composition from the natural abundance.
It is interesting that the frequency of observation of light water LENR elements
is not significantly different from heavy water LENR (for the latter see Ref. 37).
Table 2. The total numbers of reports that state the elements were
produced in their experiment
One way to evaluate this data is to consider a confidence level of >6 observations.
Then Ni, K, Ca, Cr, In, Cu, and Fe meet the criteria (Fig. 2). However, it can be
argued that the potential impurity levels for some of the less frequently observed
elements are very low, raising the signal/noise confidence level for those observations
despite their less frequent observation.
38
Figure 2. This graph shows the frequency of observation for various transmutated elements des-
ignated by atomic number.
steam leaving the cell; energy lost by thermal and electromagnetic radiation; and
loss of heat through the insulation. 9
Dash et al. have performed extensive light-water experiments and report that
excess heat generated in their light water LENR experiment was only slightly lower
than in "equivalent" heavy water experiment. 10 In their pioneering studies Mills and
Kneizys reported 130 mW of excess heat. 18 Noninski repeated Mills and Kneizys
light water Ni electrode experiment independently and reported 26-160% excess
energy compared to input energy.23 Dufour et al. reported excess energy of 7mW in
their H 2 gas loading experiment, corresponding to —25-30% of the input energy.13
Ohmori and Enyo reported 907mW of excess energy in a K 2 C 0 3 , Sn electrode
electrolysis experiment. 32 Fujii et al. reported having excess energy of 7.8 W in a
Li2SC>4, Pd/Ni electrode electrolysis experiment, which is more than 5% excess. 14
However, this excess heat was always reproducible.
It is not conclusive whether using light water or heavy water produces more
excess heat. Some research has reported that heavy water produced relatively larger
excess heat and more transmutation products, 7 ' 1 0 while some have indicated that in
both cases the excess heat and reaction products were similar. 31 Direct comparison
is complicated since many parameters are modified with an electrolyte substitution.
Thus, much work is required before carrying out a meaningful comparison.
The excess energy for light water/H 2 LENR reported by various researchers
tends to be either low (<10%) or high (>25%), with few reports of intermediate
values (see Table 3, Fig. 3). More quantitative analysis is required to understand if
this "two tier" result has a basic cause.
0-5 2
6-10 2
11-15 0
16-20 0
21-25 1
26-30 3
31-35 0
35+ 2
This suggests that some time was required for researchers to digest the early
work and become interested in devoting time to this new area of LENR.
3. Theory
Many different theories have been proposed for the mechanism of reactions that
takes place in LENR. However, a definitive match of theory and experiment has yet
to be achieved. Thus the "best" theory remains unclear. In order to explain how
the large Coulombic barrier is overcome, many theories introduce a neutral particle
in the reaction matrix. Some of the theories of this type include Neutron Cluster
formation by Fisher, 40 Free Neutron Reactions by Kozima, 41 R-Matrix Theory by
Chubb, 42 Shrunken Hydrogen by Mills,43 Electron-Proton capture by Stoppini 44
and Proton/Deuteron Cluster by Dufour.45 The challenge now is to sort out how any
of these theories can explain the unique signatures of heat and varied transmutation
products reported experimentally.
Table 4. Survey of the year and the key signatures of LENR focused in the study
Years
Type of study 1990-1994 1995-1999 2000-2005 Total
4. Conclusions
Acknowledgments
We would like to t h a n k all the researchers in the field who has provided significant
contribution in preparation of this paper. This work was partially supported by a
grant from the New York Community Trust.
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Prog. New Hydrogen Energy 2, 629 (1997).
2. J. Dash, G. Noble, and D. Diman, Trans. Fusion Technol. 24, 299 (1994).
3. J. Dash, G. Noble, and D. Diman, Surface Morphology and Microcomposition of Pal-
ladium Cathodes After Electrolysis in Acidified Light and Heavy Water: Correlation
With Excess Heat, ICCF 4, Lahaina, Maui (1994).
4. J. Dufour, J. Foos, J.P. Millot, and X. Dufour, Fusion Technol. 31 198 (1997).
5. A. Arapi, R. Ito, N. Sato, M. Itagaki, S. Narita, and H. Yamada, Experimental ob-
servation of the new elements production in the deuterated and/or hydride palla-
dium electrodes, exposed to low energy DC glow discharge, ICCF-9, Tsinghua Univ.,
Beijing, China, May 19-24 (2002).
6. R.T. Bush, Fusion Technol. 22, 301 (1992).
7. C.S. Cano, Comparison of Heat Output and Microchemical Changes of Palladium
Cathodes under Electrolysis in Acidified Light and Heavy Water, MS Thesis, Portland
State University (2002).
8. C.H. Castano, A.G. Lipson, S.O. Kim, and G.H. Miley, Calorimetric Measurements
during Pd-Ni thin film-cathodes Electrolysis in L12SO4/H2O Solution, Proc. ICCF-9,
Beijing, China, pp. 24-28, May 19-24 (2002).
9. D. Cirillo and V. lorio, Transmutation of metal at low energy in a confined plasma in
water, ICCF11, Marseille, France (2004).
42
10. J. Dash and G. Noble, Intern'l. Symp. On Cold Fusion and Advanced Energy Sources,
Belarusian State University, Minsk, Belarus, May 24-26 (1994a).
11. J. Dash and D. Chicea, Changes In The Radioactivity, Topography, And Surface Com-
position Of Uranium After Hydrogen Loading By Aqueous Electrolysis, ICCF-10, Cam-
bridge, MA (2003).
12. M. Di Giulio, E. Filipppo, D. Manno, and V. Nassisi, Intrn'l J. Hydrogen Energy 27,
527 (2002).
13. J. Dufour, J. Foos, and J.P. Millot. Measurement of Excess Energy and Isotope For-
mation in the Palladium-Hydrogen System, ICCF-5, Monte-Carlo, Monaco: IMRA
Europe, Sophia Antipolis Cedex, France (1995).
14. M. Fujii, S. Mitsushima, N. Kamiya, and K.Ota, Heat measurement during light water
electrolysis using Pd/Ni rod cathodes, ICCF9, Beijing, China, May 19-24 (2002).
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ICCF-8, Italy, 147 (2000).
16. X.Z. Li, Y. Deng, Y.J. Yan, H.F. Huang, W.Z. Yu, and C.X. Li, J. New Energy 6, 1,
80 (2001).
17. G.H. Miley, Product characteristics and energetics in Thin-Film electrolysis experi-
ments, Proc. ICCF-7, Vancouver, Canada, 241, April 19-24 (1998).
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43
1. Introduction
In order to understand the function of the Double Structure Reactor (DS-reactor),
it is important to know the principle of DS-cell/DS-cathode. 1 DS-cell is constructed
with electrolyte ( D 2 0 / H 2 0 + LiOH) and DS-cathode together with Pt-cylindrical
anode, and structure of DS-cathode is constructed with closed Pd-cylinder in
which sample (nano Pd/Zr3NiO/Pd black, ...) is kept inside ultrahigh vacuum
hollow space. When DS-cell is electrolyzed, the vacuum hollow space is filled up
easily with ultrahigh pressure gas (D 2 /H 2 : 10 3 -10 4 atm) and the innumerable
solid "Pycnodeuteriums" are produced inside the Sample.2 We discovered that the
"Pycnodeuterium" cause easily nuclear reaction ("cold fusion") using not only DS-
cell but also laser welding solid fusion reactor, sonoimplantation solid fusion reactor,
44
45
which were invented by us. However, these devices gave "bad efficiency; that is,
their input energy was too large. Figure f shows principle of "DS-cell" and it will
be given intuitive understanding for the principle. 3
©
t
ID
1-
2-
<>
Samples enclosed This white space becomes
inside high vaccum ultrahigh pressure Ds gas
Pd vessel (~104 atm) in this patent
Q DS-cathode
(Pd-olosed cylinder)
© Anode
(Pt-cylinder)
Heater Heater
Pd vessel
• Stainless
steel vessel
DS-reactor
Figure 2. "DS-reactor" was developed based on the "DS-cell", that is, the same principle in both
methods. "DS-reactor" corresponds to "DS-cell" without electrolyte, and it is considered that
"DS-reactor" includes A- and B-systems.
47
Condition
( No sample + D2 )
Pd vessel
• ^ Sample: no sample
05/10/11-12 (purs Dj)
Heat-Current \
•o
3
120 180 240 300 360 420 480 540 600 660 720 60 120 180 240 300 360 420 480 540 600 660 720
3. Experiment
3.1. "Experiment-1" ([A]: No Sample + D2)
Figure 3 shows the results in the first set of the experiment. ("Experiment 1", [A]).
In this case, inside the Pd vessel (white zone) is vacant (no sample) and D2 gas
48
filling up with 40 atm as the outside pressure (P ou t) of Pd vessel (gray zone) as the
set-conditions before the experiment.
When D 2 gas under P o u t of 40 atm is heated to 140°C as the giving temperature
(Tout = 140°C), Pd vessel is heated by such D 2 gas accordingly, temperature of Pd
vessel never goes higher temperature than the D 2 gas. When Pd vessel reaches
to 70-100°C, D 2 molecules passing through the wall of Pd vessel as D + and enter
inside the Pd vessel as D atom and becomes to mixed gas [D + D 2 (= D + D)] as
time passes.
As a final result, inner temperature of Pd vessel (white zone), T;n, never exceed
the outer temperature as the giving temperature of the D 2 gas (gray zone), T o u t ,
that is always T out > T-m. These results were exactly confirmed by the experiment
shown in Fig. 3, Namely, experimental results of left side AQ in Fig. 3 indicates the
relation between D 2 gas pressure (P ou t = 40 atm) and temperature (T out = 140°C),
which were supplied into the outside Pd-vessel (gray zone) and the penetrated inner
D(D 2 ) gas pressure {P-m) and temperature (Tin) inside the Pd vessel (white zone), In
other words, ( P n , T in ) never exceeds (P ou t, T o u t ): always P i n < P o u t and T in < T o u t .
On the right-hand side Ai, only the scale of the temperature axis of Ao shown on
left-hand side is enlarged to give distinct difference between Tout and T-m.
120 180 240 300 360 420 480 540 600 660 720 0 60 120 180 240 300 360 420 480 540 600 660 720 7
Figure 4. Comparison between figures A and B (Ai is the same with Ai in Fig. 3).
49
-^ out ^ -^ in-
And both temperatures were never reversed. This result is extremely important.
We have expected that nano Pd is far better than Pd black as a sample because 1,2
we have obtained that nano Pd generated excess heat with much higher rate than
D
( Sample: Pd black; gas: D; Sample: nano Pd + D2
" \ W • :
N
— Sample: Pd black »
05/10/11-12 (pure D2)
141 /"in
140
139
ff 'out
/ Heat-Current \
\ stop )
-0 O TO
Pout ? ?
13R ^ ™
. - Tl CD ^3
=s
137
^^--^ CO
136 m 2.
Q-
: tem
sure
135
Pi
134
v a h-°
hf 133 -! h~,-
'
132
131
/
0 60 120 180 240 300 360 420 480 540 600 660 720 780 840 ) 120180 240 300 360 420 480 540 600 660 720 780 840
No sample + D2
Sample + H2
Sample
4. Conclusion
Figure 7 shows the conclusion of the experiments already described, and demon-
strates the present situation of "DS-reactor" as the practical reactor of "cold-
fusion". From the left-hand side of the horizontal line, the thick black and thin
black dots correspond to Experiments 1-4.
The vertical axis represents the T;n, which is inner temperature in the gray zone
of the DS-reactor. For Experiments 1 and 2, Tjn's are lower than T o u t , that is, the
efficiencies are always negative.
For Experiments 3 and 4, T in *'s are higher than the given temperature T o u t .
This means that these efficiencies were always positive and moreover, almost of the
input energy was collectable.
It is emphasized that T;n for Experiments 1 and 2 are always lower than T o u t and
higher for Experiments 3 and 4. The excess energy obtained with the Experiments
3 and 4 should come from deuterium nuclear fusion reaction. What else explanation
exists for this result? Chemical reaction energy is very small and never gives the
explanation. We concluded that this should come from fusion. Also it is considered
that the "DS-reactor" demonstrated to reach the practical level with high efficiency.
It was concluded that the principles of the DS-reactor is the same as that
of DS-cell with "DS-cathode", and the "DS-cell" was an excellent system to
52
Outer vessel
Generation of nuclear
Pd vessel /Nano Pd\
energy inside Pd-vessel
(outer vessel) V D2 gas /
/Pdblack\
\ D2 gas /
Temperature given to
outside (D2/H2 gas) (7 0u t> 100°C)<8>
of Pd-reactor vessel ®
- Actual basic line
I Pd black\ for (sample + D 3 gas)
D 2 gas /
Tin
Never nuclear reaction
demonstrate exactly the existence of cold fusion, but gives a bad "efficiency" as
a reactor, because in DS-cell, electrolyte is used essentially, then the most of the
input energy is consumed inside the electrolyte itself, and then consequently, the
"DS-reactor" which is "DS-cell" with no electrolyte will be utilized as a Practical
Reactor.
/^->
Tcout
Heater
160-, Sample: Pd black; gas: D2 0.8
-24
0.5- -16
Temperature (°C)
100-
Current (A)
-14
80-
60-
0.4- -12
0.3-
-10
1
-8
Current /
40 H 0.2- - 6
- -4
20- Input power Win 0.1-
- 9
0- 1 • • 0.0- - 0
*
c 50 100 150 200 250 300
Time (min)
Figure 8. Characteristics of controlling current (input power) to make the constant "giving
temperature".
reacted is injected into the "QMS". The period between B and C shows a part of
M4-spectrum of the reacted gas, (the gas volume 5 Torr cm 3 ) which was injected
to the special gas tank (volume 2000 cm 3 ) with Getter pump and the high vacuum
10~ 8 Torr, and the gas was kept inside the tank, 3 min, then the gases were injected
into "closed QMS" (which was developed and published by us in 1995), And one
pair spectrum of M4 (4He, D2) was more exactly shown in the period between C
and D. The period from D to E exhibits the spectrums, 15 min, after starting, and
remained almost of only He.
54
8x10"
c
CD
4x10" 12
Figure 9. Spectral analysis of the inner gases in the "DS-reactor" using sample (Pd black) and
D 2 gas.
Acknowledgments
References
1. Y. Arata and Y. C. Zhang: Proc. Japan Acad., 70B, 106 (1994); 71B, 304 (1995); J.
High Temp. Soc. Jpn. 20, 148 (1994); (Special Vol.) 23, 1-56 (1997); (Special Vol.) 29,
1-44 (2003); Jpn. J. Appl. Phys. 37, L1274 (1998); 38, L774 (1999); 39, L4198 (2000).
2. Y. Arata and Y. C. Zhang: J. High Temp. Soc. Jpn. (Special Vol.) 29, 1-44 (2003); Y.
Arata, II Nuovo Saggiatore (Italy phys. Soc) 20, 66 (2004).
3. Y. Arata, Methode of producing ultrahigh pressure gas, US-Patent, No.5, 647, 970
(1997).
4. 21st. Century Science and Technology, Summer (21st Century Science. Associates,
Washington DC, 1995), p. 37.
P R O G R E S S IN EXCESS OF P O W E R E X P E R I M E N T S W I T H
ELECTROCHEMICAL LOADING OF D E U T E R I U M IN
PALLADIUM
V. V I O L A N T E A N D S. M O R E T T I *
Associazione EURATOM-ENEA sulla Fusione, Centro Ricerche Frascati, C.P. 65-00044
Frascati, Rome, Italy
E-mail: crescentini@frascati.enea.it
M. B E R T O L O T T I , E. C A S T A G N A , A N D C. SIBILIA
Universita di Roma "La Sapienza" Dip. di Energetica. Via A. Scarpa, 14, Rome, Italy
F. SARTO
ENEA, Centro Ricerche Casaccia Rome, Italy
M. M C K U B R E A N D F . T A N Z E L L A
SRI International, 333 Ravenswood Avenue, Menlo Park, CA 94025, USA
I. D A R D I K , S. L E S I N , A N D T. ZILOV
Energetics LLC, 7 Fieldview Lane, California, NJ, USA or Energetic Technologies, Omer
Industrial Park, Israel
A research activity has been carried out, during the last 3 years, in the field of
triggering anomalous heat effects in palladium deuteride. An enhancement of the
excess of power reproducibility in deuterated palladium was obtained by using
He—Ne Laser irradiation during electrochemical loading. A preliminary correlation
between excess of energy and 4 He concentration increasing above the background
was found. The continuation of the experimental program confirmed that Laser
triggering produce an interesting gain of reproducibility. An upgrade of the exper-
imental set-up has been realized.
1. Introduction
The material science research oriented to improve the effect of excess of power pro-
duction into palladium cathodes loaded electrochemically with deuterium confirmed
that the high concentration of deuterium into the lattice (d/Pd > 0.9) is a neces-
sary condition to observe the phenomenon but not enough. Several research groups
have been working in order to identify the most appropriate techniques to trigger
*ENEA guest.
55
56
such an effect. The study presented in this work is leading with the development
of the triggering by means of Laser irradiation during the electrochemical loading
of palladium with deuterium in heavy water electrolyte.
An isoperibolic calorimetric system has been developed allowing a Laser irradi-
ation during the electrochemical loading.
According to the idea that collective electron oscillations have a key role in
LENR processes a proper trigger has been introduced to create surface plasmons
(polaritons). 1
Laser triggering was selected because of it results to be the most appropriate
under electrochemical loading. Plasmons are longitudinal plasma oscillations that
do not couple with external radiation. A proper surface corrugation may produce
such a coupling between the electronic oscillation and the external radiation. For
such a reason, a proper acid etching has been done on the Pd samples used as
cathodes into the electrochemical cell. In addition to that one may consider that
a p-polarized Laser beam is the appropriate one to create charge separation on the
surface of the specimen.
PT100-- PT100
SS cap and ring
Glass
window
for laser
beam
Teflon cell
2. Experiments
The electrochemical cell (Fig. 1), tested for He leakage (2 x 10~ 10 mbar 1/s),
equipped with two small glass windows was placed into a thermostatic box (Fig. 2)
(±0.15°C) also equipped with a window for the Laser beam (5 or 33 mW, 632 nm).
The closed electrochemical cell is equipped with a recombiner. Cell power supply is
an AMEL galvanostat, modulated, during the HI-LO current mode by an HP 33120
wave function generator. Output power is measured by means of the calibration
performed by means of the average temperature given by the PT100 thermometers
57
mm Temperature monitor
wi Multimeter
Data acquisition
'—- switch unit
LCR meter 1—
Wave generator
.... ff- Laser
Box
Galvanostat
Calibration 25-5-2004
^—*
^^^^"^
o ^^--Jr'
S_ 30- —*-T (average)
^ " - — Pdi. (T (average))
20-
10-
( 1 2 3 4 5 6
Pin ( W )
An improvement of the system was carried out both to increase the number of
thermometers into the cell and to use high ultra-vacuum technology for the cap and
the glass windows of the cell.
A particular effort was done in order to take into account the convective heat
exchange due to the electrolyte fluid dynamics due to the gas bubble formation
during the electrochemical process.
Laser 4 experiment was carried out by applying a continuous electrochemical
current. After achieving a loading threshold of 0.95, the cathode was continuously
irradiated by using a 632 nm, 33 mW red Laser. Calorimetry gave 30.3 kJ of
produced energy (19.4 MJ per mol Pd). Figure 4 shows the input and output
power and energy evolution after applying the Laser irradiation.
The gas produced at the electrodes (Pd foil cathode and Pt wire anode) acts
on the electrolyte producing a fluid dynamic regime that affects the temperature
distribution, then the temperature field for the considered cell results to be correctly
described by including the convective terms into the heat transfer equation:
dT ( dT dT dT\
div(Xgrad(T)) + Q = pcp— + pcp [Vx— + Vy— +Vz—j, (1)
Assumptions
• 3D transient.
• Isotropic (Kx = Ky = Kz).
59
Gas velocity Va2 is calculated by means of the current density. Let us assume
the cathode to be a Pd foil having height h and width L. The bubbles of hydrogen
form a layer that we measured to be S (2-3 mm) in our cell configuration. The laws
of Faraday and of the gas give
8.00
;-4= 7.50
6.50
6.00
5.50
5.00
4.50
4.00
3.50
3.00
2.50
Ilr-
mm_ 2.00
1.50
••--- 1.00
0.50
0.00
Figure 6. Velocity field into the electrochemical cell due to bubbles at the cathode.
The approximate solution will be carried out by solving iteratively the two equations
with the following assumptions:
• axial symmetry,
• density and viscosity be constant,
• steady state,
• negligible effect of pressure and mass.
The velocity of the liquid in contact with gas is estimated as 3 - 5
VA IO„B
12/^
0.093, (8)
V? ii + 7/iiE
K
where
9 x 106 Pa s,
(9)
= 1.095 x 1 0 ~ 3 P a s ,
then
V* 0.093V1 (10)
61
Step 1:
Step 2:
1 C/V (Jl)
-vr + — h -7-^ = 0 (continuity equation). (13)
r o r oz
By calculating the derivative of w^and by taking into account that VQ(Z) = Kz/6,
dvz K InR K lnr K\n{r/R)
(14)
dz 5 In (a/R) 5 In (a/R) 5 In (a/R):
the substitution of (14) into the continuity equation leads to
()_C1n_ JTr-[21n(r/r)-l]
Vr{r
>- r 46ln(a/R) ' '(15)
The integration constant is calculated by imposing the condition of zero flow rate
in radial direction
J~~l_ Ifl sX
Temp on
max: 314.9
q: 314.0
p: 313.0
o; 312.0
n: 311.0
m: 310.0
I: 309.0
k: 308.0
j : 307.0
i: 306.0
h: 305.0
g: 304.0
f; 303.0
e: 302.0
d: 301.0
c: 300.0
b: 299.0
a: 298.0
0 3 6 min: 297,7
Model
P(W)
of the electrolyte is included into the system description, in particular for power
values larger t h a n 2 W.
A new experimental campaign has been carried out giving one excess of power
production over two experiments. T h e excess of power is shown in Fig. 9. T h e
effects started after achieving a loading around D / P d = 0.94 and survived, under
Laser irradiation for more t h e n 100 h. T h e maximum gain was about 15% of the
input. T h e excess was stopped by current inversion t h a t produced a fast de-loading.
After de-loading the difference between the input and the o u t p u t power disappeared.
T h e effect is clearly shown in Fig. 9. T h e total energy gain was 49 kJ.
1-
49 kJ excess of Current
0.9
0.8
"W.WW
0.7
R/Ro<
0.6
- Pin (W)
5 0.5
Pout (W)
I 0.4
0.3
0.2
0.1
Time (h)
3. Conclusions
T h e results of the additional investigation performed with the new experimental
campaign are in good agreement with the results obtained into the first run of the
work. It is confirmed t h a t the relevant effect of the Laser trigger, under appropriate
conditions, to obtain excess of power production in deuterated palladium when the
D concentration is close to the literature threshold.
References
1. V. Violante et al., Analysis of Ni-hydride thin film after surface plasmons generation by
laser technique, in Tenth International Conference on Cold Fusion, Cambridge, MA:
LENR-CANR.org, 2003.
64
1. Introduction
The cell was placed inside a constant temperature air-cooled incubator (Yamato
1L-6) with the outer door open, and the inner Plexiglas safety door closed. The
event occurred in the first stage of the experiment before plasma normally forms.
Soon after ordinary electrolysis began, voltage was increased to 20 V and current
rose up to 1.5 A. Within 10 s, the cell temperature rose steeply up to 80°C and
a bright white flash surrounded the cathode. The light expanded to the solution
and at the same instant the cell exploded. The explosion blew off the Plexiglas
safety door and spread shards of Pyrex glass and electrolyte up to 5-6 m into the
surrounding area.
The cell is equipped with a magnetic stirrer and the fluid mixes rapidly. Three
separate platinum resistance temperature detectors (RTD) in the electrolyte all
recorded ^80°C just before the explosion. This means the water in the cell was
well mixed and the entire 700 ml volume of water heated up from 30°C to 80°C
in 10 s. This is 35,000 calories or 147,000 J, which is ~800 more energy than was
input into the cell before the explosion. Table 1 shows the rapid temperature rise
recorded by the three RTDs just prior to the explosion, and it also shows that the
fluid was well mixed.
The effluent hydrogen and oxygen were mixed in the cell headspace. (Note that
the inverted funnel described in Ref. 1 was not in use during this experiment.)
There were 2-3 cm 3 of free hydrogen at the time, although this is an open cell so
only minimal amounts of gas remain in the headspace. Oxygen gas and hydrogen gas
were also mixed in with the electrolyte solution. It is likely that the platinum mesh
65
66
anode catalyzed the hydrogen and oxygen to recombine rapidly in the electrolyte,
triggering the explosion in the headspace.
The vessel was old and may have had a scratch on the inner surface. It is possible
that the tungsten cathode may have been exposed to the gas in the headspace.
2. Experiment
2.1. Electrolysis Cell
Figure 1 shows the experimental setup, which is described in Refs. 1 and 2. We
measure many parameters including sample surface temperature, neutron and X-
ray emission, mass spectrum of gas, input and output power, and so on. Figure 2
shows the schematic sketch of the cell and gas measurement system. 1 ' 2 The cell is
made of Pyrex glass. It is 10 cm diameter and 17 cm in height and 1000 cm 3 in
solution capacity. It is closed with a Teflon rubber cap, 7 cm in diameter. The cap
has several holes in it, three for platinum resistance temperature detectors (RTD)
(Netsushin Co., Plamic Pt-100 Jl), two for the inlet and outlet of the flowing coolant
water, and one to hold a funnel that captures the effluent gas from the cathode. The
funnel is made of quartz glass, and is 5 cm in the diameter at the top of the cell, and
12 cm in length. Gas leaving from the top of the funnel flows into a water-cooled
condenser, which is connected to the funnel with another Teflon rubber cap.
\ ">VEimgen gas
Cooler inlet
Electrolyte cap
2.3. Calorimetry
Temperature measurements were made with 1.5 mm diameter RTDs. Calorimetry
was performed by combining the flow and isoperibolic method. Flow calorimetry
is based on the temperature change of the cooling water. The cooling water is tap
water flowing through Tigon tubing. It passes first through a constant temperature
68
bath to keep the temperature constant. Prom there, it flows through the outer
jacket of the condenser, and then through the coil of tubing wrapped around the
funnel. (The outside of this cooling water coil is covered with the anode, a platinum
mesh.) The flow rate is measured with a turbine meter (Japan Flow Control Ltd.,
model T-1965B). The inlet temperature is measured before the cooling water enters
the condenser, and outlet temperature is measured, where it exits the cell. Heat
from both condensation and glow discharge electrolysis is combined together.
Isoperibolic calorimetry is performed by placing three other RTDs in the cell
electrolyte at different depths in the solution to measure the temperature. The
solution is mixed with a magnetic stirrer.
Figure 3 shows the notional sketch for heat measurement. Heat out can be
divided into several factors. These are energy for water decomposition, heat of
electrolyte, heat bring by the coolant, heat releasing from the cell wall and heat
releasing with the vapor through the cell plug.
.it: • i
•i;j l o c i .v
'
• -
;i
f
,i, ^JL.,^J,
Hw: « « « % $ # JWfli
The heat balance is estimated by input and output formulas, input and output
power is given in the following equations:
Input (J) = I (current) x V (Volt) x t,
Out Hg + Hw + HC + Hx,
here
Wc is the coolant weight, Cc the heat capacity, and dT is the temperature difference.
gas generated were collected by a data logger (Agilent Co., model 34970A), and
stored in a personal computer.
Parameter change
300
1! 200
o
1 c
55
O =5
100
=>
0)
Q.
E
2 4
cf data ¥W 40803 # 1
Time (1000 s)
3. R e s u l t s a n d Discussion
Figure 4 shows the changes of input voltage, cell temperature, and current for a
typical experiment. Input voltage was usually increased stepwise from 0 V to more
than 100 V and then decreased to 0 V. The input current usually rose to a maximum
71
Parameter change
100 6
i - V
Current (A)
60 3
C
ro
O
40 2
llf
ro S ^
a. 20 1
£ //'
|2 /•
0 i /
i ^ i i •
1
'u
1! 0 15 0 190 210 2. 0 250
I""""""1 A !ime(s)
100 5
I
> — Terr
t»
80 4
-- Cur J\
f 60
-Volt
I \
3 g
1 \ 3
40 1 V^ 2 >
1
! 20
J- \
1
1
.
n * , i 0
c 23 A0 60 80 1 )0
| ddaia\\V»l24«l |
Time (s)
t
1E + 0 4 k /
•#• Input
/
F -©-Outpu t
5 1E + 03 /
B-
"3 | /
o /
1 1E + 02
i
1
1E + 01 y /
# ;*A
L
1 1 1
J 1 L_L_ L
20 40 60 80 100
However, the changes of temperature during the explosive reaction were different
from the usual experiment. The input voltage and current were 15 V and 1.5 A at
40 s, respectively; that equals 22.5 W, as shown in Fig. 8. The input power was
supplied for 10 s; total input was roughly 300 J. The electrolyte temperature rose
steeply from 40 to 60 s, within 20 s. After that, the electrolyte cell was shattered by
the sharp increase of inner pressure. The heat out was estimated 800 times higher
than the input power, based on the remaining output data.
,<^:
EDX aliased
1E + 04
1E + 03
^
1E + 02U 1 1 1 1 1 1 L
5 10 15
Energy (keV)
There were many elements deposited on the electrode surface. The major ele-
ments were Ca and S and the total mol was roughly estimated at 10~ 6 , as shown
in Fig. 10.
1E + 04
1E + 03
1E + 02 l-J 1 1 J I I ! I I I l_
5 10 15
Energy (keV)
- • 136Xe +50 C r+ n 7 4 Me y
138 48
-> B a + T i + 1 1 7 . 4 MeV
142
-• Ce + 4 4 Ca + 107.2 MeV
154
-• S m + 3 2 S + 7 9 . 2 MeV
^158Gd+28gi+727MeV
References
1. Tadahiko Mizuno, Tadayoshi Ohmori, Tadashi Akimoto, and Akito Takahashi, Pro-
duction of heat during plasma electrolysis in liquid, Jpn. J. Appl. Phys. 39, 6055-6061
(2000).
2. Tadahiko Mizuno, Tadashi Akimoto, Kazuhisa Azumi, Tadayoshi Ohmori, Yoshiaki
Aoki, and Akito Takahashi, Hydrogen evolution by plasma electrolysis in aqueous so-
lution, Jpn. J. Appl. Phys. 44(1 A), 396-401 (2005).
"EXCESS HEAT" I N D U C E D B Y D E U T E R I U M FLUX IN
PALLADIUM FILM
N. M U E L L E R , P. S C H O C H , A N D H. O E H R E
Inficon Limited, Alte Landstrasse 6, LI-9496 Balzers
Principality of Liechtenstein
1. Introduction
Early in 1989, G. C. Fralick et al., of NASA, USA conducted an important ex-
periment to search for the neutron radiation using gas-loading method in a D/Pd
system instead of electrolysis.1 They could not find any evidences for the neutron
radiation in a D/Pd system; however, they discovered unexpectedly the "excess
heat" in a D/Pd system. Thanks to J. P. Biberian, we became aware of this NASA
work after ICCF-11. This NASA experiment was very similar to our gas-loading
experiments, which have been conducted at Tsinghua University since 1989. 2 ~ 4 The
excess heat appeared in both our experiments and in NASA experiments whenever
deuterium gas was pumped out from the Pd samples. In our early work,2 we used
palladium wire only and heated Pd wire using the electrical current through it. G.
C. Fralick et al. utilized the Pd-alloy tube in a hydrogen purifier, and heated this
tube using an external electrical heater from outside of tube. Nevertheless, in W.
Wu and X. Z. Li's work,3 we utilized Pd tube also, but we heated the Pd tube using
electrical current through Pd tube. This is different from Fralick's heating from
external heater. On the other hand, X. Z. Li and J. Tian 4 were using an external
heater, but the pumping was done only at one side of the Pd tube. However, G.
C. Fralick et al. pumped deuterium gas from both sides of the Pd-alloy tube. We
now use a Pd disk heated by an external heater, and pump down from both sides of
the Pd film (Fig. 1). Although the configuration varied in various experiments, the
results are all similar, i.e., the "excess heat" appears while a deuterium flux leaving
palladium is created.
75
76
Swagelok connection
Thermocouple
Heating coil
Figure 1. A thin palladium film is sealed between two tubes using a Swaglok connection structure.
There are two small holes on the nut. Thermocouples are inserted into holes in order to measure
the temperature of the edge of the Pd film. The heating coil winding is wrapped around the nut
to hea.t the Pd film.
Figure 2. Hydrogen purifier is utilized as a palladium tube-deuterium system with heating ele-
ment wrapped in the insulator. The helical stainless tube on the top is for cooling the purified
gas.
77
With the assistance of INFICON R&D Laboratory, this NASA experiment was
repeated and the gas sample was analyzed using high-resolution quadruple mass
spectrometer. This paper would report the result of excess heat first. The result of
quadruple mass spectrometer analysis would be reported in another paper. 5
4. Discussion
The absorption of deuterium gas into palladium is an exothermic process. Hence,
the degassing of deuterium from the palladium is supposed to be an endother-
mic process. We were supposed to observe the temperature drop when we started
pumping. This was true, when the data acquisition system was able to catch that
78
short temperature drop just after the starting point of pumping. It was caused by
both the endothermic degassing and the adiabatic expansion. However, this short
drop in temperature was always followed by a temperature rising which was cor-
responding to the correlation between heat and deuterium flux. This phenomenon
was discovered in the study of gas-loading in palladium wire, 2 and was named as
"pumping effect". The careful study using high precision calorimetry confirmed this
phenomenon, and called it as correlation between heat flow and abnormal deuterium
flux.3,4 The early NASA gas-loading experiment provided a strong evidence to this
phenomenon unexpectedly.1 The collaboration with INFICON R&D laboratory has
made us even more confident about this phenomenon.
**
rf
\ \k ^ 1000
100
/ 10 "a
/
\t8 rong
pump ing
,
3
1 0.01 —
\ 1E-3
Stop pun. >ing
*
*•" "
1E-4
?S0-
' * " •
Jr 1E-5
20:09 20:38 21:07 21:36 22:04 22:33 23:02 23:31 24:00 24:28 24:57
Time
Figure 3. Solid line shows the temperature at the edge of the Pd film. Dash-dotted line shows
the pressure around the Pd film. The temperature started increasing when pumping was started.
However, temperature dropped later even if the pumping was continuing.
We may estimate the excess power in this pumping period. The resistance of
the heater was 433 fi at 330°C, it provides an effective heating power of 113 W
at 221.2 V. This heating power was able to maintain a temperature difference of
(330.2-24.0) = 306.2°C. Hence, the temperature difference of (339.8-330.2) =
9.6°C might imply an "excess power" of 3.5 W. The volume of the Pd film was
about 0.031 cm 3 ; hence, the power density for the palladium was about 114 W/cm 3 .
It is about the power density in a modern nuclear fission reactor.
Acknowledgments
This work is supported by the Natural Science Foundation of China (No. 10475045),
Ministry of Science and Technology (Division of Fundamental Research), and
Tsinghua University (985-11, Basic Research Funds).
References
1. G. C. Fralick et al., Technical Memorandum 102430 (1989).
2. X. Z. Li et at, The Proceedings of ICCF9, Beijing, China, May 19-24, 2002, Edited by
Xing Z. Li, Tsinghua University Press (2003), p. 197.
79
JEAN-FRANgOIS FAUVARQUE,
P I E R R E PAUL CLAUZON AND G E R A R D JEAN-MICHEL LALLEVE
Laboratoire d'Electrochimie Industrielle, Conservatoire National des Arts et Metiers, 292,
rue Saint Martin, F-75141 Paris Cedex 03, France
E-mail: fauvarqu@cnam.fr
A simple calorimeter has been designed that works at constant temperature; that
of boiling water. Heat losses can be estimated accurately with an ohmic heater. As
expected, losses are independent of the electric power input to the heater and the
amount of evaporated water is linearly dependant on the power input. The device
has been used to determine the heating power of a plasma electrolysis (the Ohmori—
Mizuno experiment). We confirm that in this experiment, the heat output from
electrolysis is greater than the electrical power input. The excess energy increases
as the electrolysis voltage is increased from 200 up to 350 V (400 W input). The
excess energy may be as high as 120 W.
1. Introduction
Our experiment is an electrolysis experiment made in plasma mode with a tungsten
cathode, a platinized titanium wire as an anode, and as electrolyte a water solu-
tion of potassium carbonate (K2CO3 at 0.2 M). In the same type of experiments,
Mizuno 1 ' 2 reported both excess heat and excess hydrogen production.
The explanations found in the bibliography for this phenomenon are, for
example, transmutations in the cathode material. 3 The abnormal observations are
concerned with the appearance of osmium, iridium platinum, and gold, without
quantitative measurements. 3
We thought it would be quite interesting to confirm these results with the help
of a simplified experimental setup.
2. Experimental
We decided to do our experiments at a constant temperature, the boiling point
of water, and to measure the heat emissions only by weighing the mass of water
in the experimental device. A water storage container inside the device allows us
to maintain the electrolyte at a constant water level, and thus keep the K2CO3
concentration constant. This container, being graduated, also gives us a way to
confirm the mass of water boiled off.
An interesting repercussion of this operating mode concerns the thermal losses.
Once the boiling temperature is reached and overall thermal stability is achieved,
80
81
the thermal losses, which depend only on the temperature, remain constant, and
this is true whatever thermal emissions are observed. This allowed us to hold the
experiment in a simple beaker of an appropriate size and then to avoid the of an
opaque Dewar vessel. This allows us to visually observe the cathode condition.
Finally, the use of an ohmic heater allowed us to bring the device at the suitable
boiling temperature and to maintain this temperature at this level much more
quickly than by electrolysis alone. We also verified that other sources of inaccuracy
were insignificant. For example, in the range of power used, the recondensation level
inside the device was low, and few unboiled droplets of water sprayed outside the
beaker. The excess heat that we were trying to measure is quite large (30-100%).
So, it is not necessary to obtain very precise measurements.
Glass tube
Distilled
water
Anode4
reserve
Ohmic
heater
Electrolyte
reserve 1 i
ooo.o g
((Sartorius)},^-
balance
Figure 1. Experimental setup. Electrolyte reserve is 2 1. The tripod used to hold components in
position is not shown.
82
The input energy was also frequently measured by use of the inlet voltage and
the mean current intensity as given by a recorder. These results were compared the
wattmeter data.
® A tungsten cathode of 2.4 mm diameter made with 2% of thorium (this
type of electrode is often used for commercial scale welding).
This cathode rod is shielded with a Pyrex tube. About 15 mm of the rod extends
out from the tube, where it is exposed to electrolysis. In some experiments, ceramic
tubes were used instead of Pyrex.
4.2. Results
We made a parametrical study on the influence of the voltage applied during glow
discharge electrolysis. The temperature was brought to the boiling point (100°C)
600
« 400"
0- 300
30 40
m (g/300s)
with the auxiliary resistance heater. Then electrolysis was begun at 200 V. This
high voltage is needed to produce a suitable plasma around the cathode. Plasma
generation is greatly enhanced by the high-electrolyte temperature. The Joule heat-
ing effect during electrolysis immediately gives rise to an envelope of steam around
the cathode, and a plasma, that is supposed to be hydrogen plasma according to
Mizuno. Table 1 gives the value of the COP, which is the ratio of the energy of
vaporization divided by the electrical energy supplied to the device (which of course
includes energy consumed by the ohmic heater). It is very important to confirm
that the device is thermally stable. The selected definitive values for the inlet en-
ergies are the values of the wattmeter, considered to be more reliable than those
based on voltage and mean registered current.
200 1.0 3
250 1.05-1.12 8
300 1.12-1.15 8
350 1.31-1.41 4
4.3. Remarks
(1) The calculation of the COP is straightforward. Let us take the 200-volt
data. The mass of evaporated water is 63 g, with for 34 g due to auxiliary
resistance heater. The mean current was 1.25 A, and the duration of the
test is 300 s (5min).
Energy out: 63 g - 34 g (auxiliary resistance) x 2594 J = 75,226 J.
Energy in: 200 V x 1.25 A x 300 s = 75,000 J.
The COP is then: 1.0.
(2) The COP values bands are not correlated with the inaccuracy of the mea-
surements. The results presented here were collected over several hours of
operation of the cathode. The cathode is corroded at the very high temper-
atures of the experiment, so between experimental runs we push more of the
cathode through the Pyrex shield, keeping the length of exposed cathode at
about 15 mm. That explains the variation bands.
(3) Reproducibility is within a range of about 5%.
4.4. Discussion
The very simple device used allowed us to highlight with reproducibility an abnor-
mal excess heat, which increases with voltage.
We believe that we have confirmed abnormal excess energy for voltages higher
than 200 V with our present device. The data presented here for 350 V correspond
to input power exceeding 400 W. The abnormal excess heat exceeds 120 W without
85
taking into account the gas formation or luminous radiation. This power is therefore
definitely significant. We did not find any classical explanation for this thermal
effect, and we are examining the possibility of less classical explanations.
5. Conclusion
The initial purpose of these experiments was to investigate the potential of a simple
experimental device to confirm the results obtained by Mizuno. 1 ' 2 We think that
this first step has been accomplished and that we can say that ratios between
output and input energy (COP) of 1.3 and 1.4 have been reached with satisfactory
reproducibility.
In a second step, we will try to explain this phenomenon in order to increase
the COP.
In any case, the device presented in this paper is a very simple device, which can
be used to rapidly verify hypotheses without sophisticated means. For example, we
have verified that this phenomenon does not seem related with the heavy water,
which is found at one part in 7000 in natural water. We increased the concentration
of heavy water by a factor of 100 in our electrolyte, i.e. to 1 part in 70. We did not
see any perceptible change in our results.
Acknowledgments
The authors want to express our deep appreciation to M. M. D. Noel, J-L. Naudin,
and O. Horner of "EDF Les Renardieres" for fruitful discussions.
References
1. D.Y. Chung, Y. Aoki, F. Senftle, and T. Mizuno, ICCF11 Conf. (Marseille, 2004).
2. T. Mizuno, T. Akimoto, and T. Ohmori, Fourth Meeting of Japan CF Research Society
(Iwate University, Japan, 2003).
3. D. Cirillo, A. Dattilo, and V. Iorio, ICCF11 Conf. (Marseille, 2004).
SEEBECK E N V E L O P E CALORIMETRY W I T H A P d | D 2 0 + H 2 S 0 4
ELECTROLYTIC CELL
W U - S H O U ZHANG, 1 " J O H N D A S H , A N D Q I O N G S H U W A N G
Low Energy Nuclear Laboratory, Portland State University, Portland,
OR 97207-0751, USA
E-mail: dashj@pdx. edu
1. Introduction
After the successful public demonstrations of excess heat in Pd|D20 + H2SO4 elec-
trolytic cells at Boston (ICCF10) in 2003,1'2 we confirmed this anomalous effect
using a more accurate calorimeter: a Seebeck Envelope Calorimeter (SEC). The
SEC is a cube; the electrolysis cell is placed inside it. The SEC converts the heat
flux through the six walls of the cube into a voltage signal using many thermocou-
ples distributed uniformly in the walls. Many problems of isoperibolic calorimetry
and mass flow calorimetry can be avoided by this method. 3,4
In this report we present the calorimetric results for the Pd|D20 + H2SO4 elec-
trolytic cell, results with Ti added to the D 2 0 + H2SO4 electrolyte, and the results
of analysis of the Pd cathodes.
2. Experimental Setup
Closed cells are similar to that used before1'2 except that the height is less in order
to fit into the SEC as shown in Fig. 1(a) and described below. The electrolytic cell
is a Pyrex cylinder (capacity is about 280 ml, 4>-m = 50.7 mm and <^0ut = 57.0 mm,
tAlso at: Institute of Chemistry, Chinese Academy of Sciences, P.O. Box 2709, Beijing 100080,
China.
86
87
wall thickness = 3.2 mm, h = 142 mm). A PTFE female top cap is <f) 65 mm x 20 mm
outside dimensions and <j) 57 mm x 16 mm of inside. It has two holes, 0.5 mm
diameter each, for the electrode lead wires. A PTFE plate (<fi 50 mm x 8 mm) is
used to suspend the recombination catalyst above the electrode. It has many holes of
<t> 0.8 mm, and also has two holes, 1 mm diameter each, for the electrode lead wires.
A PTFE rod is fastened to the perforated plate and the top cap ensures that the
perforated plate is at a fixed distance above the electrolyte. A gasket (<j)-m = 35 mm,
<^out = 57 mm, wall thickness = 2.5 mm) made of ethylene propylene (resistant to
sulfuric acid) is used to seal the top cap against the top edge of Pyrex cylinder.
PFTE cap
PFTE rod
Tape
PFTE tube - -
PFTE plate with - -
many holes
Pyrex cylinder —
-280 ml
Anode
Cathode
(a)
SEC (sat
j DC power
(b)
The electrolyte is heavy water (99.9 at.%, Aldrich catalog No. 347167) mixed
with 96.4% H 2 S0 4 (J.T. Baker, lot No. K10030) by the volume ratio of 6.7:1.
Two types of catalysts were used in these experiments, one contains 0.5% Pd on
coconut charcoal (United Catalysis); another contains 0.5% Pt on 1/8 in. diameter
alumina pellets (Alfa Aesar). Before each experiment, the catalyst was thoroughly
dried in an oven at 88° C in order to drive out the liquid adsorbed during previous
electrolysis.
A schematic of the calorimetry system is shown in Fig. 1(b). The SEC (Ther-
monetics Corp.) has inner dimensions of 18.3 x 18.3 x 18 cm 3 (W x D x H). A
fan (Panaflo®, Model FBA08A12H1A, 80 x 80 x 25.5 mm 3 , DC12 V, 173 mA,
2.08 W) is used to eliminate temperature gradients in the SEC. 3 The temperature
of the SEC wall (TSEC wail) is controlled by a constant temperature bath (NESLAB,
RTE-111); the temperature stability is ±0.1°C. The SEC is covered with Styrofoam
to avoid the influences of room temperature fluctuations on calorimetry.
A HP 6267B DC power supply (0-40 V, 0-10 A) is used for galvanostatic electrol-
ysis. The electrolysis current is measured with a shunt resistor, which is a standard
resistor of 0.1 fl with 0.04% precision (Leed & Northrup 4360). The electrolytic cell
is placed in the center of the SEC. Eight K-type thermocouples are used to monitor
temperatures: one is for ambient temperature outside the SEC; one is for air tem-
perature in the SEC; two are attached on the outside of the cell wall at the middle
height of electrolyte; four are attached on the wall at the middle height of catalyst.
All the data are monitored by a Keithley 2000-20+scan digital multimeter. The
data are automatically logged every minute using TestPoint 3.3 software.
The mass of the cell was measured before and after electrolysis using a My Weigh
i500 balance (max. 500 g, d = 0.1 g). After Jan 1, 2005 this was replaced with an
Ohaus D54 balance (max. 2000 g, d = 0.01 g). The Pd sample is weighed with a
Mettler H70 (max. 160 g, d = 0.1 mg).
Calibration experiments are conducted using a Pt|H20 + H2S04 electrolysis cell,
a pure resistor, or a dummy cell with a resistor in it. Calibrations are carried out
before and after every electrolysis experiments.
Surface topography and element analysis of the palladium cathode surface is
performed using an ISI-SS40 scanning electron microscope (SEM) with an attached
Oxford model 5565 energy dispersive spectrometer (EDS).
3. Results
3.1. Calorimetric Results
First, we present calibration results. A resistor provided by the SEC manufacturer
was placed at the center of the SEC. TSEC wail was the same as that used for
the experimental P d | D 2 0 electrochemical cell calorimetry. After the calorimeter
reached steady state with the fan turned on, the background signal was stable.
Then, power was applied to the resistor. After the output signal reached steady
state, the power was turned off. The output signal was monitored during the cool
89
down. The device constant is the quotient of average stable input power to the
average net output signal at steady state. The net output signal is the gross output
signal minus the signal produced by the power supplied to the fan. For input
power of 11 W, the fan power decreases by 23 ± 3 mW (1.4%) during calibration or
calorimetry. The decrease in fan power during calibration is the same magnitude as
the decrease during calorimetry, so there should be no net effect on the calculated
excess power. One calibration requires about 12 h.
Figure 2(a) shows the results of one of the calibration experiments. It gave the
device constant of 182.34 ± 0.20 W/V. The time constant is 15 min here. Due to
the large inner volume (6 1), the time constant of the SEC is mostly determined by
the heat capacity and conductivity of the sample under test, rather than the SEC
itself.
(a)
20 -P(W) = (0.18761 + 0.0034) Vout (mV) f -
60 5
,"f~ " _ pin (W) -(2.12 x 10~ ±3.9x io- e )(i/ o u (mV|f/ ,
i« V0M (mV) . £ 2
= 2 . e x-\0-*, Ff = 0.99999 S
? '5 - x
i? a. j /
TsECwal = 20°C
utpu t signal:
o
I J 20 ° — 5 /
' 8
• j CD (b)
0
20 40 60 80 100
•
Net SEC signal output: l/oll, (mV)
Time (h)
Figure 2. (a) An example of calibration (Exp. No. 051005); (b) calibrations at different input
power, where x 2 is the sum of squared residuals; R2 is the coefficient of determination (Exp. No.
041228).
(b)
80
70
O
*2 60
7"sECWal|-35°C
13
01 50
Q.
E
I2 40
12 16 Time (h)
Time (h)
working cell and calibration resistor. The results showed that those three different
calibrations gave the same device constant within experimental error.
Seven Pd samples have been tested in experiments; four of them gave repro-
ducible excess heat. The calorimetric results for the best sample, Pd-A, are pre-
sented here in detail. The sample Pd-A (9.0x37.2x0.35 mm 3 , total area of 7.08 cm 2 ,
weight 1.3418 g) was cold rolled from 0.5 to 0.35 mm thickness. One example of
excess heat production and related parameters is shown in Fig. 3.
Figure 3(a) shows that the power input decreases rapidly in the first two hours
because the input power heats the cell, as shown in Fig. 3(b); therefore the elec-
y*=*i
0? i *
y _
Time (h)
Time (h)
Figure 4. Other examples of excess heat produced in the P d | D 2 0 + H2SO4 cell for sample Pd-
A. (a) The maximum excess power in Exp. No. 041125. Parameters: average current density is
0.42 A / c m 2 , total input heat is 592.24 k j , excess heat is 44.05 kJ, average input power is 13.143 W,
average excess power is 0.978±0.032 W (without including mass loss) to 1.273±0.065 W (including
mass loss of 0.9 g). (b) An example of heat bursts during excess power production in Exp. No.
041122.
91
Table 1. Excess heats at different temperatures for sample Pd-A, with ~ 0.02 g/ml Ti
added to the electrolyte.
Exp. No. T S E C wall (°C) Electrolysis time (h) Average input Average excess
power (W) power including
mass loss (W)
trolyte conductivity increases and over-voltages on the two electrodes decrease with
time. These factors make the cell voltage decrease correspondingly.
Another phenomenon is that the catalyst temperature (indirectly measured on
the outer wall of the cell) has some fluctuation possibly because of the coarse
grains of charcoal (about 2 x 3 x 6 mm 3 ) and the inhomogeneous properties of
the solid/gas reaction. Fine particles of catalyst produced by pulverizing the large
grains can improve the stability and uniformity of temperature. However, this
method does not improve the catalysis and it makes the catalyst more difficult to
handle.
Part of the water produced by the recombination of oxygen and deuterium gases
is adsorbed by the catalyst. The fraction of the water adsorbed depends on elec-
trolysis current and time, and the temperature and activity of the catalyst. It is
from 40 to 80% in our experiments.
Heat bursts have been observed from sample Pd-A, in addition to the stable
excess heat, in three different experiments. One example is shown in Fig. 4(b).
The excess heat was measured at different SEC wall temperatures; one set of re-
sults is shown in Table 1 and Fig. 5. We have conducted calorimetry with TSEC wail
0.5
o.o
10 20 30
SEC wall temperature (°C)
Figure 5. Dependence of excess power on temperature of SEC wall for Sample Pd-A, the current
is 3 A (the corresponding current density is 0.42 A / c m 2 ) ; the input power is 11-13 W.
92
Electrolysis current density (A/cm 2 ) Excess power including mass loss (W)
Figure 6. Dependences of excess power on current density for sample Pd-A (Exp. No. 041115).
93
Table 3. Summary of excess powers for different samples from Oct. 2004 to Nov. 2005.
effects on excess heat are also shown in Table 3. The concentration of titanium is
expressed by the mass of titanium per unit volume of electrolyte. The data in Table
3 indicate that titanium in the electrolyte enhances excess heat production. 7
(a)
30,000— (b) pd
PdLB
J — ^ - = 0.41
PdLa
20,000- No Ag detected
10,000~
U
Pd ji \
X - . f"
o i - • - . j . . . . . . . . .
Energy (keV)
Figure 7. (a) SEM image of a Pd sample before electrolysis, (b) X-ray spectrum on the total area
of (a) measured by EDS.
94
iflsg \* . •,
"! $
(a) (b)
Figure 8. (a) Light microscope photo of sample Pd-A after electrolysis for 429 hours, (b) SEM
picture of square region shown in bottom right corner of sample Pd-A in (a).
a deposit. The EDS results of Table 4 show that this deposit is mostly Pt, which
dissolves from the anode.
Figure 9 shows part of the characteristic X-ray spectrum from the dark spot S2
in Fig. 8(b). Spot S2 is from a hole in the surface. It should be the bare Pd surface.
Bright spot S3 is at the edge of the hole, wiiere the Pt is deposited. It seems likely
that the holey regions are places where palladium-deuterium electrode reactions
occur after some time electrolysis. Figure 9 shows an increase in Pd L/3/LOJ. Using
deconvolution software, it is found that S2 has 6.5 at.% Ag and S3 has no Ag. Other
results in our group show that Pd Lfi/La may be 1 or greater on the Pd cathode
after electrolysis in heavy water. This is convincing evidence of the presence of
localized concentrations of Ag. 7
Besides sample Pd-A, we also measured silver on other Pd samples after electrol-
ysis. Another example is shown in Fig. 10 and Table 5; this sample also produced
excess heat. Because the results are qualitatively the same as those of sample Pd-A,
we will not discuss them in detail.
S2
Pd
30,000-™:
ft PdLB
PdLa
=0.47
Z A g = 6.5%
Pd
20,000-:
1 Ag
10,000-^ Ag r
TAg
Figure 10. (a) Light microscope photo of sample Pd-E after electrolysis for 93 hours, (b) SEM
picture of square area shown around the top left corner of sample Pd-E in (a).
Acknowledgments
References
1. A. Ambadkar and J. Dash, Electrolysis of D2O with a palladium cathode compared
with electrolysis of H2O with a platinum electrode: procedure and experimental details,
see: http://www.newenergytimes.com/Library/2003DashJ-ColdFusionRecipe.pdf
2. J. Dash and A. Ambadkar, Proc. ICCF11, Marseille, France, Oct. 31-Nov. 5 (2004),
p. 477.
3. E. Storms, Proc. ICCF10, Cambridge, MA, USA, Aug 24-29 (2003), p. 183.
4. B. Bush and J.J. Lagowski, Proc. ICCF7, Vancouver, Canada, Apr. 19-24 (1998),
p. 38.
5. F. Fleischmann, S. Pons, and M. Hawkins, J. Electroanal. Chem. 26, 301 (1989).
6. S. Miguet and J. Dash, J. New Energy 1, 23 (1996).
7. Q. Wang and J. Dash, Proc. ICCF12, Yokohama, Japan, Nov. 27-Dec. 2 (2005).
OBSERVATION A N D INVESTIGATION OF N U C L E A R F U S I O N
A N D SELF-INDUCED ELECTRIC D I S C H A R G E S
IN T U R B U L E N T LIQUIDS
ALEXANDR I. KOLDAMASOV
Scientific Center of System Research and Technology, Moscow, Russia
HYUN IK YANG
Hanyang University, Ansan, Korea
ALLA A. KORNILOVA
Moscow State University, 119899, Moscow, Russia
VLADIMIR I. VYSOTSKII
Kiev National Shevchenko University, Vladimirskaya St. 64, 01033, Kiev, Ukraine
E-mail: viv@vhome.kiev.ua
ANDREY V. DESYATOV
Federal State Unitary Enterprise "Keldysh Research Center", Moscow, Russia
1. Introduction
The aim of this report is to present some preliminary results of experimental and
theoretical investigations of the processes and phenomena connected with optimal
fusion reactions in turbulent liquid targets.
It is well known that one of the most promising and ecologically safe types
of fusion reactions is the p + B 1 1 —> 3He4 reaction with AE = 8.7 MeV energy
release and without the creation of neutrons or formation of radioactive waste.
For this reaction the optimal energy for interacting with moving protons is about
-EpBiopt = 675 keV. In the usual uniform systems like cold or warm stationary
plasma the probability of such a reaction is very low. This is the direct result of
the high Coulomb potential barrier.
97
98
In our opinion one of the most promising methods for enhancing the probability
of this reaction is connected with the use of turbulence and cavitation phenomena
in the volume of a liquid (in this case, light water).
We believe that the same enhancement should generally take place for any type
of fusion reactions with positive energy release, during the cavitation of bubbles in
an appropriate liquid.
There are several theoretical models for such enhancement.
One of them ("coherent non-stationary interference model") is connected with
the process of barrier-free fusion in the volume of a non-stationary (e.g., self-
compressing) microcavity (e.g., Refs. 1-4). In this non-stationary model the barrier-
free fusion is possible for any over-threshold reaction with positive energy release.
Other ("direct") models are connected with both high-impulse pressure and high
temperature during collisions of atoms of the cavity walls during bubble collapse.
In fact such models are connected with the microaccelerating (microhot) method
of fusion using surface forces. We believe that these "direct" models are not able
to ensure the necessary requirements for effective fusion because of the relatively
low temperature (no more than 5000-10,000K in multibubble systems) and the
relatively low pressure in a cavitation region.5 It is also evident that tunneling
quantum processes cannot provide a sufficient probability of nuclear transmutation.
2. E x p e r i m e n t a l S e t u p
Schematic and general views of the installation for the production of controlled tur-
bulence and formation of cavitation bubbles in the working chamber are presented
in Fig. 1.
The total volume of circulating liquid is 201. The working chamber is made
from plexiglas tube with diameter of about 8 cm and length of about 15 cm. The
chamber wall is about 3 cm thick. A special insert (hermetic plastic plug) with
an orifice hole is situated inside the working chamber. The diameter of the orifice
hole is about 1 mm. In the experiments, different kinds of orifice hole with special
variable profile and variable cross-section have been used. In these experiments two
different liquids were investigated; machine oil and distilled light water.
3. E x p e r i m e n t s a n d R e s u l t s of Investigation of C a v i t a t i o n in P u r e
Machine Oil
In the first case we have studied the optical and nuclear processes that take place
during cavitation of machine oil. In this case different successive phenomena were
observed as the pressure was increased. Several stages of the cavitation process
were observed:
Stage 1. At low pressures (less than 20-30 atmospheres) and low velocity of
machine oil (see Fig. 2; flow is from left to right) the color of the moving liquid in
the working chamber is tawny.
Figure 2, The view of the working chamber at very low pressure of machine oil.
Figure '\. T\\v \\r\v of the working chamber nt low prcsMiu- o;" iiia<-liine oil.
Figure 1. Increasing of the cavitation marhin^ oil transparency in the working chamber at pres-
sure increasing: Pi < P% < P3.
101
Figure 5. Generation of the directed bright light beam in the turbulent machine oil.
The color of the beam is blue-white and is very bright. The diameter is
about 6 mm.
The main question is: what is the nature and origin of the directed luminous
beam?
It was not a directed light beam from the internal part of the hole because the
initial diameter of the directed beam is four times greater than the diameter of the
output aperture of the insert (orifice hole). It also was not equilibrium thermal radi-
ation (sonoluminescence) from the region of cavitation. Several arguments support
these conclusions:
Argument 1. The length (about 5-10 cm) and very narrow cylindrical form of
the beam are sharply different from the dimensions and shape of the usual cavita-
tion region (jet-like cone, sphere or short cylinder). This is supported by a simple
calculation:
The processes of formation and collapse of bubbles take place immediately down-
stream of the transition zone at the exit of the orifice hole. The size of this transition
zone approximately equals the diameter of the orifice hole (D = 1-1.3mm).
It is well known (e.g., Ref. 6) that the time for the collapse of cavitation bub-
bles with typical initial radius JR0 « 5/xm does not usually exceed r m a x « 20 ns.
Approximately the same amount of time is needed for formation of bubbles in the
volume of moving liquid behind the orifice hole. It is also well known from hydro-
dynamic principles that the longitudinal velocity of moving fluid (moving bubbles)
at P < 100 atmospheres does not exceed ti m a x « 10 4 -10 5 cm/s. Hence the size of
the cavitation region does not exceed L m a x « D + 2v m a x r m a x « 1-1.3 mm. This is
very small compared to the length of the observed directed beam (5-10cm).
102
The angular properties of this directed light beam are similar to those of a laser
beam.
Argument 2. The rather bright observed luminescence and rather high derived
temperature (about 105 K) are comparable only to the intensity and temperature
spectrum from sonoluminescence of single bubbles, and are the direct result of the
spherical symmetry of the bubble at collapse. In the case of multibubble cavitation,
the sonoluminescence spectrum indicates that the temperature inside a bubble at
collapse is relatively low (2000-5000 K), and the intensity of the sonoluminescence
is also low ("cold sonoluminescence").7"9
Argument 3. The intensity of sonoluminescence decreases strongly with increas-
ing temperature of the cavitating liquid (e.g., at increasing temperature from 1°C
up to 40°C the intensity decreases by 100 times 8 ). But in our system the intensity
of radiation does not depend on the temperature in the explored interval from 20
to 60°C.
So, the observed phenomenon is not the usual kind of sonoluminescence. There
are reasons to believe that the intense directed beam could arise from one of the
following three possible mechanisms:
In view of these results, the directed beam is not believed to be connected with
Cherenkov radiation.
(2) The possible mechanism of single-pass induced laser generation is connected
with the ionization and recombination of oil molecules in the cavitation region
(similar to the processes in a gas-dynamic laser).
103
The first step would be intense ionization of the moving atoms and molecules.
Formation of a moving hot plasma would then take place in the region of cavitation
immediately downstream of the orifice hole. During the second step the process
of recombination of moving atoms and molecules and the formation of inverted
states in the active medium would contribute to self-cooling of the moving plasma
farther downstream. Such a two-stage process could be steady and thus could lead
to single-pass generation of a steady laser beam.
The central question is—what could be the pumping source for such a laser-like
regime?
It is well known from fundamental laser and plasma physics that for pumping of
a plasma laser (which is based on ionization and recombination) the temperature T
of the active medium must be such that k^T > 5cpi- Here ipi is the ionization
potential of the lasing atoms in the oil (</?; = 11.2-14.5eV for C, H, O or N atoms).
For a plasma laser generating blue or shorter wavelengths, the pumping source
must have a temperature such that kBT > (50-100) eV [i.e., T > (0.5-1) x 10 6 K].
Since the temperature in the centers of cavitation in a multibubble system is
no more than (0.5-1)xl0 4 K (e.g., Ref. 5), a much more energetic pumping source
is required for the lasing to arise from the cavitation process. We believe that one
possible source of energetic plasma for the hypothetical laser mechanism may be
fusion reactions in bubbles in the cavitation region or the turbulent jet zone.
(3) Nuclear processes would also be needed for the generation of spontaneous
optical radiation in the directional turbulent oil jet.
In both cases 2 and 3 a source of nuclear energy would be necessary. There are
many reactions that might occur in cavitating machine oil (e.g., carbon-nitrogen
cycle). These reactions are being researched now and results will be reported in the
future.
During steady operation of the chamber we also observed another phenomenon—
formation of self-induced electric discharges ('lightnings') near the plasma jet (along
the exterior surface of the insert). The average length of the lightnings was several
cm. Such discharges are connected with ionization in the region near the orifice
hole and the accompanying accumulation of free charges on the exterior surface of
the insert. The typical frequency of such lightnings is several Hertz. Examples are
presented in Fig. 5.
Stage 6. At increasing pressures of up to 90-95 atmospheres the process of
rapidly increasing intensity of the blue-white directed beam takes place. The fre-
quency of lightnings also increases.
At this time, in the space upstream of the orifice hole, an additional short intense
green jet appears (see Fig. 6).
The green jets are not in the region of turbulence and cavitation. The color of
the oil in the area upstream of the orifice hole remains tawny and the motion of
the liquid appears laminar. To stimulate the formation of the green jet we used a
ground connection to neutralize separated volume charges in the chamber. There
are two possible mechanisms for formation of the green jet.
104
pressure was likewise low. The formation of cavitation bubbles and their collapse
at pressures near 30-40 atmospheres are shown in Fig. 7.
At pressures above 50-60 atmospheres, weak sonoluminescence of cavitating
bubbles takes place (see Fig. 8).
The color of the low-intensity sonoluminescence is blue, and is located on the left-
hand side of the photograph. The size of sonoluminescence area is about 1-2 mm.
The luminescence in the central and right-hand side parts of the photograph is the
result of the scattering of light in pure turbulent water. The intensity of radiation
weakly depends on the pressure in the interval 60-90 atmospheres and decreases
with the increase of the water temperature. According to all the tests that were
discussed above it is the usual multibubble sonoluminescence.
The spectrum of hydrogen from this sonoluminescence area was investigated.
Spectra of the two most intense lines are shown in Fig. 9.
By analyzing the relative intensities of the two lines with wavelengths A = 656.28
and 486.13nm (550-600 and 15-20 AU, respectively), the temperature of the lumi-
nescing centers was calculated to be T « 3000 K. This is a temperature typical of
multibubble sonoluminescence.
5. Additional Studies
Additional physical and nuclear tests on cavitating machine oil and distilled water
have also been carried out.
1 1
Amplitude
m«iift»»wnii<M'*
>.„nm X im
3
Figure 9. Spectra of two measured lines of hydrogen radiation of the sonoluminescence area.
References
1. V. I. Vysotskii, On possibility of non-barrier dd-fusion in volume of boiling D2O.
Proceedings ICCF4, 1994, 4, pp. 6-1-6-3.
2. V. I. Vysotskii, Conditions and mechanism of non-barrier double-particle fusion in
potential pits. Proceedings ICCF4, 1994, 4, pp. 20-2-20.5.
3. V. I. Vysotskii and R. N. Kuzmin, Nonequilibrium fermi - condensate of deuterium
atoms in microcavity of crystals and the problem of nonbarrier cold nuclear fusion
realization, Soviet Phys. - J.T.P. 64(7), 56 (1994).
107
EDMUND STORMS
Lattice Energy, LLC, Santa Fe, NM, USA
E-mail: storms2@ix. netcom.com
1. Introduction
Heat production is an essential feature of the cold fusion effect and its measurement
has been a frequent object of criticism.1 Since 1989 when Profs. Fleischmann and
Pons (F-P) 2 first revealed their observations, calorimetry has evolved from the
simple isoperibolic design and become increasingly accurate 3 with use of the Seebeck
type. 4 " 7
The Seebeck (Kelvin) calorimeter consists of thermal-electric converters that
completely surround the source of heat. Temperature at the outside of these con-
verters is held constant while temperature at the inside is allowed to increase. The
average temperature difference generates a voltage that is used, after calibration,
to determine the rate at which heat passes through the thermal barrier created by
the converters. Because the design is very simple, operation is easy to understand
and potential errors are easy to determine.
When used in a study of cold fusion, a gas-tight glass cell containing an elec-
trolyte and electrodes is placed in the enclosure. Because the measured voltage
represents an average of heat loss through all parts of the barrier, the device is only
slightly sensitive to where the cell is placed within the enclosure. A fan is used to
distribute heat more evenly and to reduce the cell temperature by removing heat
from it more rapidly. The calorimeter is completely insensitive to where heat is
being generated within the cell.
A calorimeter suitable for measuring the cold fusion effect must be sufficiently
sensitive to detect a few tens of milliwatts superimposed on tens of watts. In
addition, it must remain stable over long periods of time. The method of calibration
must define the same characteristics as when heat is produced by an unknown
source. Power production can be calibrated by generating heat using a resistor
contained in the device. A dead cell or conditions expected to produce no anomalous
energy can also be used. If the calorimeter is sufficiently sensitive, the total amount
of energy given off by a known chemical reaction can also be measured. In this
108
109
work, power is calibrated using a resistor in the cell or by using a Pt cathode and
a quadratic equation, watt = A + B x V + C x V 2 , shows the relationship between
generated voltage (V) and applied watts (W). In addition, the calorimeter is used
to measure the total amount of energy absorbed when a Pd cathode is loaded with
D. Because this quantity is well known, 8,9 the method gives further demonstration
that the calorimeter is indeed accurate and able to detect small amounts of energy.
Defining the accuracy of a calorimeter using a few numbers is not practical
because several different and independent potential errors exist. Because of bubble
action at high current, the amount of power being applied to a F^P cell is noisy.
In addition, use of a fan adds additional noise, especially at low applied current as
is the case during this study. This causes random fluctuations in measured power,
which are as much as ±10 mW during this study. If this fluctuation is too great,
it can mask small changes in anomalous power, but it does not introduce an error
that might be interpreted as anomalous power. On the other hand, the calibration
constant or the sensitivity of the calorimeter can change with time. These changes
can be produced by changes in reference temperature, in room temperature, in
the amount of recombination taking place in the cell, or in physical parameters
when new samples are placed in the cell. This potential drift is the main source of
incorrect results. These potential errors are explored in this work.
2. Description
The device described here is made by gluing together commercially available ther-
moelectric converters, as shown in Fig. 1, using waterproof epoxy glue.
The panels are connected electrically in series. Once assembled, the outer surface
is covered with an electrically insulating, waterproof epoxy paint. The electrical
resistance of this coating must be tested and found to be high (>1 Mohm) before
final assembly. If the resistance is too low, unwanted voltages will be generated by
chemical reaction between the cooling water and the metal plates. These assemblies
Figure 1. Glued panels assembled into two haves of a calorimeter. The length is 13.9 cm, the
width is 6.9 cm and the total depth when assembled is 14.8 cm.
110
Figure 2. Assembled calorimeter with \vat<T cooling jacket m plar<> In lliis design, the wires pass
out of the cell through plastic water cooled channels.
are placed within watertight plastic boxes that are designed to cause even water flow
over the outside surface. When assembled, the two boxes are stacked one on top
the other as shown in Fig. 2. Figure 3 shows a typical open calorimeter containing
an electrolytic cell and a small fan. Baffles are provided to insure air is passed over
and around the cell.
Wires and plastic tubes are passed into the cell through channels that are in
good thermal contact with the cooling water. In one design, these channels, visible
in Fig. 3, are stainless steel tubes, which pass the length of the device within the
Figure 3. Completed calorimeter with cell and fan in place. Notice that the wires pass into the
calorimeter through metal tubing so as to isolate the interior from changes in room temperature.
The cell is attached to the calorimeter using plugs to allow easy removal. The stack of resistors
at lower left is used to measure current through the cell and fan.
Ill
cooling water. These wires carry current to the cell and fan and allow applied
voltage to be measured at the calorimeter boundary. Circuits are arranged so that
current and voltage used for calibration and for electrolysis are measured using the
same resistor and DA channels. In this way, any measurement errors caused by
errors in the DA channels are cancelled. Measurements are made using National
Instruments data acquisition boards and Labview.
Switching from electrolysis to calibration can be accomplished by throwing one
hardware and one software switch, which allows automatic calibration over the
entire power range. A typical result is shown in Fig. 4. Table 1 lists calibration
equations obtained over 5 months of examination. Experience and analysis of this
information indicate that the uncertainty immediately after calibration is about
±16 mW, while drift caused by changes in room temperature and other factors can
introduce an additional uncertainty of ±25 mW during long runs. If the average
coefficients are assumed to be constant during the time shown in the table, the
maximum uncertainty at 8.3 W of total power would be ±60 mW. In other words,
the calorimeter is stable to within ±60 mW or 0.7% over 5 months if no effort is
made to recalibrate. Because calibration is so easy, these small drifts can be easily
identified as error. At no time has anomalous power outside of this uncertainty
suddenly appeared without being related to something done on purpose to the
surface of the cathode. Notice also, that calibration values based on Joule heating
of a resistor located in the cell agree very well with values obtained by using a
platinum cathode. This shows that the location of heat production within the cell
has no effect on measured values.
Because the cell contains a recombiner, no gas (except orphaned oxygen) is
expected to leave the cell. To determine if the recombiner is working and to measure
20 -i -7
16- /
14- j /
I 12- /
10
8. - /
f 8- /
9- y o Joule heat
6
" / * Electrolysis
4
" j *
2- y
/ PI (8-23-05)
Seebeck voltage
Figure 4. Typical calibration using an internal resistor. Four points are taken going u p in power
and four are taken going down, in sequence. The random error is the standard deviation of points
from the drawn line. Data are taken after a delay of 90 min to allow the calorimeter to reach
steady state.
112
Table 1.
A B C
the D/Pd ratio using the orphaned oxygen method, a small plastic tube carries gas
from the cell to a reservoir of oil. Any change in gas pressure within the cell
is detected as a weight change of oil applied to a balance (±0.01 g), as is visible
in Fig. 5. This method allows the amount of orphaned oxygen resulting from D
entering the Pd cathode to be determined and, from this, the D/Pd ratio. The
method is calibrated by weighing the sample (±0.00005 g) at the end of the study
to determine the amount of contained deuterium. Because D2 is lost from the
Figure 5. View of calorimeter and oil reservoir for measuring D / P d ratio. The switch in the
foreground allows change from electrolysis to calibration. Water is circulated using a pumped
(1.5 l/min) constant temperature bath (±0.01° C).
113
1.0774-
1.0772-
3
TL
F 1.0770 -
s
o
Weigh
1.0768 -
1.0766 -
Figure 6. Determination of deuterium content of sample. Notice that the sample can be removed
from the calorimeter and weighed within 2 min after turning off the current. The sample is dried
quickly by washing with acetone.
*
•
"i
0.00-
•J^vfcV* * ... ° * V „A!'".-•'•-...
" •
0.05-
I "^'£t'-" - 0.152 A
-0.10- F' '• 0.069 A
A I ' 0.041 A
1/
-0.15-
100 200 300 400 500 600
Time (min)
uses energy, measured as power, that can be calculated from the reaction
Figure 8. Composition of a cathode during loading. Note that at low current, loading of the
alpha phase becomes visible. The lines show the loading rate if all D2 produced by the current
entered the Pd cathode. The horizontal line shows the published composition at the /3-PdD phase
boundary at 1 atm D2 and room temperature in the presence of a-PdD.
Because of scatter in the power measurements and because the sample does not have
a uniform composition, the potential error in this measurement is about ±2 kJ/mol.
Agreement with the previous measurement is well within the possible error of both
results, thereby demonstrating the potential accuracy of this calorimeter.
Figure 9. Data used to calculate enthalpy of formation of PdDo.go using 0.00974 mol of Pd.
The first three points were taken while the calorimeter was approaching steady state and must be
ignored.
4. Summary
A Seebeck calorimeter can easily be constructed with characteristics that eliminate
most errors thought to cause anomalous energy from cold fusion. In addition to
being stable and accurate, the calorimeter is sufficiently sensitive to accurately
measure the enthalpy of formation of PdD x to give 11.8 kJ/mol using only 1 g of
palladium.
References
1. J.R. Huizenga, Cold Fusion: The Scientific Fiasco of the Century, 2nd edn. (Oxford
University Press, New York, 1993), p . 319.
116
M. A P I C E L L A , E. C A S T A G N A , L. C A P O B I A N C O , L. D ' A U L E R I O , G. M A Z Z I T E L L I ,
F . S A R T O , A. R O S A D A , E. S A N T O R O , A N D V. V I O L A N T E
ENEA Frascati Research Center V.le E. Fermi, 45 00044 Frascati (RM), Italy
E-mail: violanteQfrascati. enea.it
M. M C K U B R E A N D F . T A N Z E L L A
SRI International, 333 Ravenswood Ave., Menlo Park, CA 94025, USA
C. SIBILIA
La Sapienza University, Via Scarpa, 14 00100 (Roma), Italy
Recent research activity at ENEA, in the field of Condensed Matter Nuclear Sci-
ence, has been oriented to material science and Laser triggering in order to increase
the reproducibility of excess of power production during loading of palladium with
deuterium. Isoperibolic calorimetry in gas phase, isoperibolic and flow calorimetry
with electrochemical systems have been carried out. Nuclear ashes detection was
done by means of high resolution and high sensitivity mass spectrometer. Material
science studies allowed to obtain a palladium showing high solubility for hydrogen
isotopes and giving deuterium concentration at equilibrium larger than 0.95 (as
D / P d atomic fraction) with a reproducibility larger than 90%. Excess of power
production by using the above-mentioned material achieves a reproducibility up
to 30% without triggering. Laser irradiation with a proper polarization seems to
have a significant role in further increasing of the excess of power production repro-
ducibility. Heat bursts exhibit an integrated energy at least 10 times greater than
the sum of all possible chemical reactions within a closed cell. The energy gain
calculated at the end of the experiments is observed with deuterium but not with
hydrogen. Preliminary measurements give a 4 He signal in reasonable agreement
with the expected values by assuming a D + D = 4 He + heat (24 MeV for event)
reaction.
1. Introduction
The dissolution of hydrogen isotopes into a metal lattice is not only a problem of
thermodynamic equilibrium between the hydrogen inside the lattice and the hydro-
gen in the external phase (gas or liquid) but is also a problem of not equilibrium
because of the occurrence of a transport process. Both aspects of the phenomenon
are correlated since the equilibrium concentration of the solute is achieved when the
chemical potentials of the hydrogen in both phases are equal and since the transport
process inside the metal lattice is driven by the gradient of the chemical potential.
The migration of interstitials in a metal under an applied external bending is
well known as Gorsky effect.1 The deformation field produces the defects migration
117
118
toward the expanded areas. Lewis and co-workers 2-4 showed that internal stresses
are generated during insertion and diffusion of interstitial hydrogen and that the
resulting strain production represents an opposing force to the flux produced by the
concentration gradient.
The effect of the stress as limiting factor in achieving the deuterium-loading
threshold in palladium to have excess of power production is studied.
Figure 1. The effect of the hydrogen concentration profile on the stress field.
Therefore, the loading process may be inhibited by a stress gradient, for instance
behind the external surface, where the effect is traceable to the effect of a strong
temperature gradient. Thus, in the zone at high concentration, compressed by the
zone at low concentration, the chemical potential of the solute increases and the
loading can be inhibited.
In the following such a problem will be approached in order to have an ana-
lytical tool to estimate the effect of the stress field on the loading and to identify
the metallurgical conditions that can reduce this effect allowing the increasing of
the amount of hydrogen dissolved in the metal. Chemical potential of hydrogen
119
where fi* is the hydrogen chemical potential into the lattice without stress, Fis the
partial molar volume of the solute and <7h the trace of the stress tensor.
where M is the mobility, c the solute concentration, and F is the vector given by
the sum of the applied forces acting on the hydrogen interstitially dissolved in the
solid.
By replacing the relationship between diffusion coefficient and chemical poten-
tial, D = Mc(dn/dc), into Eq. (2) it follows:
J-
=~DVc+^m- (3)
„,_, DFc
where <x is the local stress. The analysis allows us to study the mass transfer problem
when the stress field is created during the loading. In the following, we will consider
a system where the diffusion is well described by one-dimensional time-dependent
model (foil, membrane or wire). 6
By introducing the fraction of relaxed stress ry into the flux equation it follows:
^-K-i-'1-'^!)- (6)
A mass balance on a foil leads to:
dc _, d (dc V da\ . .
m=DI-x\d-x-{l~7l)RrcTx)- (7)
where E is the Young's module. The relationship between strain and concentration
for Pd /3-phase (assuming that it may be extrapolated up to a loading atomic
fraction close to one)
e(c) = [l + b(c-c/3min)}, (9)
where cp m ; n is the hydrogen concentration value for the a + (3 phases coexistence
limit, b = 0.044 and c = C/CQ the dimensionless concentration (co is the metal atoms
concentration). Let us introduce the following dimensionless parameters
x = x/L, T = L2/D, (10)
where L is the characteristic length of the system (typically the thickness or the
radius), so that the resulting dimensionless transport equation is
0.8
Pd Young module 1010 Pa
0.6
I 0.4
0.2
0.0 +. •( |. 1 ( + — ) _(_ 1 1
0 0.25 0.5
Equation (11) describes the interstitial diffusion of hydrogen into a metal (e.g.
palladium) under a stress field. The effect of stress at steady state translates on a
different concentration profile, then a different loading that depends on the proper-
ties of the material such as the Young's module.
The transport equation (11) is solved with the boundary conditions c = 1, x = 0
and dc/dx = 0, x = L/2 and including the calculation of the relaxed stress on the
basis of the mechanical properties of the material (ay). Some calculations have
been done by using indicative values of the Young's module in order to make more
121
o 0.25 0.5
Space coordinate (arb. units)
Figure 3. Equilibrium H concentration profile within a Pd foil with Young's module = 1 0 n Pa.
clearer the effect. Figures 2 and 3 show the equilibrium concentration profile, from
the external side up to the symmetry plane, for two palladium foils with different
Young's module. In the first case the value of the Young's module is 1.0 x 10 10 Pa
while in the second case the value is 1.0 x 10 11 Pa (these value are chosen in order
to magnify the effect). It is clear that the loading reduces when the Young's module
increases. The calculation of the concentration profiles evolutions has been used to
calculate also the evolution of the R/RQ ratio by assuming the foil as a parallel of
electric resistances and by considering the well-known Baranowsky curves. Figures
4 and 5 show the evolution of the R/Ro ratio for the two considered above-described
loading conditions.
Figures 4 and 5 reproduce typical situations that one may observe experimen-
tally.
(1) High loading: after achieving the maximum the R/Ro reduces to 1.4 and to
1.6 for H and D, respectively.
(2) Low loading: after achieving the maximum R/Ro reduces only a little bit
since the dissolution of H or D stops because of the stress (unless a contam-
inant on the surface inhibits the dissolution of H or D).
2.0
Figure 4. Calculated evolution of R/Ro for high solubility (reduced stress) material.
122
t
2.0 r
0.5 L
0.0
200 400 600 800 1000
Time (arb. units)
Figure 5. Calculated evolution of R/RQ for low solubility (high stress) material.
The model allowed us to seek for a material showing a homogeneous loading able
to minimize the concentration gradients and then the stress field. Some treatments,
based on cold and annealing steps allowed us to optimize metallurgical structure of
the materials in order to increase the H(D) loading. The row material was palladium
foil 0.5 mm thick able to reach a loading ratio of about 0.8 (hydrogen atomic ratio).
The treatment has been done in two steps:
Figure 6 shows a simply cold worked sample. Figure 7 shows the effect of the
annealing (1100°C for 5 h) after rolling , the sample microstructure is changed and
it is clear the growth of the grains. Figure 8 shows the microstructure of a sample
annealed for 1 h at 850°C after rolling.
Figure 9 shov/s the effect of the treatment (i.e. of the metallurgical structure on
the H (D) loading). H/Pd = 0.97 has been obtained in the sample cold worked and
annealed at 850° C for 1 h.
A possible interpretation of. such a results is that in the last considered sample
the concentration profiles are maintained relatively flat because of the reduced size
of the grains. The above-described tests have shown a satisfactory reproducibility.
Another interesting effect found in the experiments is the correlation, that some
time occurs, between the loading dynamics and the loading ratio. One may observe
that after loading at constant current density for a certain time, the concentration of
the solute in the metal does not increase any more and sometimes a de-loading takes
place. On the basis of the concepts exposed in the previous section, we assumed
that such a behavior was promoted by the creation of a stress field very close to the
surface of the sample under the electrochemical loading. Stress removal has been
performed by applying a low-high current mode, just to avoid the creation of a new
stress field. The effect of this technique is well described in Ref. 6.
0.6
—.
I
0.0
600 700 800 900 1000 1100 1200 1300
Temperature (°C)
4. Calorimetric Results
Flow and isoperibolic calorirnetric measurements have been performed by using
pre-treated palladium into electrochemical cells with LiOD 0.1 M electrolyte.
4000
I
3500
3000
N§i
2500
2000
2* ] - P|„ (mW)
1500
! •3&fe*&ss$ \
-PM(mW)
1000
500
0 \,.^ \
20,000 40,000 60,000 80,000 100,000
Time (s)
Figure 11. Input and output power during an experiment performed with LiOH 0.1 M electrolyte
LiOH.
temperatures of the coolant are measured with two Pt 100 thermometers (four wires
measurement). The closed electrochemical cell is equipped with a recombiner. Cell
power supply is an AMEL galvanostat, modulated, during the HI-LO current mode
by an HP 33120 wave function generator. Output power is measured by means of
the mass flow rate and coolant temperatures, R/RQ measurement is done by means
of an HP-4284 (four wires measurement). Figure 10 shows a schematic view of the
flow calorimetric system.
Several experiments have been done by using light water (LiOH 0.1 M elec-
trolyte) obtaining a calorimeter efficiency of 97.5% (output = 0.975 input, because
of the heat losses). No excess of power production has been observed by using H2O
despites a very high loading (H/Pd = 0.97) was always achieved.
A different behavior has been observed in several cases by using LiOD electrolyte.
Excess of power has been obtained in CI, C3, and C4 experiments under high
loading of D into Pd (D/Pd > 0.92). Figures 11 and 12 show the input and
! Output energy
p-N
[Calorimetric efficiency - 97.5%|"
60,000,000 6000 of
UJ 40,000,000- 4000
20,000,000
0
20,000 40,000 60,000 80,000 100,000
Time (s)
Figure 12. Plot of energy and power (input and output) for calibration with H2O 0.1 M.
120
£ P„ (mW)
- P«* (mW)
Time (s)
Figure 13. Experiment C3: excess of power versus time (input and output). C3 experiment: plot
of energy and power.
output power and energy for an experiment that may be considered as a reference
experiment performed with light water. No evidences of excess of power are observed
and the output energy perfectly respects the efficiency of the caloriinetric system
that recover 97.5 of the input power, so that the output energy curves always
maintains below the input.
Figures 13 and 14 show the C3 experiment evolution of the input and output
power and energy. After 25,000 s, at high loading (D/Pd > 0.92) the output power
overcame the input one and the bursts survived up to 60,000 s giving an output
power 80% larger than the input-
Despites the short lifetime of the burst a completely different behavior, of the en-
ergy curves (Fig. 14) (if compared with the reference experiment) may be observed:
during the excess of power production also the output energy curve overcome the
input one. A similar behavior has been observed in C I and C4 experiments. Three
excesses of powers have been observed over nine experiments although the achieved
D concentration in Pd (atomic fraction) was always larger than 0.9. Then the load-
100.000.000
Time (s)
Figure 14. Isoperibolic calorimeter and electrochemical cell for Laser triggering.
127
ing threshold D/Pd > 0.9 is clearly only a necessary condition. An upgrade of the
experiment has been conceived in order to increase the reproducibility of the excess
of power production.
Calibration 25-5-2004
- . • . - : -. .•- •- 3 6 2 6 * + 24.337A" = 1
~+~ T (average)
Pdi. (T (average))
0 1 2 3 4 5 6
An(W)
excess of power, ranging from 60 mW up to «300 mW (see Fig. 16), was revealed.
At the end of the experiment the excess of energy was 23.5 kJ (17.3 MJ/mol Pd).
In Laser 3 experiment a 33 mW, 632 nm Laser was applied after achieving a
loading D/Pd = 0.95 under square wave current mode. During the experiment the
Laser polarization was changed from "p" to "s" and vice versa. The effect is shown
in Figs. 17 and 18. Seems clear, as expected, that the excess of power takes place
under "p" polarization and disappears by applying "s" polarization. An amount of
3.4 kJ of energy (2.5 MJ/mol Pd) was produced during the experiment.
Laser 4 experiment was carried out by applying a continuous electrochemical
current. After achieving a loading threshold of 0.95 the cathode was continuously
irradiated by using a 632 nm, 33 mW red Laser. Calorimetry gave 30.3 kJ of
produced energy (19.4 MJ/mol Pd). Figure 19 shows the input and output power
and energy evolution after applying the Laser irradiation.
Figure 16. Evolution of the input and output power, last 30 h under Laser irradiation (p-
polarization), 632 nm, 5 mW. 4 He production estimate 6.12 X 10 1 5 .
129
— /cell (A) .
— P.(W)
P... (bar)
—fliflicoretla
Time (h)
Figure 17. Excess of power under Laser triggering (p and s-polarization effect). 632 nm, 33 m W
HI LO current mode.
4
5. H e Measurements
Increasing of 4 He concentration in the electrochemical cell was expected, by assum-
ing that the excess of energy produced was created by a D + D = 4 He + 24 MeV
reaction. He tight cells (2 x 1 0 - 1 0 mbar 1/s He leakage test) have been used in both
flow and isoperibolic calorimeters. The gas in the cell was analyzed at the beginning
of the experiment, during the experiment when no excess of heat was observed and
at the end of the experiment. A gas sample was sent from the cell to an inlet system
for the mass spectrometer.
All the manifolds were realized by using VCR fitting and maintained un-
der baking before and during measurements. The manifold is under vacuum at
2 x 1 0 - 5 mbar before sending a gas sample. The whole line was checked for He
J.b
\
x
33
3.2
i
— (cell (A)
— P„(W)
P.-(bar)
— MR, coretla
— PW(W)
. P.pol
2 6
7Z. 103
Time (h)
Figure 18. Excess of power under Laser triggering (Laser off effect). HI-LO current mode.
130
A £ = 30kJ-
| Inptttetjierjgy
2.20 S
g 150,000
leakage giving 10~ 10 mbar 1/s. A 707 Saes getter was used to trap deuterium,
oxygen and nitrogen from the sample gas before sending it to the MS.
Figure 20 shows a scheme of the system. The mass spectrometer used was a
high resolution and high sensitivity Jeol CG-Mate. Figure 21 shows the resolution
for mass 4. It is clear that the resolution is high enough to separate 4 He and D 2
(resolution limit is 10~ 4 amu).
Figure 22 shows the results of the analysis giving the 4 He concentration measured
in the cells at the end Lasers 2-4, experimental values are also compared with the
expected values and with the background.
6. Conclusions
Heat effects are observed with D, but not with H, under similar (or more severe)
conditions.
MKSbaraton MKSbaraton
JEOL GC-MATE
Peak profile for mass i
Sensitivity in SIM mode is up to some fm-gr
D2
f
AM = 0.0256 amu
j
4
He i
_Jl I
_J
j
Figure 21. Jeol GC Mate mass 4 resolution.
Heat bursts exhibit an integrated energy at least 10 x greater than the sum
of all possible chemical reactions within a closed cell. Experiments reproducibility
was significantly improved as a result of material science study. Some conditions
are required to have a reproducible excess of power:
1. Loading threshold D/Pd > 0.9 (necessary condition).
2. Suitable material to have a reproducible loading above the threshold.
3. Trigger.
4. Suitable status of the material to have coupling with trigger.
Three excess of power over three effective experiments have been achieved by
respecting these conditions during electrochemical experiment! The accordance
O 0.80x10'°^.
X 0.60x10"
Figure 22. The expected amount of increasing of 4 He is in accordance with the energy gain by
assuming a D + D = 4 He + 24 MeV reaction.
132
Acknowledgments
T h e authors would like to t h a n k Dr. Guido Petrini of Sued Chemie for his support
for all the scientific aspects concerning catalytic materials. In particular, for giving
b o t h the catalysts t h a t have been used for MATRIX experiment and for closed
electrochemical cells. Dr. R. Hartens, Dr. 0 . Seguin, Dr. S. Quill, Dr. A. Kusai,
and Dr. F . Dalia of J E O L for their help in optimizing for the experiments the J E O L
J C - M a t e Mass spectrometer used. Mr. D. Lecci, Mr. F . Marini, Mr. Polinari, Mr.
Marcelli, and Mr. Bettinali of E N E A for their technical support. Dr. S. Lesin,
Dr. A. El Boher, and Dr. Tanya Zilov of Energetics Technologies Ltd. for the very
useful interaction t h a t positively affected t h e research work.
References
1. H. Wipf, J. Less-Common Met. 49, 291 (1976).
2. F. A. Lewis, J. P. Magennis, S. G. McKee, and P. J. M. Sebuwufu, Nature (London)
306, 673 (1983).
3. F. A. Lewis, B. Baranowski, and K. Kandasamy, J. Less Common Met. 134, L27
(1987).
4. F. A. Lewis, X. Tong, K. Kandasamy, R. V. Bucur, and Y. Sakamoto, Electrochem.
Acta 218, 57 (1993).
5. R. A. Oriani, Trans. Fusion Technol. 26, 235-266 (1994).
6. A. De Ninno, A. La Barbera, and V. Violante, Consequences of lattice expansive strain
gradients on hydrogen loading in palladium. Phys. Rev. B, 56 (5), 2417-2420 (1997).
HEAT M E A S U R E M E N T D U R I N G P L A S M A ELECTROLYSIS
K. I I Z U M I , M. F U J I I , S. M I T S U S H I M A , N. K A M I Y A A N D K.-I. O T A
Chemical Energy Laboratory, Yokohama National University 79-5, Tokiwadai,
Hodogaya-ku, Yokohama 240-8501, Japan
E-mail: ken-ota@ynu.ac.jp
1. Introduction
Mizuno et al. reported excess heat and hydrogen generation during plasma
electrolysis. 1,2 To confirm them, an accurate determination of energy balance that
includes the sum of latent and sensible heat is required. To determinate the sensi-
ble heat an accurate measurement is difficult because of the high input energy of
plasma electrolysis.
In this study, to perform accurate heat measurements, we developed a flow
calorimetry system using a flow cell system, and we measured the energy balance
during plasma electrolysis.
2. E x p e r i m e n t
Figure 1 is a schematic diagram of the electrolytic flow cell. The cell was composed
of acrylic tubing. It had an internal diameter of 2 cm, an external diameter of 5 cm,
and was about 30 cm in length. The anode was a 2 cm diameter hollow cylindrical
platinum mesh (99.99% purity, 55 mesh). The cathode was a 1.5mm diameter
tungsten rod (99.95% purity). It was placed at the center of the cylindrical anode.
The distance between the electrodes was 1 cm.
The electrolyte was 0.2 M K 2 C 0 3 light water solution or 0.3 M N a 2 C 0 3 light
water solution. The electrolyte circulated in this system, passing through a reser-
voir. The temperature difference between the inlet and outlet of the electrolyte
was measured with Pt resistance thermometers. Hydrogen and oxygen generated
133
134
W cathode
Teflon coating
99.95%, 1.5mm
1.5 cm in length
.I I .—K Electrolyte
|h ,^ outlet
Acrylic plastic
tubing
Pt anode
99.99%
2cm,
55 meshs
1.0 cm in length
__ Pt resistance
1_J~ thermometer
Electrolyte inlet
Figure 1. Schematic diagram of a flow calorimetry cell.
during electrolysis were collected in the reservoir, and the rate of gas generation
was measured.
During electrolysis, the cell voltage and the current, the inlet and outlet tem-
peratures of the electrolyte, room temperature, reservoir temperature, and the elec-
trolyte flow rate were measured.
The heat loss through radiation from our system should be negligible, because
the flow of the electrolyte was controlled so that the temperature increase of the
electrolyte was kept under 5°C, and the electrolyte temperature was kept very close
to the room temperature.
Table 1 shows the experimental conditions during the energy balance measure-
ments in 0.3 M Na2CC>3 light water solution. The inlet temperature of the elec-
trolyte were kept at 26°C. The flow rates of the electrolyte were fixed at the range
of 681-825 ml/min. Electrolysis was conducted at constant voltage. The energy
balances were determined by the experimental operation times of 1, 2, 3, and 4h,
respectively. The energy balances of the run numbers hl-h4 were measured dur-
ing plasma electrolysis at 95 V, and that of run number h5 and h6 were measured
during normal electrolysis at 34 and 39 V, respectively. Also, cell voltages, inlet
temperatures and flow rates of the electrolyte were kept constant during the energy
balance measurements.
135
Inlet temperature of
Run Operation time (h) the electrolyte (°C) Flow rate (ml/min) Cell voltage (V)
hi 1 26 688 95
h2 2 26 707 95
h3 3 26 710 95
h4 4 26 681 95
h5 1 26 684 34
h6 1 26 684 39
The input energy was measured as the product of the cell voltage and the current.
The output energy was the sum of sensible and latent heat. The sensible heat
was determined by the temperature difference between the outlet and inlet of the
electrolyte. The latent heat was determined from the flow rate of the gaseous
product. The energy balances were calculated by the following equations.
EB = *£*. (5)
Here, Ein, U, I, Hs, / E , AT, d, Cp, H^, fg, AH, Eout, and EB were the input
energy, the cell voltage, the cell current, the sensible energy that was obtained by
the temperature increase of the electrolyte, the electrolyte flow rate, the increase
between the inlet and outlet of the electrolyte temperature, the density of the
electrolyte, heat capacity of the electrolyte, the latent energy of the H2 and O2
evolution, the generated gas flow rate, the enthalpy change of the water electrolysis,
the output energy, and the energy balance, respectively. The current efficiency is the
gas generation amount per the theoretical amount by the Faraday's law. Therefore,
the details are as follows:
V = /g//th- (7)
Here, n, /th, F, R, T gas , P a ; r , J3H2O, and 77 were gas generation amount per electron,
theoretical generated gas flow rate, Faraday constant, gas constant, temperature of
the H2 and O2 produced during electrolysis, atmospheric pressure, vapor pressure,
and current efficiency, respectively. The theoretical generated gas flow rate was de-
termined from Faraday's law of water electrolysis. Therefore, the ratio of hydrogen
to oxygen was 2:1.
136
200
160 -
12
>"
•— 1 2 0
(D
D) c
CD
\1 - 4
3
O
J
Plasma discharge i
Yl-
egjon
0 1 1 1 1
0 2 4 6 8 10
Time (min)
Figure 2. Trend of input voltage and current during normal and plasma electrolysis in 0.2 M
K2CO3 light water solution.
Figure 3 shows the current as a function of time during normal and plasma
electrolysis. The experimental conditions are shown in Table 1. Before plasma
electrolysis at 95 V, the current increased to 130 V by lOV/s. After bright plasma
formed, the voltage decreased to 95 V by 50mV/s and the energy measurements
were started. At the beginning, the currents were ca. 2.2 A for the plasma elec-
trolysis and the currents decreased to 1.9 A after 100 min of operation. After the
plasma electrolysis, the consumption of the tungsten cathodes was observed. On
the other hand, the current was constant due to the constant voltage during normal
electrolysis.
Figure 4 shows photos of tungsten cathodes before and after plasma electrolysis
at 95 V in 0.3 M Na2C03 light water solution. The tungsten cathodes were con-
sumed by means of plasma electrolysis. For 1 h operation, the cathode decreased
0.5 mm in length and 0.09 g of the tungsten was consumed. For 4h operation, the
cathode decreased 3.6 mm in length and 0.30 g was consumed. During plasma elec-
trolysis, much of the cathode was consumed, and the electrode surface area was
reduced.
137
A hi
A-*A O h2
O h3
•-•-* Q h4
- • h5
A h6
3
o
^ ^ e ^
100 200 300
Time (min)
Figure 3. Cell currents during normal and plasma electrolyes in 0.3 M N a 2 C 0 3 light water
solution.
Figure 5 shows the outlet temperatures of the electrolytes during normal and
plasma electrolysis. The inlet temperatures were 26°C in all cases. The outlet
temperatures decreased due to the current decreases during plasma electrolysis. On
the other hand, the outlet temperatures were constant due to the constant voltages
and currents during normal electrolysis.
Figure 6 shows the current efficiency during normal and plasma electrolysis. The
current efficiency of the plasma electrolysis were 115-122% except the fluctuation
of h4 after 100 min and these of normal electrolysis were 91-98%. The excess gas
generation could not be explained by Faraday's law. Therefore, the excess gas must
have been generated by the plasma process. Also, a small amount of CO2 was
detected during plasma electrolysis by means of a gas chromatograph.
Figure 7 shows the energy balances during normal and plasma electrolysis. The
energy balances of the plasma electrolysis were 100-102% except during a period of
fluctuation shown in the data for h3. The energy balance for normal electrolysis was
91-98%. Although, a small amount of excess energy was detected during plasma
electrolysis, clear excess was not observed.
^mm
jnii mi
Figure 4. Photos of tungsten cathode before and after plasma electrolyes at 95 V in 0.3 M Na2CC>3
light water solution, (a) Before electrolysis, (b) after 1 h, and (c) after 4 h.
138
31.0
A hi
30.5 ° h2
R
^W
O h3
CD 30.0 a h4
•3
•<-• • h5
2
CD
29.5 A h6
O.
fc 29.0
.C *** \
28.5
28.0 I 1
Figure 5. Outlet temperatures of the electrlolytes in during normal and plasma electrolyses in
0.3 M Na2CC)3 light water solution.
4. Conclusions
The energy balance during plasma electrolysis was 100-102%. Clear excess en-
ergy could not be detected. The current efficiency during plasma electrolysis was
115-122%. A small amount of CO2 was also detected during plasma electroly-
sis by means of a gas chromatograph. A gas generation reaction other than the
electrochemical process took place during the plasma electrolysis, and generated
excess gas. Further study is necessary, especially, related to the composition of the
effluent gas.
140
108
106
>
en 104
o
cCO
CO 102 A hi
X!
O h2
ergy
100 O h3
c • h4
LU • h5
98
A h6
1 1
96
100 200 300
Time (min)
Figure 7. Energy balances during normal and plasma electrolyses in 0.3 M Na2CC>3 light water
solution.
References
1. T. Mizuno, T. O h m o r i , T . A k i m o t o , a n d A. Takahashi, Jpn. J. Appl. Phys. 3 9 , 6055
(2000).
2. T . Mizuno, T . A k i m o t o , K. A z u m i , a n d T. O h m o r i , Jpn. J. Appl. Phys. 4 4 , 396 (2005).
EFFECT OF A N A D D I T I V E ON T H E R M A L O U T P U T D U R I N G
ELECTROLYSIS OF HEAVY WATER W I T H A PALLADIUM
CATHODE
Q. W A N G A N D J. D A S H
Low Energy Nuclear Laboratory, Portland State University, Portland, OR 97207, USA
E-mail: dashjQpdx. edu
1. Introduction
During electrolysis of D2O-H2SO4 electrolyte with a Ti cathode and a Pt anode,
Ti erodes from the cathode and dissolves in the electrolyte. 1 When this electrolyte
containing dissolved Ti was used for electrolysis with a Pd cathode and a Pt anode,
enhanced excess heat was observed. Also, localized concentrations of unexpected
elements were found on the surface of the Pd cathode. This report contains data
on the variation of excess heat production with concentration of Ti in the elec-
trolyte and on the variation of the magnitude of the excess thermal power over a
period of 16 days. Data on the distribution of elements on the Pd cathode are also
presented.
EbOin the ratio 1:12.3. The experimental cell electrolyte contained the same batch
of concentrated H2SO4 and Aldrich D 2 0 (catalog number 34,716-7) in the ratio
1:6.7. The average current density on the Pd cathode was about 0.3 A/cm 2 .
Figure 1. Circuit containing a constant current DC power supply and a control cell in series with
an experimental cell. The black circles indicate the locations of eight thermocouples attached to
the outside of each cell. The output of the thermocouples and the cell voltages were monitored
with a computer. The cell temperature was then calculated as the arithmetic average of these
eight readings.
(3-23-05)-(5-9-05)
Excess thermal power versus Ti content of the electrolyte
CO
x
a 1.5
£ 0.5
Figure 2. Excess heat approximately doubled after Ti content of the electrolyte was increased
from 0.011 to 0.022 g/ml. At higher concentrations of Ti, a Ti compound deposited on the cell
wall.
lost ~ 1 g more mass than the experimental cell, and the calculated excess thermal
power is not accurate. For the other runs, both cells lost less than 0.5 g, and the
calculated excess thermal power is thought to be accurate.
The Pd electrode used for the data in Fig. 3 was examined with a scanning elec-
tron microscope equipped with an energy dispersive spectrometer. Characteristic
X-ray spectra were taken from each of the rectangles, on both the concave and the
convex sides shown in Fig. 4.
Figure 4 shows light microscope photographs of the two sides of the Pd cathode
from which excess heat reported in Fig. 3 was obtained. The electrode is approxi-
mately 2.3 cm wide and 2.5 cm height. The EDS spectra were obtained by scanning
the area in each rectangle. Examples of the spectra are shown in Fig. 5.
CO 3
x 9 O o
2.5 0
- 0 • *
o 2 • • 0
Q.
- •
"CO 1.5 -
• •
4 -XS with mass correction
E ;
1 •
CO
co
CD
0.5 0 B -XS with mass correction no Ti
o
X -_ jtV -XS without mass correction no Ti
HI
0 —' B ' "
8/1 8/6 8/11 8/16 8/21 8/26
Date
Figure 3. Excess thermal power with and without mass correction. Average excess is 1.8 W. Mass
correction was calculated in order to account for the loss of recombination heat due the escape of
gases from the cells.
143
iflsRp (•ikt^'iP
gj&'K
""" X"
•f "•- j l
*' i
• /A
!P*(WP
l |
f
¥$••••••
4k'r
1 ''
'
Figure 4. (a) Side facing anode (concave), (b) Back side (convex).
The upper spectrum in Fig. 5 was taken from the rectangle on the left-hand
side of center in Fig. 4a, and the lower spectrum in Fig. 5 was taken from the
rectangle in the upper left corner of Fig. 4a. Both spectra have predominant Pd La
peaks at 2.84 keV, but the Pd L/3 peak at 2.99 keV is far more intense in the lower
PdLcc
No Ag detected
3 4
Energy (keV)
PdLp ,
Figure 5. The upper spectrum was taken from the rectangle on the left-hand side of center in
Fig. 4a, and the lower spectrum was taken from the rectangle in the upper left corner of Fig. 4a.
144
3. Discussion
Acknowledgments
This research was supported by a grant from t h e New York Community Trust.
References
1. J. Warner and J. Dash, Proc. 8th Int. Conf. on Cold Fusion; SIF Conf. Proc.,Vo\. 70
(Edited by F. Scaramuzzi), Bologna (2000), p. 161.
2. J. Dash and A. Ambadkar, Proc. 11th Int. Conf. on Cold Fusion (Marseille, France,
2004), p. 477.
3. G. G. Johnson, Jr. and E. W. White, American Society for Testing and Materials Data
Series DS 46 (1970).
4. J. Dash, G. Noble, and D. Diman, Trans. Fusion Technol. 26, 299 (1994).
5. J. Liu, Y. Yu, Y. Li, H. He, H. Tan, and K. Xu, Chem. Abstr. 131, 1303 (1999).
T H E R M A L ANALYSIS OF CALORIMETRIC SYSTEMS
L. D ' A U L E R I O , V. V I O L A N T E , E. C A S T A G N A , R. F I O R E , A N D L . C A P O B I A N C O
ENEA Frascati Research Center, V.Le E. Fermi 45, 00044 Frascati (RM), Italy
E-mail: violanteQfrascati.enea.it
PR. DEL P R E T E
La Sapienza University, Via Eudossiana 18, 1-00184 Roma, Italy
F . T A N Z E L L A A N D M. M C K U B R E
SRI International, 333 Ravenswood Ave., Menlo Park, CA 94025, USA
Calorimetric analysis has been carried out for both electrochemical and gas load-
ing experiment. A finite element modeling for steady state and transient gave
a satisfactory agreement with the experimental results. For electrochemical cells
modeling was applied for isoperibolic and flow calorimeters with the main goal
to optimize the system. For high-temperature gas loading experiments the mod-
eling was applied to translate the temperature field (steady state and transient
three-dimensional analysis), then, in such a case calculations allowed to perform
the calorimetry. This experiment was a replication of the MATRIX experiment
performed at SRI by some of the authors. 1 , 2 A correlation between 4 He production
and excess of power during gas loading of deuterium in palladium was observed.
Excess of power was estimated by means of the temperature measurements and
by comparing experimental data with both the calibration data and the model-
ing results. Also the effect of the room temperature evolution was considered in
the mathematical model of the experiment. 4 He tights stainless steel cell have
been filled first with a Pd-based catalyst then loaded with deuterium or hydrogen
(blank). After filling cells with gas we observed a different thermal behavior of
the cells CI and C2 containing deuterium, compared to the cell C4 containing
hydrogen. The temperature increasing in cells CI and C2 was estimated to be
produced by an additional power source of 0.1 W. The measured excess of helium
was consistent with expected value obtained by assuming that the excess of en-
ergy was produced by a D + D reaction giving 4 He+heat (24 MeV). The slope of
the temperature increasing was larger in cells CI and C2, and after achieving a
stationary condition for the system the temperature of cells CI and C2 increased
again. During the thermal effect an analysis of the gas was done for the cells CI
and C2. An increasing of the helium content was revealed for both the cells. The
He concentration increased up to a factor larger than 2 in both cells CI and C2.
145
146
to characterize correctly all the system, thus improving the response level of the
calorimetric apparatus in term of efficiency and heat excess signal. In a following
step an accurate comparative study of heat and gasses out of cells will be performed.
An important aspect is the evolution of the room temperature (T am b); it will
be observed that a variation of few degrees in the room produces a corresponding
variation in the active zone, although lower because smoothed by the inertia of
the device. In order to separate the effect of heat excess from the effect of the
room temperature evolution, a transient calorimetric description of the system is
required, considering the effect of the room temperature evolution and oscillations
in the mathematical description of the experiment.
H
1
h Cells Feeding
Sampling System
N
Known
Volume
Mass
Spectrometer
|_ Cataly_sts j
The model studies the transient system by taking into account the non-linearity
given by the radiative heat transfer, that couples with the convective mechanism
on the top of the cell, and the time-dependent boundary conditions given by the
room temperature behavior.
147
3D Domain 7
achieved by solving the transient heat transfer equation over the three-dimensional
domain shown below (Fig. 3) with the relative boundary conditions marked over a
significative section represented in Fig. 4.
The heat transfer mechanism can be assumed to be convective around the ex-
perimental device but coupled with a radiative mechanism on the top due to the
local high temperature.
The environment temperature is time-dependent, so that the boundary condi-
tions are moving: the first problem to solve is to obtain a proper approximating
function for the room temperature. The domain can be assumed composed by nine
regions each one different for chemical and physical parameters but homogeneous
and isotropous (Ax = Xy = Xz); the model does not take into account the convective
effect within the cells.
CZZ1 Kn =-H(T-Ta)-OE(T4-Tg)
dn
I 1 K„ =0
dn
• Kn ?L=-H(T-Ta)
dn
where H is the convective heat transfer coefficient (W/cm 2 K), T a the room tem-
perature, e and s, respectively, the emissivity and the Boltzmann coefficient.
During this analysis we have consider two external zones with different thermal
features: on the top the temperature is more elevated than elsewhere.
We can observe that the noise in the room temperature is smoothed by the
device thermal inertia; so we can assume that the real forcing function, that should
be applied as moving boundary condition, is a function obtained by filtering the
noise from the room temperature. This condition can be obtained by mens of a
Fourier's series development of the experimental data:
Tb
Tb Fourier
in
500
495
39
185
180
0 15 30 45 60 75
30 45 60 75
Time (h)
Calculated
Experimental
2. Isoperibolic C a l o r i m e t r y at Low T e m p e r a t u r e
The isoperibolic calorimeter for the characterization of deuterium loading on Palla-
dium foils by electrolytic method Fig. 8 shows both a picture of the apparatus and
its axial section, which allows to high light the most significant elements are shown.
The experimental cell is formed by a Teflon shell closed on the upper side by
a stainless steel cap; two circular quartz windows are placed for laser excitation of
;J^"
Palladium surface. Inside a thin palladium plate constitutes the cathodic element
surrounded by an anodic platinum wire.
The temperature is continuously monitored through two Pt 100 sensors inserted
in suitable measurement seats; a capacitive pressure sensor and a safety mechanical
valve complete the experimental set-up.
The calorimetric apparatus is entirely inserted in a thermostatic box to allow a
stationary room temperature (24°C). Like for the previous one, also for this calori-
metric device a numerical simulation with FEM method could represent a helpful
tool to translate the temperature map into heat flux evaluation: a three-dimensional
Palladium Measurement
cathode
Quartz
window for
Teflon
Sensitivity
304
303 _*
302 ^^~
301 ^*^* --"""
7"(K) 300 ^** J--*"" '""
299 ^rC-~-""*"
298 ^-r^-"""""4"
297 ,s**^
296 —*— S calc
0 0.2 0.4 0.6 0.8 1 1.2 -*— S exp
P(W)
temperature difference between the coming in and coming out water is proportional
to the power produced inside the cell. Then the efficiency of the calorimeter is
represented by the heat recovering capacity of water coil. The goal is to keep heat
losses as lower as possible.
The aim of this paper is to describe a possible approach to characterize the
thermal behavior of flow calorimeter, such obtaining an accurate efficiency mea-
surement: a multi-step procedure which links the heat generated by cell with the
temperature profile of coil axis is described.
In first approximation, it was considered that the entire heat produced is trans-
ferred to the coil water with 100% of efficiency and uniform power distribution,
then, through a monodimensional approach, the temperature profile along coil axis
is calculated by the equation below:
rVcpdT=(W/L)dxJ1 (4)
where r is the density of water, V the volumetric flov/, L the coil length, and x is the
abscissa of coil axis. In the following step a FEM calculation model was realized: the
heat transfer equation in steady state is calculated over the two-dimensional domain
shown in Fig. 12, with the same hypothesis described for isoperibolic calorimeter.
The temperatures calculated in the first step are put inside the coil trace as inner
boundary condition (2"), thus obtaining the temperature T around coil surface.
Water temperature T w
Coil surface
temperature=P
Fourier equation is
div(A * grad (T)) + Q = 0. (5)
Outer boundary condition
Kn(dT/dn) = H(T-Text). (6)
Inner boundary condition
Kn{dT/dn) = H(T - Tw). (7)
Equations (5)-(7) allow us to calculate the temperature profile along coil axis: the
solution is obtained by numerical calculation through Fortran code application.
rVcpdT = Hp(T' - T)dx, (8)
First step
27.4
27.2
27 HT!~ltti
2 6 8
o
°L 26.6
K l^TT
26.4
, rjL.-"
26.2
26
25.8 100
50 150 200
s(cm)
Figure 13. Coil temperature profiles in the first step and second steps.
155
4. Conclusions
References
1. M. McKubre, F. Tanzella, P. Tripodi, D. Di Gioacchino, and V. Violante, ICCF8 Lerici
(May 21-26, 2000) Conf. Proceed., Edited by Italian Phys. Soc. Vol. 70, p. 23.
2. M. McKubre, F. Tanzella, P. Tripodi, and P. Hagelstein, ICCF8 Lerici (May 21-26,
2000) Conf. Proceed., Edited by Italian Phys. Soc. Vol. 70, p. 3.
SURFACE P L A S M O N S A N D LOW-ENERGY N U C L E A R
REACTIONS TRIGGERING
E. C A S T A G N A , C. SIBILIA A N D S. P A O L O N I
La Sapienza University, Via Scarpa, 14, 00100 (Roma), Italy
V. V I O L A N T E A N D F . S A R T O
ENEA Frascati Research Center, V.le E. Fermi 45, 00044 Frascati (Roma), Italy
E-mail: violante@frascati.enea.it; emanuele.castagna@uniromal.it
The study presented deals about both theoretical and experimental aspects of
Surface Plasmons (SP) excitation. The principles of phenomenon rising are showed,
together with the description of experimental devices needed to obtain such an
excitation. The correlation between SP occurrence and electrochemical conditions
is approached.
1. Introduction
Surface Plasmons (SP) (polaritons) are quantum of plasma oscillations created by
the collective oscillation of electrons on a solid surface. SP may be generated by
mechanisms able to produce charge separation between Fermi level electrons and a
background of positive charges (i.e. lattice atoms):
• Electrons beam.
• Laser stimulation.
• Lattice vibrations = Phonons.
• Charged particles on a surface.
Existence of plasmons has been revealed at the gas/metal and electrolyte/metal
Interfaces.1
A strong electric field enhancement arises during SP excitation. This phe-
nomenon could be explained both with classical2 or quantum mechanical3 con-
siderations.
2. Theoretical Aspects
Bulk plasmon frequency is
<4 = , 2.1
where N is the electron density at the Fermi level, e the electron electric charge,
mefr the electron effective mass, £0 = 8.854 x 10~ 12 F i n - 1 the vacuum dielectric
constant, and u is the separation distance.
156
157
of the plasma oscillation from the frequency at the surface of two semi-infinite
mediums (Fig. 1) is the dispersion relation, which under certain conditions could
be written as 4
, UJ j E\E'
K
C\ £!+£'' (2.4)
„ LO jsie' e"
K - .,
x
C V £i + e' 2e'2
If conditions
e'<0, e"<|e'|, £i < |e'| (2.5)
Y.
«1
y « ._, —.-«..
\s\- ""'" ' • •
Expression (2.6) can be easily plotted (Fig. 2). Surface plasmons (polaritons)
excitation by electromagnetic stimulation comes out when the real part of the x
component of the wave vector of the incident wave results to be equal to the one of
the SP (Fig. 2).
The laser beam dispersion relation is
K^ \Je\ sin#. (2.7)
C
Electric field has to belong to the incidence plane, i.e. the wave has to be polarized in
the p mode: if the electric field is perpendicular to incidence plane, and thus parallel
to the interface (s-type polarization), it would assume the same value in the two
mediums, without giving rise to the charge displacement needed to excite SP.
158
16
5x10
3x10
1
2x10
1 x10
K>"1)
Figure 2. Surface plasmons dispersion law for a Pd-air interface and a Pd-glass interface.
The comparison between the expressions (2.6) and (2.7) gives the following plot
(Fig. 3).
No matching condition results to be possible between light lines and SP dis-
persion curve at an air-Pd interface: the matching condition cannot be satisfied
on smooth surface, because the interaction between photons and plasmons cannot
simultaneously satisfy the energy and momentum conservation.4
It is possible to obtain SP excitation also using a corrugation lattice or by
corrugating the metal surface itself: such a corrugation increases the x component
of the laser beam wave vector, making thus possible the coincidence with SP wave
vector:6
Kx = -sm6±AKx = KSP, (2.8)
c
where AKX is defined as
AKX = ±ng, (2.9)
2TT
9 = — • (2.10)
The plot (Fig. 4) shows the possibility to satisfy the matching condition between
the wave vectors of the two curves of interest.
5x10 16
4X10 1
<3? 3 x 1 0 '
i3
2x10 1 6
Pd-air interface
K x '=co/c
K'= a>/tcsin(30")
1x10'
E2
K. (3.2)
c V E + Ex
The field enhancement could be in a phenomenological way expressed as: 2
,16
5x10
/ /
,16
4x10 ^ y /
: ~—-^^ /
% /
3x10
16 /
1 im.
sp,a /
Z
/
3
2x1016 /
Pd-air interface
K^ = co/csin(30")
1 /
16 - 1 /
1x10
? , i-f i
2.0x10',8
B
0.5x10 1.0x10s 1.5x10B
<(m"1)
Figure 4. Increment h.Kx of laser beam wave vector due to roughness, giving rise to SP resonance.
Above equation shows that the change in zero-point energy of the SP oscillator
system precisely corresponds to the classical image potential energy. External point
charge induces a polarization charge density in a metal that is identical to the
distribution induced by a set of SP. In principle, an electrochemical interface may
be equivalent to a system with SP excitation.
At the interface between metal and electrolyte the electrode potential EQ is given
by:9
eE0 = AG A + Ad + AG Id Vc, (4.3)
where AG A is the free energy of atomization of the metal, AGj the free energy of
ionization (that is the ionization potential), AG Hid the free energy of hydration,
and 6 is the metal work function.
161
To create the double layer the minimum value of cathodic fall (Vc)min has just
to overcome the coulombic attraction between the positive surface ions and the
electron gas wave at metal surface:
5. Conclusions
External charges on a surface act as a set of SP: an external triggering, such as a
laser beam, could force the electrolytic system to realize the same conditions causing
the rise of events perhaps proving the occurrence of L E N R . T h e electrode potentials
appropriate to the cathode-electrolyte interfaces (i.e. cathode falls) are related to
the interfacial plasmon energies.
This picture creates a link between the electrochemical interface structure and
the electrodynamics processes occurring at the interface.
References
1. A.M. Brodskii, Electrokhimiya 22(2), 270 (1986).
2. W.H. Weber and G.W. Ford, Opt. Lett. 6(3), 122-124 (1981).
3. A.K. Sarychev, V.A. Shubin, and V.M. Shalaev, Physics B 279, 87-89 (2000).
4. H. Raether, Surface Plasmons on Smooth and Rough Surfaces and on Gratings
(Springer-Verlag, Berlin Heidelberg, 1988).
5. V. Fano, J. Opt. Soc. Am. 3 1 , 213 (1941).
6. A. Otto, Z. Phys. 216, 368 (1968).
7. A.Z. Zangwill, Physics at Surfaces (Cambridge Press, Cambridge, London).
8. A.K. Vijh, Electrode potentials and interface plasmons in the metal/gaseous
electrolyte (i.e. plasma) interphasic Region, Mat. Chem. Phys. 14, 47-56 (1986).
9. A.K. Vijh, J. Chem. Phys. 71, 812 (1975).
PRODUCTION METHOD FOR VIOLENT TCB JET PLASMA
FROM CAVITY
FARZAN AMINI
Department of Mechanical Engineering, Farab Company, No. 30,
Mirhadi St. Vali-e-Asr Ave., Tehran, Iran
E-mail: farzanaminiQyahoo. com
The present paper aims at studying transient cavitation bubbles (TCB) jet plasma
when such phenomenon like load rejection happens in a hydropower plant; this
phenomenon creates a significant cavity at downstream. This process generates
abundant tiny bubbles at the micro or nanolevels. The cavity collapses more
violently; therefore, higher energy density in the cavity contents is produced. The
level of collapsed energy and frequency is controllable by the use of air injection.
The load rejection tests at a specific operating regime are utilized to investigate
the released energy, which is much more than that of regular TCB experiments.
Nomenclature
AQ sectional area of draft t u b e exit
Cp pressure coefficient
Cpa area-mean pressure recovery coefficient
Ha atmospheric pressure
Hs Suction head
Hu vapor pressure
K polytropic index
Leq equivalent length of foot portion
p'v saturated vapor pressure at liquid temperature
p'L liquid density
p'0 initial liquid pressure at equilibrium
P pressure
Pai area mean static pressure at inlet section
Pc inner pressure of cavity
PQ static pressure at the exit of draft tube
Q flow r a t e
r radial position
rc radius of cavitation rope
rv core radius of Rankine vortex
R radius of pip wall
i?H dimensionless bubble radius
Re Reynolds number
R'0 initial equilibrium bubble radius
vc cavitation volume
163
164
Greek symbols
F circulation
a cavitation number
p density
1. Introduction
One of our hydropower plants (Masjed - E - Soleyman, Iran) has four Francis tur-
bines. Two units on the right side (looking downstream) share a common penstock
and a common long tailrace tunnel, and the other two units on the left also share
a penstock and tailrace tunnel.
Upon commissioning of one unit, the hydraulic transient in the draft tube during
load rejection above 75% was excessive. It was apparent that the guide vane closing
law that had been adopted would result in water column separation during load
rejection at full power. Tests with a slower closing rate showed that the risk of
column separation was reduced, but a violent surge developed in the draft tube
close to maximum over speed.
The energy level and cavity volume that are produced are much more than those
of regular transient cavitation bubbles (TCB) experiments, and therefore, we should
expect more intense effects than a regular TCB jet produces.
f °lw/1.
+
log of the acoustic wave
% bar %
Test results
Also one pressure transducer measuring —1.0 to 25.0 bar located at the spiral case.
T h e flow in the draft t u b e is complex because the turbine often operates outside
166
-5 0 5 10 15 20 26 30 35
Figure 2. The decreasing of the draft tube pressure peak upon load rejection with the increase
air quantity.
its best efficiency point. The first and best-known surging problem is caused by
the helical vortex cavity that causes pressure fluctuations in the range of 50-70%
of the output at the best efficiency point. The draft tube cavity is filled with water
vapor, and air if the turbine has provision for air admission in the center of runner.
Air admission was proposed as a method of damping or suppressing the surge, as
shown in Fig. 2.
The frequency of this partial load pressure fluctuation is often referred to as the
"Rheingans frequency," and it is approximately one-third of the rotational speed of
machine. The runner and draft tube design as well as operating conditions influ-
ence the frequency and amplitude of fluctuations. Currently, available theoretical
approaches are not able to model this phenomenon accurately.
In turbine model tests with provision for the observation of draft tube flow at
the partial load conditions, the cavity is visible at low sigma values (low suction
pressure) as a helical void rotating in the same direction as the runner (Fig. 3).
For operation at full power, the helical cavity evolves into an axially symmetrical
cavity with rotation in the direction opposite to the runner rotation. This may be
accompanied by pressure fluctuations and possible auto-excitation.
4. Cavity M o d e l
The natural frequency cavity of draft tube vibrating system with cavitation region
is expressed as the following relationship: 3
1 AQrc
/s (1)
2w y pLeqVc
See the "Nomenclature." All parameters except the cavitation volume Vc in the
above equation can be determined. Observation of the cavitation vortex rope in a
draft tube indicates that its radius decreases gradually from the inlet to the elbow.
In operating condition where a single, cavitation vortex rope is observed, we see the
root of the rope usually locates at the center in the inlet section of a draft tube.
Thus, the flow field can be regarded as axisymmetric at the inlet. The distribution
of circumferential velocity is assumed to be that of the Rankine vortex. Then, the
velocity and static pressure distributions are expressed as follows:
pT2(r2 rc2)
Pe-
rn
168
Vu=^, (4)
2irr'
prVi i V pr2(r2v-r 2
c; c)
P =^ (
2 ^ 2- ^ )
8ir V r 2 + ^r;" 42'
r / 87r r
+pc (5)
As a representative averaged pressure at the inlet section is required for deter-
mining the radius of cavitation rope r c , we use the area-mean pressure recovery
coefficient defined as follows:
(6)
^-pM + Vv&p
where
(7)
TTJ?2'
p W 2 / r2c \ pY2 ( 1 3 f T iA
P + +P (9)
- = ^ M l ^ ~ J "^Ul " 16^ " 4 ^ ] -
Substituting Eq. (9) into Eq. (26), and using the following equations:
Ha-Hs-Hv
Kl (10)
~ ul,2g '
Po h + Ha-Hs. (11)
P5
We have
r4 i? 2 r 2 /i?2 3 1 R\ TZ ( Q 1
I n - - Ki [£-) + Cp, + 0. (12)
8r 4 4r 4 \ Irl 8 2 rv / \TR TRJ 4
In violent bubble collapses, as observed in caviting flows, the bubbles can break
up into many smaller fragments. Following the recent work of Brennen, depending
on either Reyleigh-Taylor instability or micro-jet formation mechanisms, a simple
bubble fission model is introduced to explore the rebound structure after fission and
the energy dissipated in the process.4
As mentioned a bubble fission model to describe the rebound structure of the
fission fragments, thereby, the energy dissipated due to bubble fission, using a mod-
ified Rayleigh-Plesset equation. It is difficult to determine the number of product
bubbles that would come out following bubble fission.
Where
Cp = Vo (14)
WLU'2
Re = PLU'R'O (15)
ME
and
PLU'2R'O
We = (16)
According to Eq. (12), during load rejection test, the volume of the cavity is
highly dependent on the speed and position of wicket gates, and the rate of change of
wicket gate position causes an initial pressure drop for cavity surroundings followed
by an increase in that pressure. Therefore, cavity bubbles are affected according to
Eq. (13), breaking into smaller fragments. In the transition time, Fig. 1 shows that
the energy dissipated due to fission when the number of fission products is large.
This process generates many tiny bubbles at the micro or nanolevels, which is one
of the characteristics of hydroturbines.
50.00 200.0
47.50 65- _" _ ,_ _ 190.0
45 00 180.0
6 0
42.50 170.0
40.00 55- 160.0
37.50 5 0 150.0
35.00 4 5 140.0
32.50 4 0 130.0
30.00 120.0
35-
27.50 110.0
25.00 3 0 100.0
22.50 2 5 90.0
20.00 2 0 80.0
17.50 70.0
1 5-
15 00 60.0
12.50 1 0- 50.0
10 00 05- 40.0
7.50 30.0
00-
5.00 >• % - * - - ~ „- *r - - - , S&^<J,fiuio< 20.0
2.50 -0 5- 10.0
0.00 -1 tv 0.0
) 5 10 15 20 25 30 35 40 45 50 55 60 65 70 75 80 85 90
•«*• Penstock [bar] — Draftjubel [bar]^Draft„tube2 [bar]™ Speed_U4[%] «~S.M. opening_U4[%] •— Headcover press, [bar]
— Flap gate pressure [bar] — Air press, vessel [bar] Air press, a. valve [bar] Deflection [mm]
Figure 4. Several examples of TCB jet plasma generation by opening and closing of the wicket
gates.
5. Conclusion
A helical cavity, which is formed in hydropower plants during load rejection, can
collapse, and violent TCB jet plasma can be implanted. It appears possible to
170
simulate these phenomena (load rejection). Its energy is achievable and controllable.
T h e level of collapse energy and frequency is controllable by the use of air injection.
It is possible to generate T C B jet plasma when the wicket gates open and close
several times during load rejection.
Acknowledgment
References
1. R. Stringham, Cavitation and fusion, in: Tenth International Conference on Cold Fu-
sion (2003).
2. R. Stringham, Pinched cavitation jets and fusion events, in: The Ninth International
Conference on Cold Fusion, Condensed Matter Nuclear Science (Tsinghua University
Press, Beijing, China, 2002).
3. X. Wang, M. Nishi, and H. Tsukamoto, A simple model for predicting the draft tube
surge, in: XVII IAHR Symposium, Section on Hydraulic Machinery and Cavitation,
Beijing (1994).
4. M. Tunc and F. Delale, Energy dissipation due to fission of cavitating bubbles, in: Fifth
International Symposium on Cavitation (Osaka, Japan, 1-4 November 2003).
N E W RESULTS A N D A N ONGOING EXCESS HEAT
CONTROVERSY
L. KOWALSKI
Montclair State University, Montcalir, NJ, USA
E-mail: kowalskil@mail. montclair. edu
R. SLAUGHTER
Advanced Energy Industries, Fort Collins, CL, USA
E-mail: rslaughterQcompuserve. com
Mizuno-type cells (glow discharge plasma electrolysis) were used to measure ex-
cess heat generated at several potentials between 250 and 650 V. No significant
amounts of excess heat were detected. That conclusion contradicts findings of
several researchers.
1. I n t r o d u c t i o n
This report describes results of two separate experiments, one conducted in the
EarthTech laboratory (Austin, T X , USA) and another in the laboratory of Richard
Slaughter (Boulder, CL, USA). T h e purpose was to either confirm or refute reality
of excess heat in a plasma electrolysis cell. Our experimental setup was similar to
t h a t of Fauvarque et al.1 It is a jar with an electrolyte (K2CO3, 0.2 M) containing
two electrodes: a cylindrical anode (platinized niobium) and a tungsten cathode
(welding rod). A constant difference of potential, for example, 400 V, is applied
to electrodes and a glowing layer of gas is formed around the cathode. Three
parameters are measured during each test: the electric energy delivered to the cell,
E, the amount of heat lost through water evaporation, Q i , and the amount of water
lost through conduction and radiation Q2. T h e difference between Q i + Q2 and E,
if any, is called excess heat. As in Ref. 1, our experimental results are reported in
terms of the coefficients of performance ( C O P ) . T h a t coefficient is simply the ratio
(Qi+Q2)/£-
171
172
2. Experimental Results
According to Ref. 1, the COP, at 350V, is approximately 1.35. Our results, 2 ' 3
shown in Table 1, conflict with that conclusion.
Volts 250 250 300 300 300 355 350 350 400 650
COP 1.00 0.99 0.97 1.00 1.00 1.02 1.03 0.98 1.05 1.05
The first nine results are based on experiments performed in Texas 2 ' 3 , the last
result is based on experiments performed in Colorado. 4 The Colorado setup was
similar, in principle, to that in Texas except for the power supply (see Appendix 1).
An important observation concerning both experiments can be seen in Appendix 2.
The Colorado experiment was simply a 21 beaker, mounted on a balance, with two
electrodes.
Another difference between our two experiments was that the diameter of the
anode in Texas was 6 cm while in Colorado it was 3 cm. The range of potential
differences in Colorado was from 500 to 700 V. The mean value of COP in that region
turned out to be 0.90±0.2. The last value 1.02, shown in Table 1, resulted from eight
separate tests. The standard deviation calculated from these tests turned out to be
0.11. It is interesting that foaming and splashing in Colorado was so insignificant
that an experiment could be conducted in an open beaker. We believe that this was
due to the differences between the power supplies used in two experiments.
3. Discussion
Favarque et al. report observing COP's up to 1.4 in their experiments. Similar
values were observed by other researchers. Clearly we have not replicated such
results. How can this be explained? By experimental errors (measuring E, Qi,
and Q2), or by unrecognized, but significant differences in experimental setups.
Conditions under which experiments were performed might also have been different.
Our anodes, for example, were made from platinized niobium while the anode used
in Ref. 1 was made from platinized titanium. Instruments used to measure E were
also very different. Accurate measurement of the electrical input power during
plasma operation is complicated by the highly erratic current.
In Texas, for example, the average current drawn by the cell was 2-3 A but the
waveform peaks frequently exceeded 10 A. A sophisticated Clarke-Hess instrument
was able to recognize overloads and signal them by flashing. On a less sophisticated
instrument such conditions might be overlooked and will lead to underestimation
of the average power being delivered to the cell. Overloads were observed during
the initial testing; they were eliminated by placing a large filter capacitor between
the Clarke-Hess instrument and the cell, as described in Ref. 8. Possible errors in
measuring Qx and Q2 are discussed in Ref. 3.
173
Let us mention that appearances of the cathode glow discharge in Texas and in
Colorado were quite different. In the first case, we occasionally observed white light
flashes coming from large regions inside the cell, in the second only a steady yellow
light was seen from a small region surrounding the cathode. Intense white light
coming from large regions inside the electrolyte can also be seen on the Internet
pictures of similar experiments performed by other researchers. Another difference
worth mentioning was the fact that a typical current (for a given voltage) in Texas
was about four times higher than in Colorado. The plasma differences between
Texas and Colorado experiments were probably due to the arc suppression abilities
of the Colorado power supply (see Appendix 1).
Why is excess heat observed in some recent experimental s e t u p s 1 ' 5 - 7 and not in
others? 8 Are the discrepancies due to experimental errors or to unrecognized, but
essential, ingredients present in some setups and absent in others? It is difficult to
answer such questions. Scientific disputes are not resolved by voting but a large
number of confirmations of excess heat, by qualified researchers in many countries,
should not be ignored. The existing controversy would be eliminated if a highly
reliable portable excess heat generator could be built. Such generator would then
be studied in different laboratories. How else can a consensus be reached?
Referring to the issue Jed Rothwell9 wrote: "This is more art than science.
Direct, hands-on learning may be the only way to grasp these things; Mizuno himself
does not know what is going on in many ways. Building devices on the basis of
described protocols does not seem to be sufficient." That is a very good point. A
tentatively accepted theoretical model would certainly synchronize our efforts to
make sense out of what is going on in the CMNS field. Trying to confirm or to
refute claims made by individual researchers is certainly much less effective than
testing various aspects of a tentatively accepted model.
The supply provides very accurate power measurements and the ability to control
how the power is delivered to the cell. Pinnacle can be used as a source of constant
voltage, constant current, or constant power, depending on what is chosen. The
other two parameters are then determined by the load. The output voltage, current,
or power will hold to within ± 1 % as long as the load impedance stays within the
voltage and current limits of the unit. Our tests were performed by using the
constant voltage mode, in the voltage range between 400 and 800.
The low-stored energy of the output filters of the Pinnacle allows the regulation
system of the supply to rapidly respond to changes in the cell impedance. The low-
stored energy also prevents the supply from dumping large amounts of energy into
the cell as its impedance changes. The low-stored energy is probably one reason
that we did not experience the violent reactions in the electrolyte. The other reason
was probably the built-in arc suppression.
The pinnacle has several methods of arc suppression. The one we used is called
"micro-arc suppression." When an arc of less than 10 (is occurs, the stored energy is
diverted from the cell and the growing arc is extinguished. The voltage is restored,
approximately 5 ^s later. This ability is used in industry to maintain steady even
plasma that are required for precise deposition of material on the manufactured
product.
This arc suppression in combination with the low-stored output energy of the
Pinnacle was most likely the reason that we were able to increase the potential
difference to over 700 V without the violent reactions in the electrolyte. The arc
suppression might also be a reason that our results are different from those reported
in Ref. 1.
According to Ref. 9, Mizuno says "anyone can generate plasma with hundreds
of volts. The trick is to generate it and then gradually reduce input power to the
minimum." In one of his papers he writes: "Some researchers have attempted to
replicate the phenomenon, but it has been difficult for them to generate large excess
heat. They have tended to increase voltage to a very high value, around several
hundred volts, but they measured no excess heat." Mizuno also indicates that when
the cell begins to produce excess heat the conditions inside the cell are placid. These
are the same conditions that we observed in Colorado.
We recognize that the cost of the Pinnacle would make it prohibitive for most
experimenters. There are, however, less expensive techniques for arc suppression
that could be added to power supplies. It is likely that arc suppression will help
to minimize the power delivered to the cell, at a given voltage. This might be an
important precondition for the generation of excess heat, as indicated by Mizuno.
175
is to focus on the most interesting new results. But is this appropriate? I do not
think so. Negative results should not be confused with unreliable results ..."
But the situation is complicated by the fact that some researchers might be
hesitant to publish negative results. They might fear that negative statements,
taken out of context, can be quoted by pathological skeptics criticizing the field.
In our opinion, such fears are not justified; benefits from sharing all reliable results
far outweigh negative consequences of self-imposed secrecy. Unscrupulous critics,
such as Dr. Richard Park, should not be feared by honest researchers. The issue of
publishing negative results goes to the heart of scientific methodology. Here is what
Ed Storm wrote about publishing negative results (a private message, 11/19/05):
"I would like to throw out some counter thoughts. I think publishing negative
results is a waste of time unless these results reveal a useful pattern. For most
phenomena, millions of ways are available that will fail to generate the desired
results. In contrast, many fewer methods will give the desired results. When isolated
negative results are reported, they provide no guidance because they are only a few
of so many possible ways to fail. The negative results must be shown to relate to a
pattern or a general characteristic. For example in CF, if the H2O content of the
electrolyte is too high, the results will be negative over a wide range of concentration.
Unless this fact is related to a positive result obtained when the H2O content is
low, the observations have little value. My point is that people reporting negative
results should be required to show an understanding of their meaning just as people
reporting positive results must show what their results mean. However, this does
not mean that negative results can be used to deny the possibility of positive results.
The two kinds of results have very little relationship to each other until the positive
results are well understood, because as I said at the start of these comments, many
ways exist for a real result to fail."
We do not agree with this. Negative results are worth sharing and discussing. In
this report, for example, one of us (R.L.) speculated that our negative results might
be associated with the absence of arcing (collecting data when arcing was not too
intensive in Texas and suppressing arcing electronically in Clorado). Is it possible
that arcing superimposed on the quite glow discharge is an essential component of
a device generating excess heat? R.L. plans to answer this question experimentally
in the near future. We think that negative results are worth sharing because, like
positive results, they guide our attempts to understand what is going on.
At one point, two of us (R.L. and L.K.) were discussing the magnificent Naudin's
report:
http://jlnlabs.imars.com/cfr/html/cfdatas.htm
The scatter plot called "efficiency..." shows results from a large number of
experiments that were similar to ours. We noticed that in all 22 experiments (per-
formed at 200 V or above) the excess heat was larger than 20% of the input energy.
That is a highly significant result; the voltage-dependence trend seems to be consis-
tent with what was reported in Ref. 1. That is how the issue of "publishing positive
results only" came about. Negative results were not mentioned. We assumed that
177
P.S.
Subsequently Ed wrote: "You may quote me and even use my name. However,
your counter argument to my comment missed the point I was making. As I said,
"I think publishing negative results is a waste of time unless these results reveal a
useful pattern." T h e "useful pattern" is the important aspect of my comment. In
your reply, you showed t h a t your negative results were being used to reveal a useful
pattern, i.e. t h a t the nature of arcing was a possible important v a r i a b l e . . . During
my present study of the F - P effect, I have had many "negative" results. However,
I know t h a t certain variables are important and must be controlled. For example,
no excess energy is possible unless the D / P d ratio in the surface is very high, which
is a difficult condition to achieve. Therefore, I a m investigating the processes t h a t
affect this composition. If I report all the negative results without relating t h e m to
the important variables, I would be wasting everyone's time.
References
1. J. Fauvarque, P. Clauzon, and G. Lalleve, Abnormal excess heat observed during
Mizuno-type experiments. Laboratoire d'Electrochimie Industrielle, Conservatoire
National des Arts et Metiers: Paris (2005). Available as: (http://www.lenr-
canr.org/acrobat/FauvarqueJabnormalex.pdf)
2. See (http://www.earthtech.org/experiments/Inc-W/Fauvarque)
3. See (http://blake.montclair.edu/~kowalskil/cf/2671ittle.html)
4. See (http://blake.montclair.edu/~kowalskil/cf/270slaughter.html)
5. T. Mizuno, D. Chang, F. Sesftel, and Y. Aoki Generation of Heat and Products Dur-
ing Plasma Electrolysis, in Eleventh International Conference on Condensed Mat-
ter Nuclear Science, (Marseille, France, 2004). Downloadable from the library at
(http://www.lenr-canr.org)
6. D. Cirillo, A. Dattilo, and V. Iorio, Transmutation of metal to low energy in confined
plasma in the water (electrochemical plasma cell), in Eleventh International Confer-
ence on Condensed Matter Nuclear Science (Marseille, France, 2004). Downloadable
from the library at (http://www.lenr-canr.org)
7. Jean-Louis, Naudin et al. Several illustrations and references are downloadable
from (http://jlnlabs.imars.com/cfr/index.htm) and from (http://jlnlabs.imars.com/
cfr/html/ cfrtpwr.htm)
8. Scott R. Little, H.E. Puthoff, and Marissa E. Little, Search for excess heat from
Pt electrolyte discharge in K2C03-H20 and K2C03-D20 electrolysis. Downloadable
from (http://www.earthtech.org/experiments/Inc-W/Mizuno.html)
9. Jed Rothwell, private communication (November, 2005).
10. The Advanced Energy Industry Inc, Fort Collins, Colorado, 80525
(http://www.advanced-energy.com/upload/Pinnacle%20Series%20DC%
20Magnetron%20Power%20Supplies.pdf)
OBSERVATION OF SURFACE D I S T R I B U T I O N OF P R O D U C T S B Y
X-RAY FLUORESCENCE S P E C T R O M E T R Y D U R I N G D2 GAS
P E R M E A T I O N T H R O U G H Pd COMPLEXES
YASUKO TERADA
Japan Synchrotron Radiation Research Institute, 1-1-1 Kouto, Sayo-cho, Sayo-gun,
Hyogo 679-5148, Japan
T E T S U Y A ISHIKAWA
Coherent X-Ray Optics Laboratory, RIKEN Harima Institute, 1-1-1 Kouto, Sayo-cho,
Sayo-gun, Hyogo 679-5148, Japan
1. Introduction
Low-energy nuclear transmutations in condensed matter have been observed in Pd
complexes which are composed of Pd and CaO thin film and Pd substrate, induced
by £>2 gas permeation through Pd multilayer complexes. We already reported
transmutation reactions of Cs into Pr, Ba into Sm and Sr into Mo, respectively.1_5
Figure 1 shows schematic of our method. Our experimental method can be char-
acterized by the permeation of D2 gas through the Pd complex and the addition of
an element that is specifically targeted to be transmuted. Permeation of deuterium
is attained by exposing one side of the Pd complex to D2 gas while maintaining
178
179
the other side under vacuum conditions. On the D 2 gas side of the Pd complex,
dissociative absorption causes the D 2 molecules to separate into D atoms, which
diffuse through the Pd metal toward the vacuum side, where they emerge from the
Pd metal, combine and are released as D 2 gas.
D permeation
t i i
I D flux
I Vacuum 1
2. E x p e r i m e n t a l
Fabrication of Pd complex is basically the same as before. 1-5 A Pd was washed with
acetone and annealed in vacuum (<10~ 7 torr) at 900°C for 10 h. It was then cooled
to room temperature in furnace and washed with aqua regia to remove impurities
on the surface of the Pd plate. The surface of the plate was covered by layers
of CaO and Pd, which were obtained by five times alternatingly sputtering 20 A
thick CaO and 200 A thick Pd layers. Then a 400 A thick Pd layer was sputtered
on the surface of the CaO and Pd layers. These processes are performed by Ar
ion beam sputtering method or magnetron sputtering method. After forming a Pd
complex, Cs was deposited on the surface of the thin Pd layer. Cs was deposited
by electrochemical method or ion implantation method.
180
D2 gas inlet
Figure 2 shows the experimental setup for in-situ measurement. Synchrotron or-
bital radiation X-ray (5.97 keV) is introduced into the permeation chamber through
a Be window and attacks on the surface of Pd complex sample. X-ray intensity is
about from 1012 to 10 13 photons/s. Cs-L and Pr-L lines can be detected by a Silicon
Drift Detector (SDD). The SDD is covered by a CI filter for suppression of Pd-L
X-ray. We made D2 gas permeated through a Pd complex with Cs for 10-14 days.
D2 gas pressure is about 170 kPa and the temperature was 70°C. X-ray fluorescence
spectrometry was performed during D2 permeation in-situ at the beginning and the
end of experiments.
Surface distribution of Cs and Pr can be measured by the experimental setup
shown in Fig. 3. The synchrotron radiation X-ray is divided by slits and we get
rectangular micro X-ray beam. In this study, we use 500 and 100 /im beams. The Pd
complex sample is attached on an X-Y stage that can be moved by stepping motors,
two-dimensional XRF spectra can be obtained by this setup. Surface images can
be taken by a microscope that is equipped for this two-dimensional XRF spectrum
analysis. We can obtain the information about correlation between distribution of
elements and surface images.
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Energy (keV)
Figure 4. Confirmation of transmutation of Cs into Pr using ion beam implanted sample (SP-24)
by in-situ measurement.
(voltage: 5kV, dose: 2.5 x 10 1 4 /cm 2 ). In this case, we use 1mm 2 X-ray beam. As
shown here, Cs peaks decreases and Pr peak emerge after D2 gas permeation at
the shown point. It can be seen that transmutation of Cs into Pr occurred at this
point. However, no Cs was changed and no Pr was seen except this point in the
case of SP-24.
Another example of in-situ measurement is shown in Fig. 5. Electrochemical
deposition 1 was applied to this sample (SP-33). Pr was detected at points 2, 3,
8, and 9, although no Pr was detected at the points 4-6, 10-12. We could not
see initial Cs at the points 1, 7, 13-15 because Cs distribution is not uniform if
we applied electrochemical Cs deposition method. Initial and final XRF spectra at
point 2 are shown in Fig. 2. Cs peaks decreased and a Pr peak emerged after D2
gas permeation. The ratio of minor peak of Cs-L to major peak of Cs-L is always
constant, so we can judge that the peak near 5keV is attributed to Pr-L X-ray.
This result also demonstrates that transmutation reaction of Cs into Pr occurs in
this experimental system.
Let us move on to the next point. Figure 6 shows Pr detection by XRF method
performed in 2003. FG1 was fabricated by the Ar ion beam sputtering method and
permeated for 97 h by D2 gas at 70°C. FG2 was made by the magnetron sputtering
method and permeated for 96 h by D2 gas at 70°C. Pr-L lines were clearly in both
foreground samples, while no Pr peak could be seen in the background sample.
Pr surface distribution measurements were done for FG1, FG2, and SP-24 by
small size X-ray beams in 100 and 500jum2.
182
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Energy (keV)
Mapping data of Pr for FGl analyzed by 500 fjm X-ray beam is shown in
Fig. 7(a). Pr could be detected from all the points (400 points) in the analyzed
region in 10 mm x 10 mm. Detection of Pr is consistent with the above XRF mea-
surement in 2003. In addition to Pr, we detected the other peaks for 27 points.
A peak around 4.5 keV can be seen at point 284. Levels of Pr seem to be almost
uniform for these points. We can estimate that these peaks correspond to about
5 x 10 13 atoms/cm 2 by the comparison with XRF spectra using a reference sample
2 3 4
X-ray energy (keV)
Figure 6. Detection of Pr by XRF in 2003 (FGl and FG2; D 2 permeated samples, BG; No
permeated sample).
183
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Figure 7. Surface distribution of Pr for F G l using 500 (im X-ray beam; (a) Mapping of Pr and
unidentified element, (b) X R F spectra for the points 281-285, (c) surface image of F G l for the
points 282-286.
in which Pr was already implanted. Figure 7(c) shows corresponding surface image
taken by a microscope. It seems that there are no specific or special features for
the point. 284 under this measurement condition.
Mapping data of Pr for FG2 analyzed by 500 fim X-ray beam is shown in Fig. 8(a)
P r was observed at 61% points (74 points) in the analyzed region in 5.5 mmx 5.5 mm.
Detection of Pr is consistent with the 2003 XRF measurement shown Fig. 6. In this
case, we could not see any "unidentified peaks" shown in Fig. 7 (FGl). No Pr was
184
5.5 mm
5.5 mm
detected in 39% of the points. XRF spectra for points 75-79 by 500 /an beam are
shown in Fig. 9(a). The strengths of Pr seem to be slightly changed depending on
measured points, however, no clear difference seems to be seen as shown in Fig. 9(b).
XRF spectra using 100 /im beam for the point 27 are illustrated in Fig. 9(c)
and the surface image for the corresponding region is shown in Fig. 9(d). The
"unidentified peak" emerged at the point 5-1 in the point 27, although we could
not observe the "unidentified peak" if we used a 500 /an beam. This fact suggests
that the "unidentified" element was so localized and so small that the signal from
the element was buried when we used large beam (500/an). It also seems there are
specific or special features for the point 5-1; or if there are specific structures, they
might be much smaller than this image.
Based on the XRF spectra, La, Ba, and Ti are candidates for the unidentified
peak. At the present stage, we cannot completely exclude the possibility that the
peak is derived from a localized impurity. Further investigation by other measure-
ment methods is necessary.
Sample SP-24, originally measured in-situ, was analyzed by small size X-ray
beams in 100 and 500/an 2 5 months after the permeation experiment. Pr could
be observed again in the same region as the in-situ measurement. The surface
distribution of Pr for SP-24 by 500 /an X-ray beam is shown in Fig. 9(a). Pr was
observed only at six points and the "unidentified" peak was observed at two points
even though we used 500 /an X-ray beam. As for SP-24, reaction rate is lower than
FGl and FG2. At present, the authors cannot explain completely the difference of
185
77
Energy (keV)
(a) (b)
Energy (keV)
(c) (d)
Figure 9. Surface Distribution of P r for FG2 using 500/im and 100 /im X-ray beams, continued:
(a) X R F spectra for the points 75-79 by 500 pm beam, (b) surface image of FG2 for points 75-77,
(c) X R F spectra using 100 /ini beam for the point 27, (d) surface image of FG2 for the point 27.
reaction rates between these three samples. It should be investigated further, since
clarifying the factors that make influence on the transmutation rate is an important
and valuable task to increase transmutation rate.
Figure 9(b) and (c) shows surface distribution of Pr and XRF spectra obtained
by 100/an X-ray beam for point 13-4 shown in Fig. 9(a). The amount of Pr changed
greatly depending on the locations of the Pd surface. Pr is localized at the specific
points shown in Fig. 9(c). Surface image for the corresponding region is shown in
Fig. 9(d). No clear correlation between the localized Pr and surface image could be
observed.
These experimental results suggests that transmutation reaction rate varies de-
pend on the Pd surface region. And if we postulate that the unidentified peak is
derived from a transmuted element, transmutation pass might be changed depend-
186
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Figure 10. Surface Distribution of Pr for SP-24 using 500/im and 100 /mi X-ray beams, (a) map-
ping of P r by 500 jim beam, (b) mapping of P r by 100 /im beam a t point 13-4, (c) X R F spectra
depending on location obtained by 100 mn beam, (d) Surface image of SP-24 corresponding to
X R F spectra.
4. Concluding R e m a r k s
One of our experimental apparatus was carried to SPring-8 for the purpose of in-situ
measurement and we obtained clear Pr signals after D2 gas permeation by the X-ray
fluorescence method. According to the micro X-ray beam measurement, we noticed
that Pr was localized greatly. At present, the correlation between products and the
surface structures is not clear. Further investigations are necessary, for example,
using smaller X-ray beam or analyzing these samples by the other methods.
187
Acknowledgments
References
1. Y. Iwamura, M. Sakano and T. Itoh, Jpn. J. Appl. Phys. 4 1 , 4642-4648 (2002).
2. Y. Iwamura, T. Itoh, M. Sakano, S.Kuribayashi, Y. Terada, T. Ishikawa and J.Kasagi,
Proc. ICCF11, Marseilles, France, Oct. 31—Nov. 5 (2004), World Scientific, Singapore,
pp. 339-350.
3. Y. Iwamura, T. Itoh, M. Sakano, S. Sakai and S. Kuribayashi,. Proc. ICCF10, Cam-
bridge, USA, 24—29 August (2003), World Scientific, Singapore, pp. 435-446.
4. Y. Iwamura, T. Itoh, M. Sakano and S. Sakai, Proc. ICCF9, Beijing, China, 19-24 May
(2002), pp. 141-146.
5. Y. Iwamura, T. Itoh and M. Sakano, Proc. ICCF8, 21—26 May (200 ) Lerici, Italy,
SIF Conf. Proc. 70, 141-146.
D I S C H A R G E E X P E R I M E N T USING P d / C a O / P d
MULTI-LAYERED CATHODE
S. N A R I T A , H. Y A M A D A , D . T A K A H A S H I , Y . W A G A T S U M A , S. T A N I G U C H I A N D
M. I T A G A K I
Department of Electrical and Electronic Engineering, Iwate University, J^-3-5 Ueda,
Morioka, Iwate 0208551, Japan
E-mail: narita@iwate-u. ac.jp
1. Introduction
For the study of low-energy nuclear reaction in condensed matter, the discharge
method is thought to be one of the effective ones and the advantages have been
shown by several researchers. We have performed discharge experiment exposing Pd
or Pd deuteride in high-purity deuterium gas changing the experimental conditions;
the pressure of deuterium in the chamber, electrode shape, duration time and so on.
In such experiments, we have demonstrated that anomalous gamma radiation with
energy around ^100 keV, and it was suggested that some short-lived radioisotopes
were produced. 1 However, the reproducibility of the phenomena was quite low and
we have not specified the origin of the radiations.
Besides the discharge experiment, there is a well-established technique for low-
energy transmutation study, that is, deuterium permeation method using multi-
layered Pd/CaO complex sample. In the method, the transmutation from Cs to
Pr, Sr to Mo, and Ba to Sm was observed with good reproducibility. 2 ' 3 Although
the reaction mechanism has not been clarified theoretically, it has been claimed
that sufficient D flux in the permeation through the sample and Pd/CaO multi-
layered structure of the sample, especially for existing CaO layer, are necessary for
triggering the phenomenon in the method.
In this study, considering those experimental results, we performed discharge
experiment in deuterium gas using Pd/CaO multi-layered cathode on which Cs
188
189
is deposited and searched for peculiar phenomena, which suggests that occurring
nuclear reactions especially for Pr production by the transmutation from Cs, just as
observing in the permeation experiment. In addition, we investigated the possibility
of other element production and the isotopic abundance of the elements detected can
be an evidence of nuclear reaction. According to recent reports, laser irradiation
to hydrated/deuterated metal sample is supposed to initiate and/or amplify the
nuclear effect in condensed matter, even the power is just a few 10 mW. 4 , 5 Then,
we also tested the effect of irradiating the laser light to the cathode sample during
discharge in this experiment.
2. Experiment
We tested two sets of experimental conditions. One is the so-called our conventional
glow discharge under low-deuterium pressure with foil type anode. The other set
is corona discharge (partially breakdown discharge). This is under higher pressure
with needle type anode. The energy of deuterium ions irradiated to the cathode is
supposed be lower than that in glow discharge. In terms of the motion of D ions on
the sample surface, this condition is thought to be more similar to permeation's.
We used two different types of samples for each experimental condition. One
is the sample with Pd and CaO thin layers on Pd substrate (type-1). The other
is five alternate thin layers of Pd and CaO on the Pd substrate (type-2), which
has the same structure as that used in the permeation experiment by Iwamura
et al.2 These types 1 and 2 samples were used for the glow discharge experiment
and the corona discharge experiment, respectively. The sample was prepared in the
following procedure. The Pd foil (12.5 x 12.5 x 0.1mm 3 ) was washed with acetone
and aqua regia. For type-1 sample, 10 nm CaO and 40 nm Pd layers were formed
on the Pd foil by Ar ion beam sputtering. For type-2 sample, 2 nm CaO and 20 nm
Pd layers formed alternately on Pd substrate by sputtering, and there are five sets
of layers. The fifth, most surface, Pd layer was made thicker, it was 40 nm. On
sputtering, the thickness of CaO and Pd layers was adjusted by sputtering time.
After making thin layers, Cs was deposited onto the sample by electrolysis. In the
electrolysis, the plastic cell was used and the sample was set as cathode and the
anode was platinum foil. The electrolyte was a few mM CS2CO3. The applied
voltage was 1V and the electrolysis time was several 10 s.
After sample preparation, it was placed in the discharge cell as the cathode.
The discharge cell is shown in Fig. 1. The cell made of Pyrex glass has a spherical
shape with a volume of ~ 1500cm 3 . The thickness of the glass is 5 mm. The cell
is connected to a vacuum system through the port so that we can drive out the
gaseous impurities in the cell and control the pressure inside the vessel. Au foil
(0.1mm in thickness) or Pd needle (0.2 mm in diameter) was used as anode. The
former was used for glow discharge experiment, and the latter was used for corona
discharge.
Under the discharge, it is possible that the elements on the cathode surface are
diffused by sputtering, so that small amount of elements produced by the nuclear
190
Valve
reactions (if it happens) can be flown away. In order to detect such elements,
a high-pure Au foil (5 x 10 x 0.1 mm 3 ) was placed 2 cm away from the cathode. One
of the surfaces of each foil faced to the cathode to receive the elements sputtered.
The Au foil is called "Au side-foil" hereafter.
After the discharge, the cathode sample was taken out from the cell and the
elemental composition was analyzed by the inductively coupled plasma mass spec-
trometry (ICP-MS) and atomic emission spectrometry (ICP-AES). These are used
for measuring Cs and Pr density and also detected the elements contained as well.
The sensitivity of ICP-MS is so high that it can detect the element with density
above 0.1 ppb. The ICP-AES is less sensitive and it was mainly used for checking
the elements detected by ICP-MS in qualitative analysis. In pre-processing ICP-
MS and ICP-AES, the multi-layered cathode sample was immersed in 1 cm 3 of ultra
pure nitric acid for 30 s, and the elements on/in the sample were dissolved in it.
Then it was diluted by adding pure water to be totally 50 cm 3 . This sample solution
was analyzed by ICP-MS and ICP-AES. We evaluated the quantity of each element
by the density of the elements measured in this solution
In addition, the surface composition of Au side-foil was analyzed by time-of-
flight secondary ion mass spectroscopy (TOF-SIMS). In this analysis, we checked
Pr signal and any other elements detected by ICP-MS and ICP-AES. TOF-SIMS
is capable of analyzing all the elements including their isotopes, then, we surveyed
over all elements and investigated the anomaly in the isotopic abundance. Also,
we analyzed the reference sample which was prepared by the same process as the
191
standard sample was but not exposed to the discharge. Comparing the elemental
composition of those two samples, we specified the candidates of products by nuclear
reaction.
For testing the effect by laser irradiation, we utilized semiconductor laser (690 nm
in wave length and ~20mW in output power), and we investigated the difference
in the phenomena for runs with or without laser irradiation. Table 1 shows the
summary of run conditions. Four types of conditions were tested in this study. The
run Nos. 1 and 2 were for glow discharge condition, and run Nos. 3 and 4 were for
corona discharge condition.
Run No. Cathode Anode D2 pressure Voltage Current Time (h) Laser
We now consider the D fluence to the cathode during the discharge. In per-
meation experiment, it is thought to determine the conversion rate of Cs to Pr
transmutation, and a sufficient deuterium flux is an important factor to obtain a
significant yield. Here, we assume that the current is determined mainly by D ions
and the discharge area on the sample is ~ 1 cm 2 , about 1022 D ions are irradiated to
the cathode during the discharge. From the results of the permeation experiment,
Iwamura et al. have estimated the cross-section of transmutation of Cs to Pr and
its conversion rate assuming the deuterium flux permeation through the sample
being equivalent to deuterium beam irradiation. 6 They found that the conversion
rate is proportional to average flow rate and they obtained ~0.3 for irradiating
^ 3 x 10 23 deuterium atoms. Considering our experimental conditions (Table 1),
roughly speaking, the fluence estimated in our case is comparable value which gives
~10% conversion rate of Cs to Pr in permeation experiment. By ICP-MS analysis
for the reference sample, the Cs concentration on the sample was measured to be
10-100 ppb (it cannot controlled uniformly in the current method and varied run
by run), then we may expect the Pr density in the same analysis 1-10ppb.
initial density of the Cs on the sample and the conversion rate estimated from the
D fluence.
Table 2. Cs and Pr density analyzed by ICP-MS
T a b l e 3 . C o r r e s p o n d i n g e l e m e n t s for t h e signals d e t e c t e d b y I C P - M S or
ICP-AES
Corresponding element
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Mass
Figure 3. Mass spectrum measured by TOF-SIMS for Au side-foil used in corona discharge
experiment.
anomaly in abundance for some isotopes, the signal with large mass number can be
affected by the fragmentation of molecular ions. Therefore, we should still consider
the possibility of miss-identified and miss-counted of the signal corresponding. We
cannot give a conclusion only with the current information, and further study is
necessary.
4. Summary
We performed the discharge experiment under two different types of condition, i.e.
the glow discharge and the corona discharge, with multi-layered Pd/CaO cathode
to investigate the nuclear transmutation. Depositing Cs to the multi-layered cath-
ode, we tried to induce transmutation of Cs to Pr just as observing in permeation
experiment, but we did not see the evidence of Pr production with some analysis
methods. Some problems in the experimental conditions still remain, and those
should be solved in the next step.
The possibility of production of some elements was shown in the corona dis-
charge experiment. Further study to identify such candidates correctly by various
methods, are necessary. Irradiating the laser to the deuterated metal is interest-
ing idea in terms of improving the efficiency for the low-energy nuclear reaction
in condensed matter. We made the first trial to investigate the effect irradiating
the semiconductor laser to the cathode sample in the discharge experiment, and we
could not obtain any symptom showing the effect in this study.
195
References
1. S. Narita et al, Proc. JCF5 (2004) pp. 14-18.
2. Y. Iwamura, M. Sakano, and T. Itoh, Jpn. J. Appl. Phys. 4 1 , 4642-4650 (2002).
3. Y. Iwamura, T. Itoh, M. Sakano, S. Kuribayashi, Y. Terada, T. Ishikawa, and J. Kasagi,
Proc. ICCF11 (Marseilles, France, 2004).
4. D. Letts, Proc. ICCF10 (Cambridge, USA, 2003).
5. V. Violante, Proc. ICCF11 (Marseilles, France, 2004).
6. Y. Iwamura et al, Proc JCF5 (2004) pp. 60-64.
P R O D U C I N G T R A N S M U T A T I O N E L E M E N T ON
MULTI-LAYERED Pd SAMPLE B Y D E U T E R I U M P E R M E A T I O N
H. Y A M A D A , S. N A R I T A , S. T A N I G U C H I , T . U S H I R O Z A W A , S. K U R I H A R A ,
M. H I G A S H I Z A W A , H. SAWADA A N D M. I T A G A K I
Department of Electrical and Electric Engineering, Iwate University, Ueda 4-3-5,
Morioka 020-8551, Japan
E-mail: yamadahi@iwate-u. ac.jp
T. ODASHIMA
Department of Chemical Engineering, Ichinoseki National College of Technology, Hagiso,
Takanashi, Ichinoseki 021-8511, Japan
1. Introduction
The phenomena on nuclear reactions at low temperature in solid-state have been
widely investigated for these 17years. Among several experimental methods for the
reaction, the gas permeation method is one of the promising methods. Iwamura
et al.1 have studied using this method with Pd film complexes, which consist of Pd
layers, CaO layers and a bulk Pd. They have reported a low-energy nuclear reaction
such as the transmutation of Cs into Pr in deuterium permeation experiment and
have recently found a certain rule of nuclear transmutation, that is, 8 mass number
and 4 atomic number increase in the process. The phenomenon has been observed
with good reproducibility.
While, we have been taking account of the possibility of nuclear transmutation
not only in such Pd film complexes but also in plain Pd foil by hydrogen gas per-
meation at room temperature. We have performed an elemental analysis on the
Pd foil and have reported increases in count intensity of several elements includ-
ing Ag after hydrogen permeation. 2 The count intensity of Fe has been sometimes
observed to increase significantly after the permeation of highly pressurized hydro-
gen gas through Pd samples of 0.1 and 0.3 mm thickness. This result would show a
pressure effect on the reaction of transmutation. Furthermore, the isotopic compo-
sition of Ti and Cr has been observed to differ from the natural isotopic abundance
of those elements. These results have suggested that several elements were produced
196
197
by a nuclear transmutation and that the reaction could occur in hydrogen system
as some researchers have claimed in various experiments. 3-5
The aforementioned results suggest that there is a key to understand the reac-
tion in terms of the mobility of proton or deuteron in Pd lattice. These reports
caused us to study the phenomena systematically by the permeation experiment
for deuterium as well as hydrogen using multi-layered Pd samples. Thus, in this
present investigation, we have performed a deuterium permeation experiment using
Pd samples6 including a multi-layered sample consisting of single couple of CaO
and Pd thin films and a bulk Pd foil.
On the basis of the reports on transmutation of 133 Cs into 141 Pr, production of
elements with mass number ranging between 133 and 141 could be expected before
Pr production. Therefore, we have focused our attention to this mass number range
to search for the producing elements as a result of low-energy nuclear reaction. The
amount of newly producing elements in this range would be so little; it is desirable
to employ an instrument having a good sensitivity for a very small quantity of the
elements on the sample with high resolution in mass number. Consequently, we have
performed the element analysis using time-of-flight secondary ion mass spectroscopy
(TOF-SIMS).
2. Experimental
A base Pd foil (99.95% pure) of 0.1 x 12.5 x 12.5mm 3 in size was rinsed with acetone
and pure water, and then washed by aqua regia to remove impurities on the Pd foil
surface. Next, the Pd was annealed at 900°C for 8h, followed by being cooled to
room temperature in furnace and washed again with aqua regia. Using the base
Pd foil, we prepared three types of samples. The first one was a plain Pd sample
just as the base Pd foil was. It had no deposition of any additional elements. The
second one had small amount of Cs deposited on the base Pd foil. The last one
had small amount of Cs on the uppermost of multi-layered Pd sample. The multi-
layered sample consisted of a couple of CaO and Pd thin films on the base Pd foil.
The CaO and Pd thin films were formed on the Pd foil by Ar ion beam sputtering
under the input energy of 30 W for 5min and 20 W for 1 min, respectively. After
forming the thin films, small amount of Cs was deposited on the multi-layered Pd
sample by an electrochemical method. In this method, the Cs was deposited by
applying an electric field to 0.5mM CS2CO3 solution; a I V negative voltage was
applied to the multi-layered Pd sample for 10 s. A Pt foil of 10 x 10 mm 2 in size
was utilized as a counter-electrode. The thickness of CaO and Pd films formed
were 2 and 40 nm, respectively. No deuterium gas was loaded to the samples before
deuterium permeation experiment.
Figure 1 shows the deuterium permeation system to investigate the transmuta-
tion of Cs into other elements of lager mass number. Whole the permeation system
was constructed at Ulvac Techno, Ltd. in Japan. The surface inside of chamber
was finished by electro polishing method to reduce amount of impurity molecules
deposited on the surface as low as possible. A stainless steel sample holder for
198
N 2 gas
/T^ZHX}
the deuterium permeation system is shown in Fig. 2. The vacuum chamber and
the sample holder were baked at 200°C sufficiently before setting the sample. The
chamber is usually filled with N2 gas under non-experiment condition.
Just before the permeation experiment, the Pd samples were set into the sample
holder in an air environment and it was placed at the vacuum chamber. Then,
the chamber was filled with deuterium gas at a pressure 0.1 MPa; the thin Pd
film side of multi-layered Pd sample was exposed to D2 gas. The other side of
D 2 gas
Sample
Sample holder
O ring
sample was evacuated by a turbo molecular pump to prevent the Pd sample being
contaminated from the atmosphere. The deuterium permeated from the chamber
through the Pd sample to the evacuated side by the pressure gradient for about
1 month. A heater was employed to keep the temperature of the chamber at 70°C
during the experiment. After the permeation experiment, the heater is turned
off and the chamber was filled with N2 gas, then the sample ("after permeation
sample") was taken out from the holder. Before the element analysis, the sample
was not treated for purging the deuteron atoms remaining in. The sample surface
of gas-filled side was analyzed by TOF-SIMS (ULVAC-PHI: TFS-2100).
TOF-SIMS has a good sensitivity for a very small quantity of the elements on
the sample with high resolution in mass number although it is difficult to deduce the
absolute quantities from its output data alone. The primary ion in TOF-SIMS was
Ga + and we measured three randomly selected areas of 40 x 40/xm2. The spectra,
given in this paper, were obtained after sputter cleaning of upper most surfaces of
samples by the G a + for 10 s. In order to take into account the contamination from
the environment, we prepared the control sample ("control sample") without flowing
the deuterium gas, which was prepared by the same procedure for the permeation
samples. Comparing the composition of the elements on the surface of "Control
sample" with that of "after permeation sample", or comparing that of plain Pd
sample with that of multi-layered Pd sample, we tried to specify newly produced
elements during the deuterium permeation.
133 C S _ _ _ _ _ ; _ _ _ _ _ _ ,
4
i /S
•f ["*" " " . " . . I ' d — Pd foil: 0.1mm
i 12.5 x 12.5mm
-£ 400 4
o
O 300
I
200 S 69Ga2
i 1
100
O O O O O O O O O O O O O O O O O O O
o i f i o i / i O L o o L n o m o m o L n o m o i f i o
( N w c ^ c o ^ - ^ i r i L r i t D c d f ^ r ^ o d c d c r i a i o d ' r ^
Mass
Figure 3. TOF-SIMS spectrum of mass number range 132-141 without deuterium permeation
for Cs deposited on plain P d foil.
200
25000
J3
Cs
*. 15000 Cs
c j i^ Pd film-. 40nm
o ^ f — C a O film: 2nm
O -Pd foil: 0.1mm
12.5 x 12.5mm
5000
Mass
Figure 4. TOF-SIMS spectrum of mass number range 132-141 without deuterium permeation
for Cs deposited on multi-layered Pd sample.
J
count, except Cs and Ga2 was seen in this spectrum for this control
sample. A TOF-SIMS spectrum of mass number range 132-141 without deu-
terium permeation for Cs deposited on the multi-layered Pd sample is shown
in Fig. 4. The sample was used for another control one and the schematic
view of sample is shown in this figure. No marked count was again observed,
even though only a few count due to a molecule contaminant at mass number
136 was detected. A TOF-SIMS spectrum of mass number range 132-141 after
deuterium permeation at 70°C for the plain Pd foil is shown in Fig. 5, where no
500
69
Ga 2
450
400
350
c 300
o 250
o
200
• P d f o i l : 0.1mm
150 12.5 x 12.5mm
100
50
£
Mass
Figure 5. TOF-SIMS spectrum of mass number range 132-141 after deuterium permeation at
70°C for plain Pd foil.
201
8000
133CS
7000
6000
Cs
Pd foil: 0.1mm
12.5 x 12.5mm
4000
Mass
Figure 6. TOF-SIMS spectrum of mass number range 132-141 after deuterium permeation at
70°C for Cs deposited on plain Pd foil.
marked count except 69Ga2 was detected in this mass number range. A TOF-SIMS
spectrum of mass number range 132-141 after deuterium permeation at 70°C for
Cs deposited on plain Pd foil is shown in Fig. 6. Three peaks at mass number 133,
136, and 138 can be seen in the spectra; these count peaks correspond to Cs, a
molecule and Ga2, respectively.
TOF-SIMS spectra of the multi-layered sample with small amount of Cs after
deuterium permeation at 70°C are shown in Figs. 7-11. Figure 7 shows a spectrum
60000
133CS
ar-
cs
^ 40000 / Pd film: 40nm
c Cao film: 2nm
^ Pd foil: 0.1mm
O 12.5 x 12.5mm
O 30000
20000
10000
070-
o
050
060
CO CO CO CO CO 00 Ol o
CVJ CM CO CO CO CO CO CO CO CO
CO CO CO CO CO CO CO CO CO CO
Mass
Figure 7. TOF-SIMS spectrum around mass number 133 after deuterium permeation at 70°C
for Cs deposited on multi-layered Pd sample.
202
100
80
OR
60
/ . . . . . ^ P d f i l m : 40nm
3 1 + — CaO film: 2nm
o 12.5 x 12.5mm
O
40
20
00 CO CO 00
CO CO CO CO
CO CO CO CO CO CO CO CO CO CO CO
Mass
Figure 8. TOF-SIMS spectrum around mass number 134 after deuterium permeation at 70°C
for Cs deposited on multi-layered Pd sample.
around mass number 133, where only the counts corresponding to Cs is seen at
mass number 133. Figures 8 and 9 show spectra around mass number 134 and 141,
respectively. No marked count was observed in both the spectra. It was not likely
that the element 1 4 1 Pr was produced using the multi-layered sample prepared. How-
ever, one can recognize a small peak at mass number 141; which may imply a very
small amount of Pr production.
To the contrary, we have found anomalous peaks at mass number 135 and 137,
as shown in Figs. 10 and 11, respectively. The substance, corresponding to mass
100
80
•** Ajj»
Mass
Figure 9. TOF-SIMS spectrum around mass number 141 after deuterium permeation at 70° C
for Cs deposited on multi-layered Pd sample.
203
Mass
Figure 10. TOF-SIMS spectrum around mass number 135 after deuterium permeation at 70°C
for Cs deposited on multi-layered Pd sample.
CO O) O T- CJ
o o o o o o o o o o o o o o o o
o o o
in in in in in ID C D < D C O CD cd (b to to to r ^ h ^ r ^ t ^ N LO 00 CM
CO CO CO
n n m n n n cororo m co m en m co cococococo C3 C3 CO CO CO
Mass
Figure 11. TOF-SIMS spectrum around mass number 137 after deuterium permeation at 70° C
for Cs deposited on multi-layered Pd sample.
204
might be formed during the experiment, cannot account for these anomalous counts
at mass number 135 and 137. Because no peak appeared at mass numbers 134
and 138 even though Pd has large national isotopic ratios in mass number 105, 106,
and 108.
The candidate elements and molecules detected by TOF-SIMS in mass number
range 133-141 are compiled into Table 1. Most of all the sections are blank. This
means almost no count was detected at each mass number. Since no substance
with mass number 137 was registered in a control multi-layered Pd sample and in a
plain Pd sample with Cs after the permeation, the process of forming multi-layered
sample and of depositing Cs seemed to present almost no amount of contaminant
of mass number 137 to these samples. Thus, the substance with mass number 137
observed after deuterium permeation is unlikely to be contaminant but would be
an element such as 137 La or 137 Ba. The results suggest an impotent role of alpha
cluster in the transmutation process of 8 and 12 mass number increasing.
Table 1. Candidate elements and molecules detected by TOF-SIMS at mass number range
133-141; blank means almost no count being observed
133 Cs Cs Cs Cs
134
135 Ba CsD
136 Molecule Molecule Molecule
137 Ba La
138
141
4. Conclusion
Elements analysis on the Pd samples was performed after deuterium permeation ex-
periment and for control Pd samples using TOF-SIMS. The TOF-SIMS has provided
the marked count peaks at mass numbers 135 and 137 in spectra after deuterium
permeation at 70° C, only when the multi-layered Pd sample with a small amount
of Cs was used. The substance with mass number 137 could be 137 La or 137 Ba
produced during deuterium permeation by some nuclear transmutation occurring
on/in the uppermost of multi-layered Pd sample. The single couple of Pd/CaO
thin films on Pd foil might contribute to induce production of an element with
mass number 137. This would imply a transmutation of 4 mass number increasing
before 1 4 1 Pr production.
References
1. Y. Iwamura, T. Itoh, and M. Sakano, Jpn. J. Appl. Phys. 41, 4642 (2002).
2. H. Yamada, S. Narita, H. Onodera, H. Suzuki, N. Tanaka, T. Nyui, and T. Ushirozawa,
Proc. 5th Meeting of Japan CF Research Society (2004), p. 69.
205
V L A D I M I R I. V Y S O T S K I I
Kiev National Shevchenko University, Vladimirskaya St. 64, 01033 Kiev, Ukraine
E-mail: viv@vhome.kiev.ua
A L L A A. K O R N I L O V A
Moscow State University, 119899 Moscow, Russia
A L E X A N D R B. TASHIREV
Kiev Institute of Microbiology, Kiev, Ukraine
JULIA KORNILOVA
Scientific Center of System Investigation and Technologies, Moscow, Russia
1. I n t r o d u c t i o n a n d G e n e r a l Consideration
Several years ago, we have studied and reported the process of transmutation of
stable isotopes in growing "one-line" (one type, "clean") microbiological cultures
like Escherichia coli or Deinicocus Radiodurans.1
It was shown that the transmutation process during the growth of such microbi-
ological cultures had taken place but its effectiveness had been low and had equaled
A « 1 0 _ 8 s _ 1 in the case of the reaction with light isotope Mn 55 + d2 = Fe 57 and
A « 10~ 10 s _ 1 in the reaction with middle range mass isotopes Na 23 + P 3 1 = Fe 54 .
The typical Mossbauer spectrum of "one-line" culture Saccharomyces cerevisiae
T-8 grown in D2O with the presence of Mn 55 isotope 1 is presented in Fig. 1.
The low amplitude of Mossbauer resonance (A J / J « 0.2%) in these experiments
was the result of low absolute and relative concentration of created Fe 57 isotope in
the culture.
206
207
Velocity, mm/s
Figure 1. Mossbauer spectra of grown cultures in different identical flasks. Culture Saccha-
romyces cerevisiae T-8 grown in D2O with presence of M n 5 5 isotope. 1
Figure 2. Symbolic scheme of different types of intraspecific and interspecific connections between
arbitrary selected culture and different cultures in the volume of syntrophin association. The same
connections are related to each culture.
Directions of symbiosis
and synergism to optimal
cultures from all members
of association V?'"-IfHtllllHiiilHffrtBiUm
• Metabolic shift at L
(b)
Initial chemical
composition and
i \ \ One-line culture, slowed growth
biochemical
properties of >
nutrient media at fn ,'\ / One-line culture, maximal growth
(the optimal
conditions in
brightly area)
Figure 3. Change the directions of symbiosis and synergism in microbiological association (case a)
to optimal growing cultures at change of chemistry composition and biochemical properties of
nutrient media and environment. Change of type of optimal cultures is the result of metabolic
shift of chemical composition and biochemical properties of nutrient media. The case b presents
the process of growth impairment in "one-line" culture at metabolic shift.
Figure 4. Mossbauer specter of microbiological MCT grown in the volume with presence of H2O
and Mn 5 5 isotope (control): A J m a x / J f» 1.1% is the magnitude of Mossbauer resonance.
211
Absorption, %
1"
2-
3-
; 3.4%
4-
H • r ' 1 ' 1 ' 1 • r 1 1 1 1 1
- 4 - 3 - 2 - 1 0 1 2 3 4
v (mm/s)
Figure 5. Mossbauer specter of microbiological MCT grown in the volume with presence of
D2O and Mn 5 5 isotope (experiments on transmutation): A J m a x / J ~ 3.4% is the magnitude
of Mossbauer resonance.
X/Fe 56 (relative
(a) X/Fe 56 (relative
concentration of isotopes) concentration of isotopes)
1 •
• •
• 0.15
0.15
0.1 0.1 1
0.05
1
Iki "1"' t
0.0
3. Conclusions
References
1. V.I Vysotskii and A.A. Kornilova, Nuclear Fusion and Transmutation of Isotopes in
Biological Systems. MIR Publishing House, Moscow (2003).
2. V.I.Vysotskii, A. Odintsov, V.N. Pavlovich, A.B.Tashirev, and A.A.Kornilova, Exper-
iments on controlled decontamination of water mixture of long-lived active isotopes in
biological cells. Proc. IGCF-11, Marseilles, France, pp. 530-536 (2004).
R E S E A R C H INTO LOW-ENERGY N U C L E A R REACTIONS IN
CATHODE SAMPLE SOLID W I T H P R O D U C T I O N OF EXCESS
HEAT, STABLE A N D R A D I O A C T I V E I M P U R I T Y NUCLIDES
A.B. K A R A B U T
FSUE "LUCH" 24 Zheleznodorozhnaya St, Podolsk, Moscow Region U2100, Russia
E-mail: karab.ab@g23.relcom.ru
1. Introduction
Measurements of the excess heat, isotopic impurities, heavy particles emission, and
soft X-ray emission in high-current density glow discharge have been carried out
for years. Further experimental evidence is required to elaborate a reliable theory
explaining the phenomena under discussion. The present research is focused on this
problem.
214
215
Figure 1. Experimental glow discharge device (flow continuous calorimeter). (1) vacuum dis-
charge chamber, (2) cathode holder unit, (3) cathode sample, (4) anode unit, (5) input and output
of water cooling system, (6) out channel of X-ray emission, (7) 15 fim Be shield, (8) X-ray detector
of the different kinds, (9) heat insulation cover, and (10) windows in heat insulation cover.
channel incorporated thermal sensor (at the input and output) connected differ-
entially and a water flow meter. The device was placed into a thermal insulation
package, comprising the flow calorimeter.
The pulse-periodic electric power supply was used. The thermal (signals from
thermal sensor and the flow-meter) and the electric parameters (the GD current
and voltage) were recorded using a data acquisition board. The values obtained
were processed by a computer. The excess heat power PEH value was determined
by
PEH = (PHC + ^HA + Pnch) - Pei ± AP e r r o r ,
where Pei is the GD input electric power; PHC, -PHA; and PHCh represent the output
heat power carried away by the cooling water from the cathode, anode and chamber,
respectively; AP e r r o r stands for the systematic error of the power measurement for
the given measuring system. Calibration of the measurement system was carried
out in the following way: a water-cooled electric resistive heater wrapped into an
insulating package was placed among the thermistors inside each thermal power
measuring channel. The amount of the consumed cooling water corresponded to
that inside the GDD. The resistive heater was powered by a pulse-periodic power
supply. The heater electric parameters were identical to those of the GD. The
measured heat power of the resistive heater was equated to the heater measured
electric power. The calibration relationship was estimated at different values of the
input electric power.
216
The Pd samples used in tests with Xe and Kr GD were not deuterium pre-
charged. The measurement system allowed to record the GD input electric power
and the thermal power output by the cooling water with accuracy of 0.6 W at the
absolute value of the electrical power up to 120 W (relative error ±0.5%).
In this set of the experiments the current density did not exceed 100 mA/cm 2 .
At such values of the discharge current in D 2 , a continuous loading of D 2 into Pd ran
up to saturation. The experiments were carried out with Pd cathode samples in D 2
GD, and with deuterium pre-charged Pd cathode samples in Xe and Kr discharges.
The amount of the loaded D 2 was estimated by the pressure drop in the chamber.
D 2 was periodically supplied into the chamber to maintain the required pressure.
The amount of deuterium loaded into palladium was determined by the volume of
the gas absorbed from the discharge chamber. When saturation was achieved, the
value of the D/Pd ratio was close to 1.
t(W)
8
7 #-PdD-D
6 ©-PdD-Xe
B-PdD- Kr
5
4
3
2
1
i i i J I L J I
0 2 4 6 8 10 12 14 16 p l m
' e l . input l v v >
Figure 2. Excess heat power in relation to the input electric power. Pd cathode sample, d = 9 mm;
Deuterium pre-charged Pd cathode samples in Xe and Kr discharges. (1) Optimal (1100-1300 V)
Glow Discharge voltage and (2) not optimal glow discharge voltage.
Heat measurements were carried out for Pd cathode samples in GD while chang-
ing the following parameters: GD current density, voltage, duration of current
pulses, and the time between current pulses (from the power supply). The absolute
value of the excess heat power and thermal efficiency grew with increasing the power
input into the discharge (Fig. 2). Relatively high values of the excess heat power
and thermal efficiency were achieved for deuterium pre-charged cathode samples in
Xe and Kr discharges. No excess heat power production was observed in the cath-
ode samples made of pure Pd (not deuterium pre-charged) in Xe and Kr discharges
(Fig. 3, curve 3).
Two typical groups of the results can be noted: relatively large values of the
excess heat power and efficiency coefficient (curve 1) and the group the results with
lower values of the excess heat power and efficiency coefficient (curve 2). The large
217
100
90 J I I I I I I I L
0 2 4 6 8 10 12 14 16
el.input (W)
Figure 3. Dependence of the output heat power to the input electric power ratio of the input
electric power. (1, 2) Deuterium pre-charged Pd cathode samples in D2, Xe, and Kr discharges,
d = 9 mm. (1) optimal (1100-1300 V) glow discharge voltage, and (2) not optimal glow discharge
voltage, and (3) non-deuterium-charged Pd cathode.
values of the excess heat power and efficiency coefficient were observed under the
modes when the GD operational voltage ranging 1000-1300 V (Fig. 5).
The three-channel system of separate measurements of the output excess heat
power (for the anode, cathode, and chamber) allowed to define the structure of
the excess heat power output in the GD. Large efficiency values were achieved in
experiments with high relative heat release on the cathode. This data prove that
the excess heat power was produced mainly on the cathode (Fig. 4).
Thus, it was experimentally shown that the excess heat power production was
determined by two processes: (1) deuterium should be loaded into the medium of
,(W)
•*-PdD-D
©PdD-Xe
E-PdD-Kr
• - Pd-Kr
I I I I I
0 10 12 14 16
Pe,,npu,(W)
Figure 4. Dependence of the cathode output heat power of the input electric power. (1) Deu-
terium pre-charged Pd cathode samples in D2, Xe and Kr discharges, d = 9mm, optimal (1100-
1300 V) Glow Discharge voltage, (2) Non-deuterium-charged Pd cathode, in Kr discharge.
218
1
"heat out' °el.input \'°) «-PdD-D
170 o-PdD-Xe
160 H-PdD-Kr
150
140
130
120
110
100 .1 I I I I I I I I L
0.8 1.0 1.2 1.4 1.6
Ue, (keV)
Figure 5. Dependence of the output heat power and the input electric power ratio of the GD
voltage. Deuterium pre-charged Pd cathode samples in D2, Xe, and Kr discharges.
the solid crystal lattice and (2) the crystal lattice should get initial excitation, so
that high-energy long-lived excited levels were created in the cathode solid. These
excited conditions could be created by an additional source (e.g., by a flow of inert
gas ions).
Table 2. The content of produced impurity nuclides in the cathode sample after Glow Dis-
charge experiment. The cathode-plasma forming gaze forming system is Pd-D2; current:
35 mA; time of the experiment: 4 h. Analysis made by X-ray fluorescent spectrometry method.
Impurity element Na Mg Al Ca Si Ti Br Sr Y Mo Tc
Content (%) 0.07 0.01 0.04 0.04 0.015 0.01 0.03 0.07 0.4 0.15 0.2
The following methods were used: secondary ionic mass spectrometry (for Pd
samples), and secondary neutral mass spectrometry (for V, Nb, and Ta samples).
These techniques were used to analyze the impurity content in the cathode samples
material before, and after, the experiment. The Pd cathode samples were analyzed
for impurities after their exposure to D2 discharge. The cathode samples made of
mono-isotopic metals (V, Nb, and Ta) were studied after the exposure to D2 and
H2 at the same GD operational regimes.
The difference in the content of the impurity elements before, and after, the
experiment was defined as storage of the elements during the experiment. The
procedure for determining the impurities by the method of the secondary ion mass
spectrometry included the following stages: (a) removal the upper 1.5-nm-thick de-
fect layer by plasma etching, (b) scanning the first and the second layers in 5 nm
increments, while determining the content of the impurity nuclides, and (c) removal
of a layer with the thickness of 700 nm and repeated scanning of the third and
fourth layers in 5 nm increments while again determining the content of the impu-
rity nuclides (Fig. 6). The maximum quantity of impurity nuclides was registered
in Pd samples after exposure to D2 discharge. Elemental impurities with masses
approximately half the Pd mass or close to Pd mass were recorded in the 100 nm
thick near-surface layer in amount up to some tens percents.
The main impurity elements (isotopes) with more than 1% content included:
7
Li, 1 2 C, 15 N, 20 Ne, 29 Si, 44 Ca, 48 Ca, 56 Fe, 57 Fe, 59 Co, 64 Zn, 66 Zn, 75 As, 107 Ag,
109
Ag, 110 Cg, m C g , 112 Cg, 114 Cg, and 115 In (Table 3). The impurity content in
the cathode sample volume was defined at different depths.
800 nm
Figure 6. Registration procedure for the impurity contents in the cathode samples (methods
SIMS and SNMS). 1-dirty superficial layer, 2, 3-analyzed layers 1, 2 scans, 4-surface of the cathode
samples, 5-removal of a metal layer, 6, 7- analyzed layers, 3, 4 scans.
220
Table 3. The impurity nuclides content in the cathode sample surface layer after Glow Discharge
experiment. The cathode-plasma forming gaze system is Pd-D2; current: 100 mA; time of the
experiment: 22 h. Analysis made by SIMS method.
Table 4. The impurity nuclides content in the cathode sample surface layer after Glow Discharge
experiment. The cathode-plasma forming gaze systems are V-H2 and V-D2; current: 100 mA; time
of the experiment: 4h. Analysis made by SIMS method.
V-H V-D
Table 5. The impurity nuclides content in the cathode sample surface layer after Glow Discharge
experiment. The cathode-plasma forming gaze systems are Nb-H2 and Nb-D2; current: 100mA;
time of the experiment: 4h. Analysis made by SIMS method.
Nb-H Nb-D
(including rare-earth nuclides) was registered for Ta. After exposure to H2 and
D2 discharge these metals showed great variety (in form and quantity) of impurity
nuclides. This may suggest nuclear origin of the phenomenon in question, since
the chemical, and thermo-physical characteristics of H2 and D2 are practically the
same. Alongside with formation of impurity nuclides with V, Nb, and Ta cathode
Table 6. The impurity nuclides content in the cathode sample surface layer after Glow Discharge
experiment. The cathode-plasma forming gaze systems are Ta-H2 and Ta-D2j current: 100 mA;
time of the experiment: 4h. Analysis made by SIMS method.
Ta-H Ta-D
samples, considerable reduction (by tens of times) in the content of some light
elemental impurities (which had been present in the samples before the experiment)
was observed.
4. Gamma-emission Registration
Weak gamma emission was registered in certain experimental conditions (specific
geometry of the discharge chamber, cathode, and anode). The gamma emission was
recorded over the whole volume of the discharge chamber. The gamma-emission
registration was carried out using HPGe detectors and a multi-channel spectrum
analyzer. The detector with the glow discharge device with the detector was placed
into the shield made of lead with thickness of 10 mm.
Gamma-emission ranging 0.1-3.0 MeV was observed during the GD operation
and within 8 days after the discharge current switch off. In the course of long
intervals between the experiments (up to some months) the repeated measurement
of the background spectra was also carried out. The value of gamma - emission
was determined taking into account the geometrical and physical efficiency of the
detector and the registered background value. The value of gamma background
fluctuation did not exceed 10% during the experiment (5 months).
2 3 p _ ^ 23 Ne -> 23 Na
2 4 p _ ,2i Ne ->24 Na - 24 Mg
3 9 g _ > CI -+ 39 Ar
39
59
Cr -V^Mn - 5 9 Fe --. 5 9 Co
67
Ni- ^ 7 Cu --+ 67 Zn
69
Ni- -^69 Cu --^69 Zn -^69 G a ^ 6 9 G e
73
Zn -^ 73 Ga - 7 3 G e
81
Ga ^ 8 1 G e ^ 8 1 As --.81 g e ^ 8 1 B r
83
Ge ^ 8 3 As -- 8 3 Se -^83 B r ^ 8 3 K r
84
As- - 8 4 Se -^ 8 4 Br -H• 8 4 K r
87
As- - 8 7 Se --+87 Br -,87 fo ^ 8 7 R b
9 3 B r .- 9 3 Kr -^ 9 3 Rb -^93 g r ^ 9 3 Y ^ 9 3 &
94
Kr ^ 9 4 Rb ^ 9 4 Sr -4 94 Y ^ 9 4 ^ j .
99
Rb - + " Sr -_^99 y _> 99 Zr ^ " Nb - > " Mo
100y ^ 1 0 ° Zr ^ 1 0 ° Nb ^ 1 0 ° Mo
101y ^ 1 0 1 Zr -^ 1 0 1 Nb _ ^ i o i M o ^ i o i T c ^ i
105Nb ^105 M Q ^105 T(, ^105 R u ^105 R h ^105 p d
A/j
1 I I i i i
600
% • d
400 i" ! /'
'f fk
200
W L & H - T A .1. 1 -Je. -,
1
IW!^KH , &'MS ^ M *
Figure 7. Gamma emission spectrum recorded by Ge-Li detector from the GD device after, the
discharge current switch off. Pd cathode placed in D2 discharge. The part of the spectrum area
("d" - area) is presented in greater detail (see Fig. 8.).
background (a) is not a large factor a (a = 2.5-5). The value for the continuum is
a = 8-10. The gamma spectra obtained during the GD operation and after the GD
current switch off were processed with the help of a database to identify gamma lines
of radioactive nuclides.2 For each /^-transition 30 or 40 gamma lines were identified.
For a single /3-radioactive decay chain (one atomic mass of radioactive nuclides)
100-200 gamma-lines were identified.
The gamma emission spectrum registered after the GD current switch off con-
tains gamma lines of short-lived (3- radioactive chains (Figs. 7 and 8). Presumably
after the GD current switch off there appear certain conditions for initiating nu-
clear reactions. The total number of radioactive atoms was determined taking into
account the values of gamma-line areas, the value of the detector efficiency, and the
,1
Ru, 306.8 !3
Na, 440.0
'Br, 334.0 ^Rh, 374.3 101Tc, 408.7
E E aaSr, 307.0 , , , — 374.9
i9
Zn, 438.6
r
84
m,n 336 2 Br, 408.2 Cd, 481.0
2% i«Tc, 309.5, ' - 105
Rh, 407.6 'Cd, 478.7
-MO, 348.5 ' " N b , 373.9
42 107
250 Ca^312.6 Pd, 348.2 r°lNb 83
12,
ln, 313.7
I
200
150
100
50 a
Br, 345.2
105
Pd, 344.5
115
Ag, 342.7
300 400 E, (keV)51
Figure 8. Part of gamma emission spectrum indicating identified gamma-lines The duration of
the discharge operation was 10,000 s. The duration of the gamma spectrum registration was
60,000 s after the discharge current switch off. The background spectrum (60,000 s duration) was
subtracted from the operational spectrum. The lines are identified as related to excited nuclei of
beta-decay chains.
224
value of the quantum yield. The /3-radioactive chains with masses of A = 23, 24,
39, 59, 67, 69, 73, 81, 83, 84, 87, 93, 94, 99, 100, 101, 105, and 115, make the main
contribution into gamma-radiation (operating time for radioactive nuclides is up to
10 5 atoms).
Figure 9. The diagram of the X-ray image registration using the pinhole. The objective with 2.0
mm diameter closes by the 15(im Be shield. The system Pd-D2, the discharge current: 150 mA;
voltage is 1850 V; the exposure time: 10,000 s. (a) X-ray image registration without superimpo-
sition of the cross magnetic field; (b) X-ray image registration with superimposition of the cross
magnetic field 0.3 T. The image is positive. (1) anode, (2) discharge plasma area, and (3) cathode.
The evaluation of the X-ray emission was made with reference to the change
in the radiation dose absorbed by thermo-luminescent detectors covered with Be
foils of varying thickness. The experimentally determined value of the X-ray energy
increased from 1.2 to 1.5 keV when the thickness of the Be shield increased from
225
Table 7. The characteristic of X-ray emission from different cathode samples in Glow Discharge
experiment.
Material of cathode Al Sc Ti Ni Mo Pd Ta Re Pt Pb
Glow discharge voltage (V) 1650 1540 1730 1650 1420 1650 1600 1520 1650 1610
Glow discharge current (mA) 130 130 170 150 210 138 138 125 138 138
X-ray energy during passing 1.54 1.26 1.45 1.91 1.48 1.98 1.62 1.36 1.47 1.36
the discharge current, J3x—ray
(keV)
X-ray energy without current, 1.68 1.5 1.46 1.96 1.33 1.71 1.62 1.38 1.75 1.45
J^X-ray (keV)
15 to 300 /jm. X-ray emission as a function of time was studied with scintillator
detectors and photomultipliers (PM).
For different cathode materials the X-ray energy values obtained with the help
of scintillator detectors, PM and 15 and 30 /iin-thick beryllium foils amounted to
Ex-ra,y ~ 1.0-2.5 keV (Table 7), which showed good agreement with the TLD data.
The X-ray spectra were determined using the curved mica crystal X-ray spec-
trometer fixed (positioned) on an X-ray film (Fig. 10). The X-ray wave length was
evaluated by the expression: m x A = 2 x d x sin#, where A is the wave length, d
stands for the distance between crystallographic planes of the mica crystal, 2 x d =
2nm; 9 represents Bragg divergence (angle); m stands for the diffraction order.
The spectrum was registered both as bands of the continuum with energies rang-
ing 0.6-10.0 keV and as spots resulting from the emission of series of high-density
mono-energetic X-ray beams (with energies up to 0.6-10.0 keV) characterized by
small angular divergence. The energetic position within the spectrum depended
upon the cathode material used (was specific for a given cathode material) and was
similar to characteristic X-ray spectra. Of particular interest was the persistence
of the X-ray spectrum registration for several hours after turning off the GD cur-
rent. Presumably, some long-lived excited levels with energies up to several keV are
formed in the cathode solid-state medium, and after the GD current is cut off, the
excitation persists maintained by the X-ray emission. The spectrum band ranging
in energy 1.2-1.3 keV was defined for Pd cathode samples in D2 and Kr GD (during
its operation, and after, the discharge current switch off) (Fig. 10). This result is
in good agreement with the maximum value of excess heat power at 1000-1300 V
GD voltage.
6. Discussion
Experiments on anomalies in high-current glow discharge carried out for several
years allow to outline the basic processes and conditions of their occurrence.
(1) Excess heat production. Excess heat was produced in the volume of the
solid-state medium of the cathode sample under the following conditions:
• Deuterium should be loaded into the solid-state cathode medium.
226
Pd-D
^ ? # ^ r : < r : . ; r •; • Pd_Kr
„ "#., JO
y VVj- Pd-Xe
v
v * -\
20 10 5.0 4.0 3.6 " "' 20 18 16 1.4
- ^ ^Tgrggjgip
Figure 10. The outline of X-ray spectrum registration from the Pd cathode sample using the
curved mica crystal spectrometer. (a5 b, c, d) during the GD operation, the exposure time is
18,000 s. (a) during the GD operation in D2; (b, c, d) the Pd cathode samples are non deuterium-
charged, (b) GD in Ar, (c) GD in Kr, (d) GD in Xe, (e) the spectrum registered after the GD in
D2 current switch off.
A + m B ^ [AB]*,
A + A + m B ^ [2AB]*,
[AB]* - ^ F * - ^ F + Heat,
[AB]* -> C * +D* - • C + D + Heat,
where A is Pd or the nucleus of another element; B stands for deuterium
or hydrogen; [AB]* represents short-lived intermediate compound nucleus;
m = 1, 2, 3 , . . . , C*, D* are the nuclear isomers of nuclides with masses less
than that of Pd; C,D are stable nuclides, F stands for a nuclide with mass
more than that of Pd. First a composite compound-nucleus in the excited
state is formed. Then one of the two possible modes is realized:
(a) The compound-nucleus could lose its excitation and form a stable nu-
cleus, being heavier than Pd; (b) the compound nucleus could fission
into two nuclear fragments with masses less than that of Pd. In doing
so, the two nuclei should be in excited isomeric states (experiments
showed that the nuclear reactions energy was not produced as a kinetic
energy).
(6) To determine the specific physical mechanism for these reactions requires
some additional research. One possible type of reaction for forming the
impurity nuclides can be long-range (resonant) nuclear reactions.
The mechanism of such long-range reactions can be explained using as an exam-
ple a specific transmutation reaction for Pd + D (Fig. 11a) and Pd + 2D (Fig. l i b ) .
229
According to the laws of momentum and energy conservation, the formed nuclide
13
C should receive the energy of 6.8609 MeV. The nuclide 93 Nb should receive the
energy of 0.959 MeV. The nuclear excited state (nuclear isomer) with the energy of
6.864 MeV and excited level width of 6 keV exists for 1 3 C. The excited level with the
energy of 0.94983 MeV exists for 93 Nb. The difference between the energy received
by nuclide 13 C and the energy of one of the excited nucleus equals to 3.f keV. At
the excitation energy of the crystalline lattice of 1.5 keV, and width of the excited
energy level of 6.0 keV, these conditions resulted in a high probability for occurrence
of the long-range (resonant) nuclear reaction.
105
Pd + 2 2 D - • [Pd2D]* -^ 9 3 Rh + b Li + 11.794 MeV.
According to the laws of momentum and energy conservation, the formed nuclide
6
Li should receive the energy of 8.880 MeV. The nuclide 93 Nb should receive the
energy of 0.959 MeV. The nuclear excited state (nuclear isomer) with the energy of
6.864 MeV and excited level width of 6 keV exists for 1 3 C. The excited level with the
energy of 0.94983 MeV exists for 93 Nb. The difference between the energy received
by nuclide 13 C and the energy of one of the excited nucleus equals to 3.1 keV.
r^j I
ev. CD
I
3.1
>
CD
^ n
Ul
• >
CD +
5/2
O
CD
< O
CD rt
CD
686
1
'
93 13 103 6
[PdD]* Nb stable C stable [Pd2D]* Rh stable Li stable
Figure 11. Assumed plan of carrying out long-ranged (resonant) nuclear reactions, (a) for Pd
D transmutation reaction and (b) for Pd + 2D transmutation reaction.
The totality of the experimental results allows to assume that the energy of
the excited nuclear levels of the formed nuclides converts into heat. The specific
physical mechanism of such conversion requires additional research.
230
7. Conclusions
T h e results obtained (the glow discharge device producing the excess heat power up
to 5 W / c m 2 at an efficiency up to 150%) allow the development of a demonstration
source of heat power. The technology for development of multi-element cathode fuel
elements with plasma anodes has been worked out. The development of new nuclear
engineering is possible based on non-equilibrium nuclear t r a n s m u t a t i o n reactions in
the solid-state medium. This type of engineering can be called "Third way" in
nuclear engineering in comparison with the nuclear engineering based on uranium
nuclear fission, and thermonuclear synthesis.
References
1. A.B. Karabut, Ya.R. Kucherov, and I.V. Savvanimova, Nuclear product ratio for glow
discharge in deuterium, Phys. Lett. A, 170, 265, 1992.
2. Richard B. Firestone, Table of Isotopes, 8th Edition, Vols. 1 and 2, Appendix G - 1 ,
John Wiley & Sons, Inc., New York, 1996.
I N F L U E N C E OF P A R A M E T E R S OF T H E GLOW D I S C H A R G E ON
C H A N G E OF S T R U C T U R E A N D T H E ISOTOPE COMPOSITION
OF THE CATHODE MATERIALS
L B . SAVVATIMOVA A N D D.V. G A V R I T E N K O V
Federal State Unitarian Enterprise Scientific Research Institute "Luch",
Zheleznodorozhnaya, 24 Podolsk, Moscow region 142116, Russia
E-mail: Ul0492@dialup.podolsk.ru
1. Introduction
As is known, the ionic processing of materials results in changing surface properties.
It has been shown earlier that physical-mechanical properties, element, and isotope
compositions in plasma of a glow discharge change. 1_9
The majority of the "additional" elements found after ion irradiation and
not found before irradiation is distributed at the boundaries of grains 1 and in
231
232
local spots. 3 ' 4,9 They make up from the 10th fractions of a percent up to
several percents. Thus in initial samples the content of separate impurity elements
did not exceed 10~ 3 -10~ 4 at.% and EDX analysis could not reveal it. Groups of
such elements as Sc, Ti, V, Ag, Cd, In, P, CI, Br, Ge, As, Kr, Sr, Y, Ru, and Xe
have been found in Pd after irradiation by ions of all the types (D, H, Ar, and
Ar+Xe), but in various quantities. 2 Elements with atom numbers Z = 26-31 (Fe,
Cu, Zn, and Ga) were observed by the method of energy-dispersion X-ray spectral
analysis (EDX) preferentially after irradiation by deuterium ions.
As a result of EDX and radiography, it was supposed that nuclear transmu-
tations occur more intensively on local sites. 1 - 4 Distinctions in the characteristic
spectrums corresponding to various combinations confirmed the nuclear processes
in local zones. 3 ' 9 Considerable changes of the isotope relations were observed for
10
B / n B , 1 2 C/ 1 3 C, 6 0 Ni/ 6 1 Ni/ 6 2 , 4 0 Ca/ 4 4 Ca, and 9 0 Zr/ 9 1 Zr. 3 Change of the iso-
tope relation in i 09 / 107 Ag from 3/1 up to 9/1 was observed in different series of
experiments. 3 ' 9
In this paper, the changes of structure, element, and isotope composition of pal-
ladium for various parameters of the discharge are compared. The role of the current
sort in transmutation intensity is shown. The possible types of nuclear reactions
for pairs of the elements observed in the cathodes after experiments are shown.
of low-energy actions in glow discharge plasma with the participation, for example,
of hydrogen or deuterium, or processes of heavier elements fission. The increase
in the content of Zr by a factor of <~570-340 (rows 15 and 16), V by a factor of
100 (row 5), Cr by a factor of 160 (row 6), Fe by a factor of 2-4 (rows 8 and 9),
and Ni - 5-30 (rows 10 and 11) can also be a result of nuclear transmutations.
The experimental time of this series was ~30min. The increase of the impurity
elements at the backside was observed only for Li. "Dot" aggregations of Zn, Co,
Br, and Mg located preferentially on boundaries of subgrains, with a density of
~ ( 1 - I 0 ) x l 0 6 cm~ 2 (for Zn the density of such places made up ~ ( l - 2 ) xlO 6 cm" 2 ,
for B r ^ ( 2 - 4 ) x l 0 6 c m - 2 ) 1 are found during scanning the surface of a sample.
The comparison of the new elements quantity shows that an increase in experi-
mental time (fiuence) by a factor of 10 times (data EDX) leads only to an increase
in Mo which is an element of construction (the a pressure holder of the sample,
screening a part of surface during sample irradiation). Therefore, it is not surpris-
ing that irradiation time increase leads to Mo quantity increase. The quantity of
other "additional" elements (Br, Sr, and Te which are absent in the sample before
experiment) does not change largely with an increase of experimental time (a dose
of irradiation) by a factor of 10.
The reason for such an effect can be both preferred formation of these elements in
the sample at the initial stage of the discharge burning, having significant quantity of
After experiment
Before
experiment Irradiated side Back side
Thickness of the samples ~ 100 jira. Depth of analyzed layer was ~ 100 A.
Method of the analysis secondary ionic mass spectrometry.
Li, B, V, Sr, and Zr were not present at the discharge chamber earlier.
The source of possible impurity is absent.
235
different defects on its surface and possible preferable sputtering of lighter elements
at the following experimental stage. Another reason for the absence of growth of the
"additional" elements quantity with an increase in discharge burning time can be
participation of the forming elements in the secondary reactions. It is impossible to
exclude the contribution of irradiated surface screening by sputtered. However, the
analysis of the same samples by spark mass spectrometry method does not confirm
the explanation of the results obtained by the surface screening by molybdenum
precipitation because an increase of other elements such as 7 Li, n B , K, Rb, In, and
Nb in a longer experiment was observed both on irradiated and on the backside of
the same sample.
Table 2. Additional atoms on palladium surface after glow discharge in deuterium (EDX). 1
4h 40 h
backside of the sample. Similar changes are also observed for 90 Zr isotope on the
surface irradiated by palladium ions where the increase is ^500 times after 4-hour
discharges and 1200 times for 40 h. On the backside, the quantity of 90 Zr increases
by a factor of ~4.4. The quantity of 91 Zr isotope increases ~1000 and ^1200 times
with a 10-fold increase in discharge time. The 80 Se increasing was ~100 times on
Table 3. Quantity of the impurity atoms on palladium surface after deuterium ions irradiation
at glow discharge (SMS). 1
No. Mass Element Content before Additional element content in Pd for different
number ( x l 0 — 4 at. %) experiment duration ( x l O - 4 at. %)
(X100 ppm)
4h 40 h
Upper Lower Upper Lower
1 6 Li 0.06 0.15
2 7 Li 0.06 0.33 0.40 0.90 0.50
3 10 B 0.07 0.15
4 11 B 0.07 0.30 0.20 0.20 0.70
5 23 Na 0.44 4.40 1.00 2.00 6.00
6 27 Al 6.00 96.00 10.00 300.00 25.00
7 28 Si** 9.00 18.00 9.00 3.00
8 29 Si** 7.00 21.00 11.00 10.00
9 30 Si** 6.00 18.00 4.50 15.00 66.00
10 32 S 7.00 14.00 2.00 3.50 2.00
11 39 K 3.00 9.00 12.00 4.50
12 41 K 3.00 12.00 1.00 18.00 9.00
13 47 Ti* 1.20 1.80 60.00
14 48 Ti* 1.40 580.00 2.50 3.50
15 49 Ti* 1.30 680.00 3.25 130.00 2.60
16 50 Ti* 1.70 3.40 130.00
17 78 Se* 0.23 0.23 0.20 0.20 4.00
18 80 Se* 0.30 0.20 0.20 0.20 33.00
19 85 Rb* < 0.03 0.01 0.05 90.00 51.00
20 90 Zr* < 0.05 25.00 0.05 60.00 0.22
21 91 Zr* < 0.05 50.00 0.05 61.00
22 93 Nb* < 2.00 40.00 2.00 7200.00 4.00
23 98 Mo** 0.40 3.00
24 100 Mo** 1.80 4500.00 1.80 2880.00
25 103 Rh* 7.00 21.00 21.00 25.00 7.00
26 107 Ag* 1.00 63.00 3.00 1.00 3.20
27 109 Ag* 1.00 50.00 1.50 2.50
28 115 In* <0.04 0.48 0.04 0.80 0.16
backside for 40-hour experiment. Authors could not explain a significant increase
in n B , 115 In, 93 Nb, 80 Se II 91 Zr on the backside of the sample by other non-nuclear
processes.
107 109
1
Initial 0 1.7 x 10 2.2 x 10 1
3
5j) x 10 5.2 x 10 3 -2.5 x 10 2
1666 35 D2 2.1 x 10
3
2J2 x 10 3 -1.0 x 10 2
<1.5 x 10 1 < 5
1.1 x 10 2 7.7 x 10 1 -4.0
1667** 35 <2.0 x 10 1 <2.0 x 10 1
<2.0 x 10 1 <2.0 x 10 1
5/7x 10 2 5Ji x 10 2 -2.5 x 10 1
1668 25 H2D2 M x 10 2
2
7 4 x 10 2 - 3.5 x 10 1
1.2 x 10 1.3 x 10 2 - 5.0
2
l O x 10 3 - 5.0 x 10 1
1670 25 H2 9/7 x 102
10 4.5 x 10 2 -2.0 x 10 1
4.5 x
10 3 2 7 x 10 3 -1.2 x 10 2
1671 25 D2 2.6 x 2
10 1.9 x 10 2 -9.0
1.8 x
*1, 2, 3 depth of analyzed layer is 10 /jm: (1, 2) the upper irradiated sample; (3) unirradiated
lower sample.
**1668 - discharge in hydrogen, and then in deuterium.
ppm: impurities particles per million.
One can see that the maximal Ag increase after deuterium discharge at greater
density of current (35 mA) in the near-surface layer of 10 um was 250 times (from
20 ppm in an initial state up to 5000 ppm after irradiation by deuterium). The
following layer ~10 um thick only showed ~ a 100-fold Ag increase. A lower increase
(~120 times) of Ag content was observed at smaller current density (25 mA). A less
increase was observed in hydrogen at greater current density.
It can be explained by easier output of hydrogen implanted into palladium lattice
at a higher temperature of the sample (and accordingly by a smaller hydrogen con-
tent in palladium lattice), i.e. by closely related velocities of hydrogen implantation
238
Table 5. Change of In, Ni, and Zr quantity in Pd cathode at deuterium discharge (SMS).
Cr and Fe were not available in the discharge chamber parts (water-cooled stainless
steel holder was placed under eight Pd foils 100 //m thick each and one molybdenum
foil 0.1 mm thick). Cobalt and manganese have not also been found in initial Pd
and in background measurement. Cr, Fe, Co, and Mn were observed in the second
sample in smaller quantities. Therefore, Mn intensity in the upper sample was 4000
cps and only ~30 cps in the lower Pd sample. Cobalt quantity was found to be
~380 cps in the upper sample and 20 cps in the lower sample, 52 Cr was ~10000
and ~3400 cps, respectively. Only 44 Ca, 24 Mg, and Al were found to be in bigger
quantities in lower Pd sample as compared with the upper sample.
Table 6. Isotope and element composition of Pd samples irradiated by deuterium ions under
direct current discharge (TIMS).
1610(1)—irradiated sample (JVi); 1610 (2)—screened sample located under irradiated sample (N2)
240
A change of the isotope ratio in samples after carrying out deuterium bom-
bardment was observed from several percent up to hundreds. 1,2 The quantities of
"additional" elements were from 0.1 at.% up to ~ 5 at.%. The most considerable
difference in the isotope ratio was observed for Mg, Si, K, S, Ca, and Fe isotopes
after deuterium discharge.
A comparison of the chemical composition and isotope ratio on palladium sam-
ples after experiments in deuterium discharge with direct current and pulsing cur-
rent by thermo-ionization mass spectrometry is shown in Tables 7-10.
One can see from Table 8 that the quantity of Mg (24-26) and Si (28-30) isotopes
in the lower layers of the sample are higher; therefore it is impossible to explain this
fact by "impurity" from the surface.
Table 7. Change of Fe, Cr, and Ti isotope ratio with direct current by TIMS (No. 1610).
*(1) An irradiated sample, (2) the sample located under irradiated one.
** K = Nn/Nexp: natural ratio/ratio after experiments.
1 2 3 4 5 6 7 8 9
2
24 Mg 78.99 0 50/8 X 10 24/25 ~ 8 24/25 - 12 ~0.7 + 8 x 10 2
25 10 0 0/67 25/26 ~ 1 25/26 ~ 1/0.5 ~2 +67
26 11 0 0/38 24/26 ~ 8 24/26 ~ 1/0.5 ~8 +38
28 Si 92.23 0 1 x 10 2 / > 1 x 10 2 28/29 ~ 20 28/29 ~ 0.16 1 x 10 2 + 1 x 10 2
29 4.67 0 6.3 x 102/1 x 103 + 1 x 10 3
30 3.1 0 2.2 x 102/5 x 102 28/30 ~ 30 28/30 ~ 0.5 ~60 + 5 x 10 2
40 Ca 96.86 1 x 10 6 40/44 ~ 50 40/44 ~ 5 ~10
42 0.6 3 x 103 2 x 10 B 44/42 ~ 3 44/42 ~ 2.5 x 1 0 ~ 2 1,2 x 10 2 +1,97 x 10 6
43 0.15 2 x 102 ~ 4 x 10 3 44/42 - 13.3 44/42 ~ 1.25 ~10.6 +3,8 x 10 2
44 2.0 1 X 103 ~ 5 x 10 3 + 4 x 10 3
45 Sc 100 0 2 x 10 2 + 2 x 10 2
46 Ti 8 65 1.3 x 10 3 48/46 ~ 6.2 48/46 ~ 5.46 ~1.14 +1235
47 7.3 95 0 -95
48 73.8 1 X 103 7 x 10 3 + 6 x 10 3
56 Fe 91.7 2.8;<10 3 4.5 x 10 3 56/57 ~ 41.7 56/57 ~ 18 -2.3 +1.7 x 10 3
57 2.2 50 2.5 x 10 2 + 2 x 10 2
59 Co 100 0 1.5 x 10 3 + 1.5 x 10 3
Ne 20 90,5 2.0 x 10 1
21 0,27 3.0 x 10 1
22 9,32 5.0 x 10 1
Ni 58 68.1 1.5 x 10 2
60 26.2 6.5 x 10 2
Ni 61 1.25 3.0 x 10 1
62 3.6 1.3 x 10 2
Fe 56 91.7 1.6 x 10 2
57 2.2 4.0 x 10 3
Cr 52 83.8 4.8 x 10 2
53 9.5 4.5 x 10 2
Ti 48 73.8 2.0 x 10 2
47 8 1.0 x 10 1
Ga 69 60 3.0 x 10 2
71 40 1.8 x 10 2
Ba 138 71.7 3.0 x 10 3
137 11.3 1.9 x 10 2
136 7.85 1.2 x 10 2
135 6.6 2.2 x 10 2
134 2.4 2.5 x 10 2
Pb 206 23.6 4.0 x 10 1
207 22.6 4.8 x 10 1
208 52.3 1.0 x 10 2
Table 10. Isotope ratio change in 'additional" elements of Pd sample after pulsing current
experiment.
Element Isotopes Natural isotopes ratio (Nn) Ratio after experiment (Nexp) j{**
K**\ A factor of change in natural isotopes ratio to isotopes ratio after experiment (N„/Ncxp).
The "geometric" factor shows the influence of boundary conditions (Fig. 3a and
b). The maximal surface change was observed at the interfaces between radiated
and unirradiated (screened) areas. The screened areas had the insignificant change
in topological structure and chemical structure.
Mg 3.1 ± 0.2 -
Fe 6 ± 0.2 ~ 5.0xl03±2.5xl02
Al 3.7 ± 0.2 ~9.0xl05±2.5xl03
Ga 2.4 ± 0.4 ~ 7.0xl03±2.5xl02
O 50 ± 1.5 -
Ca 2.7 ± 0.3 ~ 2.2 x 1 0 3 ± 1 x 10 2
(42, 43, 44 isotopes)
Ti 4.3 ± 0.3 -
* The volume of analysis by X-ray spectral method (EDX)
on electronic microscope JEOL JSM ~ I/un .
** TIMS: thermo-ionization method; cps: impulses (ions)
per second in the sample after experiment minus the ac-
count in the initial sample. Using TIMS method, analyzed
a Pd strip 1-2 mm thick and 20 mm in length, includ-
ing a zone under the screen. The field volatilizes tens of
angstrom unit from the sample surface during the analysis.
244
**
Fig. 1. Blisters on Pd surface after 22-hour deuterium discharge exposure. Marks on the figure
are 10, 50 and 100/mi, respectively.
'^pp*
„ \ 4
Fig. 2. New formations on Pd surface after deuterium bombardment. Marks on the figure are
10, 20 and 20/xm, respectively.
As can see in Table 13, the composition (in quantity and element content) of
each element in the 1 /im-diameter point do not coincide (do not equal) with all
analyzed Fig. 4a area 250 x 200/mi 2 . The sample (1610/2) is one upper in eight
foils-multilayer sample in this experiment. Upper sample was partly melted during
experiment. However, heat balance was not estimated in this experiment.
The separate elements content, analyzed of 1610/2 area ~ 300x220 /im 2 , with
elements content on the 1/xm diameter area were compared. Data of Table 13
showed same difference in additional elements content and close values for main
elements for homogenious place of the surface.
Fig. 3. New formations on the boundary (a) of radiated and unirradiated areas (b) radiated area
on the left Fig. 4c. The screened area from glow discharge radiation. Marks on the figure are 100
and 500 /zm, respectively.
245
Table 12. Chemical composit:ion change in new formations areas (Fig. 2c).
V % <:V ^\;,
\ *V V . - / ' > • > ^ ' * ;
# ^
a. b.
Fig. 4. (a) Pd surface after deuterium irradiation by dose ~ 8 x 10 2 1 sm" - 2 (Pd # 1610, 30 mA,
400±20 V, P ~ 5 Torr, 4 h in H ^ D . Set included eight foils. Three P d foils were partially melted),
(b) Crater on the end of crack on back side of sample, (c) Screening zones.
56/57pe j s o t 0 p e r a tio by a factor of more than 100 for comparative experiments with
pulsing current and direct current was observed.
For the same Sample 1610 the isotope ratio of 4 8 / 4 7 Ti increases ~2.5 times and
48 46
/ Ti increases almost ~3.8 times due to a decrease of contribution of a heavier
isotope (the most spread 4 8 Ti isotope). The 5 2 / 5 3 Cr isotope ratio also decreases
due to a decrease of contribution of heavier isotope 53. Thus, it is impossible to
explain this effect by sputtering of a lighter isotope or by isotopes separation. Also
it is impossible to explain it by diffusion coefficient.
The 56 / 57 Fe isotope ratio in 1694 as compared with natural ratio of isotopes
is ^2.3 (Table 8). The 4 8 / 4 6 Ti isotope ratio comparison is about ~5.46. Samples
No. 1610 and No. 1694 had different experimental conditions. So No. 1610 was a
multilayered compound and after experiment some melting areas and even cracks
were found on it and No. 1694 was single-layered and its surface after experiment
was more homogeneous.
We would like to pay special attention to detection of isotopes with mass number
59 (Co), cps of which was ~10 3 cps, for 55 (Mn) ~10 3 cps, for 45 (Sc) ~ 102 cps.
They were found in a plenty in the samples after experiment but they not were
found in initial samples.
The comparison of the quantity of the elements analyzed by method SMS with
possible reactions of fusion-fission of nucleus is given in Table 15 in view of con-
formity of their masses, their spin and parity. The opportunity of simultaneous
appearance of particular isotopes groups in samples is supposed, i.e. formation
of such elements as Mg and Br (1); Mg and As (2); Si and As (3) in the same
low-energy process in glow discharge.
The variants of the reactions given in the table are possible from the results of
the analysis. It is possible to see the presence of isotopes with mass numbers 26
and 80 as results of reactions (1-4), 19 and 88 - reaction (5), 50 and 56 - reaction
(6) in one analyzed sample.
It could be possible to explain the appearance of chemical elements in the sam-
ples irradiated by ions in glow discharge by such reactions, but the high Coulomb
barrier makes the probability of such processes insignificant. Rodionov 12 paid at-
tention to the fact that the Coulomb barrier is a classical concept and the repre-
sentation of it at nuclear distances does not work. It means that the concept of the
Coulomb barrier is not meaningful in quantum ensembles for low energies of inter-
acting particles. It makes possible multinuclear reactions in low-energy processes.
Therefore, it is supposed that Fe, Ni, and Ti can appear in the following
reactions:
2
a + ^ P d ^ T i + ^Fe*+20.1MeV, (7)
o r ^ g T i + | | F e + 25.1MeV, (8)
oNa 73.3+0.7 69.3+0.7 43.4+1.2 16.4+1.5 4.3+1.3 26.4+0.2 22.4+2.1 38.3+1.3 66.2+0.7
0.13+0.05 0.13+0.10 1.7+0.4 3.1+0.3 0.63+0.25
Mg 0.12+0.04 0.2+0.1 1.0+ 0.2 1.2+0.3 1.1+0.2 0.9+0.3 1.6+0.3 0.8+0.2 1.6+0.1 0.96+0.2 0.75+0.19 0.30+0.06 1.54+0.3
Al 2.05+0.04 1.8+0.1 3.4+0.2 2.2+0.1 0.5+0.13 3.8+0.1 10.8+0.1
Si 0.3+0.1 0.3+0.1 1.0+0.1 0.4+0.1 0.6+0.1 0.5+0.1 0.3+0.15 0.27+0.1
K 0.8+0.1
S 4.1+0.2
Fe 0.06+0.03 0.2+0.1 0.20+0.07 0.12+0.06
Ni 0.2+0.1
Ga 0.22+0.05 0.4+0.1 0.8+0.2 2.2+0.2 1.6 ± 0.1 1.6+0.2 2.3+0.2 1.1+0.2 2.0+0.2 1.5+0.2 1.35+0.13 0.37+0.05 2.1+0.2
Sr 0.06+0.03 0.2+0.1
Mo 9.4+0.1 8.0+0.1 0.6+0.1 0.4+0.1 0.16+0.08 0.10+0.04
Pd 13.6+0.1 19.2+0.1 44.5+0.3 92.6+0.7 74.1 + 1.1 92.3+0.4 95.0+0.3 66.3+0.3 95.0+0.3 70.8+0.3 54.5+0.3 22.1+0.1 95.9+0.3
Cd 0.17+0.5 0.14+0.05 0.2+0.1 0.4+ 0.1
Ac 0.35+0.05 0.5+0.06 1.2+0.1 2.8+0.3 2.9+0.25
Pb 0.14+0.04 0.2+0.05 0.2+0.06 0.2+0.1 0.17+0.08 0.16+0.08 0.04+0.02
Sn 0.54+0.1 0.15+0.1
W 0.6+0.1 0.6+0.1 0.21+0.07 0.16+0.06 0.08+0.04 0.07+0.02
*EDX voltage 25 kV, # 1694.
**Columns 2—6 are the fragments of boundary of glow discharge and screening zones.
• • Columns 8—14 are the fragments of irradiated zone.
N2
CO
250
However, for reactions (7-9) with the participation of oj-particles, first the fol-
lowing possible reactions are to proceed:
Table 15. Isotopes ratio in possible nuclear reactions in Sample No. 1734 (SMS).
26 40 d + 4 ° 4 P d - • 12 2 6 Mg + |gBr* + 15.8;
§°Br* -> 17.66M:/5-2.00 : 76I6.6 ->§° Kr;
or |°Br* -> 17.66MeV : /3+.85 : X76I6.6 --> 3 4 oe 1
d + 4 g 8 Pd -> 2 | M g + |§As* + a + 12.2; 2
d + i°4Pd - ?°P*+^Zn*+a-r-9.64MeV,
a + IfPd ->?§Ne+§tSr +3.16 MeV,
a + 4°2Pd - -> i§Ne* + §§Sr + 2.92 MeV,
Masses 22 and 82 were also present in TIMS spectrums of this sample in quan-
tities of 60 and 540 count per second (cps). It is necessary to note that the instable
finding of Ag by method EDX 6 could be a result of formation
108 A „* 106A * 108 A * 110A *
47 A 6 , 47 A 6 , 47 A 6 , 47 A 6
in the following reactions with the further transmutation of these isotopes into
stable.
The opportunity of going above described reactions with the formation of argen-
tums isotopes in an excited state and their subsequent transition into stable state
can help to understand that the results of finding many elements change with a
change in the interval of the samples analysis time after the experiment termina-
tion. This fact is undoubtedly important, and it is necessary to take into account
when isotopes quantity and their composition are to be correctly estimated, as the
performance of the analysis at the time planned after the experiment termination
is not always feasible.
5. Conclusion
1. The complex of examinations showed that changes of structure and element
composition in the samples irradiated by glow discharge ions depended on:
(a) density of ions flow, (b) dose of irradiating ions, (c) kind of irradiating
ions, and (d) sort of current and other parameters of process.
2. Dependence on parameters is ambiguous as some factors simultaneously
effect (influence) the change of composition.
3. More homogeneous structure and more homogeneous change of composition
are observed for long experiments.
252
Acknowledgements
Authors express the gratitude to corresponding member of the Academy of Sciences
LI. Fedik ("Lutch") and Professor, Dr. B.U. Rodionov (MEPhI) for valuable notes
by preparation of this article.
References
1. I. Savvatimova, Ya. Kucherov, and A. Karabut, Transaction of Fusion Technology 26,
4T, 389 (1994).
2. I. Savvatimova, A. Senchukov, and I. Chernov , ICCF6, Progress in new hydrogen
energy. Japan (1996), p. 575.
3. I. Savvatimova, A. Karabut, Nuclear Reaction Products Registration. Surface,
Moscow: RAN (1996), Vol. 1, p. 63.
4. I. Savvatimova B, Karabut A.B., Radioactivity of the Pd cathode after GD. Surface,
Moscow: RAN (1996), Vol. 1, p. 76.
5. I. Savvatimova, Transmutation in cathode materials at GD. ICCF-7, Canada (1998),
p. 342.
6. I. Savvatimova, Reproducibility of experiments in GD, ICCF8, Italian Phys. Society,
Italy (2000), p. 277.
7. J. Dash, I. Savvatimova and H. Kozima, Effects of GD on Radioactivity Proc. ICENES
2002 (2002), p. 122
8. J. Dash, and I. Savvatimova, Effects of glow discharge with hydrogen isotope plasmas
on radioactivity of uranium, Proc. ICCF10, Bejing, China, 2002.
9. I. Savvatimova and D. Gavritenkov, Results of Ti analysis after GD. Proc. ICCF11
(2004).
10. A. Karabut, Ya. Kucherov, and I. Savvatimova, Possible nuclear reactions mechanisms
at glow discharge in dseuterium. Proc. ICCF3, Japan (1992), p. 165
11. V. Ivanov, Excitation and effect of microplasma discharges on metals and alloys in a
microwave plasma torch, Applied Physics B2, 5(2001).
12. Rodionov, Proc. 12 Rus. CF Conf. 2004, Moscow (2005), p. 110.
13. Ya. Kucherov, A. Karabut, and I. Savvatimova, Phys. Let. A170, 265 (1992).
14. G. Vorontzova, and I. Savvatimova, Atomic Energy 69(5), 297 (1990).
ELEMENTAL ANALYSIS OF PALLADIUM ELECTRODES A F T E R
P d / P d LIGHT WATER CRITICAL ELECTROLYSIS
YU TORIYABE
Division of Quantum Science and Engineering, Graduate School of Engineering,
Hokkaido University, North 13, West 8, Kita-ku, Sapporo 060-8628, Japan
E-mail: torigoya@pop.qe.eng.hokudai. ac.jp
TADAHIKO MIZUNO
Division of Energy and Environmental System, Graduate School of Engineering,
Hokkaido University, North 13, West 8, Kita-ku, Sapporo 060-8628, Japan
TADAYOSHI OHMORI
Advanced Technology, Inc., Hokkaido Institute of Technology, Maeda, Teine-ku,
Sapporo 006-8585, Japan
YOSHIAKI AOKI
Technology and Electronics College of Hokkaido, Nakanoshima, Toyohira-ku,
Sapporo 062-0922, Japan
1. Introduction
Since Ohmori et al. reported nuclear transmutation reactions with anomalous iso-
topic yields in his light water electrolysis system, 1_4 many researchers still have
claimed various kinds of low energy nuclear reactions. At the same time they
observed continuous excess heat as results and countless craters as an evidence
of nuclear reactions. A chain of their results in light water system deserves close
attention that strongly suggest the existence of condensed matter nuclear reactions.
It is, however, still difficult to replicate that reaction in normal electrolysis con-
dition. Through our previous experiments and the other reports, 5 ~ 8 we conjecture
253
254
Figure 1. Surface damage as an indirect evidence of nuclear reactions occurred at the electrode
surface. These craters were observed on gold electrode after normal electrolysis, with current
density of 0.5 A / c m 2 for 30days in 0.5 M Na2CC>3 solution. 9
that the electrolysis system and electrical parameters are very important factors to
induce nuclear reactions. We have investigated an optimum electrolysis system and
condition and describe details in this paper.
Both transmutation products and surface damage are needed to prove that a
nuclear reaction has occurred. Figure 1 shows an example of damages in a gold
electrode reported by Ohmori et al9 Although many researchers have reported
nuclear transmutation, as far as we know, there has been no other reports of the
Ohmori-type craters. If the nuclear reactions occur on the electrode surface, the
surface damages like Ohmori-type craters should be found after the experiment.
2. P l a s m a Electrolysis
2.1. Time Variations
It is widely recognized that plasma electrolysis can produce a large amount of excess
heat, and nuclear transmutation products. When the temperature of an electrode
exceeds the boiling temperature of electrolyte due to intense polarization, a thin
vapor layer is generated at the electrode/electrolyte interface in which high electric
field ionize vapor molecules to generate the plasma state. Formation of this vapor
film is the first key factor to achieve the plasma electrolysis condition.
Time variations of cell voltage and current during the plasma electrolysis are
shown in Fig. 2. In this case the axis of ordinates indicates not only current but
also current density because the electrode surface of cathode is ca. 1cm 2 . The
period of electrolysis is divided into six regions for the sake of convenience, namely
conventional region, critical region, breakdown point, transitional region, partial
plasma region, and full plasma region.
The electrical current increases with applied voltage up to the breakdown point
at which time the sheath of vapor film is generated. Then the current drops down
through the transitional region because the electrode and the electrolyte cannot
touch each other directly owing to the vapor layer.
255
320
2 swH
280 1 <3 4 •••-•-M JSL
>^
<D 160
m
V
"o
= 120
o
JV
80
(w^Um,
0.5
"M I I :
0 2000 4000 6000 8000 10000
Time (s)
Figure 2. Time variations of cell voltage and current during plasma electrolysis with 1.5 mm
diameter tungsten cathode in 0.2mol/dm 3 K2CO3 solution. (1) Normal region, (2) critical region,
(3) breakdown point, (4) transitional region, (5) partial plasma region, and (6) full plasma region.
If cell voltage is sufficiently high, some atoms or molecules in that gas phase are
ionized. Therefore, current does not drop to zero and the electrode temperature
remains high due to the good electrical conductivity and reduced thermal loss of
the gas phase. Starting from this region, light emission occurs. The color of light
depends on the electrolyte solution. Light emission area expands with increasing the
cell voltage. Finally, in region-6, the glow covers the entire surface of the electrode
and the intensity of light becomes strong. We defined these two regions, regions 5
and 6, as plasma region.
2.2. VI Relation
A voltage-current relation of plasma electrolysis is shown in Fig. 3, which is con-
verted from Fig. 2. When the current density increases above approximately
2.5 A/cm 2 , the type of electrolysis changes to the plasma where the current is
almost constant. This critical value also supports the experimental result reported
by Ohmori et al.w It is necessary to select an experimental condition, current and
voltage, from this VI curve.
2.3. Shortcomings
Although the plasma electrolysis can induce a large amount of excess heat with
hydrogen and anomalous nuclear transmutation, 11 ' 12 this type of electrolysis has
some and fatal shortcomings.
At the boundary between regions 5 and 6, that is, at the time when whole area of
the electrode surface is covered with the glow, the temperature of the surface rises
to 1400°C. Furthermore the local temperature exceeds the melting point of the
electrode at where the sparks like arc discharges occur due to current flow paths
between the electrode and the electrolyte. Therefore, the electrode cannot survive
more than 30 min without being melted or broken. And the electrolyte solution is
also pyrolyzed by the high-temperature plasma.
The most serious problem is that the rare nuclear transmutation products on
the electrode surface are lost from this damage. Therefore another, milder type of
electrolysis, which does not severely damage or disintegrate the electrode, is called
for to prove that nuclear reactions occur.
3. Critical Electrolysis
3.1. Optimum Region
We assume the positive correlation between the excess heat and the current density
exists in normal region, while the excess heat increases with the input voltage in
plasma region. This assumption is illustrated in Fig. 4 with the VI relation described
in Fig. 3. In fact, some researchers have reported these correlations. 13~15
Since the plasma region is inappropriate, Ohmori et al. specified that region-2 is
most favorable one to obtain the excess heat and the transmutation in electrolysis
system, and they referred to this type of electrolysis as Critical Electrolysis. 7 ' 8
Although the exact condition required depend on the experimental system, a target
2.5
2
<
I" 1
0.5
Figure 4. An optimum region to induce nuclear reaction without disintegrating the electrode.
257
3.2. Results
We had conducted critical electrolyses with nickel cathodes in 1M Na2CC>3
solutions. 5 Figure 5 shows EDX spectrums of nickel electrodes after the experi-
ment through which the current density was kept ca. 2.6 A/cm 2 for 15 days. The
mean voltage applied was 14 V and solution temperature raised up to 80°C.
Detected strong platinum peaks are probably originated from a counter electrode
though the isotopic ratio for this platinum has not been confirmed yet. In gen-
eral, the platinum anode is less dissolved and electrodeposited in alkaline solution,
especially K2CO3 or Na2CC>3. However the experimental results suggest that this
unusual reaction is accelerated in certain conditions, and this platinum compli-
cates transmutation processes such as photofission.16 Then that electrodeposited
platinum makes an evaluation of process difficult. Therefore in the experimental
system the anode material should be the same as the cathode.
1000000
100000
I 10000
o
O
1000
Energy (keV)
Figure 5. EDX spectrums of nickel electrodes before and after the critical electrolysis with current
density of 2.6 A / c m 2 for 15 days in 1 M Na2C03 solution.
4. P d / P d Critical Electrolysis
4.1. Experimental Set-up
P d / P d Critical Electrolysis is defined as the optimum condition to evaluate
the transmutation process precisely. In this system, the effect of materials
electrodeposited from the anode is avoided by making the anode from the same
element as the cathode. This limits the elements detected on the cathode to being
either impurities from elsewhere in the cell, or from transmutation. Furthermore,
if these elements are transmutation products, evaluating them is simpler.
258
Hose |
^iftCOtl fuB*>^
A Teflon (PFA) cell (Flon Industry Co. Ltd., Tokyo, Japan) whose capacitance,
diameter and height are 300 cm 3 , 80 mm and 70 mm, respectively is capped with a
silicon rubber. Although vapor cannot leak from this system, hydrogen can easily
leak from a hole with another silicon rubber to add the Milli-Q water to restore the
volume of the electrolyte, which decreases due to the decomposition.
In this experiment the anode and cathode are made from identical palladium
wires (Tanaka Kikinzoku Kogyo, Tokyo, Japan) taken from the same stock. Both
are 99.95% pure Pd, 1.0mm diameter, 15.7rnm long, with ca. 0.5cm 2 surface area.
They were polished up by emery papers (No. 1500 and No. 2000), and washed with
acetone. After being covered with Teflon (PTFE) tubes, they were located at the
both side of the cell symmetrically. Before the experiment, the cell and electrodes
were cleaned carefully with nitric acid or sometimes mixed acid (1:1 H2SO4+HNO3),
and rinsed with Milli-Q water.
The electrolyte solution of 1M and 200 cm 3 was prepared by K2CO3 (Kanto
Chemical Co. Inc., Tokyo, Japan) whose purity is over 99.95% and Milli-Q water
whose specific resistance is over 18.0Mf2cm. Isotopic abundant of hydrogen and
deutrium atoms of this Milli-Q water is natural since ordinary water was used. The
natural concentration of D 2 0 is so low the influence from it is negligible.
The cell was placed in a constant temperature chamber (MIR-151, Sanyo Electric
Co. Ltd., Osaka, Japan). The solution temperature was roughly measured by two
thermo couples, which located at the center and edge of the cell. Air temperature
v/as also monitored and kept 22.0-24.0°C.
The current density exceeded 2.5 A/cm 2 controlled by a constant current/voltage
power supply (GP0250-3R, Takasago Ltd., Hyogo, Japan). The experiments were
continued for 7 or 10 days, while various data was collected on a data logger (8421-
50, Hioki E. E. Co., Nagano, Japan). During the electrolysis, Milli-Q water was
added every 12 h to restore the volume of electrolyte lost to decomposition.
259
' Pdi
Cathode 1
Anode |
»Pd
1 --P-d-i
'"Cu"" Fe
W/Mg Fe Cu
0
^ ^
Figure 7. EDX spectrums of palladium electrodes, cathode and anode, after the P d / P d critical
electrolysis with current density of 3.2 A / c m 2 for 7days in 1 M K2CO3 solution. Counts of anode
spectrum are multiplied 1.18 to be overlapped with the cathode spectrum.
The elements shown in bold letters iron, titanium, chromium, manganese, and
nickel were detected from the cathode palladium only, on the other hands, the
elements shown in italic letters, copper, zinc, and magnesium were detected from
both electrodes in this case. Therefore, we consider the elements shown in bold
letters must be transmutation products. Especially, the iron peaks were detected
from all cathode samples after P d / P d critical electrolysis.
The elements shown in italics may have originated from two possible sources:
transmutations or impurities. If these were transmutation products, at least two
processes may explain their existence. The first nuclear reaction presumably oc-
curred at the cathode and only produced the bold letter elements, while the second
reaction occurred at both electrodes, and produced the italic letter elements.
Since we have not analyzed the samples by the other methods, we cannot de-
termine the origin of these elements yet. If we confirm the isotopic distribution
is anomalous, we will then be prepared to discuss the origin and transmutation
processes of the detected elements, whether they are electrodeposited impurities or
transmutations.
4.3. Micro-Structure
Figures 8 and 9 are the SEM photographs of the anode palladium surfaces and
the cathode surfaces after the P d / P d critical electrolysis, respectively. The anode
palladium has some cracks due to the oxidation.
260
Figure 8. SEM photographs of the anode palladium surfaces after P d / P d critical electrolysis
with current density of 3.6A/cm 2 , for 10days in I M K2CO3 solution. Magnifying power and
scale standard line are shown at the bottom of each photograph.
Figure 9. SEM photographs of Olnnori-tYpe palladium crater^ un the cathode sui(Vu«> after
P d / P d critical electrolysis with current density of 3.6 A / c m 2 , for 10days in I M K2CO3 solution.
Magnifying power and scale standard line are shown at the bottom of each photograph. The
craters whose maximum size is over 10 fim. are located along the surface cracks.
261
4.4. Discussion
To our knowledge, this is the first report of the Ohmori-type craters observed on
the palladium electrodes. The characteristics of these palladium craters are similar
to the gold craters first reported by Ohmori et al.3 Although the report was made
10 years ago, the formation mechanism is still unknown.
Kamada et al. reported anomalous heat evolution and surface melting of
deuteron implanted aluminum foil upon electron bombardment. 17 They estimated
that the amount of anomalous heat exceeds the total amount of any kind of chem-
ical reactions and, therefore, concluded a novel nuclear reaction had been occurred
in the deuterated aluminum. If palladium electrode were melted due to this type of
nuclear reaction, the palladium gas should be erupted. Then it should have cooled
down in the solution to be recrystallized like the crater.
Numata et al. found vortex patterns on well annealed thick palladium electrodes
after a long-term heavy water electrolysis,18 and simulated a magnetic interaction
of hypothetical particles to elucidate an evolution mechanism of vortexes. 19 They
showed the vortex can be formed at the electrode/electrolyte interface by FEM
method. If charged palladium particles dissolved from the anode were caught in
a vortex, which is generated at the electrode/electrolyte interface, they might be
accumulated to the cylindrical shape like the vortex to form the craters.
Mizuno et al. described a large explosion that occurred during a normal light
water electrolysis. 20,21 They made a rough estimate of the energy balance and
concluded that it could not be a simple explosion, but rather it must have been
caused by a large burst of anomalous heat. If micro explosions occurred on the
electrode surface from this same type of heat, craters could be generated.
It is still difficult to explain the mechanism by these theories. Although they
may be impurities electrodeposited uniformly, we claim that the crater is an indirect
evidence of nuclear reaction occurred at the electrode surface.
5. Conclusion
P d / P d light water critical electrolyses were performed as the optimum condition
and system to induce nuclear reactions. In this study the shape of both electrodes
262
was just same and the current density was over 2.5 A / c m 2 , for 7 or 10days, in 1 M
K2CO3 solution whose t e m p e r a t u r e was u p to 70-90°C.
After the experiment, the obvious t r a n s m u t a t i o n products namely iron, tita-
nium, chromium, manganese, and nickel were detected by EDX. In particular, the
iron peaks are very strong and detected from all cathode samples. The anomalous
isotopic yield of detected iron should be expected since the anomaly has already
claimed by many researchers. 3 ' 4 ' 2 2 T h e elements detected from the b o t h electrodes,
namely, copper, zinc, and magnesium, however, cannot indicate their origin at this
time. If they are t r a n s m u t a t i o n products, at least two mechanisms exist.
T h e analysis of isotopic yields for all elements detected by SIMS must be indis-
pensable to prove nuclear reactions. Quantitative analysis of the detected elements,
distribution especially around craters, and isotopic yields are under considerations.
Moreover, nuclear radiation detection could give important information to evaluate
the process. Precise heat measurement is also required. Accurate estimation and
reduction of impurities is also vital.
Although the isotopic yields have not confirmed yet in this study, Ohmori et al.
have already reported anomalous isotopic distribution of palladium with excess heat
in their P d / P t critical electrolysis s y s t e m . 7 , 8 Furthermore the indirect evidence of
nuclear reactions, namely Ohmori-type palladium craters were observed for the first
time. Since the t r a n s m u t a t i o n products and the surface damages have been found,
P d / P d critical electrolysis is optimum to induce condensed m a t t e r nuclear reactions.
References
1. T. Ohmori and M. Enyo, Proc. ICCF4 1, N2.3 (1993).
2. T. Ohmori and M. Enyo, J. New Energy 1(1), 15 (1996).
3. T. Ohmori, T. Mizuno, and M. Enyo, J. New Energy 1(15), 90 (1996).
4. T. Ohmori, M. Enyo, T. Mizuno, Y. Nodasaka, and H. Minagawa, Fusion Technol.
31, 210 (1997).
5. Y. Toriyabe, T. Mizuno, T. Ohmori, and Y. Aoki, Proc. JCF6 11 (2005).
6. T. Mizuno, T. Ohmori, and T. Akimoto, Proc. ICCF10 (2003).
7. T. Ohmori, S. Narita, H. Yamada, T. Mizuno, and Y. Aoki, Proc. JCF4 22 (2003).
8. T. Ohmori, T. Mizuno, H. Yamada, and S. Narita, Proc. JCF5 36 (2004).
9. A. Takahashi, H. Numata, H. Yamada, Y. Iwamura, T. Ohmori, T. Mizuno, and T.
Akimoto, Study Nucl. React. Solid 159 (1999).
10. T. Ohmori, Curr. Top. Electrochemistry 7, 102 (2000).
11. T. Mizuno, T. Ohmori, T. Akimoto, and A. Takahashi, Jpn. J. Appl. Phys. 39, 6055
(2000).
12. T. Mizuno, T. Akimoto, K. Azumi, T. Ohmori, Y. Aoki, and A. Takahashi, Jpn. J.
Appl. Phys. 44(1A), 396 (2005).
13. T. Ohmori and T. Mizuno, Curr. Top. Electrochemistry 5, 37 (1997).
14. M.C.H. McKubre, S. Crouch-Baker, A.M. Riley, S.I. Smedley, and F.L. Tanzella, Proc.
ICCF3 5 (1993).
15. K. Kunimatsu, N. Hasegawa, A. Kubota, N. Imai, M. Ishikawa, H. Akita, and Y.
Tsuchida, Proc. ICCF3 31 (1993).
16. A. Takahashi, M. Ohta, and T. Mizuno, Jpn. J. Appl. Phys. 40, 7031 (2001).
17. K. Kamada, H. Kinoshita, and H. Takahashi, Jpn. J. Appl. Phys. 35, 738 (1996).
263
M. A P I C E L L A A N D V. V I O L A N T E
ENEA Frascati Research Center, V. le E. Fermi 45, 00044 Frascati (Roma), Italy
E-mail: violante®frascati. enea.it
F . S A R T O , A. R O S A D A A N D E. S A N T O R O
ENEA Casaccia Research Center, V. Anguillarese 301, 00060 S.Maria di Galeria
(Roma), Italy
E. C A S T A G N A A N D C. SIBILIA
La Sapienza University, Via Scarpa, 14, 00100 (Roma), Italy
M. M C K U B R E A N D F . T A N Z E L L A
SRI International, 333 Ravenswood Ave, Menlo Park, CA 94025, USA
G. H U B L E R
Naval Research Laboratory, 4555 Overlook Ave., S.W. Washington, DC 20375, USA
A research activity has started some years ago in the framework of collabora-
tion between the ENEA (Italy) and the SRI (USA), aimed to the identification
of traces of nuclear reactions in condensed matter. This work has also involved
cross-linked analysis in order to identify effects due to contaminants that could
affect the isotopic shift estimate. Nickel thin films have been sputtered on a poly-
meric substrate and loaded with hydrogen by electrolysis. Reference and active
thin films have been prepared contemporaneously during the same sputtering pro-
cess to have on both the same deposition and the same impurities composition.
Secondary Ion Mass Spectroscopy (SIMS) has been used to analyze the isotopic
composition of the electrolyzed and blank substrates. Preliminary results (Violante
et al, Proc. 10th Int. Conf. Cold Fusion (ICCF-10), Cambridge, 2003) indicated
that a reasonable reproducible apparent shift of the isotopic composition of the
Cu element occurred in some of the electrolyzed films, with an increasing of mass
65, while the natural value was always observed for all the blank samples. Cu was
particularly suitable for being used as a marker elements because of its only two
mass isotopes (63/65) that do not overlap with isotopes of other elements having
the same masses. In this work, new experiments have been reproduced to increase
the statitistics and further analysis has been performed in order to exclude that
the revealed shift was traceable to an artifact.These included SIMS scanning of the
sample surface, depth profile analysis by SIMS, mass spectrometric analysis of the
electrolyte, SUPER-SIMS [2] analysis of one couple of reference and active films. In
particular, the possible contribution from mass interferences on the 65-mass extra-
signal has been considered, coming from contaminants or double ionized species.
On the basis of the new results, a more complex scenario has been evidenced,
264
265
1. Introduction
The detection of nuclear ashes inside metallic hydrides is one of the most direct
evidences of the happening of nuclear reaction in the condensed matter. But this
topic is also a very complex and delicate issue, first of all because of the low level
of the signals to be detected, which can be easily overlapped by instrumental noise
or background interferences.
The measurement of the isotopic composition of metallic hydrides is an efficient
method to reveal nuclear products eventually formed during the hydrogen loading.
Actually, the presence of "new" (i.e. "not detected before") elements in the metal
specimens cannot be assessed as products of a nuclear reactions, because the pos-
sibility of contamination from the environment or the diffusion of impurities inside
the sample to the detection areas are very difficult to be excluded completely.
A research activity has started some years ago in the framework of collaboration
between the ENEA (Italy) and the SRI (USA), aimed to the identification of traces
of nuclear reactions in condensed matter.
Preliminary results 1 by Neutron Activation Analysis (NAA) have given indica-
tion of Ag isotopic shift occurring in Pd thin films after electrolysis. A first screening
by Secondary Ion Mass Spectrometry (SIMS) of the isotopic composition of Nickel
thin films undergone to similar experiments has also pointed out an isotopic ratio
different from the natural one on the 63/65 masses imputable to copper. 2
In this work, further reproduction of the previous experiments and a more accu-
rate analysis of the experimental data have been performed. Cross-linked analysis
has also been involved, in order to identify artifacts that could affect the isotopic
shift estimate.
2. Experimental
The typical experiment, already described in Ref. 2, consisted in three steps:
• Deposition of two identical Reference and Active nickel films during the
same deposition run;
• Hydrogen loading of the Active film by electrolysis;
• SIMS analysis of both Reference and an Active sample isotopic composition,
to search deviations from the natural abundances.
266
Steps (1) and (2) have been carried out in a class 1000 clean room laboratory, by
using clean room grade gloves and papers in order to reduce source of contaminants.
To the same aim, a reduced number of high-purity materials have been used both
for sample production and electrolysis cell assembling.
3. Results
Preliminary results reported in Ref. 2 showed an apparent isotopic shift on the
63
Cu/ 6 5 Cu masses in nickel thin films undergone to electrolysis (active films),
whereas an isotopic composition matching the natural abundance was always de-
tected in the not-electrolysed (reference) films.
267
Ni Ibis Ok Yes No
Ni 3bis Ok Yes No
Ni P2 Ok Yes No
Ni P3 Ok No No
Ni 4 Ok Yes No
The tuning of the SIMS instrumentation was checked during each of the analysis
runs, by moving the sputtering argon beam on the stainless steal sample-holder
where the Cu isotopic composition was always found to be the natural one. We
have repeated the same experiment in order to increase the statistics and evaluate
its reproducibility.
A synoptic of the new experiments has been reported in Table 1, giving evidence
of the apparent isotopic shift in 4/5 cases.
The SIMS analysis has been carried out on different points of the sample surface,
showing a more relevant effect in the middle of the sample (see Fig. 1).
Furthermore, a dynamic SIMS analysis has been done in order to check if the
shifted isotopic ratio was maintained below the surface. The depth profile of the
63, 65, 58, and 12 masses has been recorded, showing that the 63/65 shift survives
beyond the surface down to the film/substrate interface, and it is not coupled with
the C 12 signal of carbon but with the Ni 58 signal, originated by from the main
constituent of the film (see discussion below).
In addition, a cross-linked analysis has been done by using the SUPER-SIMS
facility located at the ETH, in Zurich (Switzerland). 3 The instrument used Cs +
primary ions and the analysis revealed negative secondary ions. A couple of Ref-
erence and Active samples have been analyzed to verify the above results. Due to
unwanted charging of some parts of the extraction section, causing signal instability,
the Cu 63 /Cu 65 isotopic ratio measurement needed calibration by a pure standard.
Then, a sequential procedure has been followed to carry out the measurements,
consisting in the analysis of a pure Cu standard, the Reference sample, the pure Cu
standard again and the Active sample. The values measured for each sample, after
calibration, showed some discrepancies with the measurements performed in Rome,
giving Cu 6 3 /Cu 6 5 = 2.40 ±0.31 for the Active sample and Cu 6 3 /Cu 6 5 = 1.79 ±0.02
for the Reference sample. In the following discussion, both results are carefully
analyzed, in order to get informing conclusions.
4. Discussion
An alteration of the isotopic ratio of the copper is relatively simple to detect because
copper has only two stable isotopes, which do not overlap with isotopes of other
elements having the same masses. However, mass interferences on the considered
268
1.00e+003
SINS-SNNS
cps Mass scan
65 Datapoints/[amu] 54
1 Scan speed
[sec/amu] 6.000
Resolution 7.0
Smoothing ON
Vertical scale LIN
J=3
r
63 1 V 1 ',
i \
1.00e+000
If
52 5 0 0
>f
Ni/Pe
i1 V *
Pos 6=340 Z=57.5 66.500 [amu]
s.
5.00e+002
SINS-SNNS
cps
Mass scan
Datapoints/[amu] 64
Scan speed
! i [sec/amu] 6.000
Resolution 7.0
A Smoothing ON
Vertical scale LIN
! Current 10
i
i in Speed 6
f I 63
i * • A
As
1-OOe+OOO
If
1
'/
«
\ m
«—-^
61.500 Ni/Pe Pos. 57.5 9=335 65.500 [amu]
Figure 1. SIMS spectrum of the Active sample in the midway of the specimen (left) and close to
the edge of the specimen (right).
65 and 63m/e signals from compounds or double ionized species could affect the
results, when using a conventional SIMS facility with limited resolution. Therefore,
a careful analysis of all possible contribution to the 65-m/e signal in the SIMS
spectrum has to be done, concerning the above described results.
Ni 64 H (65 mass) detection has been considered unlikely, because the isotopic
ratio Ni 62 H (63 mass)/Ni 64 H (65 mass) of Ni more abundant isotopes did not match
the natural value (3.9), being the observed isotopic shift just into the opposite
direction.
The contribution to the 65 m/e signal from double ionized ions had also to be
excluded because of the absence of signals at 130 m/e, relative to the corresponding
single ionized elements (Te 130 or Ba 130 ?).
A more complicate issue consisted in excluding possible interferences from or-
ganic contaminants, which could produce positive ion fragments having 65 molecu-
lar masses. Actually, 65 mass C 5 H^ ion is very reactive, but it could be produced
269
Ni58/C12 35 ± 2 8.1 ± 0 . 5
Ni58/mass65 65 ± 6 49 ± 16
during the SIMS analysis by fragmentation of higher mass organic molecules (hy-
drocarbons).
Typical spectra of hydrocarbon contaminants show groups of odd mass peaks
with 12a.m.u. periodicity (due to 1 C atom increment in the chain fragment). 4
Fragmentation patterns of hydrocarbons involving 65-mass positive ion are reported
in literature, 4 ~ 6 but they were not clearly readable in our SIMS spectrum [see Fig. 2:
masses 15, 43, 69 are not detected masses 51, 53, 55, 57 are masked by signals due
to isotopes of clearly identified elements, present also in the reference sample (V 51 ,
Cr 53 53, Mn 55 , Fe 57 )].
10 20 30 40 50 60 70 80 90
m/e (a.m.u.)
Figure 2. SIMS spectrum of the Active film in the wide mass range.
The possibility of organic contamination of the film surface from the electrolytic
solution has been also considered. Gas chromatography analysis of the electrolyte
has been performed, showing that organic contaminants are less than 1 ppb.
On the basis of the above-mentioned observations, one should exclude a con-
tamination due to organic substances at mass 65.
Finally, the possible interference from inorganic compound contaminant match-
ing 65 mass has been considered. By seeing at the more abundant elements re-
vealed in the whole range SIMS spectrum, detection of Ni 58 Li 7 (total mass = 65)
compound could be expected. In fact, despite of NiLi is not a stable compound; Li
is clearly detected on the active film surface, coming from the electrolytic solution.
Supporting this assignation is the detection in our SIMS spectrum of the 65, 67, 82,
and 84 mass peaks, which can be associated to the isotopes of the NiLi and NiL-
iOH compounds (mass 65 =4> Ni 58 Li 7 , mass 67 =4> Ni 60 Li 7 , mass 82 => Ni 58 Li 7 OH,
mass 84 =>• Ni 60 Li 7 OH). In Table 3 are reported the intensity ratios between the
SIMS peaks associated with the above compounds. The obtained values match the
natural isotopic ratios in the case of the Ni 58 and Ni 60 isotopes, but nothing can be
said in the case of Li 7 , Li6 isotopes, due to the poor accuracy of the data, affected
by the Ni 64 contribution to the 64 peak.
In conclusion, the contribution to the 65 mass peak from Ni 58 Li compound
seems to be the only reasonable explanations of the reported results, out of the
copper isotopic shift hypothesis.
This supposition could also be consistent with the SUPER-SIMS results, which
indicated a value for the isotopic composition of copper similar to the natural one
for both the active and reference films analyzed.
Some uncertainty still affect our results, concerning the fact that Li contami-
nation from the electrolyte is expected in all electrolyzed samples while in some of
them the 65 extra signal has not been revealed. As concerning the SUPER-SIMS
measurements, the information is limited to a restricted area of the film surface,
because only one point of the surface of each sample has been analyzed, which
could be not representative of the whole sample surface, since a gradient effect in
the isotopic composition has been demonstrated by the conventional SIMS surface
scanning analysis.
Further experiments and tests could be useful in the future, to completely
understand the present data. In particular, surface scanning by ultra-high res-
olution SIMS apparatus (m/<5m > 3000, enough to resolve mass interferences),
Table 3. Intensity ratios between the SIMS peaks associated with the
NiLi and NiLiOH compounds
5. Conclusions
Acknowledgments
References
1. V. Violante, M. L. Apicella, L. Capobianco, F. Sarto, A. Rosada, E. Santoro,
M. McKubre, F. Tanzella, and C. Sibilia - Search for nuclear ashes in electrochem-
ical experiments. Proc. of 10th International Conference on Cold Fusion (ICCF-10),
Cambridge, MA, August 24-29 (2003), World Scientific Inc., Singapore.
2. SUPER-SIMS analysis has been performed by the facility located at ETH, by Dr. M.
Doebely.
3. V.Violante, P.TYipodi, D. Di Gioacchino, R. Borelli, L.Bettinali, E.Santoro, A. Rosada,
F.Sarto, A.Pizzuto, M.McKubre, F.Tanzella, X-ray emission during electrolysis of light
water on palladium and nickel thin films. Proc. of 9th International Conference on Cold
Fusion, (ICCF9), Beijing, May 19-24 (2002).
4. SIMS technical report by RIBER Instrumentation Ultra-vide, France.
5. Integrated Spectral Data Base System for Organic Compounds by National Insti-
tute of Advanced Industrial Science & Technology, SDBSWeb: http://www.aist.go.jp/
RIODB/SDBS/.
6. Organic Compound Database by Harold M. Bell at Virginia Tech., http://www.colby.
edu/ chemistry/cmp/cmp.html.
IN SITU ACCELERATOR ANALYSES OF PALLADIUM COMPLEX
UNDER DEUTERIUM PERMEATION
1. Introduction
It has been claimed 1 ' 2 that forced permeation of deuterium through
P d / ( C a O + P d ) / P d samples doped with some element X induced nuclear trans-
mutations from X to X', where (X, X') being ( 133 Cs, 1 4 1 Pr), (88Sr, 96 Mo), ( 138 Ba,
150
Sm), and ( 137 Ba, 149 Sm). The main diagnostic methods in these studies were
X-ray photoelectron spectroscopy (XPS), time-of-flight secondary-ion mass spec-
troscopy (TOF-SIMS), and X-ray fluorescence (XRF). To confirm and investigate
the phenomena, it is essential that the same results be obtained in different labo-
ratories with different analytical methods.
We have constructed an experimental system, with which accelerator anal-
yses of the samples including particle induced X-ray emission (PIXE), elastic
recoil detection analysis (ERDA), nuclear reaction analysis (NRA), and Rutherford
backscattering spectroscopy (RBS) can be made in situ and simultaneously with
gas permeation through the samples.
In the present work, we use a sample similar to, but somewhat different from
those used in Refs. 1 and 2: vacuum/CaO/Sr/PdD a ; /D2. Here we report preliminary
experimental results on the transmutation diagnosed by conventional XPS method.
Results from the in situ analyses will be published later, elsewhere.
272
273
I I I I I I l I l
0 2 4 6 8 10
Time [s]
Figure 1. (a) Schematic of deuterium permeation in situ accelerator analyses system, (b) the
CaO/Sr/PdDj; sample structure, and (c) electrochemical method used for Sr deposition onto the
Pd sample.
regia/D20. Sr atoms were then deposited on one side of the Pd surface using a
method similar to electroplating: as shown in Fig. 1(c), the Pd sheet was carefully
placed on the surface of the 10 mM Sr(N03)2/D20 solution, so that only one side of
the sheet was in contact with the solution. A bias voltage of 1V was applied between
the Pd cathode and a Pt anode wire immersed in the solution. The ion flow onto the
Pd cathode was appreciable only at the beginning of the electroplating process, as
can be seen in the graph, implying a saturation of the surface with contamination
layer containing Sr. Neither further increase in the processing time nor multiple
immersions and biasing resulted in any increase in the areal density of Sr deposited.
Next, a CaO layer was deposited on the Sr/Pd surface by RF sputtering for
5-20 min. The thickness of the CaO layer was deduced from variation of the XPS
spectral intensities. As shown in Fig. 2(a), the peak intensities of Pd-3d and Ca-2p
photoelectrons vary with surface etching time. The CaO layer thickness x is cal-
culated from the intensity ratio of these peaks, Ica^p/ypd-sd: using the following
equation:
_ " P d <7Pd Apd-Pd frba-2p
exp 1 — exp (1)
, AcaO-Pd J \ *" V AcaO-Ca J J " C a OCa AcaO-Ca ^Pd-3d '
where n C a , "Pd, cca, opd, ACao-Ca, A Pd _ Pd , and ACao-Pd are the atomic density
of Ca and Pd, the differential photoelectron emission cross-section for Ca-2p and
Pd-3d, and the mean free path 3 of Ca-2p photoelectrons in the CaO layer, that of
Pd-3d photoelectrons in the bulk Pd and that of Pd-3d photoelectrons in the CaO
layer, respectively. For samples thicker than several nano meters, an extrapolation
of the thickness to the null etching time is necessary to deduce the initial thickness
of the CaO layer as shown in Fig. 2(b).
Pd-3d Ca-2p
• Sample#1
A. Sample#2
• Sample#3
• Sample#4
Figure 2. (a) XPS analysis of C a O / P d samples and (b) determination of the CaO layer thickness
from the XPS peak intensities.
3. Deuterium Permeation
A disc-shaped sample thus prepared with a diameter of 26 mm was placed in the
vacuum chamber as shown in Fig. 1. Its rear surface was exposed to D2 gas at a
275
pressure of 0.1 MPa, while the front surface was faced to vacuum with an effective
area of 2.5 cm 2 .
Variation of the D2 gas pressure after its introduction into the reservoir was
monitored to give the number of deuterium atoms absorbed in and/or transmitted
through the sample as shown in Fig. 3(a). If the CaO layer acted as a barrier for
deuterium permeation to allow negligible transmission into the vacuum, the sample
would have become saturated with deuterium, i.e., PdD0.86, at about 100h.
This process of deuterium charging is described by a 1-dimensional solution
of the diffusion equation for the sample with a thickness and area of a and S,
respectively. One side of the sample is opaque for deuterium, while the other faces
hydrogen gas to give a boundary condition for the deuterium density; n(a) = no-
The number of deuterium atoms absorbed in the sample, Na(t), is given as a function
of time by
OO
;2s + i ) ^
Na(t) = aSn0 1 E (2s-
exp 2a
Dt (2)
s=0
A characteristic time £i/ 2 for the number of deuterium atoms absorbed to reach
a half of the saturation value, i.e., Na(ti/2)/aS = Na(oo)/2aS = 2.9 x 1022 c m - 3 ,
is therefore given by
0.1967a2
h/2 — 6 x lO's. (3)
D
The observed value is more than three orders of magnitude larger than this
value. This fact implies that there is another barrier on the rear surface facing the
D2 gas, possibly due to contamination. Figure 3(a) shows that the deuterium flux
through the sample should have been about 2.5xl0 1 5 cm 2 /s.
After 10 days of permeation with deuterium, desorption of the D 2 gas from the
sample was so severe that an outgassing procedure was necessary for the sample
3
-
"
J-
2
- fty !
\
\ ^
/ / •
Figure 3. (a) Number of D atoms absorbed and/or transmitted during permeation and (b) num-
ber of D atoms desorbed from the sample after finishing the permeation procedure.
276
to be introduced into the XPS vacuum system. The sample was then introduced
into a vacuum chamber to measure the D2 partial pressure with a quadruple mass
spectrometer. Variation of the integrated number of deuterium atoms released
during the outgassing in vacuum calculated from the partial pressure is shown as
the solid line in Fig. 3(b). The outgas measurement was started 120 h after finishing
the permeation. Correction for the release into atmosphere before the measurement
have been made by extrapolating the measured variation to time t = 0. The sudden
increase at about 150 h is due to a deliberate elevation of the temperature.
The total amount of deuterium atoms desorbed from the sample, 8.7 x 10 20 ,
corresponds to the composition of PdDrj.24- This does not always mean that the
whole sample did not saturate with deuterium, when we take account of possible
error in the partial pressure measurement. However, the fact that the time necessary
for the release of deuterium was also of the order of 100 h again implies that the
deuterium flow was recombination limited on both surfaces of the sample during
the deuterium permeation.
Figure 4. (a) XPS spectra for the sample before (thin line) and after (thick line) the permeation
process and (b) depth profiles of the Sr (solid circle) and Mo (open circle) densities calculated from
the XPS peak intensities for the sample before (thin) and after (thick) the permeation process.
5. Summary
References
1. Y. Iwamura, M. Sakano and T. Itoh, Jpn. J. Appl. Phys. 4 1 , 4642-4650 (2002).
2. Y. Iwamura, T. Itoh, M. Sakano, S. Kuribayashi, Y. Terada, T. Ishikawa and J. Kasagi,
Proc. ICCF11, Marseilles, France (2004).
3. e.g., The Surface Science Society of Japan (ed.); X-ray Photoelectron Spectroscopy
(Maruzen, Tokyo, 1998).
HIGH-RESOLUTION M A S S S P E C T R U M FOR D E U T E R I U M
( H Y D R O G E N ) GAS P E R M E A T I N G PALLADIUM FILM
Q I N G M. W E I , X I N G Z. LI A N D BIN LIU
Department of Physics, Tsinghua University, Beijing 100084, China
lxz-dmp@tsinghua. edu. en
N. M U E L L E R , P. S C H O C H A N D H. O E H R E
Inficon Limited, LI-9496 Balzers, Principality of Liechtenstein, Yokohoma, Japan
High-resolution mass spectrometer was used to analyze the gas from a deuterium
flux maker. Mass 3 components were analyzed carefully to inspect any anomaly
from the deuterium gas permeating a palladium film. Mass 3 component is con-
firmed again, but more work is needed to separate the signal of the helium-3 (if
any) from the heavy background of D - T molecules.
1. Introduction
More than 100 years have been past since the discovery of the strong absorption rate
of hydrogen in palladium; however, only a little has been revealed about the process
of absorption. An experiment based on Hall effect1 showed that hydrogen molecules
are dissociated and ionized when they are absorbed in palladium. Usually, it was
thought that those hydrogen atoms would be recombined again as molecules when
they permeated through the palladium thin film. Thanks to INFICON, experiment
has been conducted using the high-resolution mass spectrometer in their R&D lab-
oratory. It has been found that only part of the deuterons were recombined into the
deuterium molecules after permeation through the Pd film, most of the deuterons
were combined with the residual hydrogen atoms into D-H molecules, and other
deuterons remain in the atomic status in the vacuum environment. The mass 3
components were carefully analyzed in order to see if there was any trace of helium-3
or tritium.
2. Apparatus
There were two sets of experiments, which were conducted in the INFICON R&D
Laboratory. In one set, the palladium tube was heated by the electrical heater at one
end of palladium tube. The second set utilized the electrical heater surrounding the
palladium film. This paper presents this second set of experiment. A palladium film
(020 x 0.1mm) was sealed in a Swagelok connection as Fig. 1. An electrical heater
was wrapped around the stainless steel nut to heat the Pd film through the nut.
278
279
Swagelok connection
Thermal couple
Heating coil
MkMm 1
D2
Figure 1. A thin palladium film is sealed between two tubes using a Swaglok connection structure.
There are two small holes on the nut. Thermal couples are inserted into holes in order to measure
the temperature at the edge of the Pd film. The heating coil winding is wrapped around the
stainless steel nut to heat the Pd film.
Thermal couples were inserted through the small holes on the nut, and monitored
the temperature at the edge of the Pd film. Deuterium gas was fed from both sides
of the Pd film, and might be evacuated from both sides using the turbo-molecular
pumps (Fig. 2). When the pressure was down to less than 10~ 5 mbar, the system
was connected to a high-resolution quadruple mass spectrometer in order to analyze
the components of the remaining gas. This QMS422 was designed for running in the
second stability zone, which was particularly designed for the operation at low-mass
region. It was able to find the D2 molecules in the heavy background of helium-4.
Even if the ratio of He:D2 is about 99:1, this QMS422 was still able to clearly
distinguish them. 2 For the helium 3, the FWHM resolution of 0.0035 amu and a
10%-peak-height resolution of 0.0065 amu were obtained. 2 Hence, if we were able to
produce any trace of helium-3 in the deuterium flux maker, possibly we might be
able to find them in the QMS analysis.
3. Experiment
One atmosphere deuterium gas was fed into a thin palladium film at 330°C. After
1 h, when the deuterium gas was pumped out, a temperature rising was recorded
which is reported in another presentation. 3 In parallel, the outgoing gas was sent
to a high-resolution quadruple mass spectrometer. Figure 3 shows the results of
the QMS analysis. The first row of Fig. 3 shows the ion currents collected for mass
numbers 1, 2, 3, 4, 5, and 6 in each window. The mass number for each peak is
shown by the abscissa (multiplied by a factor of 100). The original deuterium was of
280
Figure 2. Schematics of the connection between deuterium flux maker (Pd) and the QMS422.
The left-hand side shows the manifold, pumps, and valves, which might feed various gases during
the experiment, and measure the volume of the system.
high purity. The mass 2 and mass 3 components in the original deuterium gas were
relatively low. There was no signal for mass 5, but a little peak for mass 6. It can
be explained as the Longevine effect (i.e. the ion may polarize and dissociate the
neutral molecule; then, combine with one of the resultant atoms 4 ). The high con-
centration of deuterium molecules in the ionization chamber enhanced the reaction
channel: D^ + D2 —> D j + D; which is proportional to the square of the concentra-
tion of deuterium molecules. Thus mass 6 corresponds to the molecular ion D3". Be-
cause the concentration of hydrogen molecules is much lower than that of deuterium
molecules; hence, its Longevine effect for reaction channel, Do*" + H2 —> D 2 H + + H, is
still negligible. That is, the ion current for mass 5 (D2H + ) is much lower than that
of mass 6. The situation changed dramatically, when the gas sample was pumped
from the palladium film. The second row of Fig. 3 shows the result of QMS analysis.
The mass 4 component is much lower than that of mass 2. It means that most of the
deuterons remained in the atomic state (mass 2, D) instead of recombination into
molecules (mass 4, D2). The mass 3 peak was almost as high as mass 2. It might
be explained as the Longevine effect of reaction channel: D + + H2 —> DH + + H. 5 ' 6
This effect is enhanced because of the high density of D-atoms and some hydro-
281
ffjHypftayr....; .*)&£&.
0ri innal Deuterium Gas
(..item JA, , „ „ Ion C m * [A]
'it,y k B
"'#M Ui HAJWF I "-liiiiil v ">'uu4 " uLMNu
,<*'*!*j C» sl> <t? 1st m Q ** ,,-y, 'j t **?,^! i ,^ ,*T.. H JBH'*'»'
'II I , 0.SO000
,...„ |l
22000 1i o.o?ooo
o afisno
20000
006OOO
10000 ; o IMSOII
0 25000^
14000
1 1 & D35O0
D ZUDOO
:
0*1000- ;
00000
w * ;~ O D 05011 - >
VJJk DilfL
Q u n o o D %— , 1
30D 6 3030
4U0O
3000
ZOOO-
Figure 3. Plots of QMS analysis. First row—original deuterium gas; second row—gas sample
permeating through P d film; third row—mass 3 peak in linear scale for gas sample permeating
through Pd film; fourth row—standard helium 3 gas.
282
gen molecules (H 2 ), which was released from the stainless steel parts of Swagelok
connection due to the heating (330°C). However, one might still wonder if there
was any helium-3 or tritium involved in peak of the mass 3. In the third row and
the fourth row of Fig. 3, standard helium-3 sample was used to calibrate the peak
position of mass 3. The logarithmic scale in ordinate was switched to linear scale
in order to clearly show the peak position. The third row shows the mass 3 peak
from the gas sample permeating from the palladium film, and the fourth row shows
the helium-3 peak from the standard helium 3 sample [m(3He) = 3.016], which is
on the left-hand side of the mass 3 peak in the third row. It is clear that the major
part of mass 3 peak in the third row is from the DH + [m(DH) = 3.021] due to the
Longevine effect. The mass 1 peak supports this assumption of residual hydrogen
gas during the heating.
Nevertheless, we might suspect if any helium-3 was covered by the strong HD
peak. In Fig. 4, a careful analysis was done for the strong peak in mass 3. The width
of the slot in front of the Faraday collector in QMS was narrowing down gradually
in order to improve the resolution further at the cost of reducing sensitivity.
E-13-i I, i , i • i , , i
300 301 302 303 304 305
Figure 4. Mass 3 peak was re-analyzed in terms of narrowing slot in Faraday collector. A turning
point appeared near the 3.016 might imply a trace of helium-3 covered by strong HD peak.
283
Acknowledgments
This work is supported by the Natural Science Foundation of China (no. 10475045),
Ministry of Science and Technology (Division of Fundamental Research), and
Tsinghua University (985-11, Basic Research Funds).
References
1. A.H. Verbruggen et al, Phys. Rev. Lett. 52, 1625 (1984).
2. P.H. Dawson, J. Vac. Sci. Technol. 11(6), 1151 (1974).
3. B. Liu, X.Z. Li et al, in: A. Takahashi, Y. Iwamura, and K. Ota (eds), Proc. ICCF-12,
Yokohama, Japan (Nov. 27-Dec. 2, 2005).
4. P. Langevin, Ann. Chem. Phys. 5, 245 (1905).
5. X.Z. Li, G. L. Schmidt and J. Tian, The Proceedings of the 5th Asti Workshop on
Anomalies in Hydrogen/Deuterium Loaded Metals, Asti, Italy (19-21 March 2004).
6. Q.M. Wei, X.Z. Li et al, in: J.-P. Biberian (ed.), Proc. Iccf-11, Marseilles, France
(31 Oct.-5 Nov. 2006, 2004), p. 351.
ICP MS ANALYSIS OF ELECTRODES A N D ELECTROLYTES
A F T E R H N 0 3 / H 2 0 ELECTROLYSIS
S. T A N I G U C H I , S. S H I M A D U , H. Y A M A D A A N D S. N A R I T A
Department of Electrical and Electronic Engineering, Iwate University, Ueda If-3-5,
Morioka 020-8551, Japan
E-mail: t5304007@iwate-u.ac.jp
T . O D A S H I M A A N D N. T E S H I M A
Department of Chemical Engineering, Ichinoseki National College of Technology, Hagiso,
Takanashi, Ichinoseki 021-8511, Japan
T. O H M O R I
Advanced Technology Inc., Hokkaido Institute Technology, Maeda 7-15, Teineku,
Sapporo 006-8585, Japan
We carried out light water electrolysis with Pd cathode and Pt anode. The compo-
sition of both electrodes and the electrolytes were analyzed by Inductively Coupled
Plasma-Mass Spectrometry to search for the evidence of the nuclear transmutation.
In the light water electrolysis experiment, various elements have been observed on
the metallic electrodes and in the solution after the electrolysis. In particular,
amount of P b increased remarkably after the electrolysis, and this result gave
good reproducibility. There was no difference between the isotopic ratio of P b
detected and natural one
1. Introduction
In light water electrolysis experiments, elements production has been reported. 1 In
most of them, only the surface compositions of the electrodes were analyzed. In
addition to analysis of the electrodes, it is desirable to investigate electrolytes since
elements on/in the electrodes can be dissolved in it. In this study, both solutions
of electrodes and electrolyte were analyzed by Inductively Coupled Plasma-Mass
Spectrometry (ICP-MS)(SII : SPQ9000). The sample solution introduced into the
ICP MS should be acid in general. Then, we utilized HNO3/H2O as electrolytic
solution instead of Na2S04/H 2 0 or K2SO4/H2O, that we previously used in our
experiment so that the electrolytes can be directly introduced into the device.
2. Experimental
We employed a PTEF test cell in this study. The cell is shown in Fig. 1. The
cell was 73 mm in diameter, 175 mm of height, and cylindrical shape with volume
capacity of 500 ml. The Pd foil (99.95% pure) for cathode was 0.1 x 5x10 mm 3 in
284
285
size and the Pt foil (99.98% pure) for anode was 0.1 x 5 x 10 mm 3 in size. The
gap was about 3 cm. A Pd lead wire (4>1 mm) and a Pt lead wire (<j>l mm) were
used for connecting cathode and anode to a power supply, respectively. They were
coated with Teflon heat-shrinkable tubes. Before the electrolysis, the electrodes
were washed with acetone and aqua-regia to remove the impurity. The electrolytes
used were ultrapure nitric acid (Ultrapure reagent, Kanto kagaku, Tokyo, Japan).
The volume of electrolyte solution was 500 ml.
J DC 2 or 1 A
Pt
(i|>1 mm)
Pd
(<|>1 mm)
, Cathode ^ Anode
Pd 3 cm
(0.1 x5x10mm)
< Pt
to 1 x5x10mm)
(a) (b)
Figure 1. P T F E cell.
2
Amount dissolved (mg) 0.04 0.01 0.56 0.49
Depth (nm) 19.0 4.7 5.0 X 10 2 4.0 X 10 2
1
Amount dissolved (mg) 0.02 0.02 0.20 0.02
Depth (nm) 9.4 9.4 2.0 x 10 2 16.4
To estimate the depth of samples dissolved in the nitric acid, we compared the
weight of samples before the pre-processing with that after the pre-processing. The
depth was calculated using the density of the electrodes, 21.37g/cm 3 for Pt and
12.16g/cm 3 for Pd. Table 1 shows the amount dissolved and the depth of Pt and
Pd electrodes in HNO3.
After treatment by the nitric acid, the dissolved amount for both "Before sam-
ples" of Pt and Pd is large than that for "After samples" under the test condition of
current 2 A. In case of current 2 A for Pd sample, the dissolved amount 0.56 mg of
"Before sample" and that 0.49 mg of "After sample" correspond to dissolved depth
5.0 x 102 and 4.0 x 102 nm, respectively. This indicates that amount of impurity
from "After sample" of Pd should be less than that of "Before sample" of Pd. Under
the same test condition of 2 A for Pt, similar result can be deduced from comparing
weight of "Before sample" with that of "After sample".
Pb
2 — — — 9.1406 — 6.401
1 — 2.7842 — 6.7815 — 14.1592
287
8.0
• 2A
6.0
5 4.0 -
2.0
0.0
Pt Electrolyte
(Anode)
ICP-MS. It should be noticed that the change in weight of "Before sample" was
larger than that of "After sample" for both Pt and Pd electrode, as mentioned
above.
From these results, it is unlikely that those Pb was impurity originating from
bulk Pd and Pt electrodes. Since the volume of electrolyte is 10 times larger than
that of the thin acid solution, the amount of Pb in the electrolyte is larger than these
on electrodes. On the other hand, the density of Pb in air environment is generally
thought to be 0.6 ng/m 3 . 4 Taking account of this low value, the Pb detected in
this experiment is not considered to be impurities from the air environment. The
deduced amount of Pb from the density values in Table 2, on both electrodes and
in the electrolyte, is given in Fig. 2.
Pt Pd Electrolyte
(Anode) (Cathode)
Figure 3. Isotope distribution of P b in the thin nitric acid solutions and electrolytes.
4. Conclusion
References
1. J. Dash, R. Kopecek, and S. Miguet, The 32nd intersociety energy conversion engineer-
ing conference, vol. 2, pp. 1350-1355 (1997).
2. H. Yamada, S. Narita, Y. Fujii, T. Sato, S. Sasaki, and T. Omori, Proc. 9th Interna-
tional Conference on Cold Fusion, pp. 420-423 (2003).
3. T. Sato, S. Sasaki, T. Kubozono, S. Narita, H. Yamada, and T. Ohmori, Proc. J^th
Meeting of Japan CF Research Society (October 17-18, 2002), pp. 9-12.
4. The periodic table of the elements, http://home.hiroshima-u.ac.jp/er/
Rmin_GL.html#anchor646130
THE ITALY-JAPAN PROJECT FUNDAMENTAL RESEARCH ON
COLD T R A N S M U T A T I O N P R O C E S S FOR T R E A T M E N T OF
NUCLEAR WASTES
AKITO TAKAHASHI
Osaka University, 2-2 Yamadaoka Suita, Osaka 565-0871, Japan
E-mail: akito@sutv.zaq.ne.jp
FRANCESCO CELANI
INFN, Via Enrico Fermi, 40-00044 Frascati (Rome), Italy
YASUHIRO IWAMURA
Mitsubishi Heavy Industries Ltd., 16-5, Konan 2-chome, Minato-ku Tokyo 108-8215,
Japan
The IJ Project proposes, as the first phase of research, that confirmation of the
cold transmutation using radioactive isotopes such as 1 3 7 C s , 9 0 Sr, and 1 3 6 Cs
to non-radioactive elements will be implemented based on the Mitsubishi Heavy
Industries, Ltd. (MHI) method. A theoretical background has been given by the
TSC-induced nuclear reactions (Proc. ICCF 10). Charge-neutral pseudo-particle
of 4d/TSC can become as small as 10 fm radius in its minimum state of squeezing
motion, and will make 4D-capture reaction with host metal (or added metal) nuclei
in the surface region of permeation {Proc. ICCF 9, 10) samples. Major reaction
will be:
M(A, Z) + 4 d / T S C - • M(A + 8, Z + 4) + Q.
Theoretical modeling of the process is briefly explained and resulting reaction
products, their decays and final stable isotopes are predicted for 1 3 7 Cs, 9 0 Sr, and
135
Cs transmutation.
1. Introduction
Recent studies on condensed matter nuclear effects in/on near surface regions of
metal deuterides and hydrides have provided some confident experimental results
about occurrence of cold transmutations in condensed matter containing deuterium
and hydrogen. 1_3 Especially the latest works by Iwamura et al.4'5 are novel enough
to be considered important new findings in condensed matter nuclear effects.
Iwamura et al. have repeatedly shown that there occurs selective transmutation
from 133 Cs to 1 4 1 Pr (or 88 Sr to 96 Mo) in the experimental system of D-gas per-
meation through Pd-complex samples. Pd-complex samples are made with multi-
layered P d / C a O / P d plates in nm size processing.
The IJ-Project aims at confirming the selective transmutation process by using
special samples containing radioactive Cs and Sr. This is a pure basic science
project.
289
290
2. Selective Transmutation
This new type of transmutation is the process of adding 4D or 8 Be to the host ele-
ment M(A, Z) and to transmute to M'(A+8, Z+A). Therefore, some kind of coher-
ent multi-body process in condensed matter should exist as the underlying physics
mechanism. One theoretical interpretation has been proposed by Takahashi. 6
A theoretical background has been given by the TSC-induced nuclear reactions. 3
Charge-neutral pseudo-particle of 4d/TSC can become as small as 10 fm radius in
its minimum state of squeezing motion and will make 4D-capture reaction with host
metal (or added metal) nuclei in the surface region of permeation 1,2 samples. The
major reaction will be:
M(A, Z) + 4d/TSC - • M{A + 8, Z + 4) + Q. (1)
Iwamura et al. has also reported that 6D added transmutation. Takahashi 6
7
Image of surface
Dimer •
/ W w W W « U
/o o _o^o o! W
• - >
Adatom
o• o • • °„ •o
o • *^
o*>«-
O A Corner-hole
with
dangling-bonds
° o° °2W
TSC is born
here?
o Pd
. ^BF
O
CaO Cs Deuteron
137
Cs- 4d/TSC -^ 1 4 5 Pr(Ex = 45.63MeV) - • Fission - Products (in 10fs) or
145 145
Pr(5.98 h) Nd(stable) + gammas (in few fs). (3)
During the beta-decay of 1 4 5 Pr with 5.98 h half-life, there should be a small
fraction (1%) of gamma-rays at £ 7 = 675.8 and 748.28 keV, which we can detect
with HpGe detector to identify the occurrence of reaction (3).
135
Cs + 4d/TSC ^ 1 4 3 Pr(Ex = 48.03 MeV) - • Fission-Products (in f 0 fs) or
143
Pr(f 3.57days) 143 Nd + gamma (in few fs), (4)
90
Sr + 4d/TSC ^ 9 S Mo(Ex = 54.71 MeV) -> Fission-Products (in 10 fs) or
98
Mo(stable) + gammas (in few fs). (5)
For all cases, fission channels may be opened due to very high-excited energies
of intermediate compound nuclei. However, we predict gamma transitions will be
more dominant than fission, due to shorter transition times (few fs) than about
10 fs life for fission break up by collective deformation of excited nuclei (dumbbell
oscillation).
Gamma-transition from highly excited states may emit very high-energy gamma
quanta in about 50 MeV range. To detect and identify these very high-energy
gamma-rays is difficult and money consuming effort is needed, because the process
for detection is mostly by Compton scattering and we do not have definite method
292
M-nucleus
Figure 2. Strong interaction (PEF) between TSC-minimum-size and host-metal M-nucleus. The
admixture of 4d/TSC forms 8 Be* compound state for short time.
for unfolding broadened pulse height spectra of observation with usual detectors
(Nal, Ge, etc.).
5. C o n c l u s i o n s
References
1. Proc. ICCF9, Tsinhua University Press (see also; http://www.lenr-canr-org/).
2. Proc. ICCF10, Boston (2003) to be published (see also the above site).
3. Proc. ICCF11, Marseilles (2004) to be published (see also the above site and
http://www.iscmns.org/).
4. Y. Iwamura et al, Jpn. J. Appl. Phys. 4 1 , 4642 (2002).
5. Y. Iwamura et al., Proc. ICCF10, Boston (2003).
6. A. Takahashi, TSC-induced nuclear reactions and cold transmutations, Proc. Siena
Workshop, http://www.iscmns.org/ (2005).
7. A. Takahashi, Recent Res. Dev. Phys. 6, 1-28 (2005).
R E P R O D U C I B L E N U C L E A R EMISSIONS FROM Pd/PdOiDa:
H E T E R O S T R U C T U R E D U R I N G CONTROLLED E X O T H E R M I C
DEUTERIUM DESORPTION
A . G . L I P S O N A N D G.H. M I L E Y
University of Illinois at Urbana- Champaign, Department of Nuclear, Plasma and
Radiological Engineering, Urbana, IL 61801, USA
E-mail: lipson@uiuc.edu
A.S. R O U S S E T S K I
P.N. Lebedev Physics Institute, Russian Academy of Sciences, Moscow 119285, Russia
A . G . L I P S O N , B . F . L Y A K H O V A N D E.I. S A U N I N
Institute of Physical Chemistry, Russian Academy of Sciences, Moscow 199991, Russia
1. Introduction
Weak nuclear emissions accompanied deuterium loading/deloading into Ti and Pd
matrix have been studied for more than a dozen years. 1 ' 2 It was found that in
some cases neutrons and charged particles (protons and tritons) are observed in
Pd cathodes during electrolysis, glow discharge bombardment and deuterium des-
orption from these samples. The rate of those emissions considering as a signature
of low-energy DD-reaction is very low and still unpredictable. This indicates low
reproducibility of low-energy DD-reaction in deuterium-loaded metals and makes
doubtful existence of entire low-energy nuclear processes in non-equilibrium solids.
Moreover, the existence of nuclear processes of any type in D-loaded Pd requires
observation of X-rays accompanying charged particles braking in solids. So far,
there were no unambiguous reports concerning X-ray generation from PdDa; during
and after electrochemical loading with deuterium.
Meanwhile, earlier we just have reported observation of 2.45 MeV neutrons and
high-energy alpha particles during exothermic deuterium desorption from specially
293
294
prepared Pd/PdOiDz heterostructure. 3 ' 4 It was also shown that Pd/PdO samples
demonstrate highest screening potential and highest deuterium diffusivity (com-
pared to other metals including pure Pd) in experiments on 2.5-10 keV deuteron
bombardment with accelerator. 5 ' 6 These facts allow to assume that Pd/PdO:Da;
heterostructure samples could serve as a good candidate to achieve reproducible
LENR effects in exothermic deuterium desorption process, including both nuclear
and X-ray emissions. Thus, to verify our assumption concerning unique nuclear
properties of Pd/PdO:Da; system during D-desorption the objectives of this research
were directed to:
• Obtain reproducible nuclear emissions in controlled conditions of exother-
mic D-desorption from PdO/Pd/PdOiDrr heterostructure.
• DD-reaction yield (3.0 MeV protons).
• Energetic alphas.
• Soft X-rays.
• Control of sample temperature and D-desorption rate on-line.
• To figure out how these emissions could be linked via D-desorption.
In the present paper, we show new reproducible results on DD-reaction products,
energetic alpha particles and soft X-ray emissions detected in controlled conditions of
exothermic deuterium desorption from the surface of Pd/PdChDa, heterostructure.
2. E x p e r i m e n t a l
The samples of Pd/PdO were synthesized by thermal growing of thin oxide layer
(PdO y ) of 20 nm thick on top of 110 ^m thick annealed cold worked Pd foils
(area 2.3 x 1.1cm2) using an oxygen-propane torch. The electrochemical loading of
Pd/PdO cathodes by x = D/Pd = 0.7 has been carried out with low current density
(j ~ 20mA/cm ) electrolysis in lM-LiOD/D20 solution using a special cell with
divided cathode and anodic spaces. Immediately after achieving an x = 0.7 load-
ing ratio, the electrolysis was interrupted. The Pd/PdOiDa, sample with attached
CR-39 or thermal luminescent (TLD) detectors is placed under mechanical load-
ing (m = 150 g) for one hour at T = 20°C. During this time the Pd/PdOiDz
sample showed signs of heating up to 7.0°C caused by exothermic deuterium des-
orption. Loading ratio x = D/Pd has been measured using both thermal desorption
and anodic polarization techniques. 2 In order to determine x = D/Pd value, the
sample was underwent by vacuum heating or anodic polarization after each cath-
ode loading time interval t. About 90% of initial deuterium content was found
to be desorbed through Pd-PdO interface during t = 1.0 h. In control experi-
ments a similar Pd/PdO sample electrochemically loaded with hydrogen in 1-M
NaOH/H 2 0 electrolyte and exposed to CR-39 detectors has been employed. In
blank/background experiments, unloaded Pd/PdO heterostructure samples were
used with CR-39.Both open and filtered CR-39 track detectors have been applied
in our experiments in order to estimate type and energy distributions of emitted
295
particles. The photo-insensitive X8 LiF TLD (Landauer) units used for soft X-ray
detection were filtered by 1-4 layers of 15 /im polypropylene.
3. Experimental Results
Kinetics of integral deuterium desorption from Pd/PdO:Da; and its rate for first 70
min after exposure are shown in Fig. la and b, respectively. As seen, the desorption
rate demonstrate maximum near t — 10-15 min elapsed after the loading interrup-
tion. It was also found that about 90% of all deuterium absorbed by P d / P d O
sample leaves heterostructure during 60 min of its exposure at room temperature.
During D-desorption the ambient temperature and temperature of the sample
were measured simultaneously using to independent thermocouples. It was found
that from the start of exposure in air atmosphere (immediately after interruption
of loading and drying the sample) the temperature of Pd/PdO:Dir sample jumps
five degrees above the ambient one (Fig. 2). The temperature of the sample has
tend to increase two degrees more during following 20 min and then exponentially
decreases with decrease in loading ratio x = D/Pd and (Fig. la) and desorption
rate (Fig. lb). Notice that shape of the Pd/PdO:D:r T(t) (Fig. 2) curve is roughly
repeat the shape of desorption rate curve (Fig. lb). The coincidence of T(i) and
desorption rate curves give rise to conclusion that observed heating of the sample
is referred to exothermic deuterium desorption from the surface of Pd/PdO:Da;
heterostructure in air (oxygen) atmosphere. In this condition the PdO surface may
catalyze exothermic D + D —> D2 +Q moleculization reaction at room temperature.
Pd/PdO:Dj; runs with CR-39 detectors showed a highly reproducible yield of
3 MeV protons from DD-reaction accompanied by energetic alpha emission in the
range of 11-16 MeV. These emissions are not detected in the blank experiments
with unloaded Pd/PdO heterostructure. Integral charged particle spectra obtained
with open CR-39 detectors (without filter) during 12 runs with duration ~ 1 h
0,025
& 0,020
• x=D/Pd measurement
Exponential fit 1 • I •/ I
' 0,015 . \ 1 Ii \
3 '
" 0 3 § 0,010
D. i \ •
° 0,005
o
I—J 1 • ^
0,0- 0,000 4.1. i — > — i — i — i — i — i — i —
10 20 30 40 50 60 70 80 10 20 30 40 50 60 70
Elapsed time (min) Elapsed time (min)
(a) (b)
Fig. 1. Integral deuterium desorption (a) and desorption rate (b) from 110 (an P d / P d O i D x
heterostructure electrochemically loaded with deuterium versus elapsed time at T = 18°C. Notice
that ~ 90% of absorbed deuterium escapes the sample during 1 h of its exposure.
296
OA m
0*3 •
c.O "
y •s
/i • Sample temperature
9
3
2?-
•
s —•—Room temperature
|<«. 0
on.
£ 1Q .
1Q , 11
IO '
17,
I / "
L,_^ , ,_ .
0 10 20 30 40 50 60 70 80
Elapsed time (min)
Fig. 2. P d / P d O : D i and ambient temperatures vs. elapsed time: Notice that maximal tempera-
ture at the surface is ~ 7°C higher than ambient one.
7 8 9 10 11
Track diameter (urn)
Fig. 3. Foreground and background counts from P d / P d O : D x and P d / P d O , respectively: open
CR-39 detector. Pay attention to high foreground/background ratio, especially below d = 8/im.
297
and alpha beams 3 ' 4 the maximum near d = 5 fim belongs to 3 MeV protons; the
group of counts near d = 6.2 fim can be ascribed to lower energy protons/deuterons
( £ , / E d ~ 1.7/2.8 MeV) and counts around d = 7.2 fim were associated with high-
energy alphas in the range of 11-16 MeV.
In order to confirm our assumption concerning presence of 3 MeV protons
as DD-reaction signature we compared open CR-39 spectra for Pd/PdO:Drr and
Pd/PdO:Ha; samples (Fig. 4).
As seen from Fig. 4, the spectra of Pd/PdO:D.Tand Pd/PdO:Ha;look similar with
only one exclusion: there are no counts at d < 6 /an have been found for Pd/PdO:Hx
heterostructure. Thus, the group of counts associated with 5 fim peak belongs only
to deuterated P d / P d O sample. This peculiarity confirms our assumption concerning
emission of 3 MeV protons (DD-reaction signature) in Pd/PdO:Da; heterostructure.
On the other hand, the groups of counts around 6.2 and 7-2 fim are appeared in
both Pd/PdO:Dz and Pd/PdO:Ha; samples . This fact does not contradict to our
earlier data showing presence of energetic alpha and proton/deuteron emissions
independently on hydrogen or deuterium loading in Pd/PdO.
50-
[Pd/PdO:Dx-Pd/PdO], open CR-39
40-
(Pd/PdO:Hx-Pd/PdO], open CR-39
.•e 3 0 -
A4>
10 11
Track diameter (urn)
Dv jllLrji
5 6 7 8 9 10 11
Track diameter (um)
Al foil is in good agreement with 3.0 MeV proton stopping range in Al. The splitting
of 7.2 /an maximum in open detector to 7.3 and 8.0 [im bands indicates appearance
of two groups of alphas with the energies ranging near 12 and 14-16 MeV. This
result is in agreement with our earlier data on energetic alpha emissions obtained
for Pd:D(H) and Ti:D(H) foils.3-4
Presence of 1.7 MeV protons per 2.8 MeV deuterons in charged particle spectra
of Pd/PdO:Ha; and Pd/PdO:Da; is supported by experiments with 11 /tm Al filtered
CR-39 (Fig. 6).
Shift of 6 /mi track band (open detector, see Fig. 4) to 6.4-6.6 /<m after appli-
cation of 11 /im Al foil for Pd/PdO:H(D)a; is consistent with emission of 1.6 ± 0.2
MeV protons (Pd/PdO:Hx) and/or 2.8 ±0.4 MeV deuterons (Pd/PdO:Dx).
The other example of charged particle filtering with 25 urn Cu foil for both
Pd/PdO:Dz and Pd/PdO:Hz samples is shown in Fig. 7:
As seen from Fig. 6 the 3.0 MeV proton band in Pd/PdO:D.T shifts further
compared to the run with 44 /an Al filter to diameter ranging d = 6.2-6.6 /mi.
This shift is expected accordingly to stopping range of 3.0 MeV protons in copper.
Notice that no counts were detected in this range for Pd/PdO:H.T sample. The
shifts and amplitudes of alpha particle spectra for both H and D-loaded Pd/PdO
samples look similar and indicate presence of the same groups of alphas with energies
11-12 MeV (9.2-9.8 um band) and 14-16 MeV(7.4-7.6 /tm band) as were detected
in experiment with 44 um Al filter.
The shift of 5.0 um proton band (open CR-39) with respect to thickness of Al
and Cu filters is shown in Fig. 7.
299
Pd/PdO:Hx, CR-39/11um A
30- Pd/PdO:Dx, CR-39/11umA
7 25-
E
o
20-
| 15H
I 1(H
o 5-
ra
lijin
0
6 7 8 9 10 ' 11 '1
-5^
Track diameter (um)
Fig. 6. CR-39 charged particle spectra of P d / P d O : D z and P d / P d O : H i samples filtered with
11 )im Al foil.
This picture finally show that band of d = 5.0/zm detected by open CR-39
corresponds to protons of 3.0 ± 0.3 MeV initial energy emitted from near-surface
layer of Pd/PdO:D.T. Estimated energies after passing the metal filters are consistent
with the stopping power of these Al and Cu filters resulting in shift of d = 5 /an peak
(open CR-39) to larger diameters. At the same time we did not find any direct sign
of energetic triton (E ~ 1 MeV) emission in Pd/PdO:Da; that could be considered
as an additional signature of d(d,p)t reaction. The absence of energetic tritons
indicates that effective depth beneath the PdO:Dx surface where DD-reaction occurs
would be h < 2.0/an. At depth h — 2.0/<m the effective energy losses of 1 MeV
triton in Pd is estimated as A.E ~ 0.6 MeV resulting in very low initial energy
30
[Pd/PdO:DX-Pd/PdO], CR-39/25 (im Cu
25 [Pd/PdO:HX-Pd/PdO], CR-39/25 (im Cu
1 20
f 15
10
I 5
Fig. 7. Charged particle spectra for P d / P d O : D z and P d / P d O : H i filtered with 25 (im Cu (with
background subtraction). Alpha particle spectra of both H and D-loaded samples look similar.
300
of triton bombarding CR-39 surface {Et = 0.4 MeV). The stopping range of this
triton in CR-39 material is too small (several microns) compared to etched layer
of detector at etching time t = 7 h (9.1 um). As a result we cannot detect triton
tracks at this effective depth of DD-reaction. At the same time at h — 2.0 /zm in
Pd/PdO:D.T the proton energy would be Ep ~ 2.85 MeV that is consistent with our
estimate shown in Fig. 8. This explanation makes us still convinced in DD-reaction,
which is occurred in Pd/PdO:D.T heterostracture at some effective depth.
Thus, exothermic deuterium desorption from Pd/PdO:D.i-heteiostructure causes
a reproducible yield of DD-reaction from near-surface layer with depth ~ 2 /im.
Taking into account detection efficiency e = 1/2(1 —cos0 C ), where 0 C is the critical
angle for 3 MeV protons (32-37°, Ref. 7) we obtain this yield as Yp(DD) = (1.15±
0.13) x 1 0 - 2 p/s-cm 2 . The yield of 3 MeV proton is by order of magnitude in
agreement with 2.45 MeV neutron yield obtained with NE-213 detector pair for
similar samples during D-desorption: Yn(DD) = (1.8 ±0.19) x 1 0 - 2 n/s-sample. 2
Notice that calculated mean D-desorption rate from Pd/PdO:D.i; surface (Fig. 1) or
deuteron current (D+) from the sample is found to be {AN/At) = 20 niA/cm . The
DD-reaction yield in that case was Y(DD) = 0.5p/C(D). This result suggests very
high screening potential Ue > 1.0 keV in Pd/PdO:Da; that exceeds the value of Ue
deduced for PdO from accelerator experiment. 6
The process of exothermic deuterium/hydrogen desorption is also responsible
for triggering of energetic alpha (11 16 MeV) and 1.6 MeV proton emissions in
Pd/PdO:D(H).x- heteiostructure cathodes. This finding only confirms our previous
CR-39-open
CR-39 + 11 umAI
CR-39 + 44 um Al
3.0± 0.3 MeV CR-39 + 25 umCu
50-
1.85± 0.35 MeV
40-
10-
!•••••••*
5,0 5,5 6,0
M6,5 7,0
Track diameter (um)
Fig. 8. Proton band position versus CR-39 filter thickness and quality.
301
1
>~ : •: : s : ;
1%, 0 , 8 -
c" 0,6 - -j-
o
8 0,4-
11
c 0,2-
<0 1rv^^
_£
•" 0,0-
-0,2- 1 i i 1 1 1
10 20 30 40 50 60
PPE filter thickness, h (|im)
Fig. 9. Transmission of polypropylene filters (a = Ih/Io, where 1^ is the X-ray dose in TLD
filtered with P P E of h /an thick and IQ is the X-ray dose in an open TLD at h = 0) versus
thickness of P P E filter.
302
during exothermic D-desorption (Fig. 9). The fit of transmission curve showed
mass-absorption coefficient /i(PPE) = 893 c m - 1 , corresponding to mean energy of
X-ray quanta (Ex) = 1.30 ± 0.15 keV.
The open TLD showed dose D = 12 ± 2 mrad = 120 /uGy with background
subtracted (£>(Fg) = 21.0 ± 1.0mrad, D(Bg) = 9.0 ± 1.0mrad). In SI sys-
tem the equation connecting the dose Dx (Gy) absorbed by LiF TLD with area
s = 0.04 cm2 and mean flux ($>x) would be written as follows:8
(*„,) = 2 D a ; p ( L i F ) / 1 . 6 x l O - 1 3 ( J / M e V ) x J E ; ; E X / i m x ( s / l c m 2 ) T
^ (8 ± 2)X - quanta/cm 2 - s,
where /a(LiF) is the density of LiF, Ex = 1.3 keV is the X-ray quanta energy and
r = 7 x 105 s is the total time of TLD exposure with Pd/PdO:Da; sample;
/um(1.3keV) = 7 x 10 5 cm 2 /g is the LiF mass-absorption coefficient for 1.3 keV
quanta obtained by extrapolation of known data in the range of 4-10 keV to lower
energies.8
Note that estimated dose obtained from the charged particle absorption by LiF
TLD (i.e., emitted from the surface of Pd/PdO:Da;) would be less than 1 mrad
(below detection limit).
Thus, here we first detected soft X-ray emission accompanying the exothermic
deuterium desorption from the Pd/PdO:D:r heterostructure cathode alongside with
charged particles and estimated energy of those X-ray quanta.
4. Conclusions
Thus in this research the following new results have been achieved.
• Good reproducibility of charged particle emissions during controlled
exothermic D-desorption from Pd/PdO:Da;.
• Relatively high 3 MeV proton yield indicating large DD-reaction enhance-
ment during D-desorption.
• No direct sign of 1 MeV tritons: means that effective depth where DD-
reaction originates is ~2 /an from the surface. This estimate is in good
agreement with energy losses for 3 MeV protons
• Identity between energetic alphas spectra resulting of D and H-desorption
from Pd/PdO.
• The energy of X-ray quanta emitted from Pd/PdO:Da; is in good agreement
with Karabut's glow discharge results. 4 This suggests similar mechanism of
X-ray emission caused by D-desorption.
• Phonon energy of D-desorption focusing or/and concentration in some spe-
cific lattice sites near surface (the sites of a high internal strain?).
• DD-reaction, energetic alphas and X-ray emissions suggest anomalous
energy release via the "active" lattice sites of non-equilibrium metal
deuterides.
303
References
1. S.E. Jones et al, in ICCF 10 Proc, Boston, MA, 24-30 August. 2003
2. A.G. Lipson et al, Fusion Tech. 38, 257 (2000).
3. A.G. Lipson et al, in ICCF 10 Proc, Boston, MA, 24-30 August, 2003.
4. A.G. Lipson et al., JETP 100, 1175 (2005).
5. H. Yuki et al, JETP Lett. 68(11) , 785 (1998).
6. J. Kasagi et al, J. Phys. Soc. Jpn. 71(12), 2881-2885 (2002).
7. B. Dorschel et al., Rad. Measurements 3 1 , 103 (1999).
8. H. Cember, Introduction to Health Physics, 2nd ed., Pergamon Press, New York, 1985.
C O R R E C T IDENTIFICATION OF E N E R G E T I C A L P H A A N D
P R O T O N T R A C K S I N E X P E R I M E N T S O N CR-39 C H A R G E D
PARTICLE D E T E C T I O N D U R I N G H Y D R O G E N D E S O R P T I O N
FROM Pd/PdOtHa H E T E R O S T R U C T U R E
A.S. R O U S S E T S K I
P.N. Lebedev Physical Institute, Russian Academy of Sciences, Moscow, 119991 Russia
E-mail rusets@x4u.lebedev.ru
A.G. L I P S O N
Department of Nuclear, Plasma and Radiological Engineering, University of Illinois,
Urbana, IL 61801, USA; Institute of Physical Chemistry, Russian Academy of Sciences,
Moscow 117915, Russia
B . F . L Y A K H O V A N D E.I. S A U N I N
Institute of Physical Chemistry, Russian Academy of Sciences, Moscow 117915, Russia
Results of correct identification of energetic alpha and proton tracks, observed after
hydrogen desorption from P d / P d O : ! ! ^ samples, are presented. Using CR-39 plastic
track detector we unambiguously identified tracks of as minimum two groups of
alpha particles with energies 10—13 and 15—17.5 MeV. It was also confirmed the
emission of protons with energies ~1.7—1.9 MeV.
1. Introduction
Earlier experiments 1 ' 2 have showed emissions of energetic charged particles
(a-particles and protons) during exothermic H desorption from the Pd/PdOiH^
heterostructures. The occurrence of these emissions was confirmed by independent
experiments using both Si-surface barrier and CR-39 plastic track detectors. Earlier
we already showed that purified CR-39 plastic track detectors can be considered as
an adequate scientific instrument, which suitable for detection of individual uni-
formly distributed charged particles and also for the groups of these particles being
emitted from the active spots ("hot zones") attributed to the maximum internal
strain area at the surface of Pd/Ti:D samples. The analysis of CR-39 data showed
that in some cases energetic charged particle tracks (a-particles and protons) con-
centrated inside the small spots of detector. The typical "hot zone" with <~102
tracks within the area with the size of 0.25 x 0.5 mm 2 were found to be appeared
during the hydrogen desorption experiments with Pd/PdOrH-,; samples.2
In present work we demonstrate the advance of track detection technique
allowing perform an unambiguous identification of CR-39 tracks in order to obtain
304
305
full information about type and energy of detected particles as well as to distinguish
them from usual background events and surface defects
2. Experimental Technique
Track parameters (coordinates and diameters) measurements have been carried
out with automated microscope facility (PAVICOM).2-3 In order to obtain correct
particle identification, in-depth track etching and comparison of their parameters
(including diameters and etching rates) with those for calibration tracks (obtained
with accelerator alpha and proton bombardment of CR-39) have been performed.
The detectors were etched in 6N solution of NaOH at 70°C, during the time inter-
vals corresponded to 7, 14, 21, 28, and 35 h. After the etching during every specific
time interval, the diameters were measured for each individually selected track.
Thus, the measurements of parameters for individual tracks in the "hot zone" and
calibration detectors were carried out after each 7 h of etching. Using the results
of these measurements we plotted the functions of track opening diameter versus
etching time and the rate of etching inside the track versus removed layer depth. 4
The results of calibration (the dependence of track diameter from etching time) for
a-particles and protons are presented in Figs. 1 and 2, respectively.
In this experiment, we used the sample of Pd/PdOtH^ heterostructure with the
thickness of 50 ^m that was loaded by hydrogen during electrolysis in solution 1M
Li2S04/H20 during 20 min (current density j = 10 mA/cm 2 ).
After electrolysis, the sample was attached to the CR-39 detector with shielding
of 11 fj,ra of Al. After ~ 1 h of exposition, the sample was repeatedly loaded by hy-
drogen during electrolysis. Then the cycle of measurements was repeated 10 times.
Total time of exposition was 14 h.
Figure 1. Calibration dependence of track diameter of alpha-particles versus etching time with
their logarithmic approximation.
306
13,5
13,0
12,5-]
12,0-1
11,5
11,(H
10,5
10,0-1
9,5
9,0-1
8,5
8,0
7,5
7,0-1
6,5
6,0
5,5
5,0
4,5
10 15 20 25 30 35
Etching time (h)
Figure 2. Calibration dependence of track diameter of protons versus etching time with their
linear approximation.
Figure 3. Photomicrographs of tracks in "hot zone" with dimensions of 250x500 |im 2 . Image
size~120x90 /im 2 .
307
ۥ
4**-
(a) (b)
I (c)
lb* k
*r^ I
•%& & 3r
(d) (e)
Figure 4. Etch dynamic of spot with coordinates [-71, -1972] at etching time (a) 7 h, (b) 14 h,
(c) 21 h, (d) 28 h, and (e) 35 h.
close to normal and we can to compare them with calibration tracks. Track 1 looks
like proton candidate.
The comparison of track etch dynamic of track 1 from Fig. 4 with that for 1 and
1.5 MeV calibration protons is shown in Fig. 5.
Figure 6 demonstrates the comparison of functions track diameter versus etching
time for track 1 with one of 1 and 1.5 MeV calibration protons. The dependence of
track diameter from etching time for protons was found to be linear. According to
our estimation track 1 belongs to proton with energy 1.35 MeV.
Pictures in Fig. 7 demonstrates etch dynamic of another spot with coordinates
[-116,-1621]. We choose track 1 as alpha particle candidate. The comparison of
1 MeV proton
Figure 5. Comparison of track etch dynamic of track 1 from Fig. 4 with that of 1 and 1.5 MeV
proton calibration tracks. Etching time: 7, 14, 21, 28 and 35 h from left to right.
308
# 1 MeV proton
• 1.5 MeV
proton
-Linear (1 MeV
proton)
-Linear (1.5
MeV proton)
Linear (#1 [-
10 20
71,-1972])
Etch time (h)
Figure 6. Comparison of function track diameter versus etching time for track 1 from spot [-71,-
1972] with one of 1 and 1.5 MeV calibration protons.
track etch dynamic of track 1 with one of 11 and 12.8 MeV alpha particle calibration
tracks is shown in Fig. 8.
The comparison of functions track diameter versus etching time for track 1 with
one of 11 and 12.8 MeV calibration alpha-particles are presented in Fig. 9. The
dependence of track diameter from etching time for alpha particles was found to be
logarithmic.
Another important function for track identification is dependence of track etch
rate from removable depth. In simple model of track formation 4?5 track etch rate
Vtj bulk etch rate VJ> connected with track diameter D and removable depth h by
formula:
Vt/V„ = phf - D 2 ]/[(2/i) 2 + D'\.
It*
^
M
K ,
Figure 7. Etch dynamic of spot with coordinates [-116,-1621]. Etching time: 7, 14, 21, 28, and
35 h from left to right.
309
fe.-
# ' - •
12.8 MeV alphas
Trackl [-116,-1621]
Figure 8. Comparison of track etch dynamic of track 1 from Fig. 7 with that of 11 and 12.8 MeV
alpha calibration tracks. Etching time: 7, 14, 21, 28 and 35 h from left to right.
Here h = Vbtj where t is the etching time. For our conditions of etching
Vb = 1.3 /xm/h.
25 Alphas £=11
MeV
s,9?43
20 Alphas £=12.8
2
R ^ 0,9508 MeV
15 Track #1
[-116-1621]
10 Log. (alphas
£=12.8 MeV)
Log. (alphas
£=11 MeV)
Log. (track #1
10 20 30
—1 [-116-1621])
Etching time (h) 40
Figure 9. Comparison of track 1 from spot [-116,-1621] etch dynamic with that of calibration
alphas.
310
The comparison of functions track etch rate versus removable depth for alpha
candidate mentioned above and 11 and 12.8 MeV calibration alphas is presented
in Fig. 10. We estimate that track 1 [-116,-1621] belongs to alpha particle with
energy ~12 MeV. Another example of identification of high energy alpha track will
be showed bellow (see Fig. 11).
The comparison of etch dynamic of track 1 from spot [-433,-2285] with that of
12.8 and 16.7 calibration alphas is presented in Fig. 12.
The comparison of functions track etch rate versus removable depth for alpha
candidate mentioned above and 16.7 and 12.8 MeV calibration alphas is presented in
Fig. 12. We estimate that this track belongs to alpha particle with energy ~16 MeV.
The track diameter distributions of tracks inside hot zone for 7 and 35 h of
etching are showed in Fig. 13a and b, respectively. There are three peaks for track
diameter distribution with 7 h of etching (Fig. 13a). By longer etching time (35 h)
they are shifted and splintered a few bands (Fig. 13b). Thus we can estimate the
energies of these particles with more high accuracy. On the distribution in Fig. 13b
the peaks, that corresponded protons with energy ~1.5 MeV, possible 1.35 MeV
protons or 18.8 MeV alphas, alphas with energies 16.6; 16; 14.1; 12; 10.6; 10.2;
9.2 MeV, are observed. The main peak is under question because it is belongs to
both alpha particle and proton range of diameters.
The same track diameter distributions were obtained for all surface of detector
0.9422
10 20 30 40 50
Removed depth (jim)
Figure 10. Track etching rate versus removed depth for track 1 from spot [-116,-1621] , 11 and
12.8 MeV calibration alphas.
311
*%B. 5 : "A
%w*t-
12.8 MeV alphas
mm mi
& • " «
[-433;-2285], track
'VST%
Figure 11. Comparison of track etch dynamic of track 1 from spot [-433,-2285] with that of 11
and 12.8 MeV alpha calibration tracks. Etching time - 7, 14, 21, 28 and 35 h from left to right.
~ 1 cm 2 (see Fig. 14). You can see that track diameters are distributed in the same
bands like in Fig. 13. This is the proof of that the charge particle emission (with
energies mentioned above) took place not only in "hot zone" but also was on all
surface of sample.
A Alpha 12.8
8
^J MeV
£
A Alpha 16.7
MeV
I14 mm
T3 —IBI— Track #1
10 Alpha 20 MeV
-*
18 27 36
Etching time (h)
Figure 12. Comparison of track 1 from spot [-433,-2285] etch dynamic with that of calibration
alphas.
312
p1.35ora18.8MeV(?)
ft] ,JEL„
12 14 16 18 20 22 24 26 28 30
Track diameter (urn) Track diameter (nm)
Figure 13. Track diameter distributions in "hot zone" after 7 h (a) and 35 h (b) of etching.
4. Conclusion
• We unambiguously identified tracks of as minimum two groups of alpha
particles with energies 10-13 and 15-17.5 MeV. The emission of such alphas
was previously measured by CR-39 detectors with different shielding.
• We confirmed the emission of protons with energies ~1.7-1.9 MeV during
of exothermic hydrogen desorption from Pd/PdO:H K samples.
• The comparison of track etch dynamic of calibration alpha particles and
protons including functions D = /(£) and Vt = f(h) with that of individ-
ual tracks, unambiguously confirms the effect of energetic charged particle
emission from surface of metals with high affinity to hydrogen.
• Method of track depth measurement to improve the energy resolution and
separation different types of particles is on the way.
50
» 40
o
| 30
CO
f 20-I
z
10-
0 -t-i,.. -i X flpPfr an-
6,0 6,5 7,0 7,5 8,0 8,5 9,0 12 14 16 18 20 22 24 26 28 30
Track diameter (urn)
Track diameter (|im)
Figure 14. Track diameter distributions on 1 cm 2 of detector (including "hot zone") after 7 h (a)
and 35 h (b) of etching.
313
References
1. A.G. Lipson et al., Fusion Technology 38, 238 (2000).
2. A.S. Roussetski, Proc. of ICCF-11, Marseilles, France (2004).
3. A.B. Aleksandrov et al, Nucl. Instr. and Meth. A535 542-545 (2004).
4. B. Dorschel et al., Radiation Measurements 31 103-108 (1999).
5. D. Nicezic and K.N. Yu. Materials, Science and Engineering, R(46) 51-123 (2004).
I N T E N S E N O N - L I N E A R SOFT X-RAY EMISSION FROM A
H Y D R I D E TARGET D U R I N G P U L S E D D B O M B A R D M E N T
G E O R G E H. M I L E Y , Y A N G Y A N G , A N D R E I L I P S O N , M U N I M A H A Q U E A N D
IAN P E R C E L
Department of Nuclear, Plasma and Radiological Engineering, University of Illinois,
103 S. Goodwin Ave., Urbana, IL 61801, USA.
E-mail: ghmiley@uiuc. edu
MICHAEL ROMER
Department of Electrical and Computer Engineering, University of Illinois,
1406 W. Green St., Urbana, IL 61801, USA.
1. Introduction
Karabut in the LUTCH Laboratory in Russia recently reported X-ray laser
(~1.5keV) emission from metal targets such as Ti and Pd, which served as the
cathode in a high-current pulsed deuterium glow discharge (PGD) plasma diode. 1 ' 2
Later, he vividly demonstrated the potential capability of this type of laser with
a small follow-up 10 W "prototype" unit, which "drilled" a 9 mm diameter hole
in a 3 cm thick plastic target. This remarkable unit is more compact and pro-
vides a shorter wavelength than any prior "table top" X-ray laser. Staff at the
University of Illinois at Urbana-Champaign (UIUC) have undertaken theoretical
and experimental studies of the mechanisms involved in this unique X-ray emission
phenomenon. 2 ' 3
In UIUC's experiments, it was established that anomalous X-ray emission is ob-
served during PGD operation at a pressure of 0.1-0.5 Torr and at a spacing of about
4.0 mm between the cathode and anode. The current pulses have a square shape
314
315
with 0.2-2.0 ms duration and a rise time of 0.1 /xs. The glow discharge operated at
a voltage as low as 300 V with a pulsed current up to 2 A. These crucial conditions
are similar to those in Karabut's earlier studies, 1,2 but the voltage operation down
to 300 V represents a new region.
This paper will briefly describe the UIUC pulsed deuterium bombardment glow
discharge project. The X-ray diagnostics employed and their calibration will be
discussed. The calibration will be applied to discharge data to determine the power,
intensity, dosage, and efficiency of the X-ray observed. Finally a brief discussion
is given of related experiments using a deuterium flux created by desorption of D
loaded in a Pd target electrolytically. These experiments have much lower D-fluxes
than PGD, but low level X-ray production thought to be related to the discharge
phenomenon.
2. E x p e r i m e n t a l S e t u p
The UIUC staff have designed and fabricated a unique new type of discharge cham-
ber (Fig. 1), which contains a water-cooled cathode (the target can be mounted
easily, and is capable of linear motion), a stainless steel anode (capable of angular
motion), and a photodiode soft X-ray detector (which will be discussed in-depth
shortly). A beryllium filter was placed in front of the detector to prevent detection
of visible light. In order to reduce the electrical leakage current between the an-
ode and the ground and to confine the plasma to a smaller volume, a glass tube is
added to surround the electrodes, as shown in Fig. 1. On both ends of the tube,
plates covered by insulating material are used to provide a sealed boundary for the
discharge. Steady state I-V curves obtained after the addition of the glass tube
showed that the applied voltage increased by 50%. A hole of 1cm diameter was
drilled into one side of the tube to allow X-rays to reach the detector with minimum
absorption.
Figure 1. Experimental chamber diagram (a) and discharge view showing glass tube (b).
316
3. A X U V D e t e c t o r T h e o r y / O p e r a t i o n
The AXUV-100 detector is a silicon p-n junction photodiode that is well suited
for the measurement of soft X-rays. Incoming photons or charged particles create
electron-hole pairs in the junction of the photodiode. The total number of electron-
hole pairs generated depends on the materials used in the photodiode and the
incoming particle energy. For the AXUV, the average energy for electron-hole
pair creation £"e-h is 3.7eV. 4 However, phenomenons that also require some of
the incident energy include "dead" doped regions and surface recombination. The
percentage of the total incident energy E\ going into electron-hole pairs is the
"quantum efficiency" r/Q. Fortunately, the AXUV used has been engineered to
approach theoretical quantum efficiency.4 Thus, the number of electron-hole pairs
is E\ divided by -Ee-h- The p-n junction of the photodiode sweeps the electrons and
holes across the junction and out through contacts. Thus, if the number of electron-
hole pairs is known, the current they create can be calculated, or vice versa.
The measured current production characteristics of the AXUV are shown in
Fig. 2. 4 The y-axis of Fig. 2 is the responsivity of the photodiode, which is mea-
sured in A/W. With the responsivity information, it is simple to backtrack from
the measured current to calculate the power incident on the detector. However, an
oscilloscope was used to measure the voltage created. Thus, a basic circuit con-
sisting of the AXUV photodiode and the oscilloscope is needed to understand the
measurement (Fig. 3).
As seen in Fig. 3, the AXUV photodiode is modeled as a current source accom-
panied by an inevitable series resistance i?s - due to the silicon that the electrons
0.2
iC
' Photons
0.1
* " Electrons
- Hydrogen ions
0 '••
100 1,000 10,000 40,000
RS
~5
I
+
Vos
Rl
AXUV
1 M or 50
Oscilloscope
Figure 3. Basic circuit of the AXUV (including a series resistance) and the oscilloscope.
and holes must travel through to escape. The series resistance is assumed to be
5 O.4 The oscilloscope has an input resistance i?i, which can be set at either 1 MO
or 50 0. In the AXUV setup, the voltage read by the oscilloscope is
where /AXUV is the current generated by the AXUV photodiode. The fraction of
the total current that this corresponds to is
//AXUV =
Ri + Rsw (2)
Equations (1) and (2) show that a large input resistance R\ gives a high am-
plification, hence an accurate reading. However, the photodiode is a capacitive
device, and the rise time of its response is directly proportional to the resistance it
is discharged over:
Series resistance Rs Q 5
Oscilloscope high-input resistance -Rl-High n 10 6
Photodiode capacitance C pF 4
Fraction of measured current fl-lMfl ~1.00
Rise time TlMfl s 8.8 x l O " 6
4. Calibration
The calibration of the AXUV photodiode was done with a 7.5 mCi 14 C source.
Carbon-14 is a beta emitter with average beta energy Ep of 49.5 keV.5 Although
14
C is a beta source rather than an X-ray source, responsivity data is available up
to 30keV for electrons. While this is 20keV short of Ep, the scale of Fig. 2 is
logarithmic, and the electron responsivity slope at the highest graphed energy is
nearly flat. Responsivity data from Fig. 2 is extrapolated to the energy of 14 C in
Table 2. If the measurement techniques for 14 C are accurate, they should also be
accurate for soft X-rays; the only difference being the responsivity of the AXUV.
To match the measured results with the source intensity, the power that the 14 C
source delivers to the collector must first be calculated:
PB = AEpAB-^(W), (4)
As
where A is the source activity (decays/s), Ep the average beta energy (J), AD the
detector surface area (cm 2 ), and Ag is the beta source surface area (cm 2 ).
The oscilloscope voltage can then be calculated by
VOS = 3 ? C I 4 P D J R I ( V ) , (5)
where 5R(^14 is the responsivity of the AXUV for 14 C betas (A/W), P D the power
delivered to the detector by the 14 C source (W), and R\ is the input resistance of
the oscilloscope (f2). The calculated oscilloscope voltage and associated parameters
are given in Table 3 for comparison with measured values cited later.
To eliminate background light, the photodiode was placed in a container that
blocked out light on all sides but the entrance. The detector head was faced away
from the entrance to minimize the light. A 20 MHz low-pass filter was used with
15 0.237
20 0.238
30 0.240
50 0.244 (extrapolated)
319
the oscilloscope to reduce the noise to a //V magnitude. The 14 C source was then
placed in the container and gently pressed against the detector face. Since the 14 C
source completely covered the detector face, essentially no light reached the AXUV.
Several consecutive measurements were taken to find a stable, reproducible signal.
The final measurement gave a voltage of 2.70 ± 0.25 mV.
This result is about a fifth of the projected voltage in Table 3. However, a thin
layer of glass covers the 14 C source, and this is thought to attenuate the emitted
betas, resulting in the smaller measured voltage.
The chord subtended by the hole was measured to be 400 mm. Then the total
subtended angle #TOT is found to be 1.63 radians. To calculate the surface area
of the vessel, hence detector, that this corresponds to, a solid angle surface area
equation is used:
SA de
•#TC 2vr
sin(/>d0d6> = r227r( 1 - c o s f - ^ ) )• (6)
The total angle subtended is divided by two here because the <j> angle is measured
from the vertical (z-axis) in the spherical coordinate system. Next, SA can be used
0.20- 0.25
p = 500 mTorr
nal (vo
0.15- 0.20
cd
c 0.15
5 o.io- u>
(0 0.10
% o 0 05
V,
tl)
JU 0.05
8 ^JUUUV\AJU
8 0.00
0.00" -0.05
0.0&
-0.10-
•S2.
">
0.10
0.05
p = 5 0 0 mTorr
k
!
15 0.00
a
0.05
T i m e (s)
Figure 4. Three measurements of the X-ray emission pulse at 500 mTorr. Measurement 1 is the
top left graph, measurement 2 is the top right, and measurement 3 is on the second row.
321
Hole in glass
cylinder
X-ray laser
vessel
to calculate the X-ray power at the source by using (7). A beryllium filter was used
to prevent transmission of unwanted photons and charged particles to the detector
(the detector's transmission curve is shown in Fig. 6). Therefore, a transmission
compensation factor is included in the X-ray power calculation.
Px-ray = V 0 s ^ ^ — j ~ - ^ S A - J - ( W ) , (7)
-Kl «X-ray JF ^-D JE
where V"os is the voltage read from the oscilloscope (V), R\ the oscilloscope input
resistance (0), 3?x-ray the responsivity for the soft X-rays (A/W), / F the average
transmission fraction through the Be filter, AD the surface area of the detector face
(cm 2 ), SA the surface area subtended by the hole (cm 2 ), and / E is the fraction of
X-rays escaping through the hole in the glass cylinder.
Note from Fig. 6 that the Be window cuts off all X-rays below 600 V. Thus, as
stressed earlier relative to Fig. 4, the observed X-rays must have energies >600V
(despite the <~300V discharge energy). In view of Karabut's earlier work, 1 ' 2 it
seems logical that these X-rays have energy of ~1.5-2.0keV.
Once the power is obtained, the intensity of the X-rays is simply
/X-ray = ^X-ray AT ( W / c m 2 ) , (8)
where AT is the exposed surface area of the target. Additionally, the dose over a
pulse is defined as
where tx-ray is the duration of the X-ray pulse. Finally, the X-ray production
efficiency (X-ray power out/electrical power in) can be defined as
I.U
Be
Thickness = 12.5 microns
0.8 " /
0.6-
0.4 - /
//
0.2 " //
00 -
500 1000 1500 2000
Photon energy (eV)
Figure 6. Beryllium filter transmission rate as a function of photon energy.
where Vm is the input voltage, I[n the input current, and t-m is the duration of the
input pulse. Values for the constants are listed in Table 4, while the calculated
values for the X-ray power, intensity, dose, and efficiency are tabulated in Table 5.
Assuming an X-ray quanta energy of Ex = 1.3 keV, the 13.4mW/cm 2 intensity
shown in Table 5 corresponds to 6.4 x 1013q/s-cm 2 . While the dose per pulse
is small, the instantaneous X-ray power over the pulse is in the mW range. The
X-ray efficiency is quite low, suggesting improved operation may be sought in future
experiments.
1.4.
X8-LJFTLD/PPE filters
1.2
-Fit: / t // 0 = exp(-|+n/?PPE), \im = 893cm
1.0- <E x ) = 1.30±0.25keV
</ 0 )=9.0 + 2.0 X / s - c m 2 in 4n ster.
0.8
0.6-
0.4.
0.2.
0.0
-0.2-
,— 20 30 40 50 ~eo
10
PPE filter thickness, h (urn)
Figure 7. X-ray spectral measurements from a Pd:Dx cathode using a set of TLDs with P P E
filters 0-60 /im thick.
324
7. Conclusions
Strongly non-linear X-ray emission occurs and has been measured during intense
D-bombardment of a P d target using a pulsed deuterium discharge method. It is
noted t h a t there is a delay time preceding emission, but the key feature is t h a t the
X-ray energy Ex is greater t h a n the discharge voltage. The P G D setup and diag-
nostics used in the experiment have been discussed in detail to aid others who may
wish to adopt these techniques. Deuterium diffusion and desorption are thought
to be vital steps in the X-ray emission mechanism. This seems consistent with the
o u t p u t data, and an auxiliary experiment provides supporting evidence.
References
1. A.B. Karabut, Research into powerful solid X-ray laser with excitation of high current
glow discharge ions, Proceedings, 11th Inter. Conference on Emerging Nuclear Energy
Systems, Albuquerque, NM, pp. 374-382 (2002).
2. G.H. Miley, A.G. Lipson, and A. B. Karabut, ICFA-6, Novel Accelerators and Laser-
Beam Interactions, Oxford, England (2003).
3. P.B. Corkum, Phys. Rev. Lett. 71, 001994 (1993).
4. International Radiation Detectors Inc. (Oct. 2005), http://www.ird-inc.com/
frontpage.html.
5. Health Physics Society, Radionuclide decay data (Oct. 2005), http://hps.org/
publicinformation/radardecaydata.cfm.
6. A.G. Lipson, C.H. Castano, G.H. Miley, B. F. Lyakhov, A. Tsivadze, A. Yu, and
A.V. Mitin, ICCF-12, International Conference on Condensed Matter Nuclear Science,
Yokohama, Japan (2005).
E N H A N C E M E N T OF FIRST WALL D A M A G E IN ITER T Y P E
T O K A M A K D U E TO LENR EFFECTS
A N D R E I G. L I P S O N , G E O R G E H. M I L E Y A N D H I R O M U M O M O T A
University of Illinois at Urbana-Champaign, Department of Nuclear,
Plasma and Radiological Engineering, Urbana, IL 61801, USA
E-mail: lipson@uiuc.edu
1. Introduction
So far, the evaluation of DD/DT-reactions at the first wall surface of fusion reactors
like ITER has not taken into consideration nonlinear processes during high current,
low-energy bombardment of the metal first wall. Indeed, accordingly to DD-reaction
cross-section for free space the probability of DD-reactions at E^ < 2.0 keV would
be negligible.1 During bombardment of a target, where the embedded ion den-
sity builds up in the lattice, conditions are quite different. It was recently shown
that a majority of metal targets subjected by low-energy deuteron bombardment
have a DD-reaction yield orders of magnitude higher than predicted by extrap-
olation of the standard (free space) DD-reaction cross-section to lower deuteron
energies. These enhancement (nonlinear) effects came from a drastic increase in
the deuteron screening potential in the metal targets at E& ~ 1.0 keV, especially
at a high deuteron current density, where the ion density in the target can become
quite large. Our recent experiments using a pulse glow discharge to simulate these
conditions 2 showed about nine order of magnitude enhancement for the d(d,p)t
reaction yield at E& = 1.0 keV in a Ti target, compared to an extrapolation of
the standard cross-section to that energy. Strong enhancements have also been
reported by several groups studying astrophysical phenomenon. 3_7 These reports
suggest an enhanced DD-reaction yield may also occur during edge plasma wall
bombardment of fusion devices like ITER since the energy range is consistent with
deuteron accelerated by the electrostatic sheath at the plasma-wall.8 Understanding
such effects becomes important relative to the possible wall damage. The enhanced
325
326
yield of alphas from DT reaction at the edge metallic sites, create vacancy sites,
including stresses and allowing accumulation causing surface blistering. Knowledge
of the magnitude of the enhancement effect in various metals will enable selection
of reactors first wall materials that minimize such damage.
We propose to simulate such phenomenon using a high-current pulsed Glow Dis-
charge (PGD) in deuterium. Preliminary studies have shown that the PGD method
can generate deuterons with energies ranging from 0.8 to 2.5 keV and a current den-
sity 300-600 niA/cm 2 . The corresponding deuteron bombardment current density
on the cathode is about three orders of magnitude above that for the best low-
energy accelerators. This will enable detection of the reaction products down to
E<\ < 1.0keV (using several tens hours of GD operation per data point). Moreover,
this high-current bombardment should induce a measurable level of X-ray emission
that is predicted for DD-reaction in the target lattice environment, 9 allowing it's
detection using both X-ray and charged particle diagnostics. The correlation be-
tween the DD-reaction and X-ray yields will provide an important data base for an
improved theoretical understanding of electron screening effects under these target
conditions.
2. Background
Recent accelerator experiments at (-E'pr)iab < 5.0keV 3 ~ 7 ' 1 0 - 1 4 show enhanced elec-
tron screening effects at the deuteron/electron densities encountered in a majority
of deuterated metallic targets. These measurements show a significant increase
("enhancement") in the reaction rate (i.e. increased astrophysical factor S) at
lower energies. Even for a low-density gaseous D2 target bombarded with low-
energy deuterons down to (-Epr)iab = 3.0 keV, the screening potential (measured as
Ue = 25 ± 5 eV) was found to be remarkably higher than the adiabatic limit for
DD-reactions in a deuterium molecule (fad. = 14.0 eV). 10
Raiola et al.6'7,11 systematically measured the low-energy (down to E^ = 5 keV)
yields of D(d,p)T reactions and corresponding screening potentials for deuterated
targets using about 30 different elements over the Periodic Table, including both
metals and some nonmetal elements. (This extensive study was done at LUNA,
the European astrophysical laboratory, as a part of their attempt to understand
deuterium reactions at low energies and high electron densities). It was found
that majority of the targets resulted in a "large" screening potential Ue > 100 eV,
excluding, mainly, metals of group 4 (Ti, Zr, and Hf) and group 1 (Cu, Ag, and
Au). The accelerator they used had a weak deuteron beam current, ranging from 1
to 54 j(iA. Therefore, reactions could only be measured at a relatively high energy
(£iab > 5.0 keV). Still, the striking results provide strong motivation to extend these
data to yet lower energies as proposed here.
Kasagi et al.12'13 in Japan, operating with a higher-current low-energy accel-
erator (D+ beam current ranging 60-400 fiA), recently measured D(d,p)T yields
in several metal and metal oxide targets down to E^ = 2.5 keV and found that
the screening potential value Ue at such beam intensity is strongly effected by
327
This comparison show that available high-current pulsed GD might well simulate
the edge-plasma effects at the first wall of ITER.
H
Figure 1. High-current pulsed glow discharge set up. 1: vacuum chamber; 2: cathode holder; 3:
Ti cathode; 4: Mo anode; 5: Be window; 6: CR-39 detectors; 7: glow discharge area.
Due to the electrical noise during pulsing, a key to successful use of this technique
is employment of CR-39 track detectors. With proper calibration these detectors
provide a sensitive measure of the particle (protons in the present case) energy. The
track hole diameter on particle energy entering the CR-39 provide this data while
electrical noise is eliminated, some natural defects in the CR-39 are always present.
These can be minimized by proper handling and annealing prior to use. Since the
proton fluxes in this low-energy range are extremely low, the foils are left position
for hours while the device is pulsed (as much as ten hours in present work). This
provides a time integration of the signal which is essential. Fortunately the GD
apparatus can operate very stably for long periods. 2
329
200
150
100
50-
4.5 5.0
I 5.5
Track diameter (|rm)
Figure 2. The 3.0 MeV proton yield detected by 11 p Al covered CR-39 detectors in deuterium
GD at the same current and different accelerating voltages: U\ = 805 V and U2 = 2175 V.
The yields of 3.0 MeV protons obtained at different deuteron energies ranging
from 0.8 to 2.45 keV were normalized to those at maximal voltage U = 2.45 kV, tak-
ing into account the power of discharge or effective temperature at the target surface
that both affect the change of effective deuteron concentration in the Ti (N-&(x)).
This correction is needed to account for the change in deuterium concentration in
the Ti-target surface. The correction coefficient k can be derived as: 2
£ d AT
k{W,T) =exp (Wm/Wx) (2)
k^TmTQ
where £d = 0.04 eV is the activation energy of deuteron escape from the Ti surface
during bombardment; Tm = 1941 K is the Ti melting point, T0 = 290 K is the
initial target temperature, A T = T m — To, Wm = 906.5 W is a max amplitude
power at _Ed = e Um = 2.45 keV and 7m = 370 mA; Wx is a current amplitude power
corresponding to any other (lower) voltage and current in GD with Ti-target. The
value of Ed is determined from accelerator data 12 using an Arrhenius plot of 3.0
MeV proton yields for Ti-target at 180-195 K, Ed = 10.0 keV.
Figure 3 shows the results of normalization of DD-proton yields Yx at lower
energies to those at E<i = 2.45 keV compared to the standard DD-reaction yield
behavior (solid line) calculated in accordance with Bosch and Halle DD-cross-section
approximation, similarly to. 1 2 ' 1 3 Clearly there is a strong enhancement in the yield
at these lower energies compared to B and H unscreened ("bare") values. 1
331
Ed (keV)
Figure 3. Experimental yield of 3.0 MeV protons at 0.8 < E^ < 2.45 keV normalized to that at
E<± = 2.45 keV. The bare cross-section corresponded to B and H approximation to E^ <2.45 keV
is marked by a solid line. The dashed line is a DD-reaction yield in accordance with a screening
potential value Ue = 610 eV. 2
where YP(E) is the experimental yield of DD-protons in GD, Y\,(E) is the bare
cross-section yield at the same energy determined by the B and H approximation;
2 2
2-KTJ = 31.29Z (n/Ey/ is the Sommerfeld parameter (here Z is the charge number
of deuteron in the case of D+ projectile and target, /j, is the reduced mass and E-is
the center of mass deuteron energy), respectively. Thus f(E) is directly related to
the screening effect on the reaction rate. This is further illustrated in Fig. 4, where
data obtained from accelerator experiments 9 (curve 1) and GD experiments with a
Ti-target/cathode (curve 2) are shown.
In accelerator measurements with the Ti-target at 2.5 < E& < 10.0 keV, the
deduced screening potential is Ue = 65 ± 10 eV.4 However, for the PGD exper-
iment, the screening potential is as large as Us = 620 ± 140 eV. Put another
way, this experimental enhancement for GD in terms of DD-proton yield even at
Ed = 1.0 keV is about nine orders of magnitude larger than that predicted with
bare (B and H) cross-section (Fig. 4, curve 2). This striking result illustrates how
important the higher deuteron/electron densities in the target (due to the higher
currents in the GD) can be.
332
1l
io9-
10 6 -
10 7 -
106'
10 5
ue~- 610±150eV
10 4 -
10 3 -
\ Y
1
&
i \
/
* | AS Ue=65±10eV
10 2
\ , ,
10- \\
1 £ d (keV)
Figure 4. DD-reaction enhancement factor calculated with formula (4) for the Ti target during
deuteron bombardment with accelerator 1 3 (curve 1) and glow discharge 2 (curve 2). The solid
parts of the curves are corresponded to the deuteron energy ranges where DD-reaction yield was
measured experimentally.
The screening potential Ue increases roughly logarithmicly with increase in deuteron cur-
rent J. The various metal-host (Ti) electron shell energy is consistent with the screening
potential values Ue.2
Thus, when the GD low-energy yields are analyzed in the same way as accelerator
data, 12,13 they exhibit a larger enhancement at very low D-energy (Ed < 2.45 keV)
than was expected from the accelerator bombardment. Further increase in current
density (say in TOKAMAK devices) could lead to enormous enhancement of fusion
reaction rate in construction metals from which the first wall is built. Note that
the enhancement data on tungsten obtained even with low-current accelerator 7 ' n
gives high screening potential value Ue = 220 eV. Thus, suggesting same logarithmic
333
(a) (b)
Figure 5. (a)- X-ray image of the Ti-cathode using the pin-hole camera. The objective of 0.3 mm
diameter is narrowed by use of a 15 (im Be shield in front of the camera. The image is a positive
imprint, (b) - Correlation between X-ray and current pulses in GD (Ix ~ 10 1 4 . 1.5
keV).
334
The X-ray yield per deuteron increases exponentially with the applied deuteron
current at E& ~ 1.5-2.0 keV as it is shown in Fig. 6
3.50E 04
3.00E 04
^=0.977
2.50E-04
2.00E-04
1.50E-04
1.00E-04
5.00E 05
COOEiOO
40
Power p* (W)
Figure 6. Yield of X-ray quanta per bombarding deuteron from the Ti-cathode versus effective
discharge power at p — 4.2 torr.
4. Conclusions
• At Ja > 1.0 A / c m 2 and E& ~ l - 2 k e V , the total yield of DT-reaction (scaled
to GD with Ti target) for ~ 10 years of operation is found to be ~ 10 1 4 H e ~ 4
atoms, stopped at depth ~ 5.0 m m from the surface. This corresponds to
~ 10 1 7 c m ~ 3 H e - 4 concentration beneath the surface.
• T h e 4 He-atoms will be precipitated along dislocations or captured in metal
vacancies serving as obstacles for dislocation motion resulting in additional
stress.
• Reduction in plasticity (e.g. in W ) due to the He capture is caused a
microcrack generation at the near-the surface layer and fracture of the first
wall.
• Intense soft X-ray emission at the surface may also enhance ero-
sion/sputtering process at the surface of the first wall caused by X-ray
energy deposition in the near-the-surface layer during charged particle bom-
bardment.
• T h e edge plasma effects at the first wall, including blistering, cracking
and erosion, would be significantly underestimated because the enhance-
ment of D D / D T reaction and accompanying radiation processes at very
low deuteron energy are neglected.
• T h e high current pulsed GD testing appropriate cathode materials (W, St.
steel) could be a suitable instrument to simulate edge plasma effects at
ITER'S first wall.
References
1. H.S. Bosch and G.M. Halle, Nucl. Fusion 32, 611-631 (1992).
2. A.G. Lipson, A.S. Roussetski, A.B. Karabut, and G.H. Miley, JETP 100, 1175 (2005).
3. M. Junker, A. D'Alessandro, S. Zavatarelli et al, Phys. Rev. C57, 2700 (1998).
4. M. Aliotta, F. Raiola, G. Gyurky et al, Nucl. Phys. A690, 790 (2001).
5. K. Czerski, A. Hulke, A. Biller et al, Europhys. Lett. 54, 449 (2001).
6. F. Raiola, P. Migliardi, G. Gyurky et al, Eur. Phys. J. A13, 377 (2002).
7. F. Raiola, P. Migliardi, L. Gang et al, Phys. Lett. B547, 193 (2002).
8. D. Reiter, Edge plasma physics overview, Trans. Fusion Tech. 33, 249 (1998).
9. V. Violante, A. Torre, G. Silvaggi, and G.H. Miley, Fusion Tech. 39, 266 (2001).
10. U. Greife, F. Gorris, M. Junker et al, Z. Phys. A465, 150 (1995).
11. F. Raiola et al. (LUNA collaboration), Electron screening in d(d,p)t for deuterated
metals, Nucl. Phys. A719, 61C (2003).
12. H. Yuki, J. Kasagi, A.G. Lipson et al, JETP Lett. 68(11), 785 (1998).
13. J. Kasagi, H.Yuki, T. Baba et al., J. Phys. Soc. Jpn. 71(12), 2881 (2002).
14. K. Eder, D. Semard, P. Bauer et al, Phys. Rev. Lett. 79, 4112 (1997).
15. S.P. Moller, A. Csete, T. Ichioka et al, Phys. Rev. Lett. 88, 193201 (2002).
16. For He-4 blistering in ITER first wall see: Fusion Sci. Tech. 47 (4), 821-1295 (2005).
G E N E R A T I O N OF D D - R E A C T I O N S IN A F E R R O E L E C T R I C
K D 2 P 0 4 SINGLE CRYSTAL D U R I N G TRANSITION T H R O U G H
C U R I E P O I N T (Tc = 220 K)
A.G. L I P S O N A N D G.H. M I L E Y
Department of Nuclear, Plasma and Radiological Engineering, University of Illinois at
Urbana- Champaign, Urbana, IL 61801, USA
E-mail: lipson@uiuc. edu
A.S. R O U S S E T S K I
Lebedev Physics Institute, The Russian Academy of Sciences, Moscow 117285, Russia
A.G. L I P S O N A N D E.I. S A U N I N
Institute of Physical Chemistry, The Russian Academy of Sciences,
Moscow 117915, Russia
1. Introduction
Naranjo et al.1 presented a desktop neutron generator based on deuteron beam
ionized and accelerated up to 100 keV by electric field arising from the spontaneous
polarization of ferro/pyroelectric LiTa03 crystal at a low-pressure deuterium gas
adsorption in their Letter to Nature. The results of this work are appeared to be
solid with respect to both experimental and theoretical aspects of 2.45 MeV DD-
neutron production. However, a certain early history exists on a deuteron fusion
driven by a strong crystalline electric field.
The fracto-fusion caused by a weak neutron emission has been observed dur-
ing the fracture of deuterated dielectric crystals (i.e., induced polarization), where
cracks serve as tiny accelerators. 2,3 Such crack propagation in crystalline dielectrics
is accompanied by high-energy electron and X-ray emissions up to 100 keV (see
Refs. 2, 3 and references therein), similarly to that emitted by pyroelectrics with
336
337
2. Experimental
• Transitions of KD2PO4 (98% D purity) single crystals through Curie point
Tc = 220 K by heating-cooling cycle using LN2 cryostate. Control of tran-
sition with thermally stimulated depolarization (TSD).
• Neutron measurements with BF3 - seven counter proportional neutron
detector.
• Tritium measurements with liquid scintillator technique with dissolving of
DKDP crystals in H 2 0 .
• Recently done: 3.0 MeV proton measurement with CR-39 (open and filtered
with Al foils) attached to DKDP plates cycled through Curie point.
3. Experimental Results
The amplitude-differential spectra of neutron emission are presented in Fig. 1. As
seen, the sum of spectra for DKDP exposed at the neutron detector during ferro-
electric phase transition near 220 K are in good agreement with Cf-252 amplitude
spectrum.
800
a
700
600
u,
'c 500
g 400
30
O °"
- 200"
•g 100-
2
50 • b
40
30
20
10
5 10 15 20 25 30
cChannel
Figure 1. Distributiion of the pulses arriving at the neutron detector channels of the pulse height
analyzer, (a) From the Cf252 neutron source; (b) during temprature cycling of DKDP crystals
near T c .
0
o
1 3
-2
Figure 2. (a) Spectrum of thermal depolarization during the heating of DKDP sample near T c ;
(b) corresponding histograms of neutron bursts. Here L, a is the confidence level of the observed
neutron bursts, and Nb is the average background level.
As seen from Table 1, the neutron emission is occurred only in DKDP crystals
(not in KDP) and strictly in the temperature range corresponding to spontaneous
polarization (219-223K).
Generation of DD-reaction in DKDP crystals during transition through Curie
point is confirmed by measurement of 3.0 MeV protons emission (d(d, p)t reaction)
during similar transitions (Fig. 3).
Tritium concentration in DKDP has been measured by liquid scintillation tech-
nique. The samples were 100 times cycled through Curie point in a glass capsule.
After the cycling the crystals, glass, and gas atmosphere of the ampule were ana-
lyzed. The results (in units of 109 T-atoms per gram of DKDP) are presented in
Table 2.
Table 1. Parameters of neutron emission in KH2PO4 and KD2PO4 single crystals in various
temperature intervals
open CR-39
3.0 ± 0.2 MeV 11 mAI/CR-39
18 44 mAI/CR-39
" 6-
2-
0
4,8 5,0
Jj
52 5,4
Track diameter (m)
5,6 5,{
J 6,0 62
Figure 3. Three MeV proton emission: 40 transitions through Curie point in a row with attached
open and filtered CR-39 detectors: the detected track diameters are consistent with 3 MeV proton
energy losses in Al foils.8
Neutron and proton emission yields per transition through Curie point:
*The DKDP sample m = 0.5 g was subjected to 100 heating-cooling cycles in isolated
glass cell at atmospheric pressure. Accordingly to this measurement the yield of tritium
was found to be Yt = (1.82 ± 0.25) x 10 8 (t/transition).
341
recovered, resulting in multiple usage of the source (passage through Tc) to generate
neutrons.
The proposed neutron source can be further modified resulting in production
of enhanced stationary neutron yield by application of pulsed voltage (several kV)
between cathode and anode at constant temperature T < Tc (e.g. T = 77 K). This
application provides polarization reversal at spontaneously polarized ferroelectric
state by triggering electric dipole moment orientation by AC electric field.
Figure 4. Diagram of cryo-set up of 2.45 MeV neutron source based on a high-voltage discharge
between DKDP single crystalline cathode and anode during their passage through Curie point. 1 0
5. Conclusions
Generation of DD-reaction resulting in neutron and 3 MeV proton emissions
in DKDP ferroelectric crystal during passage through Curie point has been
established.
It was shown that neutron and proton channels in DKDP crystal give com-
parable nuclear yields. Large amount of tritium production ( ~ 2 x 10 8 T 3
at./transition) cannot be referred to usual DD-reaction.
The factor of spatial separation of deuteron source and target in deuterated
ferroelectrics can be used to obtain large neutron yield during transition of
these ferroelectrics to spontaneously polarized state.
New type of neutron source based on electric discharge between two fer-
roelectric KD2PO4 (DKDP) crystals during their polarization reversal at
T = 220 K in D2/T2 atmosphere is proposed. No high voltage power supply.
Small size. Projected intensity Yn = 10 6 (D 2 )-10 8 (T 2 ) n/s.
Potential applications include Homeland security and oil exploration as a
borehole source.
343
References
1. B. Naranjo, J.K. Gimzewski, and S. Putterman, Nature 434, 1115-1117 (2005).
2. V.A. Klyuev, A.G. Lipson, B.V. Deryagin et al, Sov. Tech. Phys. Lett. 12 551-555
(1986).
3. B.V. Deryaguin, A.G. Lipson, V.A. Kluev et al., Nature 341, 492 (1989).
4. A.G. Lipson, D.M. Sakov, V.B. Kalinin, and B.V. Deryaguin, Sov. Tech. Phys. Lett.
18, 90-95 (1992).
5. A.G. Lipson, D.M. Sakov, E.I. Saunin et al, JETP 76(6), 1070-1076 (1993).
6. M. Chiba et al, Nuovo Cimento A108(10), 1277-1280 (1995).
7. M. Fuji et al, Jpn. J. Appl. Phys., 41(4A), 2115-2119 (2002).
8. A. G. Lipson et al., Proc ICCF-10 (Boston, MS, 2003).
9. J.A. Geuther and Y. Danon, J. Appl. Phys., 97, 074109 (2005).
10. A.G. Lipson and G.H. Miley, A novel portable ferroelectric source of fast MeV neutrons
for homeland security applications. Transactions of American Nuclear Society, 2006
(in press).
S T U D Y OF ENERGETIC A N D T E M P O R A L CHARACTERISTICS
OF X - R A Y EMISSION F R O M SOLID-STATE C A T H O D E M E D I U M
OF H I G H - C U R R E N T GLOW DISCHARGE
A.B. K A R A B U T
FSUE "LUCH" 24 Zheleznodorozhnaya St, Podolsk, Moscow Region 14-2100, Russia
E-mail: karab.ab@g23.relcom.ru
1. Introduction
Experiments aimed at illuminating the anomalous high-energy phenomena in the
solid-state cathode medium of the high-current glow-discharge were carried out for
years. Earlier experimental results showed that the character of detected X-ray
emission was essentially different from the known X-ray emission types.
344
345
The window was shielded by 15/im-thick Be foil for protecting the detectors from
visual and ultraviolet radiation. Various detectors were installed by the window to
measure the output penetrating radiation (Fig. 1).
To estimate the intensity and evaluate the mean energy of the soft X-ray emission
in the GD, thermo-luminescent detectors (TLD) based on crystalline AI2O3 and,
covered by Be foils of varying thickness were used. The temporal characteristics of
the penetrating radiation were determined with the help of scintillation detectors
with the photomultipliers (PM). Two modes of radiation emission were observed
in the experiments: (1) diffusion X-ray emission (Fig. 2) and X-ray emission in the
form of laser beams (Fig. 3). The diffusion X-ray emission occurs mainly during the
current running in the form of flashes and conforming to the law 1/r2. The value
of X-ray emission energy was estimated for the experiments with using system
scintillator- PM and the beryllium foil shields for the foil with thickness of 15 and
30/um (Fig. 2a and b).
8 Be =15-300um
9
A s
view A * -
Figure 1. Schematic representation of an experiment, (a) pinhole, (b) TLD detectors and ab-
sorbing Be screens of various thickness, (c) PM-scintillator system, and (d) X-ray spectrometer.
(1) Cathode sample; (2) anode; (3) discharge chamber, (4) Be foil screens; (5) X-ray output chan-
nel, (6) pinhole objective, (7) X-ray film, (8) absorbing Be foil screens with thickness ranging
15-300 lira, (9) TLD detectors, (10) absorbing Be foil screens for scintillator, (11) scintillator, (12)
photomultiplier, and (13) mica crystal spectrometer.
By using the PM scintillation detector the relative intensity of the X-rays was
determined as the total sum of the amplitudes HAH a n d H,A2j of all the X-ray
bursts within the time interval of 1 second (Fig. 2a and b). The experiments using
the scintillator - PM measurement system, and, 15 and 30 /xm-thick Be foil shields
allowed to evaluate of the X-ray energy value as J5x- ra y ~ 1.3-2.5 keV (for different
cathode materials). Then the relative intensity was reduced to a physical magnitude
by the intensity value measured with the TLD detectors (.Ex-ray ~ 1.5-1.8 keV).
The generation of X-ray emission in the form of laser beams and began when the
GD operational parameters increased (duration of current pulses, current density,
GD voltage) and was observed as powerful flashes. The production of X-ray laser
beams occurred in pulse-periodic GD some time after ( A T delay time) the GD
current pulse trailing. The temporal spectrum of the X-ray emission made up a
346
correlation: the quantity of pulses per a T period of time (T stands for the time
period between the GD current pulses) versus the time period between the current
trailing edge and the X-ray pulse leading edge. The temporal spectra are discrete
in character, consisting of separate lines. The specific pattern of each spectrum is
dependent upon the cathode material used. The secondary penetrating radiation
(in the form of bursts of fast electrons with small angular divergence) occurred
when the targets made of different materials were exposed to X-ray laser beams.
The generation of electron bursts was observed in the experiment when the primary
X-ray beams passed through Pb targets (of up to 3 mm thickness). Presumably,
some multi-photon processes were initiated.
/(mA)
200
Figure 2. The typical oscillograms of the X-ray emission signal from the system PM -scintillator
covered with the Be foil with the different thicknes: (a) with covered the 15 /^m Be shield and
(b) with covered the 30/im Be shield. The system Pd—D2, the discharge current — 150 mA.
The X-ray emission spectra were measured using the curved mica crystal (50 mm
diameter) X-ray spectrometer, the spectrum being recorded on an X-ray film
(Fig. 4). Reflection and refraction spectra were registered in the experiment. Re-
flection spectra being used for data processing. The wave length and the energy of
the X-ray were determined according to the expression The energy of the X-ray
mX = 2dsin 0; EX-ra,y = 1.235/A,
where m is the spectrum order, A stands for the X-ray emission wave length in nm,
2d is the constant of the mica crystal lattice (2d = 2.0 nm), and 6 represents the
reflection angle. The spectra were repeatedly recorded during the GD operation
and after the GD current switch off (for up to 20 h afterward). The spectra pattern
347
includes bands, dark and light spots (consisting of multiple tiny dark and light
dots) and separate dark and light small spots. The bands and spots were located
in spectral areas specific for a given cathode material used (Fig. 4). The registered
energy of the X-ray emission bands and spots (the energetic position of the bands
and spots within the spectrum) was dependent upon the cathode material used. The
registered X-ray spectra in experiments was similar to characteristic X-ray spectra.
It was assumed that the diffusion component of the X-ray emission was registered
on the spectrum as a series of bands.
/x-ray, photons/beam
1.2x1(
0.8 x10s Pd-D
0.4X10B
0
/(mA)
100
0
/x-ray, photons/beam
1.2x108-
0.8x10s
Pd-Xe
0.4 x10s
0
/(mA)t
100
/v.
u4 : ml; mZ
o -- Af=100us-«-l—i— f(ns)
Figure 3. The typical oscillograms of bursts from X-ray laser beams (PM—scintillator) in the
discharge for different kind of gases. The cathode sample is Pd, current: 50 mA. *The pulse peak
was cut a discriminator of amplifier, (a) D2, (b) Xe, and (c) Kr.
The X-ray emission bands energy do not correlated with L, M energy of the
electron levels (Fig. 4).
The laser beams were recorded as dark spots and in case of the emission beam
high density they assumed white color (solarization of the photoemulsion) (Fig. 5b-
d). In certain experiments radiation and thermal destruction of the X-ray film was
observed (Fig. 5a).
348
8
(^X-rayl)
12 3 4 8 10 12 14 1€ 17 16
^X-ray (A)
„ I i- -J
10 54 3 2.0 1.0 0.9 0.8 0.7 0.68 0.66
Figure 4. X-ray reflection spectra. Voltage GD: 2350 V, Current: 150 mA. Exposition time
18 000 s (a) X-ray spectrometer measurement diagram; (1) Cathode, (2) Be shield, (3) X-ray
cathode emission, (4) spectrometer chamber, (5) slit, (6) curved mica crystal, (7) X-ray film,
spectrometer, slit, (8, 9) reflected spectrum X-ray, (10) reflection spectra area, (b) Spectrum of
Al-D Glow Discharge system, (c) Ni-D, (d) V-D, (e) Pd-D, (f) Mo-D, and (g) Ta-D.
349
3. Discussion
Presumably, some long-lived excited levels with energies up to several keV are
formed in the cathode solid-state medium when its surface is exposed bombardment
E
E
o
• T ^ ^ * *
1
- 2
m E.
E •
in
d
4
.<#*
Figure 5. X-ray energy spectra areas with the spots from monoenergy X-ray beams (laser beams).
Pd-D Glow Discharge system, Voltage GD: 2350 V, Current: 150 mA. (a) Area of X-ray film
with the thermal and radiation destruction spots, (1) the normal darkness spots, (2) the spots of
solarization of the photoemulsion, (3) the spots of X-ray film destruction; (b, c) areas of X-ray film
with the normal darkness spots; (c, d) areas of X-ray film with the spots from intensity radiation
X-ray beams.
350
by the discharge plasma ions. These levels are characterized by fixed discreet values
of energy and lifetime. T h e registered X-ray emission results from re-excitation of
these levels. T h e spectral energy values of the recorded X-ray emission differs sig-
nificantly from L, M energies of internal electronic transitions for the given cathode
material. T h e formation of excited levels may be associated with the distortion of
the solid electron-nuclear system.
4. Conclusion
T h e results obtained show t h a t it is possible to create in the solid body optically
active medium with long-lived meta-stable levels with energy ranging 0.6-3 keV and
more.
T h e experimental research of this fundamental phenomenon has allowed to cre-
ate a basically new type of the device: "The X-ray solid-state laser with 0.6-0.8 nm
radiation wave length, 1 0 ~ n - 1 0 ~ 1 3 s duration of separate pulses, and, up to 10 7 W
beam power in the pulses.
References
1. A.B Karabut, Research into powerful solid X-ray laser (wave length is 0.8-1.2 nm)
with excitation of high current glow discharge ions, Proceedings of the 11 International
Conference on Emerging Nuclear Energy Systems, 29 September-4 October 2002, Al-
buquerque, New Mexico, USA, pp. 374-381.
A NOVEL LiF-BASED D E T E C T O R FOR X-RAY IMAGING IN
H Y D R O G E N LOADED Ni FILMS U N D E R LASER IRRADIATION
R . M . M O N T E R E A L I , S. ALMAVIVA, T . M A R O L O , M.A. V I N C E N T I
ENEA, Advanced Physics Technologies, C.R. Frascati, V.E. Fermi, 45,
00044 Frascati (RM), Italy
E-mail: montereali©frascati.enea.it
F. SARTO
ENEA, Advanced Physics Technologies, C.R. Casaccia, V. Anguillarese, 301,
00060 S. Maria di Galeria (RM), Italy
C. SIBILIA
Universita' di Roma "La Sapienza", Dipartimento di Energetica, Via A. Scarpa, 16,
00161 Roma, Italy
E. C A S T A G N A A N D V. V I O L A N T E
Associazione Euratom-ENEA sulla Fusione, C.R. Frascati, V.E. Fermi, 45, 00044
Frascati (RM), Italy
A novel soft X-rays imaging film detector, based on optically stimulated lumi-
nescence of active color centers in lithium fluoride, LiF, has been used to obtain
the image of radiation emitted from a nickel film, hydrogen loaded by electrolysis,
under light coupling with an He-Ne laser.
1. Introduction
An innovative film-like soft X-rays imaging detector, 1 based on optically stimulated
luminescence of radiation-induced active color centers (CCs) in lithium fluoride
(LiF) thin layers,2 has been used to obtain the image of radiation emitted from a
nickel film, hydrogen loaded by electrolysis, under light coupling with an He-Ne
laser.
The novel detector, recently proposed 3 and developed for soft X-ray micro-
radiography and microscopy applications, as well as for intense extreme ultraviolet
sources characterization, 4 consists of a radiation-sensitive thin film of LiF, ther-
mally evaporated on a glass substrate. Irradiation of this material with several
kinds of ionizing radiation, like charged and neutral particles (electrons, ions, and
neutrons) as well as gamma and X-rays, induces the stable formation of electronic
defects, known as CCs. 2 Primary and aggregate point defects are stable at room
temperature (RT) in LiF, and few of them emit intense visible photoluminescence
from the exposed areas, even at RT.
351
352
The peculiar optical and spectroscopic properties of this material allow imaging
with a sub-micrometric spatial resolution, simply by reading the green and red
photoluminescence of F j" and F 2 centers (two electrons bound to three and two close
anion vacancies, respectively) stored in the LiF-based imaging plate. Irradiation
with blue light excites the visible photoluminescence of the FJ" and F 2 defects
locally created in the areas previously exposed to the X-ray beam. The image can
be directly read in an optical microscope operating in fluorescence mode. 1 ' 4
2. Experimental
The LiF film (t = 1.9/zm) detector has been mounted in contact with the back-side
of a 1 mm thick polyethylene (PE) substrate, covered by a 45 nm thick sputtered Ni
film, previously loaded with hydrogen by electrolysis with 1 M Li 2 S04 electrolyte
in light water (40min, current ranging from 10 to 30mA). 5
The sample has been positioned on a rotating support and, by selecting the
proper incidence angle, a CW He-Ne laser (632.8 nm, 5mW) has been coupled in
the black metallic layer trough a glass cylindrical lens placed in close contact with
the Ni surface for an irradiation time of 3 h. In this configuration, the He-Ne light
can be coupled in the Ni metallic layer by tightly focusing the laser beam in the
contact region between the glass lens base and the black Ni surface and detecting
a reflectance minimum through a Si photodiode. A rough scheme of the entire
structure is sketched in Fig. 1.
After removing the imaging LiF sensor, a carefully inspection of its surface
has been performed in a conventional optical microscope operating in transmission
Figure 1. Sketch of the layered structure exposed to He—Ne irradiation. The upper triangle
represents the glass lens, and the underlying layer the Ni film surface roughness, responsible of
light coupling.
353
mode with white light illumination and in conventional fluorescence mode, under
blue light from a Hg arc lamp.
A more complete and detailed optical investigation has been performed in a
confocal laser scanning microscope (CLSM) Nikon Eclipse Cl-80i equipped with
a Coherent CW Argon laser operating at 458 nm, utilized to excite the photolu-
minescence of active CCs eventually produced in this radiation-sensitive thin film.
The CLSM system provides the opportunity to collect, acquire and store these im-
ages, and to reach a spatial resolution of few hundreds of nanometers at the used
wavelengths.6
Figure 2. Optical images of the exposed LiF film surface obtained in different microscope oper-
ation mode. Transmission mode, dark field, (a) Fluorescence mode, UV illumination, (b) Trans-
mission mode, white light, (c) Transmission mode, phase contrast, (d) Reference line = 50/jm.
354
Figure 3. CLSM optical image in fluorescence mode of the exposed LiF film surface. Reference
line = 100/im.
In the light-emitting areas of Fig. 2b, interesting features have been observed in
confocal laser scanning mode. The higher sensitivity and spatial resolution allows
us to identify several light-emitting spots, closely grouped, with typical spatial
dimension from tens to hundreds of micrometers, which are shown in Fig. 3.
The brightest areas are the same observed in Fig. 2b and could be attributed
to light scattering phenomena from dust and/or other surface imperfections, while
the observed fluorescent image appears ascribed to the photolumiiiescence of F j
and F2 centers, created by ionizing radiation impinging the LiF-based imaging film
during He-Ne irradiation of the Ni-Hydride film.
Surface plasmons (polaritons) are quantum of plasma oscillations created by
the collective oscillation of electrons on a solid surface. They may be generated
by mechanisms able to produce charge separation between Fermi level electrons
and a background of positive charges (i.e., lattice atoms). The coupled em wave
can produce coherent oscillations of the Fermi-level electrons in the metal lattice,
as its frequency is quasi-resonant with electronic plasma one. According with, 7
the excitation could produce local intense electric field, and soft X-ray emission at
energies below the Ni Ka edge (8.333 keV) can take place. The transmission of
a 1 mm thick PE substrate has been reported as a function of the X-rays energy
in Fig. 4 and it is not negligible for X-ray energies above 3keV. 8 Depending on
the X-rays energy, their penetration in LiF ranges from few tens of nanometers to
several hundreds of micrometers. 1 ' 4
Our novel detector integrates all the emitted radiation and indicates that its
production is confined in an area of spatial dimensions comparable with the coupling
355
1.0
0.8
I 0.6
tn
to
E
<ii
| 0.4
H
0.2
region between the evanescent wave and the black Ni surface. T h e spot n a t u r e of the
image in Fig. 3 would be compatible with localized radiation sources, as observed
in Ref. 9.
Acknowledgments
We are indebted with G. Baldacchini, F. Bonfigli and F. Flora for fruitful discussions
and with I. Franzini for useful suggestions.
References
1. G. Baldacchini, F. Bonfigli, A. Faenov, F. Flora, R.M. Montereali, A. Pace, T. Pikuz
and L. Reale, J. Nanoscience Nanotechnology 3(6), 483 (2003).
2. R.M. Montereali, Point Defects in Thin Insulating Films of Lithium Fluoride for Optical
Microsystems, in Handbook of Thin Film Materials, H.S. Nalwa (ed.), Ferroelectric and
Dielectric Thin Films, Vol. 3, Ch. 7, Academic Press, New York, pp. 399-431 (2002).
3. ENEA Patent TO2002A000575, G. Baldacchini, F. Bonfigli, A. Faenov, F. Flora, R.M.
Montereali, A. Pace, T. Pikuz and L. Reale (International N: WO 2004/005906 Al).
4. G.Baldacchini, S. Bollanti, F. Bonfigli, F. Flora, P. Di Lazzaro, A. Lai, T. Marolo,
R.M. Montereali, D. Murra, A. Faenov, T. Pikuz, E. Nichelatti, G. Tomassetti, A.
Reale, L. Reale, A. Ritucci, T. Limongi, L. Palladino, M. Francucci, S. Martellucci and
G. Petrocelli, Rev. Sci. Instrum. 76, 113104 (2005).
5. V. Violante, P. Tripodi, D. Di Gioacchino, R. Borelli, L. Bettinali, E. Santoro,
A. Rosada, F. Sarto, A. Pizzuto, M. McKubre and F. Tanzella, Proc. 9th Int. Conf.
Cold Fusion (ICCF9), Beijing, 19-24 May (2002).
6. A. Diaspro, Confocal and Two-Photon Microscopy. Foundations, Applications, and Ad-
vances, A. Diaspro (ed.), Wiley-Liss (2002).
7. V. Violante, A. Torre, G. Selvaggi and G.H. Miley, Fusion Technol. 39, 266 (2001).
8. http://www-cxro.lbl.gov/optical_constants.
9. D. Gozzi, F. Cellucci, P.L. Cignini, G. Gigli, M. Tomellini, E. Cisbani, S. Frullani and
G.M. Urcioli, J. Electroanalyt. Chem. 452, 253 (1998).
OBSERVATION A N D MODELING OF T H E O R D E R E D MOTION
OF H Y P O T H E T I C A L MAGNETICALLY C H A R G E D PARTICLES
ON T H E MULTILAYER SURFACE A N D T H E PROBLEM OF
LOW-ENERGY FUSION
STANISLAV V. A D A M E N K O A N D VLADIMIR I. V Y S O T S K I I
Electrodynamics Laboratory "Proton-21", Kiev National Shevchenko University,
Vladimirskaya St. 64, 01033, Kiev, Ukraine
1. Introduction
During the experiments at Kiev Electrodynamics Laboratory "Proton-21" on
achieving the superdense state of the matter (the state of electron-nuclear
collapse 1-3 ) by using the high-current electron driver, the traces of ordered thermo-
mechanical impact on surfaces of the "metal-dielectric-semiconductor" (MDS) tar-
gets, remote from the collapse zone, were registered. By their configuration, these
macrotracks are analogous to those observed on photoplates and presented in work.4
But the energy expenditures on the formation of the former turn out to be by many
orders higher. The origin of these macrotracks can be ascribed to none of the well-
known particles. Below, we present the results of the analysis of the characteristics
of these macrotracks and the properties of particles (particles with magnetic charge)
which can form macrotracks.
356
357
Cathode
Distant
Azimuth multi layer
magnetic target
field H( (MDS-structure)
Anode
Al Si0 2 Si plate
Figure 1. General scheme of the experiment.
Under the action of the pulse current, the zone of a collapsing part of the anode
substance is formed in the anode. 1 ' 2 A target was positioned at the distance of about
10 cm from the collapse region and was the standard MDS-structure consisting of
a Si plate covered by both a thin layer of SiC>2 and a thicker layer of Al. On
the surface of Al, we have found a very thin film of oil compounds (H, C), whose
origin is related to the operation of an oil vacuum pump. The registered object
was a macroscopic hollow track (channel) in the form of an oscillating trajectory
with a constant period A s=s 60/Ltm. This track deepens periodically in the target
volume through the Al layer (and partly through Si02) and appears on its surface,
by simultaneously oscillating with an amplitude of about 20 /iin in parallel to the
target surface. The total length of the continuous part of the track A « 2000/im, its
width is 3.5 /an, and the thickness is about 1.3 /im (approximately equal to the Al
layer thickness). On the target surface near the places of the periodic appearance
of the track from the volume of melted and then solidified Al, a small amount of
solidified Si is present. The direction of the symmetry axis of the trajectory of the
main extended track (consisting of two segments) corresponds to the vector of the
azimuthal magnetic field.
The general view of the shape MDS-structure surface with an oscillating track
and the separate fragments of the track on the surface and in the volume of Al
coating the Si substrate are given in Figs. 2-4. It follows from Figs. 2 and 3 that
the track is present only in those spatially separated regions of the target sur-
face (regions 1 and 2), where the Al coating is present on the surface. Moreover,
the tracks on these two regions were the obvious continuation of the trajectory of
a single moving nonidentifiable particle. At the same time, we see no evidences for
the interaction in the space between two regions with Al coatings. We note that
the Al layer is a paramagnetic, and two remaining layers of the MDS-structure (Si
358
Figure 2. The general view of MDS-structure with the tracks; (b) and (c) - fragments of track, 1
and 2 - thin Al layers on Si surface.
and Si02) are diamagnetics. Thus, the strong thermo-mechanical action occurred
only in the scope of the paramagnetic. This effect is clearly demonstrated in Fig. 4,
where we see the inlet of a track on the end surface of AL
The volume and mass of melted Al in the scope of the macrotrack are, respec-
tively, VAI ~ 10" 8 cm 3 . MAI ^ 2.7 x 10~~8g. The minimum energy which must be
spent for the heating and melting of Al in the volume of the macrotrack is
With regard for the additional energy spent for the heating and ejection of
Si, the heating of the remaining unmelted part of Al, and the ionization of all
the products in the region of the macrotrack, we can estimate the total energy as
Qtot ^ 2 x 105 GeV. The specific energy release is very great and equals
We note that results (1) and (2) differ by 106 times from the data presented in
Ref. 4.
1 «^
fettle
Figure 4. The photos of the same fragment of the track. Two l«ii photos present the inlet.of
track in volume of a Si02 layer.
Below, we will show that the simple braking of particles (including those with
magnetic charge) cannot ensure both the energy release (1) and (2) and the observed
form of tracks. The natural question arises: Which particle can form such a strictly
ordered track?
The invariable value of the period of oscillations of the trajectory of the type of
a "caterpillar trace" and the identical character of damages of the Al surface in the
limits of all the parts of the track testify to that the average linear velocity of the
nonidentifiable particle along the entire trajectory was constant. With regard for
all the features of the trajectory and the great energy release it becomes obvious
that the formation of such a trajectory can be related to two scenarios:
• The target surface has interacted with a particle possessing a great kinetic
energy W\ which exceeds the quantity Qtot by many times, and, therefore,
the great energy release dQ/dl did not affect Wk, the character of the
motion and interaction of the particle (e.g. this. particle consisted from
10 16 or more atoms with 0.1 eV moving energy which may cause totally
more than 105 GeV energy).
• The particle had a small velocity v and a relatively small kinetic energy
Wk, and the very great energy release registered in experiments and the
formation of a macroscopic track are related to that the moving noniden-
tifiable particle stimulated the running of energy-gained nuclear reactions
along the trajectory of motion.
The first scenario is logically contradictory and does not agree with experimental
data. This is conditioned by the fact that a particle with great kinetic energy
must have a great momentum. However, this contradicts the fact that the particle
changed the own trajectory and the direction of motion frequently and in the ordered
way. Moreover, we observe the very sharp change in the direction of motion (by
an angle close to 180°) at a single point. Such a character of motion corresponds
360
to particles with small energy and small momentum. But such particles cannot
execute the great work on the fracture of the target surface!
The second scenario seems to be more grounded, and we consider it in detail.
In the framework of this scenario, the hypothetical particle, whose interaction with
the target forms a specific macrotrack, must satisfy a number of requirements:
• The particle must stimulate the running of nuclear reactions with the very
great energy release and the local fracture of a target.
• The specific energy release stimulated by the particle should be the same
along the whole track.
• The particle must not participate in nuclear reactions, i.e. it must come
into the reaction zone and leave it in the invariable form.
• The particle itself must affect the formation of the own ordered trajectory.
• Its motion must be different in the paramagnetic and diamagnetic media.
It is obvious that such requirements do not allow one to identify the particle
under consideration with one of the known neutral particles or particles with electric
charge. There are very weighty reasons to assume that such peculiarities of the
interaction can be related to the motion of a particle with magnetic charge (it can
be one of the modifications of the Dirac monopole). Below, we will consider this
hypothesis in detail.
It is seen that dAWjjvi/dZ turns out 10 8 -10 9 times weaker than the experimen-
tally registered energy release dQtot/dl on the target surface. Hence, the released
energy cannot be directly related to the acceleration of the magnetic charge by the
magnetic field.
Consider the features of the interaction of such particles with a substance. The
formula for the specific loss of energy of a magnetic charge
Xsi = -0.53 x 10" 6 , X si0 2 = -1.13 x 10" 6 , XAI = 1-65 x lO" 6 , Xvacuum = 0.
(8)
The character of the interaction of a magnetic charge with the magnetic field
is defined by that any diamagnetic is pushed out from the region with the strong
magnetic field (this is equivalent to the repulsion of the magnetic charge from a
diamagnetic), whereas any paramagnetic is pulled in the region with a strong field
and, respectively, attracts the magnetic charge. This interaction yields that the Al
layer is a potential well for the magnetic charge, and the layers of Si and Si02 are
362
Si SiO„ Al Si SiO.
1
charge charge and after destruction
of Al layer
V(x)
Figure 5. Surface of MDS-structure and its potential energy before interaction with magnetic
charge and after such interaction.
potential barriers with different heights (if we consider the sliding fall of a particle
on the MDS-structure surface from the side of vacuum). To confirm the reality of
this interaction, we determine the height of the effective potential barrier, which
corresponds to the surface of a diamagnetic and is able to reflect a particle with
magnetic charge, if its kinetic energy in the direction normal to the surface is less
than the barrier height AW = iirxg2 /?*u- This value is defined by the difference of
the total energy of the magnetic field H(r) = g/r2 of the particle with a magnetic
charge g in vacuum and that in a medium with some specific value of the permeabil-
ity x- Here, rn is the minimum distance from the magnetic charge to the medium,
at which the idea of the permeability as a mean characteristic of this medium is
valid. We may accept that it equals the classical radius of an atom (rn ~ 0.5 A).
If we take into account that the typical value of |x| ~ 1 0 - 6 , then the height of
the potential barrier for a magnetic charge on the boundary of a diamagnetic and
vacuum is AW « 10 eV.
Consider a possible character of the interaction of a magnetic charge with this
structure (Fig. 5). We assume that the magnetic charge moves at first from right to
left at a small (sliding) angle 6 in the direction to the surface (Fig. 5a), so that its
relative kinetic energy (pg sin8)2/2Mg is less than the barrier height AW. While
approaching the surface, the magnetic charge is pulled in the region with Al due to
the attraction to the paramagnetic (Al) and then is pushed out away from the
potential barrier formed by the layers of SiC>2 and Si.
In the scope of the Al layer, this charge can stimulate the running of various
nuclear reactions, including the synthesis reactions Al + P 1 = Si 28 , Al 27 -|-C 12 ' 13 =
K 39 ' 40 with participation of Al, H, and C entering the composition of a very thin
oil film on the surface of Al and release of a great energy (A_ER = 12-17 MeV).
The running of these reactions is indirectly confirmed by the following.
363
Nucleus
r Typical electron
shell of an atom Electron shell of the
same atom in very
strong magnetic field
The detailed study of the isotope composition of the substance, being present on
the surface of Al on both edges (banks) of a periodic track, with the help of a SIMS
spectroscope revealed the presence of a very small amount of extrinsic elements,
whose mass corresponded to the isotopes with mass number A = 39 and 40.
Upon the application of a very strong magnetic field He (if Ee^(r) S> Ea{r) or
if Z <C 137), the electron shells of atoms take the needle-like form of extremely
elongated ellipsoids instead of those of the ordinary form close to the spherical one
(see Fig. 6). Their transverse axis (and screening radius) sharply decreases. The de-
crease in the transverse size of electron shells corresponds to the sharp decrease of
the electron screening radius r scree n and, respectively, to a very significant increase
of the probability of the tunnel effect upon the interaction with the nuclei of neigh-
boring atoms. This can lead to a sharp increase of the probability of reactions.
Figure 7. The trajectory of motion of a magnetic charge in a simplified form after its falling on
the MDS-structure surface in several periods of the spiral.
repulsion from the diamagnetic (Si02 and Si) and by the action of the magnetic
field of the current on the charge. In this region, a magnetic monopole moves along
the surface of Si not penetrating into the volume and not inducing any damage,
which is observed in experiments.
It is worth noting one more circumstance. In view of the form of a macrotrack
(great number of strictly periodic oscillations), we may conclude that the controlling
magnetic field is approximately the same along the entire trajectory. This corre-
sponds to that the duration of the formation of the mentioned part of the track is
significantly less than the total duration of the current pulse equal to T « 30-50 ns.
This allows us to assume that the duration of the formation of this part of the
track with the length L ?» 2 mm is at most T\ < 10 ns, and the mean longitudinal
velocity of motion of the hypothetical magnetically charged particle is greater than
L/Ti > 2 x 107 cm/s.
5. Conclusion
The above-presented scenario allows us to explain and to quantitatively substantiate
the majority of the observed regularities of oscillating hollow macrotracks, by basing
on the assumptions that magnetically charged particles are generated in the collapse
region in a hard-current diode and these particles can be highly efficient catalysts
of nuclear reactions. The periodic character of the macrotrack trajectory can be
related to the specificity of the interaction of the hypothetical magnetic charge with
the system of paramagnetic and diamagnetic layers on the MDS-structure surface.
Basing on the general reasoning, we may assume that the particles with magnetic
charge can be formed in the electron-nucleus collapse zone during the shock action
366
References
1. S.V. Adamenko and V.I. Vysotskii, Found. Phys. Lett. 17, 203 (2004).
2. S.V. Adamenko and V.I. Vysotskii, Found. Phys. 34, 1801 (2004).
3. S.V. Adamenko, A.S. Adamenko, and V.I. Vysotskii, Infin. Energy 9 (54), 23 (2004).
4. L.I. Urutskoev, V.I. Liksonov, and V.G. Tsinoev, Prikladnaia Fizika (Appl. Phys.) 4,
83 (2000) (in Russian).
E V I D E N C E OF SUPERSTOICHIOMETRIC H / D LENR ACTIVE
SITES A N D H I G H - T E M P E R A T U R E S U P E R C O N D U C T I V I T Y IN A
HYDROGEN-CYCLED Pd/PdO
A.V. M I T I N
P. Kapitza Institute of Physical Problems, The Russian Academy of Sciences,
Moscow 119334, Russia
Electron transport and magnetic properties have been studied in a 12.5 /Ltm thick
Pd foil with a thermally grown oxide and a low-residual concentration of hydrogen.
This foil was deformed by cycling across the Pd hydride miscibility gap and the
residual hydrogen was trapped at dislocation cores. Anomalies of both resistance
and magnetic susceptibility have been observed below 70 K, indicating the appear-
ance of excess conductivity and a diamagnetic response that we interpret in terms
of filamentary superconductivity. These anomalies are attributed to a condensed
hydrogen-rich phase at dislocation cores. The role of deuterium rich dislocation
cores as LENR active sites is discussed.
1. Introduction
Recently Ashcroft has presented arguments that hydrogen dominant metal alloys
may exhibit high-temperature superconductivity (HTSC) over a modest external
pressure range. 1 The advantage of saturated hydrides in terms of achieving HTSC
is that in a chemical sense it has already undergone a form of pre-compression and
once impelled by further external pressure to enter metallic phase, the electrons
from both hydrogen and metal may participate in common overlapping bands. 1
There is another approach to achieve a compressed, metallic hydride state with a
high-coupling constant and this is the topic of the work presented here. Dislocation
defects are strong, abundant traps of interstitial hydrogen and deuterium, as has
been previously demonstrated in small angle neutron scattering measurements. 2 - 4
*Also at Institute of Physical Chemistry, The Russian Academy of Sciences, Moscow 119915,
Russia.
367
368
the post-cycle annealed sample constitutes the foreground measurement and is re-
ferred to as Pd/PdO:H x below. The residual hydrogen concentration (x) was deter-
mined by thermal desorption analysis (TDA) using a procedure described elsewhere6
after the foreground resistance and magnetic susceptibility measurements. Current-
voltage characteristics were measured with the standard four probe technique over a
range of 4.2-295 K. The voltage was measured with Keithleyl82 digital voltmeter by
passing rectangular current pulses of 1-10 s through the sample with fixed amplitude
that varied over a range of 1-10 mA. Magnetic property measurements were per-
formed with IT-SQUID Quantum Design MPMS-3 using both DC-magnetization
and AC-susceptibility modes. Samples were mounted inside a gelatin capsule with
the applied magnetic field both parallel (H\\) and perpendicular (H±) to the foil
surface, the latter of which was measured with a sandwich of six pieces (resulting
in an effective sample thickness of 75 /im) to increase the total volume of material.
Thermal desorption analysis measurements of the Pd/PdOiHz and P d / P d O
samples are shown in Fig. 1. A sharp primary release peak near 430°C superim-
posed on a much broader peak is evident in the Pd/PdO:Ha; measurement. The
binding energies corresponding to the sharp and broad peaks are estimated as
£H = 0.65±0.10eV and £H = 0.16±0.05eV, respectively, using the Garlick-Gibson
model. 13 The higher energy is consistent with the result of Kirchheim for hydrogen
trapping at dislocation core sites in cycled Pd. 5 The lower energy is consistent with
1.60x 10
1.40x 10
1.20 x 10
i£ I . O O x io 7
a>
CO -8
c/> 8.00 x 10
CD
CL
1
6.00 x 108
4.00 x 10S
2.00 x 108
0.00
0 100 200 300 400 500 600 700 800
Temperature (°C)
28.0
24.0
20.0
0)
O
c
range 4.2 < T < 203 K. The non-linear behavior at low current (<0.0f mA) and
low temperature (<50K) indicates enhanced transport properties consistent with
uncorrelated supercurrents 16 that break down at high current and high tempera-
ture (T > 67K). In the present case, the non-linear behavior may be associated
with the suppression of weak superconductivity along a network of condensed hy-
drogen at dislocation cores analogous to a Josephson medium. Similar filamentary
superconductivity has been previously observed in high-Tc superconductors. 17 ' 18
DC susceptibility measurements of both samples are shown in Fig. 4. The
zero-field-cooled (ZFC) measurement of Pd/PdOiH^ at 1.0 and 1.5 Oe exhibits a
transition below ~70K, manifested as a reduction of the DC susceptibility (the
sharp increase in susceptibility below 5K is due to ferromagnetic impurities 19 and
non-stoichiometric oxygen in the PdO layer). This transition not present at larger
applied field, in the field-cooled (FC) condition, nor in the Pd/PdO ZFC background
measurement at 1.0 Oe. The transition is attributed to a diamagnetic contribution
to the paramagnetic response of Pd resulting from condensation of the trapped resid-
ual hydrogen. Additional proof is found in the magnetization versus applied field
372
15.0
-* 4.2 K
-* 13.5 K
-m 23.5 K
34 K
40 K
47 K
50 K
67 K
90 K
100 K
203 K
0.00
0.001 0.01 0.1
Current (mA)
Figure 3. Normalized voltage versus DC current characteristics, V(I), for the temperatures as
labeled. The normalized voltage is the ratio of y(Pd/PdO:Ha;) to V ( P d / P d O ) . Non-linear behavior
is observed below 0.01 mA for temperatures below 67 K.
shown in the inset of Fig. 4. The 5, 10, and 50 K measurements of the Pd/PdO:H x
sample exhibit an inflection between 5 and 7.5 Oe that are not observed in param-
agnetic materials. The change in slope is absent below 5 and above 50 K consistent
with the paramagnetic response of Pd containing ferromagnetic impurities.
AC susceptibility measurements were performed to provide a more sensitive
verification of the diamagnetic contribution. Real and imagninary AC suseptibility
components for the two samples are shown in Fig. 5. The real component of the
Pd/PdOiH^ is weakly diamagnetic below ~40K, while that of the Pd/PdO sam-
ple is weakly paramagnetic. The imaginary components differ as well, with the
Pd/PdOiH-E sample exhibiting a peak that is absent in the Pd/PdO sample. The
onset of the weak diamagnetic behavior and the peak in the imaginary suscepti-
bility coincide with a magnetic phase transformation. The diamagnetic response is
enhanced by a factor of 30 when the Pd/PdO:Ha; sample is perpendicular to the
applied AC field, as shown in the inset of Fig. 5a.
One possible origin of the diamagnetic response from Pd/PdOiH^ is magnetic
field expulsion due to skin effect under applied AC field. The skin depth is propo-
tional to 5(T) <~ [cr(T)] — 1/2, where <r(T) is the conductivity corresponding to the
resistance of Pd/PdOiH^ in Fig. 2. The estimated skin depth (S ~ 2.9-3.6 mm
over the temperature range of 5-60 K) is much greater than the effective sample
373
1x10
-5
6.4x10
-5 /
5.6x10
1x10 /'2K
4.8x10
O•
^4.0x10
5K
/ '• /
6 x 10 - — £3.2x10
/lOK/
8o" 50 K ,
(ft - -/
CO
4x10' ^•^
O 100 K
Q
2x10
0
if -L -L -L _L
0x10
0 50 100 150 200 250 300
Temperature (K)
Figure 4. DC susceptibility versus temperature for Pd/PdO:Ha; under ZFC at 1.0 Oe (open
boxes), 1.5 Oe (open triangles), and 5.0 Oe (solid diamonds), under FC conditions at 1.0 Oe (solid
circles), and for P d / P d O under ZFC at 1.0 Oe (open circles). Inset shows low-field magnetization
versus field at the temperatures as labeled.
thickness of 75 fan. Flux expulsion from the foil can account for at most 5% of the
observed diamagnetic response in the perpendicular field condition. We therefore
assign the diamagnetic transition observed in the AC susceptibility measurements
to the presence of a minute fraction of superconducting phase in the Pd/PdO:H^
matrix. Accordingly, the behavior of the low-temperature AC susceptibility in the
parallel- and perpendicular-field conditions is in agreement with two-dimensional
type II superconductivity when the coherence length is larger than the width of the
superconducting layer.20
The emergence of a superconducting network observed here is consistent with
McMillan's estimate of the critical temperature; 21
1.04(1 +A)
Tc = ((hw)/1.2 kB) x exp (2)
A - / i * ( l + 0.62A)
where (fko) ~ 58-105 meV is the characteristic average of phonon energy in the
condensed phase, A = A(Pd)+A(H) is the electron-phonon coupling constant from
the Pd and hydrogen subsystems, and fi* ~ 0.1 is the Coulomb pseudo-potential
374
Figure 5. Imaginary (a) and real (b) AC susceptibility versus temperature for P d / P d O : H z (solid
circles) and P d / P d O (open boxes) with parallel applied field. Measurements were performed with
H = 0, a driving amplitude of 1 Oe, and a frequency of 992 Hz. The real component of the
Pd/PdO:Hj; exhibits a slightly diamagnetic response below 40 K that is amplified by placing the
foil surface perpendicular to the applied field (5a inset).
that accounts for the repulsive effect between electrons. The values for (fku) and fi*
used here have been discussed previously.6 The electron-phonon coupling constant
is estimated as A = 0.89 for (x) = 1.8 based on a linear extrapolation of coherent
inelastic neutron diffraction data from Rowe et at6'22 The estimated Tc ~ 40-70K
agrees with the onset of both excess conductivity and diamagnetism observed in
the Pd/PdOtHz sample. 23
In summary, we have observed anomalies in the electron transport and mag-
netic properties in a deformed Pd foil with a thermally grown oxide layer and a
small residual hydrogen concentration trapped at dislocations. The anomalies are
375
Acknowledgments
This work was partially supported by the NSF under Grant No. DMR-9982520
and by New York Community Trust. The magnetic property measurements were
performed at the Frederick Seitz Material Research Laboratory at UIUC supported
by the U.S. Department of Energy under Grant No. DEFG02-91-ER45439. The
authors would like to thank Dr. A. Bezryadin (UIUC) and Dr. R. Prozorov (Uni-
versity of South Carolina) for useful comments.
References
1. N.W. Ashcroft, Phys. Rev. Lett. 92, 187002 (2004).
2. B.J. Heuser and J.S. King, J. Alloys Compd. 261, 225 (1997).
3. B.J. Heuser and J.S. King, Metal. Mater. Trans A 29, 1594 (1998).
4. M. Maxelon et al., Acta Mater. 49, 2625 (2001).
5. R. Kirchheim, Acta Metall. 29, 845 (1981).
376
F R A N C E S C O C E L A N I , A. S P A L L O N E , E. R I G H I , G. T R E N T A , G. D ' A G O S T A R O ,
P. Q U E R C I A , V. A N D R E A S S I , A N D O. G I A C I N T I
INFN-LNF Via E. Fermi 40, 00044 Frascati (Rome), Italy
E-mail: francesco.celani@lnf.infn.it
P. M A R I N I , V. DI S T E F A N O , M. N A K A M U R A , F . T O D A R E L L O , A N D E. P U R C H I
EURESYS, Via hero 30, 00129 Rome, Italy
A. M A N C I N I
ORIM SpA, Via Concordia 65, 62100 Piediripa (Macerata), Italy
P. G. S O N A
Via S. Carlo 12, 20090 Segrate (Milan), Italy
F . F O N T A N A , L. G A M B E R A L E , A N D D. G A R B E L L I
Pirelli Labs SpA, Viale Sarca 222, 20126 Milan, Italy
E. C E L I A , F . F A L C I O N I , M. M A R C H E S I N I , A N D E. N O V A R O
CSM SpA, Via di Castel Romano 100, 00129 Rome, Italy
U. M A S T R O M A T T E O
ST Microelectronics SpA, Via Tolomeo 1, 20010 Cornaredo, Italy
In the framework of anomalous effects coming out because very close interaction
of some specific gas [usually Deuterium (D), some times hydrogen (H)] with some
specific solid materials [usually Palladium (Pd), some times Nickel or others] is an
emerging evidence that the physical condition at the surface of the host element
play a crucial role. It has been experimentally demonstrated, by Yoshiaki Arata at
Osaka University, that nano-particles of Pd, embedded in a matrix of Zr02, are able
to absorb extremely large amounts of H and/or D, at even room temperature and
pressure. Because of such results, we re-analyzed some of our previous experiments
under the new point of view and were convinced that most of our "positive" results
in Condensed Matter Nuclear Science come because of lucky, specific condition of
our Pd cathode. We decided to improve the quality of Pd, from the point of view
of production of nanostructure at its surface as large (and stable) as possible, in a
controllable way, using both electrolytic procedure and special preparation of Pd
before the use. Some of our efforts seemed to give positive results, although the
stability at long time as to be improved.
377
378
1. Introduction
In the framework of Condensed Matter Nuclear Science, it has been recently shown,
by Yoshiaki Arata at Osaka University,1 that nano-structures of metallic palladium,
stabilized in a matrix of ZrC>2, can rapidly absorb surprisingly large amount of H 2
or D 2 .
According to Arata's results and to the Akito Takahashi2 theoretical model,
atomic ratios (H, D)/Pd ;§> 1 can be easily accomplished at a pressure of only
a few bars into Pd nano-particles, stabilized in a Z r 0 2 matrix. In the Arata's
experiments, together with the abnormally high D/Pd ratios, a remarkable excess
heat and production of 4 He were detected.
On the basis of such results (and new deeper interpretation of some of our pre-
vious experimental results 3 that, although quite interesting from the point of view
of experimental effects, did not get at that time a satisfactory explanation), we are
now convinced that most of the high loading ratios (H-D/Pd) and/or anomalous
effects, both thermal and nuclear (by using D), obtained (generally in a not repro-
ducible way) by the people involved in cold fusion experiments, can be reasonably
attributed to the spontaneous and uncontrolled growing-up of fractal nanostructures
on the Pd surface.
In our opinion, even the Sr and Cs transmutations obtained in the experiments
carried out by Iwamura et al.A at Mitsubishi Heavy Industries, Yokohama, Japan,
which occur on the surface of the P d / P d - C a O / P d multilayer, could be due to
the formation of fractal-like structures produced during the multilayer fabrication
process.
The present work deals with experiments aimed at the production of nano-
structures on Pd wires both by anodic oxidation (in situ) and air oxidation (in situ
and ex situ).
2. Experimental Procedures
2.1. Cells and Electrolytes
The cell geometry and the experimental set-up were reported in detail in our pre-
vious papers.5"8Along the last year, about usual electrolytic experiments, we make
two specific one in order to compare and cross check the results about new elements
detected by ICP-MS, using light and heavy electrolytes. The cell and experimental
set-up were almost the same as described in Refs. 5-8. We just changed the compo-
sition of cell (from chemical glass to quartz) in the last experiment with deuterium
(b-type), as detailed in Ref. 8.
(1) Hydrogen loading: main solution 750 cm 3 (C 2 H 5 OH 95%, H 2 0 5%);
Th(N0 3 ) 4 = 5 cm 3 (with 1 cm 3 = 1 mg of Th in D 2 0); Hg 2 S0 4 = 7 cm 3
(concentration 1 0 - 3 M, in D 2 0) - Chemical glass (Schott Duran like, brand
Fortuna) cell.
(2) Deuterium loading: main solution: C 2 H 5 OD = 1005 cm 3 , D 2 0 = 89 cm3;
Th(N0 3 ) 4 = 6 cm 3 (with 1 cm 3 = 1 mg of Th in D 2 0 ) ; Hg 2 S0 4 = 8 cm 3
379
28ago05a-10_17
1.8
120
1.6
E
8 1.4
Of
-40
1.2
-80
-120
1
Figure 1. R/Ro ratio versus time using optimized anodic oxidation and electrolyte composition.
The solution is quite insulating (main liquid is vacuum-distilled andlOO nm filtered C2H5OH+H2O,
few salt are dissolved): the cell voltage is 135 V even at only 30 mA with an anode-cathode distance
of 4 cm.
These results indicate that a proper anodic oxidation produces a very active
surface. On the basis of Arata experiments, such activity could be explained as due
to the formation, just at the surface of the wire, of something similar to Arata's
true nano-particles (embedded in a matrix of ZrO^)-
Table 1. Main new elements detected in light alcohol-water (Scott Duran type) and heavy
alcohol-water (quartz) cell. All the reagents Th(NOs)4 (at 1 rng/ml concentration) and Hg2S04
(10~ 3 M) are i n D 2 0 . BKG and reagents subtracted. 1 Count = about 5 X 10 1 0 atoms. In bold
characters are reported value of new elements, about deuterium experiments, larger than a
factor 10 in respect to hydrogen one.
19-20JAN05
2.68 x10 5 2.7 x105 2.72 x10 5 2.74 x10 5 2.76 x10 5 2.78 x10 5
Time (s)
Figure 2. R/Ro versus time (seconds) with the effects of D2 - ^ A r ^ D 2 intake and anodic stripping
current (A). The values of R/Ro are "twin" because we introduced the procedure to measure also
the Resistive Thermal Coefficient (RTC), see later.
382
the deuterium dissolved in the solution and the R/Ro increased from about 1.05 to
about 1.405. At the time 273,500 s large amount of Argon gas was introduced, by
bubbling it inside the solution. Immediately, the R/Ro started to decrease. At the
time 275,500 s, after the R/Ro decreasing (because of argon effect) from 1.405 to
1.375, D2 gas was added again. The R/Ro value again increased, showing reversible
and controllable effects. At the time 277,300 s, when the R/Ro increased to 1.45,
the intake of D2 was stopped and Argon was added again. At the end, another
anodic de-loading was carried out (at -6 mA) in order to fully de-load the wire.
Moreover, observing Fig. 3, we would like to stress that there is unquestionable
experimental evidence that the spontaneous self-loading following anodic oxidation
reaches values of D/Pd over the well-known thermodynamic limit. In other words,
we expected a R/RQ ratio less than 1.8 but we observed a value much larger, close
to 1.95-2.0. Such value is equivalent to a deuterium pressure of about 8-10 times
larger than 1 bar, i.e. the D2 pressure used in the cell (e.g. time 287,000-300,000 s).
19-20JAN05
0.002
- -0.008
the value in such experiment because we decided to "monitor" the value of the
residual stress versus time.
Figure 4. SEM picture of Pd virgin wire, before electrolysis. The wire is contiguous to used one
of Fig. 4.
It is clearly shown the problem coming out from anode dissolution and its deposit
at Pd cathode surface. Such deleterious effect, in respect to H and D absorption in
Pd, is not yet solved (despite our deep efforts). We recall that, unfortunately, the
over-volt age of H and D at Pt surface is close to zero. We are convinced that one
of most important reasons of poor deuterium loading into palladium, as reported
from several researchers, is very often the platinum coating (from the anode) at
palladium cathode surface, specially at large current density (over 500 mA/cm 2 in
water solution).
It is interesting to note that, apart sensitivity, the same elements are detected
from both SEM and ICP-MS. In other words, the ICP-MS results are "safe" and
are not instrumental fakes.
384
Figure 5. SK\! picture of a usf\l wire, heavy solution clc-tmlysis. The "new" HIMIUMIIS and P t
deposit (from anode) are concentrated in few spot area (about 15% of wire length).
tests, we realized that large self-loading occurred only at the end of certain anodic
cycles, in specific electrolytes. In particular, we found that the self-loading effect
obtained with water electrolytes was almost negligible (R/RQ « 1.1), while with
hydro-alcoholic electrolytes, both a- and b-types, the effect was higher. By opti-
mizing the anodic cycle it was possible to reach self-loadings up to R/RQ = 1.75
(left-hand side of the Baranowski curve) with H 2 and R/R0 = 1.95 (left-hand side
of the Baranowski curve) with D2.
5000
Pt
Counts
0.000 keV
20.480
Figure 7. SEM elemental analysis of one of "white" area has shown in Fig. 5. The, unwanted,
large deposition of Pt at Pd surface is clearly detected. Moreover, also Zn and Cu, detected by
ICP-MS analysis, are re-confirmed.
01-03MAR05_KI
I
a&%Stt)»»a«S&>
1.8 * - -
0.6
1.6
cf?
- 0.4
1.4 1
- R/Ro_d
|
1.2 0.2
0
fe^SU^SSSUKSS*
4 5 s s 5
5x10 1x10 1.5 x 1 0 2 x10 2.5 x 1 0 3 x10s
Time (s)
Figure 8. Loading characteristic of a virgin palladium wire: loaded at room temperature with
lbar of deuterium gas. In order to "activate" the Pd surface, it was made a preloading cycle (from
time 0 to about 60,000 s) with D2 gas, 293 K, 1 bar and later allowed to decrease, very slowly, the
deuterium content in the cell. Even neglecting the activation time, the time needed to reach the
thermodynamic limit of R/Ro = 1-82 is as large as 220,000 s. Such values (i.e. R/RQ and time)
are in agreement with data usually reported in the literature. As standard in our procedure from
about 2 years, we cyclically inject electromigration ac current (square wave, 10 kHz) with low
(about 10-15 m W ) and high power (700-800 mW) in order to calculate the Resistive Thermal
Coefficient versus D / P d ratio.
After such a heat-treatment the wire was immerged into a diluted solution of
colloidal silica, and then heated-^cooled^heated^cooled again several times.
2.3.2. Measurements
Virgin Pd wires (no treatment) exposed to D2 gas at 1 atm and ambient tempera-
ture, usually reach a maximum loading, corresponding to an electric resistance ratio
R/R0 « 1.82, in over 2 days (Fig. 8).
387
19APR05.196
0.15
0.05
Figure 9. Loading ratio versus time of a Pd wire treated by oxidation and silica. D gas loading
(1 bar).
It was also found that if during the treatment procedure of the wires, the step
involving the immersion in colloidal silica is omitted, the loading rates are signifi-
cantly lower and after a couple of hours R/RQ starts to decrease (de-loading).
3. Safety Rules-Procedures
The following procedures have to be carefully followed to avoid explosions because
possible mixing of hydrogen (and or deuterium) with oxygen and highly catalytic
effect of palladium surface, activated because growing of nano-structure at its sur-
face.
We remark the safety procedures are quite easy in our experimental setup be-
cause we take fully advantage of our procedure to measure both the R/RQ value
and the Resistive Thermal Coefficient (RTC) of Pd wire versus loading (see our
388
reports at, Asti5, ICCF11, and JCF6 for further details). In such a case, we used
the ratio between the RTC value made by injecting alternatively low (about 15 mA
equivalent to about 10 mW of power dissipated, called R/R0JL) and high (about
120 mA, equivalent to abut 700 mW power dissipated, called R/R0J1) AC current
along the thin Pd wire. Because very different thermal conductibility of gas was
adsorbed (H 2 , D 2 , He, Ar, Air, and "vacuum"), after proper calibration once for
ever, it is very easy to understand the real composition of gas atmosphere inside
the cell.
(2) Increase, slowly, the DC I_electromigration (/.em), from 0 to 350 mA, keep-
ing Ar flux at low values.
(3) Observe deloading.
(4) Wait for complete deloading (10-30 min, depending on wire coating). De-
crease 7_em from 350 to 0 mA.
(5) Check R/RQ-L value: if close to 1.0, go to step 6, otherwise wait until full
deloading by injecting 7_em again at large value (350 mA).
(6) Intake of He for test: the ratio of R/RQJI versus R/R0-L as to decrease
largely in respect to Ar filling, due to the larger thermal conductivity of
He(142.64 mW/m*K) in respect to Ar.
(7) Make vacuum (e.g. oil-free membrane pump, limit about 10 mbar) to pump-
out He.
(8) Intake of dry air (thermal conductivity, at 0°C 1.013 bar, 23.94 mW/m*K)
at STP. I.em = 0 mA. Measure R/R0-L only.
(9) Increase Lem from 0 to about 600 mA. Wait 1 m at 600 mA. Observe
the R/RQ instantaneous increasing due to large Lem: R/Ro about 3. At
R/Ro = 3 the wire temperature is about 700°C.
(10) Decrease slowly (in about 2 m) /.em from 600 to 0 mA. Repeat the cycle
three times.
(11) Check the R/Ro value and recalibrate the value, if necessary.
389
4. Conclusions
According to us, almost all of positive experimental results (excess heat, trans-
mutation, and particle emissions) in cold fusion experiments (Fleischmann, Taka-
hashi, Arata, Iwamura, Mizuno, Celani, McKubre, Swartz, Storms, Preparata-De
Ninno-Del Giudice, Miley, Violante, etc.) can be rationalized as the effect of nano-
structures at the Pd surface.
It is very difficult to produce such nano-structures (almost all, except Arata,
Iwamura, and Celani) obtained just by chance. Moreover, such nano-structures are
not stable over time.
We begin to develop a simple procedure to obtain nano-structures, both by
electrolysis (routinely produced also during the usual cathodic regime: specific elec-
tronic circuit and procedure developed from our Group since 2004, patenting) and
by addition of colloidal silica on oxidised Pd surface (since March 2005, gas load-
ing). In some aspects, the latter method is similar to Yoshiaki Arata procedure that
was the Pioneer about nano-particles production for cold fusion studies. The kind
of colloidal silica (5-10 nm dimension, low Na content), that up to now gives the
best results, was specially developed (after 5 years of efforts), by an Italian chemical
company, according to our request.
We think that the nano-structure interpretation of anomalous effect in deuter-
ated metals will bring soon to some technological device: boiler using liquid elec-
trolyte, even some turbine engine using pressurised high temperature gas loading
method.
More systematic work is necessary in order to elucidate all the possibilities that
come because nano-size materials (specially pure Pd and/or Pd-based alloys) prop-
erly coated/embedded by a third element.
Finally, as shortly shown also during ICCF12, we get indications that some
anomalous heat seems coming out, from a new pressurised (4 bar) cell (SS), using
even the hydrogen gas when the temperature of the wire, heavy coated by colloidal
silica, was forced to reach about 200°C (by Joule heating).
390
Acknowledgements
We are really indebted to Prof. Akito Takahashi (Osaka University, J a p a n ) , Prof.
Yoshiaki A r a t a (Osaka University) and Dr. Yasuhiro Iwamura (Mitsubishi Heavy
Industries, J a p a n ) , because stimulating discussions, critics and suggestions about
the role of nanostructures in Condensed Matter Nuclear Science experiments. We
cannot forget t h a t the pioneer work of Prof. A r a t a about nano-particles (starting
with the use of "palladium black" at different grain sizes) which opened our eyes
about new interpretation of some of our old d a t a t h a t never get satisfactory expla-
nation. Other general and long discussions with Prof. H. Y a m a d a and S. Narita
(both at Iwate University, J a p a n ) , Prof. A. K i t a m u r a (Kobe University, J a p a n ) ,
Prof. T. Mizuno (Okkaido University, J a p a n ) , Prof. S.E. Jones (BYU, Utah, USA),
Dr. E. Storms (Lattice Energy LLC, New Mexico, USA) helped us to elucidate the
very complex behaviour of P d surface during and after, very different, electrolysis
operating conditions. Dr. W . Collis (Heidi Limited, 14055 Boglietto di Costigli-
ole, Italy) helped us during the very long a n d tedious analysis of possible elements
coming out by ICP-MS instrument. T h e special software program (ENSAT) he
developed, about possible "transmutation" channels, was really useful to speed-up
the analysis.
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6. F. Celani et al, Further tests on composition and isotopic anomalies when Pd thin
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391
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7. F. Celani et al., Innovative procedure to measure, in situ, resistive thermal coefficient of
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Pd-D(H) electrolysis cells, Proc. of the ICCF11, Marseilles, France, 01-05 November
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also at h t t p : / / wwwcf.elc.iwate-u.ac.jp/jcf/
9. F. Celani, A. Spallone et al. Proc. of the 4 Meeting of Japan CF Research So-
ciety, 17-18 October 2002, Japan (Edited by H. Yamada), pp. 17-21, also at
http://wwwcf.elc.iwate-u.ac.jp/jcf/
USING RESISTIVITY TO M E A S U R E H / P d A N D D / P d LOADING:
M E T H O D A N D SIGNIFICANCE
M . C . H . M C K U B R E A N D F.L. T A N Z E L L A
SRI International, Materials Research Laboratory, 333 Ravenswood Avenue, Menlo Park,
CA 94025, USA
E-mail:michael.mckubre@sri.com
The resistance ratio method is the most frequent technique used to determine
the extent of interstitial loading of hydrogen or deuterium atoms into palladium
electrodes, or extended structures used in electrolytic or gas phase cold fusion ex-
periments. Specifically, advantage is taken of an empirical relationship between
the measured resistance, R, normalized to that of the same body at the same
temperature in the absence of hydrogen isotope, Rg, hence R/Ro, and the atomic
fraction occupancy of octahedral interstitials, x = H / P d or D / P d . This method
was first suggested and employed in cold fusion studies by the present authors, and
received immediate and widespread acceptance because of the ease with which this
experimental technique could be used to make in situ, real-time measurements of a
parameter, D/Pd, anticipated or hypothesized at that time to relate to cold fusion
heat excess or nuclear production. We take up this topic again 15 years later in an
attempt to clear up some errors and misunderstandings regarding the resistance
ratio method and its application in cold fusion studies. The relationship between
R/Ro and x is empirical. That is, calibrations are only as good as the experi-
ments that support the shape of the curve and cannot be used outside the range
(P, T, x) in which data are taken. The original calibration (unaccountably and
erroneously immortalized as the "famous Baranowski curve") involved an extrapo-
lation of known data into the region of cold fusion interest in the D - P d system, at
x > 0.6. Present theory and results focus new attention on the very high loading
region as x approaches or even exceeds unity, where double occupation of octahe-
dral sites, tetrahedral site occupancy, new phase formation or new electrical states,
may be relevant to the underlying physical process of excess heat and nuclear pro-
duction. Rather than simply using the resistance ratio as a qualitative tool to
determine whether an electrode is better or lesser loaded, it is now important to
obtain accurate quantitative information for x close to unity. With further exper-
imentation and analysis of published data it is apparent that the curve originally
published in 1990 is in error in the high loading condition. This paper describes
how this empirical fit has been improved over the years for both H / P d and D / P d
by employing new data, new analysis of old data, new experimental methods and
results.
1. Introduction
The first paper drawing attention to resistance ratio measurement as a means to
quantify deuterium loading in Fleischmann-Pons electrolytic cold fusion experi-
ments was presented by the present authors at the First Annual Cold Fusion
392
393
Conference held in Salt Lake City in March 1990, and published in the ensuing
proceeding.1'* The authors of that paper made three introductory comments:
1. None of the "cold fusion" electrolysis experiments described to data con-
tain any means of determining the D/Pd content in situ. Yet this ratio
may be a crucial difference between those experiments that have produced a
Fleischmann-Pons effect and those that have not.
2. The resistance of Pd metal is a function of its hydrogen content and is in
principle, the easiest way of determining the state of the Pd electrode as the
experiment proceeds. 7
3. The relationship between the resistance and the D/Pd ratio is known only up
to 0.65. Comparison can be made with the H/Pd system which is calibrated
in resistance up to H/Pd = l.l. 8
The first two comments proved to be prophetic. A clear distinction can be made on
the basis of average D/Pd loading measured by resistance ratio between successful
and unsuccessful excess heat production in electrolytic Fleischmann-Pons experi-
ments. Resistance ratio measurements quickly became and remain the most widely
used method of determining loading in situ. Here we expand point 3.
2. Experimental
In 1990 the resistance versus composition function had been characterized for the
light hydrogen system up to H/Pd = l.l. 8 This function was less well specified
for D/Pd. Our initial attempt to estimate the curve based on known data 9 up to
D/Pd = 0.65 combined with the assertion that the resistance ratio maxima would
occur at the same composition of H and D, resulted in the somewhat distorted curve
presented at ACCFl 1 and replotted here as Fig. 1. The fourth-order polynomial
extrapolation plotted as a grey line in Fig. 1 formed the basis of all early estimates
of D/Pd loading from resistance ratio measurements.
Between 1990 and 1993 a campaign of measurements was undertaken to refine
the calibration of the resistance curve for D/Pd. A number of methods were used to
measure composition independent of resistance in the D/Pd system, each with im-
portant advantages and disadvantages. Some of these methods are briefly reviewed
here:
I. Macro-gravimetric. The most direct method to determine the extent of ab-
sorbed hydrogen isotope is to weigh the cathode after prolonged loading. Both
the resistance and mass measurement can be performed ex situ after washing
and drying the electrode. The primary disadvantages being relatively low
accuracy because of systematic errors due to the presence of surface adsorbed
non-hydrogen species and absorbed but non-interstitial hydrogen, and the
lack of access to the high loading region because of rapid deloading.
*Although the atomic ratio D / P d had been anticipated 2 and hypothesized 3 - 8 at that time to
relate to cold fusion heat excess or nuclear production.
Micro-gravimetric. An in situ gravimetric measurement was reported by NRL
also at ACCF1. 2 Cheek and O'Grady used a quartz crystal microbalance to
measure the mass of a deposited palladium surface film operated as a cathode.
A critical difficulty with this method is the lack of access to the high loading
region due to buoyancy effects associated with the presence of internal D 2 -
filled voids and surface attached D 2 bubbles at current densities sufficient
to produce high loading. This method is also affected by roughening and
spallation of the Pd film from the quartz support at high loading and has
seldom been used.
Dilatometry. A number of people but notably Storms 10 took advantage of the
lattice expansion that occurs when hydrogen isotopes occupy the octahedral
interstitial sites in the fee Pd lattice. Either linear extension or volumetric ex-
pansion measurements can be used to estimate the extent of hydrogen isotope
absorption provided this is wholly interstitial. A very important outcome of
the extensive work by Storms using the technique was that a significant frac-
tion of the hydrogen or deuterium atoms absorbed by palladium recombine in
closed voids within the metal causing compressive stress and volume expan-
sion greater than that attributable to the change in lattice parameter. Storms
called this parameter "free volume". Electrodes with a large fraction of free
volume tend to load poorly and to not produce excess heat. 10
Oxygen displacement in closed cells. The equations that govern the cathodic
absorption of H (or D) in thermodynamically closed cells can be written for
2.1
CD
1.6
V \
V_ \
CD
o 1.5
c \
CO
1.4
*—>
c/j
CO 1.3
CD
cr 1.2
1.1 V
1.0 i. !
0.1 0.2
-- -r - ^ r
* "' - _ .
0.3' '"0.4
- 1 U .. rn
J • i i I ill 111 LiH
0.5 0.6 0.7 0.8 0.9 1.0 1.1
Mole fraction (H,D)/Pd
Figure 1. Original calibration curves. 1
395
we have constructed new curves for H-Pd and D-Pd in the high loading region.
These curves are presented in Fig. 5. Also plotted in Fig. 5 are the equilibrium gas
pressures needed to achieve the specified atomic ratios.
The square points in Fig. 5 taken from the Baranowski data 19 exhibit an inter-
esting kink or second order transition at D/Pd > 1.02. The origin of this feature
is not known although it appears not to be present for H in the same region of
composition.
Another attempt to specify the resistance/loading functions for palladium made
by Zhang et al.21 resulted in the curves replotted in Fig. 6. While the difference be-
tween the Zhang and SRI curves is subtle we believe that Zhang's curves fall outside
the uncertainty in the literature data for H 20 and the precision of the Baranowski
data for D. 19 It is also notable, although not diagnostic, that Zhang's curves for H
and D exhibit maxima at different atomic ratios (cf. rule "2"above).
A test of accuracy of the H-Pd curve was made directly by Tripodi and the
present authors. 22 The coulometric stripping method described in method V above
was used to directly correlate resistance and loading of two sections of fine Pd wire
cathodes (diameter 50 ^m, length 10 cm) loaded to H/Pd « 0.98, sealed by co-
deposition of Hg 12,13 and then stripped at very small anodic current density. The
results shown in Fig. 7 do not provide a strong basis to distinguish between the
Zhang and SRI curves. The knee at H/Pd ~0.57 is interesting and appears to
be a real feature. Because of this knee, Zhang's attempt to accommodate data at
loading H/Pd < 0.6 (not attempted by SRI) appears to have moved their predicted
resistance maximum to lower loading and higher maximum value.
3. Discussion
The various attempts to characterize the position of the resistance versus loading
curves for H-Pd and D-Pd can be summarized in terms of a few critical constants:
1. The maximum resistance value of the resistance ratio, -R/_Romax-
2. The value of the atomic ratio at the point of maximum resistance, x m a x
3. The value of the resistance ratio at a loading x = 1, R/Ro x=\.
Table 1 shows how values of these constants have changed in 16 years of exper-
imentation and analysis.
RIR
° 1 +3x-15.13x 2 +44.16x 3 -49.12x 4 +17.58x 5
FURo T1-2.0HFI-3
2
Figure 4. Showing the correlation between maximum loading measured by resistance ratio and
successful (red) and unsuccessful (green) heat production in Fleischmann-Pons electrolysis exper-
iments performed at SRI.
Some changes have occurred in the curve for H-Pd; a small increase in the
resistance maximum and a significant increase in the position of the maximum for
the SRI curve but not for Zhang's. Of far more significance to cold fusion workers
Figure 5. Improved calibration curves based on new data, reanalysis of H-Pd literature 2 0 and
Baranowski data for D-Pd (square points 1 9 ).
400
1
o.2o 0.30 0.40 0.50 0.60 0.70 0.80 0.90 1.00
Atomic ratio
Figure 6. SRI 2 0 and Zhang et al.21 curves and Tripodi et al.22 stripping data.
the value of the resistance at H/Pd = 1, R/RQ X=I, has dropped from ~1.35 to
1.067 for the SRI curve and below unity to 0.926 for Zhang's curve.
Turning attention to the D-Pd system the expected value of maximum resistance
has changed very little with reanalysis. The position of maximum resistance in D -
Pd has increased following that of H-Pd for the SRI curve using rule 2. The increase
in this parameter for Zhang's curve is even larger. Of much greater significance in
cold fusion studies the expected resistance at D/Pd = 1 has dropped from 1.5 in
1990-1994 to 1.43 in 1996 to 1.245 in the SRI curve circa 1998. The value for Zhang
calibration published in 2002 is even lower at 1.222.
The combined effect of moving the position of the resistance maximum to higher
loading, and the expected resistance at D/Pd = 1 to lower resistance value results in
a much steeper calibration curve on the right-hand side of the resistance maximum.
As a consequence, when comparing the old calibration to the new, resistance ratio
values interpreted as loadings in the region of interest for Fleischmann-Pons effect
studies (D/Pd > 0.85) have consistently overestimated the interstitial deuterium
content of the palladium. This systematic error is not large, but it may have
important physical significance.
Table 2 recalculates the maximum loading based on the minimum resistance
ratio measured on the right-hand side of the resistance maximum for five historic
heat producing cells operated at SRI. 12 What had previously been interpreted as
maximum average loadings at or above unity when evaluated with the new SRI
calibration curve result in loadings D/Pd approaching unity. Only P l a indicates a
D / P d m a x > 1. This cell was operated at 4°C where the calibration curve is likely
to be different. In any case, the calculated loading maximum is not outside the
estimated 1% uncertainty. Thus, in experiments conducted at SRI, we have no
evidence that palladium cathodes can be loaded by electrolysis to atomic ratios
greater than unity.
At this point it is worth discussing what is the relevance of a resistance ratio
measurement of deuterium loading. The evidence is overwhelming that deuterium
does not load homogeneously into polycrystalline palladium. Observations made
of Pd cathode surfaces reveal that different crystalline facets load and expand at
different rates, and the grain boundaries absorb (and release) D at very different
rates from the bulk. Electronic transitions observed at low temperatures in highly
loaded thin wires clearly indicate the presence of small zones of very differently
(presumably higher) loaded material. 14 Hot spots observed either in situ with ther-
mal imaging or retrospectively by autoradiography, 1 and local melting or isotopic
effects, all suggest that the Fleischmann-Pons effect, whatever its cause, occurs
heterogeneously throughout the bulk or on the surface. Indeed, since deuterium
flux appears with equal footing to loading in quantifying excess heat power,23 the
existence of heterogeneity (or time variability) in surface chemical potential appears
to be crucial in producing excess heat in electrolytic D-Pd experiments.
Given these observations and the occasional solid report of excess heat at
low loading one might question the deterministic power of four terminal macro-
resistance ratio measurements that necessarily access a volume averaged electrode
property. What might be important is simply that this property is monotonically re-
lated to the chemical potential of deuterium in the sample. The various mechanisms
involved in attempts to explain the Fleischmann-Pons heat effect, the existence of
a new phase or band structure, atom or ion pairing, lattice deformation to produce
occupiable host sites, all depend critically on the chemical potential of absorbed
References
1. M. McKubre et al., Calorimetry and electrochemistry of the D-Pd system, in Proc.
First Annual Cold Fusion Conference, Salt Lake City, F. Will, Ed. (1990).
2. G. Cheek and W. O'Grady, Quartz crystal microbalance study of Pd/H interactions,
ibid.
3. G. Preparata, Theoretical ideas on cold fusion, ibid.
4. P. Hagelstein, Status of coherent fusion theory, ibid.
403
5. S. Chubb and T. Chubb, Quantum mechanics of 'cold' and 'not-so-cold' fusion, ibid.
6. J. Schwinger, Nuclear energy in an atomic lattice, ibid.
7. D. Macdonald, M. McKubre, A. Scott, and P. Wentrcek, Continuous in situ method
for the measurement of dissolved hydrogen, I&EC Fundamentals 20, 290 (1981).
8. B. Baranowski and R. Wisniewski, Phys., Stat. Sol. p. 539 (1969).
9. F. A. Lewis, The Palladium-Hydrogen System (Academic Press, New York, 1967).
10. E. Storms, Fusion Technol. 29, 261 (1996).
11. A. M. Riley et al., Measurement of absorption of deuterium in palladium during
electrolysis of heavy water, NCFI Final Report II, 2-123 (1991).
12. McKubre et al, EPRI TR-104195 (1993).
13. A. Spallone, F. Celani, P. Marini, and V. Di Stefano, New electrolytic procedure for
the obtainment of very high H/Pd loading ratios, Proc. ICCF8 (1990), p. 191.
14. P. Tripodi, M. McKubre, and F. Tanzella, Temperature coefficient of resistivity at
composition approaching PdH, Phys. Lett. A (2000).
15. G. Hubler and V. Violante, Personal communication (2005).
16. McKubre et al., Loading, calorimetric and nuclear investigations of the D-Pd system,
Proc. ICCF4 (1993), p. 5-1.
17. McKubre et al., Isothermal flow calorimetric investigations of the D/Pd and h/pd
systems, J. Electroanal. Chem. 368, 55 (1994).
18. McKubre et al., Chemical and metallurgical issues in the loading of D into Pd, Proc.
International Symposium on Cold Fusion and Advanced Energy Sources, Minsk (1994).
19. B. Baranowski, S. Filipek, M. Szustakowski, J. Farny, and W. Wornya, J. Less Com-
mon Met. 158, 347 (1990).
20. S. Crouch-Baker, M. McKubre, and F. Tanzella, Variation of resistance with compo-
sition on the /3-phase of the H-Pd system at 298 K, Z. Fur Phys. Chemie. 204, 247
(1998).
21. W.-S. Zhang, Z-F Zhang, and Z-L Zhang, J. Electroanal. Chem. 528, 1 (2002); 571,
81 (2004).
22. P. Tripodi, F. Tanzella, and M. McKubre, Unpublished results (1999).
23. McKubre et al, Concerning reproducibility of excess power, Proc. ICCF5 (1995),
p. 17.
M E A S U R E M E N T S OF T H E T E M P E R A T U R E COEFFICIENT OF
ELECTRIC RESISTIVITY OF H Y D R O G E N O V E R L O A D E D Pd*
404
405
1. Historical Background
1.1. H/Pd Loading Measurements
It is common opinion that to observe heat in excess from Pd-D system it is necessary
to obtain very high values (>0.95) of D/Pd atomic ratio. 1 _ 3
Starting from 1998 we decided to perform systematic tests in order to achieve
very high H/Pd loading ratio using very diluted electrolytes and thin (50 or 100 /im
in diameter) Pd wires as cathodes. 4 Different electrolytic solutions have been tested
by adding to the acid solution very low amounts of Ca, Sr, Li and Hg ions. In
this way high H/Pd loading ratios have been achieved with a satisfactory grade of
reproducibility. Several loading procedures have been performed in a wide range
of electrolysis current (from a few mA up to one hundred mA) and at different
Hg ion concentrations. The obtained results allowed for the definition of a loading
protocol capable to insure very high H/Pd over-loading. Stable R/RQ < 1.2 values
(corresponding to H/Pd ratios >0.97) can be currently achieved with an extremely
low electrolytic power supply (10 V; 5 mA). 5
This procedure is based on the increase of the cathodic over-voltage (which is
known to be the main controlling parameter of the H(D)-Pd loading) obtained by
modifying the nature of the cathodic surface (i.e. by inducing the formation of a
very thin layer of an alkaline-earth carbonate on its surface).
1.8
1.6
1.4
1.2
Time (s) 3
Figure 1. R/Ro data are meanly stable for a enough long time (from 30,000 to 90,000 s range
Generally, as in the latter case, it is possible to check the R/Ro curve tracing
back to the peak value (R/Ro = 1-78, H/Pd = 0.75) and returning to the initial value
of R/Ro = 1. By considering the data in the range where the loading is stable, it
is possible to record the dependence of the wire resistance on the wire temperature
(homogenous with the cell temperature) and once the linearity of these data is
confirmed (Fig. 2), we can make a fit to calculate the Kg coefficient according the
relation (A.l) reported in the Appendix.
To be considered valid to our purpose, resistance data have to be repetitive after
each temperature cycle. In Fig. 1, it is reported that the load/deload procedure
(V-I ON/OFF) up to R/RQ = 1.1 and R/Ro fluctuation with temperature cycles
("measure"); evidence of the /3-transition occurs during the de-loading procedure.
407
1.18
y=08tU)0ni13AP-0PS4
1.17
- I ' «,=-!?. 8x 10 *t C )
1.16
r, 1.15
^ 1.14
1.13
1.12
1.11
20 21 22 23 24 25 26
Temperature-cell (°C)
Figure 2. Partial data of a full temperature cycle (40,000-60,000 s) well fitted by a simple line.
2.3. Results
Out of several hundred tests, only a few tens have shown a loading stability suit-
able for the calculation of the Kg parameter. We report in Table 1 some values
corresponding to different values of Pd loading.
In this table, measured values of R/Ro are reported for each of the two wire
sectors "up" and "down" (generally showing similar loading values); tests ranged
along a period of a year during which different wires, electrolytes and procedures
were used.
H/Pd Up Down
1
R/Ro ± 0 . 1 Kg (mK- ) R/Ro ± 0 . 1 KgimK-1)
(a) The first value is in agreement with the expected value for Kg = 4 . 1 .
(b) At the R/Ro peak value the thermal coefficient is a little higher (30%)
than the one reported in the literature (Kg = 2.0).
(c) All the values, beyond the R/Ro peak, the thermal coefficient shows
rapid increase.
408
H/Pd values reported in the table are taken from literature data up to R/RQ
peak value and after this point we refer to Mc Kubre experimental and theoretical
data, as previously reported. 12
In Fig. 3, we report known literature data ("+" points below the R/RQ peak) in
addition to the new experimental data ("0" points beyond the R/RQ peak) which
show the progressive increase of Kg as the H/Pd value increases (overloading); the
arrows show the trend of Kg with increasing loading ratio.
14 14
•i
12 12
+
1 0 10 - ^
r %
CO Q
3
y
<5 8 3
3
v** 6 §
\ CA
,!*«!*'«•!.. c
. CD
*** '.B-l,
4 n>
.• 3
2
- i — i . - L - i i ,...., I. .i i.....J..t-1-j-U-,
1 1.11.21.31.41.51.61.71.8
Similarly, in Fig. 4 we report data from the literature and the experiments; they
show clearly the rapid progressive increase of Kg at H/Pd overloading.
3. Discussion
3.1. Phase Hypothesis
From the literature, 2,3 ' 6 it is known that at room temperature the system Pd-Hx
occurs in different phase conditions (a-phase at H/Pd = 0-0.1 and a + ft phase at
H/Pd = 0.1-0.6). Because of the change of dimension occurring for R/Ro at the
peak value of 1.8 when H/Pd is ranging from 0.7 to 0.8,1 it is possible to suppose a
phase transition is taking place as it is pointed by an arrow in Fig. 1 at R/RQ = 1.7.
At this R/RQ peak we hypothesize a new phase, named "/3 + 7" phase. If, at high
H/Pd loading, this R/RQ peak is surpassed, we can assume that a peculiar 7-phase
409
I -16 $
1 - rn
c
—*:
CD
occurs in correlation with the change of slope of the Kg vs temperature curve (Fig.
4) so that this new phase is peculiar of H/Pd high loadings.
3.2. Conclusion
In conclusion, we stress the following points:
Acknowledgments
We are indebted to Eng. Alfredo Mancini for his precious support. We are grateful
to Dr. Daniele Garbelli and Dr. Luca Gamberale for their important help and we
want to t h a n k Dr. Mike McKubre for his useful suggestions. We like to stress the
expertness of Mr. Vincenzo Andreassi, our skill technician.
Appendix
References
1. M.C.H. McKubre et al., Frontiers of cold fusion, Proc. ICCF3, 1992, Nagoya, Japan
(1993), p. 5.
2. B. Baranowski et al, J. Less Common Met. 158, 347 (1990).
3. B. Baranowski and R. Wisniewski, Phys. Stat. Sol. 35, 539 (1969).
4. A. Spallone, F. Celani, P. Marini, and V. Di Stefano, Experimental studies to achieve
H/Pd loading ratio close to 1 in thin wires, using different electrolytic solutions,
Proceedings of the 9th International Conference on Cold Fusion, "Condensed Mat-
ter Nuclear Science" (Edited by Xing Z. Li.), Beijing (China), May 19-24 (2002),
pp. 319-322.
5. A. Spallone et al., An overview of experimental studies about H / P d over-loading with
thin Pd wires and several different electrolytic solutions, Proceedings of the 11th In-
ternational Conference on Cold Fusion (Edited by J.P. Biberian), Marseilles (France),
Nov. 01-05 (2004).
6. J.C. Barton, F.A. Lewis, and I. Woodward, Trans. Faraday Soc. 59, 1201 (1963).
7. M.C.H. McKubre et at, Galorimetry and electrochemistry in the D / P d systems, Pro-
ceedings of the First Annual Conference on Cold Fusion, Salt Lake City, Utah, March
28-31 (1990).
8. P. Marini, A. Spallone etal., XXISecolo Scienza e Tecnologia, AnnoX (1), 34-41 (1999).
9. F.Celani, A. Spallone et al., High hydrogen loading of thin palladium wires through
alkaline-earth carbonates' precipitation on the cathodic surface. Evidence of a new
phase in the Pd-H system, INFN: LNF-00/006 (P), 6 Marzo 2000, To be published
by Physics Letter A.
10. P. Tripodi, M. McKubre et al., Phy.Lett. A 276, 122-126 (2000).
11. L. Gamberale, D. Garbelli, and G. Piana, Measurement of Heat Capacity of PdHx,
Proceedings of the 9th International Conference on Cold Fusion, "Condensed Matter
Nuclear Science" (Edited by Xing Z.Li), Beijing, China, 19-24 May (2002), pp. 105-108.
12. M.C.H. McKubre (Data reported at the same Conference and Private Communica-
tions).
M A G N E T I C I N T E R A C T I O N OF H Y P O T H E T I C A L PARTICLES
MOVING B E N E A T H T H E ELECTRODE/ELECTROLYTE
INTERFACE TO ELUCIDATE EVOLUTION M E C H A N I S M OF
VORTEX A P P E A R E D ON P d SURFACE A F T E R LONG-TERM
EVOLUTION OF D E U T E R I U M IN 0.1M LiOD
HIROO NUMATA
Tokyo Institute of Technology, 1-12-1 O-okayama, Meguro-ku, Tokyo 152-8552, Japan
E-mail: numata@mtl.titech.ac.jp
MASANOBU BAN
Tokyo Metropolitan Industrial Technology Research Institute, 3-13-10 Nisigaoka Kita-ku,
Tokyo 115-8586, Japan
Long-term electrolysis for well-annealed thick Pd rod (9.0 mm <j>) in 0.1M LiOD was
performed. Microscopic observation of a postelectrolysis Pd surface showed that
long-term electrolysis did not result in any cracking but surface voids, two long
faults, voids arranged in a straight line and peculiar surface traces: vortex. N-cycle
model was developed to explain the cold fusion reaction and the related phenomena
resulting in improved reproducibility of cold fusion experiments. An important
process in that model is the motion of deuterium from a vessel to other ones,
which might occur the observed vortex patterns on a postelectrolysis Pd surface.
However, there has been remained unsolved yet a phenomenological explanation for
the process of the vortex formation. The lattice gas cellular automata method was
utilized for simulating a simple 2D flow with the boundary conditions incorporating
the motion of the coincidental flow of the hypothetical particles. The vortex pattern
was obtained behind the obstacle, though the axis appeared along the electrode
surface. However, by comparing the vortex patterns obtained by the Lattice gas
cellular automata method simulation and a postelectrolysis Pd surface the vortex
with the leaned axis along the electrode can only be acceptable to describe the
motion of the hypothetical particles. The vortex of the massive electron appeared
to be modified by Lorenz force during traveling the interface assuming a 2D circular
motion.
1. Introduction
Ever since the announcement of Fleischmann and Pons, and Jones et al. of the
generation of neutron and thermal energy accompanied with electrolysis on Pd in
0.1M LiOD, there still has been remaining the questions about the mechanism of the
cold fusion reaction. What kind of phenomenon occurs when deuterium is absorbed
in Pd metal by electrolysis is unknown, it is believed, is one of the reasons never
expelled from the above doubt. Numata 1 , 2 ' 4 proposed a nuclear reaction cycle
model (thereafter shortened to N-cycle model illustrated in Fig. 3) to explain the
411
412
2. Experimental
2.1. Long-Term Evolution of Deuterium on Thick Rod Pd
Electrode in O.IM LiOD
Cold fusion experiments at ambient temperatures have been conducted by elec-
trolysis of heavy water on a Pd electrode or the other stable metals, e.g., Ni, Ti,
and Au electrodes. In Fig. 1, the electrolysis equipment, especially the geometrical
shape and arrangement of the electrode, the counter electrode and an electrolyte
are shown, and the measurement systems with respect to excess heat, neutron emis-
sion, and an isothermal water bath are not drawn. Using a potentiostat (or current
supply) a constant cathodic current was applied to a Pd electrode on which an
evolution of deuterium gas was occurred. By continuing a state where deuterium
is strongly absorbed in a Pd electrode, heat generation or emissions of neutrons
or charged particles is observed. We successfully performed non-intermittent elec-
trolysis for two and ca. 6 months with two experimental runs, referred to Exp. 1
and Exp. 2, respectively. The characteristics of the experimental apparatus and
413
1. Pd rod cathode
2. Anode
3.0.1M LiOD electrolyte
4. Double jacketed
transparent quartz cell
5. Addition tube
6. Thermocouple
7. Guide for Deuterium gas
8. Guide for Oxygen gas
9. Circulating water inlet
10. Circulating water outlet
11 - Current supply
procedures are: (1) cast rod Pd electrode, (2) thicker rod Pd electrodes (rods with 9
and 21 mm diameters 3,4 ), (3) preparatory gas phase absorption of D 2 (D/Pd 0.36),
(4) increase in electrolysis current density in a form of stepwise, and (5) tempera-
ture cycling. The experimental runs were conducted twice in 0.1M LiOD by using
the rod Pd electrodes with a diameter of 9 mm referred to Exp. I, 5 and a diameter
of 21mm referred to Exp. 2. 3 , 4 The surface pretreatment and electrolysis condi-
tions are shown in Table 1 and the results of neutron measurement are described
elsewhere. 3,4
2
Run no. Current (mAcm ) Pretreatment
Gold plated
titanium wire
I
Gold electric
leading wire
Cross sectional
Teflon sheath area of electrode
9<|>Pd
rod Epoxy resin *
TC
Figure 2. Schematic of Pd electrode and optical micrograph of cross sectional surface area of
electrode.
electrode is unexpected, since the temperature of the electrode and that out side
of the counter electrode showed no significant change corresponding to heat bursts.
Hence, this is well acceptable, only when the small heat evolution in the interior
of the electrode lasted long time so as to promote abnormal grain growth. Cou-
pland et a/.10 found the recrystalline grain near the area of electrical connection.
Thus, during emission of neutron, the heat evolution in the interior occurred slowly
showing the symmetrical crystal structure.
Since the above result obtained by microscopic observation is not the in situ mea-
suremnt, it is impossible to give an answer to the matter when such a microscopic
structure appeared or to the time correlation with neutron count rate. However, it
was possible to estimate such problems by an analogy with a natural phenomenon,
as shown below.
<*0
H Electrode Electrolyte
Obstacle
I 6% expansion 1
Perspective view: outflow of
Absorption of deuterium hypothetical particle mass
of the hypothetical particles mass (once these particles were denned as charged par-
ticles, deuterium or reaction products) might occur toward 360° radial direction as
the scavenger process of N-cycle model (also see the right of Fig. 4). Such motions
of the particles mass might be realized from the geometry of the reaction vessel
formed during the absorption/compression process shown in the left. That is, in
a long prism crystal absorbed reaction products or deuterium under high pressure
coincidently spout out with sufficient energy where the motion of the flows are ex-
pressed as 'simulate flow' vectors normal to the electrode interface as shown in the
right. Importantly all the flows synchronize with the occurrence of the reactions. It
is known that nuclear reaction instantaneously occurs during which the hypothetical
particles surrounding the site coincidently gain momentum converted by the energy
of force evolved multiplied by time in an adiabatic sense. In addition obstacles might
be embedded under beneath the surface due to inhomogeneity. Thus, N-cycle model
predicts that the flows occur coincidently through the electrode/electrolyte inter-
face (formerly shown in Fig. 3 as the motion of reaction products and deuterium
to neighboring vessels and/or surface of the electrode), however, phenomenological
evidence has not yet been shown, which is substantiated next by a postelectrolysis
Pd surface observation and numerical simulation of the fluid flow.
other in their sizes were left on the surface. Thus, the locus of the vortex observed
on the Pd surface after long-term electrolysis in 0.1M LiOD is considered to be
an occurrence of energetic particles emission. At this stage the mechanism of such
vortex evolution stayed in the guess.
Figure 5. Vortex appeared on Pd electrode surface after long-term electrolysis in 0.1M LiOD,
(a) Duplicate of SEM picture, (b) Vortex evolved normal to electrode surface. Dashed line shows
locus of vortex.
Figure 6. Schematic view of vortex with axis along electrode obtained by numerical simulation.
At the electrode surface, strictly the interface between the electrode surface
and the bulk of the electrolyte, there is a potential difference, where electrons flow
toward outside in the electrode and ions in the same magnitude transfer in the
electrolyte. Under the circumstance of a constant current the induced magnetic
field (obeying the Maxwell equation) was numerically analyzed using Finite Element
Method (FEM). 6 The full 3-D FEM program (ANSYS) was used for the analysis
of magnetic field in the vicinity of the electrode surface and of the electrolyte bulk
in the electrolytic cell where the geometrical model (Fig. 1) was made for the
boundary conditions. The values of the magnetic flux density of the electrolyte
were in the range of 1.91xlO~ 3 T with some regional scattering, while those of the
electrode in the range of 0.0055 T within narrowed region. Apparently the amplitude
of the electrode vectors exhibits almost three times higher value than that of the
electrolyte.
(a) (b)
Interface
\
+ }<&'
***** ->
-?-
Electrolyte Electrolyte
Interface
Figure 7. Schematic of vortex string without magnetic interaction (a), locus left at the interface,
where radius of circular motion is modified under influence of varing magnetic fields (b).
can be evaluated as
r = mv/eB, (1)
where r is a circular orbital radius, and m and e are a mass and charge of a given
particle, e.g., electron, and B is a magnetic flux density. The reasonable value of r is
given under orthogonal velocity and magnetic flux vectors. Inspecting the appeared
vortex (Fig. 5), the above events occurred several times leaving the accumulated
circules. In Fig. 5 minimum radius was extrapolated taking into account all the
circumferences projected on the leaned base plane. Using the experimental data:
r = 41.7 ± 0.3 /jm the maxuimum velocities for electron mass and deuteron mass
are calculated as 4.6 ± 0.33 x 104 and 12.5 ± 0.90 m/s, respectively.
Although more accurate simulation might be needed to reach a definitive con-
clusion, it is noted that the motion of the hypothetical particles, e.g., electrons
exhibits significant kinetic energy to account for the further interaction.
4. Conclusions
The reality of the scavenging in N-cycle model (proposed by H.N.) was proved by
LGCA and FEM numerical simulation methods. We investigated vortex pattern
appeared on Pd surface after long-term electrolysis in 0.1M LiOD. The N-cycle
model predicted that the hypothetical particle mass flow coincidently through the
electrode surface/electrolyte interface. By LGCA method simulating the motion
of such particles mass the formation of vortex along the electrode (not normal to
the electrode surface) was proved. From the comparison of these vortices from
simulation and the result of experiment it is elucidated that the magnetic flux
density at the interface has the influence on the motion of these particles mass.
420
Acknowledgement
I would like to t h a n k Dr. Naoki Takada at t h e National Institution of Advances
Industrial Science and Technology for helpful discussion.
References
1. H. Numata and I. Ohno, Fusion Technol. 38, 206 (2000).
2. H. Numata and I. Ohno, Proc. 6th Int. Conf. Cold Fusion, Toya Japan, vol. 1, p. 213,
NEDO, The Inst, of Appl. Energy, (1997).
3. R. Takagi et al, Fusion Technol, 19, 2135 (1991).
4. H. Numata et al, Proc. Conf. Sci. Cold Fusion, 33, p. 71, in: T. Bressani, E. Del
Giudice, and G. Preparata (eds), SIF, Bologna, Italy (1991).
5. H. Numata et al, Proc. Mini Symp. Cold Fusion, Tokyo Metropolitan University,
pp. 129 (1990).
6. H. Numata and M. Ban, Proc. JCF6, 32 (2005), http://wwwcf.elc.iwate-u.ac.jp/jcf/
file/jcf6/jcf6 _proceedings.pdf.
7. E. Lewis, Proc. ICCF10, MA, USA (2003).
8. T. Ohmori et al, Fusion Technol, 33, 367 (1998).
9. Y. Toriyabe et al, Proc. ICCF12, Yokohama, Japan (2005).
10. D. Coupland et al, Proc. 1st Annu. Conf. Cold Fusion, 299, Utah (1990).
11. H. Numata , in book "Cyber X" No.ll, pp. 37 (1999) Kougakusha.
12. A. Takahashi et al, Nuclear Reaction Study In Condensed Matter No. 1, Chapter 4,
p. 124 (1999) Kougakusha.
13. Y. Matsukuma and R.Takahashi, Trans. JSME, 61-588, B, 2826 (1995).
U N U S U A L S T R U C T U R E S O N THE MATERIAL SURFACES
I R R A D I A T E D B Y L O W - E N E R G Y IONS
B. R O D I O N O V
Moscow Engineering Physical Institute (State University), Kashirskoe shossse, 31,
Moscow 115407, Russia
I. SAVVATIMOVA
Federal State Unitarian Enterprise Scientific Research Institute "Luch",
Zheleznodorozhnaya, 24 Podolsk, Moscow region 142116, Russia
E-mail: U10492@dialup.podosk.ru
Some unusual structures on the surface of metals and films (various X-ray films
and nuclear emulsions) caused by exposure to bombardment by low-energy ions in
glow discharge plasma, in electrolysis and other low-energy processes (when energy
of particles does not exceed several keV) have been f o u n d . 1 _ s The mechanism and
model of the strange tracks formations and explanation of their structure change
are suggested.
1. Introduction
For a number of years in various laboratories of the world physicists discover strange
tracks (which we call traces, whereas the objects that cause them are termed as
tracers). 1 _ 5 The traces, as a rule, are characterized by a microscopic width (usually
about 10 /im), but their length is presumably unlimited (mm and more). Sometimes
the traces look like a repeated pattern, similar to the tread design of a motorcar
tire or a necklace (Fig. 4). Sometimes the pattern forms a continuous line or a
group of parallel lines, differing from the standard tracks left by heavy charged
particles in nuclear photo-emulsions by their angularity or enormous length (up to
cm). Occasional flaws of the samples containing traces (on the polished surface of
metals or in photo-emulsions) do not explain the connected occurrence of the traces
at the places of local energy generation: electrical discharges, particle accelerator
targets, and the areas of natural disasters or technogenic ones, which are caused by
the human activity. This feature of the phenomenon in question may be used to
predict or to avoid the technogenic disasters, for example, the search of traces or
tracers can help in analyzing the causes of the Chernobyl Catastrophe.
421
422
and others), placed both on the inside and the outside of the glow discharge
chamber (Fig. 2). The similar tracks formations (with periodical repeating struc-
ture) were found on the nuclear emulsion films after the neutron generator exposure
(Fig. 3). Such tracks structures as demonstrated in Figs. 1-3 (regular structures,
spirals, chains, chains of voids, and others) need the comprehensible explanation
from the viewpoint of material science and demand special physical interpretation.
However, the classical approach to the study of physical phenomena requires
not only substantiation of the principal possibility of the process in question, but
also its detailed description including illustrative examples. The latter may become
possible on the basis of a model of filiform (thread-like filament) matter, i.e. fluxes.
Some components of the "flux theory" will be discussed below in application to the
problem under discussion.
Along with traces (in metals to the depth of 1-2 cm), changes in physical and
chemical properties of underlying layers from the viewpoint of their composition
and structure are observed (see table for Fig. 4). Under the surface of previously
monolithic sample some micro-tunnels and "holes" appear (Figs. 1-4). On the sur-
face of the samples examined before the exposure without any distinctive properties,
not only traces, but also some microscopic structures - films, hollow spheres and
cylinders, threads, spirals, complex spherical and cylindrical formations looking like
"cabbages" or "sausages" - were discovered after the exposure to low-energy ions
(Figs. 1-4), electrons or, ultrasound action . Sometimes these structures remind
bacteria or a colony of bacteria, which may glow (fluoresce) in the dark. These
objects move randomly and appear on the surface or "plunge" back into the depth
of the previously monolithic material. This activity of "live" bacteria objects may
continue for weeks after the energetic influence (after it has been finished).4
Each of these objects is unusual in the shape, surface structure, and the chemical
composition. The chemical composition in these formations is sharply distinguished
from the composition of the basic material on which these formations had arisen
(table to Fig. 4 with chemical composition). We shall take into account that all
these objects have been obtained under conditions of low-energy particles influence
when the nuclear processes in materials from the traditional point of view could not
exist. Therefore, at present there is no comprehensible hypothesis for the forma-
tion of such structures from the impurities. We shall also take into account, that
the majority of the chemical elements forming unusual structures were not present
in the initial material, and in the composition of the surrounding medium or in
constructive details of the experimental installations.
Thus, the shape, structure, and composition of unusual objects demands special
explanation, probably, based on new physical concept. This unusual concept, as
well as their possible practical application requires further examination of unusual
structures.
423
; • >
* n*^
*^P
Figure 1. Tracks on Pd surface after deuterium glow discharge exposure (optical microscopes (a,
b5 d-f) - Pd surface after deuterium bombardment, (c) back side, marks (a, c, and e) 100 /xm, (b
and d) 70 /im, and (f) 200 fim. (a) The micro-tunnels, (b-d, f) The spiral formations, (d) The
spiral curve and straight lines formations on Pd surface, (f) The spiral broken lines formation.
if^
(b) (c)
•t
(d) (e)
Figure 2. The structure on the films placed outside of the glow discharge chamber with stainless
steel wall (a, d) and quartz walls (b, c, e) after deuterium glow discharge with Pd (a, d), and
with Zr (e), with W (b, c). (a) "Melting bubble" on X-ray film (RT-2 type) after deuterium glow
discharge with Pd. (b) The parallel tracks on X-ray film (Kodak Bio Max) after deuterium glow
discharge with W-W cathodes, (c) "Cylindroid" (like "sausage") on the nuclear emulsion after
deuterium glow discharge with W-W cathodes, (a-c) Marks are 100 /xm; (d, e) 50 /xm.
424
(a) (b)
Figure 3. The periodical structure track on the nuclear emulsion after neutron generator exposure
(b) three-ray "star" (—•) is the results of fast neutron interaction with carbon nuclei with three
alpha particles formation: 1 2 C + n -—> 3OJ + n. (a, b) Marks are 100 ^m,
The dark matter can have filamentary structure. If diameter of filament is closed
to the diameter of atomic nucleus, they will easily pass through any dense substance
of usual nuclear-molecular structure (through any solids, planets or stars).
In the author's model such filaments - fluxes - can be cylindrical atoms. The
nucleus of such a cylindrical atom can represent a quark - gluon filament stabilized
by quanta of magnetic flux, and an electronic shell - an electronic Bose-liquid with
properties of super fluidity and superconductivity. The diameter of flux electronic
shell according to calculations is ~60 f.11
Fluxes can create an invisible grid, which wrap round not only far Cosmos, but
also all our planets, penetrating all bodies (solids) existing on the Earth (including
us with you) and influencing them in the various ways. Interaction of invisible fluxes
with usual nuclear-molecular substance could be in the various ways. 11,12
The huge gradient of a magnetic field promotes an attraction to magnetic poles of
particles with nonzero magnetic dipole moment (electrons, protons, neutrons, many
atomic nucleus, atoms, molecules, and ions) which can enter in nuclear interaction.
Elementary calculation shows that frequency of nuclear processes on magnetic
poles of hypothetical filaments - fluxes should reach 10 14 -10 15 s _ 1 , which enables
evolution of an output power of 100 W. The approximate, rough estimation (rough
guess) is given below.
Assuming the magnetic moment n of the shell of paramagnetic atom (molecule,
ion with radius « 1 0 - 8 cm) to be of Bohr magneton and equivalent magnetic charge
of the flux end (magnetic pole) to be minimal Dirac's magnetic charge em RS 70e
(e is electron charge), one can estimate magnetic attracting force of the atomic
particle to the flux end, F = 2 / ue m /a 3 ss 1 0 - 3 dyne, and the time of flight of the
captured atomic particle with mass of ^ 1 0 - 2 3 g to the flux end to be about 10~ 14 s.
This magnetic attraction determines the "self-aiming" of the atomic nucleus to the
flux end. Besides, if the flux end is situated inside or on the surface of the dense
(solid or liquid) paramagnetic matter, there may happen up to A x 10 14 nuclear
interactions per second, where A is the mass number of the captured nucleus. At the
nuclear distance, rN w 10~ 12 cm, the attracting force of the nuclear particle with a
magnetic moment fiN nearly equal to the nuclear magneton (fi/fiN ~ 2000) to the
flux end (magnetic pole) is FN = 2^Mem/riN ~ 5 x 105 dyne and the magnetic
N N
energy of one nucleon capture is F r ~ 1 MeV or A MeV per one captured
nucleus (atom). For A ~ 10 this corresponds to the power of approximately 100 W.
Nuclear reactions can also go on lateral surface of fluxes in an electronic Bose-
liquid, which shields the electric charges of nuclei. 11 In the end, plenty atomic nuclei
in the usual nuclear-molecular substance forming lengthways ensembles of fluxes
quanta with the cross sizes about 100 /xm 13 ' 14 can interact simultaneously. Thus,
the problem of cold nuclear fusion and nuclear transmutations in the fluxes model
is authorized by three ways: transformation of atomic nuclei on magnetic poles -
ends of fluxes, in electronic liquid on a lateral surface fluxes and in multinuclear
reactions in associates of fluxes nuclear ensembles.
426
Figure 4. The structure formations (traces) on the P d surface after deuterium glow discharge,
(a) Mark is 5 jtxm. (b) Mark is 10 //m. (c) Mark is 10 /im. (d) Mark is 20 /im.
with zero magnetic dipole moment. They should scatter, forming a "hot" shell of
these "new" nuclei near fluxes filament, which are inside dense nuclear-molecular
substance. Due to melting and evaporation of nuclear-molecular substance with
its subsequent condensation on cold parts of the sample, nuclear active fluxes leave
their complex structured traces both on the surface and inside samples in which
they are formed (Fig. 1). The nuclear active fluxes or complex fluxes object (we
name such an object TRACER) can move along trace (trajectory) in the substance.
The filamentary tracer of the structure can leave the trace without moving at
all or moving, for example, in the perpendicular direction to a line. In Fig. 5 the
presumed mechanism of formation of the various-shaped tracers is shown. The
atom-molecular quantum ensembles surrounding fluxes (the grey colored cylin-
der in Fig. 5) push out the fluxes (the white colored cylinder) to the periphery
of the ensemble where the temperature of ensemble substance is lower, the den-
sity of atoms is higher and probability of polynuclear reactions is the highest, too
(Fig. 5b). Such pushing-out results in bending of flux and atomic-molecular ensem-
ble surrounding it and interacting with it (Fig. 5c). In turn, the bend of ensemble
with fluxes can lead to turning the ensemble with fluxes into a ring or a spiral
(Fig. 5 d,e).
Figure 5. Flux model of strange tracks formation (5 a : top row of Fig. 5, 5b: bottom row of
Fig. 5).
Let us note that sometimes geologists found out such spirals of microscopic
sizes, for example, of refractory tungsten inside various compact samples (in rock)
in reality.
Geologist Elena Matveeva found tungsten spirals inside 200,000-year-aged rock
(Fig. 6). Formation of more complicated bodies of cylindrical or spherical symmetry
during warming-up by nuclear reactions (Fig. 5b f,g) is also possible. The formation
of hollow cylinders and spheres is possible as a result of oozed gases in chemical and
nuclear reactions in environmental substance around fluxes (Fig. 5bh). Sometimes
428
it is possible that such elementary processes create hollow quasi sphere particles
("blobs") and extensive hollow "cylindroids" on surfaces of a metal sample (Fig. 5b
a-c). "Blobs" and "cylindroids" can be broken off on the surface (or near surface)
of the sample by internal pressure of gases contained in them, leaving in the local
zones of metal surface the melt films formed near nuclear active fluxes. Helicoid
atom-molecular shells of nuclear active fluxes in projection to the flat surface of
sample frequently give the sine "paths" - "trajectory" with changed composition of
the basic material (traces in Fig. 5b). From known mathematical Fourier's theorem
it follows that the sum of sinusoids (or cosinusoids) with different amplitude and
period can give a track of any shape, the geometrical pattern repeating periodically.
Such kind of double spiral object we found on the X-ray film, exposed outside of
glow discharge chamber after deuterium experiment (Fig. 2d). 2
In our opinion, the origin of mysterious periodic patterns (chains and more
complex trajectories, Figs. 1-4) on the surface of the samples (Fig. 5b d-f) can
be explained by such kind of processes. Thus, concentration of the fluxes earlier
not participating in the process of nuclear interaction with substance (Fig. 5b e,f),
but activated by electromagnetic and nuclear processes in various places of trace is
possible.
This secondary interaction of the fluxes can considerably complicate the trace
figure. Especially the composite figure can arise from the cooperative action (com-
bined effect) of several nuclear active fluxes, which form, for example, enclosed
spirals (Fig. 5b f), and from activation of earlier passive secondary (tertiary) fluxes,
transiting through a trace.
^*
4K mmk
Figure 6. The tungsten spirals 200,000-year-aged inside the bore pit rock was found by geologist
E. Matveeva.
4. Conclusion
We hope that further investigations of these unusual strange formations on the
surfaces of various materials subjected to various low-energy exposures, will allow
429
References
1. T. Matsumoto, Steps to the discovery of electro-nuclear 060-0813, Japan (1999), p.
289.
2. I. Savvatimova, Reproducibility of experimental in GD. ICCF8, Italy (2000), p. 277.
3. M. Solin, Experimental facts of F initiation. 11th Rus. Conf. Moscow (2004), p. 90.
4. A. Agapov S. and L.I. Urutskoev, Proc.lSth Rus. Conf. on CF, Moscow (2005), p. 25.
5. B. Bogdanovich, Applied Physics, Moscow, MEPhI (2000).
6. J. Wheeler and R. Feynman, Rev. Mod. Phys. 24, 425 (1949).
7. Yu. Vladimirov, Moscow University Press (1996), p. 264.
8. Yu. Vladimirov, Theory of Phys. Interactions, Moscow University Press (1998), p.
448.
9. B. Rodionov, Proc. of 12th Rus. Conf. on CF 2004, Moscow (2005), pp. 136.
10. R. Laughlin, The Quantum Hall Effect (Springer, Heidelberg, 1987), p. 233.
11. B. Rodionov, Gravitation and Cosmology 8 (Supplement), 214 (2002).
12. B. Rodionov, CF of the 10th Rus. Conf. 2002. Moscow (2003), p. 50.
13. B. Rodionov, Proc. 11th Rus. CF Conf. Moscow (2004), p. 189.
14. B. Rodionov, Proc. 12th Rus. CF Conf, Sochy 2004, Moscow (2005), p. 110.
C O N T E X T FOR U N D E R S T A N D I N G W H Y PARTICULAR
N A N O S C A L E CRYSTALS T U R N - O N FASTER A N D OTHER LENR
EFFECTS
SCOTT R CHUBB
Research Systems Inc., 9822 Pebble Weigh Ct. Burke, VA 22015-3378, USA
E-maihchubbscott@aol.com
Two persistent questions have been: (1) Why is it often necessary to wait for a
finite period of time before the Excess Heat effect is observed after palladium (Pd)
has been sufficiently loaded with deuterium (D), that the near full-loading condi-
tion (PdDz, 0.85 ~ < x —> 1) that is required for Excess Heat, has been achieved?
(2) Is it possible to identify physical properties of the materials and/or crystals that
are used that might be playing a role in the interval of time associated with this
phenomenon? Recently, I generalized conventional energy band theory to address
both questions. The new theory can explain these experimental results but will be
ignored by most scientists. I suggest that this is expected: The context of energy
band and Ion Band State (IBS) theory is very different from the context of hot fu-
sion theory. Even within the Low-Energy Nuclear Reactions (LENR) field, hidden,
simplifying assumptions exist, which implicitly reflect biases associated with the
context of hot fusion. A typical example is the idea that a single, particular form
of reaction or environment can explain all LENR phenomena. As opposed to such
a picture, involving a single "nuclear active environment" ("NAE"), the context of
IBS theory and many-body physics suggests a more realistic and useful description
of LENR involves a multiplicity of "nuclear active environments" (NAEs).
1. Introduction
Context can profoundly affect discourse and debate. Facts taken out of context
can significantly misrepresent opinions or statements. Also, incorrect assumptions,
resulting from context, can result in false conclusions. Thus, context can profoundly
affect communication: For example, if a man yells "fire" or a fire alarm goes off in
a crowded movie theatre, considerably greater harm can result, through potential
panic, than if the same thing happens in a movie theatre containing a small number
of people.
Over the years, Ion Band State (IBS) theory papers have focused on particular
effects but have not included a complete description of the limitations and applica-
bility of the theory. Thus, qualitative language, involving quasiparticles (for exam-
ple) and other terminology has been used; while, in later discussions of the theory, a
highly mathematical formulation was presented that many readers found difficult to
follow. A useful context for understanding the IBS theory of Low-Energy Nuclear
Reactions (LENR) and its relationship to other theories or effects involving either
hot fusion or LENR has not appeared. In particular, despite the apparent successes
430
431
of the IBS theory, not only has the theory failed to be accepted, it has provoked un-
usual responses, including inaccurate statements, in separate Editorial comments in
Nature magazine 1 and one of the ICCF conference proceedings. 2 ' 3 These responses
have a plausible explanation: IBS theory follows from a known context 4 - 6 (hydrogen
in metals) that should apply to Cold Fusion (CF) but is inconsistent with hot fusion.
As the theory has evolved, more general ideas 7 - 9 have justified the underlying
physics. Despite the fact that to date, no unifying theme or context for under-
standing the IBS theory in CF has appeared, the more general ideas relate to an
important, unifying idea: The problem of relating crystal size to transport phenom-
ena involving charged or neutral particles in finite lattices. 10 In particular, transport
phenomena, in general, can become quite complicated in finite solids. But partial
periodic symmetry can be used to identify a hierarchy of processes, in which all of
the particles located in some "periodically ordered" region, or some subset of it, can
"move" coherently in a perfectly rigid manner (similar to the rigid, lattice recoil,
in the Mossbauer effect) that preserves the separation between each particle with
the remaining particles. These effects are the basis of a known phenomenon (an
Umklapp process) that occurs in phonon scattering and electrical conductivity. In
infinitely-repeating lattices, this process is described by a resonant effect, in which
momentum is not conserved between "quasiparticles." Instead, the momentum is
transferred to the lattice elastically. But momentum conservation requires that
quantitative bounds exist for the amounts of momentum that can be transferred
to a surface or interface (and vice versa) through these kinds of processes. Tradi-
tionally, in models in which the lattice is infinitely repeating and periodic, these
bounds have been poorly defined. In finite solids, at low, but finite temperature T,
precise, size-dependent bounds can be identified. In larger crystals, collisions with
phonons tend to reduce the magnitudes of these effects. In smaller crystals (or in
optical lattices 11 ), this is not the case. In the case of palladium-deuteride (PdD),
the effects can be quite large and can lead to coherent forms of interaction 12 and
potentially LENR.
Initial estimates of the magnitude of the effects suggest a particular time scale
for triggering the coherence that can be related to the incubation time 13 associated
with CF. But, as in the past, this material was not introduced within the context, of
a more complete theory. 10 ' 12 The present paper includes a more detailed description,
involving the context of the more complete theory. 10 ' 12
This material, which is presented in the next section, provides a useful context
for understanding the importance of the complete theory and its application in
problems involving LENR. It includes a discussion of some of the earlier motivating
work that led to the theory and material that provides a context for generalizing
earlier results to more general problems involving LENR. The next and final section
summarize how the more complete theory can explain triggering in d + d —• 4 He in
finite size PdD crystals.
432
large distances and when the externally applied fields vary sufficiently slowly, ft
was not at all obvious, within this context, that the associated picture could apply
in a problem involving d+d fusion, where large changes in external fields could be
required over short distances.
An important goal of the more complete theory 10 ' 12 was to address both of these
limitations from the outset. In order to accomplish this, a mathematically rigorous
formalism, based on a generalized form of multiple scattering was developed,7 that
could apply in finite lattices, was derived that potentially can also explain why high
energy particles are not required in CF reactions. This formalism provided a way
to generalize conventional band theory to cases involving finite lattices.
Within this context, it was possible to generalize conventional band theory by
requiring that it apply to the ground state (GS) and lowest lying excitations and
that the GS have minimal coupling to outside processes. Then, the lowest energy
excitations of a solid, by construction, are required to conserve charge in some
finite volume of the solid and are required to be unaffected by a symmetry: rigid
translations (Umklapp processes) that preserve the separation between any two
particles within this region. 10,12 ' 13
We have made other predictions that have not been tested: (1) That when 4 He
is externally introduced into the surface region and the region immediately outside
heat-producing materials, might catalyze the d + d —» 4 He reactions through a form
of Bose-induced stimulation, similar to stimulated light emission in lasers 20 and (2)
that the observed anomaly (associated with the substitution of PdD for PdH) in
the value of superconducting critical temperature Tc (in which Tc is higher than in
the case of PdD) might be the result of "Cold Fusion" at low temperature. 21
Because in the initial announcements, PF suggested that Excess Heat was the
result of a colder version of conventional fusion, ideas, even tangentially related to
cooperative forms of reaction, were entirely ignored. In an entirely unconventional
and unjust manner, David Lindley1 explicitly criticized these ideas and our the-
ory almost a year after he received our first paper, 22 without explicitly referring
to our work, through his derisive commentsl (about Bloch and Wannier states,
and Bose condensates): "[A] broad category of cold fusion theories rested on more
sophisticated uses of collective effects [in solids]"...
These theories had the special attraction that they could easily be decorated with
the jargon, at once forbidding and enticing, of solid-state physics: Bose-condensates,
Bloch states, Wannier functions... like the Paris fashions, they outface mockery...
"Nevertheless they were all wrong, and for a straightforward reason. The fusion
rate for two deuterons is calculated from their two wavefunctions, multiplied by the
nuclear interaction rate. The latter is a very short-range force, only at separations of
a few nuclear radii is the nuclear reaction rate significant. The only important con-
tribution to the fusion rate, therefore, comes from the product of the wavefunctions
when the deuterons are very close. But the wavefunctions in the Bose-condensed
state are calculated explicitly by ignoring the nuclear interactions; they are valid
everywhere except at close range." 1
434
During ICCF2, 2 Giuliano Preparata also criticized our theory 2,3 because it
appeared to ignore the key problem (involving the Coulomb barrier) that seemed
to be relevant in the CF problem. In fact, both sets of comments reflected bi-
ases, associated with conventional fusion. However, as opposed to Lindley's ap-
proach, which involved first ignoring the relevant science in our paper, not publish-
ing the material, and then criticizing its ideas (based on incorrect information about
the relevant physics), without appropriately referencing the material, not only did
Giuliano Preparata allow our ideas to be published, but he actively participated in
a useful scientific debate about their relevance.
Lindley's comments had some value. He pointed out (as in conventional fusion)
close proximity between d's, at a single location, is required for a nuclear reaction to
occur, and effects of electromagnetism (EM) can be treated as being static, relative
to the dynamical effects involving the nuclear forces (NFs). This picture applies to
conventional situations involving higher energy incident particles in nuclear reac-
tions, and especially in hot fusion, where deuterons have a sufficiently large incident
kinetic energy. Then , the time- and length-scales involving EM and NFs are so
different that the total wave function $ can be factored into the product of separate
components $ n u c and $em (through the d-d separation variable r):
* = $nuc(r)$em(r). (1)
4
In ordinary d + d —> He + 7, in fact, at all times, the dependence of the coupling
to the electromagnetic field must be included. 23 Although this fact has been known
since the early 1970s, it does not appear in conventional fusion literature because
the d + d —> 4 He + 7 occurs at a rate that is ~ 107 times slower than the comparable
rates associated with the dominant (d + d —> 3 H + p and d + d —> 3 He + n) reactions.
On the other hand, the reverse reaction, 4 He + 7 —> d + d has been studied in
detail. Here, it is known in fact, as opposed to the reaction involving the simple
form, associated with Eq. (1), a comparable factorization between NF and EM
wave functions is not possible because the associated dynamics requires detailed
information 23 about the coupling of the EM interaction with the NF.
Lindley misquoted this as well as a number of additional facts, including the na-
ture of the d + d —> 4 He reaction, which he had not investigated, and the fact that
d's have unit spin. Also, at the time, important information about the nature of
products was not known. With hindsight, his comments illustrate a misunderstand-
ing of fundamental aspects of many-body physics. In particular, although in 1989,
Bose-Einstein condensates (BECs) had only been observed in natural processes in
cryogenic environments, involving near absolute zero T in helium, noncryogenic
procedures involving laser-cooling were being developed for creating BECs. Begin-
ning in 1995, these procedures made it possible to dynamically create BECs. Since
that time, not only has it become possible to create, manipulate, and alter BECs,
using lasers but to artificially stimulate phase transitions, in which states involving
an initial configuration of localized bosonic atoms (that remain confined in regions
of space, defined by particular lattice sites in an optical lattice) into delocalized
435
(coherent) states in which the bosonic atoms exhibit the kinds of wave-like behav-
ior, that we suggested might be relevant, are produced routinely.
that are asymptotically far from the location of any possible NF overlap. In fact,
in the more rigorous formulation, all possible forms of overlap become possible, and
the comparable constraints need not apply except either near the GS or when the
system is prepared appropriately. However, a generalized result also is appropriate:
Eq. (1) still applies in the most coherent forms of reaction, provided the defini-
tions of $ n u c (r) and <&EM(?") are generalized: As opposed to referring to the wave
functions describing proton-neutron (p-n) pairs, in any particular reaction rate, the
associated wave functions can be interpreted as describing the CM motion of col-
lections of p-n pairs, or p-n pairs coupled to p's and/or n's, or, more generally, of
collections of charged particles (p-n pairs, p-n pairs with p's or n's, or p-n pairs,
with p's and/or n's and electrons).
An important point is that although larger clusters of charged particles (in
the relevant portions of a particular matrix element) can be viewed as generalized
forms of quasiparticles, need not be forbidden, with increasing size, possible effects
involving broken symmetry (through alternative forms of overlap in other matrix
elements) become more likely and: The most coherent coupling involves simpler
configurations, but these can cause greater degeneracy and greater instability. The
key point is that the states that have the greatest overlap with the GS are required
to not alter the relative coordinates between charged particles or clusters of particles
in the regions (associated with EM interaction) far from the locations of nucleon
overlap and NF interaction. From earlier arguments, 24 this more general context can
be used to generalize the earlier selection rule. 14 ' 15 ' 22 The lowest energy excitations
require that when &em(r) is a boson (i.e., its total spin is an integer multiple of h),
$,iUC(r) is also a boson; and when <&em{r) is a fermion (i.e., when its total spin is
an odd multiple of ft/2), <I?nuc(fnuc) is a fermion.
An important point is that this last set of rules is approximate and is only re-
quired to apply in crystals that are sufficiently large or when other factors (e.g.,
through changes in the fluxes of particles into and away from the solid, or through
external fields) might require that these rules apply. An unfortunate result of the
history of CF and LENR, and in the initial context of hot fusion, is that it has been
frequently assumed that a single set of conditions, associated with what has been
called a "nuclear active environment" 25 (NAE) has been believed to be responsible
for LENR. Gauge symmetry, and broken or approximately broken gauge symmetry
imply a considerably richer, different scenario. To the degree that particular gauge
symmetries (e.g., those associated with an applied electric field) can be important,
specific triggering phenomena can be important. In other situations (e.g., those
involving a magnetic field, or varying flux of charged and/or neutral particles), de-
pending upon the potential overlap between possibly degenerate states with external
fields, many different effects can take place. Magnetic coupling, in particular, can
alter potential channels for nuclear reaction in profoundly different ways involving
"bosonic" or "fermionic" coupling. Also, it certainly is not required that Eq. (1)
apply either to pairs of deuterons or charged (fermionic or bosonic) "clusters" of
particles, or that when it does, the lifetime of the associated state is sufficiently
438
long that appreciable overlap with NF processes take place. In fact, whether or
not a particular kind of reaction will take place involves a complicated reaction
rate expression, based on a true many-body configuration. In particular limits, loss
of symmetry and gauge symmetry (through broken gauge symmetry) can become
important. But this certainly is not a requirement for LENR.
References
1. David Lindley, The embarrassment of cold fusion, Nature 344, 375 (1990).
2. ICCF1 and ICCF2 were called ACCF1 and ACCF2. ICCF3 replaced ACCF3.
3. G. Preparata, Editorial Note, in Proc. ICCF2 (see Ref. 2) (1991), p. 204
4. M.J. Puska et al, Phys. Rev. Lett. 51, 1081 (1983).
5. C. Astaldi, A. Bianco, S. Modesti, S., et al, Phys Rev Lett. 8, 90 (1992).
6. R.C. Casella, Phys. Rev. B 27, 5943 (1983).
7. S.R. Chubb and T.A. Chubb, Proc. ICCF8 (2000), p. 385.
8. S.R. Chubb and T.A. Chubb, Proc. ICCF9 (2002), p. 57.
9. S.R. Chubb, Proc ICCF10 (2005), p. 735.
10. S.R. Chubb, Spawar, T.R. 1862, Szpak et al. (eds.) vol. 3 (in press).
11. I.H. Deutsch and P.S. Jessen, Phys. Rev. A 57, 1972 (1998).
12. S.R. Chubb, http://arxiv.org/cond-mat/0512363.
13. S.R. Chubb, Proc. ICCF11 p. 646 (2005) .
14. S.R. Chubb and T.A. Chubb, Proc. ICCF1 (1990), p. 119.
15. S.R. Chubb and T.A. Chubb, Lattice induced nuclear chemistry, in: S.E. Jones, F.
Scaramuzzi, D. Worledge (eds.) Anomalous Nuclear Effects in Deuterium/Solid Sys-
tems, AIP Conference Proceedings 228 (AIP, New York. 1991), pp. 691-710.
16. M.C.H. McKubre et al, Proc ICCF2 (1991), pp.419-444.
17. B.F. Bush et al, J. Electroanal. Chem. 304, 271 (1991).
18. T.A. Chubb, T.A. and S.R. Chubb, Fus. Tech. 20, 93 (1991).
19. S.R. Chubb and T.A. Chubb, Really cold 'coldfusion', Proc ICCF7 (1998), p.78.
20. S.R. and T.A. Chubb, NRL MR-6600, Naval Research Laboratory (1989).
21. D.R. Thompson, Nucl. Phys. A154, 442 (1970).
22. S.R. Chubb and T.A. Chubb, Fus. Tech. 24, 403 (1993).
23. E. Storms, http://www.lenr-canr.org/acrobat/StormsEthenatureo.pdf
440
24. C.G. Beaudette, Excess Heat: Why Cold Fusion Research Prevailed (Oak Grove Press,
Bristol, ME, 2002), pp. 365.
25. C. Zener, Proc. R. Soc. A145, 523-529 (1934).
26. Y. Arata and Y.-C. Zhang, Proc. ICCFIO (2005), p. 139.
27. Y. Arata and Y.-C. Zhang, Proc ICCF12 (in press).
MODELS FOR ANOMALIES IN
CONDENSED MATTER DEUTERIDES
P E T E R L. H A G E L S T E I N
Research Laboratory of Electronics,
Massachusetts Institute of Technology,
Cambridge, MA 02139 , USA
and
Spindletop Corporation, Mountain View, CA 94040
E-mail: plh@mit.edu
1. Introduction
In 1989 there were announcements made of observations of anomalies in metal
deuterides: Fleischmann and Pons presented observations of an excess heat effect
in PdD, 1 and Jones presented observations of low-level neutron emission in TiD. 2
Since then, considerable experimental and theoretical work has been reported on
these and on other anomalies. As has been noted often over the years, the existence
of any such effects would require a significant revision of our understanding of
nuclear physics to explain. We have focused our efforts on the implications of
these new experiments on theory, as well as on the development of models that
may be relevant.3~5 In the nuclear physics literature, the predominant view is that
nuclear fusion reactions that occur in condensed matter can be understood from
idealized models in which the local environment is replaced by vacuum. The basic
argument is that in order to react, nuclei must approach to within a few fermis,
and the resulting reaction is completed with fast-moving well-separated product
nuclei long before information concerning the reaction can reach neighboring atoms
on an atomic scale. Such a picture cannot be relevant to the excess heat effect in
Fleischmann-Pons type experiments, in which a large amount of energy (apparently
of nuclear origin) appears and commensurate 4 He is detected. The experimental
results are consistent with some new kind of reaction mechanism that acts as if
441
442
Do
n + 3He Aj*
Conversion
\ of nuclear
I / energy to
other modes
_>L.., Macroscopic
4
He AZ
excited mode
Figure 1. Scheme proposed for excess energy production. Molecular deuterium in condensed
matter makes transitions to 4 He states through intermediate n + 3 H e states, with stabilization of
the intermediate state through large angular momentum transfer associated with phonon exchange.
The excitation is transferred to other species, which undergo fast phonon-mediated excitation
transfer reactions among themselves, transferring energy to the excited phonon mode a few tens
of phonons at a time.
H = ^ S « + ^ S ^ + fiwoa^a + ^ e " G S « ( a + a ^
h z h z h x
2
+ JLs^(a + a^. (1)
In this model the D 2 / 4 He system is represented by the first set of two-level systems,
under the assumption that sufficient phonon exchange is present to allow transitions
through the n+ 3 He intermediate state with negligible loss. The D 2 and 4 He states
are modeled as equivalent two-level systems (superscript I here), with transitions
between these states represented with a hindered (by a tunneling factor e _ G ) tran-
sition involving the exchange of up to mi phonons. The receiver side nuclear states
are also modeled as equivalent two-level systems (superscript 2) with unhindered
transitions involving the exchange of up to m 2 phonons.
444
Coupled
Dicke system
and oscillator
»U Q
Figure 2. In the limit that the receiver-side two-level systems are strongly coupled to the
oscillator, then it is useful to think in terms of two-level systems coupled to a coupled oscillator
and Dicke system hybrid.
-M,n
T f 2gAE \ f 2gAE \ „
J
(M-M0+n-n0)/2 [~ A E + hLjQ ) J(M-M0-n+n0)/2 [~ A E _ ^ ) >M + n even
>
0, M + n odd.
(4)
The associated eigenvalues are given by
EMo,n0 = M0AE + n0fuj0. (5)
Very similar eigenfunctions occur for M0 + n0 odd. One sees that in this limit, the
coupled oscillator and Dicke system have a comb of eigenvalues spaced uniformly
every HLOQ.
30
c20
<
10
* - ^ — ^ * * ^ ^ ^ m * — m ^ ^ +
"-8 - 6 - 4 - 2 0 2 4 6 8
<M>
Figure 3. Calculation of the spread in oscillator number A n (upper curves) and spread in Dicke
number A M (lower curves) for the distinct even eigenfunctions with £ = 8, AE/fiwa = 15, and
g = 1.5. A solitary point at M = 0 marks the analytic result for the localized Bessel function
approximate eigenfunction.
In the large n limit, the coupling coefficients are nearly constant around M = 0, but
they vary increasingly as one moves away from M = 0. Localized eigenfunctions
are obtained near M = 0, but away the eigenfunctions become more delocalized.
This is illustrated in Fig. 3 where we show the spread in oscillator number An
as a function of the average Dicke number (M). Near M — 0, one sees that the
spread in both n and M approach the constant g result, with minor deviations seen
since the eigenfunctions extend slightly into regions where the coupling coefficient
depends on M. Away from M = 0, one sees a significant spreading in n, which is an
indication of derealization. The spread in M becomes reduced as the boundaries
are approached.
This result is interesting since it illustrates that if the local symmetry of the
coupling constants is broken, that delocalization can result. Also, that the amount
of delocalization is stronger the more that the symmetry is broken. However,
the resulting eigenfunctions do not closely follow the constant energy line. For
example, we illustrate in Fig. 4 a representative eigenfunction that is close to the
M-boundary. One sees a relatively large spread in oscillator number. Such behavior
is typical for coupled systems with a modest number of two-level systems.
Figure 4. Example of eigenfunction for coupled two-level system and oscillator for large n limit.
The vertical axis is the associated spin quantum number M, and the horizontal axis is relative
oscillator number n = n - no-
that correspond to the analytic solutions discussed above, which are static. The cou-
pled system is capable of large scale energy exchange between the two degrees of free-
dom, as is completely clear from the numerical results that we have seen (and is also
completely clear from the literature on this kind of model). We can construct what
amount to classical states of the system from a superposition of the eigenfunctions
in the large n limit, and track the resulting dynamics (since wavepackets in the
configuration space can keep their shape approximately). We see net motion that
is oscillatory in the two dimensions, with wavepacket motion in M very roughly
oscillatory with a frequency on the order of AE/li, and wavepacket motion in n
with a frequency on the order of UIQ. We can understand the results in terms of
simple notions of potential and kinetic energy in the (M, n) configuration space.
In these simulations, the wavepacket moves from one position with an associated
potential energy (AeM +frwoii),with the velocity of the wavepacket associated with
the system kinetic energy. Hence, if the wavepacket follows a trajectory that goes
between regions with different amounts of oscillator or Dicke excitation, because of
the system kinetic energy the wavepacket. will shortly move on.
d .. n2(t) ,. d , . V2(t)
^n2(t) + - ^ i = v2(t), -v2(t) + -^- = -ait), (9)
where
a
W = p { [Nl ~ Mt)\[N2 ~ n2(t)][n2(t) - nx(t)]
Here n\{t) and n2(t) are the average number of excited states in system 1 (D2 side)
and system 2 (receiver side), and v\{t) and v2{t) are the associated velocities. The
acceleration is a{t). The Dicke number for the two sides are iVi and N2l which can
be as large as the total number of nuclei involved on each side.
4.2. Example
In Fig. 5 we show results from a numerical calculation of the evolution equations
for resonantly coupled Dicke systems. In this calculation, we have assumed that
there are 10 times more receiver side nuclei in the ground state than there are
D2 molecules in the upper state. In addition, we have set the relaxation time
to be matched to the coherent transfer rate. If we use a much slower relaxation
time, then we observe population returning from the receiver side. If we use a
much faster relaxation time, then we observe a slower net transfer of excitation.
The problem in this case is that if the receiver-side nuclei decay rapidly, then there
are relatively few around to provide a (receiver-side) Dicke enhancement of the
acceleration. In essence, the fastest net energy generation rate is obtained when we
match the excitation transfer rate with the receiver-side loss.
450
10 20 30
12 _G
(2A/1A/2) ' V e f / h b a r
5. Avoidance of Loss
We have noted previously that the probability amplitude tends to avoid regions of
high loss. A very much simplified version of this argument can be given. Consider
the situation of two states that are coupled, one loss free and the other with high
loss:
d
ih—co(t) = flocoW + V&icift), (11)
.fill
Hi ci(t) + Vi0co(t). (12)
We initialize the system such that c0(0) = 1, and ask what happens later on. The
exact solution is more complicated than what we are interested in here; however,
a useful simplification is allowed if we assume that the level 1 loss is very strong.
In this case, CQ decays slowly as we will find, and we may assume that the a(t)
probability amplitude is determined in the steady state by
( t ) = W ) + (14)
^ F&^
451
= [Vbil2 ' n ,.
Increasing the level 1 loss 71 to ever larger values has the perhaps unexpected
effect of decreasing the level 0 loss. In essence, the probability amplitude tends to
avoid level 1 as it gets increasingly lossy. Alternatively, one can view this result as
indicated that the maximum loss from level 0 is obtained when the loss is matched
to the coherent transition rate.
6. Nuclear Models
We have made progress on the other half of the problem which involves the calcula-
tion of the nuclear response in the presence of phonon-mediated excitation transfer.
The calculation of phonon exchange matrix elements requires the inclusion of the
nuclear center of mass coordinates as phonon operators. Results relevant to such
calculations for the four-body problem is discussed in another paper submitted to
this proceedings.6
We have in addition developed a new strategy for the calculation of the nuclear
response which may be worth discussing briefly. The lattice generalization of the
resonating group method that we have developed allows us to include phonon ex-
change explicitly in calculating nuclear interaction matrix elements. It seems that
the most relevant and perhaps cleanest calculation which is needed is a second-order
process in which an initial nuclear system receives energy via excitation transfer in
a first phonon mediated strong force interaction, then evolves as a daughter plus
neutral, and after a while makes a transition to a final state nuclear system. The
basic interaction matrix element can be represented as
Mfl(E) = J2(^f(^f(^'---^A)\VN\^>mt[E-Hmt}-1
int
x{*int\VN\MZu---,U)*i{<l))\ (16)
In the initial state, we see an internal nuclear wavefunction <&i(£i,..., £A), with £j
as relative nucleon coordinates, embedded in a lattice (or condensed matter system)
described by \Pj(q). Transitions are mediated by the strong force, described here
by the nuclear potential Vjv- The intermediate internal nuclear wavefunctions for
the different possible intermediate configurations are <I>int • The lattice wavefunction
in the intermediate state is implied through the specific bra and ket arrangements,
but since there is a neutral involved in the intermediate state, the phonon modes
of the lattice wavefunction are rotated through a Duschinsky transform (leading
to intermediate wavefunctions of the form *i n t (A • q). Finally, the neutral and
daughter come back together through the second potential interaction, producing
452
Yint(A-q, rn)Ointfe,...,y
Figure 6. Feynman-type diagram for matrix element involving intermediate lattice plus neutral
states.
final state nuclear $ f ( £ i , . . . , £A) a n d lattice wavefunctions \&f (q). In this case, the
phonon basis for the initial and final state lattice wavefunctions are locally the
same, since there is no net mass change. There could be rearrangements in either
the initial or final state systems, such as would occur if D2 or HT molecular systems
are involved. However, when the nuclei are close enough to interact, the lattice will
simply see four nucleons and two charges.
This basic calculation is involved both in phonon-mediated transitions of the
form D 2 —> n+ 3 He —> 4 He on the D 2 side, as well as AZ —> n m + A _ m Z —> A Z transi-
tions on the receiver side. The matrix element can be represented by a Feynman-like
diagram that is illustrated in Fig. 6. Implicit in the expression for the matrix el-
ement and also in the diagram is the point of view that the lattice (or condensed
matter system) separates from a neutral (in association with an excitation transfer
event), evolves as a daughter lattice plus neutral in the intermediate state, and then
comes back together to form the final state lattice. Instead of a vacuum language
that focuses on nuclei and nucleons, in the formulation under discussion, the in-
teraction is with a nuclei which is part of a lattice, and it is helpful to think of it
as a neutral plus lattice separation. Such a view makes plain what the calculation
involves at the outset, and makes clear that it is in fact a fundamentally different
calculation than what is involved in related vacuum calculations.
7. Summary
We are moving toward viewing relevant models as involving the hindered coupling
between a Dicke system for the D2/ 4 He side and a hybrid quantum system on the
receiver side composed of one or more Dicke systems strongly coupled to one or more
highly excited oscillators. In previous work, we have discussed the possibility that
loss can break the symmetry of the coupled oscillator and Dicke Hamiltonian in order
to allow the conversion of nuclear energy to phonon energy. Here we have shown that
453
the n a t u r a l boundaries associated with the Dicke system can accomplish the same
basic function in a relevant strong coupling limit. Energy transfer between the Dicke
system and the oscillator can occur naturally on timescales of the oscillator and
two-level system generally in coupled Dicke oscillator systems. In strongly coupled
systems in which the coupling strength between nearly degenerate eigenfunctions
exceeds the oscillator energy, free energy exchange is expected. This corresponds
to the situation we expect in the case of coupling between receiver nuclei and a
highly excited acoustical phonon mode. It also is closely related to the coupling
mechanism we discussed in the I C C F l l proceeding for a closely related model of
two Dicke systems coupled to an oscillator with different coupling strengths in the
classical limit. We presented the results of an Ehrenfest analysis of coupled resonant
Dicke systems, augmented with loss to take into account energy coupling with the
lattice in an empirical way. T h e resulting evolution equations should be relevant
to the dynamics of fusion reactions under conditions where the D2 source is not
replenished. Progress on the nuclear calculations was discussed briefly as well.
References
1. M. Fleischmann, S. Pons and M. Hawkins, J. Electroanal Chem. 201, 301 (1989);
Errata, 263, 187 (1990). See also M. Fleischmann, S. Pons, M.W. Anderson, L.J. Li
and M. Hawkins, J. Electroanal. Chem. 287, 293 (1990).
2. S.E. Jones, E.P. Palmer, J.B. Czirr, D.L. Decker, G.L. Jensen, J.M. Thorne, S.F. Taylor
and J. Rafelski, "Observation of cold nuclear fusion in condensed matter," Nature 338
737 (1989).
3. P.L. Hagelstein, Proceedings of the Ninth International Conference on Cold Fusion,
May 2002, Beijing, China, in: X.Z. Li (ed.), p. 121.
4. P.L. Hagelstein Proceedings of the Tenth International Conference on Cold Fusion, Aug.
2003, Cambridge, MA, in: P.L. Hagelstein and S.R. Chubb (eds), p. 837.
5. P.L. Hagelstein Proceedings of the Eleventh International Conference on Cold Fusion,
Nov. 2004 Marseilles, France, in: J.P. Biberian (ed.), (in press).
6. I. Chaudhary and P.L. Hagelstein, this proceedings.
T I M E - D E P E N D E N T E Q P E T ANALYSIS OF TSC
AKITO TAKAHASHI1
Osaka University, Yarnadaoka 2-1, Suita, Osaka 565-0871, Japan
e-mail: akito@sutv.zaq.ne.jp
Time-dependent fusion rates for 2D and 4D reactions are calculated for squeezing
of tetrahedral symmetric condensate (TSC) from about 100 pm size to its minimum
size (about 10 fm), within about 75 fs squeezing motion. Life time of the minimum
TSC state is yet to be studied. Time-averaged fusion rates are given by assuming
the life time of minimum TSC state is negligible. Time-averaged 2D fusion rate was
given as 2 . 9 x l 0 ~ 2 6 f/s/pair, and time-averaged 4D fusion rate was 5 . 5 x l 0 - 8 f/s/cl.
These values are compared with 1.0xl0~ 2 0 f/s/pair for 2D and 1.0 X 1 0 - 9 f/s/cl
for 4D, respectively, of previously estimated values by electronic quasi-particle
expansion theory/TSC m o d e l s . 1 _ 3 Effective fusion time by the TSC squeezing
motion was estimated as 0.04 fs: namely fusions may happen in very short time
interval.
1. Introduction
For a consistent theoretical model of various condensed matter nuclear effects,
namely clean 4 He producing fusion and cold transmutation, electronic quasi-particle
expansion theory (EQPET)/tetrahedral symmetric condensate (TSC) models have
been developed by the author. 1_4 Transient motion of TSC by four deuterons plus
four electrons has been treated with a primitive approximation using the linear com-
bination (EQPET) of wave-functions for pseudo-molecular states of d-d pairs with
normal electrons and quasi-particle-electron states e*(2,2) and e*(4,4) as steady-
state solutions for narrow time-window. This was a model for "bosonized conden-
sate" of squeezed mode, which can be treated as a kind of steady state in very
narrow time-window of squeezed motion.
Since the barrier factor changes drastically with astrophysical orders according
to the assumed pseudo-molecular states, numerical studies based on time-dependent
treatment are expected to know more accurate values of fusion rates of multi-body
deuteron interactions in the transient process.
This work reports a trial study of time-dependent EQPET analysis for TSC
squeezing motion to estimate time-averaged fusion rates of 4D/TSC.
454
455
2. E Q P E T Model
Starting with the formation of TSC state (t = 0) with six-wings wave function which
is composed of six dde* molecular wave functions with six orthogonal single spin
wave functions, time-dependent screening potentials are adiabatically approximated
with pseudo-molecular potentials for ddee, dde* (2,2) and dde*(4,4) according to the
change of mean d-d distance i?dd- Semi-classical treatment is done for the time-
dependent reduction of mean d-d distance. Using this algorithm, a computer code
is made.
4re = 4x2.8 fm
Electron
r~\
>
4
<$> <8>
4
He He
Deutron
15fm
(3) 8 Be* formation (4) Break U
P
the Pauli's limit, we used the classical electron radius of 2.8 fm. In Step 3, mutual
charged-pion exchange between four deuterons forms 8 Be* intermediate compound
state with much smaller radius and the charge neutrality in average of 4D/TSC is
broken simultaneously to kick out four electrons. In Step 4, 8 Be* which is collec-
tively deformed with two alpha-clusters promptly breaks up to two 4 He particles.
The initial state TSC wave function, when TSC is just formed at t = 0, can be
written using combination of six wings of D2 molecule wave functions on six surfaces
of the TSC cube, as illustrated in Fig. 2. Here, the wave function of D2 molecule is
written with combination of two 1 S wave functions \&ioo of hydrogen atom, as also
illustrated in Fig. 2. This feature is obtained by assuming the TSC wave function
to be the following Eq. (1) and using the three-dimensional symmetric constraint of
TSC squeezing motion in applying the quantum mechanical variational principle of
minimizing system energy. The new aspect of the problem is that we are treating
"bosonized condensate" of TSC under the environment of ordered dynamic motion
(in other words, symmetrically constrained squeezing motion) in the lattice of PdDx
condensed matter.
*ioo(r) = ( l A ) 1 / 2 ( l / a B ) 3 / 2 e x p ( - r / a B ) . (2)
Here subscripts A-D denote positions of deuterons at vertexes of cube.
And subscripts 1-4 denote positions of four electrons. XS(S{, Sj) is singlet spin
wave function for bosonized (anti-parallel spins) pair of electrons. Bohr radius ae
is 52.9 pm.
Coefficients a\-a% are vectors on six surfaces of the cube, and are usually deter-
mined by the variational method to minimize system energy as,
<S{<*4D|ff|*4D>/<*4D|tf4D>} = 0. (3)
Since the solution of Eq. (3), with partial derivatives for coefficients a\-a§, gives
sixth order (18th order in exact, taking three-dimensional components of vector aj)
secular equation which cannot be solved uniquely. However, the requirement of
ordered squeezing, namely the three-dimensionally symmetric constraint of TSC
motion in PdDx lattice, gives constraints as,
Deutron
v_y
(c) 4D/TSC (life time about 60 fs)
73 pm
(b) D2 molecule (stable): V 2 D = (2+2Ar 1/2 [ Vl00 (r A1 ) ¥ioo(%z) + Vioot'Aa) ¥IOO('BI)]^S(SI. S2)
Figure 2. Features of QM electron clouds for (a) D atom, (b) D2 molecule, and (c) 4D/TSC at
t = 0. Bosonized electron center torus of D 2 molecule is a unit of bond for orbits of bosonized
electron coupling of TSC (t = 0).
3. Time-Dependent E Q P E T Analysis
The basic equation of time-dependent EQPET is written as
*4D(r, t)at = a i ( t ) * ( l , l)(r, t) + o 2 (t)*(2,2)(r, t) + a 4 (t)¥(4,4)(r, t), (6)
(r(t)) = <r(0)> - (v)t, (7)
458
?
60
-Ram da2d (1,1)
50
-o
E 40 - Ram da2d (2,2)
CO
CC
30
ra
_o «d^^
I Ram da4d (4,4)
20 •^s^aS^ass -
10
0
0.01 1
Figure 3. Calculated time-dependent cluster fusion rates for TSC squeezing motion.
We found time-averaged 2D fusion rate 2.9 x 10~ 25 f/s/pair is about five orders
of magnitude smaller than the steady squeezed mode analysis, but time-averaged
4D-fusion rate 5.5 x 10" 8 f/s/cl is rather closer value. Of course we should prefer
values by the present time-dependent analysis.
5. Conclusions
1. Simplified trial of time-dependent analysis on TSC was made.
2. TDEQPET (time-dependent code) gave several orders of magnitude differ-
ent fusion rates from those by EQPET (Squeezed Mode Model).
3. 4D fusion takes place in 0.04 fs effective reaction time: It is very impulsive.
4. TSC as bosonized condensate has been proposed as SEED of Condensed
Matter Nuclear Effects to induce clean 4D fusion.
Table 2. Time-averaged modal fusion rates and initial fusion rates for
4D/TSC squeezing motion, calculated by T D E Q P E T code
t Virtual value.
461
References
1. A. Takahashi, Deuteron cluster fusion and related nuclear reactions in metal-
deuterium/hydrogen systems, Recent Research Developments in Physics, Transworld
Research Network, India, 6, 1-28 (2005), ISBN = 81-7895-171-1.
2. A. Takahashi, TSC-induced nuclear reactions and cold transmutations, Siena Work-
shop on Anomalies in D/H loaded metals, Siena, Italy, 13-16 May (2005),
http://www.iscmns.org/.
3. A. Takahashi, A theoretical summary of condensed matter nuclear effects, ibid.
4. A. Takahashi, Condensed Matter Nuclear Effects, Proc. IMFP2005, Int. Meet. Frontiers
Physics, 25-29 July (2005), Kuala Lumpur, Malays. J. Phys., to be published.
5. A. Takahashi, Mechanism of deuteron cluster fusion by EQPET model, Condensed
Matter Nuclear Science, Proc. ICCF10, World Scientific Publ. Co., pp. 809-818 (2006),
http://www.lenr-canr.org/.
6. A. Takahashi, Drastic enhancement of deuteron cluster fusion by transient electronic
quasi-particle screening, Proc. JCF4, pp. 74-78, A. Takahashi, Deuteron cluster fusion
and ash, Proc. Asti Workshop (2004) http://www.iscmns.org/.
U N I F Y I N G T H E O R Y OF L O W - E N E R G Y N U C L E A R R E A C T I O N
A N D T R A N S M U T A T I O N PROCESSES IN
D E U T E R A T E D / H Y D R O G E N A T E D METALS, ACOUSTIC
CAVITATION, GLOW DISCHARGE, A N D D E U T E R O N
BEAM EXPERIMENTS
Y E O N G E. K I M A N D A L E X A N D E R L. Z U B A R E V
Department of Physics, Purdue University, 525 Northwestern Avenue,
West Lafayette, IN 47907, USA
E-mail: yekim@physics.purdue.edu; zubarev@physics.purdue.edu
1. Introduction
There have been many reports of experimental evidences for low-energy nuclear
reaction (LENR) processes in condensed matters as documented in a recent docu-
ment submitted for a DOE review1 and as reported in Proceedings of ICCF-10. 2
However, most of experimental results cannot be reproduced on demand. This sit-
uation has prevented us from development of a coherent theoretical understanding
or working theoretical model of the phenomenon which can be used to guide us in
designing and carrying out new experimental tests to sort out essential parameters
and controls needed to achieve reproducibility on demand (ROD). In this paper,
it is shown that recently developed theoretical model based on Bose-Einstein Fu-
sion (BEF) mechanism and Quantum Plasma Nuclear Fusion (QPNF) mechanism
are applicable to the results of many different types of LENR and transmutation
experiments.
Both the BEF and the QPNF mechanisms are based on a same physical model,
which assumes that deuterium/hydrogen is in a plasma* state and is mobile in a
deuterated/hydrogenated metal as deuteron/proton ion.t
*In this paper, we use a general definition of "plasma" as given in the report: National Research
Council, "Plasma Science", National Academic Press, Washington DC (1995), p. 1, "Plasma
science is the study of the ionized states of matter".
* Experimental evidences for the ionization and mobility of deuteron/proton in metal are given in
Refs. 14-16.
462
463
Theoretical studies of BEF mechanism have been carried out using an approx-
imate solution to the many-body Schroedinger equation for a system of N identi-
cal charged, integer-spin nuclei ("Bose" nuclei) confined in micro- and nano-scale
cavities. 3-6 The ground-state (superfluidity state) solution is used to obtain theo-
retical formulae for estimating the probabilities and rates of nuclear fusion for N
identical Bose nuclei confined in a ion trap or an atomic cluster.
Most recently, we have investigated the effect of a generalized particle momen-
tum distribution derived by Galitskii and Yakimets (GY) 7 on nuclear reaction rates
in plasma. 8 ' 9 We have derived an approximate semi-analytical formula for nuclear
fusion reaction rate between nuclei in a plasma. The formula is applied to calcu-
late deuteron-deuteron fusion rate in a plasma, and the results are compared with
the calculated results of the conventional Maxwell-Boltzmann (MB) velocity dis-
tribution. As an application, we investigate the deuteron-deuteron fusion rate for
mobile deuterons in a deuterated metal/alloy. The calculated deuteron-deuteron
fusion rates at low energies are enormously enhanced due to the modified tail of the
GY's generalized momentum distribution. Our preliminary estimates indicate also
that the deuteron-lithium (D + Li) fusion rate, the proton-boron (p+B) fusion rate,
and the proton-lithium (p + Li) fusion rate in a metal/alloy at ambient tempera-
tures are also substantially enhanced due to this QPNF mechanism. Implications
of our results and other potential applications are discussed.
In this section, we describe a QPNF mechanism, which includes the effect of GY's
generalized momentum distribution on the nuclear fusion rates in a plasma. 8 ' 9 The
calculated results based on the QPNF mechanism for deuteron-deuteron fusion rates
are compared with the results of the conventional calculation with MB distribution.
As applications of the QPNF mechanism, we investigate other nuclear fusion rates
for (D + Li), (p + Li), and (p + B) reactions in metals/alloys.
£p) {Z)
^ -irl(E-Sp-A(E,p)y+1i(E,p)Y
where e p = p2/2/x is the kinetic energy in the center of mass coordinate of an
interacting pair of particles, u is the reduced mass, A(E,p) is the energy shift
due to the interaction (screening energy, etc.), and j(E,p) is the line width of the
momentum-energy dispersion due to collision. ^{E^p) RJ hpcac^2E/n, where pc is
( 2 2 2
the number density of Coulomb scattering centers (nuclei), ac = Tr(ZfZ je ) /s is
the Coulomb scattering cross section, and Zfe is an effective charge which depends
on e p . For small values of e p , Zf is expected to be much smaller than Z*, Zf <C Zj.
However, for larger values of e p , it is expected that Zf approaches to Zi, Zf « Zj.
This Lorentzian distribution, Eq. (2), reduces to the 8-function in the limit of
A -> 0 and 7 ->• 0,
S1(E-ep) = S(E-sp). (3)
The nuclear fusion rate for two nuclei is given by
where
/ ( p ) » / dEn(E)67(E-ep), (5)
Jo
and the normalization N is given by
NJd£pf(p) = l. (6)
For a high-energy region, e p 3> kT, 7 and A we obtain approximately
Gr
jMES^E-eJ-^-JW^M, (10)
where f(p) is the distribution function, given by Eq. (5). Since the integral on
the left-hand side of Eq. (10) is a divergent integral, the GY parameterization of
~f(E,p) in 81(E — ep) needed to be corrected for large £ >fcTto satisfy the above
sum rule. However, Eqs. (4-9) are still valid since our results for the distribution
function f(p) do not depend on j(E,p) in the region where E 3> kT due to the
presence of n(E) oc e~E/kT in Eq. (5).
I
I
b icr 33 i
^
^T
-****
* * * * * * *
i
J^
Ja » w * "* Maxwell-Boltzmann
_ j. « « » ™
'
10 4 1
10" 43
'
theory
p-independent
.....
^
I
'
X;
0.01 0.1 1 10 100
Temperature (eV)
Figure 1. Fusion reactivity, (crv), of D(d,p) 3 H reaction in units of c m 3 / s as a function of tem-
perature kT in units of eV. The dashed line, the solid line, and the dotted line corresponds the
results calculated using the MB distribution, the GY distribution with p = 10 c m - 3 , and the
GY distribution with p = 10 1 5 c m - 3 , respectively.
when the fusion rate is equal for MB and the QPNF processes. This comparison
shows that quantum effects are important at low temperatures even for the Debye-
Hiickel plasma, p <C (kT/e2)3 while they are negligible for the conventional high-
temperature (kT ~ 5-10 keV) plasma fusion such as for the proposed international
experimental fusion reactor (ITER). The goal of the ITER project is to achieve a
plasma density of 10 15 c m - 3 while hydride densities in metals are in the range of
1022 cm" 3 .
This comparison then explains why the QPNF process is not important in high-
temperature fusion observations and calculations.
(a) Nuclei i and j are the same specie and mobile in a plasma with a GY velocity
distribution (For example i and j are both deuterons yielding the (D + D)
fusion reaction rate).
(b) Nuclei i and j are two different species and both mobile in a mixed two-
species plasma with velocity distributions (For example i is for protons and
j is for deuterons yielding the (p + D) fusion reaction).
(c) Nucleus i is mobile and from a single-specie plasma with a velocity distri-
bution, but nucleus j is stationary and imbedded in a metal/alloy matrix.
Nuclei i and j are the same specie (For example i and j are both protons or
both deuterons or nuclei i and j are two different species yielding (D + Li),
(p + Li), and (p + B) fusion reactions).
Our results of surprisingly large fusion rates for the DD fusion reaction in a
deuterated metal/alloy at ambient temperatures may offer a sound, conventional
theoretical explanation for most of the nuclear emissions results reported from the
previous LENR experiments. 22
Given similar conditions as for the DD fusion, the fusion rate for the D 6 Li fusion
reaction is estimated to be ~10% of the DD fusion rate, R^6Li ~ 0.1i?j5D.
For two cases, (p + Li) and (p + B), the fusion reaction rate has been estimated
and is shown in Table 2 as a function of the fraction of hydrogen that is mobile
within the lattice. In the calculation £jj(0) = 4.5 MeV-barn and 197 MeV-barn
are used for 6 Li(p,a) 3 He (Q = 4.02 MeV) and u B(p,a)2 4 He (Q = 8.69 MeV),
respectively.
Based on the calculated results of fusion rates with the QPNF mechanism shown
in Table 2, we see that nuclear fusion rates for (p+ 6 Li) and (p+ 11 B) LENR processes
in hydrogenated metals/alloys are sufficiently high for practical energy generation.
If we could achieve sufficiently high fusion rates for 6 Li(p, 3 He) 4 He and 11 B(p,
a)2 4 He fusion reactions with the LENR processes in hydrogenated metals/alloys,
they could become attractive alternative methods for generating clean nuclear fusion
energy.
reported the observation of tritium and neutron production during their ACE using
deuterated acetone and a pulsed neutron generator. Most recently, the temperature
measurement of a single bubble acousitic cavitation has been made. 34
We plan to investigate the role of the QPNF mechanism in the ACE in our
future work.
References
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for a review, July 2004, and references therein. This report was posted December 1,
2004 at the DOE website: http://www.sc.doe.gov. Published in the Proceedings of
11th International Conference on Cold Fusion ICCF-11 (Marseille, France, 2004; Con-
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2. See experimental papers in the Proceedings of the 10th International Conference on
Cold Fusion ICCF-10 (Cambridge, MA, USA, 2003; Condensed Matter Nuclear Sci-
ence, World Scientific Publishing Co. Singapore, 2006).
3. Y.E. Kim and A.L. Zubarev, Fusion Technol. 37, 151 (2000). . ..
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6. Y.E. Kim, Progress of Theoretical Physics (Supplement) 154, 379 (2004).
7. V.M. Galitskii and V.V. Yakimets, J. Exp. Theor. Phys. (USSR) 51, 957 (1966).
8. Y.E. Kim and A.L. Zubarev, Quantum plasma nuclear fusion, Purdue Nuclear and
Many-Body Nuclear Theory Group (PNMBTG), Preprint PNMBTG-4-05 (November
2005).
9. Y.E. Kim and A.L. Zubarev, Effect of a generalized particle momentum distribution
on plasma nuclear fusion rates, PNMBTG-5-05 (December, 2005), to be published in
Japanese Journal of Applied Physics, Vol. 45, No. 22, L552-L554 (June 2, 2006).
10. Y.E. Kim, D.S. Koltick, R. Pringer, J. Myers, and R. Koltick, in Proceedings of ICCF-
10 (Cambridge, MA, USA, 2003), pp. 789-799.
11. Y.E. Kim, D.S. Koltick, and A.L. Zubarev, in Proceedings of the ICCF-10 (Cambridge,
MA, USA, 2003), pp. 779-787.
12. YE. Kim and A.L. Zubarev, Mixture of charged bosons confined in harmonic traps and
Bose-Einstein condensation mechanism for low energy nuclear reactions and trans-
mutation processes in condensed matters, in Proceedings of the ICCF-11 (Marseille,
France, 2004), pp. 711-717.
13. Coraddu et al., Physica A 340, 490 (2004); 496 (2004) and references therein.
14. F.A. Lewis, Platinum Metals Reviews 26, 20, 70, 121, (1982).
15. Q.M. Barer, Diffusion in and through Solids (Cambridge University Press, New York,
1941).
16. Y. Fukai, The Metal-Hydrogen System, 2nd edn. (Springer, Berlin, Heidelberg, New
York, 2005).
17. R.A. Rice, G.S. Chulick, and Y.E. Kim, The effect of velocity distribution and electron
screening on cold fusion, Proceedings of the First International Conference on Cold
Fusion, pp. 185-193, March 1990, Salt Lake City, Utah, edited by F. Will.
18. R.A. Rice, G.S. Chulick, Y.E. Kim, and J.-H. Yoon, The role of velocity distribution
in cold deuterium-deuterium fusion, Fusion Technol. 18, 147 (1990).
19. Y.E. Kim, R. S. Rice, and G. S. Chulick, The effect of Coulomb screening and velocity
distribution on fusion cross-sections and rates in physical processes, Mod. Phys. Lett. A
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20. J. Kasagi, Progress of Theoretical Physics Supplement No. 154, 365 (2004); Kasagi
et al, J. Phys. Soc. Jpn. 73, 608 (2004).
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during Mizuno-type experiments, in Condensed Matter Nuclear Science: Proceedings
of ICCF-12 (Yokohama, Japan, November 28-December 2, 2005), to be published.
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34. D. Flannigan and K. Suslick, Nature 424, 52 (2005).
35. Y.E. Kim, R.A. Rice, and G.S. Chulick, The role of the low-energy proton-deuteron
fusion cross-section in physical processes, Fusion Technol. 19, 74 (1991).
36. S.E. Jones et al, Nature 338, 737 (1989).
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40. R.A. Hanel et al, J. Geophys. Res. 86, 8705 (1981).
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42. J.B. Pollack et al, Icarus 65, 442 (1986).
43. B. Conrath et al, Science 246, 1454 (1989).
CATALYTIC F U S I O N A N D T H E INTERFACE B E T W E E N
INSULATORS A N D T R A N S I T I O N METALS
TALBOT A. CHUBB
Greenwich Corp., 5023 N. 38th St., Arlington, VA 22207, USA
E-mail: tchubb@aol.com
Cold fusion uses a catalyzed configuration change to replace plasma fusion's need
for high-energy particle collisions. 1 In radiationless cold fusion, the configuration
change is a coherent partitioning of deuterons into fractional pieces within a set
of potential wells provided by a hosting lattice. 2 The coherently partitioned mat-
ter distribution is a Bloch wave function. Alpha addition transmutations 3 require
active deuterium in the form of Bloch function deuterons with 2-dimensional pe-
riodic symmetry. 4 , s The configuration change to Bloch form has been modeled
as occurring in the interface volume between a salt and Pd metal. In Arata and
Zhang radiationless cold fusion 6 - 8 reactive deuterons are modeled by Bloch ions
with 3-dimensional periodic symmetry hosted in metallic nano crystals. 5 The nano
crystals are isolated by salt-metal interfaces. In both cases, the fusion process is
modeled as a Li—Feshbach resonance transition to an excited nucleus state, with
subsequent energy transfer to a metal lattice by phonon cascade. 5 The lattice struc-
ture of the deuterons is preserved in the product nucleus until the energy transfer
is completed. For the 2-dimensional symmetry case, the intermediate nucleus or
many-body nuclear system can sometimes be observed in "flake" lattice form, pro-
viding insight about the process. 5 Research on salt-metal interfaces could facilitate
cold fusion technology.
1. Introduction
This paper builds on modeling published in the Proceedings of ICCF10 and ICCF11
and in the ANS meeting held in Washington in November 2005. Research results
presented at ICCF12 clarify the picture of the cold fusion process, causing some
revisions to the thinking presented in the ICCF11 Proceedings. New results influ-
encing this paper are gas loading studies by Arata and Zhang, 8 and observations
of abnormal nuclear products presented by Lipson et al.,9 Roussetski et al.10 and
Savatimova.11
The paper discusses the following topics: the catalytic nature of radiationless
cold fusion;1 the proposed role of insulator-metal interfaces in promoting the co-
herent partitioning of deuterons in Iwamura's alpha addition transmutations; 4 the
proposed role of insulator-metal interfaces in heat-generating Zr02,Pd nano crystal
powder; 7,8 a discussion of Oriani-Fisher energetic showers and their relation to ob-
servations by Lipson,9 Roussetski, 10 and Savvatimova;11 and a preferred picture of
cold fusion reactions by Li-Feshbach resonance reactions involving excited product
nuclei in lattice-geometry states. 5
473
474
particles and gamma rays cannot match onto the multiple-maximum array density
structure of the Bloch ion. On the other hand, because Bloch deuterons and Bloch
helium products have an array structure, they are small crystals that can store
energy in their lattice degrees of freedom. Energy is stored in the form of excitations
of lattice vibrations and in phonon excitations. If the product nucleus is produced
in an excited nucleus state, some of the energy contained in the nuclear phonon
modes can be resonantly transferred to the metal lattice provided that the difference
between a pair of nuclear excitation levels matches the energy of a metal phonon
mode, or multiple thereof. Phonon energy transfer appears to be the most likely
mode of energy transfer that occurs in radiationless cold fusion.
These observations suggest the need for a program to study and more fully
understand the properties of insulator-metal interfaces and their applicability to the
development of cold fusion heaters. Experiments are needed to more fully define
the Iwamura and Arata type processes. There is need to study insulator-metal
interfaces, and to determine whether or not a fully loaded deuterium interface is
needed for configuring deuterium into active Bloch form. Recent condensed matter
physics studies by Ichitsubo et al.13 and Barcaro et al.14 illustrate two types of
interface study that could be helpful. The Barcaro et al. paper points out that
metal-metal bonding competes with surface adhesion during the formation of a salt-
metal interface. Also, it is of interest to know whether a thin coating of adsorbed
water on Pd powder can preserve the 2-dimensional periodic geometry of a "flake"
nucleus that had previously been formed inside the periodic environment of the
ZrC>2, Pd interface volume. Adsorbed water was measured in a post-run study of
an Arata-type cathode containing Pd-black. 15
4. Flake Nuclei
An important characteristic of dd fusion reactions occurring in accord with imposed
Bloch geometry is that both initial state and final state wave functions preserve the
coherent partitioning of ions described by Bloch functions. The geometry is that
of a Bravais lattice. This geometry is imposed on weakly trapped deuterons by
the electron lattice within which the deuterons are embedded or in contact. When
2-dimensional Bloch symmetry applies, the product nucleus has a Bloch symmetry
form that resembles a 2-dimensional crystal, e.g., the geometry of a 1-atom thick
flake of graphite. 16 However, unlike a 1-atom thick crystal, the Bloch geometry
nucleus contains only a 1/Nwe\\ fraction of a deuteron centered on each potential well
position, instead of a full deuteron. Here, potential well means the localized volume
containing a local minimum in the lattice potential as it attracts dressed-deuteron
matter. Under normal circumstances, the flakes are viewed as being planar and
embedded within the interstitial volume of a salt-metal interface. Under abnormal
conditions, the flake is viewed as being able to move from its creation site within
its hosting interface lattice, and to expand or migrate to another location in or on
the metal. In extreme CclSGS, El flake nucleus is thought to be able to dissolve into
a polarizable solvent like water, and subsequently become air-borne without losing
its lattice form, i.e. without collapsing to the "point" form of a normal nucleus.5
At ICCF12, Savvatimova11 reported on a post-run metal surface showing a
parallel-to-the-surface etched structure that looked much like the cast of a metal-
strip coil, with the axis of the coil parallel to the metal surface. In another case
she showed a linear series of etch pits arranged in a straight line and spaced with
a strictly periodic order, such as an almost-buried cylindrical coil might cause if
it were to periodically touch the metal surface. Neither of these types of struc-
tures had ever been seen under conditions not associated with processes designed
to induce cold fusion. To me, the observations suggest a flake-like piece of nuclear
matter with the geometry of a metal strip coil, such as is sometimes produced during
machining of metal on a lathe. The flat strip geometry seems consistent with the
477
still remains to energize the alpha particle emissions. In the new picture, there is
no need for a "Maxwell demon" energization process, as suggested in Ref. 5. In the
revised picture, the physically large nuclear flake structures causing major shower
events could be of the same type as those causing the surface anomalies observed
by Savvatimova.
the hosting lattice is lost. However, if the nucleus product remains closely coupled
to the hosting lattice by being part of a many-body Bloch system that is electro-
statically coupled to the lattice, a cascade of energy transfer events can occur by
acoustic phonon transfers from the Bloch nucleus with its lattice-geometry to the
much more dense continuous spectrum of phonon states characterizing the host
lattice. A first energy transfer to the host lattice changes an otherwise reversible
fluctuation (a coalescence fluctuation) into an irreversible reaction. Subsequent cas-
cading energy transfers lower the energy of an initially produced excited nucleus to
its ground state energy.5
Mossbauer transitions can, in principle, directly transfer momentum and energy
from a Bloch subsystem to a hosting lattice during a fusion reaction. However, there
is indirect way by which fusion energy can be transferred to the lattice without
producing a direct fusion product. One can produce a transient excited Bloch
nucleus and subsequently consume it in a transmutation reaction, as seemingly
occurs in Iwamura et al. It is not yet clear how prevalent consumption of the direct
fusion product is. It might be occurring in Arata-Zhang experiments. Post-run
4
He has been proven to be present in post-run residual gas of an Arata-Zhang
DS-cathode, but only at ~0.05% of that necessary to explain the generated heat. 19
However, I am inclined to think that the anomalously low-helium content in the
sampled ullage gas is an experiment problem caused by helium loss through micro-
cracks in the stressed wall of the DS-cathodes. 20 Further experiment is required to
resolve this issue.
The primary dd fusion reaction is considered to be enabled by a Li-Feshbach res-
onance. This means that the reaction takes place with near-zero energy dissipation.
Li models this low-energy dissipation by adding an imaginary component to the
strong force interaction potential. 21 The resonating initial and final nucleus states,
though nearly identical in energy, are different in either their internal nuclear con-
figuration and/or in their internal nucleus vibration plus phonon excitation profile.
Any configuration or excitation change occurring during a Li-Feshbach transition
allows additional time for the irreversible transfer of a small quantum of energy to
the hosting environment. Alternatively, an energy transfer may occur during the
initial coalescence fluctuation.
With dd fusion, the strong force reaction occurs within a many-body
subsystem 22 with Bloch geometry, and involves a spin-zero coordinate-exchanged
dd coupling within the many-body system. Sometimes, a many-body system might
contain only two Bloch deuterons within a nano-crystal of Pd. The 2-body case is
the case modeled in Refs. 2 and 5. The nuclear transition is a 0+ to 0+ transition.
No orbital angular momentum is introduced by the coalescence process.
Much of the above is discussed as involving deuterons with 2-dimensional Bloch
symmetry, patterned after a modeling of the Iwamura et al. process. However,
because of the much higher, multi-Watt powers generated by Arata and Zhang,
I continue to believe that their heat generation is based on 3-dimensional Bloch sym-
metry. Bloch deuterons are envisioned as being partitioned into a communicating
480
network of shallow-well sites, consisting of two tetrahedral sites plus one peripheral,
already-occupied octahedral site per unit cell.
References
1. T.A. Chubb, Three types of dd fusion, ANS Transactions 93, 895 (2005).
2. T.A. Chubb, I. Bloch Ions, Proc. ICCF11, 665 (2006).
3. Y.Iwamura. M. -, and T. Itoh, Elemental analysis of Pd complexes: effects of D2 gas
permeation, Jpn. J. Appl. Phys. 4 1 , 4642 (2002).
4. T.A. Chubb, II. Inhibited diffusion and surface transmutations, Proc. ICCF11, 678
(2006).
5. T.A. Chubb, III. Bloch Nuclides, Iwamura Transmutations, and Oriani Showers, Proc.
ICCF11, 685 (2006).
6. Y. Arata and Y.-C Zhang, A new energy caused by spillover-deuterium, Proc. Jpn.
Acad. 70B, 107 (1994).
7. Y. Arata and Y.-C Zhang, Formation of condensed metallic deuterium lattice and
nuclear fusion, Proc. Jpn. Acad. 78B, 57 (2002).
8. Y. Arata and Y.-C Zhang, Development of 'DS-Reactor' as the practical reactor of
'Cold Fusion' based on the 'DS-cell' with 'DS-Cathode', ICCF12 Abstracts.
9. A.G. Lipson, A.S. Roussetski, G.H. Miley, B.F. Lyakhov, and E.I. Saunin, Repro-
ducible nuclear emissions from Pd/PdO:D K heterostructure during controlled exother-
mic deuterium desorption, ICCF12 Abstracts.
10. A.S. Roussetski, Correct identification of energetic alpha and proton tracks in ex-
periments on CR-39 charged particle detection during hydrogen desorption from
P d / P d O : H x heterostructure, ICCF12 Abstracts.
11. I. Savvatimova, Unusual structures on the material surfaces irradiated by low energy
ions and in other various process, ICCF12 Abstracts.
12. J.D. Jackson, Catalysis of nuclear reactions between Hydrogen Isotopes by fi~~ Mesons
Phys. Rev. 106, 330 (1957).
13. T. Ichitsubo, E. Matsubara, T. Yamamoto, H.S. Chen, N. Nishiyama, J. Saidi,
and K. Anazawa, Microstructure of Fragile Metallic Glasses Inferred for Ultrasound-
Acceletared Crysltallization of Pd-Based Metallic Glasses, Phys. Rev. Lett. 95, 245501
(2005).
14. G. Barcaro, A. Fortunelli, F. Nita, and R. Ferrando, Diffusion of palladium clusters
on magnesium oside, Phys Rev. Lett. 95, 246103 (2005).
15. W.B. Clarke, B.M. Oliver, M. McKubre, F.L. Tanzella, and P. Tripodi, Search for
He and He in arata-style palladium cathodes II: evidence for tritium production,
Fus. Sci. Technolog. 40, 152, (2001).
16. K.S. Novoselov, D. Jiang, F. Schedin, T.J. Booth, V.V. Khotkevich, S.V. Morozov,
and A.K. Geim, Two-dimensional atomic crystals, PNAS 103, 10451 (2005).
17. R.A. Oriani and J.C. Fisher, Energetic charge particles produced in the gas phase by
electrolysis, Proc. ICCF10, 567 (2006).
18. W.A. Ranken, T.W. Bonner, and J.H. McCrary. Energy dependence of F 1 9 + p reac-
tions, Phys. Rev. 109, 1646 (1958).
19. Y. Arata and Y.-C Zhang, Anomalous production of gaseous He at the inside of
'DS-cathode' during D 2 0-electrolysis Proc. Jpn. Acad. 75B, 281 (1999).
20. T.A. Chubb, Modeling the He concentration in a clarke et al. gas sample from an
arata-style cathode, Proc. ICCF9, 67 (2002).
21. X.Z. Li, M.Y. Mei, J. Tian, D.X. Cao, and C.X. Li, Coherence in cold and hot fusion,
ICCF8, Conference Proceedings. Vol. 70 in: F. Scaramuzzi (ed.), SIF, Bologna, (2000)
p. 357; X. Z. Li.
481
22. LP. Chernov, Y.P. Cherndantzev, A.M. Lider, and G.V. Garanin, Excess heat re-
leased upon Hydrogen isotopes electrolytical saturation into Metals covered by porous
film, Proc. 8th Russian Conf. Cold Nuclear Transmutation of Chemical Elements, 133
(2001).
MULTIPLE SCATTERING OF D E U T E R I U M WAVE F U N C T I O N
N E A R SURFACE OF PALLADIUM LATTICE
SHU X. Z H E N G A N D D O N G X. C A O
Department of Engineering Physics, Tsinghua University, Beijing 100084, China
The wave property of deuterons and the periodicity of the lattice introduce the
coherences in various aspects of the interaction between the deuterons and the lat-
tice. Multiple scattering of deuterium wave function inside a super-lattice would
manifest itself through an example where the coefficients of the reflection, pene-
tration, and absorption are calculated while a deuterium flux permeates through
a palladium foil coated with alternative layers of titanium carbide and palladium.
When the resonance condition is satisfied, the maximized total absorption coeffi-
cient might be greater than 50%, even if the absorption coefficient of each single
layer is only less than 1%.
1. Introduction
Coherence has been an important issue to explain the abnormal phenomena in the
palladium deuteride since 1989. However, the word of "Coherence" was used in a
variety of situations such as "Q.E.D. Coherence in Matter", 1 "Ion Band State", 2
"Swimming Electron Layer Model" , 3 "Selective Resonant Tunneling" , 4 etc. If we
dug into the essence of "Coherence", we might find two important factors: the
periodicity of the lattice and the wave nature of the deuteron. These will be the
starting points of this paper.
482
483
the equilibrium between the hydrogen inside and outside palladium is still sensitive
to the surface condition of the palladium. 7 It was familiar that a coating layer
of palladium black would work like a catalyst to speed this equilibrium, but the
mechanism of these anomalies are not clear. The only thing we know is that these
anomalies are not explainable in terms of diffusion model. Since the discovery of
the correlation between deuterium flux and heat flow in the gas-loading phase, 8 ' 9
we studied the dependence of the deuterium flux on the number of coating layers,
and its dependence on the palladium temperature. 1 0 ' 1 1 Both of these dependences
are not explainable in terms of diffusion model either.
100 100
45000 50000 55000 60000
Time (s)
Figure 1. The solid line in the upper plot shows the deuterium flux, and the solid line in the
lower plot shows the temperature of the D / P d system. Two peaks appear clearly between 150 and
140° C.
25
(f) PO-
OJ
LU)
LU
:?" 15-
T ° "
10 v i o -
+J
? ~y
0 5"
0 5=
§ O
Temperature (°C)
Figure 2. A deuterium flux peak appears near 140° C when the temperature of D / P d system in-
creases. There were three alternative coating layers (Pd-TiC) on the surface of a Pd-foil (thickness
0.1mm).
485
= h 20
« O)
alu eof
O 15
X
10
V X
5
Pea
0
0 1 2 3 4 5 6
Number of layers
Figure 3. The peak flux value as a function of the number of the alternative coating layers on
the surface of the Pd foil (thickness 0.1 mm).
electrons; hence, one might wonder if the vibration of the lattice might destroy the
Coherence.
the surface. As a result, we have the relation for two components of the momentum
in two directions:
k2=kf+k2±. (1)
Here, k is the total momentum, fcy the component of the momentum of the
deuteron moving in the direction lying on the surface of the palladium; k± is the
component of the momentum of the deuteron in the direction perpendicular to
the surface of palladium. As above mentioned, the periodicity in the surface layer
requires that:
2ir
fell = k0 H n. (2)
" a
Here, n is an integer, a the lattice constant, and fco is the eigenvector in the first
Brillouin region.
For the permeation in the k± direction, instead of diffusion coefficient the wave
theory would give the reflection, transmission, and absorption coefficients, respec-
tively.
4. Some Qualitative Comparison between Theory and Experiment
Before a quantitative comparison available, we may study some of the qualitative
feature for any coherence.
4 . 1 . Temperature Effect
Temperature may change the kinetic energy of the deuteron; hence, the wavelength
of deuteron. Thus the wave property should be affected by the temperature. In
Eq. (1), the total momentum k is determined by the kinetic energy of the deuteron;
hence, k is a function of temperature. It is known that there are several tempera-
ture intervals where we have seen the anomalous phenomena in the D/Pd systems.
The famous "Heat after Death" phenomenon appears near 100°C;14 the nuclear
transmutation experiments were done preferably near 70°C; 15 Arata and Zhang's
new Double-Structure experiments were done near 140°C,16 and we discovered the
correlation between anomalous deuterium flux and heat flow just near 140-150°C
as well. 8,9 These specific temperatures might be the result of some coherence ef-
fects between deuteron wave and the periodicity of the lattice. When temperature
increases, both the lattice constant and the kinetic energy of the deuteron may
increase. However, the effect of kinetic energy dominates. When more specific tem-
peratures are available we may find their relation with some integers just like that
of low energy electron diffraction.12
the layer next to the surface layer. The destructive interference might greatly reduce
the total reflection wave, and enhance the permeation of the deuteron through the
palladium foil. A high gradient of deuteron density would appear near the surface
to accommodate this enhanced permeation. This high gradient of deuteron density
might be a good region to sustain some coherence. Iwamura's nuclear transmutation
experiment supported this surface effect.15
5. Numerical Calculation
5.1. New Paradigm of Theoretical Description
Reflection, absorption and transmission coefficients are introduced instead of cross-
section or life-time here, because we are supposed to set up a model to describe the
interaction between the deuteron wave and the periodical lattice well in a steady
state. Cross-section is not suitable here, because we are no longer dealing with
a beam-target configuration. In the lattice-well-confinement configuration, the re-
flected wave from the Coulomb barrier may be reflected again by the lattice well.
The bouncing back and forth motion happens not only inside the nuclear well, but
also inside the lattice well. It is a new kind of resonant interaction between nuclear
scale and lattice scale. Hence it is a new paradigm of theoretical description.
We would not use the concept of decay-time of a resonant state here either,
because we prefer to study a steady state, i.e., a self-sustaining state maintained by
a constant flux.
There are three kinds of coherence: the resonance inside the nuclear well; the
coherence in multiple scattering of deuteron wave by the symmetric lattice centers;
and the coherence between different layers in parallel to the surface layer. In order
to simplify the calculation, we start from the simplest configuration, and attempt
to answer the most important question: i.e., is it feasible to confine the deuterons
inside the lattice well in order to enhance the d + d fusion reaction rate dramatically
at low energy in terms of multiple scattering mechanism.
A(N) T(N)
R(N)
R(1),/\(1)
Figure 4. Multiple layer model. Coefficient of absorption and reflection (A(N) and R(N)) of
multiple layer are function of single layer properties (A(l) and R ( l ) ) .
*in(l)=M(l)*out(l). (3)
489
This matrix is written in the plane-wave representation. For example in the case
of outgoing wave only (see right-hand-side of Fig. 4),
*out(l) (4)
(7)
We have,
"M(l)n+M(l)2
a arccos
A(l) A(l)
arccos< 1 cos(2c/>) -i —^sin(2</>) (8)
T(1)L
This a is different from 0, because a is calculated for an incident wave, which
is a combination of two plane-waves traveling in both directions. For the case of
iV-layers, the scattering matrix equation should be written as
* in (JV) = M(iV)* out (7V). (9)
If we keep the outgoing wave function same as before; then,
WW) (10)
We may assume
M(JV)n M(N)12
M{N) (11)
M{N)2l M(N)22
490
Hence,
'M(N)u
*in(iV) (12)
_M{N)21
Based on matrix algebra, it can been proved that
Wl ^M(1)ll.*iM. (13)
sin [a] sin[aj
M(Nhl s * 1 M ( 1 ) 2 , (14)
sin[a]
The reflection coefficient, penetration coefficient, and the absorption coefficient
may be written as the function of the elements of the scattering matrix:
|M(1) |2
fl 1 5
(!)= u ,
|M(1) • ( )
ii
T ( 1 ) 3 ( 1 6 )
« '
A(l)sl-i!(l)-r(l). (17)
The similar definition is valid for iV-layers
_ |M(AQ 21 | 2
R{N) (18)
= WW'
T (19)
w = mkrf'
A(7V) EE 1 - R(N) - T(N). (20)
An important conclusion may be drawn from this very general relationship be-
tween M(iV) 2 i and M ( l ) 2 i Eq. (14): when the reflection rate for single cell is not
zero; the total reflection rate for N cell might be zero as long as
Sin[j
^ = 0. (21)
sin[aj
In physics, this is the result of destructive interference among all the reflected
waves. At the same time R{N) = 0 implies T(N) —> 1 when there is no absorp-
tion. It means a constructive interference among all the propagating waves inside
A^-layers, which enhances the penetration rate greatly. The conservation of the
probability guarantees the eventual penetration after all the reflections and pene-
trations in layers.
Now we may introduce a small absorption coefficient, A(l) <g; 1, for a single layer.
Every time the deuteron flux passing through a single layer would be absorbed by
a fraction of A(l). The multiple scattering causes a lot of scattering among all
these layers before the deuteron flux finally leaves palladium. The total absorption,
A(N), would become a greater number if the deuteron flux is bouncing back and
forth many times inside the multiple layers. Figure 5 is a numerical result for the
case ofA(l) = 0.01, N = 20. -R(l) is assumed to be equal to T(l) for simplicity. The
491
abscissa is the phase angle variation for each layer, </>. It depends on the distance
between two adjacent layers also. The ordinate is the three coefficients, A(N), T(N)
and R(N).
Figure 5. The total absorption coefficient, A(N), transmission coefficient, T(N), and reflection
coefficient, R(N) for the case of 20-layers with A(l) = 0.01 for a single layer.
6. Discussion
6.1. Positive Correlation between Total Absorption and
Transmission
The solid line, A(N), and the dash-dot line, T(N) reach the peak and valley at the
same position. This is just what we expected for a deuteron wave, which is reflected
from the surface of the palladium layers. When the reflected wave is minimized
[the dotted line, R(N) reaches the valley], the wave entering multiple layers is
maximized. Hence, both the total absorption, A(N) and the total transmission,
T(N) reach the peak.
6 . 5 . Concluding Remarks
T h e coherence between the deuteron wave and the periodic structure of the mul-
tiple layers may explain the positive correlation between the excess heat and the
deuterium flux near the surface of the palladium. We may use this coherence to
confine the deuteron wave inside the multiple layers in order to enhance the fusion
reaction rate in the metal deuterides.
Acknowledgments
This work is supported by the Natural Science Foundation of China (#10475045),
Ministry of Science and Technology (Division of Fundamental Research), and Ts-
inghua University (985-11, Basic Research Funds).
References
1. G. Preparata, Q.E.D. Coherence in matter. World Scientific, Chapter VIII (1995).
2. T.A. Chubb and S.R. Chubb, Fusion Technol. 20, 93 (1991).
3. H. Hora et al, Phys. Lett. A175, 138 (1993).
4. X.Z. Li et al., Laser Part. Beams 22(4), 469 (2004).
5. A.H. Verbruggen et al, Phys. Rev. Lett. 52, 1625 (1984).
6. X.Z. Ren et al, The Proceedings of ICCF9, in: Xing Z. Li (ed.), Tsinghua University
Press (Beijing, China, 2003) 19-24 May (2002) p. 305.
7. G. Alefeld and J. Volkl, Hydrogen in Metal Springer-Verlag, Berlin, Vol. 1 (1978).
8. X.Z. Li, et al, The Proceedings of ICCF9, in: Xing Z. Li (ed.), Tsinghua University
Press (Beijing, China, 2003), 19-24 May (2002) p. 197.
9. X.Z. Li et al, J. Phys. D: Appl. Phys. 36, 3095 (2003).
10. X.Z. Li, G. L. Schmidt, and J. Tian, The Proceedings of the 5th Asti Workshop on
Anomalies in Hydrogen/Deuterium Loaded Metals, Asti, Italy (19-21 March 2004).
493
FULVIO F R I S O N E
Department of Physics, University of Catania, Via Santa Sofia 64, 95125 Catania, Italy
E-mail: fulvio.frisone@ct.infn.it
Tel: +39-095-3785227; Fax: +39-095-3785227
1. Introduction
Over the last five years, the theoretical investigation into the phenomenon of cold
fusion of deuterons within crystalline lattices with Cubic Face Central symmetry
has repeatedly suggested that tunneling, following which fusion should occur, could
be significantly influenced by impurities present in the lattice or by variations in
the temperature of the system. 1 _ 3 In particular, we have suggested that when these
factors act simultaneously they have the effect of reducing the thickness and depth
of the attractive part of the effective potential, which describes the interaction
between deuterons, both for the pure Coulomb potential and in the case where also
the contribution from electronic screening is evaluated.
With the aim of further investigating the occurrence of effects of this type, this
paper presents an analysis of the behavior of a simplified model of a gas of interacting
neutrons, in motion within the Palladium crystalline lattice and free of interactions
with lattice ions, in order to exclude possible deformations of the effective potential
(due for example to deuteron-plasmon coupling) previously observed.1
The situation proposed is characterized by the presence of ordinary short-range
interactions between deuterons, corrected by collective type quantum effects, anal-
ogous to the formation of charge density waves (CDW) in metal lattices.
The model used is semi-classical, in the sense that it treats atoms as non-
impenetrable, deformable spheres, so as to reproduce, within the limits typical of a
494
495
The aim of the present analysis is, instead, to study the effect of interaction
between deuterons within a crystalline lattice on the process of cold fusion. Fur-
ther, the lattices available for experimental investigation always contain a certain
concentration of impurities, though small. Since one of the characteristic themes
of our research has been the elaboration of a model which better reflects "real"
processes, these two fundamental characteristics were accounted for by modifying
the expression of the probability in order to establish whether they could contribute
to the phenomenon by amplifying the tunneling effect, as previous studies 1 , 2 ' 3 in-
dicated. With regard to the influence of impurities, it was found, for example, 3
that the probability of penetrating the Coulomb barrier increases on increasing the
concentration of impurities. These appear to be able to concentrate in their vicinity
a significant fraction of the deuterons present in the metal.
The phenomenon shows characteristics analogous to the formation of a Cottrell 3
atmosphere in metals, known for some time in solid state physics. This essentially
consists of a redistribution of the impurities present in the metal around a dis-
location of the ions making up the lattice. In this case, the interaction between
impurities and dislocations can significantly modify the electrical properties of the
material. Further, particular reactions can occur, incorporating the impurities in
the core of the dislocations as a result of the different arrangement of atoms with re-
spect to that of the non-perturbed lattice. This type of process has been extensively
studied in the literature in the case of high temperature crystalline semiconductors
and metals. For the latter, it is demonstrated that the concentration of intersti-
tial impurities around a linear dislocation with point component depends on the
temperature according to a law of the type J = JQ exp((3/bkT), where Jo is the
concentration of impurities in the zone with null internal pressure, o3 ~ Vi the
volume of the ions making up the lattice, while (3 is proportional to the difference
v<i ~ vi between the volume of the impurity atoms and that of lattice ions.
In this regard, in order to evaluate the probability of quantum tunneling at con-
stant T in deuterium loaded lattices and in the presence of impurities, Eq. (All)
(valid for non-interacting particles) must be corrected to take account of the effec-
tive deuteron-deuteron interaction. We propose, therefore, to adopt the following
expression:
— — - - Ves{r) p J ) d r . (1)
Co J IT
In Eq. (1), hujp is the vibrational energy of the phonons 8 present in the metal
(e.g. palladium), VF is the frequency of the phonon, \i the reduced mass of the
deuterons, Ves(r) the effective interaction 9 potential, and J's the concentration of
impurities present in the crystalline lattice.
Since we require for Vefi(r) an expression which can be used in the case of three-
dimensional isotropic lattice geometries, and which also takes account of the inter-
action between deuterons and variations in temperature but not of deuteron-phonon
497
Eta Pre
140 10-84
150 10-81
160 10-79
170 io-75
180 lO"73
190 io-71
200 10-70
210 10-68
220 10-65
230 10 -63
240 10-62
250 10-60
E is expressed in eV.
where q is the deuteron charge, r\ the nuclear radius, and kc = l/47reo. Then
V = 0 for r > R.
498
£f» P:
140 10
150 10
160 10
170 10
180 10
190 10
200 10
210 10
220 10
230 10
240 10
250 10
E is expressed in eV.
3. Semi-Classical Model
The semi-classical probability of tunneling is given by: 5
|T| 2 = e x p ( - 2 7 ) , (5)
Ea T«
140 10~ 8 9
150 10-87
160 10-80
170 10~ 7 6
180 10-74
190 lO"73
200 io-71
210 10-69
220 10-64
230 10-61
240 10-58
250 10~53
E is expressed in eV.
The results shown in the Tables 1 and 2 are obtained using the quantum model
while the results in Tables 3 and 4 are obtained with semi-classical model. A com-
parison of the results obtained shows that the probability of tunneling varies in
a similar way to that of the energy and concentration of impurities, although the
results differ by several orders of magnitude for equal E and J. This difference is
500
£« T ',
140 io-
150 10
160 10
170 10
180 10
190 io-
200 io-
210 10
220 10
230 10
240 10
250 10
E is expressed in eV.
evidently due to the quantum corrections, considered in only the first two tables
and not in the second two.
The dependence of the probability of tunneling on the energy and concentration
of impurities is mirrored by the trend of the effective potentials, shown in Figs. 1
and 2 for the two cases.
4. Conclusions
In Ref. 2, we showed that the thickness of the Coulomb barrier varies according
to some parameters such as the concentration of impurities within the lattice, the
temperature of the system and the vibrational energy of the deuterons, etc. The
present theoretical study has shown that, unlike the quantum case, the semi-classical
tunneling effect at constant temperature is not amplified by an increase in the
concentration of impurities. The semi-classical potential (7) varies on increasing J
in a way that reduces, rather than increases, the tunneling effect. In fact, as shown
in Figs. 1 and 2, the thickness and depth of the barrier increase.
The amplification of tunneling is seen therefore as an eminently quantum effect,
lacking analogies in the semi-classical case.
The calculations were performed supposing that the interactions 7 ' 8 between
deuterons occur within a Palladium 9 lattice, with a cubic crystalline structure and
10 d-band electrons. An in-depth study of the possible effects associated with the
transition of ci-band electrons to higher bands is presently in progress.
If the trends obtained here for the potential of interaction within the lattice
are compared with previous results, 2,3 it can be seen that in a three-dimensional
geometry, temperature effects can induce several important effects. For example,
the height of the potential barrier can be reduced for impure metals (J = 0.75%)
and the corresponding probability of fusion can vary by 3-4 orders of magnitude,
while the barrier remains substantially unchanged for pure metals ( J = 0.25%).
501
150
100
50
>
£ o
c
o
a.
-50
J =0.75% J =0.25%
-100
-150
0.1 0.2 0.3 0.4 0.5 0.6 0.7
/tA)
Figure 1. In this figure a quantum model was used. The trends of the quantum potential (2),
which contains the Morse contribution (3), (curve on left) and the modified semi-classical "shell"
potential (7) (curve on right), are shown for different values of impurity concentrations. The dotted
line (Lei) indicates the lowest energy level; the lower unbroken line indicates the total energy.
APPENDIX A
The charge density in a CDW can be written as follows:
<PA{X) = 2 7 r c o s ( ^ (A2)
150
100
50
>
j§
c
0
0)
o
CL
-50
J =0.75% J =0.25%
-100
-150
0.1 0.2 0.3 0.4 0.5 0.6 0.7
/(A)
Figure 2. In this figure a semi-classical model was used. The trends of the semi-classical potential
(7), left, and quantum potential (2), right, obtained exchanging the values of J with respect to
Fig. 1. Tunneling does not appear to be amplified for those metals with a density of impurity
J Ri 0.75%. The Morse potential was calculated at T = 295 K. The Coulomb barrier is higher in
the case of pure metals ( J sa 0.25%).
which differ only in the sign of the charge, interpretable as arrays of ir solitons of
alternating sign, each of which occupy a Lee-Rice domain of length
1
r _ x -nCV (A4)
H^ (A5)
T h e energy gap A assumes a value very close to the energy of the solitons, given
by:
E<p = T T ^ I / F / ^ P / C O . (A8)
T h e probability of tunneling between the states 4>A and </>B in a Zener model (12)
is given by
exp(-2Kad), (A9)
With
E0 = ^ . (A12)
References
1. F. Frisone, Deuteron interaction within a microcrack in a lattice at room temperature,
Fusion Technol. 39, 260-265 (2001).
2. F. Frisone, Theoretical model of the probability of fusion between deuterons within
deformed crystalline lattices with microcracks at room temperature, Fusion Technol.
40, 139-146 (2001).
3. F. Frisone, Can variations in temperature influence deuteron interaction within crys-
talline lattices? Nuovo Cimento 20(10), 1567-1580 (1998).
4. M. Rabinowitz, High temperature superconductivity and cold fusion, Mod. Phys. Lett.
B 4 , 233 (1990).
5. D.M. Brink, Semi-classical methods for nucleus-nucleus scattering, In: P.V. Landshoff,
W.H. McCrea, D.W. Sciama, and S. Weinberg (eds) 1985, p. 206.
6. J. Bardeen, Macroscopic quantum tunneling in quasi one-dimensional metals. II. theory,
Phys. Rev. Lett. 55(9), (1985).
7. F. Frisone, Study on the probability of interaction between the plasmons of metal and
deuterons. Nuovo Cimento 18 (11) 1279-1286 (1996).
8. W. Wonneberger, Effect of viscosity on collective zener tunneling in charge density
wave system, Condens. Matter 50, 23-32 (1983).
9. H. Kyeong An, Analysis of deformed palladium cathodes resulting from heavy water
electrolysis Fusion Technol. 27, 408 (1995).
N E W COOPERATIVE M E C H A N I S M S OF LOW-ENERGY
N U C L E A R R E A C T I O N S U S I N G S U P E R LOW-ENERGY
E X T E R N A L FIELD
F . A. G A R E E V A N D I. E. Z H I D K O V A
Joint Institute for Nuclear Research, Dubna, Russia
E-mail: gareevQthsunl .jinr. ru
1. Introduction
A review of possible stimulation mechanisms of low-energy nuclear reaction (LENR)
is presented in Ref. 1. We have concluded that transmutation of nuclei at low en-
ergies and excess heat are possible in the framework of the known fundamental
physical laws - the universal resonance synchronization principle, 2 and different
enhancement mechanisms of reaction rates based on it are responsible for these
processes.1 The super low energy of external fields, the excitation and ionization
of atoms may play the role of a trigger for LENR. 3 We argue that the coopera-
tive mechanism can explain how the electron volt domain can influence the nuclear
mega electron volt domain. 3 Nuclear physicists are absolutely sure that this is can-
not happen. Investigation of this phenomenon requires the knowledge of different
branches of science: nuclear and atomic physics, chemistry, and electrochemistry,
condensed matter and solid state physics.
The puzzle of poor reproducibility is explained by the fact that LENR occurs
in open systems and it is extremely sensitive to parameters of external fields and
systems. The classical reproducibility principle should be reconsidered for LENR
experiments. Poor reproducibility and unexplained results do not mean that the
experiment is wrong. Our main conclusion is: LENR may be understood in terms
of the known fundamental laws without any violation of the basic physics. The
fundamental laws of physics should be the same in micro- and macrosystems.
Let us start with the description of the hydrogen atom structure in different
models.
504
505
where r is the radius of the electron orbit and v is the electron speed. The force is
central; hence from the quantization condition (1) we have
L = |r —>p| =- mvr = nh. (4)
er solving Eqs. (3) and (4) we have
e2 n2h2
v = —, r= n ao. (5)
nh me2
Following Eq. (3)-the kinetic energy is equal toi
1 e2
Ek= mv2 = (6)
2 Tr>
506
(ur2 e2
(14)
2 r '
where
mpme
(15)
77ip + m e
The Hamiltonian (14) coincides with the Hamiltonian for the fictitious material
point with reduced mass [i moving in the external field —e2/r. If we know the
trajectory of this fictitious particle f = f(t), then we can reconstruct the trajectories
of electron and proton using equations (13)
f
r P (t) = ^ (t), fe(t) = ^—f%t)- (16)
mp + me mp + me
507
It is evident from (16) that the proton and electron move in the opposite direc-
tions synchronously. So the motions of proton, electron, and their relative motion
occur with equal frequency
(17)
over the closed trajectories scaling by the ratio
Ve_ _ mp v&_ _ m^ Vj^ _ mp
(18a)
v-n me' v.. mR' vn m„
xp ,ll,e U^ llbe U-p //(.^
Schelaev4 proved that the frequency spectrum of any motion on ellipse contains
only one harmonic. We can get from (16) that
Pp = P, Pe = -P, (18b)
where — P\ = m\r\. All three impulses are equal to each other in absolute value,
which means the equality of
# 4 4 = 4-46 xlCT4.
-Ek(p)
This means that the nuclear and the corresponding atomic processes must be con-
sidered as a unified entirely determined whole process.
For example, Weisskopf 5 came to the conclusion that the maximum height H
of mountains in terms of the Bohr radius a is equal to
-=2.6xl014,
a
and water wave lengths A on the surface of a lake in terms of the Bohr radius is
equal to
A 7
- « 2TT x 107.
a
Let us introduce the quantity / = rv, which is the invariant of motion, according
to Kepler's second law, then
\iv =
= —, (20)
r r
and we can rewrite Eq. (14) in the following way:
uf2 e2
U=M---. (21)
2r2 r y
'
508
We can obtain the minimal value of (21) by taking its first derivative over r and
setting it equal to zero. The minimal value occurs at
2
M/ (22)
9 '
The values of invariant of motion vf (in MeV*s) can be calculate from (23) if we
require the equality of Em\n to the energy of the ground state of a hydrogen atom
fj,f = iivr = 6.582118 x 1(T 22 = h, (24)
(3) The conservation laws are valid for closed systems. Therefore, the failure of
parity in weak interactions means that the corresponding systems are open
systems. Periodic variations (24 h, 27, and 365 days in beta-decay rates in-
dicate that the failure of parity in weak interactions has a cosmophysical
origin. Modern quantum theory is the theory for closed systems. There-
fore, it should be reformulated for open systems. The closed systems are
idealization of nature, they do not exist in reality.
(4) The universal resonance synchronization principle is a key issue to make a
bridge between various scales of interactions and it is responsible for self-
organization of hierarchical systems independent of substance, fields, and
interactions. We give some arguments in favor of the mechanism - ORDER
BASED on ORDER, declared by Schrodinger in Ref. 7, a fundamental
problem of contemporary science.
(5) The universal resonance synchronization principle became a fruitful inter-
disciplinary science of general laws of self-organized processes in different
branches of physics, because it is the consequence of the energy conserva-
tion law and resonance character of any interaction between wave systems.
We have proved the homology of the atom, molecule and crystal structures
including living cells. Distances of these systems are commensurate with
the de Broglie wavelength of an electron in the ground state of a hydrogen
atom, it plays the role of the standard distance, for comparison.
(6) First of all, the structure of a hydrogen atom should be established. A
proton and electron in a hydrogen atom move with the same frequency that
creates attractive forces between them; their motions are synchronized. A
hydrogen atom represents the radiating and accepting antennas (dipole)
interchanging energies with the surrounding substance. The sum of radiate
and absorb energy flows by electron and proton in a stable orbit is equal to
zero 8 - the secret of success of the Bohr model (nonradiation of the electron
in a stable orbit). "The greatness of mountains, the finger sized drop, the
shiver of a lake, and the smallness of an atom are all related by simple laws
of nature." 5
(7) These flows create standing waves due to the resonance synchronization prin-
ciple. A constant energy exchange with substances (with universes) create
stable auto-oscillation systems in which the frequencies of external fields and
all subsystems are commensurate. The relict radiation (the relict isotropic
standing waves at T = 2.725 K - the Cosmic Microwave Background Ra-
diation (CMBR)) and many isotropic standing waves in cosmic medium 9
should be results of self-organization of the stable hydrogen atoms, according
to the universal resonance synchronization principle, that is a consequence
of the fundamental energy conservation law. One of the fundamental predic-
tions of the Hot Big Bang theory for the creation of the Universe is CMBR.
(8) The cosmic isotropic standing waves (many of them are not discovered yet)
should play the role of a conductor responsible for stability of elementary
510
The aim of this paper is to discuss the possibility of inducing and controlling nuclear
reactions at low temperatures and pressures by using different low-energy external
fields and various physical and chemical processes. The main question is the follow-
ing: is it possible to enhance LENR rates by using low and extremely low-energy
external fields? The review of possible stimulation mechanisms is presented in Refs.
1 and 5. We will discuss new possible ways to enhance LENR rates in condensed
matter.
The energetics of the decay can be analyzed using the concept of binding energy
and the masses of particles by their rest mass energies. The energy balance from
neutron decay can be calculated from the particle masses. The rest mass difference
0.7823 MeV/c 1 between neutron and (proton + electron) is converted to the
kinetic energy of proton, electron and neutrino. The neutron is about 0.2% more
massive than a proton, an energy difference is 1.29 MeV. A free neutron will decay
with a half-life of about 10.3 min. Neutron in a nucleus will decay if a more stable
nucleus results otherwise neutron in a nucleus will be stable. A half-life of neutron
in nuclei changes dramatically and depends on the isotopes.
The capture of electrons by protons is possible
p + e~ —» n + z/e, (26)
but for free protons and electrons this reaction has never been observed which is the
case in nuclear + atomic physics. The capture of electrons by protons in a nucleus
will occur if a more stable nucleus results.
Above and in Refs. 1-3, we have discussed the cooperative and resonance syn-
chronization enhancement mechanisms of LENR. Some of the low energy external
fields can be used as triggers for starting and enhancing of exothermic LENR. It
is natural to expect that in the case of beta-decay (capture) the external electron
flux with high density, or a laser of high intensity, or any suitable external fields
should play this role. Any external field shortening distances between protons in
nuclei and electrons in atoms should enhance beta-decay (capture) or double-beta
decay (capture).
There are a great number of experiments in Japan, Italy, Russia, US, India,
China, Israel, and Canada in which cold transmutations and excess energy were
measured (see http://www.lenr-canr.org).
It is very popular to use Ni, Pd, Pt, and W as electrodes in the condensed matter
discharge (breakdown, spark, arc, and explosion) experiments. Let us consider the
case Pd electrodes. The difference of the rest mass of
therefore, the external field can open the channel 46°Pd —> 4g°Cd with Q = 1.9989.
The experimental data 1 5 seem to confirm such expectations.
Therefore, expensive and time-consuming double beta decay experiments can
be performed in cheap and short-time experiments by using suitable external fields.
This direction of research can open production of new elements (utilization of ra-
dioactive waste) and excess heat without of ecological problem.
A careful analysis of the double beta decay shows that the 2e~ cluster can be
responsible for the double beta decay. The difference between the rest mass 56°Ba
and 52°Te, which is equal to 92.55 keV, indicates the possibilities to capture the
4e~ cluster by j ^ B a . It is a full analogy with the Iwamura reactions. 16
The lack of financial support and the ignorance from the whole physical society
of LENR lead to catastrophes. The mechanism of shortening the runaway of the
reactor at the Chernobyl Nuclear Power Plant and catastrophes induced by the
High Frequency Active Auroral Research Program (HAARP) program is based
on our postulated cooperative resonance synchronization mechanism. The same
mechanism should be responsible for the International Experimental Fusion Reactor
(ITER) explosion in future.
5. Conclusion
We proposed a new mechanism of LENR: cooperative processes in whole the system
- nuclei + atoms + condensed matter can occur at a smaller threshold energies
than the corresponding ones on free constituents. The cooperative processes can be
induced and enhanced by low energy external fields. The excess heat is the emission
of internal energy and transmutations at LENR are the result of redistribution of
inner energy of the whole system.
515
References
1. F.A. Gareev, I.E. Zhidkova, and Yu.L. Ratis, Preprint JINR P4-2004-68, Dubna, 2004
(in Russian); in: Proceedings of the 11-th Russian Conference on Cold Nuclear Trans-
mutation of Chemical Elements and Ball Lighting, Dagomys, city Sochi, September
28 - October 5, 2003, Moscow 2004, p. 169.
2. F.A. Gareev, in: FPB-98, Novosibirsk, June 1998, p. 92; F.A. Gareev, G.F. Gareeva,
in: Novosibirsk, July 2000, p. 161.
3. F.A Gareev, I.E. Zhidkova, and Yu.L. Ratis, in Program Abstracts on ICCF-11, Mar-
seille: France: 2004, 31 October - 5 November; F.A. Gareev, I.E. Zhidkova, E-print
arXiv Nucl-th/0505021 vl 8 May 2005; E-print arXiv nucl-th/0511092, Vol. I, 30
November 2005.
4. LA. Schelaev, FPV-2004 (Novosibirsk, 2004), Vol. II, p. 27.
5. V.F. Weisskopf, Am. J. Phys. 54 (2), 110 (1986).
6. M. Gryzinski, FPV-2004, Vol. I (Novosibirsk, 2004).
7. E. Schrodinger, What is Life? The Physical Aspects of the Living Cell (Cambridge
University Press, Cambridge, 1967).
8. F.A. Gareev, I.E. Zhidkova, and Yu.L. Ratis, Appl. Phys. J. N 3 , 25 (2005).
http://www.iscmns.org/siena05/program.htm.
9. A.M. Chechelnitsky, E-print arXiv: physics/0105056 (2001).
10. L.S. Bratolyubova-Tsulukidze et al, Adv. Space Res. 34, 1815 (2004).
11. L.M. Libby and H.R. Luken, J. Geophys. Res. 78, 5902 (1973).
12. LP. Selinov, Isotops (Nauka, Moscow, 1970).
13. U.S. Unan et al, Geophys. Res. Lett. 15, 172 (1988).
14. H.V. Klapdor-Kleingrothaus and A. Staudt, Teilchenphysik Ohne Besschleuniger
(B.G.Teubner, Stutgart, 1995).
15. LB. Savvatimova and A.D. Senchukov, ICCF6 2, 575 (1996).
16. Y. Iwamura, ICCF11 (2005).
17. O.R. Grogoryan, A.V. Sinyakov, and S.I. Klimov, Adv. Space Res. 20, 389 (1997).
18. L.S. Bratolyubova-Tsulukidze et al., Cosmic Res. 39, 602 (2001).
P O L Y N E U T R O N THEORY OF T R A N S M U T A T I O N
J O H N C. F I S H E R
600 Arbol Verde, Carpinteria, CA 93013, USA
E-mail: jcfisher@fisherstone.com
Polyneutron theory postulates that large clusters of neutrons are bound and stable
against strong decay and that their interactions with ordinary nuclei are responsible
for a new class of low-temperature nuclear phenomena. It is postulated that these
clusters, also termed polyneutrons or neutron isotopes, grow to include hundreds
of neutrons in chain reactions fueled by isotopes such as 2 H, 1 8 0 , and 7 Li. 1 It is
anticipated that an ordinary nucleus AX and a polyneutron B n can bind to form
a composite AXBn that subsequently decays by transfers or exchanges of nucleons
between its components. The present analysis focuses on composite formation and
on the transmutations that result from composite decay.
I assume that the neutrons in polyneutrons are paired with the BCS symmetry
first described for electrons in superconductors, 2 and that breaking a pair requires
so much energy that odd-numbered polyneutrons can be produced only in reaction
with deuterium. In the reaction 2An + 2 H —> 2A+1n + 1 H transmutation of H makes
available up to 5.847 MeV for adding the odd neutron. If the mass excess of 2A+1n
were to exceed that of 2An by (say) 5 MeV, the reaction forming it would be exother-
mic by 0.847 MeV. On the other hand the reaction 2 A + 1 n + 2 H -> 2A+2n + *H would
be exothermic by 10.847 MeV with a much larger cross section, and in a chain re-
action where polyneutrons are growing and fissioning in interaction with 2 H, as in
the experiments of Iwamura et al.,3~5 the concentration of even polyneutrons is
expected to substantially exceed that of odd ones. Hence as a first approximation
I consider only even polyneutrons.
Transmutations associated with composite formation and decay are expected to
occur at differing rates. Formation is expected to be the limiting rate, depending as
it does on the very small concentration of polyneutrons. Strong reactions that do
not require associated beta decay or electron capture are assumed to be most rapid,
and to occur during composite formation. Weak reactions that require associated
beta decay or electron capture are assumed to be slower. Weak reactions that
require associated double beta decay or double electron capture are assumed to
be slower still, followed by reactions that require three or more associated weak
516
517
reactions. With the foregoing assumptions the following procedure determines the
sequence of transmutations according to the present status of the theory:
Step 1. Consider a starting element G X for which we desire to know the isotopes
to which it may be transmuted by interaction with polyneutrons. The first step
is formation of a composite ^X B n in a reaction such as ^X + D n —> ^X B n +
G+D_yl B
^ n . Such a reaction can only occur in an environment where polyneutrons
are continuously being created, as in the active region of an ongoing chain reaction.
In a newly formed composite the value of A is that for which the composite is stable
against the strong reactions ^X B n —> A+1^.XB~Nn for all positive and negative even
values of N. These reactions must be endothermic. The energy they release is
EQ = A(-^X) — /S.(A+NZX) + NS, where S represents half the change in polyneutron
mass excess associated with adding a pair of neutrons, 5 = (l/2)[A( j 4 + 2 n) —A(' 4 n)].
The reaction is exothermic for EQ > 0. Are any such transfers exothermic? If yes,
choose the most exothermic among N = ±2, ±4, ± 6 , . . . , and go to Step 2. If no, go
directly to Step 2.
Step 2. Represent the output of the previous step by ^X. Is there an isotope
zi'i'Y of the element having one more or one less proton than AX that can be
reached by exchange or transfer of nucleons within the composite? (Each of these
reactions requires an associated beta decay or electron capture.) The energy released
is Ei = A(^X) —A( J±(Y) + N5. Are any such transfers exothermic? If yes, choose
the most exothermic among z = ± 1 and N = 0, ±2, ± 4 , . . . , and return to Step 2.
If no, go to Step 3.
Step 3. Represent the output of the previous step by AX. Is there an isotope
A
^±2^ of the element having two more or two fewer protons than AX that can be
reached by exchange or transfer of nucleons within the composite? (Each of these
transfers requires two associated beta decays or electron captures.) The energy
released is E^ = A(AX) — A( 0"±2Y) + NS. Are any such transfers exothermic?
If yes, choose the most exothermic among z ± 1 and N = 0, ±2, ± 4 , . . . , and go
to Step 2. If no, continue with three or more associated weak decays, or stop if
transmutations with such decays are neglected.
The beta decays in Steps 2 and 3 can be imagined as occurring in the polyneutron
in association with transfer of the resulting proton to the ordinary nucleus. For
N = 0 each proton so formed exchanges with a neutron from the ordinary nucleus,
accelerating the rate of N = 0 beta decays to match that of N ^ 0 decays. Electron
captures can be imagined as occurring in association with transfer of a proton from
the ordinary nucleus to the polyneutron. For N = 0 each proton so transferred
exchanges with a neutron from the polyneutron, accelerating the rate of N = 0
electron captures to match that of N ^ 0 captures.
Examples of reactions and their energies are shown here in more detail.
No beta decay:
fXBn^A+NzXB~Nn + E0,
E0 = A(AX) - A(A+N2X) + N5.
518
E2 = A{AX) - A ( ^ Y ) + NS.
In my calculations, I assume that 5 is independent of A with the value S = 1.143
as tentatively determined from transmutation of 138 Ba to 150 Sm. With this value
of 5, and assuming that the binding energy of a composite is independent of the
properties of its components, it is possible to calculate the transmutation chain for
any starting isotope. (The assumption of constant 5 holds only approximately over
a limited range of values of A, and the assumption of a constant binding energy
for composites ignores the influence of shell structure of the ordinary nucleus and
of the sizes of both components. These questions should be addressed in a more
realistic treatment of the theory.)
Transmutation chains can be more easily visualized by simplifying the notation.
Abbreviate the composite AX n as (^X) where the size of the polyneutron compo-
nent is understood. Then as an example the transmutation 139 La n —> 141 Ce ~~ n
is abbreviated ( 139 La) —> ( 141 Ce). With this notation, and neglecting transmuta-
tions with three or more associated weak interactions, the transmutation chain for
139
La is
139
La + An -+ ( 139 La) - ( 141 Ce) -+ ( 141 Pr) - ( 143 Nd).
In addition to these decay channels, each composite has a side channel that frees
the ordinary nucleus and substitutes a helium nucleus, typified by
141
CeAn^4HeA~4n + 141
Ce.
In consequence, accompanying the composite decay chain there is in its wake a
residual of free isotopes 141 Ce, 141 Pr, 143 Nb whose numbers depend on the relative
magnitudes of the side channels. To recapitulate, I assume that formation of the
initial composite ( 139 La) is the rate-limiting step. Once a composite has formed,
I assume that it decays rapidly through the chain leaving behind a residue of free
519
leaving residual amounts of 140 Ce, 144 Nd, 150 Sm, 158 Gd, and so on. It leaves
a residue of free 150 Sm nuclei only for values of S that lie in the narrow range
1.142 < S < 1.144. This is the basis for my assumption that S = 1.143.
Transmutation of 88 Sr is reported to lead to 96 Mo. The reaction chain predicted
by the theory is
88
Sr + An -+ ( 90 Sr) -> ( 92 Y) -+ ( 96 Zr) ^ ( 96 Nb) ^ ( 100 Mo) -+ ( 102 Tc) ^ • • •
leaving residual amounts of 90 Sr, 92 Y, 96 Zr, 96 Nb, 100 Mo, 102 Tc, and so on. The
96
Nb residue decays to 96 Mo with a half life of 23 h. During composite formation,
mass spectrometry will reveal a signal at mass 96 from residual 96 Zr and 96 Nb, along
with 96 Mo from decay of 96 Nb. A few days after composite formation has ceased
the mass signal will come from 96 Zr and 96 Mo with an enhanced 96 Mo component
from decay of 96 Nb. A Mo signal from XPS will be obtained from the 96 Mo and
100
Mo residuals.
Transmutation of 133 Cs is reported to lead to 141 Pr, and to as yet unidentified
isotopes with intermediate masses between 133 and 141. The theory predicts
133
Cs+A n - ( 137 Cs) -+ ( 137 Ba) - ( 139 La) - ( 141 Ce) -+ ( 141 Pr) ^ ( 143 Nd)
leaving residual amounts of 137 Cs, 137 Ba, 139 La, 141 Ce, 141 Pr, and 143 Nd. The latter
portion of this chain was treated in the example above for transmutation of 139 La,
in which a signal for 1 4 1 Pr arose from the 1 4 1 Pr residual plus additional 141 Pr from
decay of 141 Ce.
Finally transmutation of 137 Ba was reported to lead to a signal at mass 149,
tentatively attributed to 149 Sm although no XPS signal for Sm could be detected.
Theory predicts the decay chain
137Ba + An_^ (137Ba) ^ (139La) ^ (141Ce) ^ (141pr) ^ ( 143Nd)
leaving residual amounts of 139 La, 141 Ce, 141 Pr, and 143 Nd as for transmutation of
133
Cs. No signal for Sm is expected. (It may be that the reported mass 149 signal
represents 137 Ba 12 C or 1 3 3 Cs 1 6 0 from contamination by carbon or cesium during
the transmutation process.)
520
Overall the agreement between theory and the experiments of Iwamura et al. is
suggestive but not definitive. Consideration of other t r a n s m u t a t i o n chains identifies
experiments t h a t could be more definitive. T h e parameter choice 5 = 1.143 implies
t h a t 2 0 7 P b and 2 0 8 P b are absolutely stable, all potential t r a n s m u t a t i o n s involving
any number of possible associated weak interactions being endothermic. Looked
at another way, these P b isotopes are the final products of t r a n s m u t a t i o n of every
starting element, provided only t h a t sufficient time is allowed. Nuclei lighter t h a n
lead t r a n s m u t e by b e t a decay alone, as in
205 T 1 + An^(205T1)^(207pb)>
These transmutations are ideal testing grounds for the theory. T h e y suggest t h a t
polyneutrons can induce transmutations where the final nucleus differs from the
starting nucleus by addition of a proton and a neutron, by subtraction of a proton
and a neutron, or by addition of two or four neutrons. Each of these reactions
requires only a single step from composite formation to the final 2 0 7 P b or 2 0 8 P b
product. Because the product is stable, one-to-one substitution of 2 0 7 P b for 2 0 5 T1
and for 2 0 9 Bi should be seen, as should substitution of 2 0 8 P b for 2 0 4 P b and 2 0 6 P b .
T h e predictions of the theory are definite and clear-cut, although minor correc-
tions can be expected when the analysis is extended to include odd polyneutrons.
If the predictions are borne out by experiment the credibility of the theory will be
enhanced. If not the theory will face a crisis.
References
1. J. C. Fisher, Fusion Tech. 34, 66 (1998).
2. J. Bardeen, L. N. Cooper, and J. R. Schrieffer, Phys. Rev. 108, 1175 (1957).
3. Y. Iwamura, M. Sakano, and T. Itoh, Jpn. J. Appl. Phys., 4 1 , 4642 (2002).
4. Y. Iwamura, T. Itoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada, T. Ishikawa,
and J. Kasagi, Proc. ICCF 11 (World Scientific Inc., 2006), 339.
5. Y. Iwamura, T. Itoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada, and T.
Ishikawa, Proc. ICCF 12 (World Scientific Inc., 2006), to be published.
T H E T H E R M A L C O N D U C T I O N FROM THE C E N T E R S OF T H E
N U C L E A R R E A C T I O N S IN SOLIDS
KEN-ICHI TSUCHIYA
Department of Chemical Science and Engineering,
Tokyo National College of Technology,
1220-2 Kunugida, Hachioji, Tokyo 193-0997, Japan
E-mail: tsuchiya@tokyo-ct.ac.jp
If nuclear reactions happen in solids, heat generated from the reaction center is
diffused. In this study, the thermal conduction from the centers of a DD reaction
in solids induced by the Bose—Einstein condensation is considered. The voids in
solids are assumed as the sites of the reaction centers. The equations of the thermal
conduction are solved using Fourier expansion. The calculated results show the
rapid temperature relaxation. This means that nuclear reactions in solids do not
induce thermal explosions.
R= (1)
m¥)—'
where imaginary part of Fermi pseudopotential V? 2 ' 3 is written as
Ah
ImV£ = -—Sin-rj). (2)
The short-range interactions of nuclear forces between two Bose nuclei are intro-
duced by using 6 function. 2 ' 3 The constant A is given by the Bohr radius TB and the
S factor of the nuclear reaction between two nuclei as A = 2Sr-e,/-Kh. The ELTB
solution also gives the critical temperature Tc of Bose-Einstein condensation (BEC)
by well-known formula which is written as
h2 ( n \2/3
where n is the local number density of Bose particles and (,{Z) is the Riemann's
zeta function. The probability of the ground-state occupation is given by
2
/ ji \ /3
f2 = 1 - f - J forT<T c . (4)
521
522
If the ground state occupation for T < Tc is taken into account the fusion rate
is given by M l When T > Tc, no nuclear reactions happen because fi = 0. The
trapped site for a deuteron cluster is shown in Fig. 1. The calculated results for Tc
and R are listed in Table 1. When N > 4 with using nonlinear screening, 4,5 Tc is
higher than the room temperature. The ELTB solution is plotted in Fig. 2 for the
case of the 5-deuteron cluster trapped at VacO.
Figure 1. The structure of VacO in fee lattice. The black and the gray circles mean occupied and
unoccupied lattice points, respectively. These defects construct octahedral void, which is called
VacO in this paper.
TV Tc R Tc R
2. Thermal Conduction
If nuclear reactions happen in solids, heat generated from the reaction center is
diffused. In this study, the thermal conduction from the center of a DD reaction in
Pd is estimated. The equation of the thermal conduction in solid is written as
dT
fcV2T, (5)
~m
where T is the deviation of the temperature from the equivalent value and t is the
time from a reaction. The constant k is defined as
k= K/Cp, (6)
where constants K, C, and p mean the thermal conductivity (75.5 J / s m K ) , the
specific heat (25 J/mol K) and the density (12.0 g/cm 3 = 12.0 x 10 6 /166.4mol/m 3 ),
523
; 1 i i2
! p/x 2
1I 1 ---•
y
m
£ i
-1 -
" ~ ;~ ~
Figure 2. The ELTB solution for the system including five-deuterons in VacO in fee Pd. Nonlinear
screening potential is used as the DD interaction. The nondimensional quantity x is defined as
x = ^mujjhp, where to = 0.86 X 1 0 1 4 s _ 1 and p2 = Ejrf. The solid line means the ELTB solution.
The dashed lines mean each potential normalized by |e| = | — 409|. (p/x 2 ; component divided
from the operators for kinetic energy, qf/x; screened DD repulsion potential. E m ; the lattice
summation for the Coulomb potentials by host Pd ions (see Ref. 1))
respectively. The initial condition used for solving Eq. (5) is T = T0 in the dxdxd
cube and T = 0 for otherwise. In this condition, the parameter d corresponds to
the size of the deuteron cluster and the initial temperature is obtained by
To = E/CMo, (7)
where constants E and MQ mean the energy generated from a DD reaction
(23.8 MeV = 23.8 x 106 x 1.60 x 10" 1 9 J) and the number of moles in the d x d x d
cube (4/Avogadro number mol), respectively. The periodic boundary condition
used for solving Eq. (5) is written as
and
T(x,y,z,t)=X(x)Y(y)Z(z)U(t). (10)
and
1/3
riiird
(-'n -l)n<2T0 • sin • (12)
riiiT L
The parameter L means distance between two neighboring reaction centers. This
parameter is obtained by the well-known formula for the concentration of Shottky
defect in solid. It is written as
n/N = e~w/k*T, (13)
where n, N, and w mean the number of defect, the number of total atoms and
vacancy formation energy (~1 eV), respectively. Assuming the uniform distribution
of the trapped sites, the parameter L is obtained by
Q iu/3fe B T (14)
L
4V3
where a is the lattice constant of fee Pd (3.89 A). As the temperature is increased,
the concentration of the vacancy is increased and the mean distance between va-
cancies is decreased. They are shown in Figs. 3 and 5. The calculated result for
the thermal conduction is plotted in Fig. 5. The rapid relaxation can bee seen in
Fig. 5.
6 •
Temperature (K)
Figure 3. The temperature dependence of the vacancy concentration n/N, where n and N mean
the number of the vacancy and the number of the total atom, respectively.
3. Conclusions
(1) If a DD reaction happens in a void, temperature of the reaction center
becomes extremely high. However rapid recovery from the high temperature
is seen, because thermal conductivities of metals are high. For the case of
Fig. 5, recovering time is smaller than 10~ 10 s. This is smaller than the
inverse of the reaction rate 108.6 x 1 0 r s _ 1 (see Table 1).
525
E 0.005
Temperature (K)
Figure 4. The mean distance between the vacancies as a function of the temperature
Figure 5. Thermal conduction from a center of a DD reaction. Position along the line x = y = z
is normalized by the size of a deuteron cluster. In this case, d = 2.45 X 10~~ 10 (rn) for 5-deuteron
cluster trapped at VacO. This corresponds to the initial temperature To = 3.85 x 10 9 (if).
526
420
400
_, 380 Tc=403 K
for five deuteron cluster trapped at VacO
| 360
a)
a.
E
|2 340
320
300
Figure 6. The rise in temperature by the iterative DD reactions. In this case, the initial tem-
perature is 300 K. For the case of 5-deuteron cluster trapped at VacO, T c of BEC is 403 K (see
Table 1), which is shown by dashed line. After the 1.3 X 10 8 times iterative DD reactions, the
temperature becomes higher than T c and BEC is broken.
References
1. K. Tsuchiya, Q u a n t u m s t a t e s of d e u t e r o n s in P d , Int. J. Hydrogen Energy 2 9 , 1513
(2004).
2. Y . E . K i m a n d A.L. Zubarev, Nuclear fusion for Bose nuclei confined in ion t r a p , Fusion
Technol. 3 7 , 151 (2000).
3. Y . E . K i m a n d A.L. Zubalev, Equivalent linear t w o - b o d y m e t h o d for m a n y - b o d y p r o b -
lems. J. Phys. B: Atomic, Molecular and Optical Physics 3 3 , 3905 (2000).
4. H. H o h e n b e r g a n d W . K o h n , I n h o m o g e n e o u s electron gas, Phys. Rev. 1 3 6 , B864 (1964).
5. W . K o h n a n d L.J. S h a m , Self-consistent e q u a t i o n s including exchange a n d correlation
effects, Phys. Rev. 1 4 0 , A1133 (1965).
F O U R - B O D Y RST G E N E R A L N U C L E A R W A V E F U N C T I O N S A N D
MATRIX ELEMENTS
I R F A N C H A U D H A R Y A N D P E T E R L. H A G E L S T E I N
Research Laboratory of Electronics, Massachusetts Institute of Technology, Cambridge,
MA 02139, USA
E-mail: irfanc@mit.edu, plh@mit.edu
1. Introduction
Physicists have long assumed that the dynamics of nuclear reactions in condensed
matter proceeds fast enough that successful approximations can be obtained using
a vacuum approximation. Such an approach has been widely successful for many
decades in the case of nuclei that have been accelerated. The many experimen-
tal claims for anomalous effects in metal deuterides, such as excess heat, helium,
low-level fusion, and fast alpha emission, suggest that the use of the vacuum ap-
proximation may not be universally applicable. We have been interested in the
development of models in which the vacuum approximation is not made, and in
which the nuclear system interacts with the local condensed matter environment.
Our focus in recent years has been on models in which we propose that phonon
exchange takes place during a nuclear reaction that occurs in a lattice. If exchange
happens in the case of a highly excited phonon mode, quantum coupling may occur
with other processes that exchange phonons with the same phonon mode.
In the case of deuteron-deuteron (d-d) fusion reactions, the resonating group
approximation was used for many years as the primary theoretical tool with which
to understand reactions, and to predict reaction cross-sections. We have been inter-
ested in the generalization of the resonating group method to include lattice effects.
A possible generalization is one in which the channel separation factors of the res-
onating group method, which describe the center-of-mass dynamics, is replaced by
a more general channel separation factor, which describes the center-of-mass dy-
namics of the reacting nuclei on the same footing with other nuclei in the lattice.
We have termed this a "lattice resonating group method".
To make detailed calculations with this approach, we need to be able to compute
matrix elements and interaction potentials in the presence of phonon exchange. To
implement such calculations, one approach is to simply include phonon operators in
527
528
the basic description of a nucleon (i.e. proton or neutron) co-ordinate. For example,
if nucleon j were bound to a nucleus, we would be perfectly content in a vacuum
calculation thinking of the position of the nucleon as being determined relative to
the nuclear center-of-mass co-ordinate. One often finds this notion expressed as
Tj = R a + Xj, (1)
Yj = R a + Xj, (2)
with the associated interpretation that the nucleon co-ordinate Vj itself depends on
the lattice through the position of the nuclear center-of-mass co-ordinate R 0 , which
is an explicit phonon operator.
To compute nuclear matrix elements including phonon exchange, we need simply
to express the nuclear wavefunctions as explicit functions of the spatial co-ordinates,
and then perform integrations as required. Since the wavefunctions and the nuclear
interaction have spin and isospin degrees of freedom, this task very quickly becomes
much less simple.
One encounters an additional difficulty. To implement this program, we are
interested in working with general correlated wavefunctions, focusing on the spatial
dependence to implement phonon operators. Nuclear physicists instead usually
generally make use of Racah algebra for interaction matrix element calculations,
which is based on an independent nucleon (protons or neutrons) approximation.
There does not exist much in the literature, which is helpful in implementing phonon
exchange more fundamentally in the case of general wavefunctions.
Consequently, we have undertaken a program in which the wavefunctions are
written explicitly as functions of space, spin and isospin; and in which matrix
elements are reduced to sums of spatial integrals. In this paper, we focus on the
four-nucleon problem.
2. Four-nucleon Wavefunctions
Group theory and the Pauli exclusion principle place rigid constraints on the form of
the wavefunction. The exclusion principle dictates that the total wavefunction must
be totally antisymmetric. Each wavefunction can be characterized by a total spin
and isospin. However, by the Schur-Weyl duality, the spin (and isospin) determines
the irreducible representation of the symmetric group that the spin (and isospin)
wavefunction can belong to. The Clebsch-Gordan series of the symmetric group
529
* = YlCMAS\AT\j, (3)
3
where [R]j, [S]j, and [T]j are the space, spin and isospin parts, respectively, and
the Cj are the products of the Clebsch-Gordan coefficients of the symmetric group,
5(4).
In this paper, we focus on the T = 0 case only. This is the simplest case, and
contains the important example of d-d fusion reactions (in an approximation in
which the neutron and proton channels are equivalent). The generalization to other
isospins is conceptually and computationally completely straightforward. However,
the number of terms increases significantly. At this level of discussion, we neglect
the Coulomb potential, which does not conserve isospin.
4321 1
3211 2
3121 3
1321 4
2211 5
2121 6
2111 7
1211 8
1121 9
1111 10
S = 0
S = 1
S = 2
* 6 = -?= [^5S10^6 - 1p6SWt5] •
3. T h e Nuclear Potential
/ , Cj C
'k {[R]j l-ffscalari [R']k) , (5)
jk
where
H scalar ([S\An3\HHj\[S']k[T']k)
The significance of this result is that the matrix element is now expressed as a sum
of spatial integrals, with the spin and isospin algebra evaluated to contribute to the
expansion coefficients.
an = are
where ipio = V'IOC^IJ • • • >^i) d ^5 V'sC^ii • • • I^A) functions of spatial co-
ordinates alone.
532
5. T r a n s i t i o n M a t r i x E l e m e n t for a T — 0 F u s i o n R e a c t i o n
We can now formally calculate the reaction matrix elements for the d - d fusion
reactions including phonon coupling. Since we are focusing on isospin-preserving
T = 0 matrix elements, this calculation applies to isospin-preserving reaction
models. T h e relevant states are:
5 . 1 . Physical Wavefunctions
T h e wavefunctions discussed above are formal R S T objects, which are very general.
We need to focus on specific wavefunctions for the different mass 4 (T = 0) channels
in order to proceed. For example, the wavefunction for the ground state 4 He nucleus
can be taken to be just \l/i with a spatial p a r t t h a t is completely symmetric. Hence
For simplicity, we adopt a wavefunction for two deuterons t h a t are in a quintet (spin
2) state. In this case, we can use
1
V(12; 34) = Mr2 - r i ) 0 d ( r 4 - ?3) F ( j ^ , ^ ± ^ j . (9)
There are two kinds of 3 + 1 wavefunctions, including singlet and triplet states.
T h e singlet S = 0 states can be written a s b
a
We should, in general, consider the deuterons to be in a singlet or triplet as well. However, we
are only doing an example here. In this enumeration of states, we are ignoring the various Mg
values.
The subscripts 211, 121, and 111 are the Yamanouchi symbols for the 3-body wavefunctions
533
-V(123;4)^(s 8 ti2i(mT = - l / 2 ) T 4 - S 9 t 2 i i ( m T = - l / 2 ) T 4 ) ] .
(11)
We used the notation | 4 or J.4 to refer to the isospin of the fourth particle. The
spatial part of ^ i and ^'3 1 is of the form
where 03 only depends on the two co-ordinate differences such as f\ —ri and r^ — r^.
0 5 = - L [2^(12; 34) + 2^(34; 21) - 0(23; 14) - ^(14; 23) - 0>(13; 24) - </>(24; 13)],
V 12
In the case of the singlet 3+1 channel, the antisymmetrizer acts to produce a single
ladder basis state
*4{*3,i} = * i , (14)
where the associated fully symmetric spatial part -0io can be expressed as a
symmetric combination of the physical 3+1 states as
c
T h e results will only involve * i , \&4, and \&6- These wavefunctions and no others are involved
because of group theoretical considerations and our assumptions that the spatial part of the
deuteron, triton, and helium wavefunctions are symmetric under the exchange of any two particles.
534
In the case of the triplet 3+1 channel, the antisymmetrizer acts to produce a single
ladder basis state
A{*'3il} = *4) (16)
where the associated mixed symmetry spatial parts I^T, ip$, and xpg are
V9 = - ^ ( 1 3 4 ; 2 ) - V ( 2 3 4 ; l ) ] . (19)
The computation of the relevant matrix elements is made simpler because we have
a complete set of results for the matrix elements available in terms of the ladder
basis.
6. Matrix Elements
We focus here on one specific example:
The rest of the matrix elements can be calculated similarly. From our previous
example we know that
3 ^ (a 12 + iyu) Z12 ypjrn)
<*I(0)|VT|*6(1)> = / ^1*0 ^ d f\ • • • d ?4.
r
/' 12
We can use this with the appropriate definitions of the spatial wavefunctions for
the different channels:
•05 = ~4= [2^(12; 34) + 2V>(34; 21) - ^(23; 14) - ^(14; 23) - V(13; 24) - ip(24; 13)] ,
V 12
(21)
V-io = \ [V>(123; 4) + V(124; 3) + ^(134; 2) + ^(234; 1)]. (22)
7. Conclusions
To include phonon exchange in a description of nuclear reactions, we require a
description explicitly in terms of spatial wavefunctions. We have developed a com-
plete set of such nuclear wavefunctions for the 2-body, 3-body, and 4-body problems
using a ladder basis. Results for the 4-body case is presented above. A complete
set of matrix elements for the HJ potential has been developed in terms of ex-
plicit spatial integrals. Antisymmetric wavefunctions that are appropriate for d-d
fusion calculations in the T = 0 approximation have been developed, and we have
presented a specific example in this paper.
535
Acknowledgments
Support for I. C h a u d h a r y was provided by the Kimmel Fund, Bose Foundation, and
from a D a r p a subcontract.
References
1. M. Hamermesh, Group Theory and its Applications to Physical Problems (Addison-
Wesley, New York, 1962).
2. T. Hamada and I.D. Johnston, Nucl. Phys. A34, 382 (1962).
S T U D Y ON FORMATION OF T E T R A H E D R A L OR OCTAHEDRAL
S Y M M E T R I C C O N D E N S A T I O N B Y H O P P I N G OF ALKALI OR
ALKALINE-EARTH METAL ION
HIDEMI MIURA
1-27-6 Tsurugaoka, Izumi-ku, Sendai 981-3109, Japan
E-mail: miubrewer@h9. dion. ne.jp
1. Introduction
Much research on nuclear fusion and nuclear transmutation in condensed matter is
currently in progress. Recently, experiments with deuterium permeation through
Pd complex by Iwamura et al. have indicated that nuclear transmutations occur
with alternating CaO and Pd layers, but no nuclear reaction is observed when
this material is replacing it with MgO. 1 On the theoretical side, we have directed
our attention to Tetrahedral Symmetric Condensate/Octahedral Symmetric Con-
densate (TSC/OSC) model of protons/deuterons by Takahashi, which can explain
consistently the major experimental results. 2 " 4
We have examined the role of the alkali and alkaline-earth metal ions in the
crystal lattice of the host metal when TSC/OSC is formed. As a result, we have
obtained a very consistent and simple scenario as one of hypotheses about the
formation of TSC/OSC that the alkali or alkaline-earth metal ions infiltrating into
the host metal make cavities there, when they hop onto the other sites of the crystal
lattice, then through squeezing of H+/D+ ions in the cavity the protons or deuterons
undergo TSC/OSC.
2. Scenario of Formation of T S C / O S C
Experiments on nuclear fusion and nuclear transmutation in condensed matter are
performed, for example, by the electrolysis of LiOH/LiOD or K2CO electrolytic
solution using Ni or Pd cathode, and by the deuterium permeation through
alternating CaO and Pd layers, respectively. The scenario about the formation
of TSC/OSC is constructed from following five processes that would proceed in the
face-centered cubic (fee) lattice of the hydride-forming metals. This scenario would
be as simple as possible with the role of the alkali or alkaline-earth metal ions.
536
537
Tetrahedron Octahedron
Q:Ni/Pd D:Tsite O : 0 site
H+/D+ ions permeate into the fee crystal lattice of the host metal such as Ni and
Pd by electrolytic voltage and D2 gas pressure, and they are located mostly at the
O sites. Although H+/D+ ions move corresponding to the permeation rates, they
are confined at the O sites of the crystal lattice of the host metal for a short while.
infiltrate into the fee crystal lattice of it, and they come to the T sites, O sites, and
the lattice voids or defects.
In the case of electrolysis, alkali metal ions accumulating on the surface of the
host metal infiltrate into the near surface layers due to the surface vibration and
the electrolytic current, and then mostly stay at the T sites of the crystal lattice
for a long while. Each of the alkali metal ions at the T sites vibrating thermally
interacts with four H + / D + ions at the vertexes of the tetrahedron surrounding it
and vibrates them widely.
In the case of deuterium permeation, alkaline-earth metal ions staying in contact
with the surface of the host metal also infiltrate into it due to the surface vibration
and the deuterium flow, and then mostly stay at the lattice voids or defects for a long
while. Each of the alkaline-earth metal ions at the lattice void or defect vibrating
thermally also interacts with six H+/D+ ions at the vertexes of the octahedron
surrounding it and vibrates them widely.
ions hop onto the other sites of the crystal lattice of the host metal due to the
thermal vibration, electrolytic voltage and most probably some electromagnetic im-
pulses, and then make cavities at the former positions. The alkaline-earth metal ions
also hop due to thermal vibration, deuterium flux, and electromagnetic impulses,
also making cavities.
Impulse
fi#o "
V Condensed and recoiled * S • i f / K+ V Condensed and recoiled
V
4p/TSC, 4dfTSC ^ 6d/0SC
Tetrahedron 4^:Ca + Octahedron
O^Ni/Pd D:Tsite O : o site
Figure 2. Hopping of alkali or alkaline-earth metal ions, Squeezing of H + / D ions, Recoil and
Condensation of protons/deuterons (typical).
phonon of the crystal lattice of the host metal is caused by electromagnetic impulse
simultaneously with or after the hopping-out of the alkali or alkaline-earth metal
ion, and the coherent oscillation of phonon is just in the decreased mode, it might
be possible to cool down the local region effectively, although the frequencies of only
a few modes decrease almost 10 meV at the most.
4. Conclusion
Acknowledgements
T h e author wishes to t h a n k Professor Takahashi of Osaka University for valuable
information and advice.
References
1. Y. Iwamura, T. Ithoh, M. Sakano, N. Yamazaki, S. Kuribayashi, Y. Terada, T. Ishikawa,
and J. Kasadi, Low energy nuclear transmutation in condensed matter induced by
D2 gas permeation through Pd complexes, Proc. ICCF11 (in press) http://www.lenr-
canr.org/
2. A. Takahashi, Deuteron cluster fusion and related nuclear reaction in metal-
deuterium/hydrogen systems, Recent Res. Devel. Phys. 6, 1-28 (2005).
3. A. Takahashi: 3 He/ 4 He PRODUCTION RATIOS BY TETRAHEDRAL SYMM-
TERIC CONDENSATION, Proc. ICCF11 (in press) http://www.lenr-canr.org/
4. A. Takahashi, Mechanism of deuteron cluster fusion by EQPET model, Proc. ICCFIO
(in press) http://www.lenr-canr.org/
5. T. Ohshima and Y. Ohtsuki (eds.), Surface Phonons, Front of Physics Vol. 30
(Kyoritsu, 1992) (in Japanese).
CALCULATIONS OF N U C L E A R R E A C T I O N S P R O B A B I L I T Y IN A
CRYSTAL LATTICE OF L A N T H A N U M D E U T E R I D E
V . A . K I R K I N S K I I A N D Y U . A. N O V I K O V
Institute of Mineralogy and Petrography, Siberian Branch of the Russian
Academy of Sciences, Prospect Academy Koptyuga 3, Novosibirsk 630090, Russia
E-mail: kirkinsk@uiggm.nsc.ru
The dynamic model of electron orbitals deformation was previously devised for pal-
ladium deuteride. It has now been applied to calculate the probability of nuclear
reactions of hydrogen isotopes in the crystal lattice of lanthanum deuteride. In a
series of computer simulations, the probability of D—D approach for random initial
conditions was calculated, when the initial energies of the approaching deuterons
were set in the range of 0.001-9.0 eV. For each experimental value of D—D ap-
proach the reaction rate was calculated on the shifted Coulomb potential with the
shift energy, which equals to the energy of screening. The mean distance of D - D
approach on the whole series equals 0.19 A. More than 54% of all experimental val-
ues show an approach of deuterons at a distance smaller than 0.1 A. The average
reaction rate for the given set of the initial conditions is 10 3 , 2 8 s _ 1 per DD pair.
This is three orders of magnitude less than the analogous rate calculated earlier
for palladium deuteride. Allowing for the higher D content and the higher number
of adjacent tetrahedral sites in LaD3 as compared with PdDo, 6, an overall nuclear
fusion rate in lanthanum deuteride will be only slightly lower than in palladium
deuteride, that is, 1 0 ~ 1 2 - 1 0 - 1 4 s _ 1 per DD pair.
542
543
measurements of excess energy output (see, e.g. Ref. 5 and reviews in Refs. 1
and 6).
Later, using the same model, the rate of a nuclear reaction was calculated in
a titanium deuteride, where deuterium atoms are situated in tetrahedral sites of a
crystal lattice, and the limiting content corresponds to TiD2 crystal structure. 4
In the present paper, we calculate the probability of a nuclear interaction in
lanthanum deuteride, in which deuterium atoms can reside both in octahedral and
tetrahedral sites of closely packed lanthanum atoms forming the LaD3 crystal lat-
tice. The high content of deuterium in lattice should be favorable for implementing
a nuclear interaction. Studies of lanthanum deuteride are also valuable because
based on them we can draw conclusions about analogous compounds of lanthanide
elements and yttrium, which have a similar lattice with slightly diminished crystal
lattice parameters.
For calculations of probability of nuclear reactions of hydrogen isotopes in the
crystal lattice of lanthanum deuteride the dynamic model of electron orbitals defor-
mation (EODD) offered earlier for palladium deuteride was used. 1-3 The hydrogen
isotopes predominantly occupy tetrahedral sites in the face-centered cubic lattice of
lanthanum hydride. Symmetrical positions of deuterium atoms with respect to the
edge connecting two adjacent tetrahedral sites in lanthanum were selected as initial
conditions for numerical tests. The initial trajectory of lanthanum 6s-electron was
set as an ellipse, in one of its focal points a nucleus of lanthanum atom with an effec-
tive charge Z\,& is located. The effective charge Z\,a is calculated from the potential
of ionization and the maximum radial density of La 6s-orbital wave-function.7 The
electron can be found also on ellipse-like trajectories, which are distinct from the
most probable ones, at different electron distances from La atom nucleus at the
apogee. The calculations were carried out also for such trajectories using different
initial outer electron orbital radii (see below). In a series of computer simulations,
the probability of D-D approach for random initial conditions was calculated in the
initial energy range of 0.001-9.0eV of approaching deuterons (the potential barrier
for diffusion of deuterium atoms in lanthanum is about 0.43 eV). The most favorable
conditions of two deuterons approaching one another were determined by prelimi-
nary computer modeling1 within the framework of the described model to reduce
the calculation time. For each experimental value of D-D approach the reaction
rate was calculated on the shifted Coulomb potential with the shift energy, which
is equal to the energy of screening.
The series consists of 40,000 experimental values. The mean distance of D-D
approach on the whole series equals 0.19 A, however, more than 54% of all exper-
imental values show an approach of deuterons for a distance smaller than 0.1 A.
If one considers the reaction rate at each case of approach, and then averages as a
whole on the entire sample, the general reaction rate for the given set of the initial
conditions will make 10 3 2 8 s _ 1 per DD pair. It is three orders of magnitude less
than the analogous rate calculated earlier for palladium deuteride, 1_3 but more than
10 times higher than the rate calculated for titanium deuteride. 4
544
0.0 1.0 2.0 3.0 4.0 5.0 6.0 7.0 8.0 9.0
Energy (eV)
Figure 1. Distribution of minimal distances of D—D approach during their counter motions on the
boundary of the neighbor tetrahedral sites in lanthanum deuteride vs their initial kinetic energy.
4.5-1
3.5-
o
CD
H 2.54
••R 24
1.5-
0.5-I
0 1 2 3 4 5 6 7 8 9
Energy range (eV)
Figure 2. Energy dependence of D-D reaction rate in lanthanum deuteride according to EODD
simulations for the first series.
4 5
Energy range (eV)
Figure 3. Energy dependence of D-D reaction rate in lanthanum deuteride according to EODD
simulations for the second series.
546
Acknowledgement
References
1. V.A. Kirkinskii and Yu. A. Novikov, Theoretical modeling of cold fusion. Novosibirsk,
Novosibirsk State University, 105 p. (2002).
2. V.A. Kirkinskii and Yu. A. Novikov, Numerical calculations of cold fusion rates in metal
deuterides, in: Condensed Matter Nuclear Science (Xing Z. Li, ed. Proc. ICCF-9), 162
(2003).
3. V.A. Kirkinskii and Yu. A. Novikov, Modelling of dynamic screening effects in solid
states, Europhys. Lett. 67, 362 (2004).
4. V.A. Kirkinskii and Yu. A. Novikov, Calculations of nuclear reactions probabil-
ity in a crystal lattice of titanium deuteride, in Condensed Matter Nuclear Science
(P. Hagelstein and S. Chubb eds. Proc. ICCF-10) (2005).
5. V.A. Kirkinskii, V.A. Drebushchak, and A.I. Khmelnikov, Excess heat release during
deuterium sorption-desorption by finely powdered palladium deuteride, Europhys. Lett.
58, 462 (2002).
6. P. Hagelstein et al. New Physical Effects in Metal Deuterides (http://www.lenr-
canr.org/acrobat/Hagelsteinnewphysica.pdf).
7. J.T. Waber and D.T. Cromer, J. Chem. Phys. 42, 4116-4123.
POSSIBLE C O U P L E D ELECTRON A N D ELECTRON N E U T R I N O
IN N U C L E U S A N D ITS PHYSICAL CATALYSIS EFFECT ON D - D
COLD F U S I O N INTO HELIUM IN Pd
MIKIO FUKUHARA
MR Tohoku University, Sendai, Japan
E-mail: fukuhara@imr.tohoku. ac.jp
1. Introduction
An atomic nucleus is composed of neutrons and protons, but we cannot find elec-
trons and neutrinos in the nucleus at the first glance. However, it has been recog-
nized that these light particles, which are lepton with isospin 1/2, do not contain
originally in nucleus, but generates certainly in nuclear transmutation processes
such as /3 decay and helium formation in sun.
Since a composite model, which the nucleus is composed of proton and electrons,
was knocked out by discovery of neutron, wide credence has been given to a fixed
concept that the electrons cannot exist in nucleus. 1 However, as far as the nucleus
is constituent element of the atom, the distribution of the electron in nucleus is not
perfectly zero without violation of uncertainty principle in spite of its extremely
small volume. On the other hand, generation process for neutrino has not been
entirely resolved. We have another look at the generation process.
Our first interest lies in studying a possibility of coexistence of electrons and neu-
trinos in nucleus from a new angle on particle physics with lower energy. Although
the neutrinos have three families or three flavor eigenstates (ye,v^ and vT) associ-
ated with the three charged leptons: the electron, the muon and the tau, we use the
electron neutrino with the lightest mass in this study. As far as we know, no pre-
vious research has been done on coexistence of electrons and neutrinos in nucleus,
except for nuclear reaction of excited electron and neutrino in solids.2
547
548
The Pd lattice for confinement of deuteron pairs plays the same role as magnetic
field confinement in hot nuclear fusion, because the attractive interaction between
deuterium atom and electron is mediated by massive photon with 5.2 keV.
549
Neutron Proton
opposed to each other due to boson exchange. 10 Since the size of both lepton and
quark is less than 1 0 _ 1 8 m and the nucleus size is around 10~ 15 m, we can assume
that u and d quarks are surrounded by spherically symmetrical ball of electron and
neutrino blurred by a time-exposure of its rapid motion in nucleus, respectively.
Furthermore, although the standard model in particle physics does not specify how
many quark-lepton pairs constitute the family,11 a limit number exists, as far as we
treat natural atomic elements with atomic number up to around 110; three pairs
must assign for one proton-neutron pair. In other words, the three kinds of pairs
must intrinsically assign for one proton-neutron pair, but this problem has been
overlooked in the high-energy particle physics.
of boson mass. In calculation of the strength for photon, we cannot make use of the
latter's relation, because of photon with zero mass. Since Compton wavelength of
the electron is 3.86 x 1 0 - 1 3 m, we can use the wavelength as the interacting zone of
photon. Similarly, Compton wavelength, i.e., the interacting zone, of the W boson
in weak interaction is 2.46 x 10~ 18 m. Thus the zone ratio of the electromagnetic
interaction to the weak one is around 4.04 x 1 0 - 1 1 .
Here, since one electron corresponds to one proton in atom, we can assume that
the electron of atom takes one's share of both electromagnetic and weak interactions
in proportional to the effective zone ratio in normalization of electromagnetic and
weak interactions in regardless of their coupling constants. In other words, the weak
force mediator is lodged with the (u, e~) group for a brief time. From the effective
zone ratio, we can obtain 2.07 x 1 0 - 5 eV as the electron mass associated with the
weak interaction. This value is close to the electron neutrino mass, 10~ 5 —10 -6 eV, 12
extrapolated from masses of muon and tau neutrinos obtained in Super-Kamiokande
collaboration. This indicates that the ratio of the lepton mass is almost equivalent
to the ratio of quark ones, giving to a possible answer for an unexplained problem
of the standard model in particle physics, which the ratio of lepton mass within
the first family is so large compared with the ratio of quark ones. And we can also
reply why only the first family is needed to make up the ordinary protons, neutrons
and electrons in the universe? The electrons and neutrinos coexist with quarks in
"nucleon vessel" of atom which is firmly bound by electromagnetic interaction. On
the other hand, the other two families exist only ephemerally after the electrons are
completely separated from the nucleus by high-energy collisions. Although nuclear
behaviors at low temperature have not aroused researcher's interest, because most
nuclei have enormous energy of the order of a few MeV, we cannot ignore the role of
the electrons for atoms associated with u and d quarks in particle physics. Further
study for this interesting area is called for.
u + e~ <-> d + v, (7)
+
e + v ^> e~ + u, (8)
e~ + v <-• e~ + v. (9)
552
Neutron Proton
U 1
Figure 3. Schematic representation of elementary particle interactions, d + v <-• u + e~, e+S" <->
e~ + v and e~ + v <-» e~ + v, mediated by W and Z° bosons in proton and neutron of deuterium
nucleus, respectively, where u and d are up and down quarks, respectively. The black lines are
W and Z° mediated interaction between proton and neutron. W and Z° mediated interactions
among protons and neutrons are dotted and broad lines, respectively.
where Z and A are atomic and mass numbers, respectively. Equation (10) is
nonequilibrium equation. Since palladium in nature has five isotopes with even
atomic number, i.e., 102 Pd, 104 Pd, 106 Pd, 108 Pd, and 1 1 0 Pd of 0.96, 10.97, 27.3,
26.7, and 11.8%, respectively,14 the corresponding element sets for Eq. (10) are
i 0 6 p d ^ i 0 6 C d ) i 0 8 p d ^ i 0 8 C d ] a n d n o P d ^ i i o C ( 1 F o r s t a r t i n g elements, 106 Pd,
108
Pd, and 1 1 0 Pd are plausible. As far as we know, no previous research has been
done on physical role of electron and neutrino for nuclear reaction, except for nu-
clear reaction of excited electron and neutrino in solids.6 This interesting area needs
for further work.
6. Conclusion
In this study, we investigated a possibility of coexistence of coupled electron and
electron neutrino in nucleus, using electroweak interaction. In nucleus, the weak
interaction is mediated by W ^ boson between u and d quarks in proton and neutron,
respectively or neutron and proton, respectively, while neutrino and antineutrino in
proton and electron and antielectron in neutron are mediated by Z° boson. From
Compton wavelengths of the electron and the W boson, the effective zone ratio of
the electromagnetic interaction to the weak one is around 4.04 x 1 0 ~ u . Provided
that the electron of atom takes one's share of both electromagnetic and weak ones
according as the zone ratio, we obtain 2.07 x 10~ 5 eV as the electron mass for the
weak one, closing to estimated neutrino mass, 1 0 - 5 — 10~ 6 eV. This is a possible
answer why the ratio of lepton mass within the first family is so large compared
with the ratio of quark ones in the standard model. The electron and the neutrino
are coupled as s-wave boson in nucleus.
From view of particle physics by mediation of charged and neutral pion, the
introduction of s-wave coupled electron and neutrino enhances cold fusion. The
addition of neutral pions is equivalent to the double addition of Eq. (9), i.e., t w o e - —
v pairs. The electron and neutrino pair may come from double /3-decay formation
of helium,
(Z,A) -^(Z + 2,A)+2e~ + 2v. (11)
In this nonequilibrium equation, 106 Pd, 108 Pd, and 1 1 0 Pd are plausible in nature.
The sufficient conditions in this interesting area needs further study.
References
1. E. Fermi, Nuclear Physics (The University of Chicago Press, Chicago, 1950), p. 97.
2. M. Fukuhara, Proc. 4th Meeting of Japan Cold Fusion Research Society, Tokyo (2005),
p. 63.
3. M. Fukuhara, Fus. Sci. 34, 151 (1998).
4. D.F. Measday and G.A. Miller, Am. Rev. Nucl. Phys. 29, 121 (1979).
5. M. Fukuhara, Proc. 6th Meeting of Japan Cold Fusion Research Society, Tokyo (2005),
p. 53.
6. M. Fukuhara, Nuovo Cimento C27, 99 (2004).
554
MASANOBU BAN
Tokyo Metropolitan Industrial Technology Research Institute, 3-13-10 Nisigaoka Kitaku,
Tokyo 115-8586, Japan
E-mail: Masanobu-Ban@member.metro.tokyo.jp
We propose that cold fusion (CF) is fluctuation of the resonance, which happens
to the electron wave. When electricity is discharged, a special crystal is made from
free particles by the tunnel phenomenon of the electron wave. If free particles
line up in the arrangement of the crystal, and the particle shifts, the line makes
a wave. When alignment fluctuates, phase transition occurs in crystal. There is
a possibility that the distribution of energy is converted into all the combinations
for the phase transition of the crystal. The phenomenon of CF appears variously
for that.
1. Introduction
It is pointed out that cold fusion (CF) is responsible for the configuration of
deuterium atoms in crystal. The CF is connected to three kinds of resonance
occurring in electron discharge. The CF is a type of electron resonance, which
occurs in the dc circuit. I would like to propose that self-expansion tunnel
resonance of the material wave is the primary cause. In the dc circuit, the charge
causes the alignment of the free particle. 1 - 5 We found a force that the electric
charge assists to form in line for deuterium atoms in crystals.
In this study, we investigate a relation between matter wave resonance occurring
in dc discharge current and CF in view of variation of the resonance. For dc electric
discharge three noises interchange in the same condition 6 (see Figs. 12 and 13 of
Ref. 6).
The noise, which occurs in power spectral density P(f), fluctuate white, 1 / /
square, and 1 / / noises. These noises are exchangeable. We propose that the
phenomenon must be a phase transition of the crystal from the investigation.
Nanocarbons, nanotubes, and Fullerene are produced at a phase transition by
dc discharge circuit. 7 Since phase conversion of crystals awes to dc discharge, we
consider phase conversion for CF. We explain the relation for CF, using change of
resonance matter wave.8
We describe more an outline. Maeda et al. successfully found that the
noise component of 1 / / and 1 / / square was observed at discharge portion in
graphite electrode,6 and took out the noise of the electric discharge portion from
demodulation controlled by the electric discharge distance 6 (see p. 2141). In this
555
556
case, the two kinds of noise occur alternately in the circuit. Maeda's P(f) can
analyze the feature as P ( / ) / i = C or P(f)J2 = C.
Therefore, three kinds of phenomena exist in the electrical discharge part
together with P(f)fo = C of the white noise. In general, it is well known that
the white noise always exists as J. B. Johnson Noise. Indeed, the three kinds of
noises occur continuously and alternately at least. This is responsible for tunneling
in discharge at part of discharge.
Thus the tri-stable of tunneling phenomena occurs alternately. The free electrons
in discharge are emitted from metal surface into the air by tunneling. And the
electron makes standing waves and traveling waves in the electric discharge. 8
In other words, existence of the standing and traveling waves make assist to
form in line for deuterium atoms in crystals, leading to CF. Such phenomena will
occur in plasma dust from direct current glow discharge as plasma crystal. 8
Furthermore, since dust makes line up as some crystal, we propose that phase
change exists in resonance of the de Broglie wave.
A hi>
T7ff
•fAAM*
Figure 1. Tunneling out from Cathode at discharge.
557
square noise of Eq. (1). Therefore, we conclude that 1//square noise is nature of
the quantum resonance.
Then there will be many standing waves of the electron wave by the tunnel
phenomenon in the discharge. If the initial phase is a steady value for each wave
in the period, 1 / / square noise is synthesized from the standing wave that the
amplitude is in inverse proportion to frequency /.
The frequency versus power spectrum density can be written in Fig. 2, and the
envelope curve be shown in both logarithm graph by the straight line proportional
to - 2 .
1
(V sin mtof \ - 1/
•'ham
2,, 1 2
t
3
W
4 5 6 7 n„
lAAMAl-
0
Cathode
5n ion (rad)
Anode side
made in the bottom of a big well between cathode and anode. The existence prob-
ability is set to the electrode side high. When the harmonic component of the
standing wave is synthesized on an easy condition, the line of the particle is found
from the free particle group. 8 When harmonic of the standing wave are synthesized,
the free particle getting together, it lines up. 1 If the electron propagates into the
crystal on any condition, Nakamura's calculation of power spectrum density is al-
ways 1//square. 10 The crystal was self-organized from the tunnel resonance of the
electrical discharge. And the electrode in a carbon-graphitized layer exists in that
Maeda's experiment, 6 ' 9 so the amplification of the resonance is promoted. There-
fore, the layer of the electrode helps the resonance, and the result also makes the
multiple layers in the electrical discharge part. In the row of barrier on potential
well, whenever the quantum propagates, 1//square noise must be made. 10
The difference between 1//noise and white noise is caused from the initial phase
9 if) of Eq. (1). If the freedom of the phase is excluded, then 1//square can be
considered to be a basic character of the electrical discharge circuit. White noise
and 1//square noise have been explained basically.
4. Force of Resonance
Alignment appears at Yham in Fig. 3 and the electron wave build the aligned power.
Also in our paper, 8 the power of the electron wave was settled in simple Eq. (4).
560
5. 1//Noise
The 1//noise will be explained next from principle of 1//square noise. 1//noise is
explained also on the basis of the column of particles, which shows in Fig. 3 of 1 / /
square noise.
This row is same as a crystal. Therefore, the row is harmonic oscillators. If wave
packets propagate into the harmonic oscillator, the output of signal is integrated
because of Virial theorem. The meaning of integration is a low-pass filter if it
is explained as working of the electric circuit. As the result, the square of 1 / /
becomes 1 / / depending upon operation. However, action does not work always
uniformly. There will be such a resonance, and the resonance changes in tri-stable.
The structure of a repetition is increasing resonance. Accordingly resonance of
electron wave by power of l / / m a y be promoted by surface structure of an electrode.
For instance, it can be expected that a graphitized layer structure promote the
resonance more. Promoting resonance, it can expect the type of stratified structure
of graphite. As an example, if perylene is observed with STS, there is negative
resistance. 11 In the experiment there is negative resistance from resonance.
6. Parametric Amplification
The crystal is made as a free particle queues up in the electrical discharge. Then,
the quantum can propagate under the crystal similarly to a semiconductor as Fig. 4.
Then, the soliton u propagates while shaking the lattice. The lattice is made up of
Shrodinger equation and the propagation of u is made up of Soliton equation.
L4> = e^ L= - f|-x
561
It is settled to a nonlinear equation (j^r — [B, L\) <j> = 0 that causes the ampli-
tude modulation wave and the parametric amplification. The lattice of the crystal
consists of the array of the particle. Each particle vibrates. Then, the amplification
arises if the quantum passes many potential barriers by the tunnel phenomenon.
When three waves become complete in the condition for the resonance, the wave is
amplified in the parametric nonlinearly 13 (Fig. 5).
d2x0 , 2
— +01X0 = ~pxix2,
d2£i
- u2x\ = -f3x0x2,
d2X2
- UJ2X2 = ~/3x0x2,
dt2
U)Q = LJ\ + ljj2.
7. Characteristic of Resonance
When it is P(f) oc 1 / / , power spectral density P, is in inversely proportional to
the frequency / in 1 / / noise. If we display in formula, it becomes P(f) = C/f.
The C is constant. By the way, white noise indicates P(f) = C. Also it can
rewrite to P(f)fo = C. Also 1/'fz noise is P(f) oc l / / z , it can be written to
P{f)fz = C. There is always an equation P(f)fm = C that it looks like the
equation P(f)fo — C of the oscillator at Planck's black body radiation. White noise
occurs from law of equipartition of energy. Therefore, the feature of P(f)fm = C
like law of equipartition of energy is every resonance.
8. Conclusion
Free electron is discharged by tunneling at the time of electric discharge to the air
by the cathode. Therefore, free particle and matter wave exist in tunneling.
Also at least three kinds of resonances exist in electron. When it fluctuates
alternately with three interspecific, phase change occurs in "plasma crystal"of the
electron wave.
In electric discharge of a direct current, the feature of a phase transition is found
in many examples. The conduction of heat with a sudden temperature change
occurs to the electrical discharge as an example of the phase transition at the
electrostatic cooling phenomenon. 14 Graphite in electric discharge is changed into
fullerene or nanotube. 7 There is a technology to control single atom when the atom is
transported with the tunnel microscope. 15 Similarly, "the plasma crystal" is made
from the gravitation of the electron wave. We would like to propose that these
features prove phase transition.
When free particles are contained in the material placed between the
electrodes, the material wave is the same condition even if it is not an electrical
discharge. For example, if the tunnel phenomenon has occurred in a solid solution,
a semiconductor, electrolysis liquid, and gas, a phenomenon of same class will
occur. We would like to propose that CF is fluctuation of the resonance, which
happens to the material like a semiconductor.
563
Acknowledgments
I would like to t h a n k and appreciate Dr. Hiroo N u m a t a for his help. I would also
like to t h a n k J C F to make the paper successful.
References
1. http://annex.jsap.or.jp/hokkaido/ yokousyuu39th/B-29.pdf (in Japanese).
2. H.M. Thomas and G.E. Morrill, Nature (London) 379, 806 (1996).
3. F. Melandso, Phys. Plasmas 3, 3890 (1996).
4. S.V. Vladimirov and O. Ishihara, Phys. Plasmas 3, 444 (1996).
5. S.V. Vladimirov, P.V. Shevchenko, and N.F. Cramer, Phys. Plasmas 5, 4 (1998).
6. S. Sugita, Y. Mera, and K. Maeda, Origin of low frequency noise and l//fluctuations of
tunneling current in scanning tunneling microscopes, J. Appl. Phys. 79(8), 4166-4173
(1996).
7. Y. Hayashi, Dusty plasmas and carbon fine particles, J. Plasma Fusion Res. 78(4),
320-324 (2002) (in Japanese).
8. M. Ban, Composition of 1 / / amplitudes electron wave and a work of one dimension
of lattice, Proceedings of the J^th Meeting of Japan CF-Research Society, Morioka,
October 17-18, 2002, p. 90-94.
9. K. Maeda, S. Sugita, H. Kurita, M. Uota, S. Uchida, M. Hinomaru, and Y. Mera,
Spatial variation of 1//current noise in scanning tunneling microscopes, J. Vac. Sci.
Technol. B12(3), 2140-2143 (1994).
10. T. Haga, Y. Takane, and K. Nakamura, I / / 2 law in one-dimensional quantum trans-
port: an example of weak chaos in quantum systems, Chaos Soliton. Fract. 5(7),
1077-1083 (1995).
11. M. Okuda, H. Inaba, H. Naitou, J. Ehara, and T. Takagi, Negative resistance of the
organic membrane with STS, IEICE, Technical Report, OME 93-56 (1994-03) (in
Japanese).
12. K. Ueno, Suurikagaku, Soritonnga Hakobu Mugennno Sekai 387, 42-47 (1995) (in
Japanese).
13. T.Taniuti, K.Nishihara, and Iwanamisyoten, Nonlinear Waves pp.10-11, 88-91, 100-
127, 1998 (in Japanese), Pitman Advanced Publishing Program, Boston, 1983; Trans-
lated from the Japanese edition.
14. K. Kisi and H. Eda, Electrostatic cooling, J. IEIC9/77 60(9), 1044-1046 (1977) (in
Japanese).
15. D.M. Eigler and E.K. Schweizer, Positoning single atoms with a scanning tunneling
microscope, Nature 344(5), 524-526 (1990).
T Y P E S OF N U C L E A R F U S I O N IN SOLIDS
NORIO YABUUCHI
High Scientific Research Laboratory, 204 Marusen Building,
28-16 Marunouchi, Tsu City,
Mie 514-0033, Japan
E-mail: yabu333@lilac.ocn.ne.jp
The author has been fortunate enough to encounter both types of nuclear fusions,
and so hereby presents a theory regarding these two fusion types. The first phe-
nomenon that may be considered is thermonuclear d-d fusion in a vacuum crack
within a solid. When a platinum plate is connected to a positive electrode and
a palladium-alloy plate is connected to a negative electrode in deuterium and a
200-V electrolysis current is passed through them, neutrons, helium 3, and 3.27
MeV of heat are obtained. The fact that such a phenomenon is produced despite
the low voltage suggests the following: first, a vacuum microcrack is produced
within the palladium alloy. Next, a large quantity of Bose-particle deuterium nuclei
flow into the crack as impurities due to the Kondo effect. Accordingly, the effect
of the Heisenberg uncertainty principle (Ax Ap > h) is exerted, the movement-
position range of the deuterium nucleus becomes extremely small ( i - t 0), and the
movement amount gradually increases (p(mv) —> oo). Integrating this movement
amount yields J mv dv = 1/ 2mv2 + C, and when the movement energy of this 1/2
mv2 exceeds 10 keV, thermonuclear fusion occurs. The second phenomenon is that
of the experiment conducted by Iwamura et al. this is elemental transmutation
due to nonthermal nuclear fusion in a solid by deuterium permeation. In this case,
coating the surface of the palladium alloy facing the deuterium gas with cesium
resulted in the creation of praseodymium, and coating the surface with strontium
resulted in the creation of molybdenum. Common points in these phenomena are
the facts that the atomic number increased by 4 and the atomic mass by 8. In this
regard, it appears that the transmutation was the result of nuclear fusion of the
cesium or strontium with two compound nuclei of deuterium.
564
565
atmosphere; the wind energy of a hurricane caused by the inrush of air into low-
pressure areas due to a temperature differential of only 20° C can be tremendous
amount, equivalent to 300,000 thermonuclear bombs. The energy of the deuterons
that are excited in a vacuum crack can be determined by this equation:
Next,
Also,
lgNi[C, D][T] [C, D] = (4n + 4p, lOn + 10p)(4n)(4n + 4p, lOn + lOp)
This has a [T] sphere interposed between and interlinked with two [C,D] spheres.
Next,
1
£gS[T ) C,0,I,D][T 1 C ) 0][T,C ) 0 ) I ) D]
Next,
208
82 Pb[T, C, O, I, D] [C] [I, D] [C, D] [I, D] [C] [T, C, O, I, D]
P n 23n+23p
23n+23p 23n+23p
238
92 U[C, O, I, D] [T] [C, O, I, D] [C, O, I, D] [C, O, I, D] [T] [C, O, I, D]
96 T 140 + 2. (9)
238
Fission of U atom at an atomic weight of 96:140 is shown by the arrow in
Eq. (7). It is believed that two nucleons are split by collision with an incident
neutron. This explains why fission of uranium occurs at an atomic-weight ratio of
96:140 (see Fig. 1).
and bonded in blocks that have crystallized into Platonic structures. Because these
bonds are between liquid crystals, the attraction between the respective blocks is
weakened by the large distance between the blocks. Here, blocks are indicated by
square brackets ("[.]"), and the bond between two blocks by a dash ("-"). Because
the distance between two bonded blocks is large, the proton reaction can be termed
small.
At JCF4, the author described how the spherical surface of the shell is externally
and internally tangent with the Platonic Yabuuchi structure, yielding the nuclear
chemical formula for 1 | | C s shown in Fig. 2. The items have been labeled to aid
understanding.
-7 9
*
• '<•'',' * ^ , K1 •
;it ft, rn 11 • • (I
t >
" •'-''/' : »
•.s I ^ - 1 _•
•
"-'#"2»'-
# : Proton
(a) (b) (c) (d) (e) o : Neutron
The third term from the left hand side of Eq. (8) represents the outermost shell,
which in terms of Platonic structures is an icosahedron, indicated here as an
I-polyhedron. As shown here, its configuration has been stripped of seven crystalline
nucleons (here neutrons).
The state in which the two 2D units in Eq. (8) react is indicated by Eq. (9).
^ 2 ( n + p) + 2(n + p) + 1 ^ C s , (11)
Platonic structures. Further, under the solar-system model of the atomic nucleus,
the reaction between (b) and (d) seen here cannot be produced by proton reaction.
= (25n + 25p)(4n + 4p)(23n)(2n + 2p + 3n + 3p)(25n + 25p), (13)
141 P r [ T , C , 0 , I , D ] - [ C M T , C , 0 , I - 7 ] - [ T , O M T , C , 0 , I , D ] . (14)
59
Equation (11) indicates the change in the numbers of protons and neutrons that
occur due to nuclear reaction in the blocks within the atomic nucleus.
In the atomic nucleus that has undergone nuclear change to become ^gPr, in-
dicated by Eq. (12), in the second block, (2n+2p) has become (4n+4p), indicating
that the T-polyhedron (tetrahedron) has reacted to the C-polyhedron (cube) and
changed.
Similarly, in the fourth block, (2n+2n) has become (2n+2p+3n+3p), indicating
that the O-polyhedron (octahedron) has changed to a T-polyhedral structure in the
inner shell and an O-polyhedral structure in the outer shell. This is as shown in
Fig. 3.
•
m : Proton
:;; : Neutron
Because item (b) in Eq. (14) is composed entirely of neutrons and does not
attract protons, the 2D does not react. Accordingly, items (a) and (c) are each
lacking six neutrons and protons, for a total of 12, and the 2D reacts ate locations.
The riddle of nuclear fusion is thus explained. The bonds described are not
formed in a chaotic integral atomic nucleus. Fusion can take place in an atomic
nucleus having crystalline blocks with weak bonds.
570
References
1. Y. Iwamura, Detection of anomalous elements, X-ray, and excess heat in D2-Pd system
and its interpretation by the electron-induced unclear reaction model, Fusion Technol.
33(4), 387-500 (1998).
2. V.F. Weisskopf and E.P. Rosenbaum, A model of the nucleus, Sci. Am. 193(6), 4-91
(1955).
3. M. Brack, Metal clusters and magic numbers, Sci. Am. (1997).
4. W. Green, Cold Fusion 12, 28, 29, 31 (1995).
5. C. Illert, Cold Fusion 13, 28-29 (1995).
6. N. Yabuuchi, Low-speed nuclear fusion, Cold Fusion 17, 11, 16-19 (1996).
7. S.M. Austin and G.F. Bertsch, Halo Nuclei. Sci. Am. (1995).
8. N. Yabuuchi, Proceedings of the Fourth International Conference on Cold Fusion, Vol. 4;
Theory and Special Topics Papers. TR-104188-V4 Proceedings, Lahaina, Maui, Hawaii
(July 1994, December 6-9, 1993).
NEUTRINO-DINEUTRON REACTIONS
(LOW-ENERGY N U C L E A R R E A C T I O N S I N D U C E D B Y D 2 GAS
PERMEATION THROUGH PD
COMPLEXES — Y. I W A M U R A EFFECT)
V. M U R O M T S E V A N D V. P L A T O N O V
State Scientific Centre of Russian Federation Karpov Institute of Physical Chemistry, 10,
Vorontsovo Pole Street, 103064- Moscow, Russia
I. SAVVATIMOVA
Federal State Unitarian Enterprise Scientific Research Institute "Luch",
142100, Podolsk, Zhelesnodorozhnaya Street, 24, Moscow region, Russia
E-mail: ul0492@dialup.podolsk.ru
1. Introduction
Recently some experimental evidences confirming the assumed existence of the relic
neutrino and the anomalous neutrino magnetic moment have been obtained. The
said assumption is based on the concept of occurrence of stable dineutrons; the
function of neutrino and dineutrons in phenomena studied by physical chemistry
and low-energy physics. The existence of bound states of neutrino (latent) with
protons, deuterons, and other nuclei follows from the well-known estimations of
anomalous neutrino magnetic moment 1 and the Dirac's equation. 2 ' 3 The concept
of relic neutrino leads to the possibility of the neutrino component of the matter.
If we assume the existence of the neutrino component of the matter, the question
arises as to whether these neutrinos are capable of initiating nuclear transmutations.
Nuclear experimentation evidence shows that small quantities of nuclei occur in
excited meta-stable nuclear states. Capture of neutrino by the said nuclei may
trigger transition from the excited meta-stable states to the basic one and lead to
the output of energy sufficient to initiate nuclear transmutations.
571
572
The above concept provides grounds to study the problems of neutrino and the
dineutrons function in a number of processes, discovered in experiments in allied
areas of physical chemistry and nuclear physics. One of the approaches to the study
of neutrino physics may be focused on investigation of reactions of the following
type.
ue + fX - £- 2 X + 2n +i e , (1)
where 2 n represents dineutrons.
N N 4
ve + zX -^ zZp. + 2Be + 2n + i e , (2)
N
ve + zX - £r 6 14 X + l2C + 2 n + ie, (3)
The study of the assumed existence of reactions (l)-(6) may be regarded as one
of the goals of the present investigation. It is suggested that these reactions are
accounted for by the electromagnetic low-energy neutrino interaction.
According to the assumed hypothesis a number of protons p + and deuterons
D + occur in plasma in bound states (latent) of protons and deuterons with neutrino
(p+i^e and D+^ e , respectively). As a result of a collision, for example, of deuteron
with neutrino in a latent state with the Pd cathode surface, part of the neutrino
may be captured by Pd isotopes.
D+i/e + P d ^ D + + P d ^ e . (7)
The bound state of some isotopes with neutrino decays in some cases in
accordance with reactions (l)-(3).
573
v, + ^ P d - IgZr +l2C + 2
n+ie, (8)
Among stable Pd isotopes, only 1 0 5 Pd has other than zero magnetic moment. 1 0 7 Pd
isotopes were discovered in the Pd cathode. This effect can be accounted for by the
dineutron capture by 105 Pd (4).
2
n+105Pd-^ 107
*Pd + 7 . (10)
Figure 1 in Ref. 7 shows activity decrease curves in silver foils after the exposure
in the vicinity of the Pu-Be neutron 105 C _1 -active source and after the exposure
of Pd to D in the GD chamber (at the same distance). Both curves correlate with
the silver 110 half decay period. The effect of the neutrons flow upon the silver foil
may lead to 110 Ag isotope formation.
109 110m
n + Ag -• Ag + 7. (11)
C 23.68
Pd 76.32
2x104
B
Ba
4
1.5 x 1 0
1 x104
5000
JKJ^JU,
133 {134 1|35 1)36 1^37 [138 139
1500
1000
500
Figure 1. (a) The secondary ion mass spectrometry (SIMS) spectrum of natural Ba. (b) SIMS
spectrum of Pd complex with natural Ba after D2 permeation.
The second mass spectrum was obtained after D diffusion through the Pd
complex, containing Ba and Sm. A dramatic change in the intensity of the mass
peaks was observed after D diffusion. The data in Fig. 1 was obtained with natural
abundance barium isotopes. After barium had been implanted into the Pd com-
plex 146, 148, and 150 mass peaks appeared in the mass spectrum. This may be
explained by the assumption that the electrochemical process of Ba implantation
triggers reaction (3) and fusion reaction (5) and the following reactions take place
134 12/-.
56 Ba
D a + 6 ^ - 6fSm + 7, (15)
136
56 Ra
o a + 12ri
6 ^ - IfSm + 7, (16)
138 12/-.
56 Ra
u a + 6 ^ - y 8°Sm + 7- (17)
No 147 and 149 mass peaks are observed on the spectrum in Fig. 1. This suggests
that the cross-section of 12 C capture by odd 137 Ba isotopes is less than by even
Ba isotopes (Ba mass spectrum, enriched with 1 3 7 Ba). 137 Ba content is about 60
times bigger than that of 138 Ba. As a result of D diffusion through the Pd complex
(enriched with 137 Ba) 149 mass peak shows the maximal intensity. It suggests that
the nuclear reaction of the below type is going on:
137
56 Ba + iC IfSm (18)
576
5. Conclusion
T h e most controversial are the following problems: the existence of the neutrino
component of the matter, the ability of low-energy neutrino to initiate nuclear
transmutations, and the existence of stable dineutrons. Many researchers made
a t t e m p t s to find stable dineutrons, but they failed. 15 T h e experiments aimed at
discovery of stable dineutrons were based on o u t d a t e d estimation of bound energy
between two neutrons in a dineutron. According to these estimations the bound
energy between two neutrons in a dineutron was assumed equal to about 3 MeV. 1 5
New evidence shows t h a t the bound energy between two neutrons in a dineutron
amounts t o a b o u t 22 MeV. T h e system of q u a n t a states in a dineutron was studied in
Ref. 16. T h e first and the second q u a n t u m states with energies of 3.6 and 11.6 MeV,
respectively, were discovered.
References
1. A. Suzuki, M. Mori, K. Numata, and Y. Oyama, Phys. Rev. D 4 3 (10), 3557 (1991).
2. I.M. Ternov, V.G. Bagrov, and P.V. Bozrikov, News of higher educational institutions,
Physics 11, 38 (1971).
3. A.O. Barut and J. Kraus, J. Math. Phys. 17(4), 506 (1976).
4. V.I. Muromtsev, P.A. Muromtsev, and V.A. Chelishev, Gravitation and Cosmology,
(Supplement) 8, 227 (2002) Moscow.
5. V.I. Muromtsev and V.A. Chelishev, Russian Fed. Patent #2145095 (2000).
6. K.N. Mukhin and O.O. Patarakin, Successes of Phys. Sci. 170(8), 855 (2000).
7. A.V. Karabut, Ya.R. Kucherov, and LB. Savvatimova, Fus.Tech. 20, 924 (1991).
8. LB. Savvatimova and A.B. Karabut, Surface, Vol.1, Moscow: RAN (1996). pp. 63-75.
9. M. Sakisaka and M. Tomita, J.Phys. Soc. Japan 16, 2597-2598 (1961).
10. G.H. Miley and J.A. Patterson, Infinite Energy 2(9), 932 (1996).
11. Dan Chicea, ICCF9, China (2002), p. 53.
12. Y. Iwamura, T. Itoh, and M. Sakano, ICCF8 (2000), p.141.
13. Y. Iwamura, M. Sakano, and T. Itoh, Jpn J. Appl. Phys. 4 1 , 4642-4648 (2002).
14. Y. Iwamura, T. Itoh, M. Sakano et al., ICCF11, Marseilles, France (2004).
15. JU.A. Alexandrov. Fundamental properties of a neutron, I., Atomizdat, 1976.
16. D.V. Alexandrov, E.JU. Nikolsky, B.G. Novatsky et al, Letters in J. Tech. Phys. 67
(11), 860-865 (1998).
A N E X P L A N A T I O N OF E A R T H Q U A K E S B Y T H E BLACKLIGHT
PROCESS A N D H Y D R O G E N FUSION
HIROSHI YAMAMOTO
3110-17 Tsuzuki, Mikkabi-Cho, Harnamatsu-City, Shizuoka-Pref. 431-1402, Japan
E-mail: hughy@aqua.ocn.ne.jp
1. Introduction
The mechanism of earthquakes is currently explained by the plate-tectonics theory,
which claims the earth's surface is covered with a series of crustal plates that can
store elastic energy caused by relative movement of each plate. But recent obser-
vations of slow slips of crustal plates by Global Positioning System (GPS) dismiss
this idea and more plausible explanation is requested. It seems there are two ways
to generate excess energy from hydrogen and its isotope. One is fusion and the
other is to drop the electron in hydrogen atom from the ground state to the lower
one. The latter one is quite controversial to the current quantum physics and very
few scientists in cold fusion research paid attention to it, but it was shown that it
can explain anomalous combustion phenomena such as very powerful explosions of
hydrogen and oxygen mixture dissociated from water due to nuclear irradiation at
nuclear power plants. 1 If one cannot find the cause of earthquakes, then, the next
step is to study how human activities induced earthquakes and then to deduce a
possible mechanism of earthquakes from the correlations between what was done
and what happened.
577
578
that, an unusual series of earthquakes erupted in the area where earthquakes are
very seldom.
Water injection had been discontinued and the number of quakes decreased
dramatically. When the injection was resumed, quakes increased accordingly and
the link between the water injection and earthquakes was established. 2 The most
notable experience in this series of earthquakes is that many people heard extremely
loud, explosive-like earth noises.
Movement anticipated
by plate-tectonics
Figure 1. Location of a seismometer and direction of the movement at the first shock
(Source: Japan Meteorological Agency home page, http://www.seisvol.kishou.go.jp/eq/kyoshin/
jismn/041023jiiigata/1756/nigata_main.htm).
579
3Fe + 4H 2 0 - • 8H + Fe 3 0 4 (1)
The author postulated that 3-body reaction of atomic hydrogen and oxygen can
make the BlackLight Process, because ionization energy of hydrogen and oxygen is
very close as is shown below.
Hydrogen; 13.598 eV, Oxygen; 13.618 eV.
If the hydrino model holds, it can be expected that the following reactions can
take place:
0 + 0 + H ^ H [ n = l/2]+20++2e", (a)
H + H + O ^ H [ n = l/2] + H+ + 0 + + 2e-, (b)
H + H + H ^ H [ n = l/2]+2H++2e~. (c)
H[n = 1/2] designates a hydrogen whose electron orbit is shrunken to 1/2 the
radius of a normal one and these will be shrunken further to lower orbits as reaction
continues. Ions and electrons thus produced will recombine, resulting in generation
of energy.
It is reported that the BlackLight Process can produce up to 200W/cm 3 at
700mTorr. 4 If the BlackLight Process takes places at atmospheric pressure, the
power density is about 300 kW/cm 3 , powerful enough to cause an explosion.
8. C a n d i d a t e for t h e P r o o f of t h e P o s t u l a t i o n
9. Summary
In the past, it could have been hardly imagined atomic hydrogen gas can explode by
itself but the BlackLight Process by Mills opened the way to investigate the cause
of anomalous explosion of hydrogen from a new standpoint of view. Considering the
very powerful explosion caused by atomic hydrogen and oxygen during cold fusion
experiments a n d at nuclear power plants t h a t can not be explained by current com-
bustion theory but can be explained by the BlackLight Process and the relationship
between water injection into deep wells and occurrences of earthquakes, it can be
reasonably concluded t h a t earthquakes are caused by the explosion of atomic hydro-
gen gas dissociated from water t h a t is brought deep into the earth by subduction
of crustal plates. Furthermore, t h e eruption of helium gas after t h e earthquakes
strongly suggests t h a t earthquakes are caused by hydrogen fusion.
References
1. H. Yamamoto, Revisiting Anomalous Explosion of Hydrogen and Oxygen Mixture from
a View of Cold Fusion, Proc. 5th Meeting Jpn. CF Res. Soc, pp. 89-92 (2003).
2. N. Craig and R.L. Wesson, Earthquake Hazard Associated with Deep Well Injection-A
Report to the U.S. Environmental Protection Agency: U.S. Geological Survey Bulletin
1951, 74 p.
3. R.L. Mills, P. Ray, B. Dhandapani, R.M. Mayo, and J. He, Comparison of excessive
Balmer Alpha line broadening of glow discharge and microwave hydrogen plasmas with
certain catalysts. J. Appl. Phys. 92(12), 7008-7022 (2002).
4. http://www.blacklightpower.com/pdf/ItalyTech%20Paper%203.27.03.pdf
5. H. Wakita et al., Helium spots: caused by Diapiric Magma from the upper mantle,
Science 200, 430-432 (1978).
THEORETICAL MODELING OF ELECTRON FLOW ACTION
O N P R O B A B I L I T Y OF N U C L E A R F U S I O N OF D E U T E R O N S
A. I. GONCHAROV*
Department of Physics and Technology, Altai State University, Prospect Lenina,
61 Barnaul 656099, Russia
E-mail: gonch@theory.asu.ru
V. A. KIRKINSKII
Institute of Mineralogy and Petrography, Siberian Branch of the Russian Academy of
Sciences, Prospect Akad. Koptyuga, 3, Novosibirsk 630090, Russia
E-mail: kirkinsk@uiggm.nsc.ru
582
583
f(r\l)dr = 1.
o
The number I of the D* "atom" collisions with free electrons obeys Poisson
distribution Pa(l) with the parameter a; the average number of collisions a is pro-
portional to the electron flow density and time.
The main contribution to the reaction rate is made by small D* ( r ~ 1 0 - 1 1 cm)
characterized by high mobility. Therefore, the crystal lattice does not significantly
preclude D*-D*-collisions. Let us designate the concentration and the total number
of deuterons in the active volume of the crystal by n and N, respectively. The
proportion of deuterons A, which reacted in a unite time (relative reaction rate) is:
1 i AT 'max 'max
A(a) = =
"iV"dT £ £ PaQ)Pa(m)X(l,m),
1=0 m=Q
OO OO OO
where v is the relative velocity of the deuterons, E = /iv2/2; ^ stands for the
reduced mass of a deuteron pair; Fu{E) denotes the Maxwell distribution at room
temperature normalized as:
OO
jFu(E)dE=l.
o
The cross-section of D*-D*-collisions resulting in a fusion reaction in the
quasiclassical approximation is equal to a(v) = SQP(E)/E, where So = 0.55 x
19 2
lCr cm eV;
R
P{E) = exp I - y /" y/2fj,[V{r) - E]dr
o
r-l,
where R = V (E) is the turning point of a classical trajectory.
It will be assumed that D* "atoms" with the shell sizes r\, r2 move freely if the
"shells" do not overlap, i.e., if the distance between the D* "atoms" is r > r\ + r2.
If the "shells" overlap, a purely Coulomb repulsion of the D* "atoms" is observed.
The potential deuterons interaction energy in this approximation is equal to
v ^ \e2/r-Es ifr<rx+r2,
V{r) = <
[0 if r > ri + r 2 ,
2 2
where Es = e /(r\ + r2) = mec re/(ri + r2) is the screening energy, r e = 2.82 x
10~ 13 cm is the classical radius of an electron. By integration, we obtain
Since at any energy E contributing to A there holds a condition E <C Ea, the
approximation P(E) « P(0),FM(E) = 5(E - E) can be used where E = SkT/2.
Then
\{l,m) =C d n / dr2/(ri|Z)/(r2|m)W(ri+r-2),
o o
where C = (nS0/2)(2/fiE)1/2, W{n+r2) = exp (-1.39y/(n + r 2 ) / r e ) .
Taking into account the probabilistic sense of f{r\l), the reaction rates
A(7, m), A(a) could be approximately calculated by the formulas
N(l) N(m)
» » ) ^ E E »>."»+ r<»>),
A(fl) = c
^^)%o/(ri+rj)'
where r ^ , i = 1, 2, 3 , . . . , N{1) are random implementations of the D* "atom" size
with I collisions of electrons; 7-j, i — 1, 2, 3 , . . . , N* denotes the complete set of
implementations.
Let every octahedral site contain a deuterium atom. Then the deuterium con-
centration n = 6.8 x 1022 cm" 3 ; at T = 350 K, C factor = 1.2 x 10 10 s" 1 .
The calculation results are given below. Table 1 presents the sizes of 10 D*
"atoms", for which r < 2 x lO^ 1 1 cm. It follows from Table 1 that the "orbits" are
usually rather prolate: r m ; n >C r, therefore making use of the r value as the size
of the "atom" will result in the lower-bound estimate of A. By way of illustration,
Table 2 present the number of events with the size r and the number of collisions
I from the different ranges; AN* is the total number of events with I from these
ranges.
I 88 83 84 82 25 89 79 56 98 51
r 0.87 1.17 1.27 1.38 1.64 1.69 1.78 1.81 1.82 1.99
^min 0.22 0.41 0.19 0.88 0.12 0.11 0.08 0.19 0.88 0.38
Figure 1 shows the functions X(l,l) and A(a). Averaging A (a) over a < Zmax,
equivalent to the time averaging yields A f» 2 x 1 0 _ 4 s ^ 1 , which is 106 times greater
than the value obtained in Refs. 1 and 2 on the basis of the dynamic model of
electron orbital deformation (EODD). Taking into account that A(a) somewhat
increases with the increase in a, the obtained average A should be treated as a
lower-bound estimate. The contribution of 370 events presented in Table 2 to the
586
1-20 177731 0 0 0 0 2 4 7 2 0
21-40 114983 0 0 1 5 4 14 19 25 43
41-60 66531 0 0 2 10 9 16 23 25 36
61-80 39042 0 0 1 3 7 13 17 10 22
81-100 22461 1 3 2 2 2 3 8 11 18
1E+0
i
1E-1
1E-2 r /'
,A
-/
1E-3
-
^P ¥ J ! «
1E-4
1E-5 I 1 \'=:
'• HP
1E-6
1E-7
1E-8
_
xr'
1E-9
'
r /
1E-10
h
0 20 40
i
60
i i
80 100
/, a
Figure 1. Reaction rate. Dashed line denotes X(l,l)\ solid line designates A(a).
587
References
1. V. A. Kirkinskii and Yu.A. Novikov. Theoretical Modelling of Cold Fusion (Novosibirsk
State University, Novosibirsk, 2002), p. 105.
2. V. A. Kirkinskii and Yu.A. Novikov, Europhys Lett 67, 362 (2004).
3. R. H. Fowler and E. A. Guggenheim Statistical Thermodynamics (Cambridge University
Press, Cambridge, 1939).
This page is intentionally left blank
Author Index
A F
Adamenko, S. V., 356 Falcioni, F., 377
Almaviva, S., 351 Fauvarque, J.-F., 80
Amini, F., 163 Fiore, R., 145
Andreassi, V., 377 Fisher, J. C , 516
Aoki, Y., 253 Fontana, F., 377
Apicella, M., 117, 264 Frisone, F., 494
Arata, Y., 44 Fujii, M., 133
Fukuhara, M., 547
Furuyama, Y., 272
B
Ban, M., 411, 555 G
Bertolotti, M., 55 Gamberale, L., 377
Garbelli, D., 377
c Gareev, F. A., 504
Cai, N. N., 482 Gavritenkov, D. V., 231
Cao, D. X., 482 Giacinti, O., 377
Capobianco, L., 117, 145 Goncharov, A. I., 582
Castagna, E., 55, 117, 145, 156,
264, 351 H
Castano, C. H., 367 Hagelstein, P. L., 441, 527
Celani, F., 289, 377, 404 Haque, M., 314
Celia, E., 377 Higashizawa, M., 196
Chaudhary, I., 527 Hubler, G., 264
Chubb, S. R., 430
Chubb, T. A., 473 I
Clauzon, P. P., 80 Iizumi, K., 133
Ishikawa, T., 178
D Itagaki, M., 188, 196
Itoh, T., 178
D'Agostaro, G., 377
Iwai, H., 272
D'Aulerio, L., 117, 145
Iwamura, K., 178, 289
Dardik, I., 55
Dash, J., 86, 140
Del Prete, P. R., 145
K
Desyatov, A. V., 97 Kamiya, N., 133
Di Stefano, V., 377, 404 Karabut, A. B., 214, 344
589
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