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i
ii
Contents
1 Introduction 1
iii
CONTENTS
Aknowledgments 117
iv
CONTENTS
vi
Chapter 1
Introduction
The aim of this project is the design of a Prompt Gamma Neutron Activa-
tion Analysis (PGNAA) facility at the Triga Mark II Research Reactor of the
university of Pavia, in Italy. This measurement technique will be used by the
BNCT research group in order to evaluate 10 B concentrations in biological
samples.
Boron Neutron Capture Therapy (BNCT) is a binary experimental radio-
therapy exploiting the combined action of the somministration of 10 B and a
low energy neutron irradiation to cause a lethal damage to the tumoral cells
[1].
Owing to the capture of a thermal neutron in 10 B, an α particle and a 7 Li
nucleus are produced. Since their range is comparable to the cellular diameter,
the release of this high LET radiation causes a localized damage in the tissue.
The efficacy of BNCT depends on 10 B concentration ratio between the tumor
and healthy tissue: if this ratio is high enough, the tumor cells are killed with
a substantial sparing of the normal ones. For this reason, the knowledge of the
boron concentration both in tumor and in normal tissue is a crucial issue for
preclinical studies and clinical BNCT application.
1
1. Introduction
cisely evaluate the boron concentration values in the tumour and in the normal
tissues.
To perform α spectroscopy, a thin tissue slice (60 µm) cut from a cryogenic
sample is kept under vacuum and irradiated in the thermal column of the
TRIGA Mark II reactor. The samples are irradiated in front of a thin silicon
detector that collects the charged particles coming from neutron capture in
10
B and 14 N . A contiguous section of the sample is cut to perform standard
histological analysis. Then, the information resulting from the acquired charge
particles spectra are combined with spatial information from the histological
analysis to get the boron concentration in the different tissues types present in
the sample. With this method a sensitivity of 0.5 ppm of 10 B can be achieved.
The need to keep the sample under vacuum during the irradiation, makes the
analysis of biological liquid samples (such as blood and urine) impossible with
this technique.
Many other different techniques are also employed for boron measurement
in BNCT research, they are all described in [4]. These can be divided into
microscopic and macroscopic techniques, according to their spatial resolution.
The macroscopic analysis can provide an average boron concentration both in
tissue and in blood, whereas a microscopic analysis allows an evaluation of
boron distribution at cellular and subcellular level. The information obtain-
able by microscopic techniques are, of course, very important but, since they
are more expensive, they represent a further step to the macroscopic analysis.
Among the macroscopic techniques, Atomic Emission Spectroscopy (AES-
ICP), Inductive Couple Plasma-Mass Spectroscopy (ICP-MS), PGNAA and
α spectroscopy can be distinguished, while Secondary Ion Mass Spectroscopy
(SIMS), laser-Secondary Neutral Mass Spectroscopy (laser-SNMS) and High
Resolution Quantitative Autoradiograpy (HRQAR), can be mentioned for mi-
croscopic analysis.
The ICP-MS has an high sensitivity for 10 B and 11 B, it represents an efficent
method to evaluate the mean total B concentration and mean isotopic ratio in
biological matrix. On the other hand it is a destructive technique.
SIMS and laser-SNMS are both imaging boron techinques able to give the dis-
tribution map of the different element on the surface (2D image); the spatial
resolution achievable with SIMS is in the nanometer-scale. While the laser-
post ionization SNMS has an higher sensitivity allowing a subcellular distri-
bution image of 10 B and detection limits in upper-ppb range.
A very accurate radio-analytical techinque is represented by HRQAR. Boron
imaging at microscopic level and boron quantification can be performed at the
same time; this is possible by overlapping a neutron autoradiograph, i.e maps
of boron tracks, with a histological analysis, identifing the biological structures,
at the same tissue slice.
Other techinques, already well established in clinical practice and byologi-
cal studies such as Nuclear Magnetic Resonance (NMR) and Magnetice Res-
onance Imaging (MRI), Positron Emssion Tomography (PET), are also em-
2
ployed for BNCT studies. These are candidate to be applied for the real-time
10
B-enriched compound monitor, allowing the knowledge of the 10 B maps dur-
ing the treatment, leading to a more effective BNCT dose delivering.
PGNAA is based on the detection of gamma rays coming from the neu-
tron capture reaction taking place when a thermal neutron is captured in an
element. The high neutron capture cross section of 10 B (3837 b) makes boron
one of the most sensitive elements for this technique.
PGNAA has been used for boron concentration measurements for BNCT stud-
ies since many years. As an example, the PGNAA facility at the High Flux
Reactor in Petten allows accurate and non-destructive measurements of 10 B
concentrations down to 1 ppm in about 5 min for macroscopic samples (0.4 -
1.0 ml) of tissue, blood and urine [6]. In Petten prompt gamma analysis was
used to measure the 10 B concentration in blood after the administration of
sodium borocaptate, in order to to optimize the BNCT irradiation schedule
for the treatment of patients [5].
At the MIT Research Reactor a diffracted neutron beam PGNAA facility was
manly used for BNCT studies. It provided a thermal neutron flux at the sam-
ple position of 1.7 × 107 n/(cm2 s), with a sensitivity for natural boron in water
of 3750 cps/mg [18].
In Japan, maeasurements of 10 B concentration in blood, cerebrospinal fluid
(CSF) and brain tissue were performed from Mukay, Nakagawa [7]. At the
Musashi Institute of Technology evaluation of 10 B was performed in tumours,
tissue,blood and cultured cells [8]. Other institutions involved in BNCT projects
with PGNAA facilities are: the HANARO reasearch reactor in Korea Atomic
Energy Research Institute [9], the light water research reactor facility in Rez,
Czech Republic [10] and at the research reactor FRMII in Garching near Mu-
nich [11].
The implementation of a PGNAA facility at Univeristy of Pavia not only
allows improving the measurement of 10 B capability of the BNCT research
group, making possible the analysis of biological liquid samples, but it repre-
sents an important tool for a rapid evaluation of 10 B concentration during a
BNCT treatment.
A prompt gamma spectroscopy for BNCT purposes requires the evaluation of
a concentration of the order of µg/g of 10 B in tissue or blood sample with
measuring times of minutes. The mass of the sample could be of the order
of 0.05 g, such as healthy or tumoral biopsies with concentration of tenth of
ppms, or even smaller samples, of the order of 10 µl as in case of blood with-
drawal from small animal (100 ng of 10 B)). These BNCT requirements give
important constraint about some structural parameters of the facility, such as
the thermal neutron flux and the count rate background in the boron region,
being these directly related to the 10B detection capability of the measure-
ment method. In particular a minimum amount of detectable 10 B mass (DL )
of the order of hundreds of nanograms in times of minutes requires the use of
3
1. Introduction
4
1. Introduction
6
Chapter 2
The Prompt Gamma Neutron
Activation Analisys
7
2. The Prompt Gamma Neutron Activation Analisys
8
2.1. Characteristics of PGNAA
Another important quantity in PGNAA is the partial cross section gamma ray
producion:
σγ = θσPγ (2.2)
where θ and Pγ are respectively the natural isotopic abundance of the given
nuclide and the emission probability of this gamma ray.
This quantity is used to determine (ργ ), that is the count rate (s−1 ) of a
gamma peak at a given energy of the spectrum. In the simplified case of a
monocromatic beam and an ideally thin and homogeneus sample, ργ takes the
form:
ργ = ε(Eγ )nσγ Φ (2.3)
ργ is the area of the peak divided by the measuring time (live time), while n is
the number of atoms, ε(Eγ ) is the counting efficency under the photoelectric
peak of the detector and Φ is the neutron flux.
This expression becomes more complicated when a real case is considered,
where, for instance, the neutron spectrum is not monoenergetic and the thick-
ness of the sample can introduce either gamma ray attenuation or neutron self
shielding. The formula including these effect is:
� � ∞
µ(r)
ργ = NA σγ (En )Φ� (En , r)ε(Eγ , r)dEn dr (2.4)
V 0 M
where µ(r) is the mass density as a function of the position in the sample, M
is the atomic mass of the element, NA is the Avogadro number, σγ (En ) is the
partial gamma ray production cross section as a function of the neutron energy.
The neutron flux Φ� and the efficency ε� are also expressed as a function of the
position inside the sample (r) and, respectively, of the energy of the neutron
beam (En ) and of the given gamma energy (Eγ ).
In practice, some tricks can be adopted to reduce these effects, for example, a
relatively large sample-to-detector distance avoids that the counting efficency
depends on differences in samples shape. Moreover, if the sample is relatively
9
2. The Prompt Gamma Neutron Activation Analisys
thin and small, the self absorption can be neglected; otherwise in case of bulk
samples a correction factor accounting for the self absorption can be applied.
Similarly a simple equation taking in to account the self shielding effect must
be used.
In case of thin sample approximation the expression 2.4 can be simpli-
fied: the efficency and the flux values do not depend on the position inside the
sample, thus the count rate can be expressed as:
� ∞
ργ = σγ (En )Φ(En )dEn dr = σγ0 Φ0 (2.5)
0
where σγ0 is the partial gamma ray production cross section for monocro-
matic neutrons with v = 2200ms−1 , and Φ0 is the thermal equivalent neutron
flux defined as:
√
π v0
Φ0 = ΦT (2.6)
2 vT
using Φ0 , the reaction rate and the count rate become respectively:
m
R0 = nσ0 Φ0 ργ0 =
NA σγ0 Φ0 ε(Eγ ) (2.7)
M
Thus, the count rate depends only on the mass of the sample and parame-
ters like shape or position do not appear in its formula.
10
2.1. Characteristics of PGNAA
It depends on the partial gamma ray production cross section σγ,0 , the neutron
flux Φ0 and the counting efficency at the measured energy ε(E).
From the practical point of view, the sensitivity ((counts/s)/mg) for an element
is the net count rate under the measured peak, divided by the mass (m) of
that specific element in the sample:
NG − NB
S= (2.9)
tm
where NG and NB are respectively total and background counts under the peak
and t is the count time.
The detection limit (LD ) for an analyte represents the minimum detectable
amount of the element under study.
The espression for LD is derived from the theory of the ”hypotesis testing”
and from the definition of two fixed limit: α, indicating the probability of
false positive and β, that is the probability of a false negative. Their default
values are 0.05 [32]. The LD is associated to true value of the quantity of
interest. The assertion of a true value can be done comparing the outcome of
the measurement (L̂) with a critical value LC ; if L̂ > LC the decision ”detected”
can be assessed.
These quantities, LC and LD can be defined as multiple of a standard deviation
of the blank σ0 and of the sample σD respectively, according to the following:
LC = kα σ 0 (2.10)
LD = LC + kβ σD (2.11)
(2.12)
11
2. The Prompt Gamma Neutron Activation Analisys
LC = 1.645σ0 (2.13)
LD = 2LC = 3.29σ0 (2.14)
(2.15)
The highest analytical sensitivity and detection limit is shown in fig.2.1 for
different element in absence of matrix obtained with a cold neutron beam in
the JRR-3M facility at the Japan Atomic Energy Research Insititute (JAERI)
[16].
DL may vary of one order of magnitude accordingly to the matrices. Nev-
ertheless, it is possible to identify three levels of detection:
12
2.1. Characteristics of PGNAA
Figure 2.1: The highest analytical sensitivity and the lowest detection limit
of element by cold neutron beam PGNAA facility of JRR-3M at the Japan
Atomic Energy Research Insititute.
Figure 2.2: Sketches of the typical PGNAA spectra from light (left) end heavy
(right) elements. The number of full energy peaks is higher for heavy elements;
the peaks in the lower or higher energy intervals are selected for nuclide iden-
tification purpose. For light elements, the spectrum is more simple.
For heavy elements, the spectrum has a higher number of peaks overlaping
in the middle region of the energy range. Therefore, the only peaks that can
be used for the identification are located at low and high energies, and are
those originating form the direct transitions from an exited level to the ground
state. Anyway, since the high energy region has a lower number of peaks, for
a more reliable qualitative analysis it is better to use this zone.
13
2. The Prompt Gamma Neutron Activation Analisys
14
2.2. Main components of a PGNAA facility
15
2. The Prompt Gamma Neutron Activation Analisys
16
2.2. Main components of a PGNAA facility
Facility Characteristics
SNU-KAERY Thermal beam extraction: diffraction (PG)
Beam flux: 8.2 · 107 n/(cm2 s) (thermal equivalent)
Beam size: 2 × 2 cm2
Cadmium ratio: 266 (for gold)
Effective temperature: 269 K
Titanium (1382 keV) sensitivity: 2020 counts·s−1 · g−1
Detection system: single HPGe with pulse processing system
Total background counting rate: 3000 counts/s
Dalat research reactor Thermal beam extraction: moderation (graphite) and filtering (Bi)
Beam flux: 2.1 · 107 n/(cm2 s)
Beam size: 2.5 cm
Cadmium ratio: 21 (for gold)
Detection system: single HPGe with pulse processing system
NIST (cold) Cold beam extraction: filtering (Be, Bi) and mirror giude
Beam flux: 9.5 × 108 n/(cm2 s)
Beam size: 2 cm or smaller
Effective temperature: 14 K
Titanium (1382 keV) sensitivity: 7700 counts·s−1 · g −1
Detection system: HPGe and Compton suppression electronics
0.6202σrem ρ
Σrem = (2.19)
A
where ρ and A are the density and mass number of the absorber respectively.
When more than one heavy material layer is present, the macroscopic cross
section becomes: �
Σrem = Σi l i (2.20)
i
Neutron absorption The most used materials for the neutron absorption
are those containing 6 Li, 10 B, 113 Cd because of their high neutron capture
cross section. Among these, only 6 Li absorbs the neutrons without producing
gamma rays,10 B absorbs the neutrons via the (n, γα) reaction. About Cd,
altough it is easy to shape and it is a good absorber, it is not indicated in
case of high flux because of its residual radioactivity in addition to the strong
prompt 559-keV capture gamma rays that are emitted. The characteristic of
the main neutron absorbers are illustrated in fig.2.4.
As consequence of the neutron capture in 10 B , 2.8 MeV are relased, shared
18
2.2. Main components of a PGNAA facility
2.2.3 The shutter, the sample holder and the beam stop
The function of the shutter is to turn on and off the neutron beam when the
reactor is on. It is commonly located in front of the beam port and it is designed
to stop a neutron beam already filtered, therefore mainly composed of thermal
neutrons, but eventually containing also an epithermal and a fast components.
For this reason, the shutter must be made of a thermal neutrons absorber,
commonly a thick boron- or lithium-containing material, and supplemented
by thermalising materials and epithermal absorbers.
Some precautions must be taken at the beam tube, considering the scatter-
ing reactions occurring in the air contained in it: passing through 1 m of air,
about 5% of the neutrons are scattered into the surroundings. To avoid this,
the beam tube can be either evacuated or filled with helium, or alternatively
it can be lined with 6 Li enriched material.
The beam tube ends where the sample holder begins. To center the sam-
ple in front of the beam, it can be hold in a proper position by using ma-
terials that neither absorb or scattered the neutrons. Fluorocarbons such as
TeflonTM TFE or FEP (both with empirical formula CF2 ), or TeflonTM PFA
(approximately C4 F7 O), are commonly used for this purpose because of the
low capture-cross sections of fluorine and carbon. FEP is available in monofil-
ament fibers or in thin films reducing the amount of material used to hold the
sample.The target chamber should be lined with a neutron absorber, preferably
6
Li, to shield the neutrons scattered by the target. Other materials that have
been used as sample holder are: aluminum, magnesium, vanadium, graphite,
quartz, and silicon.
The final part of the facility is the beam catcher, this must be designed
in order to reduce the neutron and gamma radiation dose rate, outside the
PGNAA, to a minimum level, according to the radiation protection laws. This
structure is mainly constituted of blocks of materials properly arranged and
cutted in order to absorb those primary neutrons that crossed the sample
19
2. The Prompt Gamma Neutron Activation Analisys
without interact. Thus, the beam stop must absorb mainly thermal, but also
fast and epithermal neutrons. From the shielding point of view, the photon
sources must also be considered, that is: the gamma rays from both the core
and from the interaction of the neutrons with the surrounding materials.
20
2.3. Gamma-ray detector
the metallic atoms. Single crystals of germanium are then slowly grown from
this purified block. If the low amount of remaning impurities are donor, i.e.
with an higher number of valence electrons, then the single crystal is called
n-type, if acceptors, i.e. atoms with less valence electrons, then it is p-type.
Figure 2.5: Planar and close ended coaxial germanium detector configurations.
Among the two configurations the coaxial one has a larger active volume,
that is the region of the crystal able to detect the signal, for this reason it
is the one used in PGNAA. The contacts of the crystal do not belong to the
active volume, but they represent dead layers on the surface of the detector.
Some techniques for the contact formation are able to reduce the thickness to
few tenth of micrometers in a way that it does not affect the resolution of low
energy gamma rays.
21
2. The Prompt Gamma Neutron Activation Analisys
Each of these contributions depends on the energy of the gamma radiation and
on the dimension of the crystal. WX is the most significant for large volume
crystals; wherase WD and WE incerase with the gamma-ray energy. By the
use of the Poisson model, the fluctuation in the number of charge carriers is
E/�, where � is the ionization energy and E is the gamma-ray energy. This
evaluation requires that all the events along the track of the ionizing particle
are indipendent. Nevertheless the observed fluctuation is higher than the sta-
tistical prediction. The fraction between these two value is the Fano factor F:
observed statistical variance
F = (2.22)
E/�
A small Fano factor means a better energy resolution, being this value related
to WX2 according to the formula:
Finally, WE2 represent the broadening effect due to all the electronic component
associated to the detector.
22
2.3. Gamma-ray detector
Figure 2.6: Resoultion (FWHM) for the 1332 keV as a function of the neu-
tron fluence for a conventional and reverse electrode configuration coaxial Ge
detector.
FE Full-energy peak (FEP), when the photon loses all its energy (E) within
the active volume of the detector.
23
2. The Prompt Gamma Neutron Activation Analisys
24
Figure 2.7: Normal and Compton-suppressed spectra of N a with 1369 keV
and 2754 keV gamma energies.
S Step below the full-energy peak, when the photons lose a small amount
of energy in a small-angle Compton scattering in the collimator or in the
dead region of the detector followed by full absorption of the scattered
photon.
MC Multiple Compton scattering region below the full energy peak and above
the Compton edge.
CE Compton edge about 220 - 250 keV below the full energy peak. It is a
result of a single Compton-event and corresponds to the highest energy
left in the detector in a single scattering. The Compton edge is below
the FEP with an energy of E/(1 + E/255.5keV ), as calculated for free
electrons.
CP Compton plateau is formed, when the Compton photon leaves the detec-
tor.
SE, DE Single and double escape peaks are 511 and 1022 keV below the full en-
ergy peak of high-energy photons that can produce an electron-positron
pair. These peaks are produced when one or both annihilation photons
leave the detector.
CF Between the single escape peak and the Compton edge there are events
from single escape processes. The escaping 511 keV photons may produce
a Compton scattering before leaving the sensitive volume.
AE Between the single escape and the double escape peaks there are events
from Compton scattering of both escaping 511 keV photons, which leave
the sensitive volume. Their Compton edge is 170 keV below the single
escape peak. Sometimes a back scattered peak of one of the escaping 511
24
2.3. Gamma-ray detector
keV photons can be identified at 34 keV below the single escape peak
(too weak to be seen in Figure 2.7).
A Annihilation peak at 511 keV, when an annihilation radiation produced
in the surrounding structural material or the sample is detected.
BS Back scattering peak at 220-250 keV is produced when back-scattered
Compton-photons from the sample chamber and other structural mate-
rials in front of the detector are observed. [The exact energy is E/(1 +
E/255.5keV ).] In the special case plotted in Fig2.7 there are two back
scattering peaks according to the two gamma energies, while in the typ-
ical prompt gamma spectra it covers a wider region.
B The strongly increasing background intensity towards low energies comes
from the bremsstrahlung from photo- and Compton-electrons and also
from the β particles emitted by radioactive nuclides. The baseline at
low energy can be further increased by the multiple Compont scattering
occurring in the shielding material placed close to the detector. he slope
of this region can be especially steep, when the spectrum contains intense
high-energy components.
X Characteristic X-ray peaks also show up below 100 keV from the shielding
and other structural materials.
In case of strong pile-up 3 or random coincidences, any combinations of
the above events can happen, which produces double or higher order Compton
edges or peaks at summed energies of full energy peaks. These random coin-
cidences and peak summing must be distinguished from the true coincidence
summing of gamma rays (see next paragraph) from cascades [22].
where Cγ is the measured net peak, Rγ is the count rate, N is the number of
3
The pile-up of events occurs when a second signal arrives at the amplifier within its
resolution time, i.e. within the shaping width of a single pulse
25
2. The Prompt Gamma Neutron Activation Analisys
• The geometrical efficency is the ratio of the number of gamma rays reach-
ing the detector to the number of gamma rays started from the source.
It can be calculated by:
r2
�geom = 2 (2.25)
4d
where r is the radius of the detector surface facing the sample and d is
the source-detector distance.
26
2.3. Gamma-ray detector
Figure 2.8: Layout of the collimated detector, and transmission geometry of the
collimator (0 = the geometric center, a = sample-to-shielding distance, b = thickness
of the collimator, r = radius of the collimator, e = end of the partial illumination
region, d = the distance of the inner aperture to the sample). The thick line shows
the geometry factor, it goes for 0 to 1 in the partially illuminated zone. The hatched
circle represents the front collimator seen by the the source point. The empty circle
is the source point view of the rear aperture. (Drawing is not to scale.)
27
2. The Prompt Gamma Neutron Activation Analisys
28
2. The Prompt Gamma Neutron Activation Analisys
30
Chapter 3
Experimental boron
concentration measurement
31
3. Experimental boron concentration measurement
The course of the PhD work was almost entirely dedicated to PGNAA, from
the beam tailoring to the measurement issues related to the analysis of boron
in biological samples. To gain experience about this last point, the author of
this thesis spent a research period at the Center for Neutron Research of the
National Institute of Standars and Technologies, where two prompt gamma fa-
cilities are available: CNPGNAA and TNPGNAA, using respectively a guided
cold neutron beam and a conventional thermal neutron beam. During the
stay at NIST the author participated to different boron measurement sessions,
mainly in metallic samples embedded in epoxy. This experimental activity
allowed facing the typical issues arisen in the analysis of hydrogenous samples,
such as the biological tissues. In this chapter the measurement performed
are described together with some theoretical aspects of the prompt gamma
spectrum analysis techniques.
32
3.1. Boron measurement by α spectroscopy
is not gaussian but it has the tipical shape of an absorbed spectrum; this is due
to the fact that the 10 B and the 14 N are uniformly distributed in depth into
the sample. The charge particles produced during the irradiation start from
different positions, therefore they reach the detector with different residual en-
ergy. The interval of the spectrum used to calculate the boron concentration,
indicated in fig.3.1 by the vertical bars, is located in a region whose contribu-
tion comes only from the α particle, with no counts from the 7 Li, (1030 keV
maximum energy) and the protons (580 keV maximum energy). The selected
energy interval does not contain the α coming from the overall sample, but
only the ones emitted in a particular depth range (Δ(ρx)). The evaluation of
the parameter Δ(ρx) is most important to obtain the concentration (C) of 10 B
in the sample that can be calculated by:
k PA ΔE
C(ppm) = (3.1)
η · σ · φ · S NA Δ(ρx)
where η is the geometrical efficiency of the apparatus, φ is the thermal neutron
flux, σ is the cross section of the (n, α) reaction, k is the number of events per
unit energy and time detected in the selected ΔE, NA is the Avogadro number,
PA is the atomic weight of boron.
Once the ΔE is fixed, the corresonding depth range (Δ(ρx)) can be eval-
uated by using a curve of the residual energy of the α particle as a function
of the crossed tissue thickness. This curve describing the α particles energy
loss in lung tissue was experimentally evaluated [27] and, the procedure and
results are the topics of the next sections.
33
3. Experimental boron concentration measurement
Figure 3.2: The experimental set-up used for measuring the residual energy of
α particles after crossing lung-tissue samples of different thicknesses.
34
3.1. Boron measurement by α spectroscopy
Therefore, for each sample the mass and the area were evaluated by using,
respectively, a precision balance (Gibertini) and a Leyca stereomicroscope;
then the average thickness in mg/cm2 was calculated; the obtained values
range from 0 to about 0.7 mg/cm2 .
Figure 3.4: (a) Americium source spectrum. (b) Spectrum obtained with bare
mylar.
sian curves to take into account the 3 most probable branches of the α emitted
35
3. Experimental boron concentration measurement
by the 241 Am source; (the analysis of the experimental data, the calculations
and the plotting were performed using root [28]) . The most probable peak
was used to perform the energy calibration. The second spectrum was used to
evaluate the energy of the α particles crossing the tissue sample; a gaussian fit-
ting procedure was carried out and the resulting mean energy value was equal
to 2200 ± 80 keV.
In the next step, the spectra of the tissue samples were collected and the
residual energy of the α particles was evaluated by a fitting procedure. In
fig.3.5(a) and 3.5(b) the spectra respectively for a thin sample (0.13 mg/cm2 )
for a thick sample (0.60 mg/cm2 ) are shown. Two peaks can be observed in
Figure 3.5: (a) Spectrum of a thin sample. Two peaks are clearly visible; the
one at higher energy corresponds to a particles that just crossed the mylar; (b)
thick sample
the thinner sample; the one at higher energy value comes from the α particles
that crossed only the mylar support, this can be explained by the presence of
holes in the samples (as can be seen in fig.3.3). The broadening towards lower
energies of the most probable peak was due to the point to point variability of
the sample thickness, related to the heterogeneity of the tissue, which causes
a continuous change in the energy loss of the α particles. The increasing of
tissue thickness causes a higher broadening of the peak, as can be observed in
the fig.3.6 where spectra from samples with different thicknesses are compared.
The evaluation of the α particles energy loss crossing lung tissue samples is
affected by the broadening of the peak whose entity was supposed related to
the disomogeneus nature of the sample. Some Monte Carlo calculations were
performed in order to investigate this hypotesis.
36
3.1. Boron measurement by α spectroscopy
the resulting spectrum, obtained without any sample, was slightly different
from the experimental one expecially in the low energy region. Successively, a
depth distribution of the Americium source was introduced and its values were
gradually changed in order to obtain a good overlapping of the simulated and
experimental spectra, as can be seen in fig.3.7. Table 3.1 gives the percentages
and the corresponding depth intervals starting from the surface.
A tissue sample with thickness similar to an experimental one was simulated;
the resulting spectrum reproduced well the energy of the most probable peak,
37
3. Experimental boron concentration measurement
Depth µm 0 0 ÷ .15 .15 ÷ .28 .28 ÷ .38 .38 ÷ .68 .68 ÷ 1 1÷2 2 ÷ 10
Source percentage 62.18 19.29 7.5 3.21 3.21 2.14 1.61 .86
Table 3.1: Spatial distribution of 241 Am source into the platinum support
assumed in the MCNPX simulation to reproduce the experimental spectrum.
but not its broadening. This difference was supposed to be related to the lack
of disomogenity in the simulated sample. To verify this hypotesis a sample,
made up of different zones with a proper density, was simulated. A single par-
allelepiped of tissue with a square base of 0.01 mm2 was simulated with a fixed
thickness according to the experimental sample that was under examination.
Circular zones of density ranging from 0 (no tissue) to almost 2 g/cm3 were in-
serted into the parallelepiped fig.3.8(a). Using the MCNPX repeated-structure
capability, the modular parallelepiped was reproduced to fill the whole area of
the tissue sample (fig.3.8(b)). The densities of the different circles were grad-
Figure 3.8: The geometry of the tissue sample as reproduced in the simulation:
(left) a square base of 0.01 mm2 filled with disks of different densities; (right)
the MCNP repeated-structure capability was used to fill the whole area of the
sample.
38
3.1. Boron measurement by α spectroscopy
Figure 3.9: Comparison between the experimental and the simulated spectra
of α particles crossing a lung-tissue sample 0.334 mg/cm2 thick: experimental
spectrum (dashed line); MCNPX simulation of a heterogeneous sample (dotted
line); MCNPX simulation of a homogeneous sample 0.334 mg/cm2 thick (full
line).
only uniform samples were simulted. The results of the simulations along with
the corresponding experimental results are collected in table 3.2.
Table 3.2: Results (peak position and variance) of the simulation of alpha parti-
cles traversing a homogeneous tissue sample; three thicknesses are considered.
Experimental results for non homogeneous samples are reported in the last
two columns for comparison; a good agreement is visible for the energy peak
(columns 2 and 4); the contributions to the broadening of the spectrum due
to straggling and beam collimation from that due to the lack of homogeneity
of the sample can be separated by comparing columns 3 and 5.
3.1.5 Results
The experimental and simulated values of the residual energy of α particles as
a function of the crossed thickness of lung tissue sample were plotted (fig.3.10).
The residual energy is the most probable energy peak obtained by a gaussian
fitting procedure and the error bar is the associated standard deviation. As was
39
3. Experimental boron concentration measurement
Figure 3.10: Plot of the residual energy of the a particles as a function of the
distance crossed in dry rat-lung tissue. The MCNPX simulation results are
also shown. The continuous line is the linear best fit of the experimental data.
demonstrate by the Monte Carlo simulations, the peak broadening was related
to the heterogeneity of the tissue sample, that increases with the thickness
of the sample. The continuous line of the graph is the linear best fit of the
experimental points.
The data reported in fig.3.10 were used to plot the thickness as a function of
the residual energy, which was linearly fitted:
These results are used for the evaluation of the boron concentration present in
lung tissue treated with boron. The energy interval 1100 - 1350 keV (fig.3.1),
chosen as the portion of the spectrum to be used in the boron concentration
measurement, correspond to a tissue thickness Δ(ρx) = 0.12 ± 0.02mg/cm2 to
be used in Eq.3.1.
This experiment allowed the evaluation of boron concentration in lung tis-
sue treated with boronated substances by α spectroscopy technique.
40
3.2. Experience at NIST
41
3. Experimental boron concentration measurement
Figure 3.11: Picture of the conventional thermal neutron beam PGNAA facility
installed at the top of the NIST reactor.
42
3.2. Experience at NIST
can be preformed. The count rate of a particular gamma ray is related to the
mass of the nuclide according to the formula (already described in chapter 2):
ργ is the area of the peak divided by the measuring time (live time), while n is
the number of atoms, ε(Eγ ) is the counting efficency under the photoelectric
peak of the detector and Φ is the neutron flux. This expression comes out to
be more complex in the real case, consequently the absolute method for the
mass nuclide determination is not so straigthforward. Nevertheless, in case of
thin sample the formula for the count rate is simplify (2.5) and the mass of
the nuclide is directly proportional to the net peak area A as follows :
M A
m= (3.5)
NA ε(Eγ )tσγ0 Φ0
where M is the atomic weight, ε(Eγ ) is the counting efficency for that specific
gamma ray energy of the nuclide, t is the measurement time (live time), Φ0 is
the thermal equivalent neutron flux and σγ0 is the partial gamma ray produc-
tion cross section.
This method can be used only if the following conditions are satified:
• the live time is evaluated very accurately and the samples position does
not change for every measurement.
Nγ,x /tm
sx = (3.6)
mx
43
3. Experimental boron concentration measurement
If the neutron flux is constant and the geometry conditions are unchanged,
the sensitivity is constant, then it is possible to determine the mass of the
element in the sample by:
(Nγ,x)s /tm
(mx )s = (3.7)
sx
where sx is the sensitivity evaluated by the measurement of the standard.
Nevertheless, this method requires an accurate choice of the standard whose
chemical composition and geometry should match as much as possible with the
ones of the sample under study. Otherwise, parameters like, γ-rays detection
efficency, neutron scattering and self assorption of γ-rays and neutrons can
change, with the result of a different sensitivity for the element under study.
A more robust method consists in the internal standardization, by the use of
the parameter k0 . The relative elemental content (kr,c (x) factor) is the fraction
between the analytical sensitivity of the analyte x and a comparator element
c both contained in the standard. The elements used as internal standard
comparators are commonly H, Cl, Ti, Cr, Ni, Sm, and Hg. The k factor
is independent from the experimental conditions normalizing the sensitivities
with their detection efficencies, consequently the k0 factor is :
sx /ε(Eγ,x ) θx γx σ0,x /Mx σγ,x /Mx
k0,c (x) = = = (3.8)
sc /ε(Eγ,c ) θc γc σ0,c /Mc σγ,c /Mc
where θ is the abundance of the capturing isotope , γ is the number of γ-rays
emitted per capture, σγ is the partial gamma-ray production cross section (al-
ready defined in 2.2), M is the atomic weight.
Values of k0 and their uncertainties, relative to the hydrogen capture gamma
ray at 2223 keV, have been tabulated for more than 30000 capture lines and
are available at http://www-nds.iaea.org/pgaa.
A comparison of k0 factors obtained with four different neutron beams, the
thermal and cold neutron guide beam of JRR-3M, and cold neutron guided
beam and conventional thermal neutron beam can be found in [30]. The com-
parison shows that for elements with neutron cross section following the 1/v
law, the factors agree within 10%, whereas, in case of non-1/v elements, k0
depends on the characteristics of the neutron beam.
An effective g-factor is used in order to correct k0 for the neutron beam in
case of non-1/ν nuclides:
sx /ε(Eγ,x ) ĝc σγ,x /Mx ĝc
k0,c (x) = = (3.9)
sc /ε(Eγ,c ) ĝx σγ,c /Mc ĝx
The g-factor can be obtained by the following formula:
� ∞ �
1 2E
ĝ = σ(E) · · n(E)dE (3.10)
σ0 · ν 0 0 mN
where E is the neutron energy, σ(E) is the neutron capture cross-section as
a function of the neutron energy, mN is the mass of the neutron, and n(E) is
44
3.2. Experience at NIST
where Ax,y is the specific count rate of the element. The absolute contents
cannot be obtained directly by k0 , but require the determination of at least
one element in the sample, using other analytical methods.
Spectral interference
The high number of peak in a PGNAA spectrum, causes the spectral interfer-
ence to be one of the highes sources of error.
The doppler broadening of B peak makes it more sensitive to the problem
of the spectral interference. The peaks that could overlap in the energy region
of boron come from 11 different elements, i.e Na, Si, P, Cl, Mn, Co, Ni, Sr, Cd,
Sm, and Hg. Among these, the only important in the analysis of biological
samples is the 472 keV Na peak.
The spectral interference can be corrected by a fitting procedure or by the
reference peak method that uses other interference-free gamma ray peaks.
An example of deconvolution procedure is shown in fig.3.13 [33] where the
B peak is fitted assuming that the velocity of 7 Li is constant (v0 ), than the
Doppler shifted energy of the gamma ray is given by
v0
ΔE = E0 ( cosθ) = kcosθ (3.12)
c
45
3. Experimental boron concentration measurement
Figure 3.12: Line shapes of the doppler broadened boron peak for different
samples containing boron; (a) gaseous boron trifluoride BF3 , (b) aqueous so-
lution of boric acid H3 B03 and (c) elemental boron. For comparison a normal
peak from a stationary 24 N a nucleus (N a2 CO3 target) is shown (d).
where E0 is the γ-ray energy without Doppler shift, c the velocity of light,
and θ the recoil angle between the fly-direction and the detector axis. The
probability of recoil with angle θ is proportional to sinθdθ. The line-shape
function for the broad boron peak can be simplified as:
� π
(E − E0 + Kcosθ)2
F (E) = N exp− sinθdθ. (3.13)
0 2σ 2
46
3.2. Experience at NIST
Figure 3.13: Deconvolution of the broadened 478 keV peak by computer fitting.
neutron spectrum of the beam and were sistematically studied at the thermal
and cold neutron beam PGNAA facility.
47
3. Experimental boron concentration measurement
Figure 3.14: Hydrogen sensitivities for disk shaped samples (void square) and
for sphere (full circle) of THAM
the H sensitivity for spherical samples of different size remain constant within
the measurement uncertainty. Monte Carlo calculations [39] showed that the
scattering matrix causes a change in the neutron path lenght; depending on
the size and the shape of the target, this change in neutron path lenght may
increase or decrease the probability of neutron absorption, thus decreasing or
increasing the elemental sensitivity. This effect disappears in spherical targets
and it is relevant only for relatively small samples. Similar experiments were
also carried out with a cold neutron beam [40]. In order to minimize the errors
due to the neutron scattering, when a relative standardization is applied, it is
important to chose a standard with shape, size and H concentration as close
as possible to the sample.
The hydrogen content in the sample causes also an enhancement of the
background counting rate, due to the interactions of the neutron scattered
by the sample into the structure of the apparatus. For instance gamma rays
coming from the interactions with: H, B, C, Pb ( in the shielding materials);
N (in the liquid nitrogen); Al,Cl and Fe ( in the support structure); and N and
Ar (in the air) can be detected in the spectrum background.
48
3.2. Experience at NIST
locate the sample always at the same positions. A blank sample and a stan-
dard boron sample containing 1.09 mg of boron were irradiate to evaluate the
boron content in the samples. Considering the magnet sample composition, i.e.
N d2 F e14 B, the mass of the magnet was determined for every sample, by the
estimation of the Nd mass from PGNAA analysis. The spectra were collected
in Compton suppression mode, without evaquating the sample chamber. The
amount of boron was obtained by dividing the net count rate of the 478 keV
peak by the analytical sensitivity obtained from the natural boron standard
applying the formula 3.7. In the evaluation of the boron net count rate, results
from blank were used for a more precise estimation of the background count
rate. The spectra obtained by the irradiation of the boron standard and the
blank are represented in fig.3.15.
Figure 3.15: The spectra from the irradiation of the boron standard (black)
and the blank (green).
For each sample the net area under a full-energy-peak was determined by the
Program SUM developed at NIST [43]. The program requires as input the
peak boudaries channels L and R, (left and right respectively) and the width
of the baseline on left and right sides (BL and BR) (see fig.3.16). Then the
program calculates the centroid, the background, the net area, the FWHM,
the energy, the count rate, the percent error of the net, and the Currie quality
indicator [32].
The net area under the peak is determined subtracting from the gross area a
trapezoidal baseline evaluated by averaging the BL and BR channels to the
left and right of L and R respectively, placing these averages at the positions
49
3. Experimental boron concentration measurement
Figure 3.16: Evaluation of the net area by SUM program. The input param-
eter, that is, peak boundaries (L and R) and widths of the baseline (BL and
BR), are shown.
L and R:
� L−1 R+BR
�
R−L+1 1 � 1 �
BKGN D = Y (C) + Y (C) (3.14)
2 BL C=L−BL BR C=R+1
(NB,w − NB,bkg )
BkgH = NH,s × (3.15)
NH,w
50
3.2. Experience at NIST
Figure 3.17: Comparison between the spectrum background (black) and the
spectrum with the blank (green); the two spectra, plotted in cps, are almost
overlapped in the energy region higher than 2.2 MeV, instead, for lower energy
the Compton contribution from the 2.2 MeV peak appears in the blank sample.
where NB,bkg is the count rate of background under the boron peak without
any sample.
Thus the final net area of boron in cps is obtained by:
where mB and mN d are the mass fraction respectively 26, 7% for Nd and 1%
for B, deduced by the chemical formula of the magnet, that is N d2 F e14 B. The
sensitivity previously determined was used to obtain the Nd mass, thus the
51
3. Experimental boron concentration measurement
Figure 3.18: Spectra from the irradiation of a higher mass boron contaning
sample compared to the other magnets under study. The live time of irradi-
ation is about 1 hour. The overlapped spectrum represents an enargement in
the boron energy peak region; the doppler broadened FEP of boron and the
618 keV Nd peak are shown.
FileName mg B mg Nd mg magnet %H
MAG1-3 0.35 · 10−3 ± 0.05 · 10−3 0.283±0.010 1.06 9.8%
MAG1-4 0.17 · 10−3 ± 0.04 · 10−3 0.299±0.010 1.12 9.5%
MAG1-5 0.25 · 10−3 ± 0.04 · 10−3 0.233±0.009 0.87 9.4%
MAG1-6 9.05 · 10−3 ± 0.04 · 10−3 0.365±0.007 1.37 9.1%
MAG2-3 10.16 · 10−3 ± 0.07 · 10−3 0.261±0.008 0.98 8.9%
MAG2-4 8.78 · 10−3 ± 0.06 · 10−3 0.229±0.007 0.86 8.7%
MAG2-5 15.59 · 10−3 ± 0.09 · 10−3 0.421±0.010 1.58 9.4%
MAG2-6 12.84 · 10−3 ± 0.09 · 10−3 0.360±0.010 1.35 9.2%
Table 3.3: Results of the PGNAA analisys of the magnet samples embedded
on epoxy; the masses of the boron, neodimium, and hydrogen contained in the
sample were derived, along with the mass of the N d2 F e14 B magnet.
The values of sensitivity for boron, hydrogen and neodimium obtained by the
PGNAA analisys and used for mass determination are collected in table:3.4.
52
Nuclide Sensitivity (cps)/mg
B 1101.6
H 2.23
Nd 3.53
Table 3.4: Sensitivity for the different element B, H, and Nd obtained from
the irradiation of respectively a boron standard, a blank and from the sample
itself.
3. Experimental boron concentration measurement
54
Chapter 4
The design of a PGNAA facility
at Triga Mark II reactor
4.1 Introduction
The implementation of a new measurement method for the evaluation of boron
concentration, based on prompt gamma spectroscopy, represents an important
step forward in BNCT studies. Indeed the new facility not only allows the
analysis of biological sample in liquid form, not feasible at the moment with
the available techniques, but also it provides a quick and accurate assessment
of the 10 B in blood useful in clinical phase for the correct estimation of the
delivered dose in the BNCT irradiation.
In this chapter the design of the PGNAA facility is dealt with. The first
part is dedicated to the Monte Carlo N Particle (MCNP) simulation code used
to develop the project, whereas in the following part the different components
of the facility are descried. In the final part, the performace capability of the
designed PGNAA are explained.
55
4. The design of a PGNAA facility at Triga Mark II reactor
C is tangent to the outer edge of the core and a fourth, D, is a radial piercing
beam port that crosses the graphite reflector and stops in front of the core.
Among these channels, the one used to install the prompt gamma facility
is B; the graphite reflector thermalizes neutrons, making the epithermal and
fast components lower if compared to the others channels.
4.2.2 MCNP
The design of the PGNAA facility was achieved using a Monte Carlo particles
transport code MCNP, in the version MCNP-4c2 [44]. It is developed in the
Los Alamos National Laboratory and it can transport neutron, gamma rays
and electrons either in single or in coupled neutron/photon/electron mode.
MCNP simulates the path of each particles from the source to their death
(absorption, escape,...) and recording some important aspects (tally) specified
by the user. The average behaviour of the physical system can be deduced by
the average behaviour of the simulated particles.
The use of MCNP requires a deep knowledge of the source, the geometry of
the problem, the composition of the materials used, as well as the physical
data such as the cross sections of the different interactions radiation-material
involved in the problem.
In order to design the different components constituting a PGNAA system, an
input file describing the core and the geometry of the reactor, already built
and validated in Pavia [47], was used. In the different simulations each element
of the system was inserted in the geometry and proper tallies were chosen in
order to evaluate the suitability of the proposed solution for that particular
tasks (neutron filter, beam collimation, beam catcher design..). Moreover, the
use of non analogue tecniques1 was necessary in order to reach a good statistic
despite the long distance and the shielding material between the source and
the tally position. For the same reason, the shifting of the source from the core
to a surface close to the beam port was necessary both for the design of the
beam catcher and in the simulation of the response function of the germanium
detector.
1
see the last paragraph of this section
56
4.2. Materials and method
57
4. The design of a PGNAA facility at Triga Mark II reactor
The pulse height tally (F8) was used to simulate the germanium detector
response, it provides the distribution of the pulse energy deposition occurring
in a cell. On the contrary of the other tallies, F8 records the energy deposited in
the detector by the single physical particles adding one score in the correspond-
ing energy bin. The pulse tally is an inherently analogue process, it does not
work well with neutrons and cannot be used with any variance reduction other
than source biasing. The sintax F8:P, is equivalent to F8:E and F8:P,E; that is,
there is not discrimation in the energy deposited by photons or electrons. F8
tally was used with a ”mode n,p“ that is with a coupled transport of neutrons
and photons omitting the electron transport. Moreover for the transport of
photons with energy lower than 100 MeV a ”detailed physics“ mode was cho-
sen, e.i. scattering Thomson and fluorescent photon production were included.
As concerning the simulation of the electron produced in photon interaction,
MCNP provides 3 different model, the ”thick target brehmmstralung” (TTB)
model was chosen. It works with mode e turned off, this model generates elec-
trons, but assumes that they travel in the direction of the incident photon and
that they are immediately annihilated. Any bremsstrahlung photons produced
by the non transported electrons are then banked for later transport. Thus
electron-induced photons are not neglected, but the expensive electron transport
step is omitted. This detail about the photon transport modality can be set
by the use of the PHYS:P data card.
58
4.2. Materials and method
Concering the simulations with the gamma transport from the core, some
preliminary consideration must be done. The reactor gamma rays are gener-
ated by three different processes occurring in the core:
• fission prompt γ, occurring 5 · 10−8 s after a nuclear fission takes place;
The design of the beam catcher and of the other PGNAA components lo-
cated outside the reactor biological shield, required the shift of the neutron
source from the core to a surface close to the end of the channel. This opera-
tion was mandatory because the neutron transport from the core through the
channel, almost 350 cm long, and through a shielding structure would not have
ensured sufficient statistc with the use of non analogue techinques. In practice
this operation consisted of a first run (with the source in the core) in which all
the information, e.i. current, energy and fly direction, of the neutron passing
through a surface are collected with high accuracy. Then, starting from these
results a new surface source can be implemented, shutting down the first one
and specifing the new probability distribution functions for energy, fly direc-
tions and position of the sampled neutrons. This new source was validated by
comparing the average neutron flux in a specific cell, using the original source
and the new one.
Then, with this procedure a surface source located 30 cm before the exit of
59
4. The design of a PGNAA facility at Triga Mark II reactor
the B channel, was used in order to design the beam catcher. The neutrons
are sampled uniformly from a circle with 10 cm of radius; the cosine of the
angle between the fly direction of the neutron and the normal to the surface
(forwards), is samples according to 3 intervals whose limits are 0, 0.98481,
0.99619, 1, each with its own probability and with its own energy spectrum.
The neutron energy ranges from 0 to 14 MeV divided by 7 different energy
bins, according to the following bounds: 0, 0.4 eV, 10 keV, 500 keV, 1 MeV,
2.5 MeV, 14 MeV.
The neutron spectra in corresponence of the source was evaluated in absence
of filters in the channel, with the aim to be conservative in the design of the
shielding structure. The validation of the source by comparing the average
neutron flux in cells located at the end of the channel, respectively at 346 cm
(cell 462) and and 352 cm (cell 463) from the center of the core are shown in
fig. 4.1. The surface source gives a neutron flux higher for each energy bin that
results, on average, increased of about 10% respect to the flux obtained with
the source in the core. This source, althought does not reproduce precisely
the results obtained with the source in the core, it was nevertheless considered
appropriate to design the beam cather since its slight overestimation of the
neutron flux can result in a further conservative approximation.
A further shift of the source from the core to a surface, whose normal was
on the beam axis, was necessary to evaluate the response function of the de-
tector. The new neutron source was located close to the measurement position
(about 21 cm distance source-sample) and to the germanium detector, it was
determined considering the effects of the filters and the collimator to the neu-
tron spectrum. To get reliable results in this geometry, the simulations with
the source in the core was performed applying a non-analogue technique, Dx-
tran sphere (see forward); a Dxtran sphere enclosing the tally was implemented
in order to bias the particles transport in a partially deterministic way that
will be described later. The new neutron source was implemented sampling
uniformly the neutron position in a circle with 2.12 cm radius corresponding
to the umbra section defined by the collimator and sampling the fly direction
with a uniformly angular distribution between 0 and 1.7 degrees corresponding
to the beam divergence in that position. The neutron energy ranges between 0
and 10 eV and it is sampled from a histogram with 25 energy bins. The source
was validated by the evaluation of the total number of (n,α) reactions in a pure
10
B sample (combining a F4 with a FMn card) located at the measurement
position, using the source starting from the core and the superficial one.
Thermal treatment
Some of the materials used for this work were defined in MCNP input file along
with their S(α,β) thermal treatment, by means of MT card, most important
when the thermal neutrons are transported.
The interactions of thermal neutrons with the materials are affected by
the thermal motion of the atom, that, if neglected, can be responsible of sig-
60
4.2. Materials and method
Figure 4.1: Comparison of the neutron flux (n/(cm2 s)) in cells 462 (up) and
463 (down), located respectively at 346 and 356 cm from the core, using the
original source and the new one.
nificative error. To take into account of this effect MCNP uses normally a
thermal treatment based on free gas approximation. Anyway this approach is
not always satisfactory, therefore specific S(α, β) cross section data for energies
neutrons lower than 4eV, are available in MCNP libraries, to take into account
the effects of the chemical bound of the crystal structure. These cross section
are available in MCNP only for a small number of material, but it is possible
to add the neeeded library as we did in this work for bimuth and sapphire.
61
4. The design of a PGNAA facility at Triga Mark II reactor
62
4.2. Materials and method
and the one of the cell that is leaving. Each particle will have a lower
weight, as explained before. On the contrary, when a particles enters a
cell with lower importance, it will undergo the Russian Roulette play:
it will survive with a probability equal to the ratio of the importances
with an increased weight, otherwise it will be killed. This play ensures
that for high statistis the total weight is conserved and that less particles
(with higher weight) will be transported in less important regions of the
problem. Obviously the user must pay attention in defying the impor-
tant cells, not excluding regions that could play a role for the tally score,
as for example regions which are far from the tally but could scatter
neutrons to that cell.
Figure 4.2: Sketch of the weight particles assignment by the cell-based Weight
Windows variance reduction technique.
63
4. The design of a PGNAA facility at Triga Mark II reactor
64
4.3. The facility design
proposed (as indicated in the PGNAA facility literature) and finally, the choice
of the most suitable solution was carried out by the Monte Carlo simulations
outcome and feasibility and costs considerations. Even if no experimental
validation was carried out until now, the accuracy of the physics result is
supported, not only by the use of a simulated neutron source already validated
[47], but also by the conservative criteria applied during the Monte Carlo
definition problem.
In fig.4.3 the horizontal channels of the Triga Mark II reactor are illustrated.
The choice of the channel was based on the evaluation of the neutron spectra
at the beam port obtained for each channel in the original configuation. The
channel A faces directly the core, thus its neutron flux is higher compared to the
others but a moderator would be required to slow down the high fast neutron
component, moreover the γ rays flux coming from the core is also high. Similar
considerations can be done for the channel D, but with the difference that it is
possible to insert a block of material, or a sample, close to the outer edge of the
core; on the contrary, in the channel A an aluminum layer stops this access. At
the moment the channel D is employed for another experiment. The channel
C is the tangential one, it has the advantage to provide a beam with a low γ
rays contamination that is desirable for a PGNAA neutron beam, nevertheless
the thermal neutron flux is too low. Finally the channel B, characterized by
the precence of 30 cm of graphite was considered; the reflector provides a first
65
4. The design of a PGNAA facility at Triga Mark II reactor
attenuation of the reactor γ ray flux. By the use of F4 tally, the neutron flux,
for different energy bins, at the A, B and C beam port were simulated by
appling the geometry splitting/Russian roulette (GS/RR) to calculate a set of
cell-based weight windows. This variance reduction tecnique was mandatory
because of the long distance (almost 350 cm between the centre of the core and
the end of the channel) that the neutrons had to be cover to reach the tally
cell. The results of the Monte Carlo simulations, are summarized in table 4.1;
the corresponding calculated relative error is always < 10%.
Energy (MeV) A B C
< 2 · 10−7 3.79 · 108 1.07 · 108 2.61 · 108
2 · 10−7 ÷ 5 · 10−6 1.05 · 108 6.11 · 106 5.58 · 107
5 · 10−6 ÷ 5 · 10−1 4.69 · 108 1.47 · 107 2.38 · 108
5 · 10−1 ÷ 20 4.51 · 108 6.71 · 106 5.96 · 107
total 1.40 · 109 1.35 · 108 6.14 · 108
ϕth /ϕf ast 0.37 3.82 0.74
Table 4.1: Simulated neutron flux (n/(cm2 s)) at the beam port respectively
for channel A, B and C.
66
4.3. The facility design
Table 4.2: Results of the fitting procedure of the simulated neutron spectrum
at the end of the channel B.
Figure 4.4: Neutron spectra at the beam port B with the corresponding fits.
Filter for γ
In order to stop the reactor core γ rays, the addition of a proper shield in the
channel was studied. A poly-cristal bismuth block was chosen due to its high γ
67
4. The design of a PGNAA facility at Triga Mark II reactor
mass attenuation coefficent (Fig 4.3) and to its lower thermal absorption cross
section (0.034 b) compared, for example, to the one for lead (0.17 b) which
also stops effectively the γ rays. In Fig.4.6 the thermal neutron corss section
for Bi and Pb are comapred; the value for the total neutron cross sections at
the thermal energies are respectively 9.3 and 11.3 barns.
Figure 4.5: Values of bismuth mass attenuation coefficient, µ/ρ, and mass
energy-absorption coefficient, µen /ρ, as a function of photon energy.
68
4.3. The facility design
Figure 4.6: Comparison of the absorption neutron cross section for bismuth
and lead.
1 meter far from the bismuth block, in order to study the attenuation of the
photons as a function of the bismuth thickness. The position of the tally was
chosen to avoid the contribution to the tally coming from the secondary ra-
diation scattered at high angles, occurring when the tally is too close to the
absorber; with this choise a more correct evaluation of the γ rays flux at the
measurement position, located almost 3 m from the bismuth block, can be
obtained. A non-analogue photon transport was required (GS/RR) to get the
gamma spectrum with reliable statistic. In fig.4.9 the γ rays spectra resulting
from the different bismuth thicknesses are compared.
The intensity of the gamma source undergoes a first attenuation by almost
30 cm of graphite that, considering an exponential attenuation e−µx , is about
10−2 for 1 MeV γ, according to the value reported in Table 4.3. With the
same calculation the attenuation of 10 cm Bi is about 10−3 . An average at-
Table 4.3: Linear absorbtion coefficent µ[cm−1 ] for bismuth and graphite
tenuation factor (F) for gamma with energy < 1 MeV and energy > 1 MeV
was obtained from the simulations by averaging the ratio of the flux with and
without bismuth filter; the results are reported in table 4.4.
The average attenuation of the γ rays intensity with energy lower than 1
69
4. The design of a PGNAA facility at Triga Mark II reactor
Figure 4.7: Top: Thermal neutron flux (n/(cm2 s)) at the beam port for dif-
ferent distance from the core of the bismuth block (10 cm thick); the x axis
indicate the distance between the graphite external edge and the center of
the Bi block. Bottom: the final position of the Bi block was setted at 50 cm
from the outer reflector edge; the bismuth load rests on the concrete biological
shield.
Bi Thickness [cm] F F
E < 1MeV E > 1 MeV
5 0.016 0.143
7 0.008 0.077
10 0.008 0.036
The effect of the bismuth on neutron beam was also studied; the optimal
thickness is the one ensuring a good gamma shielding without attenuating
70
4.3. The facility design
Figure 4.8: Thermal neutron flux as a function of the distance from the center
of the core for two different channel setup, that is with 10 cm thick bismuth
and without any filter.
Figure 4.9: Comparison of γ ray flux at the middle of the channel for 5, 7 and
10 cm of bismuth thicknesses and in absence of filter.
much the thermal neutron component. The thermal treatment card (MT card)
for bismuth was necessary to take into account the effects of the lattice in the
neutron interaction, that are important especially for neutron energy lower
than 4 eV. In table 4.5 the neutron flux at the end of the channel is listed for
the three different components set as follows: thermal energy lower than 0.2
71
4. The design of a PGNAA facility at Triga Mark II reactor
eV, epithermal energy between 0.2 eV and 0.5 MeV and the fast component
higher than 0.5 MeV.
Table 4.5: Neutron flux (n/(cm2 s)) at the end of the channel, without filters
and with different bismuth thicknesses. The corresponding attenuation factor
(F) for the three neutron energy components are also indicated.
The study of thicker filters is prevented by the higher attenuation that they
would provide to the thermal neutron beam. On the basis of the results of the
simulation, 7 cm thick Bi block was chosen because the thicker filter would not
produce any advantage in terms of attenuation of γ-rays (with energy lower
than 1 MeV) causing also a higher reduction of the thermal neutron flux.
Neutron filter
In order to absorb the unwanted fast and epithermal components of the neutron
beam a filter for neutron is necessary. The addition in the channel of a proper
single crystal material was considered. The use of a single crystal material as
filter for thermal neutrons is based on the fact that its neutron scattering cross
section is of the order of few barns for fast energies and it sharply decrases
at low energies. This behaviour is mainly due to the decreasing of the elastic
(or Bragg) scattering cross section components in a specific energetic range.
When a neutron beam interacts with a poly-cristal material, only the neutrons
with a wavelenght lower than a particular cutoff value λc 2 undergoes Bragg
scattering, while for higher wavelenghts the Bragg scattering does not take
place. For λ > λc the only contributions to the cross section come from
the neutron capture and inelastic scattering processes. The best materials,
for filtering purpose, are characterized by a low cross section for these last
processes; such as graphite, Be, BeO. Those in a polycristalline form have a
cutoff wavelenght of 0.67, 0.4, 0.45 nm (corresponding to the neutron energy
values of respectively 1.82, 5, 4 meV). In particular, when it is necessary to
transmit a specific energy range (such as thermal neutron energy λ = 0.1797
nm) a proper single crystal material should be selected. Parameters, such
as orientation, mosaic spread, temperature, cutting plane, also influence the
transmission properties of the crystal, thus they must be considered within
the beam tailoring procedure [17]. A theoretical formula for the total neutron
cross section in the energetic range of 10−4 eV < E < 10eV was determined
2
λc = 2d where d is the largest lattice spacing
72
4.3. The facility design
Given these properties, a single sapphire crystal was chosen as a filter for
fast neutrons. It was placed in the channel after the bismuth block, its diam-
eter was firstly set to 15 cm (equal to the diameter of the channel), its effect
on neutron beam was calculated for two different thicknesses: 5 and 10 cm
73
4. The design of a PGNAA facility at Triga Mark II reactor
Figure 4.11: A sapphire single crystal block was inserted in the channel, after
the Bi block, as filter for fast neutrons.
In table 4.6 the combined effect on the neutron beam of the Bi shield (7
cm thick) and of the sapphire filter (5 and 10 cm thick) are summarized, along
with the attenuation factor for the different neutron components due to the
presence of the sapphire filter. A sapphire filter of 10 cm thick and 7 cm di-
ameter was chosen as neutron filter because it determines the decrease of the
unwanted fast neutron beam components of 1 order of magnitude, without af-
fecting too much the thermal neutron component. An HEM B5 sapphire filter
(0001) ± 30� with these dimensions was purchased to be inserted in the channel
B of the Triga reactor in Pavia. It is shown in fig.4.13. This crystal is made
of several single cristal disks, properly oriented, thus it is not a single crystal
block. Anyway it represents a less expensive option, showing not significative
differences in transmission properties.
74
4.3. The facility design
Figure 4.12: Sapphire total neutron cross section, in the thermal energy region,
MCNP data.
Table 4.6: Neutron flux (n/(cm2 s)) at the end of the beam port with bismuth
and monocrystal sapphire blocks in the channel. The attenuation factor (F)
due to the implementation of the sapphire is also shown. It was calculated by
the fraction between the flux with both filters (Bi and sapphire) and with only
Bi filter inserted in the channel, for all the three components.
only the Bi block, to 0.0056, with both Bi and sapphire single crystal filters
inserted in the channel.
4.3.3 Collimator
The insertion of a collimator is required to reduce the diameter of the beam
at the sample position, delimiting a uniform beam intensity irradiating the
sample as well as providing a lower neutron beam intensity in the surrounding,
75
4. The design of a PGNAA facility at Triga Mark II reactor
Figure 4.13: Picture of the crystal sapphire block that will be inserted in the
channel, it is 10 cm in lenght, 7 cm diameter.
Figure 4.14: Comparison of γ ray flux at the middle lenght of the channel,
without filter, with 7 cm of poly-crystal bismuth and with the addition of 10
cm of single crystal sapphire block. It can be seen that the presence of the
sapphire further reduces the unwanted γ flux.
76
4.3. The facility design
cm, length L=90 cm, that end at the exit of the channel, fig.4.15;
Figure 4.15: Collimator A with the filter for γ, and fast neutrons; MCNP
geometry.
Successively the filters were inserted. While the position of the bismuth
remained fixed, the sapphire filter was moved along the channel according to
the collimators position. In the three configurations, no significant difference
77
4. The design of a PGNAA facility at Triga Mark II reactor
Figure 4.16: Collimator B; the shadowed area identify the two zones defined
by a collimator: umbra (in red), where the intensity of the beam is higher and
the penumbra where the intensity decrease towards the periphery.
Figure 4.17: Collimator C with the filters for γ and for fast neutrons; MCNP
geometry.
Table 4.7: Thermal neutron flux (n/(cm2 s)) at the end of the channel in
different geometry configuration, no filters are placed in the channel. The
neutrons attenuation due to the collimator is also shown.
This set of simulation, performed with the tally close to the beam port,
confirmed that the collimator A provided the higher neutron attenuation, as
can be seen in table 4.7. Observing the filtered neutron spectra at the beam
78
4.3. The facility design
Table 4.8: Neutron flux (n/(cm2 s)) outside the channel for the different colli-
mator set-ups with the filters inserted in the channel.
port obtained with the three different collimator (table 4.8), the results ob-
tained with the collimator A are not satifactory; although it provided a lower
epithermal and fast neutron component, the thermal neutron flux at the beam
port is too low, considering that a value of about 107 n/(cm2 s) is advisable at
the measurement position. For this purpose the collimator A was discarded.
Before selecting between the remaining B and C collimator a further inves-
tigation was done observing the neutron flux at the measurement position.
In particular, the uniformity of the flux at the sample position and the fast
neutron flux directly irradiating the detector were evaluated. The collima-
tors define two zones along the beam path: the umbra, where the beam has
a constant intensity, and the penumbra, where the intensity lowers gradually
towards the periphery (see fig.4.17). To ensure the maximum uniformity, the
sample should be exposed to the umbra of the beam, while the penumbra
should be reduced as much as possible, to preserve the surrounding. Position-
ing the sample at a distance of about 50 cm from the beam port, geometrically
can be assest that both the collimator B and C fulfill this constraint. The next
step was to evaluate the neutron flux in the area outside the umbra at the
measurement position, this was done to understand which collimator provide
the best shielding of the germanium. For this purpose a new cilindrical tally
cell, 0.5 cm thick, was located at the sample position. It was divided into three
concentric circle section with radii corresponding to the umbra, penumbra and
a further halo sections defined by the collimator (Table 4.9). The so called
”halo” represents the solid angle determined by the intersection of the inlet
and outlet apertures of the collimator (see fig.4.18). Wherase, the penumbra
was evaluated by the intersection of the inlet aperture of the channel and the
outlet aperture of the collimator.
The tally cell was surrounded by a Dxtran sphere (see for example 4.19),
79
4. The design of a PGNAA facility at Triga Mark II reactor
Table 4.9: Radius (cm) of the sections, at the sample position, of the optical
zones introduced by the collimator, that is umbra, penumbra and halo.
of the fast component in the halo region of a factor four; the most important
for the detector shielding purpose; moreover it assures a thermal neutron flux
at the measurement position (in the umbra) slightly higher than B. By these
consideration the collimator C was chosen, with the further advantage that
its implementation requres a lower amount of material to be inserted in the
channel.
To get a better shielding of the germanium detector the collimator C was
extended forward keeping the convercence of its inner surface. Then a new
pierced block 30 cm long, made up of 10 cm of iron and 20 cm of lithium
polyethylene was implemented outside the reactor along the beam axis fig.4.19
The radii of the three different zones due to the collimator were geometrically
Figure 4.19: External extention of the C collimator. The blue zone represents
the halo of the collimator.
defined and the new values are reported in table ??. The divergence of the
beam was considerably reduced and the radius of the halo was about 3.4 cm
in place of the previous 10.94 cm. The thermal neutron flux at the sample
position, with this new collimator configuration, was reduced by a very low
factor (less than 1%). The values for the umbra region, evaluated without the
filters in the channel, are summarized in table 4.11
Therefore the collimator in fig.4.19 was considered as the definitive solution.
80
4.3. The facility design
Table 4.10: Radius (cm) of the sections, at the sample position, of the opti-
cal zones introduced by the extended C collimator (fig.4.10) , that is umbra,
penumbra and halo.
Table 4.11: Unfiltered neutron flux n/(cm2 s) for the three neutron components
at the measurement position obtained with the extended collimator.
The simulations performed to design the shields and the beam catcher
required the shift of the neutron source from the core to a surface close to the
beam port (see § 4.2.2). The neutron source was determined in absence of
filters in the channel, to be conservative.
The different steps performed in the beam chatcher design included:
• The design of a structure able to absorbs the primary beam; for this
purpose the tally flux were expolited during the simulations;
81
4. The design of a PGNAA facility at Triga Mark II reactor
Radiation Q factor
Photons 1
Neutrons
(En < 500 keV) 5
( 0.5 MeV< En < 1 MeV) 10
( 1 MeV< En < 2.5 MeV) 13
( 2.5 MeV < En < 20 MeV) 20
Table 4.12: Quality factor for photon and neutrons used to calculate the dose
equivalent in the design of the beam catcher of the PGNAA facility; the values
for neutrons depend on the energy range.
Figure 4.20: Position of the first tally cells used to evaluate the characteristics
of the unfiltered neutron beam that must be stopped.
spectrum in the position along the beam axis where the beam stop should
start. The caracteristics of the beam in this position determine the absorbing
materials to be used. A constraint in the beam stop development (shape and
dimention) was imposed by the available space, reduced by the thermal column
shutter when it is opened. Thus this geometrical information was implemented
in the MCNP file.
The unfiltered neutron flux was calculated at the tally cell. This gave the
information about the neutron beam that must be stopped; the results are
summarized in table 4.13
To stop the beam a cylindrical structure, 30 cm diameter and 120 cm long
was implemented (see fig.4.21), made up of a first layer of lithium carbonate
(Li2 CO3 ) and alternating layers of iron (10 cm thick) and borated concrete
82
4.3. The facility design
Table 4.13: Neutron flux evaluated at 106 cm far from the outer reactor wall,
in void channel setup.
(0.16% mass of 10 B) (20 cm thick). The first layer stops effectively the thermal
neutron component of the primary beam, avoiding also the activation of the
iron layer located after. Whereas, the following layers thermalize the fast
neutron component of the spectrum; the energy of the fast neutrons is firstly
reduced by the inelastic scattering with the iron and successively by the elastic
scattering with the hydrogen, finally, when the thermal range is reached, the
neutrons are captured in boron contained in the concrete.
The fast neutron flux into the cylindrical shielding structure is expected to
decrase exponentially according to the the removal cross section Σr theory (see
chapter 2); since the shield is made up of alternating layers of heavy and light
elements.
φ(r) = SG(r)eΣR t (4.7)
where G is:
AeΣR r
G(r) = (4.8)
4πr2
83
4. The design of a PGNAA facility at Triga Mark II reactor
To verify this a F4 tally cell was positioned for each iron/concrete layer; the
simulations showed the expected trend on the neutron flux (fig.4.22). In par-
ticular, the neutron fluxes at the beginning (tally cell 511) and at the end (tally
cell 515) of the thermalizing structure are reported in table 4.14; an overall at-
tenuation factor of 2.10 · 10−6 was obtained. This value is comparable with the
expected attenuation by applying the formula(4.7) that is equal to 9.75 · 10−7
3
.
Figure 4.22: Simulated fast neutron flux trend within the thermalizing struc-
ture of the beam catcher.
Table 4.14: Neutron fluxes at the beginning (tally cell 511) and at the end
(tally cell 515) of the thermalizing structure.
84
4.3. The facility design
Finally the neutron flux at the end of the cylindrical structure, for different
energy bins, (cell 515) assumed the value showed in table 4.15.
Table 4.15: Neutron flux evaluated at the end of the cylindrical structure.
Structure optimization
The next step dealt with the implementation of a biological shield to be lo-
cated all around the facility in order to ensure an external dose rate lower
than 10µSv/h. For this purpose the MCNP geometry was complemented by
the designed collimator and a massive borated concrete structure all around
the already described cylindrical shield. The position of the germanium de-
tector was also fixed at 15 cm (sample-detector distance) and a lead cilinder
4 cm thick was positioned along its axis. This set up was gradually modified
by monitoring the γ dose-rate at the external wall of the facility. For this pur-
pose, 24 tally cells, 5 cm thick, filled with soft tissue (ICRU44), were placed
all around the structure (see fig.4.23); 4 on the roof, 8 at the outside wall near
the detector dewar, 9 at the opposite wall and 2 at the wall ortogonal to the
beam axis. A coupled neutron/photon transport was simulated and a tally F6
for both neutrons and photons were request within the tissue cells.
The beam catecher design that gives the best results is shown in fig.4.23,
and its dimentions are summarized in table 4.16.
85
4. The design of a PGNAA facility at Triga Mark II reactor
Figure 4.23: MCNP reconstruction of the beam catcher; the pink rectangulars
located around the outside wall are the soft tissue tally cells used to evaluate
the dose rate.
As can be seen in fig.4.23 the dewar of the germanium was moved back
from the crystal, and a concrete shield was placed all around the dewar. The
layers of iron and lithium polyethylene located in the surrounding of the de-
tector worked as a thermalizing structure for the fast neutron; A cavity in the
thermalizing structure was inserted to get a further reduction of the fast flu-
ence on the germanium, in table 4.17 the dimentions of the cavity are shown.
86
4.3. The facility design
Cavity
Lenght 46 cm
Width 17.5 cm
Height 30 cm
For the final set up, the simulated annual fast neutron fluence on the detector,
evaluated considering 750 working hours per year was equal to 2 · 1010 n/cm2 in
absence of filters in the channel; considering the attenuation factors introduced
by the filters the fast neutron fluence becomes 2.2·109 n/cm2 . This value is still
higher than the desirable value since a fast neutron fluence of 1010 n/cm2 was
estimated as the maximum limit above which the detector is damaged (see §
2.3.1). Nevertheless it must be considered that the studies about the detector
damages were carried out by using a unmoderated 252 Cf source; this source
provides a fast neutron spectrum with the most probable energy value of 0.77
MeV and the average energy about 1.98 MeV. When the simulated neutron
beam is considered, the average energy of the fast neutron component (rang-
ing between 500 keV and 20 MeV) was estimate being about 0.37 MeV, lower
compared to the one provided by a 252 Cf source, therefore can be assumed
that a less important damage is induced by fast neutron component of the
simulated PGNAA neutron beam. For this reason the structure designed can
be considered efficacy in shielding the crystal from the fast neutron.
A shield for the thermal neutrons was also implemented to protect the de-
tector, in particular a 2 mm thick layer of lithium carbonate (Li2 CO3 , 16%
6
Li mass enriched) was used to line the external holder of the germanium (see
4.24). Indeed, when the low energy neutrons interact with the crystal, they
are captured in Ge isotopes producing prompt and decay γ rays. The relative
intensities of the Ge detector peaks are different from those produced by a Ge
sample, due to the true-coincidence summing effect occurring with the gamma
ray cascades inside the detector. A 596 keV peak in the background is an in-
dication of the crystal activation [21]. The thermal neutron flux in the active
volume of the crystal is lowered by a factor of about 10−2 , bringing its mean
value 62 n/(cm2 s).
The neutron and γ dose rates obtained in the soft tissue cells located outside
the beam catcher, in its final configuration, range between 0.04 (in the frontal
wall) to 5.8 µSv/h remaining below the limit value of 10 µSv/h; in particular
the values for the tally cells showed in fig.4.23 are collected in table 4.18. The
highest dose value is in the zone where the primary beam is stopped within
the first layer of the cylindrical beam catcher (tally number 10 in fig.4.23).
87
4. The design of a PGNAA facility at Triga Mark II reactor
Table 4.18: Dose rate at the outside wall of the final beam catcher design; the
position of the numbered tally cells is shown in fig.4.23
To simulate the response function, a pulse height energy tally (F8) was
88
4.4. The simulation of the germanium response function
set within the active volume of the crystal. The cross section data for the
germanium isotopes used for Monte Carlo simulations 5 are shown in fig.4.25
The energy interval of the simulated spectra was set between 0 and 2.3
5
Data available from Evaluated Nuclear Data Files (ENDF) library http://www-
nds.iaea.org/exfor/endf.htm and kindly converted in a format readable by MCNP (ACE), by
Doct. Manuel L. Sztejnberg Gonçalves - Carralves, Comisión Nacional de Energı́a Atómica,
CNEA, Buenos Aires, Argentina, using NJOY program (http://t2.lanl.gov/codes/).
89
4. The design of a PGNAA facility at Triga Mark II reactor
Figure 4.25: Neutron cross section for the Ge isotopes; that, listed by higher
isotopic abundance, are: 74 (green), 72 (purple), 70 (light green), 76 (red), 73
(blue).
MeV, firstly a fine energy bin division was chosen, equal to 0.3 keV/ch, and
the gaussian energy broadening option (GEB) was used to simulate the normal
peak broadening occurring with a physical detector. This broadening is simu-
lated by MCNP sampling the tallied energies from a Gaussian distribution:
E−E0 2
f (E) = Ce−( A
)
(4.9)
90
4.4. The simulation of the germanium response function
22
Comparison between simulated and experimental spectra of a Na
radioactive source
A 22 N a source was used to evaluate the detector efficency at the 511 keV, that
could be approximately similar to the efficeny for the 478 keV boron peak. The
same source was successively simulated and the results between simulation and
experiment were compared.
The real detector was covered by a lead empty cilinder, 4 cm thick and the
22
N a radioactive source was located 15 cm far from the endcap of the detector
on its axis, in order to reproduce the design condition. The spectrum obtained
with 350 s of live time acquisition is shown in fig.4.26. In the spectrum the
511 keV and the 1275 keV full energy peaks emitted by the radioactive source
are visible; by using these two peaks for the calibration procedure a value of
15.28 keV/ch was obtained.
The same measurement was simulated by MCNP; a similar efficiency was
obtained. In fig.4.27 the simulated and experimental spectra were compared.
To perform the comparison the room background spectrum was subtracted
from the experimental one, since the MCNP cannot consider that contribution.
A good agreement betweem the two the spectra was obtained.
91
4. The design of a PGNAA facility at Triga Mark II reactor
Figure 4.27: Comparison between the simulated (black) and experimental (red)
spectra.
The beam background was simulated firstly without the sample, succes-
sively a D2 O sample was introduced in order to evaluate the enhancement
of the background due to the scattering of the sample. Indeed, the neutrons
undergoing scattering in the sample, interact with the surrounding material
increasing the background signal. The use of heavy water as scattering sample
prevents the 2.2 MeV capture gamma rays production, occurring in light water.
92
4.4. The simulation of the germanium response function
card] together with the F4 tally within the active volume of the detector al-
lowed defining the region of the beamcatcher where the 478 keV γ-rays came
from 6 . In particular, the first borated concrete wall encountered by the pri-
mary beam, located just after the polyethylene shield (region in green color in
fig.4.30), was identified as the boron peak source. Thus the boron in concrete
was replaced with Li (0.48% percentage mass of 6 Li) in the amount corre-
6
FCn is followed by cell identificators; when a particle track leave the designed cell it is
“flagged“ and its contribution to the tally is recorded separately.
93
4. The design of a PGNAA facility at Triga Mark II reactor
sponding to the macroscopic cross section of the borated concrete. After this
modification, the simulated response function of the germanium detector was
deprived of the boron peak, as shows fig.4.31, the intensity of the hydrogen
and the annihilation peaks remained unchanged.
The origin of the 2.2 MeV γ rays is clearly due to the thermal neutron
capture in hydrogen present in the polyethylene; thus a lithium absorber, con-
sisting of a 2 mm Li2 CO3 (6 Li 0.666% mass percentage enriched), was used
to line the beam tube and the sample region in order to capture those neu-
trons scattered by the sample that may interact with the lithium polyethylene
(fig.4.30). The new beam-beackground is shown in fig.4.32; the intensity of
2.2 MeV full energy peak was decreased, with a consequent lowering of the
baseline; 511 KeV peak is the only one remaining.
A further investigation of the beam-background spectrum was carried out
by introducing a heavy water sample (1 ml), cilindrical shape, inclined by 45o
with respect to the beam line; the resulting spectrum is shown in fig.4.33, in
comparison with the beam background spectrum obtained in absence of sample
and without any structural improvements. The comparison of the two spectra
showed the effectiveness of the modifications implemented in the facility in
decrasing the background count rate, expecially in the region of boron and
hydrogen peaks.
94
4.4. The simulation of the germanium response function
95
4. The design of a PGNAA facility at Triga Mark II reactor
96
4.4. The simulation of the germanium response function
Table 4.21: Count per second under the boron peak for different spectra.
obtained by averaging the counts at right and left of the boron peak, only one
bin at each side was included. A sensitivity for natural boron of about 1033
cps/mg was obtained.
This value was compared to the one expected by applying the analytical
formula for the sensitivity (see chapter 2):
NA
S= σγ,0 Φ0 ε(E) (4.11)
M
the corresponding description and value of the parameters are collected in
97
4. The design of a PGNAA facility at Triga Mark II reactor
Table 4.22: Definition and value of the parameters used to calculate the sen-
sitivity.
table 4.22
By using the 4.11, the calculated reaction rate (number of reactions per sec-
ond) occurring for 1 mg of pure natural boron is 49.78 · 104 s−1 ; if a value of
2.1 · 10−3 is assigned to the detector efficency for the 478 keV region 7 , a sensi-
tivity for natural boron of about 1045 cps/mg can be estimated; this value is
comparable with the previous one.
The detection limit for boron (DL ), that is the smallest amount of boron
that gives rices to a true signal visible in the background, according to the Cur-
rie definition [32], was evaluated by the forumla already described in chapter
2: �
3.29 Rb
DL = (4.12)
S t
By using a sensitivity (S) of 1033 cps/mg and a background count rate, Rb =
13cps, given by the sum of the background count rate for the hydrogenous
blank sample and for the room, the detection limit for t=1000 seconds of live
time irradiation is 363 ng of natural boron, equivalent to a DL for 10 B equal
to 73 ng. With these value a detection of boron concentration of the order of
1 ppm, in sample of 0.5 ml and with irradiation times of few minutes can be
achieved.
7
The efficency for the 478 keV γ rays of the HPGe was estimated by the simulation,
that is extracting uniformly the 478 keV γ ray from the sample position and evaluating the
number of those counted by the detector.
98
4. The design of a PGNAA facility at Triga Mark II reactor
100
Chapter 5
Conclusions and future
perspectives
101
5. Conclusions and future perspectives
Figure 5.1: MCNP plot of the horizontal section of the Triga Mark II reactor
of the University of Pavia; the PGNAA facility was designed in the horizontal
B channel.
on 50 cm from the wall of the reactor, is about 107 n/(cm2 s) for the thermal
component, and the epithermal and fast neutron flux is about 105 n/(cm2 s).
With these values, the beam can be considered enough clean and potentially
able to provide a quick evaluation of 10 B-concentration of the order of ppm
required for BNCT purpose by the prompt gamma spectroscopy.
102
Further precaution was used with the aim to decrase the background; a
shield of enriched lithium carbonate, 2 mm thick, was implemented along the
beam tube, in the surroundings of the irradiation position, in order to absorb
scattered thermal neutrons that may be captured in hydrogen of the shield
materials and give rice to a strong 2.2 MeV γ signal in the germanium detector.
The massive borated concrete used as biological shield was also a source of 478
keV γ rays; the replacement of the boron with the lithium, preserving the
same macroscopic absorption cross section, in the concrete wall that faces the
irradiation position, prevents most of the 478 keV signal background.
Next to the measurement position, an absorbing structure is required in
order to stop the beam, properly shielded to fulfill the radiation protection
indications. A cylindrical structure made of different materials in-axis with
the beam was implemented to stop the primary beam. It consists of a Li2 CO3
disk containing 1.22% (mass fraction) of 6 Li, to absorb the thermal neutrons
followed by an alternating layers of iron and borated concrete to thermalize
the fast neutrons (>1MeV) and then to absorb them. A massive structure
made of borated-concrete surrounds all the components of the facility, it was
designed to ensure an external dose rate lower than 10µSv/h.
Figure 5.2: Horizontal section of the PGNAA facility. Two filters was imple-
mented in the channel B: a bismuth block and a sapphire single crystal; all
the other components are: a convergent collimator, a HPGe detector, a beam
catcher.
For the projected facility, a sensitivity for natural boron in a light water
matrix of about 1033 cps/mg was estimated by the simulations. The detection
limit for natural boron, that is the minimum detectable mass, is about 363
ng, obtained considering a background count rate under the boron peak, of
about 13 cps (counts per second). This value of the background comes from
the counts per second under the boron peak obtained by the irradiation of a
light water sample, and the room background spectrum measured in the reac-
103
5. Conclusions and future perspectives
tor hall by the HPGe that will be used for the gamma spectroscopy. With this
facility, a detection of boron concentration of the order of 1 ppm, in sample of
0.5 ml and with irradiation times of few minutes will be possible.
The construction of the facility is scheduled for the near future; most of the
materials required to built the facility were purchased (sapphire crystal and
bismuth blocks). Some practical aspect of the facility construcion are still un-
der study, for example, the sample positioning system and the implementation
of a shutter. This device system, in particular concerning the turning on and
off the beam, will allow replacing the sample without the need to shutdown
the reactor.
104
5. Conclusions and future perspectives
106
Bibliography
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(BNCT).A review Fresenius J Anal Chem 364 (1999), 391-403.
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the czeck BNCT Project, AIP Conference Proceeding (2000).
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[14] Database of Prompt Gamma Rays from Slow Neutron Capture for Ele-
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[21] Knoll G.F.; Radiation Detection and Measurement, 1989 Jhon Wiley and
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[26] SRIM - The Stopping and Range of Ions in Solids, by J. F. Ziegler and
J. P. Biersack 2010
[28] Rene Brun and Fons Rademakers, ROOT - An Object Oriented Data
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1996, NIM A 389 (1997) 81-86. See also http://root.cern.ch/.
[29] L.S. Waters (Ed.), MCNPX USER’S MANUAL Version 2.1.5, Los
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[46] T.E. Booth, A Sample Problem for Variance Reduction in MCNP LA-
10363-MS (October 1985).
[47] S. Bortolussi and S. Altieri Thermal neutron irradiation field design for
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List of publications
7-8, (2009),S332-S335.
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List of publications
tumor cells via upregulated LDL transporters, Chem. Eur. J. 17, 8479-
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List of publications
116
Aknowledgments
My first thanks goes to my supervisor Saverio Alteri for supporting and en-
couraging me during these years, thank you for the possibility you gave me to
work with your group!
I am grateful to Kent Riley for the time he spent to read my thesis, for his
corrections and suggestions.
I want to thank all my group for the frendly and collaborative work atmos-
fere that I have always found. Thanks to Silva for her friendship and for her
constant enthusiasm in each occasion; thank you for helping me many times
both in professional and in personal issues, with you I found not only a great
collegue but also a sincere friend! Thank you Nicoletta for sharing with me the
”thesis writing” syndrome and for being a great neighbour; thank you for your
friendship and you helpfulness whenever I asked you! Thank you Francesca
for the time we spent together, good luck for your new adventure! Thank you
to Piero Bruschi, grazie per la tua disponibilitá e per le discussioni in labo-
ratorio sui temi piu’ svariati. Many thanks also to the medical and biology
staff; James, Cinzia, Anna and Celicia. Thankyou to all the guys with whom I
shared the office: thankyou to Mario and Ruben for their wonderful alfajores,
thankyou to Concetta and Alessia, it was nice and productive working with
you! And thanks to Ian, goodluck for your thesis!
Sincerely thanks to Dick Lindstrom, Greg Downing e Liz Makey for receiv-
ing me at NIST with such enthusiasm, it was an honour for me meeting you!
Thank you for the time you spent with me explaining many things and intro-
ducing me many persons, you made me feel immediately part of the group.
Thankyou to Jeremy for his precious hint about Monte Carlo simulation.
Many thanks to the guys with whom I shared the breck time at NIST, you
were precious! Thanks to Russel, Richard, Shruthi, Dmitry, special thanks to
Sophia for all the nice time we spent together chatting, roaming in Washington
and shopping, without you my period in USA would not be so fun! Finally
many many thanks to Cinthia for welcoming me with open harms at her house.
I want also to thank all the guys that work at LENA; un grazie particolare
a Michele per avermi telefonato tutte le volte che la mia macchina rischiava di
rimanere bloccata al parcheggio!
117
Aknowledgments
Many many thanks to all the friends I met in the department: Susanna,
Luca, Lorenzo, Davide, Francis, Alessandro, Jacopo, Andrea; grazie a Claudio
per aver sventato tutti i possibili cali di zucchero con i tuoi fantastici dolci da
tutto il mondo, continua cosi!
Grazie infinite alle irriducibili Laura, Giusi e Mary, grazie per esserci sem-
pre tutte le volte che torno nella mia Martano! Grazie mille “cumare“ per
le lunghissime telefonate spese a parlare dei nostri progetti sempre con tanto
entusiasmo, grazie per essere sempre un punto di riferimento tutte le volte che
ho bisogno di sfogarmi.
Infine devo ringraziare tutta la mia famiglia allargata per avermi sostenuto
ed aiutato tutte le volte che ne ho avuto bisogno, aiutandomi a conciliare il
mio corso di dottorato assieme all’importantissimo ruolo di mamma; senza di
voi, questa bella esperienza non sarebbe stata possibile! Grazie a Lucia e Luigi
per esservi precipitati a Pavia tutte le volte che sono dovuta partire, siete dei
nonni fantastici! A voi, papá e mamma l’ennesimo grazie per aver appoggiato
e sostenuto in tutte le mie scelte, per essermi sempre stati vicino e per avermi
infuso costantemente il coraggio e la fiducia che servono per percorrere il tor-
tuoso e affascinante viaggio che é la nostra vita!
Grazie ai nonni per il loro calore e per la loro saggezza.
Grazie a Maria Chiara e Francesco, per avermi accolto sin da subito come una
sorella. Grazie mille a tutti voi cari fratelli, per le risate, le discussioni, per i
pranzi a casa mia, per le chiaccherate al telefono del piu e del meno...grazie
Antonio, Marco, Simone e Fabrizio, non cambiate mai!
Un grazie infinite alla mia piccola Elisa che ha stravolto e arricchito la mia
vita; grazie per la tua pazienza e per tutte le volte che mi hai staccato la spina
del computer dicendo ”mamma basta sudiare!”. Grazie mille al mio Antonio
per tutto l’amore, il sostegno e la fiducia che hai sempre saputo darmi! A voi
due, Elisa ed Antonio, grazie per esserci!
118