Monte Carlo Methods Final Project December 5, 2016 *

Estimating Ion-Irradiation-Induced hardening of Nuclear Fuel Clad

Using SRIM: Comparison Between Zircaloy-4 And AISI 348
Ahmed ElMallah

Abstract
Better mechanical properties of AISI 348 against Zircaloy-4 indicate that AISI
348 should have better performance under irradiation by heavy ions than
Zircaloy-4. This was tested using the SRIM code, which was used to predict defect
production in Zircaloy-4 and AISI 348. It was found that the number of
displacement per ion is slightly higher for AISI 348 than Zircaloy-4. However, it
was also found that defects, such as interstitial atoms, ions, and vacancies have
higher penetration depth in Zircaloy-4 than AISI 348. These two findings proved
that AISI 348 have less radiation hardening overall than Zircaloy-4.

Zirconium-based cladding has been the
favorite choice for nuclear fuel cladding for
some decades now, mainly due to its low
absorption cross section for thermal
neutrons, high corrosion resistance, as well as
many other favorable physical character-
istics. Moreover, the current zirconium-based
alloys have been optimized by means of
changes in the alloy composition to reduce
hydrogen pickup while limiting detrimental
irradiation effects compared to first
zirconium-based alloys. Nevertheless, on
accident conditions, these alloys experience
severe degradation by rapid oxidation of
zirconium at temperatures greater than
1200oc, which results in the production of
high amounts of hydrogen that might lead to
the explosion of the reactor building, as
witnessed in Fukushima Daiichi Nuclear
Plant accident in March 2011. [1]
The susceptibility of zirconium-based
cladding in the Loss of Coolant Accident
(LOCA) events have raised concern about its
safety and have stimulated efforts to develop
a more accident tolerant fuel (ATF) that
would tolerate active loss of cooling for a
considerably longer period while maintaining
or improving the fuel performance during
normal operations. One good alternative to
zirconium-based alloys is austenitic stainless
steels. In fact, the austenitic stainless steel
304 was used as cladding material in the first
PWR (Pressurized Water Reactor) registering
good performance. However, it was later
replaced by zirconium-based alloys, which
have shown better performance over the
relatively simple austenitic steel. Yet,
deficiencies of the early austenitic steels were
mitigated with the development of the AISI
347 and 348, and attention has been brought
back to these alloys as a potential ATF
cladding choice. [1]
Performance improvements in stainless
steels, which include corrosion resistance,
high-strength and other mechanical and
thermal properties were achieved by the
addition of stabilizing elements, changes in
the chemical composition of major or minor
elements, modifications in the metallurgical
structure as well as greater care in their

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 Monte Carlo Methods Final Project
fabrication conditions. Table 1 (tables are
available in the appendix) shows a
comparison between mechanical properties of
Zircaloy-4 and AISI 348. The table shows that
AISI 348 has higher ultimate and yield
strengths compared to Zircaloy-4, which is
indicative of higher mechanical performance.
Additionally, the table shows that AISI 348
present a total creep under irradiation that is
about 7 times less than that of Zircaloy-4. [1]
In addition, a detailed evaluation of stainless
steel clad for use in LWRs have concluded
that the performance of stainless steel in
PWRs is comparable to or better than that of
zircaloy. [2]
Chemical compatibility with other reactor
core components, melting temperature,
thermal conductivity, thermal neutron cross
section, manufacturability, gas retention and
radiation performance are all important
aspects to be considered when looking for
alternatives to current clad materials.
However, the focus of this paper will be the
estimation of radiation damage in clad
material done by highly energetic heavy ions
produced during fission, specifically the
radiation hardening effect. The interaction of
energetic particles with materials results in
the production of atomic scale defects from
ballistic collisions. [3] These defects harden
a material because they restrict the motion of
dislocations. This motion is what makes a
material ductile. [4] Therefore, examining
defect distributions should allow us to
evaluate ion-irradiation-induced hardening
of the materials under consideration.
The evaluation of defect production in
clad material under ion irradiation is going to
be done using the TRIM (Transport of Ions in
Matter) module of the SRIM software. TRIM
describes the range of ions into matter, as
December 5, 2016 *
well as detailing defect production in an
irradiated material. [5] The results are going
to be used to compare between zirconium
based alloys and austenitic stainless steel,
specifically Zircaloy-4 against AISI 348. Its
expected that AISI 348 will show better
performance under irradiation by heavy ions
than Zircaloy-4 since available data indicate
that AISI 348 has better mechanical
properties and generally perform better
under irradiation.
TRIM is a binary collision Monte-Carlo
calculation that works by following the ion
into the target, making detailed calculations
of the energy transferred to every target atom
collision. Almost every time the ion has a
collision with a target atom, the atom is
knocked out of its lattice forming what is
known as a primary knock-on atom (PKO)
and one vacancy is created. The PKO atom
then gains energy and recoils, leading to the
production of more recoils, known as
secondary knock-on atoms (SKO) and more
vacancies. A single recoil atom may cause up
to 1000 vacancies. [5] After the ion and target
recoil atoms lose their energies, they become
interstitial atoms in the target. They restrict
the motion of native atoms increasing the
hardness of the material. Similarly, vacancies
that result from the process deform the
material restricting the motion of target
atoms. The target recoils might fill some of
the vacancies, but most of the time they end
up as being interstitial atoms. Therefore, its
equally important to have information about
ions, vacancies, and recoil atoms distribution
to be able to evaluate radiation damage to the
target in more detail. It should be noted that
the results of TRIM calculations are
normalized over ion dose. To get exact
impurity concentrations, we can multiply by
implantation dose (ions/cm2), which would be
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 Monte Carlo Methods Final Project
a function of fission rate, ion yield, source
depth, and irradiation time. Luckily, this will
not be needed for our comparison.
TRIM only allows for the simulation of
one isotope at a time. For each simulation, the
number of ions irradiating the target is
specified by the user. Typically, a calculation
for 1000 ions will give better than 10%
accuracy. [5] However, in order to reach more
accurate results, at least two times as much
ions were specified for each of the following
simulations. Unfortunately, simulating such
many ions requires a lot of computational
time, and thus only one isotope was used for
the assessment of radiation damage by heavy
ions. The selected isotope was Xe-140, which
is one of the most probable fission products.
According to one reference, Xe-140 is emitted
with energies that range between 40 - 80
MeV. [3] TRIM GUI normally allows one fixed
ion energy to be simulated. However, its also
possible to simulate ions starting with
varying energies, angles, and depths using an
external file that contains initial information
about the simulated ions. Therefore, it was
assumed that Xe-140 ions are emitted with
energies that vary uniformly between 40-80
MeV, and Matlab was used to randomly
generate these energies. Additionally, all ions
were assumed to be emitted in the same
direction toward the target.
Specifying the target information in
TRIM is much simpler, as long as the
chemical composition and densities of the
target materials are known. The weight
percent of the atoms composing each of the
Zircaloy-4 and AISI 348 was readily obtained,
and then this information was used to
calculate atom stoichiometry to be specified
in TRIM. The composition of Zircaloy-4 and
AISI 348 are shown in tables 2 and 3. The
December 5, 2016 *
only remaining information to be specified is
the target depth, which depends on the
experimental setup. Two different setups (or
two different simulations) were conducted for
each of the two clad materials under
consideration. The first involved simply
irradiating a target of clad material with the
heavy ion emitted from the surface of the
material. This might resemble a fission
reaction taking place on the surface of the
fuel with the fuel directly in contact with the
clad. Another more realistic setup involved
simulating ions emitted a few microns deep in
the UO2 fuel toward a helium gap (0.08 mm)
before finally reaching the clad. The first
setup was used to obtain a quick estimation
of defect production, while the second was
used to obtain a more detailed information
about damage, which was found to include
sputtering and surface mixing.
Before starting our simulations, SRIM
Quick Range Table tool was used to estimate
the Xe-140 projected range in UO2, Zircaloy-
4, and AISI 348. This tool quickly creates
tables of the stopping and range of ions in
matter over a wide band of ion energies.
These tables are useful to set up the TRIM
program so that the target thickness is
adequate to contain all the ions. For the first
experimental setup, the target depth was set
to be 7 m for AISI 348 and 10 m for
Zircaloy-4. The damage calculation method
used for this setup was the Ion Distribution
and Quick Calculation of Damage option.
The damage calculated with this option will
be the quick statistical estimates based on the
Kinchin-Pease model. It provides an accurate
final distribution of ions in the target,
Ionization energy loss by the ion into the
target, and Energy transferred to recoil
atoms. However, it wont show details of
target damage or sputtering.
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 Monte Carlo Methods Final Project
After running the simulation for 10,000
ions the following results were obtained: The
projected range of Xe-140 in Zircaloy-4 is 6.40
m with longitudinal straggling (standard
deviation) of 9000 and the lateral projected
range is about 6000 with 7500 straggling,
while the projected range of Xe-140 in AISI
348 is 4.66 m with longitudinal straggling of
6000 and the lateral projected range is
about 3400 with 4300 straggling. A
summary of this data is found in table 4. In
simpler words, the Xe-140 ions reach deeper
and wider into Zircaloy-4 than AISI 348. The
distribution of ions in the target as a function
of depth is shown in figure 1. Both
distributions were found to have Gaussian
shapes with the straggling being less than
15% of the depth. Note the ordinate units:
(Atoms/cm3)/(Atoms/cm2). That is the atom
concentration normalized over the ion dose
(ions/cm2). Therefore, the area under curves
is equal to unity.
Figure 1: Ion Distributions in Clad
Additionally, the simulation results have
shown that 61,548.3 vacancies per ion is
created on average in the Zircaloy-4 target,
while only 57,300.8 vacancies per ion created
in the AISI 348 target. The distribution of
December 5, 2016 *
vacancies with respect to depth is shown in
figure 2. The area under both curves
corresponds to the number of vacancies per
ion. The figure shows that vacancies are more
deeply spread in Zirconium-4 than AISI 348.
It also shows that most vacancies are caused
by recoil atoms knocking off more target
atoms than by incident ions. In fact, incident
ions tend to lose most of their energies
interacting with target electrons rather than
interacting with recoil atoms, as shown in the
following paragraph. In conclusion, the
vacancies per ion in Zirconium-4 is higher
than that of AISI 348. Additionally, the
defects (Ions & Vacancies) penetrate further
in Zirconium-4. This would indicate that AISI
348 have less radiation hardening overall.
Figure 2: Vacancies distribution in Clad
In addition to the results shown above,
TRIM simulation shows how the energy of the
incident ions is dissipated inside the target.
This information might be less important for
the evaluation of irradiation-induced
hardening done to the target. However, it
might be interesting to know that for both
targets the ions lose about 89% of their
energy directly to the target in the form of
ionization, which appears as heat in case of
metal targets. The electrons tend to absorb
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 Monte Carlo Methods Final Project
energy most efficiently from particles whose
velocity is similar to their velocity. The ions
are moving much faster than the recoiling
target atoms, so the ions lose more energy to
the target electrons. [5] The other 11% are
transferred to the recoil atoms, which lose
half of this energy to ionization and half of it
to phonons1. Phonons energy can also be
assumed to be added directly to target
temperature. [5] A negligible amount of the
energy of the ions is lost directly to phonons.
Now, that we have a rough idea of how ion
radiation damage in Zirconium-4 compares to
AISI 348 we can add some reality to the
simulation and use the more detailed
Calculation with full Damage Cascades
TRIM option. This option tracks the incoming
ions, as well as every recoil until it stops.
Hence all collisional damage to the target is
analyzed. For these simulations, we are going
to consider a typical PWR fuel element such
as that shown in figure 3. However, we are
only interested in ions that penetrate through
the fuel pellet to the clad. Therefore, we are
going to assume that our ions can be emitted
uniformly anywhere within 2 m of the fuel
surface. Again, this was done by using a
Matlab code the randomly generated 2500
ions with energies ranging between 40-80
MeV and depths of 0-2 m. The first layer of
the target is a 2 m of UO2 (5% enriched). The
fuel was assumed to be fresh (i.e. no creep),
and thus a depth of 80 m of helium gas was
specified for the second layer. Finally, 10 m
of clad material formed the third layer. To
save computational time the plotting window
was set to only count events taking place in
the clad and the last 2 m of the helium gap.
1 Phonons are energy stored in atomic vibrations in a crystal.
December 5, 2016 *
Figure 3: Nuclear Fuel Element
After running the simulation for 2500
ions the following results were obtained: The
projected range of Xe-140 in Zircaloy-4 is 5
m with longitudinal straggling of 3.18 m
and the lateral projected range is about 4.46
m with 8.15 m straggling, while the
projected range of Xe-140 in AISI 348 is 3.7
m with longitudinal straggling of 8000
and the lateral projected range is about 4.27
m with 7.14 m straggling. The summary of
these results is shown at table 5. The ions had
to travel through two layers before reaching
the clad material. Hence, we are observing
shallower longitudinal range and wider
lateral range than the previous simulation
setup. Otherwise, the results show good
agreement with the previous simulations, i.e.
Xe-140 ions reach deeper and wider into
Zircaloy-4 than AISI 348.
The simulation results also show that
114,161 vacancies per ion out of 120,194
displacements per ion are created on average
in Zircaloy-4, while 119,465 vacancies per ion
out of 123,432 displacements per ion are
created in the AISI 348 target. Displacements
include vacancies and replacement collisions
as shown in the equation:
displacements = vacancies + replacement collisions
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 Monte Carlo Methods Final Project
These estimations are twice as high as these
calculated by the Quick Calculation
method. The change in the number of
vacancies should be expected since first
results were merely statistical estimates.
Additionally, the numbers shown above also
include the vacancies produced in the last 2
microns of the gap. However, these are so
small and can be neglected, and we can claim
that almost all the vacancies produced per ion
shown above are produced in the clad layer.
The distribution of vacancies with respect to
depth is shown in figure 4. The plots agree
qualitatively with these obtained by the
Quick Calculation method, but the peaks
are twice as much higher. They show that
vacancies are more deeply spread in
Zirconium-4 than AISI 348. Again, the figure
shows that most vacancies are caused by
recoil atoms knocking off more target atoms
than incident ions.
Figure 4: Vacancies Distribution in Clad
In addition to providing the distribution of
incident ions inside the target materials, the
Full Damage Cascades method provides the
distribution of all recoil atoms that come to
rest inside the target. These two kinds of
December 5, 2016 *
atoms, incident ions, and recoil atoms, count
as interstitial atoms, which are part of the
defect built in the target material by
radiation. The distributions of interstitial
atoms are shown in figure 5 and 6. The area
under the ion distribution curves equals
unity, while the area under the target recoils
distribution curves corresponds to the
displacements per ion if the number of atoms
leaving the target is negligible, which is the
case as shown in the next paragraph. The
exact relation between displacements and
interstitials is shown in the equation:
Displacements = Interstitials + (Atoms leaving the target)
The main difference between the target
materials is that peaks in AISI 348 are
shallower, thinner, but taller, while in
Zircaloy-4 they are deeper, wider but shorter.
Otherwise, both plots show that the main
contributor to interstitial atoms is the target
recoil atoms. Also, it is noticed that the
distribution of target recoils has a shallower
peak than that for the ions, which could be
explained by the fact that ions do not have
enough energy to create massive cascades
near the end of their tracks. [5]
Figure 5: Interstitial Atoms Distribution in Zircaloy-4
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 Monte Carlo Methods Final Project December 5, 2016 *

Figure 6: Interstitial Atoms Distribution in AISI 348

Another interesting observation is the

existence of interface mixing and sputtering
from the clad surface, as shown in figure 7. It
is noticed that for both target materials some
of the helium atoms (more in the case of AISI
348) are transported from the gap layer 0.16
m deep into the clad layer. This is
undesirable since these atoms act as
interstitial atoms. Additionally, some of the
clad surface atoms are removed by the recoil
cascades that come back out of the clad. This
is known as sputtering. The sputtering of a Figure 7: Interface Mixing and Sputtering Effects
target makes it rough and damaged. It can
rapidly erode the surface if more than 5 atoms original crystalline form. However, there are
leave the surface for each incident ion. [5] A no thermal effects in TRIM, so the damage
separate simulation was run to predict the which is calculated is that which would
number of atoms sputtering, and it was found happen for an irradiation at 0o K. Ignoring
that nearly 0.45 atoms sputter from the thermal effects changes the quantity of final
Zircaloy-4 surface, while nearly 0.8 atoms damage, but the basic damage types remain
sputter from the AISI 348 surface per ion. unchanged. [5] Second, it should be noted
that minimum energy needed for displacing a
Before going into final conclusions, target atom, known as displacement energy,
several remarks should be put down. First, it and the minimum energy needed to remove
should be noted that normally at room an atom from the target surface, known as
temperature most of the ion irradiation surface binding energy, will both decrease as
damage would self-anneal since lattice damage accumulates. This means that once
atoms will have adequate energy to allow you have a partial damage, it is easier to
simple target damage to regrow back into its

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 Monte Carlo Methods Final Project December 5, 2016 *

create more damage because lattice is more

loosely coupled and atoms are easier to References
dislodge. However, these changes in the
1. E. S. Pino, A. Y. Abe and C. Giovedi, "The
crystal integrity are not included in TRIM, so
Quest for Safe and Reliable Fuel
the damage shown above may be
Cladding," International Nuclear Atlantic
underestimated. [5]
Conference - INAC 2015, So Paulo, SP,
The two flaws of the TRIM code Brazil, 2015.
mentioned above will certainly have a huge
2. S. M. Stoller Corporation, "An Evaluation
effect on the accuracy of our results. However,
of Stainless Steel Cladding for Use in
we can reasonably assume that these flaws
Current Design LWRs," 1982.
wont have much noticeable effect on the
qualitative nature of the results, and thus our 3. W. J. WEBER, "Materials Innovation for
comparison should be valid. That being said, Nuclear Optimized Systems," CEA
the results shown above indicate that AISI INSTN , Saclay, France, 2012.
348 will have a better performance under
irradiation by heavy ions than Zircaloy-4. The 4. M. R. Tonks, "Nuclear Materials Lecture
Quick Calculation method have shown that 26: Irradiation Hardening," 2016.
the number of defects per ion, as well as the 5. Z. JF, "Stopping and Range of Ions in
penetration depth of both ions and vacancies, Matter (SRIM) Tutorials," 2013.
is higher in Zircaloy-4. However, these
statistical estimations based on the Kinchin-
Pease model was found not quite accurate
after running the Calculation with full
Damage Cascades. The more detailed
simulation has shown that the number of
defects per ion is slightly higher for AISI 348.
Nevertheless, the penetration depth of ions,
recoils, and vacancies was found higher for
Zircaloy-4. Additionally, interface mixing and
sputtering was noticed. These effects were
slightly more significant for AISI 348 than
Zircaloy-4. However, we have concluded that
sputtering is not significant since less than 5
atoms per ion are expected to leave the clad
surface of both materials. Moreover, the
defects resulting from interface mixing is only
confined within 0.16 m of the clad. All this
allows us to conclude that AISI 348 has less
radiation hardening overall than Zircaloy-4.

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 Monte Carlo Methods Final Project December 5, 2016 *

Appendix:
Table 1: Mechanical Properties of Zircaloy-4 and AISI 348

Property (units) Zircaloy-4 AISI 348

Ultimate Strength (Mpa) 413.000 655.000
Yield Strength (Mpa) 241.000 275.000
Under Irradiation Creep (%) 0.300 0.045

Table 2: Zircaloy-4 Composition2

Zircaloy-4 Alloy: density = 6.55g/cm3

Element M W% N/Na A%
Sn 118.710 1.500 0.013 1.154
Fe 55.845 0.200 0.004 0.327
Cr 51.996 0.100 0.002 0.176
Zr 91.224 98.200 1.076 98.343
100.000 1.095 100.000

Table 3: AISI 348 Composition3

Stainless Steel AISI-348: density = 8 gm/cm3

Element M W% N/Na A%
C 12.011 0.080 0.007 0.365
Cr 51.996 19.000 0.365 20.029
Ni 58.693 11.000 0.187 10.272
Si 28.085 1.000 0.036 1.952
Mn 54.938 2.000 0.036 1.995
Ta 180.948 0.100 0.001 0.030
Co 58.933 0.200 0.003 0.186
P 30.974 0.045 0.001 0.080
S 32.060 0.030 0.001 0.051
Nb 92.906 0.700 0.008 0.413
Fe 55.845 65.845 1.179 64.626
100.000 1.824 100.000

2 http://www.azom.com/article.aspx?ArticleID=7644
3 http://www.azom.com/article.aspx?ArticleID=6800

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 Monte Carlo Methods Final Project December 5, 2016 *

Table 4: "Quick Calculation" Simulation Results

Target Projected Longitudinal Lateral Vacancies

Material Range Straggling Straggling Per Ion
AISI 348 4.66 um 6000 4300 57,300.8
Zircaloy-4 6.40 um 9000 7500 61,548.3

Table 5: "Detailed Damage Calculation" Simulation Results

Target Projected Longitudinal Lateral Vacancies Displacements

Material Range Straggling Straggling Per Ion Per Ion
AISI 348 3.7 um 8000 7.14 m 119,465 123,432
Zircaloy-4 5.0 um 3.18 um 8.15 m 114,161 120,194

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