Annals of Nuclear Energy 142 (2020) 107407

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Annals of Nuclear Energy

journal homepage: www.elsevier.com/locate/anucene

Response function generation for transmutation of Technetium-99 via

high energy proton and neutron interactions in MCNP
Jason A. Hearne
Texas A&M University, Department of Nuclear Engineering, AIEN, 423 Spence St, College Station, TX 77840, USA

a r t i c l e i n f o a b s t r a c t

Article history: This study provides a discretized transmutation rate response function that is consistent with the physics
Received 20 August 2019 models used in MCNPX in order to circumvent a problem with reaction tallies not scoring in the model
Received in revised form 13 February 2020 physics regime. This is used for the estimation of the transmutation rate of 99Tc in an accelerator driven
Accepted 21 February 2020
system containing protons and spallation neutrons with energies up to 1500 MeV. To compute the inter-
Available online 28 February 2020
action response function, a modeling construct consisting of a very small 99Tc target with a mono-
directional neutron or proton source is used. The small size of the target allows attenuation and columbic
Keywords:
energy loss to be ignored for the response function generation process. The transmutation rate responses
Fission products
Transmutation
for a total of 180 neutron energy bins ranging from 8.8 MeV to 1500 MeV and 120 proton energy bins
Cross sections ranging from 1 MeV to 1500 MeV are computed.
High energy protons Ó 2020 Elsevier Ltd. All rights reserved.
Response function
MCNP

1. Introduction The transmutation analysis focuses on modeling the transmuta-

In a computational study of the transmutation of long-lived fis-
sion products using an accelerator (Hearne and Tsvetkov, 2019), it
became necessary to generate a response function for the transmu-
tation rate of 99Tc subject to high-energy proton and neutron fluxes
for use in a tally in MCNPX (Pelowitz, 2011). This response function
behaves very similarly to an interaction cross section, as it relates
an energy dependent particle flux in a medium to the resulting
reaction rate. A response function must be used to estimate the
transmutation rate in more complex targets because MCNPX does
not score interaction tallies in the model physics regime. The inter-
mediate to high-energy neutron and proton cross sections for some
nuclides have been measured experimentally (Sisterson et al.,
2005; Kim et al., 1999), and the cross sections for some low energy
interactions with 99Tc have been measured (Watanabe and Reeder,
1970; Kobayashi et al., 2004), but no measured data for intermedi-
ate to high energy (>20 MeV) interactions with 99Tc exists. Interac-
tion probabilities above the cross section table energy cutoff must
therefore be calculated using physics models (Hendricks, 2003). In
the physics regime of interest here, MCNP models interactions
using a combination of the nuclear optical model, the Cascade Exci-
tation Model (CEM) and the Los Alamos version of the Quark Gluon
String Model (LAQGSM) (Prael et al. 0000; Mashnik et al., 2018;
Mashnik and Kerby, 2014).
E-mail address: jasonhearne@email.tamu.edu
tion of 99Tc using MCNPX and progressively refines the system
involved. Initially an infinite medium of pure 99Tc is modeled, fol-
lowed by a finite Tc target and then a target containing a mixture
of 99Tc and natural lead with a graphite reflector region. The target
geometry was varied to improve the transmutation rate and energy
efficiency, with a general geometric design involving a cylinder
with a beam hole in one face so that backscattered particles from
the incident proton beam will also be caught. The general geometric
design can be seen in Fig. 1. In the pure targets, the number of trans-
mutations occurring can be calculated by taking it to be the same as
the number of protons and neutrons lost to nuclear interactions,
because every interaction results in a transmuted particle. When
the lead spallation target and graphite reflector are added to the
model, this can no longer be done, so tallies must be used.
MCNP has built in tallies to tally the number of interactions by
type and thus the number of transmutations occurring in nuclides
present in the system. These tallies use the FM tally multiplier card
to output the results as a reaction rate rather than a flux. In 99Tc,
any nuclear interaction other than scattering will transmute the
nucleus into a shorter-lived nuclide. Neutron capture, (n,2n), pro-
ton capture, spallation by neutrons or protons, etc. will all result
in the removal of an atom of 99Tc and thus a reduction in the
amount of long lived waste. The 102 capture tally will tally
(n, gamma) reactions for the nuclide specified in the range for
which MCNP has tabulated cross section data. For particles with
energies above the tabulated data range, MCNP uses models to
compute cross sections on the fly to estimate loss rates to various

https://doi.org/10.1016/j.anucene.2020.107407
0306-4549/Ó 2020 Elsevier Ltd. All rights reserved.
2 J.A. Hearne / Annals of Nuclear Energy 142 (2020) 107407
interactions. MCNP’s built in interaction tallies do not score any
interactions in the model cross section regimes, effectively ignor-
ing interactions with particles with energies above the tabulated
data cutoff. Ignoring these interactions can introduce large errors
in a system in which an accelerator is used to produce high energy
protons that transmute 99Tc nuclides both directly and through the
interactions of the resulting spallation neutrons when the neutron
and proton energy ranges reach into the hundreds of MeV. The tab-
ulated interaction data regime in MCNPX for neutrons incident on
99
Tc cuts off at 20 MeV. Therefore, transmutation causing interac-
tion tallies for any proton interaction and any neutron interaction
above 20 MeV will not successfully account for all of the interac-
tions that are occurring within the modeled system.
A custom tally with a response function for specific energy bins
can be used to estimate the number of transmutation causing
interactions. A set of cross section data could be obtained from a
separate model based library, such as the TALYS Evaluated Nuclear
Data Library (TENDL) (Koning et al., 2012; Koning and Rochman,
2012) to use as a response function, but there are some issues.
One issue with using cross section data from another library for
the tallies is that it is not always consistent with the models and
cross sections used in MCNP to transport the particles. Using a tally
that is based upon data from another library could result in a dif-
ference in the rate at which particles are lost to interactions caus-
ing transmutations and the rate at which transmutations are being
tallied. With the high importance of neutron absorption reso-
nances for Tc transmutation, this could result in large errors.
1.4
Nonscaering interacon
1.2
cross secon (b)
1
0.8
0.6 TALYS
0.4 MCNP
0.2
0
0 200
Fig. 2. Cross section for any transmuting interaction vs. Energy using TALYS and the response function generated in MCNP.
Fig. 1. General Tc transmutation target design.
Another issue is that the available TENDL library does not extend
beyond 200 MeV for interactions with 99Tc nuclei, though the
agreement below this cutoff for non-scattering proton interactions
is fairly good, as seen in Fig. 2. Therefore, a self-consistent response
function for the reaction rate in 99Tc based upon the models used
in MCNP for high-energy particle transport up to the maximum
considered energy of 1500 MeV must be used. The purpose of this
response function is to be used in a tally to be able to estimate the
number of transmuting neutron and proton interactions with 99Tc
that occur in a system containing multiple materials.
2. Response function bin generation in MCNPX
In order to tally the interactions occurring between technetium
nuclei and particles with energies above MCNP’s tabulated cross
section data, a response function must be generated. The response
function relates the neutron or proton flux within a region contain-
ing 99Tc to the rate of transmutation of 99Tc nuclei. The response
function is a discretized set of energy bins; each energy bin gives
the transmutation rate per unit of neutron or proton flux with
energies within that bin, thus it behaves vary similarly to a macro-
scopic cross section. To generate the response function for an
energy bin, a short and very thin cylindrical technetium target
was modeled with a monodirectional point source of particles axi-
ally incident on the face of the cylinder. A separate MCNP deck was
run for each energy bin, with particles being born with an energy
randomly selected from the energy bin. The target was small
400 600 800 1000 1200 1400 1600
Incident proton energy (MeV)
 J.A. Hearne / Annals of Nuclear Energy 142 (2020) 107407 3

enough that attenuation, coulombic energy loss of protons, and
scattering buildup are negligible. If these assumptions hold, the
response value for that energy bin is given by Eq. (1),
nintr
rðEÞ ¼
nps  N:z0
here r(E) is the value of the response function for the energy bin
and particle type, nintr is the number of transmutation causing
interactions of interest occurring in the model, nps is the number
of incident particles on the target, N is the atomic density of the tar-
get material in atoms/cm3, and z is the length of the target in cm
through which the incident beam passes. This simulation and corre-
sponding calculation is performed for each bin for both protons and
neutrons to produce the complete, discretized response function.
The response function value for a bin represents the average cross
section for interactions other than capture or scattering within
the energy bin because the particles interacting have a flat distribu-
tion of energies through the bin.
A smaller target requires more particles to be run to attain good
statistics, so to reduce computation time, a larger target that is still
small enough for minimal attenuation is optimal. Different sizes of
targets are used at different energies, so that enough particles
interact without reaching the level where attenuation and energy
loss effects must be accounted for. When selecting the response
function generating target thickness, the goal is that less than
10% but more than 0.1% of the particles incident on the target
interact in the target. Any target in this thickness range was
accepted to allow for the more streamlined production of the input
decks. Additionally, to cut out interactions from particles that are
at energies outside of the bin range, the energy cutoff for the par-
ticles of interest in a specific run was set to the bottom of the bin
range for which the response function is being generated.
An attempt was made to use a response function for neutron
capture, but there was difficulty accurately modeling the reso-
nance absorption region using finite custom bins, due to the fine
details of the resonance capture region. The lack of sufficient reso-
nance resolution in the resonance region can be seen in Fig. 3. The
issue is that accurately resolving resonances in a custom generated
library using the same method used for the high-energy portion of
the library would require a prohibitively large number of bins to
avoid large errors between the number of particles lost to interac-
tions in technetium and the number of interactions tallied. This
ð1Þ custom tally therefore cannot be used to accurately tally the neu-
tron absorption in the resolved resonance region. The agreement is
better above 9 MeV, where absorption interactions other than cap-
ture begin to dominate.
MCNP’s built in neutron capture tally can be used to tally the (n,
gamma) neutron captures, which fall off to near zero before the
energy exceeds the built in tally energy maximum of 20 MeV. A
custom-made tally can then be used to account for all other non-
scattering nuclear interactions, which only begin to occur above
about 9 MeV. The response function will therefore only count
transmutation-causing interactions other than capture. The proton
interactions are all tallied using custom bins. Fine energy bins for
low energy protons are not required, as protons with less than a
few MeV cannot effectively overcome the coulomb barrier to inter-
act directly with nuclei without undergoing very improbable quan-
tum tunneling. Thus, for estimating the transmutation of rate, the
(n,gamma) neutron capture reactions are counted with MCNP’s
built in tally, and other interactions are successfully tallied using
the computed non-scattering, non-capture response function, leav-
ing no major source of particle interactions uncounted. Using the
response function to calculate the transmutation rate is demon-
strated in Eq. (2):
X
particles X
bins
Transmutation rate ¼ Uðp; EÞrðp; EÞ  N  V; ð2Þ
p E
where Rparticles
p is a sum over all particle types considered (protons
and neutrons), RbinsE is the sum over all energy bins tallied for par-
ticle type p, U(p,E) is the flux of particle p within energy bin E, r(p,
E) is the response function value for particle p and energy bin E, N is
the atom density of 99Tc within the material tallied and V is the vol-
ume of the material.
Iterations of energy bin and input deck designs were performed
to obtain the final response function bins and data used. The final

10000
Total absorpon cross secon (b)

1000
Talys
100
Custom from MCNP
10

0.1

0.01

0.001
1E-12 1E-10 1E-08 0.000001 0.0001 0.01 1 100
Incident Neutron energy (MeV)
Fig. 3. Total neutron absorption cross section vs. energy using TALYS library and using the response function generation method in MCNP.
4 J.A. Hearne / Annals of Nuclear Energy 142 (2020) 107407
Fig. 4. Target used for validating
data used in the transmutation analysis (Hearne and Tsvetkov,
2019) can be found in Appendix A.
3. Response function verification
To verify the internal consistency of data collected, it was used
to estimate the number of transmutations in a pure 99Tc target, so
that the custom cross sections and tallies could be compared to the
neutrons lost to interactions method of counting transmutations in
the target. A cylindrical target with a depth of 100 cm and a radius
of 30 cm made of pure technetium-99 at a density of 11 g/cm3,
with a hole for the incident beam with a depth of 20 cm and a
radius of 12 cm is used for validation. A schematic of the target
can be seen in Fig. 4. MCNPX uses models to account for proton
and neutron creation via spallation, particle loss to nuclear interac-
tions and proton energy loss through columbic interactions.
Incident proton energies of 600 MeV and 1200 MeV with 10,000
source particles gives total interaction estimates of 111,067 and
278,427 when using the tallies. The totals obtained by counting
the number of particles lost to each interaction type are 111,997
and 279,428. The tally method yields results that are 0.81% and
0.36% lower in these two trials. Errors less than 1% are deemed
to be acceptable, as they are comparable to the uncertainties of
the Monte Carlo simulations used to obtain the data. The close
agreement in the pure target therefore verifies the use of the
response function with custom tallies in more complex targets
containing multiple different nuclides as a method consistent with
the particle loss counting method. This method estimates the
transmutation rate of 99Tc nuclei based upon the proton and neu-
tron fluxes present in the material and the density of 99Tc present.
Effects of self-shielding and energy loss to the other materials are
accounted for via their effects on the flux in the MCNP model.
4. Conclusion
The response function for 99Tc transmutation by particles in the
energy ranges involved in the supported study was generated. The
99
Tc response function.
response function method was validated against the particle loss
method of transmutation counting with a difference of less than
1%. This enables the response function to be used to calculate of
the number of Tc atoms transmuted in a heterogeneous system
in a way that is consistent with the other method used in
(Hearne and Tsvetkov, 2019).
5. Disclaimer
This paper was prepared as an account of work sponsored by an
agency of the United States Government. Neither the United States
Government nor any agency thereof, nor any of their employees,
makes any warranty, express or implied, or assumes any legal lia-
bility or responsibility for the accuracy, completeness, or useful-
ness of any information disclosed. The views and opinions of
authors expressed herein do not necessarily state or reflect those
of the United States Government or any agency thereof.
CRediT authorship contribution statement
Jason A. Hearne: Conceptualization, Methodology, Software,
Formal analysis, Investigation, Writing - original draft, Writing -
review & editing, Visualization.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
Acknowledgements
This paper is based upon work partially supported by the U.S.
Department of Energy Nuclear Energy University Program Award
Number 11-3054 under DOE contract DE-AC07-05ID14517.
The author acknowledges Dr. Pavel Tsvetkov for advising and
managing the funding of the project and Dr. Charles Stratton for
help with MCNP deck pre and post processing automation.
 J.A. Hearne / Annals of Nuclear Energy 142 (2020) 107407 5

Appendix A

Response function data tables

This response function is a representation of the model-based estimate of the total neutron cross sections for interactions other than
capture or scattering.
The energy listed for each bin is the upper energy limit for the bin. The lower limit is the energy listed for the previous bin, or zero for
the first bin.
E (MeV) sigma (b) E (MeV) sigma (b) E (MeV) sigma (b) E (MeV) sigma (b)
8.8 0 12.3 1.031544 23 1.735436 58 1.413462
8.9 0 12.4 1.05836 24 1.713668 59 1.408341
9 0 12.5 1.085295 25 1.701393 60 1.403463
9.1 0.001525 12.6 1.109612 26 1.688956 80 1.363939
9.2 0.015808 12.7 1.131142 27 1.676812 100 1.291311
9.3 0.032615 12.8 1.152528 28 1.665035 120 1.213328
9.4 0.049779 12.9 1.174108 29 1.653165 140 1.146689
9.5 0.066842 13 1.195591 30 1.641436 160 1.072798
9.6 0.094179 13.1 1.21514 31 1.62976 180 1.035614
9.7 0.13187 13.2 1.23286 32 1.61841 200 1.030469
9.8 0.169517 13.3 1.250324 33 1.607008 220 1.0275
9.9 0.207286 13.4 1.267927 34 1.595701 240 1.026294
10 0.244917 13.5 1.285569 35 1.585048 260 1.026796
10.1 0.28342 13.6 1.301691 36 1.57519 280 1.027965
10.2 0.323181 13.7 1.316336 37 1.565238 300 1.029823
10.3 0.363112 13.8 1.330958 38 1.555524 320 1.03228
10.4 0.40302 13.9 1.345383 39 1.546118 340 1.034752
10.5 0.443045 14 1.360126 40 1.536875 360 1.037437
10.6 0.481363 14.1 1.373212 41 1.528218 380 1.040962
10.7 0.518508 14.2 1.384705 42 1.519739 400 1.044231
10.8 0.555675 14.3 1.396268 43 1.511692 420 1.044384
10.9 0.592619 14.4 1.407792 44 1.503701 440 1.047284
11 0.629587 14.5 1.419389 45 1.495968 460 1.050584
11.1 0.629736 14.6 1.431122 46 1.488587 480 1.052984
11.2 0.665625 14.7 1.442624 47 1.481467 500 1.054284
11.3 0.700398 14.8 1.454185 48 1.474373 520 1.059384
11.4 0.735082 14.9 1.46566 49 1.467385 540 1.062584
11.5 0.770016 15 1.477399 50 1.460615 560 1.067984
11.6 0.805131 16 1.516287 51 1.454092 580 1.073084
11.7 0.836889 17 1.552919 52 1.447857 600 1.074084
11.8 0.865018 18 1.604381 53 1.441664 620 1.078284
11.9 0.922138 19 1.624208 54 1.435203 640 1.082284
12 0.950636 20 1.638906 55 1.429496 660 1.084584
12.1 0.978301 21 1.742518 56 1.424112 680 1.089084
12.2 1.005074 22 1.735436 57 1.418717 700 1.093684

(continued on next page)

6 J.A. Hearne / Annals of Nuclear Energy 142 (2020) 107407

Appendix A (continued)

Total neutron interaction cross sections other than capture or scattering continued
E (MeV) sigma (b) E (MeV) sigma (b)
720 1.095584 1420 1.114943
740 1.098184 1440 1.114754
760 1.100184 1460 1.114514
780 1.101184 1480 1.114239
800 1.103684 1500 1.11403
820 1.107184
840 1.109384
860 1.112484
880 1.113684
900 1.114284
920 1.115384
940 1.119784
960 1.121284
980 1.122084
1000 1.122984
1020 1.125484
1040 1.125684
1060 1.125884
1080 1.126484
1100 1.128184
1120 1.128884
1140 1.128484
1160 1.130084
1180 1.130384
1200 1.130784
1220 1.115001
1240 1.115157
1260 1.115351
1280 1.115453
1300 1.115493
1320 1.115509
1340 1.115438
1360 1.115352
1380 1.115303
1400 1.115149
 J.A. Hearne / Annals of Nuclear Energy 142 (2020) 107407 7

Response function value for transmutation by protons

The energy listed for each bin is the upper energy limit for the bin. The lower limit is the energy listed for the previous bin, or zero for
the first bin
E (MeV) sigma (b) E (MeV) sigma (b) E (MeV) sigma (b) E (MeV) sigma (b)
1 4.12E-11 90 1.127252 720 1.0531 1420 1.071894
2 3.77E-06 100 1.102454 740 1.0568 1440 1.07194
3 0.000476 110 1.080989 760 1.0591 1460 1.072229
4 0.007667 120 1.062202 780 1.0616 1480 1.072365
5 0.046823 130 1.046013 800 1.0651 1500 1.072516
6 0.153017 140 1.031677 820 1.0668
7 0.306835 150 1.018649 840 1.0686
8 0.453447 160 1.00729 860 1.0718
9 0.576031 180 0.987361 880 1.0739
10 0.67444 200 0.970346 900 1.0755
11 0.756036 220 1.0099 920 1.0776
12 0.828099 240 1.0122 940 1.08
13 0.890711 260 1.0154 960 1.0815
14 0.942091 280 1.0128 980 1.0835
15 0.983099 300 1.0155 1000 1.0836
16 1.017158 320 1.0191 1020 1.0846
17 1.046772 340 1.0212 1040 1.0867
18 1.073177 360 1.0263 1060 1.0875
19 1.09772 380 1.031 1080 1.0898
20 1.120498 400 1.0334 1100 1.0904
22 1.163876 420 0.9886 1120 1.0906
24 1.201201 440 0.9966 1140 1.0913
26 1.229436 460 1.0017 1160 1.0927
28 1.248396 480 1.0043 1180 1.0926
30 1.260454 500 1.0104 1200 1.0934
35 1.28253 520 1.0165 1220 1.067636
40 1.286651 540 1.0204 1240 1.068341
45 1.278523 560 1.0256 1260 1.068958
50 1.261939 580 1.0291 1280 1.06949
55 1.241049 600 1.0328 1300 1.069942
60 1.22594 620 1.0365 1320 1.07048
65 1.205704 640 1.0386 1340 1.07083
70 1.189514 660 1.0423 1360 1.071179
75 1.170808 680 1.0448 1380 1.071479
80 1.156483 700 1.0478 1400 1.07173

Appendix B. Supplementary data
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.anucene.2020.107407.
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