2010 Monitoring Research Review: Ground-Based Nuclear Explosion Monitoring Technologies

MODELING OF RADIOXENON PRODUCTION AND RELEASE PATHWAYS

Steven R. F. Biegalski, Mark Deinert, Carlos Rios Perez, and Justin D. Lowrey
University of Texas at Austin
Sponsored by National Nuclear Security Administration
Award No. DE-AC52-09NA28608
Proposal No. BAA09-57

ABSTRACT
Models have been developed to calculate the diffusion of radioxenon through porous environmental media such as
sand and soil. Initial experiments have also been conducted to determine the feasibility of radioxenon transport
through soil and sand columns. The initial studies investigated method detection limits for xenon detection. These
results show that stable xenon may be detected through prompt gamma activation analysis (PGAA) with detection
limits in the 10-ppm range. New experiments are being designed to measure the diffusion of xenon in a
nondestructive temporal manner. The initial goal is to measure an overall diffusion coefficient for each porous
medium. The secondary goal is to measure the isotopic fractionation resulting from the process.

567

Form Approved
OMB No. 0704-0188

Report Documentation Page

Public reporting burden for the collection of information is estimated to average 1 hour per response, including the time for reviewing instructions, searching existing data sources, gathering and
maintaining the data needed, and completing and reviewing the collection of information. Send comments regarding this burden estimate or any other aspect of this collection of information,
including suggestions for reducing this burden, to Washington Headquarters Services, Directorate for Information Operations and Reports, 1215 Jefferson Davis Highway, Suite 1204, Arlington
VA 22202-4302. Respondents should be aware that notwithstanding any other provision of law, no person shall be subject to a penalty for failing to comply with a collection of information if it
does not display a currently valid OMB control number.

1. REPORT DATE

3. DATES COVERED
2. REPORT TYPE

SEP 2010

00-00-2010 to 00-00-2010

4. TITLE AND SUBTITLE

5a. CONTRACT NUMBER

Modeling of Radioxenon Production and Release Pathways

5b. GRANT NUMBER

5c. PROGRAM ELEMENT NUMBER

6. AUTHOR(S)

5d. PROJECT NUMBER

5e. TASK NUMBER
5f. WORK UNIT NUMBER

7. PERFORMING ORGANIZATION NAME(S) AND ADDRESS(ES)

University of Texas at Austin,1 University Station ,Austin,TX,78712

9. SPONSORING/MONITORING AGENCY NAME(S) AND ADDRESS(ES)

8. PERFORMING ORGANIZATION
REPORT NUMBER
10. SPONSOR/MONITORS ACRONYM(S)
11. SPONSOR/MONITORS REPORT
NUMBER(S)

12. DISTRIBUTION/AVAILABILITY STATEMENT

Approved for public release; distribution unlimited

13. SUPPLEMENTARY NOTES

Published in Proceedings of the 2010 Monitoring Research Review - Ground-Based Nuclear Explosion
Monitoring Technologies, 21-23 September 2010, Orlando, FL. Volume II. Sponsored by the Air Force
Research Laboratory (AFRL) and the National Nuclear Security Administration (NNSA). U.S.
Government or Federal Rights License
14. ABSTRACT

Models have been developed to calculate the diffusion of radioxenon through porous environmental media
such as sand and soil. Initial experiments have also been conducted to determine the feasibility of
radioxenon transport through soil and sand columns. The initial studies investigated method detection
limits for xenon detection. These results show that stable xenon may be detected through prompt gamma
activation analysis (PGAA) with detection limits in the 10-ppm range. New experiments are being designed
to measure the diffusion of xenon in a nondestructive temporal manner. The initial goal is to measure an
overall diffusion coefficient for each porous medium. The secondary goal is to measure the isotopic
fractionation resulting from the process.
15. SUBJECT TERMS
16. SECURITY CLASSIFICATION OF:
a. REPORT

b. ABSTRACT

c. THIS PAGE

unclassified

unclassified

unclassified

17. LIMITATION OF
ABSTRACT

18. NUMBER
OF PAGES

Same as
Report (SAR)

10

19a. NAME OF
RESPONSIBLE PERSON

Standard Form 298 (Rev. 8-98)

Prescribed by ANSI Std Z39-18

2010 Monitoring Research Review: Ground-Based Nuclear Explosion Monitoring Technologies

OBJECTIVES

The two most recent nuclear weapon tests were conducted by the Democratic People's Republic of Korea (DPRK) in
October 2006 and May 2009. Prior to the DPRK tests, India and Pakistan went through a series of nuclear tests in
May 1998. It is important to recognize that all of the nuclear tests for more than 12 years have been conducted by
countries developing nuclear weapons. The nuclear test yields were relatively small (Nuclear Explosion DataBase,
2010) and were conducted underground.
Radionuclide releases from these nuclear explosions have been minimal. Some of this may be attributed to the low
yield of the devices tested, and some may be attributed to underground containment. Radionuclide releases from the
DPRK tests have provided only radioxenon measurements from the first test conducted in 2006. Radioxenon
measurements showed atmospheric concentrations that at times were close to background levels (Ringbom et al.,
2009).
The objective of this work is to develop a better understanding of radioxenon transport after an underground nuclear
explosion. The initial source signature of a nuclear weapon may be calculated with previously developed codes.
However, there is a considerably larger error in the understanding of how the source signature is perturbed as
radionuclides transport in an underground environment. Both chemical fractionation and isotopic fraction may
occur. This work focuses on the initial diffusion of xenon through porous media (e.g., soil). The transport times and
isotopic fractionation are calculated, and plans are under way to measure this processing utilizing PGAA.

RESEARCH ACCOMPLISHED
The research accomplished may be broken into three areas. The first is the calculation of a radionuclide source term
from an underground nuclear explosion. The second area is calculation of diffusion for Xe isotopes. The last area is
the initial calculations of detection limits for the measurement of Xe via PGAA.
Source-Term Calculation
As part of this work, models have been developed to calculate the radionuclides produced in a 1-kt nuclear
explosion. The code MCNP is utilized to model the neutron transport, while ORIGEN 2.2 is utilized to calculate the
production and decay of fission products, activation products, and transuranics resulting from the calculated neutron
flux profile. MONTEBURNS is a pearl script that couples the MCNP and ORIGEN 2.2 calculations.
The model used for the source-term calculation is fairly simple. A weapons-grade fissile sphere (keff ~1.0) is
surrounded by a soil or rock shell. For the uranium core case, an 8.7-cm-radius spherical core enriched to 94% 235U
was utilized; for the plutonium case, a 5.1-cm-radius spherical core enriched to 93.80% 239Pu was used. MCNP was
used to determine the thickness of soil or rock necessary to accurately model the attenuation and capture of neutrons
within the media. For most of the soil and rock samples used, a thickness of 150 cm around the core was sufficient,
such that less than 1% of neutrons escaped the system. For all cases studied, a soil/rock thickness of 2 m yielded on
the order of 0.1% neutrons escaping.
Using MONTEBURNS, a database was complied to include the resulting concentration and activity of every isotope
calculated for both a 235U and a 239Pu sphere normalized to a burn of 1 kt. Two different soil compositions and three
different rock compositions were utilized in order to model a range of environments and effectively determine a
range of resulting activities for the isotopes of concern. The resulting concentrations were then decayed in ORIGEN
2.2 to yield activities at post-burn times from 5 minutes up to 100 days. The results for the radioisotopes of concern
are summarized in Tables 1 and 2.

568

2010 Monitoring Research Review: Ground-Based Nuclear Explosion Monitoring Technologies

Table 1. Activities in Ci of xenon radioisotopes following modeled 1-kt explosion at various post-burn decay
times, assuming both uranium and plutonium cores
Initial
Uranium
Core

131m
133

Xe

133m
135

Plutonium
Core

Xe

Xe

133m
135

Xe

Xe

131m
133

Xe

Xe

Xe

5 min

1 hr

10 hr

1 day

10 days

30 days

100 days

1.361E-01

1.384E-01

7.948E-01

2.386E+01

5.972E+01

3.555E+02

2.638E+02

7.439E+00

1.964E+02

3.016E+02

6.481E+03

8.824E+04

1.709E+05

1.127E+05

8.120E+03

7.805E-01

1.560E+03

1.566E+03

1.984E+03

7.379E+03

1.208E+04

1.743E+03

3.122E+00

7.441E-10

1.109E+05

1.804E+05

6.651E+05

2.000E+06

1.329E+06

1.843E-01

2.334E-17

0.000E+00

1.811E-01

1.846E-01

9.736E-01

2.705E+01

6.791E+01

4.147E+02

3.094E+02

8.740E+00

6.991E+02

8.669E+02

7.171E+03

8.886E+04

1.717E+05

1.134E+05

8.178E+03

7.861E-01

5.446E+03

5.452E+03

5.831E+03

1.078E+04

1.490E+04

1.906E+03

3.425E+00

8.163E-10

2.648E+05

3.722E+05

9.930E+05

2.269E+06

1.459E+06

1.988E-01

2.518E-17

0.000E+00

Table 2. Activities of 37Ar in Ci resulting from modeled 1-kt explosion and subsequent neutron
activation in various surrounding soil and rock concentrations

Plutonium Core

Uranium Core

Soil Type

Initial

10 hr

1 day

10 days

30 days

100 days

Wedepohl

1.014E+03

1.005E+03

9.937E+02

8.316E+02

5.597E+02

1.401E+02

Taylor

9.455E+02

9.377E+02

9.270E+02

7.757E+02

5.222E+02

1.307E+02

Mason

4.616E+02

4.579E+02

4.526E+02

3.788E+02

2.549E+02

6.380E+01

Bowen

3.488E+02

3.460E+02

3.420E+02

2.862E+02

1.926E+02

4.820E+01

Vinogradov

3.477E+02

3.448E+02

3.409E+02

2.853E+02

1.920E+02

4.805E+01

Wedepohl

1.760E+03

1.745E+03

1.725E+03

1.444E+03

9.717E+02

2.432E+02

Taylor

1.502E+03

1.489E+03

1.472E+03

1.232E+03

8.294E+02

2.075E+02

Mason

7.241E+02

7.182E+02

7.100E+02

5.941E+02

3.999E+02

1.001E+02

Bowen

5.021E+02

4.980E+02

4.922E+02

4.119E+02

2.773E+02

6.938E+01

Vinogradov

5.011E+02

4.970E+02

4.913E+02

4.111E+02

2.767E+02

6.925E+01

Diffusion Coefficients for Xe Isotopes

Although the molecular transport of xenon in air would be more accurately modeled as a multicomponent diffusion
process, we will use first a binary diffusion scenario to analyze the transport of xenon stable isotopes through a
porous medium. Assuming that the molecular motion of each isotope is independent from the presence of other
xenon nuclides makes it possible to employ Ficks first law of diffusion in our analysis. This assumption is valid
when the amount of all but one species in the gas mixture is small (Deen 1998). Nitrogen will be used as the solvent
gas in our analysis because it is an inert gas and is the most abundant element in air. For a nonpolar binary gas
mixture at low pressure, the binary diffusion coefficient can be approximated using the correlation proposed by Bird
et al. (2007). This formula is presented in Equation 1:

569

2010 Monitoring Research Review: Ground-Based Nuclear Explosion Monitoring Technologies

#
T
"4 %
2.745x10
%
$ TcXeTcN 2

&1.823
(
=
1/ 2 (
'
pcXe pcN 2

pDXeN 2

) (T
1/ 3

5 /12

cXe cN 2

1/ 2
) 1
1 ,
++
..
+
* M Xe M N 2 -

(1)

where
p=
T=

Total absolute pressure of mixture [atm]

Temperature of mixture [K]
DXeN 2 = Binary diffusion coefficient of xenon in nitrogen or vice versa.

Table 3 provides a range of diffusion coefficients as calculated by Equation 1 for 129Xe and 131Xe in a binary mixture
with N2. Both 129Xe and 131Xe are stable isotopes with natural abundances of 26.4% and 21.2%, respectively
(Molnar, 2004). These two isotopes are chosen for this model because of their higher detection probability through
PGAA. Table 3 shows that there is about a 0.1% difference between the diffusion coefficients of 129Xe and 131Xe.
While that is not a huge difference, it will result in differential transport over time and distance. Such differences
will result in isotopic fractionation and changes in the radioxenon isotopic signature.
Table 3. Binary diffusion coefficients of 129Xe and 131Xe in a binary gas with N2
129

131

Xe

Xe

Ma

Mb

T [K]

p
[atm]

DXeN 2 [cm2 s-1]

DXeN 2 [cm2 s-1]

131

28.013

290

0.9

0.13502

0.13484

131

28.013

290

0.12152

0.12135

131

28.013

290

1.1

0.11047

0.11032

131

28.013

290

1.2

0.10127

0.10113

131

28.013

290

1.3

0.09348

0.09335

131

28.013

290

1.4

0.08680

0.08668

131

28.013

290

1.5

0.08101

0.08090

131

28.013

290

1.6

0.07595

0.07585

131

28.013

290

1.7

0.07148

0.07138

131

28.013

290

1.8

0.06751

0.06742

131

28.013

290

1.9

0.06396

0.06387

Analytical Model
The analytical model for the experiment developed for this paper assumes the following:

The diffusion of xenon isotopes occurs at uniform and constant pressure and temperature and small
concentrations.
The molecular diffusion of xenon isotopes takes place in only one direction (X direction).
The diffusion coefficient of xenon in nitrogen is independent of the mixture composition.
The external convection effects are negligible.
Each xenon isotope is treated as a different species, but all isotopes molecular diffusion is treated as in a
binary system isotope-nitrogen.
There is no chemical reaction that produces/consumes the xenon isotopes.
Both xenon and nitrogen have ideal gas behavior.

570

2010 Monitoring Research Review: Ground-Based Nuclear Explosion Monitoring Technologies

Based on these assumptions, the molar average velocity is zero, and the equation of continuity of each isotope in
molar basis is simplified to

"C # Xe
" 2C # Xe
= D# XeN
2
"t
"x 2
where

(2)

C " Xe is the molar concentration of the isotope " Xe , and D" XeN is the effective diffusion coefficient. The
2

!
!

effective diffusion coefficient takes into account the porosity and tortuosity of the porous medium. Assuming a
porosity of 0.3, a tortuosity factor of 1.96 was calculated using the experimental correlation obtained by Matyka et
al. (2008). From these two factors, the effective diffusion coefficients for 131Xe and 129Xe obtained are 0.01857 and
!
0.01854 [cm2 s-1] respectively.
!
We will assume that the length of the duct where diffusion occurs is long enough to consider a semi-infinite
medium. For this experiment, the initial and boundary conditions are
IC:

t = 0, x >0
t = 0, x = 0

BC1:

t >0, x!= 0

BC2:

!
t, x

C " Xe = 0
C " Xe = C0

C =0

" 2C $ Xe
"N o
= A# D$ XeN
2
"t
"x 2

where N o is the initial number of moles of the xenon isotope under analysis ( N o = CoVo ),
concentration of the isotope
! of interest at x = 0, and A is the cross-sectional area at x = 0.

Co is the initial

Equation 3 presents the solution for these preliminary determinations of epicenter (PDEs), and initial and boundary
conditions (Takeda et al., 2008):
!
!

!
2
# A D" t
&
#
&
A D" XeN t Ax
C " Xe (x,t)
x
XeN 2
2
%
(.
%
(
= exp%
+ () erfc
+
2
%
(
CO
V
V
V
2
D
t
"
o
o '
o
$
XeN 2 '
$

(3)

Figures 1 and 2 show the variation of the xenon concentration as a function of time and distance. Figures 3 and 4
show the variation of the ratio of molar concentrations 131Xe and 129Xe with respect to position and time,
respectively, for diffusion of 0.0053 kg of natural xenon in a duct of 0.0070 m2. According to these results, an
important ratio between the concentration of 131Xe and 129Xe could be measured at the diffusion. Conversely, at this
location, the ratio C " Xe C0 is very small. For example, at t =1 2 h, a ratio of C 131 Xe C 129 Xe = 0.7995 can be

measured at x = 1.5 m (the isotopes ratio in natural xenon is 0.803); however, at this location and
"5
"5
time, C 129 Xe /Co = 5.749x10 and C 131 Xe /Co = 5.725x10 . These small concentrations will make the analysis
of differential diffusion at the diffusion front difficult, as will be seen in the following section.

571

2010 Monitoring Research Review: Ground-Based Nuclear Explosion Monitoring Technologies

Figure 1. Variation of the Xe concentration profile at 1 h, 12 h, and 48 h.

Figure 2. Variation of the Xe concentration with respect to time.

572

2010 Monitoring Research Review: Ground-Based Nuclear Explosion Monitoring Technologies

Figure 3. Variation of the ratio 131Xe/129Xe with respect to position.

Figure 4. Variation of the ratio 131Xe/129Xe with respect to time.

573

2010 Monitoring Research Review: Ground-Based Nuclear Explosion Monitoring Technologies

Experimental Validation
This section evaluates the possibility of measuring the differential diffusion of 131Xe and 129Xe in a porous medium
such as soil utilizing PGAA. First, the minimum amount of xenon needed for detection is calculated. Second, the
effective volume of the sample is approximated. Finally, the minimum concentration of xenon required is obtained,
and the feasibility of a xenon differential diffusion testing facility is discussed.
The minimum amount of xenon required to detect 131Xe and 129Xe is calculated from the molar detection limit (Ld)
of the equipment and the isotopic composition of the inert gas. Detection limits of 6.3 10-5 and 7.7 10-5 moles
were calculated for 129Xe at 536 keV and 131Xe at 630 keV, for a total efficiency of 0.00145 (This efficiency was
estimated from the counting rates analysis of 100% and 20% xenon samples during various time spans). The
approximate percentages of 131Xe and 129Xe in natural xenon are 26.4% and 21.2%, respectively. There are two
sample volumes that are important for a PGAA: the active and the effective sample volumes (Molnar, 2004). The
following assumptions are made to calculate a first approximation of the effective volume of the sample:

The attenuation of the neutron beam along the sample is negligible (both elements have small (n-) cross
section).
The detector has a collimator of 70 mm in diameter (the end-cap diameter of the detector has to be 83 mm or
larger in order to have an efficiency of 65% [Rvay et al., 2007]).

It has been reported that the neutron beam cross section at the sample location is about 2.5 1 cm2 (Rvay et al,.
2007). From this, and from the assumptions listed before, the active volume of the sample could be approximated as
6.5 cm 2.5 cm 1 cm, i.e., 16.25 cm3 (see Figure 5). Taking into account the geometric efficiency and the
nonuniform intensity of the neutron flux, the effective sample volume is estimated to be 12 cm3.
From the results calculated above, the minimum molar concentration of xenon required for a PGAA analysis is
estimated as 2.5 10-5 molcm-3 (to detect 500 events in 1000 s). Assuming that at x = 0 we have pure xenon gas at
1 atm (molar concentration of 4.5 10-5 molcm-3), the C " Xe /Co minimum detectable is 0.556.
From Equation 3, the ratio of

C " Xe /Co = 0.556 could be obtained at x = 0 and t = 45 min. Therefore, an accurate

analysis at x = 0 m would be difficult to conduct in a noninvasive way since the detection time for the Ld predicted is
/C0 from t = 30 min to t = 45 min is about 6 10-5 1/s.
1000 s, and the average rate of change of C!
"
Xe

!
The analysis of a separated
sample would allow us to conduct the PGAA for longer times with smaller detection
limits and therefore more accuracy. For example, the Ld for 129Xe at 536 keV in a 7-h PGAA analysis is 2.5 1 0-6
moles, and the C " Xe /Co minimum
detectable in the gas mixture is 0.022. This ratio can be obtained from a sample
!
extracted at x = 0 after more than t = 150 h from initiating the diffusion experiment; i.e., a sample of gas extracted
during the first 150 h has larger concentrations of 129Xe than the Ld. Also, at t = 150 h, the ratio C 131 Xe /C 129 Xe has
changed by 0.07%. Although this change may seem very small, the analysis of the extracted gas may be prolonged
! to reach the desired accuracy without interfering with the diffusion experiment.
in order

574

2010 Monitoring Research Review: Ground-Based Nuclear Explosion Monitoring Technologies

Figure 5. Effective sample volume, assuming a collimator of 7 cm in diameter.

CONCLUSIONS AND RECOMMENDATIONS

The results shown herein lay a foundation for the modeling of Xe transport within a natural soil or sand matrix. The
computational results indicate that isotopic fractionation occurs during such transport. This is fundamentally
important to understanding the nuclear forensic signature of radioxenon emissions from an underground nuclear
explosion.
Experiments are being set up to measure the Xe diffusion through sand and soil media utilizing PGAA. The goal
would be to measure the isotopic fractionation that occurs during the diffusion process. However, initial calculations
show that measuring the differential diffusion will be a challenge. At a minimum, diffusion coefficients for Xe and
the models may be benchmarked with such experiments.

ACKNOWLEDGEMENT
We extend our gratitude to the staff of the Nuclear Engineering Teaching Laboratory at the University of Texas at
Austin for experimental support.

REFERENCES
Bird, R. B., W. E. Stewart, and E .N. Lightfoot (2007). Transport Phenomena, 2nd edition. New York, NY: John
Wiley & Sons, Inc.
Deen, W. M. (1998). Analysis of Transport Phenomena. New York: Oxford University Press, Inc.
Matyka, M., A. Khalili, and Z. Koza (2008). Tortuosity-porosity relation in porous media flow, Phys. Rev. E 78:
026306.
Molnar, G. L., Ed. (2004). Handbook of Prompt Gamma Activation Analysis with Neutron Beams. Kluwer
Academic Publishers.

575

2010 Monitoring Research Review: Ground-Based Nuclear Explosion Monitoring Technologies

Nuclear Explosion DataBase (2010). http://www.rdss.info/database/nedb/nedb_ent.html

Rvay, Z., R. K. Harrison, E. Alvarez, S. R. Biegalski, and S. Landsberger (2007). Construction and characterization
of the redesigned PGAA facility at the University of Texas at Austin. Nuclear Instruments and Methods in
Phys. Res. Sec. A: Accelerators, Spectrometers, Detectors and Associated Equipment, 577: 611618.
Ringbom, A, K. Elmgren, K. Lindh, J. Peterson, T. Bowyer, J. Hayes, J. McIntyre, M. Panisko, and R. Williams
(2009). Measurements of radioxenon in ground level air in South Korea following the claimed nuclear test
in North Korea on October 9, 2006, J. Radioanal. Nucl. Chem. 282: 773779.
Takeda, M., H. Nakajima, M. Zhang, and T. Hiratsuka (2008). Laboratory longitudinal diffusion tests: 1.
Dimensionless formulations and validity of simplified solutions. J. Contam. Hydrol. 97: 117134.

576