Nondestructive and destructive assay for forensics characterization of weapons-grade plutonium produced in LEU irradiated in a thermal neutron spectrum

Sean P. Martinson; Jenna R. Garcia; Isaac W. Haynes; Simrun P. Saini; Elisan R. Wagner; Grace R. Long; Charles M. Folden; Sunil S. Chirayath

doi:10.1016/j.anucene.2022.109645

Nondestructive and destructive assay for forensics characterization of weapons-grade plutonium produced in LEU irradiated in a thermal neutron spectrum

Sean P. Martinson, Jenna R. Garcia, Isaac W. Haynes, Simrun P. Saini, Elisan R. Wagner, Grace R. Long, Charles M. Folden, Sunil S. Chirayath

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

Abstract

A post-irradiation examination (PIE) of an enriched uranium sample was performed to advance a nuclear forensics methodology, based on intra-elemental nuclide ratios. The PIE was carried out on a few milligrams of low enriched uranium dioxide (LEUO₂) sample, irradiated to a burnup of 1 GWd/MTU. The PIE of the LEUO₂ sample provided the concentration of selected plutonium and fission product nuclides (²³⁹Pu, ²⁴⁰Pu, ²⁴¹Pu, ⁹¹Y, ⁹⁵Zr, ⁹⁵Nb, ¹⁰³Ru, ¹³³Cs, ¹³⁴Cs, ¹³⁵Cs, ¹³⁷Cs, ¹³⁶Ba, ¹³⁸Ba, ¹⁴⁰Ba, ¹⁴⁰La, ¹⁴¹Ce, ¹⁴⁴Ce, ¹⁴⁹Sm, ¹⁵⁰Sm, ¹⁵²Sm, ¹⁵³Eu, and ¹⁵⁴Eu). The PIE supported validation of the MCNP (Monte Carlo N-Particle neutronics simulation code) predicted concentration of these nuclides in the irradiated LEUO₂ sample. This study showed that most of the MCNP predicted nuclide concentrations were within 15% and several within 10% compared to the PIE results. Gamma and mass spectrometry of nuclides in irradiated LEUO₂ enabled the determination of uranium burnup and time since irradiation.

Original language	English
Article number	109645
Journal	Annals of Nuclear Energy
Volume	183
DOIs	https://doi.org/10.1016/j.anucene.2022.109645
State	Published - Apr 2023
Externally published	Yes

Funding

The LEUO2 irradiation and the work performed by Sean P. Martinson, Simrun P. Saini, Elisan R. Wagner, and Sunil S. Chirayath, were funded by the Consortium for Monitoring, Technology, and Verification under Department of Energy (DOE) National Nuclear Security Administration (NNSA) award number DE-NA0003920. Work performed by Jenna R. Garcia and Isaac W. Haynes is based upon work supported by the DOE NNSA through the Nuclear Science and Security Consortium under Award Number DE-NA0003996. The opinions expressed in this article are the authors’ own and do not necessarily state or reflect the view of the NNSA, the DOE, or the United States Government or any agency thereof. Neither the United States Government nor any agency thereof, nor any of their employees, makes any warranty, express or limited, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The authors would like to thank Dr. Craig Marianno in the Department of Nuclear Engineering at Texas A&M University for providing the Ortec Micro-Detective portable HPGe gamma detector used to acquire gamma spectra for the undissolved and dissolved sample described in the paper. Authors would also like to place on record their highest appreciation for the English language editing and proof-reading assistance provided by Ms. Kelley Holle Ragusa, Assistant Director of the Texas A&M Center for Nuclear Security Science and Policy Initiatives. The LEUO 2 irradiation and the work performed by Sean P. Martinson, Simrun P. Saini, Elisan R. Wagner, and Sunil S. Chirayath, were funded by the Consortium for Monitoring, Technology, and Verification under Department of Energy (DOE) National Nuclear Security Administration (NNSA) award number DE-NA0003920. Work performed by Jenna R. Garcia and Isaac W. Haynes is based upon work supported by the DOE NNSA through the Nuclear Science and Security Consortium under Award Number DE-NA0003996. The opinions expressed in this article are the authors’ own and do not necessarily state or reflect the view of the NNSA, the DOE, or the United States Government or any agency thereof. Neither the United States Government nor any agency thereof, nor any of their employees, makes any warranty, express or limited, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The authors would like to thank Dr. Craig Marianno in the Department of Nuclear Engineering at Texas A&M University for providing the Ortec Micro-Detective portable HPGe gamma detector used to acquire gamma spectra for the undissolved and dissolved sample described in the paper. Authors would also like to place on record their highest appreciation for the English language editing and proof-reading assistance provided by Ms. Kelley Holle Ragusa, Assistant Director of the Texas A&M Center for Nuclear Security Science and Policy Initiatives.

Keywords

Gamma radiation spectrometry
Low-burnup uranium
MCNP validation
Mass spectrometry
Nuclear forensics

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Cite this

Martinson, S. P., Garcia, J. R., Haynes, I. W., Saini, S. P., Wagner, E. R., Long, G. R., Folden, C. M., & Chirayath, S. S. (2023). Nondestructive and destructive assay for forensics characterization of weapons-grade plutonium produced in LEU irradiated in a thermal neutron spectrum. Annals of Nuclear Energy, 183, Article 109645. https://doi.org/10.1016/j.anucene.2022.109645

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abstract = "A post-irradiation examination (PIE) of an enriched uranium sample was performed to advance a nuclear forensics methodology, based on intra-elemental nuclide ratios. The PIE was carried out on a few milligrams of low enriched uranium dioxide (LEUO2) sample, irradiated to a burnup of 1 GWd/MTU. The PIE of the LEUO2 sample provided the concentration of selected plutonium and fission product nuclides (239Pu, 240Pu, 241Pu, 91Y, 95Zr, 95Nb, 103Ru, 133Cs, 134Cs, 135Cs, 137Cs, 136Ba, 138Ba, 140Ba, 140La, 141Ce, 144Ce, 149Sm, 150Sm, 152Sm, 153Eu, and 154Eu). The PIE supported validation of the MCNP (Monte Carlo N-Particle neutronics simulation code) predicted concentration of these nuclides in the irradiated LEUO2 sample. This study showed that most of the MCNP predicted nuclide concentrations were within 15% and several within 10% compared to the PIE results. Gamma and mass spectrometry of nuclides in irradiated LEUO2 enabled the determination of uranium burnup and time since irradiation.",

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AB - A post-irradiation examination (PIE) of an enriched uranium sample was performed to advance a nuclear forensics methodology, based on intra-elemental nuclide ratios. The PIE was carried out on a few milligrams of low enriched uranium dioxide (LEUO2) sample, irradiated to a burnup of 1 GWd/MTU. The PIE of the LEUO2 sample provided the concentration of selected plutonium and fission product nuclides (239Pu, 240Pu, 241Pu, 91Y, 95Zr, 95Nb, 103Ru, 133Cs, 134Cs, 135Cs, 137Cs, 136Ba, 138Ba, 140Ba, 140La, 141Ce, 144Ce, 149Sm, 150Sm, 152Sm, 153Eu, and 154Eu). The PIE supported validation of the MCNP (Monte Carlo N-Particle neutronics simulation code) predicted concentration of these nuclides in the irradiated LEUO2 sample. This study showed that most of the MCNP predicted nuclide concentrations were within 15% and several within 10% compared to the PIE results. Gamma and mass spectrometry of nuclides in irradiated LEUO2 enabled the determination of uranium burnup and time since irradiation.

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Nondestructive and destructive assay for forensics characterization of weapons-grade plutonium produced in LEU irradiated in a thermal neutron spectrum

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