Investigating rapid alpha-decay induced aging of 238PuO2 by Raman Spectroscopy

Luke R. Sadergaski; Don D. Dick; Jason R. Darvin; Eliel Villa-Aleman; David Abrecht; Lucas Sweet

doi:10.1016/j.jssc.2025.125670

Investigating rapid alpha-decay induced aging of ²³⁸PuO₂ by Raman Spectroscopy

Luke R. Sadergaski, Don D. Dick, Jason R. Darvin, Eliel Villa-Aleman, David Abrecht, Lucas Sweet

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

Abstract

Investigating alpha-decay induced aging in PuO₂ is useful in nuclear forensics; helping to determine the time since last calcination. This was previously investigate by monitoring the damage to ²⁴⁰PuO₂ over the course of a few years. The rate of alpha-decay induced aging has long been assumed to scale only with the decay rate of other isotopes without direct verification. This article reports the first alpha-decay aging study of ²³⁸PuO₂ by Raman spectroscopy. Contrary to the expected 10 days for ²³⁸PuO₂ to reach steady state based on ²⁴⁰PuO₂ studies, the alpha aging curve reached an approximate steady state ∼24–30 h after laser annealing. While the cause of the order of magnitude decrease is unknown, it is speculated that dynamic annealing could contribute to the differences in rate of induced aging. The Raman spectra of annealed and aged ²³⁸PuO₂ matched the expected features in ²³⁹PuO₂ and ²⁴⁰PuO₂ spectra; showing no formation of new stable chemical species in the material such as secondary Pu oxide phases (e.g., Pu₄O₉). Results indicate that ²³⁸Pu could be leveraged for rapid alpha-decay aging studies to characterize alpha-decay induced features and better understand matrix temperatures and the annealing of Frankel pair defects.

Original language	English
Article number	125670
Journal	Journal of Solid State Chemistry
Volume	353
DOIs	https://doi.org/10.1016/j.jssc.2025.125670
State	Published - Jan 2026

Funding

This manuscript has been authored by UT-Battelle LLC under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).This work was funded by the US Department of Energy, National Nuclear Security Administration, Office of Defense Nuclear Nonproliferation Research and Development. Oak Ridge National Laboratory is managed by UT-Battelle LLC for the US Department of Energy under contract DE-AC05-00OR22725. This work was funded by the US Department of Energy , National Nuclear Security Administration , Office of Defense Nuclear Nonproliferation Research and Development . Oak Ridge National Laboratory is managed by UT-Battelle LLC for the US Department of Energy under contract DE-AC05-00OR22725. The authors wish to thank Jeffery Sharpe, Nathan Simms, Sara Gilson, and Tony Dyer for assistance with preparing the 238 Pu sample. This work was supported by the US National Nuclear Security Administration. This manuscript has been authored by UT-Battelle LLC under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting the article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).

Keywords

Actinide
Alpha decay
Chemometrics
Nuclear forensics
Optical spectroscopy
Plutonium

Access to Document

10.1016/j.jssc.2025.125670

Cite this

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title = "Investigating rapid alpha-decay induced aging of 238PuO2 by Raman Spectroscopy",

abstract = "Investigating alpha-decay induced aging in PuO2 is useful in nuclear forensics; helping to determine the time since last calcination. This was previously investigate by monitoring the damage to 240PuO2 over the course of a few years. The rate of alpha-decay induced aging has long been assumed to scale only with the decay rate of other isotopes without direct verification. This article reports the first alpha-decay aging study of 238PuO2 by Raman spectroscopy. Contrary to the expected 10 days for 238PuO2 to reach steady state based on 240PuO2 studies, the alpha aging curve reached an approximate steady state ∼24–30 h after laser annealing. While the cause of the order of magnitude decrease is unknown, it is speculated that dynamic annealing could contribute to the differences in rate of induced aging. The Raman spectra of annealed and aged 238PuO2 matched the expected features in 239PuO2 and 240PuO2 spectra; showing no formation of new stable chemical species in the material such as secondary Pu oxide phases (e.g., Pu4O9). Results indicate that 238Pu could be leveraged for rapid alpha-decay aging studies to characterize alpha-decay induced features and better understand matrix temperatures and the annealing of Frankel pair defects.",

keywords = "Actinide, Alpha decay, Chemometrics, Nuclear forensics, Optical spectroscopy, Plutonium",

author = "Sadergaski, \{Luke R.\} and Dick, \{Don D.\} and Darvin, \{Jason R.\} and Eliel Villa-Aleman and David Abrecht and Lucas Sweet",

note = "Publisher Copyright: {\textcopyright} 2025",

year = "2026",

month = jan,

doi = "10.1016/j.jssc.2025.125670",

language = "English",

volume = "353",

journal = "Journal of Solid State Chemistry",

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T1 - Investigating rapid alpha-decay induced aging of 238PuO2 by Raman Spectroscopy

AU - Sadergaski, Luke R.

AU - Dick, Don D.

AU - Darvin, Jason R.

AU - Villa-Aleman, Eliel

AU - Abrecht, David

AU - Sweet, Lucas

PY - 2026/1

Y1 - 2026/1

N2 - Investigating alpha-decay induced aging in PuO2 is useful in nuclear forensics; helping to determine the time since last calcination. This was previously investigate by monitoring the damage to 240PuO2 over the course of a few years. The rate of alpha-decay induced aging has long been assumed to scale only with the decay rate of other isotopes without direct verification. This article reports the first alpha-decay aging study of 238PuO2 by Raman spectroscopy. Contrary to the expected 10 days for 238PuO2 to reach steady state based on 240PuO2 studies, the alpha aging curve reached an approximate steady state ∼24–30 h after laser annealing. While the cause of the order of magnitude decrease is unknown, it is speculated that dynamic annealing could contribute to the differences in rate of induced aging. The Raman spectra of annealed and aged 238PuO2 matched the expected features in 239PuO2 and 240PuO2 spectra; showing no formation of new stable chemical species in the material such as secondary Pu oxide phases (e.g., Pu4O9). Results indicate that 238Pu could be leveraged for rapid alpha-decay aging studies to characterize alpha-decay induced features and better understand matrix temperatures and the annealing of Frankel pair defects.

AB - Investigating alpha-decay induced aging in PuO2 is useful in nuclear forensics; helping to determine the time since last calcination. This was previously investigate by monitoring the damage to 240PuO2 over the course of a few years. The rate of alpha-decay induced aging has long been assumed to scale only with the decay rate of other isotopes without direct verification. This article reports the first alpha-decay aging study of 238PuO2 by Raman spectroscopy. Contrary to the expected 10 days for 238PuO2 to reach steady state based on 240PuO2 studies, the alpha aging curve reached an approximate steady state ∼24–30 h after laser annealing. While the cause of the order of magnitude decrease is unknown, it is speculated that dynamic annealing could contribute to the differences in rate of induced aging. The Raman spectra of annealed and aged 238PuO2 matched the expected features in 239PuO2 and 240PuO2 spectra; showing no formation of new stable chemical species in the material such as secondary Pu oxide phases (e.g., Pu4O9). Results indicate that 238Pu could be leveraged for rapid alpha-decay aging studies to characterize alpha-decay induced features and better understand matrix temperatures and the annealing of Frankel pair defects.

KW - Actinide

KW - Alpha decay

KW - Chemometrics

KW - Nuclear forensics

KW - Optical spectroscopy

KW - Plutonium

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