The effect of oxygen concentration on the speciation of laser ablated uranium

Burton, Mark A.; Auner, Alex W.; Crowhurst, Jonathan C.; Boone, Peter S.; Finney, Lauren A.; Weisz, David G.; Koroglu, Batikan; Jovanovic, Igor; Radousky, Harry B.; Knight, Kim B.

doi:10.1038/s41598-022-07834-9

Title: The effect of oxygen concentration on the speciation of laser ablated uranium

Journal Article · 06 March 2022 · Scientific Reports

DOI: https://doi.org/10.1038/s41598-022-07834-9 · OSTI ID:1847967

Burton, Mark A.; Auner, Alex W.; Crowhurst, Jonathan C.; Boone, Peter S.; Finney, Lauren A.; Weisz, David G.; Koroglu, Batikan; Jovanovic, Igor; Radousky, Harry B.; Knight, Kim B.

Abstract In order to model the fate and transport of particles following a nuclear explosion, there must first be an understanding of individual physical and chemical processes that affect particle formation. One interaction pertinent to fireball chemistry and resultant debris formation is that between uranium and oxygen. In this study, we use laser ablation of uranium metal in different concentrations of oxygen gas, either ¹⁶ O ₂ or ¹⁸ O ₂ , to determine the influence of oxygen on rapidly cooling uranium. Analysis of recovered particulates using infrared absorption and Raman spectroscopies indicate that the micrometer-sized particulates are predominantly amorphous UO _x (am-UO _x , where 3 ≤ x ≤ 4) and UO ₂ after ablation in 1 atm of pure O ₂ and a 1% O ₂ /Ar mixture, respectively. Energy dispersive X-ray spectroscopy (EDS) of particulates formed in pure O ₂ suggest an O/U ratio of ~ 3.7, consistent with the vibrational spectroscopy analysis. Both am-UO _x and UO ₂ particulates convert to α-U ₃ O ₈ when heated. Lastly, experiments performed in ¹⁸ O ₂ environments show the formation of ¹⁸ O-substituted uranium oxides; vibrational frequencies for am-U ¹⁸ O _x are reported for the first time. When compared to literature, this work shows that cooling timescales can affect the structural composition of uranium oxides (i.e., crystalline vs. amorphous). This indicator can be used in current models of nuclear explosions to improve our predicative capabilities of chemical speciation.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Univ. of Michigan, Ann Arbor, MI (United States)

Sponsoring Organization:: USDOE; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344; NA0003920

OSTI ID:: 1847967

Report Number(s):: LLNL-JRNL-826652; 4030; PII: 7834

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Journal Issue: 1 Vol. 12; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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Title: The effect of oxygen concentration on the speciation of laser ablated uranium

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