Computational insights into the lattice dynamics of Pu(IV) oxalates

Isbill, Sara B.; Ciprian, Elodia; Christian, Jonathan H.; Hixon, Amy; Foley, Bryan J.; Villa-Aleman, Eliel; Miskowiec, Andrew J.

doi:10.1016/j.jnucmat.2022.154106

Computational insights into the lattice dynamics of Pu(IV) oxalates

Journal Article · Sun Oct 30 00:00:00 EDT 2022 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2022.154106· OSTI ID:1899009

^[1]; Ciprian, Elodia ^[2]; Christian, Jonathan H. ^[3]; ^[2]; Foley, Bryan J. ^[4]; Villa-Aleman, Eliel ^[4]; ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Notre Dame, IN (United States)
Univ. of Notre Dame, IN (United States); Savannah River National Laboratory (SRNL), Aiken, SC (United States)
Savannah River National Laboratory (SRNL), Aiken, SC (United States)

Despite its use in PuO₂ production, the structure of anhydrous Pu(C₂O₄)₂ is still not completely understood. Recently, two candidate structures for Pu(C₂O₄)₂ were proposed via density functional theory (DFT), after which the first experimental optical vibrational spectra were reported. Here, in this study, we calculated the lattice dynamics of the candidate structures using DFT and found that the primary difference between them is the presence of a vibrational mode near 1380 cm^-1 in one structure. The frequency and optical activity of this mode agree well with the published experimental results, providing strong support for this calculated structure as that of anhydrous Pu(C₂O₄)₂.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: 89303321CEM000080; AC05-00OR22725

OSTI ID:: 1899009

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Vol. 573; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
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Computational insights into the lattice dynamics of Pu(IV) oxalates

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Figures / Tables (6)

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