Computationally Guided Investigation of the Optical Spectra of Pure β-UO3

Spano, Tyler L.; Shields, Ashley E.; Barth, Brianna S.; Gruidl, Jeremiah D.; Niedziela, Jennifer L.; Kapsimalis, Roger J.; Miskowiec, Andrew

doi:10.1021/acs.inorgchem.0c01279

Computationally Guided Investigation of the Optical Spectra of Pure β-UO₃

Journal Article · Fri Jul 24 00:00:00 EDT 2020 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.0c01279· OSTI ID:1649257

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Texas, Austin, TX (United States)

Single-phase β-UO₃ is synthesized by flash heating UO₂(NO₃)·6H₂O in air to 450 °C and annealing for 60 h under the same conditions. For the first time, we report the Raman spectra of pure β-UO₃. To facilitate the assignment of Raman and infrared vibrational modes, we use density functional theory with density functional perturbation theory. By employing a novel analysis scheme that includes the mode frequencies as well as a quantitative analysis of the mode eigenvectors, we assign the observed spectral features to individual chemical modes. In particular, the density functional theory optimized structure, observed Raman spectrum, and eigenvector analysis suggest the presence of four crystallographically distinct uranyl ions, one more than has previously been suggested.

View Accepted Manuscript (DOE)

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

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

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1649257

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 16 Vol. 59; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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