Assessment of empirical interatomic potential to predict thermal conductivity in ThO2 and UO2

Jin, Miaomiao; Khafizov, Marat; Jiang, Chao; Zhou, Shuxiang; Marianetti, Chris A.; Bryan, Matthew S.; Manley, Michael E.; Hurley, David H.

doi:10.1088/1361-648x/abdc8f

Assessment of empirical interatomic potential to predict thermal conductivity in ThO₂ and UO₂

Journal Article · Fri May 28 00:00:00 EDT 2021 · Journal of Physics. Condensed Matter

DOI:https://doi.org/10.1088/1361-648x/abdc8f· OSTI ID:1809936

^[1]; ^[2]; Jiang, Chao ^[3]; Zhou, Shuxiang ^[3]; Marianetti, Chris A. ^[4]; Bryan, Matthew S. ^[5]; ^[5]; Hurley, David H. ^[3]

Pennsylvania State Univ., University Park, PA (United States)
The Ohio State Univ., Columbus, OH (United States)
Idaho National Lab. (INL), Idaho Falls, ID (United States)
Columbia Univ., New York, NY (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Computing vibrational properties of crystals in the presence of complex defects often necessitates the use of (semi-)empirical potentials, which are typically not well characterized for perfect crystals. In this study we explore the efficacy of a commonly used embedded-atomempirical interatomic potential for the U_xTh_1-xO₂ system, to compute phonon dispersion, lifetime, and branch specific thermal conductivity. Our approach for ThO₂ involves using lattice dynamics and the linearized Boltzmann transport equation to calculate phonon transport properties based on second and third order force constants derived from the empirical potential and from first-principles calculations. For UO₂, to circumvent the accuracy issues associated with first-principles treatments of strong electronic correlations, we compare results derived from the empirical interatomic potential to previous experimental results. It is found that the empirical potential can reasonably capture the dispersion of acoustic branches, but exhibits significant discrepancies for the optical branches, leading to overestimation of phonon lifetime and thermal conductivity. The branch specific conductivity also differs significantly with either first-principles based results (ThO₂) or experimental measurements (UO₂). These findings suggest that the empirical potential needs to be further optimized for robust prediction of thermal conductivity both in perfect crystals and in the presence of complex defects.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Thermal Energy Transport under Irradiation; Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; AC07-05ID14517

OSTI ID:: 1809936

Alternate ID(s):: OSTI ID: 23181268

Journal Information:: Journal of Physics. Condensed Matter, Journal Name: Journal of Physics. Condensed Matter Journal Issue: 27 Vol. 33; ISSN 0953-8984

Publisher:: IOP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

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Assessment of empirical interatomic potential to predict thermal conductivity in ThO2 and UO2

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Assessment of empirical interatomic potential to predict thermal conductivity in ThO₂ and UO₂