Assessment of empirical interatomic potential to predict thermal conductivity in ThO2 and UO2
Abstract
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 UxTh1-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.
- Authors:
-
[1];
[2];
[5];
- 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)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Thermal Energy Transport under Irradiation
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Nuclear Energy (NE)
- OSTI Identifier:
- 1809936
- Grant/Contract Number:
- AC05-00OR22725; AC07-05ID14517
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physics. Condensed Matter
- Additional Journal Information:
- Journal Volume: 33; Journal Issue: 27; Journal ID: ISSN 0953-8984
- Publisher:
- IOP Publishing
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; phonon; thermal conductivity; phonon dispersion; phonon lifetime; density functional theory; empirical interatomic potential
Citation Formats
Jin, Miaomiao, Khafizov, Marat, Jiang, Chao, Zhou, Shuxiang, Marianetti, Chris A., Bryan, Matthew S., Manley, Michael E., and Hurley, David H. Assessment of empirical interatomic potential to predict thermal conductivity in ThO2 and UO2. United States: N. p., 2021.
Web. doi:10.1088/1361-648x/abdc8f.
Jin, Miaomiao, Khafizov, Marat, Jiang, Chao, Zhou, Shuxiang, Marianetti, Chris A., Bryan, Matthew S., Manley, Michael E., & Hurley, David H. Assessment of empirical interatomic potential to predict thermal conductivity in ThO2 and UO2. United States. https://doi.org/10.1088/1361-648x/abdc8f
Jin, Miaomiao, Khafizov, Marat, Jiang, Chao, Zhou, Shuxiang, Marianetti, Chris A., Bryan, Matthew S., Manley, Michael E., and Hurley, David H. Fri .
"Assessment of empirical interatomic potential to predict thermal conductivity in ThO2 and UO2". United States. https://doi.org/10.1088/1361-648x/abdc8f. https://www.osti.gov/servlets/purl/1809936.
@article{osti_1809936,
title = {Assessment of empirical interatomic potential to predict thermal conductivity in ThO2 and UO2},
author = {Jin, Miaomiao and Khafizov, Marat and Jiang, Chao and Zhou, Shuxiang and Marianetti, Chris A. and Bryan, Matthew S. and Manley, Michael E. and Hurley, David H.},
abstractNote = {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 UxTh1-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.},
doi = {10.1088/1361-648x/abdc8f},
journal = {Journal of Physics. Condensed Matter},
number = 27,
volume = 33,
place = {United States},
year = {Fri May 28 00:00:00 EDT 2021},
month = {Fri May 28 00:00:00 EDT 2021}
}
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