Phonon modal analysis of thermal transport in ThO2 with point defects using equilibrium molecular dynamics

Chen, Beihan; Malakkal, Linu; Khafizov, Marat; Hurley, David H.; Jin, Miaomiao

doi:10.1016/j.jnucmat.2024.155314

Phonon modal analysis of thermal transport in ThO₂ with point defects using equilibrium molecular dynamics

Journal Article · Mon Aug 05 00:00:00 EDT 2024 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2024.155314· OSTI ID:2448559

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Pennsylvania State Univ., University Park, PA (United States)
Idaho National Laboratory (INL), Idaho Falls, ID (United States)
The Ohio State Univ., Columbus, OH (United States)

Defects can significantly degrade the thermal conductivity of ThO₂, an advanced nuclear fuel material as well as a surrogate for other fluorite-structured materials. Here, we investigate how point defects in ThO₂ impact phonon mode-resolved thermal transport. By incorporating phonon modes from lattice dynamics, we decompose the trajectory and heat flux to phonon normal mode space and extract key phonon properties, including phonon relaxation times and their contributions to thermal conductivity. We implement two methods. The first method is based on the Green Kubo formalism to resolve the contribution of each phonon mode to thermal conductivity. The second resolves the lifetime of individual phonon modes and the thermal conductivity is calculated using the Boltzmann transport equation within relaxation time approximation. Notably, a lower contribution of acoustic modes is revealed compared to perturbative approaches considering only three-phonon scattering processes. The effects of four types of point defects are evaluated. The strongest impact on a reduction in thermal conductivity is from Th interstitials, followed by Th vacancies. O interstitials/vacancies have a similar impact, albeit smaller than defects on the thorium sublattice. These observations are consistent with previous studies.

View Accepted Manuscript (DOE)

Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

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

Grant/Contract Number:: AC07-05ID14517

OSTI ID:: 2448559

Report Number(s):: INL/JOU--24-76683-Rev000

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Vol. 601; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Phonon modal analysis of thermal transport in ThO2 with point defects using equilibrium molecular dynamics

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Phonon modal analysis of thermal transport in ThO₂ with point defects using equilibrium molecular dynamics