Phonon Thermal Transport in ${\mathrm{UO}}_{2}$ via Self-Consistent Perturbation Theory

Phonon Thermal Transport in ${UO}_{2}$ via Self-Consistent Perturbation Theory

Shuxiang Zhou, Enda Xiao, Hao Ma, Krzysztof Gofryk, Chao Jiang, Michael E. Manley, David H. Hurley, and Chris A. Marianetti

Phys. Rev. Lett. 132, 106502 – Published 6 March 2024

Abstract

Computing thermal transport from first-principles in ${UO}_{2}$ is complicated due to the challenges associated with Mott physics. Here, we use irreducible derivative approaches to compute the cubic and quartic phonon interactions in ${UO}_{2}$ from first principles, and we perform enhanced thermal transport computations by evaluating the phonon Green’s function via self-consistent diagrammatic perturbation theory. Our predicted phonon lifetimes at $T = 600 K$ agree well with our inelastic neutron scattering measurements across the entire Brillouin zone, and our thermal conductivity predictions agree well with previous measurements. Both the changes due to thermal expansion and self-consistent contributions are nontrivial at high temperatures, though the effects tend to cancel, and interband transitions yield a substantial contribution.

Received 13 October 2023
Revised 17 January 2024
Accepted 12 February 2024

DOI:https://doi.org/10.1103/PhysRevLett.132.106502

Physics Subject Headings (PhySH)

Lattice thermal conductivity Phonons Thermal conductivity

Mott insulators Strongly correlated systems

DFT+U Density functional theory

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Shuxiang Zhou ¹, Enda Xiao², Hao Ma ^3,4, Krzysztof Gofryk ¹, Chao Jiang¹, Michael E. Manley ³, David H. Hurley¹, and Chris A. Marianetti⁵

¹Idaho National Laboratory, Idaho Falls, Idaho 83415, USA
²Department of Chemistry, Columbia University, New York, New York 10027, USA
³Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
⁴Department of Thermal Science and Energy Engineering, University of Science and Technology of China, Hefei, Anhui 230026, China
⁵Department of Applied Physics and Applied Mathematics, Columbia University, New York, New York 10027, USA