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Phonon Thermal Transport in UO2 via Self-Consistent Perturbation Theory

Journal Article · · Physical Review Letters
 [1];  [2];  [3];  [1];  [1];  [4];  [1];  [2]
  1. Idaho National Laboratory (INL), Idaho Falls, ID (United States)
  2. Columbia Univ., New York, NY (United States)
  3. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Science and Technology of China, Hefei (China)
  4. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
+ Show Author Affiliations
Computing thermal transport from first-principles in UO2 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 UO2 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. Finally, 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.
Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Thermal Energy Transport under Irradiation (TETI); Idaho National Laboratory (INL), Idaho Falls, ID (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); 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); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-05CH11231; AC05-00OR22725; AC07-05ID14517; SC0016507
OSTI ID:
2371876
Alternate ID(s):
OSTI ID: 2428040
OSTI ID: 2474414
Report Number(s):
INL/JOU--23-74435-Rev000
Journal Information:
Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 10 Vol. 132; ISSN 0031-9007
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

36 MATERIALS SCIENCE
phonon
self-consistent perturbation theory
thermal transport
uranium dioxide