Impact of anharmonicity on the vibrational entropy and specific heat of UO2

Bryan, M. S.; Pang, J. W.  L.; Larson, B. C.; Chernatynskiy, A.; Abernathy, D. L.; Gofryk, K.; Manley, M. E.

doi:10.1103/PhysRevMaterials.3.065405

Title: Impact of anharmonicity on the vibrational entropy and specific heat of ${UO}_{2}$

Journal Article · Fri Jun 28 00:00:00 EDT 2019 · Physical Review Materials

DOI:https://doi.org/10.1103/PhysRevMaterials.3.065405· OSTI ID:1530058

Bryan, M. S. ^[1]; Pang, J. W. L. ^[1]; Larson, B. C. ^[1]; Chernatynskiy, A. ^[2];

^[1]; Gofryk, K. ^[3];

^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Missouri Univ. of Science and Technology, Rolla, MO (United States)
Idaho National Lab. (INL), Idaho Falls, ID (United States)

The impact of anharmonicity on the vibrational entropy and heat capacity of UO2 has been investigated from 10 K to 1200 K using inelastic neutron scattering measurements of the phonon density of states (PDOS). Small changes in the PDOS are observed from 10 K to 295 K, with more noticeable changes appearing in the 750 K and 1200 K data. The specific heat determined from the PDOS measurements is in agreement with macroscopic specific heat measurements and the overall impact of non-dilation anharmonicity on the specific heat has been shown to be less than 2 percent. An analysis of the phonon measurements shows that the softening of acoustic phonons with temperature is consistent with the quasiharmonic approximation. The optical phonons deviate from the quasiharmonic prediction, with the low energy optical phonons between approximately 20-50 meV softening more than expected, while the higher energy optical phonons between approximately 50-80 meV have no appreciable softening over the temperature range measured. The observation of a small anharmonic specific heat contribution has been shown to be the result of relatively large energy dependent anharmonic effects which have opposite sign, leading to a total contribution near zero.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Thermal Energy Transport under Irradiation (TETI); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Idaho National Lab. (INL), Idaho Falls, ID (United States)

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

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

OSTI ID:: 1530058

Alternate ID(s):: OSTI ID: 1546418; OSTI ID: 1558431

Report Number(s):: INL/JOU-19-54373-Rev000; PRMHAR

Journal Information:: Physical Review Materials, Vol. 3, Issue 6; ISSN 2475-9953

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 13 works

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