Impact of anharmonicity on the vibrational entropy and specific heat of
Abstract
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.
- Authors:
-
[1];
[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)
- Publication Date:
- Research Org.:
- 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 Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1530058
- Alternate Identifier(s):
- OSTI ID: 1546418; OSTI ID: 1558431
- Report Number(s):
- INL/JOU-19-54373-Rev000
Journal ID: ISSN 2475-9953; PRMHAR
- Grant/Contract Number:
- AC05-00OR22725; AC07-05ID14517
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Materials
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 6; Journal ID: ISSN 2475-9953
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; Specific Heat
Citation Formats
Bryan, M. S., Pang, J. W. L., Larson, B. C., Chernatynskiy, A., Abernathy, D. L., Gofryk, K., and Manley, M. E. Impact of anharmonicity on the vibrational entropy and specific heat of UO2. United States: N. p., 2019.
Web. doi:10.1103/PhysRevMaterials.3.065405.
Bryan, M. S., Pang, J. W. L., Larson, B. C., Chernatynskiy, A., Abernathy, D. L., Gofryk, K., & Manley, M. E. Impact of anharmonicity on the vibrational entropy and specific heat of UO2. United States. https://doi.org/10.1103/PhysRevMaterials.3.065405
Bryan, M. S., Pang, J. W. L., Larson, B. C., Chernatynskiy, A., Abernathy, D. L., Gofryk, K., and Manley, M. E. Fri .
"Impact of anharmonicity on the vibrational entropy and specific heat of UO2". United States. https://doi.org/10.1103/PhysRevMaterials.3.065405. https://www.osti.gov/servlets/purl/1530058.
@article{osti_1530058,
title = {Impact of anharmonicity on the vibrational entropy and specific heat of UO2},
author = {Bryan, M. S. and Pang, J. W. L. and Larson, B. C. and Chernatynskiy, A. and Abernathy, D. L. and Gofryk, K. and Manley, M. E.},
abstractNote = {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.},
doi = {10.1103/PhysRevMaterials.3.065405},
journal = {Physical Review Materials},
number = 6,
volume = 3,
place = {United States},
year = {2019},
month = {6}
}
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