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Title: Dominant effect of anharmonicity on the equation of state and thermal conductivity of MgO under extreme conditions

Abstract

Understanding heat transfer in the earth mantle region is of great scientific interest but highly challenging due to dissimilar conditions from our daily lives. Thermal conductivity of highly pressured and thermally activated materials can be completely different from that at ambient condition. In this study we calculate the equation of state and thermal conductivity of cubic crystalline MgO, a major component of the mantle, in such an environment. It is shown that the material properties are not accurately captured unless rigorous treatment of anharmonicity of phonon vibrational motion is explicitly applied. To predict renormalized phonon dispersion relations, interatomic force constants of high-order expansion are required, especially at elevated temperature. The anharmonicity plays an increasingly substantial role for regulating volume expansion as temperature rises, because the Gibbs free energy of MgO considerably deviates from what was predicted by the quasiharmonic approximation. We find that the lattice thermal conductivity of MgO and the heat transfer of the earth's mantle are reliably estimated only when both the temperature-dependent renormalization of phonon frequencies and four-phonon scattering effects are taken into consideration. We map the characteristics at Geotherm into contour diagrams in which equilibrium volumes and the thermal conductivities are described as functions of temperaturemore » and pressure. Furthermore, the thermal conductivity values of MgO in this study are smaller than those in previous theoretical studies due to the additional incorporation of four-phonon scatterings in the calculations. Specifically, deviation between the values in previous studies and in this study becomes larger as thermodynamic variables reach those near the core-mantle boundary. For instance, thermal conductivities of 52.15 and 23.67 Wm-1K-1 are estimated at ambient and extreme conditions (T = 4000K and P = 135 GPa), respectively.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]
  1. Yonsei Univ., Seoul (South Korea)
  2. Northwestern Univ., Evanston, IL (United States)
  3. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Research Foundation of Korea (NRF)
OSTI Identifier:
1734608
Report Number(s):
LLNL-JRNL-812456
Journal ID: ISSN 2469-9950; 1019717
Grant/Contract Number:  
AC52-07NA27344; 2016M2B2B1945254; 2017M2A8A5014754
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 102; Journal Issue: 18; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; Anharmonic lattice dynamics; equations of state; lattice dynamics; phonons; thermal conductivity; density functional calculations; first-principles calculations

Citation Formats

Kwon, Choah, Xia, Yi, Zhou, Fei, and Han, Byungchan. Dominant effect of anharmonicity on the equation of state and thermal conductivity of MgO under extreme conditions. United States: N. p., 2020. Web. https://doi.org/10.1103/physrevb.102.184309.
Kwon, Choah, Xia, Yi, Zhou, Fei, & Han, Byungchan. Dominant effect of anharmonicity on the equation of state and thermal conductivity of MgO under extreme conditions. United States. https://doi.org/10.1103/physrevb.102.184309
Kwon, Choah, Xia, Yi, Zhou, Fei, and Han, Byungchan. Mon . "Dominant effect of anharmonicity on the equation of state and thermal conductivity of MgO under extreme conditions". United States. https://doi.org/10.1103/physrevb.102.184309.
@article{osti_1734608,
title = {Dominant effect of anharmonicity on the equation of state and thermal conductivity of MgO under extreme conditions},
author = {Kwon, Choah and Xia, Yi and Zhou, Fei and Han, Byungchan},
abstractNote = {Understanding heat transfer in the earth mantle region is of great scientific interest but highly challenging due to dissimilar conditions from our daily lives. Thermal conductivity of highly pressured and thermally activated materials can be completely different from that at ambient condition. In this study we calculate the equation of state and thermal conductivity of cubic crystalline MgO, a major component of the mantle, in such an environment. It is shown that the material properties are not accurately captured unless rigorous treatment of anharmonicity of phonon vibrational motion is explicitly applied. To predict renormalized phonon dispersion relations, interatomic force constants of high-order expansion are required, especially at elevated temperature. The anharmonicity plays an increasingly substantial role for regulating volume expansion as temperature rises, because the Gibbs free energy of MgO considerably deviates from what was predicted by the quasiharmonic approximation. We find that the lattice thermal conductivity of MgO and the heat transfer of the earth's mantle are reliably estimated only when both the temperature-dependent renormalization of phonon frequencies and four-phonon scattering effects are taken into consideration. We map the characteristics at Geotherm into contour diagrams in which equilibrium volumes and the thermal conductivities are described as functions of temperature and pressure. Furthermore, the thermal conductivity values of MgO in this study are smaller than those in previous theoretical studies due to the additional incorporation of four-phonon scatterings in the calculations. Specifically, deviation between the values in previous studies and in this study becomes larger as thermodynamic variables reach those near the core-mantle boundary. For instance, thermal conductivities of 52.15 and 23.67 Wm-1K-1 are estimated at ambient and extreme conditions (T = 4000K and P = 135 GPa), respectively.},
doi = {10.1103/physrevb.102.184309},
journal = {Physical Review B},
number = 18,
volume = 102,
place = {United States},
year = {2020},
month = {11}
}

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