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Title: Revisiting lattice thermal transport in PbTe: The crucial role of quartic anharmonicity

Here, we perform a first-principles study of lattice thermal transport in PbTe by explicitly considering anharmonicity up to 4th order. To determine the temperature-dependent lattice constant of PbTe beyond quasiharmonic approximation, we introduce a simple yet effective scheme to account for anharmonic phonon renormalization at finite temperature. Moreover, we explicitly compute mode-resolved phonon lifetimes by including both three- and four-phonon scatterings. We find that (1) anharmonic phonon renormalization leads to strong vibrational frequency shifts which improve the agreement between simulated and experimental lattice constants; (2) these frequency shifts lead to a significant increase in lattice thermal conductivity (κ l) because of reduced phonon scattering phase space; and (3) four-phonon scatterings are responsible for severe reduction in κ l on top of three-phonon scatterings, making κ l consistent with experiments. Our results suggest that the predicted κ l and its temperature dependence without considering thermal expansion, anharmonic phonon renormalization and four-phonon scatterings could accidentally agree with experiments due to error cancellation. Our study not only deepens the understanding of lattice thermal transport in PbTe but also exemplifies a widely applicable approach to investigate lattice dynamics and thermal transport properties from first-principles calculations including high-order anharmonicity.
Authors:
 [1]
  1. Univ. of California, Los Angeles, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Applied Physics Letters
Additional Journal Information:
Journal Volume: 113; Journal Issue: 7; Journal ID: ISSN 0003-6951
Publisher:
American Institute of Physics (AIP)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; Midwest Integrated Center for Computational Materials (MICCoM)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1472120
Alternate Identifier(s):
OSTI ID: 1464318

Xia, Yi. Revisiting lattice thermal transport in PbTe: The crucial role of quartic anharmonicity. United States: N. p., Web. doi:10.1063/1.5040887.
Xia, Yi. Revisiting lattice thermal transport in PbTe: The crucial role of quartic anharmonicity. United States. doi:10.1063/1.5040887.
Xia, Yi. 2018. "Revisiting lattice thermal transport in PbTe: The crucial role of quartic anharmonicity". United States. doi:10.1063/1.5040887.
@article{osti_1472120,
title = {Revisiting lattice thermal transport in PbTe: The crucial role of quartic anharmonicity},
author = {Xia, Yi},
abstractNote = {Here, we perform a first-principles study of lattice thermal transport in PbTe by explicitly considering anharmonicity up to 4th order. To determine the temperature-dependent lattice constant of PbTe beyond quasiharmonic approximation, we introduce a simple yet effective scheme to account for anharmonic phonon renormalization at finite temperature. Moreover, we explicitly compute mode-resolved phonon lifetimes by including both three- and four-phonon scatterings. We find that (1) anharmonic phonon renormalization leads to strong vibrational frequency shifts which improve the agreement between simulated and experimental lattice constants; (2) these frequency shifts lead to a significant increase in lattice thermal conductivity (κl) because of reduced phonon scattering phase space; and (3) four-phonon scatterings are responsible for severe reduction in κl on top of three-phonon scatterings, making κl consistent with experiments. Our results suggest that the predicted κl and its temperature dependence without considering thermal expansion, anharmonic phonon renormalization and four-phonon scatterings could accidentally agree with experiments due to error cancellation. Our study not only deepens the understanding of lattice thermal transport in PbTe but also exemplifies a widely applicable approach to investigate lattice dynamics and thermal transport properties from first-principles calculations including high-order anharmonicity.},
doi = {10.1063/1.5040887},
journal = {Applied Physics Letters},
number = 7,
volume = 113,
place = {United States},
year = {2018},
month = {8}
}

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