Revisiting lattice thermal transport in PbTe: The crucial role of quartic anharmonicity
Here, we perform a firstprinciples study of lattice thermal transport in PbTe by explicitly considering anharmonicity up to 4th order. To determine the temperaturedependent 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 moderesolved phonon lifetimes by including both three and fourphonon 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) fourphonon scatterings are responsible for severe reduction in κ _{l} on top of threephonon 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 fourphonon 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 firstprinciples calculations including highorder anharmonicity.
 Authors:

^{[1]}
 Univ. of California, Los Angeles, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
 Publication Date:
 Grant/Contract Number:
 AC0206CH11357
 Type:
 Accepted Manuscript
 Journal Name:
 Applied Physics Letters
 Additional Journal Information:
 Journal Volume: 113; Journal Issue: 7; Journal ID: ISSN 00036951
 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) (SC22). 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 firstprinciples study of lattice thermal transport in PbTe by explicitly considering anharmonicity up to 4th order. To determine the temperaturedependent 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 moderesolved phonon lifetimes by including both three and fourphonon 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) fourphonon scatterings are responsible for severe reduction in κl on top of threephonon 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 fourphonon 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 firstprinciples calculations including highorder anharmonicity.},
doi = {10.1063/1.5040887},
journal = {Applied Physics Letters},
number = 7,
volume = 113,
place = {United States},
year = {2018},
month = {8}
}
Works referenced in this record:
High Lattice Thermal Conductivity Solids
book, January 2006
book, January 2006
 Morelli, Donald T.; Slack, Glen A.; Shind�, Subhash L.
 High Thermal Conductivity Materials, p. 3768
Generalized Gradient Approximation Made Simple
journal, October 1996
journal, October 1996
 Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
 Physical Review Letters, Vol. 77, Issue 18, p. 38653868
Giant anharmonic phonon scattering in PbTe
journal, June 2011
journal, June 2011
 Delaire, O.; Ma, J.; Marty, K.
 Nature Materials, Vol. 10, Issue 8, p. 614619
Intrinsically Minimal Thermal Conductivity in Cubic $\mathrm{I}\mathrm{\text{?}}\mathrm{V}\mathrm{\text{?}}{\mathrm{VI}}_{2}$ Semiconductors
journal, July 2008
journal, July 2008
 Morelli, D. T.; Jovovic, V.; Heremans, J. P.
 Physical Review Letters, Vol. 101, Issue 3, Article No. 035901
Convergence of electronic bands for high performance bulk thermoelectrics
journal, May 2011
journal, May 2011
 Pei, Yanzhong; Shi, Xiaoya; LaLonde, Aaron
 Nature, Vol. 473, Issue 7345, p. 6669
High Performance Thermoelectricity in EarthAbundant Compounds Based on Natural Mineral Tetrahedrites
journal, October 2012
journal, October 2012
 Lu, Xu; Morelli, Donald T.; Xia, Yi
 Advanced Energy Materials, Vol. 3, Issue 3, p. 342348
Enhancement of Thermoelectric Efficiency in PbTe by Distortion of the Electronic Density of States
journal, July 2008
journal, July 2008
 Heremans, J. P.; Jovovic, V.; Toberer, E. S.
 Science, Vol. 321, Issue 5888, p. 554557
Ultralow thermal conductivity and high thermoelectric figure of merit in SnSe crystals
journal, April 2014
journal, April 2014
 Zhao, LiDong; Lo, ShihHan; Zhang, Yongsheng
 Nature, Vol. 508, Issue 7496, p. 373377