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

Abstract

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:
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)
OSTI Identifier:
1472120
Alternate Identifier(s):
OSTI ID: 1464318
Grant/Contract Number:  
AC02-06CH11357
Resource 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)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Xia, Yi. Revisiting lattice thermal transport in PbTe: The crucial role of quartic anharmonicity. United States: N. p., 2018. 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. Mon . "Revisiting lattice thermal transport in PbTe: The crucial role of quartic anharmonicity". United States. doi:10.1063/1.5040887. https://www.osti.gov/servlets/purl/1472120.
@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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Cited by: 7 works
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Works referenced in this record:

Strong anharmonicity in the phonon spectra of PbTe and SnTe from first principles
journal, January 2018

  • Ribeiro, Guilherme A. S.; Paulatto, Lorenzo; Bianco, Raffaello
  • Physical Review B, Vol. 97, Issue 1
  • DOI: 10.1103/PhysRevB.97.014306

High Lattice Thermal Conductivity Solids
book, January 2006

  • Morelli, Donald T.; Slack, Glen A.; Shindé, Subhash L.
  • High Thermal Conductivity Materials, p. 37-68
  • DOI: 10.1007/0-387-25100-6_2

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Phonon Self-Energy and Origin of Anomalous Neutron Scattering Spectra in SnTe and PbTe Thermoelectrics
journal, April 2014


Intrinsic lattice thermal conductivity of semiconductors from first principles
journal, December 2007

  • Broido, D. A.; Malorny, M.; Birner, G.
  • Applied Physics Letters, Vol. 91, Issue 23
  • DOI: 10.1063/1.2822891

ShengBTE: A solver of the Boltzmann transport equation for phonons
journal, June 2014

  • Li, Wu; Carrete, Jesús; A. Katcho, Nebil
  • Computer Physics Communications, Vol. 185, Issue 6
  • DOI: 10.1016/j.cpc.2014.02.015

Giant anharmonic phonon scattering in PbTe
journal, June 2011

  • Delaire, O.; Ma, J.; Marty, K.
  • Nature Materials, Vol. 10, Issue 8, p. 614-619
  • DOI: 10.1038/nmat3035

Quantum mechanical prediction of four-phonon scattering rates and reduced thermal conductivity of solids
journal, January 2016


Lattice thermal transport in group II-alloyed PbTe
journal, April 2018

  • Xia, Yi; Hodges, James M.; Kanatzidis, Mercouri G.
  • Applied Physics Letters, Vol. 112, Issue 18
  • DOI: 10.1063/1.5002587

Influence of structural defects on the thermal conductivity of polycrystalline and single-crystal PbTe
journal, July 2012


Four-phonon scattering significantly reduces intrinsic thermal conductivity of solids
journal, October 2017


Thermal conductivity in PbTe from first principles
journal, June 2015


Direct Evidence of Cation Disorder in Thermoelectric Lead Chalcogenides PbTe and PbS
journal, June 2013

  • Kastbjerg, Sofie; Bindzus, Niels; Søndergaard, Martin
  • Advanced Functional Materials, Vol. 23, Issue 44
  • DOI: 10.1002/adfm.201300722

All-scale hierarchical thermoelectrics: MgTe in PbTe facilitates valence band convergence and suppresses bipolar thermal transport for high performance
journal, January 2013

  • Zhao, L. D.; Wu, H. J.; Hao, S. Q.
  • Energy & Environmental Science, Vol. 6, Issue 11
  • DOI: 10.1039/c3ee42187b

Resonant bonding leads to low lattice thermal conductivity
journal, April 2014

  • Lee, Sangyeop; Esfarjani, Keivan; Luo, Tengfei
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4525

Thermophysical properties of polycrystalline PbS, PbSe, and PbTe in the temperature range 300?700 K
journal, September 1983

  • El-Sharkawy, A. A.; Abou El-Azm, A. M.; Kenawy, M. I.
  • International Journal of Thermophysics, Vol. 4, Issue 3
  • DOI: 10.1007/BF00502357

Submillimeter spectroscopy of TO-phonon mode softening in PbTe
journal, January 1977

  • Burkhard, H.; Bauer, G.; Lopez-Otero, A.
  • Journal of the Optical Society of America, Vol. 67, Issue 7
  • DOI: 10.1364/JOSA.67.000943

Temperature dependent effective potential method for accurate free energy calculations of solids
journal, March 2013


The self-consistent ab initio lattice dynamical method
journal, January 2009


Intrinsically Minimal Thermal Conductivity in Cubic IVVI2 Semiconductors
journal, July 2008


Convergence of electronic bands for high performance bulk thermoelectrics
journal, May 2011

  • Pei, Yanzhong; Shi, Xiaoya; LaLonde, Aaron
  • Nature, Vol. 473, Issue 7345, p. 66-69
  • DOI: 10.1038/nature09996

Entropically Stabilized Local Dipole Formation in Lead Chalcogenides
journal, December 2010


High Performance Thermoelectricity in Earth-Abundant Compounds Based on Natural Mineral Tetrahedrites
journal, October 2012

  • Lu, Xu; Morelli, Donald T.; Xia, Yi
  • Advanced Energy Materials, Vol. 3, Issue 3, p. 342-348
  • DOI: 10.1002/aenm.201200650

Enhancement of Thermoelectric Efficiency in PbTe by Distortion of the Electronic Density of States
journal, July 2008

  • Heremans, J. P.; Jovovic, V.; Toberer, E. S.
  • Science, Vol. 321, Issue 5888, p. 554-557
  • DOI: 10.1126/science.1159725

Anomalous thermal conductivity and suppression of negative thermal expansion in ScF 3
journal, July 2016


Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces
journal, April 2008


Lattice dynamics of anharmonic solids from first principles
journal, November 2011


Non-equilibrium processing leads to record high thermoelectric figure of merit in PbTe–SrTe
journal, July 2016

  • Tan, Gangjian; Shi, Fengyuan; Hao, Shiqiang
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms12167

Ultralow Thermal Conductivity in Full Heusler Semiconductors
journal, July 2016


Origin of anomalous anharmonic lattice dynamics of lead telluride
journal, March 2014

  • Shiga, Takuma; Murakami, Takuru; Hori, Takuma
  • Applied Physics Express, Vol. 7, Issue 4
  • DOI: 10.7567/APEX.7.041801

Lattice Anharmonicity and Thermal Conductivity from Compressive Sensing of First-Principles Calculations
journal, October 2014


Phonon conduction in PbSe, PbTe, and PbTe 1 x Se x from first-principles calculations
journal, May 2012


Ultralow thermal conductivity and high thermoelectric figure of merit in SnSe crystals
journal, April 2014

  • Zhao, Li-Dong; Lo, Shih-Han; Zhang, Yongsheng
  • Nature, Vol. 508, Issue 7496, p. 373-377
  • DOI: 10.1038/nature13184

High Performance Na-doped PbTe–PbS Thermoelectric Materials: Electronic Density of States Modification and Shape-Controlled Nanostructures
journal, October 2011

  • Girard, Steven N.; He, Jiaqing; Zhou, Xiaoyuan
  • Journal of the American Chemical Society, Vol. 133, Issue 41
  • DOI: 10.1021/ja206380h

An iterative approach to the phonon Boltzmann equation in the theory of thermal conductivity
journal, July 1995


Microscopic mechanism of low thermal conductivity in lead telluride
journal, April 2012


First-Principles Approach to Nonlinear Lattice Dynamics: Anomalous Spectra in PbTe
journal, September 2014


Beyond the isotropic-model approximation in the theory of thermal conductivity
journal, April 1996


Thermal physics of the lead chalcogenides PbS, PbSe, and PbTe from first principles
journal, May 2014


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    Promising thermoelectric materials of Cu 3 VX 4 (X=S, Se, Te): A Cu-V-X framework plus void tunnels
    journal, August 2019

    • Liu, Xiao-Peng; Feng, Zhen-Zhen; Guo, Shu-Ping
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    • DOI: 10.1142/s0129183119500451

    Promising thermoelectric materials of Cu 3 VX 4 (X=S, Se, Te): A Cu-V-X framework plus void tunnels
    journal, August 2019

    • Liu, Xiao-Peng; Feng, Zhen-Zhen; Guo, Shu-Ping
    • International Journal of Modern Physics C, Vol. 30, Issue 08
    • DOI: 10.1142/s0129183119500451