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Title: Computational prediction of lattice thermal conductivity: A comparison of molecular dynamics and Boltzmann transport approaches

Abstract

The predictive modeling of lattice thermal conductivity is of fundamental importance for the understanding and design of materials for a wide range of applications. Two major approaches, namely molecular dynamics (MD) simulations and calculations solving approximately the Boltzmann transport equation (BTE), have been developed to compute the lattice thermal conductivity. We present a detailed direct comparison of these two approaches, using as prototypical cases MgO and PbTe. The comparison, carried out using empirical potentials, takes into account the effects of fourth order phonon scattering, temperature-dependent phonon frequencies (phonon renormalization), and investigates the effects of quantum vs classical statistics. We clarify that equipartition, as opposed to Maxwell-Boltzmann, govern the statistics of phonons in MD simulations. We find that lattice thermal conductivity values from MD and BTE show an apparent, satisfactory agreement; however such an agreement is the result of error cancellations. As a result we also show that the primary effect of statistics on thermal conductivity is via the scattering rate dependence on phonon populations.

Authors:
 [1];  [2]; ORCiD logo [2];  [3]
+ Show Author Affiliations
  1. Univ. of Chicago, Chicago, IL (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Univ. of Chicago, Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1560856
Alternate Identifier(s):
OSTI ID: 1550594
Grant/Contract Number:  
AC02-06CH11357; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 3; Journal Issue: 8; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Puligheddu, Marcello, Xia, Yi, Chan, Maria, and Galli, Giulia. Computational prediction of lattice thermal conductivity: A comparison of molecular dynamics and Boltzmann transport approaches. United States: N. p., 2019. Web. doi:10.1103/PhysRevMaterials.3.085401.
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Puligheddu, Marcello, Xia, Yi, Chan, Maria, & Galli, Giulia. Computational prediction of lattice thermal conductivity: A comparison of molecular dynamics and Boltzmann transport approaches. United States. https://doi.org/10.1103/PhysRevMaterials.3.085401
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Puligheddu, Marcello, Xia, Yi, Chan, Maria, and Galli, Giulia. Thu . "Computational prediction of lattice thermal conductivity: A comparison of molecular dynamics and Boltzmann transport approaches". United States. https://doi.org/10.1103/PhysRevMaterials.3.085401. https://www.osti.gov/servlets/purl/1560856.
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@article{osti_1560856,
title = {Computational prediction of lattice thermal conductivity: A comparison of molecular dynamics and Boltzmann transport approaches},
author = {Puligheddu, Marcello and Xia, Yi and Chan, Maria and Galli, Giulia},
abstractNote = {The predictive modeling of lattice thermal conductivity is of fundamental importance for the understanding and design of materials for a wide range of applications. Two major approaches, namely molecular dynamics (MD) simulations and calculations solving approximately the Boltzmann transport equation (BTE), have been developed to compute the lattice thermal conductivity. We present a detailed direct comparison of these two approaches, using as prototypical cases MgO and PbTe. The comparison, carried out using empirical potentials, takes into account the effects of fourth order phonon scattering, temperature-dependent phonon frequencies (phonon renormalization), and investigates the effects of quantum vs classical statistics. We clarify that equipartition, as opposed to Maxwell-Boltzmann, govern the statistics of phonons in MD simulations. We find that lattice thermal conductivity values from MD and BTE show an apparent, satisfactory agreement; however such an agreement is the result of error cancellations. As a result we also show that the primary effect of statistics on thermal conductivity is via the scattering rate dependence on phonon populations.},
doi = {10.1103/PhysRevMaterials.3.085401},
journal = {Physical Review Materials},
number = 8,
volume = 3,
place = {United States},
year = {Thu Aug 08 00:00:00 EDT 2019},
month = {Thu Aug 08 00:00:00 EDT 2019}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1103/PhysRevMaterials.3.085401
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Cited by: 28 works
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Figures / Tables:

FIG. 1 FIG. 1: Phonon occupation per mode as a function of frequency for MgO at 500K (a), 750K (b) and 1000K (c) and PbTe at 100K (d), 150K (e) and 300K (f). For all materials and temperature, we compare the energy distribution calculated in our molecular dynamics (MD) simulations against threemore » possible statistics: Bose-Einstein (BE) (blue dot-dashed lines), equipartition (EQ) (solid black lines) and Maxwell-Boltzmann (MB) (orange dashed lines).« less
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Works referenced in this record:

Unified first-principles theory of thermal properties of insulators
journal, August 2018

First-Principles Determination of the Soft Mode in Cubic ZrO 2
journal, May 1997

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

Lattice thermal conductivity of semiconducting bulk materials: atomistic simulations
journal, January 2012

  • He, Yuping; Savić, Ivana; Donadio, Davide
  • Physical Chemistry Chemical Physics, Vol. 14, Issue 47
  • DOI: 10.1039/c2cp42394d

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

Statistical Mechanics of Nonequilibrium Liquids
book, January 2007

Ab Initio Green-Kubo Approach for the Thermal Conductivity of Solids
journal, April 2017

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

Diffusons, locons and propagons: Character of atomie yibrations in amorphous Si
journal, November 1999

  • Allen, Philip B.; Feldman, Joseph L.; Fabian, Jaroslav
  • Philosophical Magazine B, Vol. 79, Issue 11-12
  • DOI: 10.1080/13642819908223054

Predicting phonon properties and thermal conductivity from anharmonic lattice dynamics calculations and molecular dynamics simulations
journal, February 2009

Microscopic theory and quantum simulation of atomic heat transport
journal, October 2015

  • Marcolongo, Aris; Umari, Paolo; Baroni, Stefano
  • Nature Physics, Vol. 12, Issue 1
  • DOI: 10.1038/nphys3509

Accurate thermal conductivities from optimally short molecular dynamics simulations
journal, November 2017

Revisiting lattice thermal transport in PbTe: The crucial role of quartic anharmonicity
journal, August 2018

First principles phonon calculations in materials science
journal, November 2015

Calculating thermal conductivity in a transient conduction regime: theory and implementation
journal, April 2014

  • Melis, Claudio; Dettori, Riccardo; Vandermeulen, Simon
  • The European Physical Journal B, Vol. 87, Issue 4
  • DOI: 10.1140/epjb/e2014-50119-0

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

First-principles simulations of heat transport
journal, November 2017

Elastic Constants, Thermal Expansion, and Debye Temperature of Lead Telluride
journal, July 1968

  • Houston, Bland; Strakna, R. E.; Belson, Henry S.
  • Journal of Applied Physics, Vol. 39, Issue 8
  • DOI: 10.1063/1.1656874

Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995

A simple nonequilibrium molecular dynamics method for calculating the thermal conductivity
journal, April 1997

  • Müller-Plathe, Florian
  • The Journal of Chemical Physics, Vol. 106, Issue 14
  • DOI: 10.1063/1.473271

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

Molecular-dynamics simulation of thermal conductivity in amorphous silicon
journal, March 1991

Thermal conductivity of bulk and nanowire Mg 2 Si x Sn 1 − x alloys from first principles
journal, November 2012

Anharmonic stabilization and lattice heat transport in rocksalt β -GeTe
journal, November 2018

  • Xia, Yi; Chan, Maria K. Y.
  • Applied Physics Letters, Vol. 113, Issue 19
  • DOI: 10.1063/1.5048814

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

Rethinking phonons: The issue of disorder
journal, November 2017

  • Seyf, Hamid Reza; Yates, Luke; Bougher, Thomas L.
  • npj Computational Materials, Vol. 3, Issue 1
  • DOI: 10.1038/s41524-017-0052-9

Scattering of Neutrons by an Anharmonic Crystal
journal, December 1962

Anharmonic Phonon Lifetimes in Semiconductors from Density-Functional Perturbation Theory
journal, August 1995

Debye temperature of MgO powder by elastic neutron scattering
journal, January 1976

Thermal transport properties of MgO and Nd2Zr2O7 pyrochlore by molecular dynamics simulation
journal, October 2008

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

Lattice thermal conductivity of silicon from empirical interatomic potentials
journal, July 2005

Tight-binding molecular-dynamics study of phonon anharmonic effects in silicon and diamond
journal, December 1990

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

Many-Particle Physics
book, January 2000

Assessing the applicability of quantum corrections to classical thermal conductivity predictions
journal, June 2009

Thermal conductivity from approach-to-equilibrium molecular dynamics
journal, July 2013

  • Lampin, E.; Palla, P. L.; Francioso, P. -A.
  • Journal of Applied Physics, Vol. 114, Issue 3
  • DOI: 10.1063/1.4815945

Molecular dynamics simulations of lattice thermal conductivity and spectral phonon mean free path of PbTe: Bulk and nanostructures
journal, February 2012

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

Ab initio calculation of the linewidth of various phonon modes in germanium and silicon
journal, April 2003

Many-Particle Physics
journal, March 1982

Four-Phonon Scattering Reduces Intrinsic Thermal Conductivity of Graphene and the Contributions from Flexural Phonons
conference, January 2018

Molecular Dynamics Simulations of Lattice Thermal Conductivity and Spectral Phonon Mean Free Path of PbTe: Bulk and Nanostructures
conference, July 2012

  • Qiu, Bo; Bao, Hua; Ruan, Xiulin
  • ASME 2012 Heat Transfer Summer Conference collocated with the ASME 2012 Fluids Engineering Division Summer Meeting and the ASME 2012 10th International Conference on Nanochannels, Microchannels, and M, Volume 1: Heat Transfer in Energy Systems; Theory and Fundamental Research; Aerospace Heat Transfer; Gas Turbine Heat Transfer; Transport Phenomena in Materials Processing and Manufacturing; Heat and
  • DOI: 10.1115/ht2012-58554

First principles phonon calculations in materials science
preprint, January 2015

Ab initio Green-Kubo Approach for the Thermal Conductivity of Solids
text, January 2016

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    Works referencing / citing this record:

    Gaussian approximation potential for studying the thermal conductivity of silicene
    journal, September 2019

    • Zhang, Cunzhi; Sun, Qiang
    • Journal of Applied Physics, Vol. 126, Issue 10
    • DOI: 10.1063/1.5119281
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      Figures / Tables found in this record:

      FIG. 1 (p. 8)figure
      FIG. 2 (p. 11)figure
      FIG. 3 (p. 14)figure
      FIG. 4 (p. 15)figure
      FIG. 5 (p. 17)figure
      FIG. 6 (p. 19)figure
      TABLE I (p. 20)table
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