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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]
  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 Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
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.
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. doi:10.1103/PhysRevMaterials.3.085401.
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. doi:10.1103/PhysRevMaterials.3.085401.
@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 = {2019},
month = {8}
}

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