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Title: Unification of nonequilibrium molecular dynamics and the mode-resolved phonon Boltzmann equation for thermal transport simulations

Abstract

Nano-size confinement induces many intriguing non-Fourier heat conduction phenomena, such as nonlinear temperature gradients, temperature jumps near the contacts, and size-dependent thermal conductivity. Over the past decades, these effects have been studied and interpreted by nonequilibrium molecular dynamics (NEMD) and phonon Boltzmann transport equation (BTE) simulations separately, but no theory that unifies these two methods has ever been established. In this work, we unify these methods using a quantitative mode-level comparison and demonstrate that they are equivalent for various thermostats. We show that different thermostats result in different non-Fourier thermal transport characteristics due to the different mode-level phonon excitations inside the thermostats, which explains the different size-dependent thermal conductivities calculated using different reservoirs, even though they give the same bulk thermal conductivity. Specifically, the Langevin thermostat behaves like a thermalizing boundary in phonon BTE and provides mode-level thermal-equilibrium phonon outlets, while the Nose-Hoover chain thermostat and velocity rescaling method behave like biased reservoirs, which provide a spatially uniform heat generation and mode-level nonequilibrium phonon outlets. These findings explain why different experimental measurement methods can yield different size-dependent thermal conductivity. They also indicate that the thermal conductivity of materials can be tuned for various applications by specifically designing thermostats. Finally, themore » unification of NEMD and phonon BTE will largely facilitate the study of thermal transport in complex systems in the future by, e.g., replacing computationally unaffordable first-principles NEMD simulations with computationally less expensive spectral BTE simulations.« less

Authors:
 [1]; ORCiD logo [2];  [1];  [3];  [4];  [4]; ORCiD logo [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Shanghai Jiao Tong Univ., Shanghai (China)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Energy and Transportation Science Division
  3. Aalto Univ. (Finland)
  4. Purdue Univ., West Lafayette, IN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1616819
Alternate Identifier(s):
OSTI ID: 1615955
Grant/Contract Number:  
AC05-00OR22725; 51676121; 51706134; 11974059
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 101; Journal Issue: 15; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; ballistic transport; heat transfer; lattice thermal conductivity; phonons; nanostructures; thin films; Boltzmann theory; molecular dynamics

Citation Formats

Hu, Yue, Feng, Tianli, Gu, Xiaokun, Fan, Zheyong, Wang, Xufeng, Lundstrom, Mark, Shrestha, Som, and Bao, Hua. Unification of nonequilibrium molecular dynamics and the mode-resolved phonon Boltzmann equation for thermal transport simulations. United States: N. p., 2020. Web. doi:10.1103/PhysRevB.101.155308.
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Hu, Yue, Feng, Tianli, Gu, Xiaokun, Fan, Zheyong, Wang, Xufeng, Lundstrom, Mark, Shrestha, Som, & Bao, Hua. Unification of nonequilibrium molecular dynamics and the mode-resolved phonon Boltzmann equation for thermal transport simulations. United States. https://doi.org/10.1103/PhysRevB.101.155308
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Hu, Yue, Feng, Tianli, Gu, Xiaokun, Fan, Zheyong, Wang, Xufeng, Lundstrom, Mark, Shrestha, Som, and Bao, Hua. Thu . "Unification of nonequilibrium molecular dynamics and the mode-resolved phonon Boltzmann equation for thermal transport simulations". United States. https://doi.org/10.1103/PhysRevB.101.155308. https://www.osti.gov/servlets/purl/1616819.
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@article{osti_1616819,
title = {Unification of nonequilibrium molecular dynamics and the mode-resolved phonon Boltzmann equation for thermal transport simulations},
author = {Hu, Yue and Feng, Tianli and Gu, Xiaokun and Fan, Zheyong and Wang, Xufeng and Lundstrom, Mark and Shrestha, Som and Bao, Hua},
abstractNote = {Nano-size confinement induces many intriguing non-Fourier heat conduction phenomena, such as nonlinear temperature gradients, temperature jumps near the contacts, and size-dependent thermal conductivity. Over the past decades, these effects have been studied and interpreted by nonequilibrium molecular dynamics (NEMD) and phonon Boltzmann transport equation (BTE) simulations separately, but no theory that unifies these two methods has ever been established. In this work, we unify these methods using a quantitative mode-level comparison and demonstrate that they are equivalent for various thermostats. We show that different thermostats result in different non-Fourier thermal transport characteristics due to the different mode-level phonon excitations inside the thermostats, which explains the different size-dependent thermal conductivities calculated using different reservoirs, even though they give the same bulk thermal conductivity. Specifically, the Langevin thermostat behaves like a thermalizing boundary in phonon BTE and provides mode-level thermal-equilibrium phonon outlets, while the Nose-Hoover chain thermostat and velocity rescaling method behave like biased reservoirs, which provide a spatially uniform heat generation and mode-level nonequilibrium phonon outlets. These findings explain why different experimental measurement methods can yield different size-dependent thermal conductivity. They also indicate that the thermal conductivity of materials can be tuned for various applications by specifically designing thermostats. Finally, the unification of NEMD and phonon BTE will largely facilitate the study of thermal transport in complex systems in the future by, e.g., replacing computationally unaffordable first-principles NEMD simulations with computationally less expensive spectral BTE simulations.},
doi = {10.1103/PhysRevB.101.155308},
journal = {Physical Review B},
number = 15,
volume = 101,
place = {United States},
year = {Thu Apr 23 00:00:00 EDT 2020},
month = {Thu Apr 23 00:00:00 EDT 2020}
}
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https://doi.org/10.1103/PhysRevB.101.155308
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