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Title: Vibrational hierarchy leads to dual-phonon transport in low thermal conductivity crystals

Abstract

Many low-thermal-conductivity (κL) crystals show intriguing temperature (T) dependence of κL: κLT-1 (crystal-like) at intermediate temperatures whereas weak T-dependence (glass-like) at high temperatures. It has been in debate whether thermal transport can still be described by phonons at the Ioffe-Regel limit. In this work, we propose that most phonons are still well defined for thermal transport, whereas they carry heat via dual channels: normal phonons described by the Boltzmann transport equation theory, and diffuson-like phonons described by the diffusion theory. Three physics-based criteria are incorporated into first-principles calculations to judge mode-by-mode between the two phonon channels. Case studies on La2Zr2O7 and Tl3VSe4 show that normal phonons dominate low temperatures while diffuson-like phonons dominate high temperatures. Our present dual-phonon theory enlightens the physics of hierarchical phonon transport as approaching the Ioffe-Regel limit and provides a numerical method that should be practically applicable to many materials with vibrational hierarchy.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [5]
  1. Purdue Univ., West Lafayette, IN (United States); Chinese Academy of Sciences (CAS), Shenyang (China)
  2. Purdue Univ., West Lafayette, IN (United States); Shenzhen Univ. (China)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Chinese Academy of Sciences (CAS), Shenyang (China)
  5. Purdue Univ., West Lafayette, IN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1631233
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING

Citation Formats

Luo, Yixiu, Yang, Xiaolong, Feng, Tianli, Wang, Jingyang, and Ruan, Xiulin. Vibrational hierarchy leads to dual-phonon transport in low thermal conductivity crystals. United States: N. p., 2020. Web. doi:10.1038/s41467-020-16371-w.
Luo, Yixiu, Yang, Xiaolong, Feng, Tianli, Wang, Jingyang, & Ruan, Xiulin. Vibrational hierarchy leads to dual-phonon transport in low thermal conductivity crystals. United States. doi:https://doi.org/10.1038/s41467-020-16371-w
Luo, Yixiu, Yang, Xiaolong, Feng, Tianli, Wang, Jingyang, and Ruan, Xiulin. Fri . "Vibrational hierarchy leads to dual-phonon transport in low thermal conductivity crystals". United States. doi:https://doi.org/10.1038/s41467-020-16371-w. https://www.osti.gov/servlets/purl/1631233.
@article{osti_1631233,
title = {Vibrational hierarchy leads to dual-phonon transport in low thermal conductivity crystals},
author = {Luo, Yixiu and Yang, Xiaolong and Feng, Tianli and Wang, Jingyang and Ruan, Xiulin},
abstractNote = {Many low-thermal-conductivity (κL) crystals show intriguing temperature (T) dependence of κL: κL ∝ T-1 (crystal-like) at intermediate temperatures whereas weak T-dependence (glass-like) at high temperatures. It has been in debate whether thermal transport can still be described by phonons at the Ioffe-Regel limit. In this work, we propose that most phonons are still well defined for thermal transport, whereas they carry heat via dual channels: normal phonons described by the Boltzmann transport equation theory, and diffuson-like phonons described by the diffusion theory. Three physics-based criteria are incorporated into first-principles calculations to judge mode-by-mode between the two phonon channels. Case studies on La2Zr2O7 and Tl3VSe4 show that normal phonons dominate low temperatures while diffuson-like phonons dominate high temperatures. Our present dual-phonon theory enlightens the physics of hierarchical phonon transport as approaching the Ioffe-Regel limit and provides a numerical method that should be practically applicable to many materials with vibrational hierarchy.},
doi = {10.1038/s41467-020-16371-w},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {2020},
month = {5}
}

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