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Title: Lattice Softening Significantly Reduces Thermal Conductivity and Leads to High Thermoelectric Efficiency

Abstract

Abstract The influence of micro/nanostructure on thermal conductivity is a topic of great scientific interest, particularly to thermoelectrics. The current understanding is that structural defects decrease thermal conductivity through phonon scattering where the phonon dispersion and speed of sound are assumed to remain constant. Experimental work on a PbTe model system is presented, which shows that the speed of sound linearly decreases with increased internal strain. This softening of the materials lattice completely accounts for the reduction in lattice thermal conductivity, without the introduction of additional phonon scattering mechanisms. Additionally, it is shown that a major contribution to the improvement in the thermoelectric figure of merit (zT > 2) of high‐efficiency Na‐doped PbTe can be attributed to lattice softening. While inhomogeneous internal strain fields are known to introduce phonon scattering centers, this study demonstrates that internal strain can modify phonon propagation speed as well. This presents new avenues to control lattice thermal conductivity, beyond phonon scattering. In practice, many engineering materials will exhibit both softening and scattering effects, as is shown in silicon. This work shines new light on studies of thermal conductivity in fields of energy materials, microelectronics, and nanoscale heat transfer.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2];  [3];  [4];  [2];  [5];  [3];  [1];  [1]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
  3. Tongji Univ., Shanghai (China)
  4. Northwestern Univ., Evanston, IL (United States); Wuhan Univ. (China)
  5. Argonne National Lab. (ANL), Lemont, IL (United States); Northwestern Univ., Evanston, IL (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Natural Science Foundation of China (NSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE
OSTI Identifier:
1513231
Alternate Identifier(s):
OSTI ID: 1506139
Grant/Contract Number:  
AC02-06CH11357; DE‐AC02‐06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 19; Journal Issue: 1900108; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; lattice dynamics; thermal conductivity; thermoelectrics

Citation Formats

Hanus, Riley, Agne, Matthias T., Rettie, Alexander J. E., Chen, Zhiwei, Tan, Gangjian, Chung, Duck Young, Kanatzidis, Mercouri G., Pei, Yanzhong, Voorhees, Peter W., and Snyder, G. Jeffrey. Lattice Softening Significantly Reduces Thermal Conductivity and Leads to High Thermoelectric Efficiency. United States: N. p., 2019. Web. doi:10.1002/adma.201900108.
Hanus, Riley, Agne, Matthias T., Rettie, Alexander J. E., Chen, Zhiwei, Tan, Gangjian, Chung, Duck Young, Kanatzidis, Mercouri G., Pei, Yanzhong, Voorhees, Peter W., & Snyder, G. Jeffrey. Lattice Softening Significantly Reduces Thermal Conductivity and Leads to High Thermoelectric Efficiency. United States. https://doi.org/10.1002/adma.201900108
Hanus, Riley, Agne, Matthias T., Rettie, Alexander J. E., Chen, Zhiwei, Tan, Gangjian, Chung, Duck Young, Kanatzidis, Mercouri G., Pei, Yanzhong, Voorhees, Peter W., and Snyder, G. Jeffrey. Wed . "Lattice Softening Significantly Reduces Thermal Conductivity and Leads to High Thermoelectric Efficiency". United States. https://doi.org/10.1002/adma.201900108. https://www.osti.gov/servlets/purl/1513231.
@article{osti_1513231,
title = {Lattice Softening Significantly Reduces Thermal Conductivity and Leads to High Thermoelectric Efficiency},
author = {Hanus, Riley and Agne, Matthias T. and Rettie, Alexander J. E. and Chen, Zhiwei and Tan, Gangjian and Chung, Duck Young and Kanatzidis, Mercouri G. and Pei, Yanzhong and Voorhees, Peter W. and Snyder, G. Jeffrey},
abstractNote = {Abstract The influence of micro/nanostructure on thermal conductivity is a topic of great scientific interest, particularly to thermoelectrics. The current understanding is that structural defects decrease thermal conductivity through phonon scattering where the phonon dispersion and speed of sound are assumed to remain constant. Experimental work on a PbTe model system is presented, which shows that the speed of sound linearly decreases with increased internal strain. This softening of the materials lattice completely accounts for the reduction in lattice thermal conductivity, without the introduction of additional phonon scattering mechanisms. Additionally, it is shown that a major contribution to the improvement in the thermoelectric figure of merit (zT > 2) of high‐efficiency Na‐doped PbTe can be attributed to lattice softening. While inhomogeneous internal strain fields are known to introduce phonon scattering centers, this study demonstrates that internal strain can modify phonon propagation speed as well. This presents new avenues to control lattice thermal conductivity, beyond phonon scattering. In practice, many engineering materials will exhibit both softening and scattering effects, as is shown in silicon. This work shines new light on studies of thermal conductivity in fields of energy materials, microelectronics, and nanoscale heat transfer.},
doi = {10.1002/adma.201900108},
journal = {Advanced Materials},
number = 1900108,
volume = 19,
place = {United States},
year = {Wed Apr 10 00:00:00 EDT 2019},
month = {Wed Apr 10 00:00:00 EDT 2019}
}

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