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Title: Electron-phonon coupling and thermal transport in the thermoelectric compound Mo3Sb7–xTex

Abstract

Phonon properties of Mo3Sb7–xTex (x = 0, 1.5, 1.7), a potential high-temperature thermoelectric material, have been studied with inelastic neutron and x-ray scattering, and with first-principles simulations. The substitution of Te for Sb leads to pronounced changes in the electronic struc- ture, local bonding, phonon density of states (DOS), dispersions, and phonon lifetimes. Alloying with tellurium shifts the Fermi level upward, near the top of the valence band, resulting in a strong suppression of electron-phonon screening, and a large overall stiffening of interatomic force- constants. The suppression in electron-phonon coupling concomitantly increases group velocities and suppresses phonon scattering rates, surpassing the effects of alloy-disorder scattering, and re- sulting in a surprising increased lattice thermal conductivity in the alloy. We also identify that the local bonding environment changes non-uniformly around different atoms, leading to variable perturbation strengths for different optical phonon branches. The respective roles of changes in phonon group velocities and phonon lifetimes on the lattice thermal conductivity are quantified. Lastly, our results highlight the importance of the electron-phonon coupling on phonon mean-free-paths in this compound, and also estimates the contributions from boundary scattering, umklapp scattering, and point-defect scattering.

Authors:
 [1];  [1];  [2];  [1];  [3];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1238024
Alternate Identifier(s):
OSTI ID: 1228414; OSTI ID: 1245023
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 92; Journal Issue: 21; Journal ID: ISSN 1098-0121
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Bansal, Dipanshu, Li, Chen W., Said, Ayman H., Abernathy, Douglas L., Yan, Jiaqiang, and Delaire, Olivier A. Electron-phonon coupling and thermal transport in the thermoelectric compound Mo3Sb7–xTex. United States: N. p., 2015. Web. doi:10.1103/PhysRevB.92.214301.
Bansal, Dipanshu, Li, Chen W., Said, Ayman H., Abernathy, Douglas L., Yan, Jiaqiang, & Delaire, Olivier A. Electron-phonon coupling and thermal transport in the thermoelectric compound Mo3Sb7–xTex. United States. doi:https://doi.org/10.1103/PhysRevB.92.214301
Bansal, Dipanshu, Li, Chen W., Said, Ayman H., Abernathy, Douglas L., Yan, Jiaqiang, and Delaire, Olivier A. Mon . "Electron-phonon coupling and thermal transport in the thermoelectric compound Mo3Sb7–xTex". United States. doi:https://doi.org/10.1103/PhysRevB.92.214301. https://www.osti.gov/servlets/purl/1238024.
@article{osti_1238024,
title = {Electron-phonon coupling and thermal transport in the thermoelectric compound Mo3Sb7–xTex},
author = {Bansal, Dipanshu and Li, Chen W. and Said, Ayman H. and Abernathy, Douglas L. and Yan, Jiaqiang and Delaire, Olivier A.},
abstractNote = {Phonon properties of Mo3Sb7–xTex (x = 0, 1.5, 1.7), a potential high-temperature thermoelectric material, have been studied with inelastic neutron and x-ray scattering, and with first-principles simulations. The substitution of Te for Sb leads to pronounced changes in the electronic struc- ture, local bonding, phonon density of states (DOS), dispersions, and phonon lifetimes. Alloying with tellurium shifts the Fermi level upward, near the top of the valence band, resulting in a strong suppression of electron-phonon screening, and a large overall stiffening of interatomic force- constants. The suppression in electron-phonon coupling concomitantly increases group velocities and suppresses phonon scattering rates, surpassing the effects of alloy-disorder scattering, and re- sulting in a surprising increased lattice thermal conductivity in the alloy. We also identify that the local bonding environment changes non-uniformly around different atoms, leading to variable perturbation strengths for different optical phonon branches. The respective roles of changes in phonon group velocities and phonon lifetimes on the lattice thermal conductivity are quantified. Lastly, our results highlight the importance of the electron-phonon coupling on phonon mean-free-paths in this compound, and also estimates the contributions from boundary scattering, umklapp scattering, and point-defect scattering.},
doi = {10.1103/PhysRevB.92.214301},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
number = 21,
volume = 92,
place = {United States},
year = {2015},
month = {12}
}

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