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Title: Lattice thermal transport in group II-alloyed PbTe

Here, PbTe, one of the most promising thermoelectric materials, has recently demonstrated a thermoelectric figure of merit ( ZT) of above 2.0 when alloyed with group II elements. The improvements are due mainly to significant reduction of lattice thermal conductivity (κ ι), which was in turn attributed to nanoparticle precipitates. However, a fundamental understanding of various phonon scattering mechanisms within the bulk alloy is still lacking. In this work, we apply the newly-developed density-functional-theory-based compressive sensing lattice dynamics approach to model lattice heat transport in PbTe, MTe, and Pb 0.94M 0.06Te (M = Mg, Ca, Sr, and Ba) and compare our results with experimental measurements, with focus on the strain effect and mass disorder scattering. We find that (1) CaTe, SrTe, and BaTe in the rock-salt structure exhibit much higher kappa(l) than PbTe, while MgTe in the same structure shows anomalously low κ ι; (2) lattice heat transport of PbTe is extremely sensitive to static strain induced by alloying atoms in solid solution form; (3) mass disorder scattering plays a major role in reducing κ ι for Mg/Ca/Sr-alloyed PbTe through strongly suppressing the lifetimes of intermediate- and high-frequency phonons, while for Ba-alloyed PbTe, precipitated nanoparticles are also important.
Authors:
 [1] ;  [2] ;  [3] ; ORCiD logo [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Northwestern Univ., Evanston, IL (United States)
  3. Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357; 5J-30161-0010A; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Applied Physics Letters
Additional Journal Information:
Journal Volume: 112; Journal Issue: 18; Journal ID: ISSN 0003-6951
Publisher:
American Institute of Physics (AIP)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; Midwest Integrated Center for Computational Materials (MICCoM); USDOE
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1461424
Alternate Identifier(s):
OSTI ID: 1435862

Xia, Yi, Hodges, James M., Kanatzidis, Mercouri G., and Chan, Maria K. Y.. Lattice thermal transport in group II-alloyed PbTe. United States: N. p., Web. doi:10.1063/1.5002587.
Xia, Yi, Hodges, James M., Kanatzidis, Mercouri G., & Chan, Maria K. Y.. Lattice thermal transport in group II-alloyed PbTe. United States. doi:10.1063/1.5002587.
Xia, Yi, Hodges, James M., Kanatzidis, Mercouri G., and Chan, Maria K. Y.. 2018. "Lattice thermal transport in group II-alloyed PbTe". United States. doi:10.1063/1.5002587.
@article{osti_1461424,
title = {Lattice thermal transport in group II-alloyed PbTe},
author = {Xia, Yi and Hodges, James M. and Kanatzidis, Mercouri G. and Chan, Maria K. Y.},
abstractNote = {Here, PbTe, one of the most promising thermoelectric materials, has recently demonstrated a thermoelectric figure of merit (ZT) of above 2.0 when alloyed with group II elements. The improvements are due mainly to significant reduction of lattice thermal conductivity (κι), which was in turn attributed to nanoparticle precipitates. However, a fundamental understanding of various phonon scattering mechanisms within the bulk alloy is still lacking. In this work, we apply the newly-developed density-functional-theory-based compressive sensing lattice dynamics approach to model lattice heat transport in PbTe, MTe, and Pb0.94M0.06Te (M = Mg, Ca, Sr, and Ba) and compare our results with experimental measurements, with focus on the strain effect and mass disorder scattering. We find that (1) CaTe, SrTe, and BaTe in the rock-salt structure exhibit much higher kappa(l) than PbTe, while MgTe in the same structure shows anomalously low κι; (2) lattice heat transport of PbTe is extremely sensitive to static strain induced by alloying atoms in solid solution form; (3) mass disorder scattering plays a major role in reducing κι for Mg/Ca/Sr-alloyed PbTe through strongly suppressing the lifetimes of intermediate- and high-frequency phonons, while for Ba-alloyed PbTe, precipitated nanoparticles are also important.},
doi = {10.1063/1.5002587},
journal = {Applied Physics Letters},
number = 18,
volume = 112,
place = {United States},
year = {2018},
month = {5}
}

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