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Title: Vacancy-induced dislocations within grains for high-performance PbSe thermoelectrics

To minimize the lattice thermal conductivity in thermoelectrics, strategies typically focus on the scattering of low-frequency phonons by interfaces and high-frequency phonons by point defects. In addition, scattering of mid-frequency phonons by dense dislocations, localized at the grain boundaries, has been shown to reduce the lattice thermal conductivity and improve the thermoelectric performance. Here we propose a vacancy engineering strategy to create dense dislocations in the grains. In Pb 1$-$xSb 2x/3Se solid solutions, cation vacancies are intentionally introduced, where after thermal annealing the vacancies can annihilate through a number of mechanisms creating the desired dislocations homogeneously distributed within the grains. This leads to a lattice thermal conductivity as low as 0.4Wm -1 K -1 and a high thermoelectric figure of merit, which can be explained by a dislocation scattering model. As a result, the vacancy engineering strategy used here should be equally applicable for solid solution thermoelectrics and provides a strategy for improving zT.
Authors:
 [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [2] ;  [3] ;  [3] ;  [1]
  1. Tongji Univ., Shanghai (China)
  2. Chinese Academy of Science, Beijing (China)
  3. Northwestern Univ., Evanston, IL (United States)
Publication Date:
Grant/Contract Number:
SC0001299
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; semiconductors; thermoelectrics
OSTI Identifier:
1345970

Chen, Zhiwei, Ge, Binghui, Li, Wen, Lin, Siqi, Shen, Jiawen, Chang, Yunjie, Hanus, Riley, Snyder, G. Jeffrey, and Pei, Yanzhong. Vacancy-induced dislocations within grains for high-performance PbSe thermoelectrics. United States: N. p., Web. doi:10.1038/ncomms13828.
Chen, Zhiwei, Ge, Binghui, Li, Wen, Lin, Siqi, Shen, Jiawen, Chang, Yunjie, Hanus, Riley, Snyder, G. Jeffrey, & Pei, Yanzhong. Vacancy-induced dislocations within grains for high-performance PbSe thermoelectrics. United States. doi:10.1038/ncomms13828.
Chen, Zhiwei, Ge, Binghui, Li, Wen, Lin, Siqi, Shen, Jiawen, Chang, Yunjie, Hanus, Riley, Snyder, G. Jeffrey, and Pei, Yanzhong. 2017. "Vacancy-induced dislocations within grains for high-performance PbSe thermoelectrics". United States. doi:10.1038/ncomms13828. https://www.osti.gov/servlets/purl/1345970.
@article{osti_1345970,
title = {Vacancy-induced dislocations within grains for high-performance PbSe thermoelectrics},
author = {Chen, Zhiwei and Ge, Binghui and Li, Wen and Lin, Siqi and Shen, Jiawen and Chang, Yunjie and Hanus, Riley and Snyder, G. Jeffrey and Pei, Yanzhong},
abstractNote = {To minimize the lattice thermal conductivity in thermoelectrics, strategies typically focus on the scattering of low-frequency phonons by interfaces and high-frequency phonons by point defects. In addition, scattering of mid-frequency phonons by dense dislocations, localized at the grain boundaries, has been shown to reduce the lattice thermal conductivity and improve the thermoelectric performance. Here we propose a vacancy engineering strategy to create dense dislocations in the grains. In Pb1$-$xSb2x/3Se solid solutions, cation vacancies are intentionally introduced, where after thermal annealing the vacancies can annihilate through a number of mechanisms creating the desired dislocations homogeneously distributed within the grains. This leads to a lattice thermal conductivity as low as 0.4Wm-1 K-1 and a high thermoelectric figure of merit, which can be explained by a dislocation scattering model. As a result, the vacancy engineering strategy used here should be equally applicable for solid solution thermoelectrics and provides a strategy for improving zT.},
doi = {10.1038/ncomms13828},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {2017},
month = {1}
}