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Title: Weak Electron Phonon Coupling and Deep Level Impurity for High Thermoelectric Performance Pb1–xGaxTe

Abstract

Abstract High ZT of 1.34 at 766 K and a record high average ZT above 1 in the temperature range of 300‐864 K are attained in n‐type PbTe by engineering the temperature‐dependent carrier concentration and weakening electron–phonon coupling upon Ga doping. The experimental studies and first principles band structure calculations show that doping with Ga introduces a shallow level impurity contributing extrinsic carriers and imparts a deeper impurity level that ionizes at higher temperatures. This adjusts the carrier concentration closer to the temperature‐dependent optimum and thus maximizes the power factor in a wide temperature range. The maximum power factor of 35 µW cm −1 K −2 is achieved for the Pb 0.98 Ga 0.02 Te compound, and is maintained over 20 µWcm −1 K −2 from 300 to 767 K. Band structure calculations and X‐ray photoelectron spectroscopy corroborate the amphoteric role of Ga in PbTe as the origin of shallow and deep levels. Additionally, Ga doping weakens the electron–phonon coupling, leading to high carrier mobilities in excess of 1200 cm 2 V −1 s −1 . Enhanced point defect phonon scattering yields a reduced lattice thermal conductivity. This work provides a new avenue, beyond the conventional shallow level doping, formore » further improving the average ZT in thermoelectric materials.« less

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [2];  [2];  [2];  [5];  [3];  [2];  [5];  [2]
  1. Wuhan Univ. of Technology (China); Northwestern Univ., Evanston, IL (United States)
  2. Northwestern Univ., Evanston, IL (United States)
  3. Univ. of Michigan, Ann Arbor, MI (United States)
  4. Wuhan Univ. of Technology (China); Univ. of Michigan, Ann Arbor, MI (United States)
  5. Wuhan Univ. of Technology (China)
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1775439
Alternate Identifier(s):
OSTI ID: 1437491
Grant/Contract Number:  
SC0014520; 51521001; 51632006; DE‐SC0014520
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 8; Journal Issue: 21; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Su, Xianli, Hao, Shiqiang, Bailey, Trevor P., Wang, Si, Hadar, Ido, Tan, Gangjian, Song, Tze‐Bin, Zhang, Qingjie, Uher, Ctirad, Wolverton, Chris, Tang, Xinfeng, and Kanatzidis, Mercouri G. Weak Electron Phonon Coupling and Deep Level Impurity for High Thermoelectric Performance Pb1–xGaxTe. United States: N. p., 2018. Web. doi:10.1002/aenm.201800659.
Su, Xianli, Hao, Shiqiang, Bailey, Trevor P., Wang, Si, Hadar, Ido, Tan, Gangjian, Song, Tze‐Bin, Zhang, Qingjie, Uher, Ctirad, Wolverton, Chris, Tang, Xinfeng, & Kanatzidis, Mercouri G. Weak Electron Phonon Coupling and Deep Level Impurity for High Thermoelectric Performance Pb1–xGaxTe. United States. https://doi.org/10.1002/aenm.201800659
Su, Xianli, Hao, Shiqiang, Bailey, Trevor P., Wang, Si, Hadar, Ido, Tan, Gangjian, Song, Tze‐Bin, Zhang, Qingjie, Uher, Ctirad, Wolverton, Chris, Tang, Xinfeng, and Kanatzidis, Mercouri G. Wed . "Weak Electron Phonon Coupling and Deep Level Impurity for High Thermoelectric Performance Pb1–xGaxTe". United States. https://doi.org/10.1002/aenm.201800659. https://www.osti.gov/servlets/purl/1775439.
@article{osti_1775439,
title = {Weak Electron Phonon Coupling and Deep Level Impurity for High Thermoelectric Performance Pb1–xGaxTe},
author = {Su, Xianli and Hao, Shiqiang and Bailey, Trevor P. and Wang, Si and Hadar, Ido and Tan, Gangjian and Song, Tze‐Bin and Zhang, Qingjie and Uher, Ctirad and Wolverton, Chris and Tang, Xinfeng and Kanatzidis, Mercouri G.},
abstractNote = {Abstract High ZT of 1.34 at 766 K and a record high average ZT above 1 in the temperature range of 300‐864 K are attained in n‐type PbTe by engineering the temperature‐dependent carrier concentration and weakening electron–phonon coupling upon Ga doping. The experimental studies and first principles band structure calculations show that doping with Ga introduces a shallow level impurity contributing extrinsic carriers and imparts a deeper impurity level that ionizes at higher temperatures. This adjusts the carrier concentration closer to the temperature‐dependent optimum and thus maximizes the power factor in a wide temperature range. The maximum power factor of 35 µW cm −1 K −2 is achieved for the Pb 0.98 Ga 0.02 Te compound, and is maintained over 20 µWcm −1 K −2 from 300 to 767 K. Band structure calculations and X‐ray photoelectron spectroscopy corroborate the amphoteric role of Ga in PbTe as the origin of shallow and deep levels. Additionally, Ga doping weakens the electron–phonon coupling, leading to high carrier mobilities in excess of 1200 cm 2 V −1 s −1 . Enhanced point defect phonon scattering yields a reduced lattice thermal conductivity. This work provides a new avenue, beyond the conventional shallow level doping, for further improving the average ZT in thermoelectric materials.},
doi = {10.1002/aenm.201800659},
journal = {Advanced Energy Materials},
number = 21,
volume = 8,
place = {United States},
year = {Wed May 16 00:00:00 EDT 2018},
month = {Wed May 16 00:00:00 EDT 2018}
}

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