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Title: High Thermoelectric Performance in the Wide Band-Gap AgGa1-xTe2 Compounds: Directional Negative Thermal Expansion and Intrinsically Low Thermal Conductivity

Abstract

Abstract A deficiency of Ga in wide band‐gap AgGa 1‐ x Te 2 semiconductors (1.2 eV) can be used to optimize the electrical transport properties and reduce the thermal conductivity to achieve ZT > 1 at 873 K. First‐principles density functional theory calculations and a Boson peak observed in the low temperature heat capacity data indicate the presence of strong coupling between optical phonons with low frequency and heat carrying acoustical phonons, resulting in a depressed maximum of Debye frequency in the first Brillouin zone and low phonon velocities. Moreover, the AgTe bond lengths and TeAgTe bond angles increase with rising temperature, leading to a significant distortion of the [AgTe 4 ] 7− tetrahedra, but an almost unmodified [GaTe 4 ] 5− tetrahedra. This behavior results in lattice expansion in the ab ‐plane and contraction along the c ‐axis, corresponding to the positive and negative Gruneisen parameters in the phonon spectral calculations. This effect gives rise to the large anharmonic behavior of the lattice. These factors together with the low frequency vibrations of Ag and Te atoms in the structure lead to an ultralow thermal conductivity of 0.18 W m −1 K −1 at 873 K.

Authors:
 [1];  [2];  [3];  [3];  [2];  [3];  [1];  [2];  [3];  [2]; ORCiD logo [3]
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  1. Wuhan Univ. of Technology (China); Northwestern Univ., Evanston, IL (United States)
  2. Wuhan Univ. of Technology (China)
  3. Northwestern Univ., Evanston, IL (United States)
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Natural Science Foundation of China
OSTI Identifier:
1777261
Alternate Identifier(s):
OSTI ID: 1785800
Grant/Contract Number:  
SC0014520; 51521001; 51632006; AC02-06CH11357; DE‐SC0014520; DE‐AC02‐06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 6; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; directional negative thermal expansion; intrinsically low thermal conductivity; phonon spectrum; thermoelectric properties; vacancy

Citation Formats

Su, Xianli, Zhao, Na, Hao, Shiqiang, Stoumpos, Constantinos C., Liu, Mengyuan, Chen, Haijie, Xie, Hongyao, Zhang, Qingjie, Wolverton, Chris, Tang, Xinfeng, and Kanatzidis, Mercouri G. High Thermoelectric Performance in the Wide Band-Gap AgGa1-xTe2 Compounds: Directional Negative Thermal Expansion and Intrinsically Low Thermal Conductivity. United States: N. p., 2018. Web. doi:10.1002/adfm.201806534.
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Su, Xianli, Zhao, Na, Hao, Shiqiang, Stoumpos, Constantinos C., Liu, Mengyuan, Chen, Haijie, Xie, Hongyao, Zhang, Qingjie, Wolverton, Chris, Tang, Xinfeng, & Kanatzidis, Mercouri G. High Thermoelectric Performance in the Wide Band-Gap AgGa1-xTe2 Compounds: Directional Negative Thermal Expansion and Intrinsically Low Thermal Conductivity. United States. https://doi.org/10.1002/adfm.201806534
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Su, Xianli, Zhao, Na, Hao, Shiqiang, Stoumpos, Constantinos C., Liu, Mengyuan, Chen, Haijie, Xie, Hongyao, Zhang, Qingjie, Wolverton, Chris, Tang, Xinfeng, and Kanatzidis, Mercouri G. Thu . "High Thermoelectric Performance in the Wide Band-Gap AgGa1-xTe2 Compounds: Directional Negative Thermal Expansion and Intrinsically Low Thermal Conductivity". United States. https://doi.org/10.1002/adfm.201806534. https://www.osti.gov/servlets/purl/1777261.
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@article{osti_1777261,
title = {High Thermoelectric Performance in the Wide Band-Gap AgGa1-xTe2 Compounds: Directional Negative Thermal Expansion and Intrinsically Low Thermal Conductivity},
author = {Su, Xianli and Zhao, Na and Hao, Shiqiang and Stoumpos, Constantinos C. and Liu, Mengyuan and Chen, Haijie and Xie, Hongyao and Zhang, Qingjie and Wolverton, Chris and Tang, Xinfeng and Kanatzidis, Mercouri G.},
abstractNote = {Abstract A deficiency of Ga in wide band‐gap AgGa 1‐ x Te 2 semiconductors (1.2 eV) can be used to optimize the electrical transport properties and reduce the thermal conductivity to achieve ZT > 1 at 873 K. First‐principles density functional theory calculations and a Boson peak observed in the low temperature heat capacity data indicate the presence of strong coupling between optical phonons with low frequency and heat carrying acoustical phonons, resulting in a depressed maximum of Debye frequency in the first Brillouin zone and low phonon velocities. Moreover, the AgTe bond lengths and TeAgTe bond angles increase with rising temperature, leading to a significant distortion of the [AgTe 4 ] 7− tetrahedra, but an almost unmodified [GaTe 4 ] 5− tetrahedra. This behavior results in lattice expansion in the ab ‐plane and contraction along the c ‐axis, corresponding to the positive and negative Gruneisen parameters in the phonon spectral calculations. This effect gives rise to the large anharmonic behavior of the lattice. These factors together with the low frequency vibrations of Ag and Te atoms in the structure lead to an ultralow thermal conductivity of 0.18 W m −1 K −1 at 873 K.},
doi = {10.1002/adfm.201806534},
journal = {Advanced Functional Materials},
number = 6,
volume = 29,
place = {United States},
year = {Thu Dec 20 00:00:00 EST 2018},
month = {Thu Dec 20 00:00:00 EST 2018}
}
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https://doi.org/10.1002/adfm.201806534
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