Rhombohedral to Cubic Conversion of GeTe via MnTe Alloying Leads to Ultralow Thermal Conductivity, Electronic Band Convergence, and High Thermoelectric Performance
Abstract
In this study, a series of Ge1–xMnxTe (x = 0–0.21) compounds were prepared by a melting–quenching–annealing process combined with spark plasma sintering (SPS). The effect of alloying MnTe into GeTe on the structure and thermoelectric properties of Ge1–xMnxTe is profound. With increasing content of MnTe, the structure of the Ge1–xMnxTe compounds gradually changes from rhombohedral to cubic, and the known R3m to Fm-3m phase transition temperature of GeTe moves from 700 K closer to room temperature. First-principles density functional theory calculations show that alloying MnTe into GeTe decreases the energy difference between the light and heavy valence bands in both the R3m and Fm-3m structures, enhancing a multiband character of the valence band edge that increases the hole carrier effective mass. The effect of this band convergence is a significant enhancement in the carrier effective mass from 1.44 m0 (GeTe) to 6.15 m0 (Ge0.85Mn0.15Te). In addition, alloying with MnTe decreases the phonon relaxation time by enhancing alloy scattering, reduces the phonon velocity, and increases Ge vacancies all of which result in an ultralow lattice thermal conductivity of 0.13 W m–1 K–1 at 823 K. Subsequent doping of the Ge0.9Mn0.1Te compositions with Sb lowers the typical very high hole carrier concentrationmore »
- Authors:
-
[2];
[3];
[3];
[3];
[1]
- Wuhan Univ. of Technology (China)
- Wuhan Univ. of Technology (China); Northwestern Univ., Evanston, IL (United States)
- Northwestern Univ., Evanston, IL (United States)
- Univ. of Michigan, Ann Arbor, MI (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:
- 1775445
- Grant/Contract Number:
- SC0014520; 51402222; 51521001; 51632006
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 140; Journal Issue: 7; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Thermal conductivity; Lattices; Scattering; Chemical structure; Transition metals
Citation Formats
Zheng, Zheng, Su, Xianli, Deng, Rigui, Stoumpos, Constantinos, Xie, Hongyao, Liu, Wei, Yan, Yonggao, Hao, Shiqiang, Uher, Ctirad, Wolverton, Chris, Kanatzidis, Mercouri G., and Tang, Xinfeng. Rhombohedral to Cubic Conversion of GeTe via MnTe Alloying Leads to Ultralow Thermal Conductivity, Electronic Band Convergence, and High Thermoelectric Performance. United States: N. p., 2018.
Web. doi:10.1021/jacs.7b13611.
Zheng, Zheng, Su, Xianli, Deng, Rigui, Stoumpos, Constantinos, Xie, Hongyao, Liu, Wei, Yan, Yonggao, Hao, Shiqiang, Uher, Ctirad, Wolverton, Chris, Kanatzidis, Mercouri G., & Tang, Xinfeng. Rhombohedral to Cubic Conversion of GeTe via MnTe Alloying Leads to Ultralow Thermal Conductivity, Electronic Band Convergence, and High Thermoelectric Performance. United States. https://doi.org/10.1021/jacs.7b13611
Zheng, Zheng, Su, Xianli, Deng, Rigui, Stoumpos, Constantinos, Xie, Hongyao, Liu, Wei, Yan, Yonggao, Hao, Shiqiang, Uher, Ctirad, Wolverton, Chris, Kanatzidis, Mercouri G., and Tang, Xinfeng. Fri .
"Rhombohedral to Cubic Conversion of GeTe via MnTe Alloying Leads to Ultralow Thermal Conductivity, Electronic Band Convergence, and High Thermoelectric Performance". United States. https://doi.org/10.1021/jacs.7b13611. https://www.osti.gov/servlets/purl/1775445.
@article{osti_1775445,
title = {Rhombohedral to Cubic Conversion of GeTe via MnTe Alloying Leads to Ultralow Thermal Conductivity, Electronic Band Convergence, and High Thermoelectric Performance},
author = {Zheng, Zheng and Su, Xianli and Deng, Rigui and Stoumpos, Constantinos and Xie, Hongyao and Liu, Wei and Yan, Yonggao and Hao, Shiqiang and Uher, Ctirad and Wolverton, Chris and Kanatzidis, Mercouri G. and Tang, Xinfeng},
abstractNote = {In this study, a series of Ge1–xMnxTe (x = 0–0.21) compounds were prepared by a melting–quenching–annealing process combined with spark plasma sintering (SPS). The effect of alloying MnTe into GeTe on the structure and thermoelectric properties of Ge1–xMnxTe is profound. With increasing content of MnTe, the structure of the Ge1–xMnxTe compounds gradually changes from rhombohedral to cubic, and the known R3m to Fm-3m phase transition temperature of GeTe moves from 700 K closer to room temperature. First-principles density functional theory calculations show that alloying MnTe into GeTe decreases the energy difference between the light and heavy valence bands in both the R3m and Fm-3m structures, enhancing a multiband character of the valence band edge that increases the hole carrier effective mass. The effect of this band convergence is a significant enhancement in the carrier effective mass from 1.44 m0 (GeTe) to 6.15 m0 (Ge0.85Mn0.15Te). In addition, alloying with MnTe decreases the phonon relaxation time by enhancing alloy scattering, reduces the phonon velocity, and increases Ge vacancies all of which result in an ultralow lattice thermal conductivity of 0.13 W m–1 K–1 at 823 K. Subsequent doping of the Ge0.9Mn0.1Te compositions with Sb lowers the typical very high hole carrier concentration and brings it closer to its optimal value enhancing the power factor, which combined with the ultralow thermal conductivity yields a maximum ZT value of 1.61 at 823 K (for Ge0.86Mn0.10Sb0.04Te). In conclusion, the average ZT value of the compound over the temperature range 400–800 K is 1.09, making it the best GeTe-based thermoelectric material.},
doi = {10.1021/jacs.7b13611},
journal = {Journal of the American Chemical Society},
number = 7,
volume = 140,
place = {United States},
year = {Fri Jan 19 00:00:00 EST 2018},
month = {Fri Jan 19 00:00:00 EST 2018}
}
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