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Title: Valence Band Modification and High Thermoelectric Performance in SnTe Heavily Alloyed with MnTe

Abstract

Herein we demonstrate a high solubility limit of >9 mol% for MnTe alloying in SnTe. The electrical conductivity of SnTe decreases gradually while the Seebeck coefficient increases remarkably with increasing MnTe content, leading to enhanced power factors. The room-temperature Seebeck coefficients of Mn-doped SnTe are significantly higher than those predicted by theoretical Pisarenko plots for pure SnTe, indicating a modified band structure. The high-temperature Hall data of Sn 1–xMn xTe show strong temperature dependence, suggestive of a two-valence-band conduction behavior. Moreover, the peak temperature of the Hall plot of Sn 1–xMn xTe shifts toward lower temperature as MnTe content is increased, which is clear evidence of decreased energy separation (band convergence) between the two valence bands. The first-principles electronic structure calculations based on density functional theory also support this point. The higher doping fraction (>9%) of Mn in comparison with ~3% for Cd and Hg in SnTe gives rise to a much better valence band convergence that is responsible for the observed highest Seebeck coefficient of ~230 μV/K at 900 K. The high doping fraction of Mn in SnTe also creates stronger point defect scattering, which when combined with ubiquitous endotaxial MnTe nanostructures when the solubility of Mn is exceededmore » scatters a wide spectrum of phonons for a low lattice thermal conductivity of 0.9 W m –1 K –1 at 800 K. The synergistic role that Mn plays in regulating the electron and phonon transport of SnTe yields a high thermoelectric figure of merit of 1.3 at 900 K.« less

Authors:
 [1];  [1];  [1];  [2];  [2];  [3];  [2];  [1];  [1];  [4]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Univ. of Michigan, Ann Arbor, MI (United States)
  3. Beihang Univ., Beijing (China)
  4. Northwestern Univ., Evanston, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Revolutionary Materials for Solid State Energy Conversion (RMSSEC); Michigan State Univ., East Lansing, MI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1370358
Grant/Contract Number:  
SC0001054
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 137; Journal Issue: 35; Related Information: RMSSEC partners with Michigan State University (lead); University of California, Los Angeles; University of Michigan; Northwestern University; Oak Ridge National Laboratory; Ohio State University; Wayne State University; 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; Alloying; Thermodynamic modeling; Lattices; Transition metals

Citation Formats

Tan, Gangjian, Shi, Fengyuan, Hao, Shiqiang, Chi, Hang, Bailey, Trevor P., Zhao, Li-Dong, Uher, Ctirad, Wolverton, Chris, Dravid, Vinayak P., and Kanatzidis, Mercouri G. Valence Band Modification and High Thermoelectric Performance in SnTe Heavily Alloyed with MnTe. United States: N. p., 2015. Web. doi:10.1021/jacs.5b07284.
Tan, Gangjian, Shi, Fengyuan, Hao, Shiqiang, Chi, Hang, Bailey, Trevor P., Zhao, Li-Dong, Uher, Ctirad, Wolverton, Chris, Dravid, Vinayak P., & Kanatzidis, Mercouri G. Valence Band Modification and High Thermoelectric Performance in SnTe Heavily Alloyed with MnTe. United States. doi:10.1021/jacs.5b07284.
Tan, Gangjian, Shi, Fengyuan, Hao, Shiqiang, Chi, Hang, Bailey, Trevor P., Zhao, Li-Dong, Uher, Ctirad, Wolverton, Chris, Dravid, Vinayak P., and Kanatzidis, Mercouri G. Wed . "Valence Band Modification and High Thermoelectric Performance in SnTe Heavily Alloyed with MnTe". United States. doi:10.1021/jacs.5b07284. https://www.osti.gov/servlets/purl/1370358.
@article{osti_1370358,
title = {Valence Band Modification and High Thermoelectric Performance in SnTe Heavily Alloyed with MnTe},
author = {Tan, Gangjian and Shi, Fengyuan and Hao, Shiqiang and Chi, Hang and Bailey, Trevor P. and Zhao, Li-Dong and Uher, Ctirad and Wolverton, Chris and Dravid, Vinayak P. and Kanatzidis, Mercouri G.},
abstractNote = {Herein we demonstrate a high solubility limit of >9 mol% for MnTe alloying in SnTe. The electrical conductivity of SnTe decreases gradually while the Seebeck coefficient increases remarkably with increasing MnTe content, leading to enhanced power factors. The room-temperature Seebeck coefficients of Mn-doped SnTe are significantly higher than those predicted by theoretical Pisarenko plots for pure SnTe, indicating a modified band structure. The high-temperature Hall data of Sn1–xMnxTe show strong temperature dependence, suggestive of a two-valence-band conduction behavior. Moreover, the peak temperature of the Hall plot of Sn1–xMnxTe shifts toward lower temperature as MnTe content is increased, which is clear evidence of decreased energy separation (band convergence) between the two valence bands. The first-principles electronic structure calculations based on density functional theory also support this point. The higher doping fraction (>9%) of Mn in comparison with ~3% for Cd and Hg in SnTe gives rise to a much better valence band convergence that is responsible for the observed highest Seebeck coefficient of ~230 μV/K at 900 K. The high doping fraction of Mn in SnTe also creates stronger point defect scattering, which when combined with ubiquitous endotaxial MnTe nanostructures when the solubility of Mn is exceeded scatters a wide spectrum of phonons for a low lattice thermal conductivity of 0.9 W m–1 K–1 at 800 K. The synergistic role that Mn plays in regulating the electron and phonon transport of SnTe yields a high thermoelectric figure of merit of 1.3 at 900 K.},
doi = {10.1021/jacs.5b07284},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 35,
volume = 137,
place = {United States},
year = {2015},
month = {8}
}

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Works referencing / citing this record:

Valleytronics in thermoelectric materials
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Understanding the asymmetrical thermoelectric performance for discovering promising thermoelectric materials
journal, June 2019