Understanding the role and interplay of heavy-hole and light-hole valence bands in the thermoelectric properties of PbSe
Abstract
The thermoelectric properties of PbSe have significantly improved in recent years reaching figures of merit ZT~1.6. The transport properties of the hole-doped high temperature thermoelectric material PbSe are particularly interesting and play a key role in this. Here, they were analyzed over wide temperature and hole concentration ranges. The special features observed in the variation of the experimental Seebeck coefficient and Hall coefficient can be accounted for within the framework of a two-band model. Two valence bands separated by a temperature dependent energy offset are considered. Furthermore, the extremum of the light-hole band has a density of states mass ~0.27mo at room temperature. It is nonparabolic and anisotropic and can be described by the Kane model. The extremum of the heavy-hole band is isotropic and parabolic with a much larger density of states mass ~2.5mo. We find that for heavily doped compositions, the high mass band contributes the Seebeck coefficient, even at room temperature. With rising temperature, holes are transferred from the light-hole to the heavy-hole branch, giving rise to the anomalous temperature dependent Hall coefficient, which is found peaked near ~650K. For Na-doped samples Pb1–xNaxSe for 0.01 ≤ x ≤ 0.03, the high thermopower values of 200–300μV/K at 900more »
- Authors:
-
- Northwestern Univ., Evanston, IL (United States)
- Aristotle Univ. of Thessaloniki (Greece)
- Univ. of Michigan, Ann Arbor, MI (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Revolutionary Materials for Solid State Energy Conversion (RMSSEC)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1370356
- Alternate Identifier(s):
- OSTI ID: 1181587
- Grant/Contract Number:
- SC0001054
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review. B, Condensed Matter and Materials Physics
- Additional Journal Information:
- Journal Volume: 91; Journal Issue: 8; 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 1098-0121
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Chasapis, Thomas C., Lee, Yeseul, Hatzikraniotis, Euripides, Paraskevopoulos, Konstantinos M., Chi, Hang, Uher, Ctirad, and Kanatzidis, Mercouri G. Understanding the role and interplay of heavy-hole and light-hole valence bands in the thermoelectric properties of PbSe. United States: N. p., 2015.
Web. doi:10.1103/PhysRevB.91.085207.
Chasapis, Thomas C., Lee, Yeseul, Hatzikraniotis, Euripides, Paraskevopoulos, Konstantinos M., Chi, Hang, Uher, Ctirad, & Kanatzidis, Mercouri G. Understanding the role and interplay of heavy-hole and light-hole valence bands in the thermoelectric properties of PbSe. United States. https://doi.org/10.1103/PhysRevB.91.085207
Chasapis, Thomas C., Lee, Yeseul, Hatzikraniotis, Euripides, Paraskevopoulos, Konstantinos M., Chi, Hang, Uher, Ctirad, and Kanatzidis, Mercouri G. Sun .
"Understanding the role and interplay of heavy-hole and light-hole valence bands in the thermoelectric properties of PbSe". United States. https://doi.org/10.1103/PhysRevB.91.085207. https://www.osti.gov/servlets/purl/1370356.
@article{osti_1370356,
title = {Understanding the role and interplay of heavy-hole and light-hole valence bands in the thermoelectric properties of PbSe},
author = {Chasapis, Thomas C. and Lee, Yeseul and Hatzikraniotis, Euripides and Paraskevopoulos, Konstantinos M. and Chi, Hang and Uher, Ctirad and Kanatzidis, Mercouri G.},
abstractNote = {The thermoelectric properties of PbSe have significantly improved in recent years reaching figures of merit ZT~1.6. The transport properties of the hole-doped high temperature thermoelectric material PbSe are particularly interesting and play a key role in this. Here, they were analyzed over wide temperature and hole concentration ranges. The special features observed in the variation of the experimental Seebeck coefficient and Hall coefficient can be accounted for within the framework of a two-band model. Two valence bands separated by a temperature dependent energy offset are considered. Furthermore, the extremum of the light-hole band has a density of states mass ~0.27mo at room temperature. It is nonparabolic and anisotropic and can be described by the Kane model. The extremum of the heavy-hole band is isotropic and parabolic with a much larger density of states mass ~2.5mo. We find that for heavily doped compositions, the high mass band contributes the Seebeck coefficient, even at room temperature. With rising temperature, holes are transferred from the light-hole to the heavy-hole branch, giving rise to the anomalous temperature dependent Hall coefficient, which is found peaked near ~650K. For Na-doped samples Pb1–xNaxSe for 0.01 ≤ x ≤ 0.03, the high thermopower values of 200–300μV/K at 900 K arise from the heavy-hole band, which are responsible for the excellent thermoelectric performance of PbSe.},
doi = {10.1103/PhysRevB.91.085207},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
number = 8,
volume = 91,
place = {United States},
year = {Sun Feb 15 00:00:00 EST 2015},
month = {Sun Feb 15 00:00:00 EST 2015}
}
Web of Science
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