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Title: Polycrystalline ZrTe 5 Parametrized as a Narrow-Band-Gap Semiconductor for Thermoelectric Performance

Abstract

The transition-metal pentatellurides HfTe5 and ZrTe5 have been studied for their exotic transport properties with much debate over the transport mechanism, band gap, and cause of the resistivity behavior, including a large low-temperature resistivity peak. Single crystals grown by the chemical-vapor-transport method have shown an n-p transition of the Seebeck coefficient at the same temperature as a peak in the resistivity. We show that behavior similar to that of single crystals can be observed in iodine-doped polycrystalline samples but that undoped polycrystalline samples exhibit drastically different properties: they are p type over the entire temperature range. Additionally, the thermal conductivity for polycrystalline samples is much lower, 1.5 Wm -1 K -1, than previously reported for single crystals. It is found that the polycrystalline ZrTe 5 system can be modeled as a simple semiconductor with conduction and valence bands both contributing to transport, separated by a band gap of 20 meV. This model demonstrates to first order that a simple two-band model can explain the transition from n- to p-type behavior and the cause of the anomalous resistivity peak. Combined with the experimental data, the two-band model shows that carrier concentration variation is responsible for differences in behavior between samples. Usingmore » the twoband model, the thermoelectric performance at different doping levels is predicted, finding zT =0.2 and 0.1 for p and n type, respectively, at 300 K, and zT= 0.23 and 0.32 for p and n type at 600 K. Given the reasonably high zT that is comparable in magnitude for both n and p type, a thermoelectric device with a single compound used for both legs is feasible.« less

Authors:
; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Solid-State Solar-Thermal Energy Conversion Center (S3TEC); Argonne National Lab. (ANL), Argonne, IL (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1423194
Alternate Identifier(s):
OSTI ID: 1417937; OSTI ID: 1419961
Report Number(s):
NREL/JA-5K00-71006
Journal ID: ISSN 2331-7019; PRAHB2; 138353
Grant/Contract Number:  
AC02-06CH11357; SC0001299; FG02-09ER46577; AC36-08GO28308
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Applied
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2331-7019
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; band gap; charge density waves; thermoelectric effects; semiconductor compounds

Citation Formats

Miller, Samuel A., Witting, Ian, Aydemir, Umut, Peng, Lintao, Rettie, Alexander J. E., Gorai, Prashun, Chung, Duck Young, Kanatzidis, Mercouri G., Grayson, Matthew, Stevanović, Vladan, Toberer, Eric S., and Snyder, G. Jeffrey. Polycrystalline ZrTe5 Parametrized as a Narrow-Band-Gap Semiconductor for Thermoelectric Performance. United States: N. p., 2018. Web. doi:10.1103/PhysRevApplied.9.014025.
Miller, Samuel A., Witting, Ian, Aydemir, Umut, Peng, Lintao, Rettie, Alexander J. E., Gorai, Prashun, Chung, Duck Young, Kanatzidis, Mercouri G., Grayson, Matthew, Stevanović, Vladan, Toberer, Eric S., & Snyder, G. Jeffrey. Polycrystalline ZrTe5 Parametrized as a Narrow-Band-Gap Semiconductor for Thermoelectric Performance. United States. doi:10.1103/PhysRevApplied.9.014025.
Miller, Samuel A., Witting, Ian, Aydemir, Umut, Peng, Lintao, Rettie, Alexander J. E., Gorai, Prashun, Chung, Duck Young, Kanatzidis, Mercouri G., Grayson, Matthew, Stevanović, Vladan, Toberer, Eric S., and Snyder, G. Jeffrey. Mon . "Polycrystalline ZrTe5 Parametrized as a Narrow-Band-Gap Semiconductor for Thermoelectric Performance". United States. doi:10.1103/PhysRevApplied.9.014025. https://www.osti.gov/servlets/purl/1423194.
@article{osti_1423194,
title = {Polycrystalline ZrTe5 Parametrized as a Narrow-Band-Gap Semiconductor for Thermoelectric Performance},
author = {Miller, Samuel A. and Witting, Ian and Aydemir, Umut and Peng, Lintao and Rettie, Alexander J. E. and Gorai, Prashun and Chung, Duck Young and Kanatzidis, Mercouri G. and Grayson, Matthew and Stevanović, Vladan and Toberer, Eric S. and Snyder, G. Jeffrey},
abstractNote = {The transition-metal pentatellurides HfTe5 and ZrTe5 have been studied for their exotic transport properties with much debate over the transport mechanism, band gap, and cause of the resistivity behavior, including a large low-temperature resistivity peak. Single crystals grown by the chemical-vapor-transport method have shown an n-p transition of the Seebeck coefficient at the same temperature as a peak in the resistivity. We show that behavior similar to that of single crystals can be observed in iodine-doped polycrystalline samples but that undoped polycrystalline samples exhibit drastically different properties: they are p type over the entire temperature range. Additionally, the thermal conductivity for polycrystalline samples is much lower, 1.5 Wm-1 K-1, than previously reported for single crystals. It is found that the polycrystalline ZrTe5 system can be modeled as a simple semiconductor with conduction and valence bands both contributing to transport, separated by a band gap of 20 meV. This model demonstrates to first order that a simple two-band model can explain the transition from n- to p-type behavior and the cause of the anomalous resistivity peak. Combined with the experimental data, the two-band model shows that carrier concentration variation is responsible for differences in behavior between samples. Using the twoband model, the thermoelectric performance at different doping levels is predicted, finding zT =0.2 and 0.1 for p and n type, respectively, at 300 K, and zT= 0.23 and 0.32 for p and n type at 600 K. Given the reasonably high zT that is comparable in magnitude for both n and p type, a thermoelectric device with a single compound used for both legs is feasible.},
doi = {10.1103/PhysRevApplied.9.014025},
journal = {Physical Review Applied},
issn = {2331-7019},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {1}
}

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Figures / Tables:

FIG. 1 FIG. 1: Schematic of two band model for iodine doped polycrystalline sample (or vapor grown single crystals) showing movement of the Fermi level with increasing temperature and the resulting properties.

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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.