Ultrahigh zT from strong electron-phonon interactions and a low-dimensional Fermi surface

V. K. Ranganayakulu; Te Hsien Wang; Cheng Lung Chen; Angus Huang; Ma Hsuan Ma; Chun Min Wu; Wei Han Tsai; Tsu Lien Hung; Min Nan Ou; Horng Tay Jeng; Chih Hao Lee; Kuei Hsien Chen; Wen Hsien Li; Madison K. Brod; G. Jeffrey Snyder; Yang Yuan Chen

doi:10.1039/d3ee04187e

Ultrahigh zT from strong electron-phonon interactions and a low-dimensional Fermi surface

V. K. Ranganayakulu, Te Hsien Wang, Cheng Lung Chen, Angus Huang, Ma Hsuan Ma, Chun Min Wu, Wei Han Tsai, Tsu Lien Hung, Min Nan Ou, Horng Tay Jeng, Chih Hao Lee, Kuei Hsien Chen, Wen Hsien Li, Madison K. Brod, G. Jeffrey Snyder, Yang Yuan Chen

Department of Physics

Research output: Contribution to journal › Article › peer-review

9 Scopus citations

Abstract

The outstanding thermoelectric performance of GeTe has attracted significant attention in the research community in recent years. However, many of the underlying physical mechanisms that contribute to GeTe's exceptionally high figure of merit (zT) remain not fully understood. In this study, an Sb-Bi codoped GeTe single crystal (Ge_0.86Sb_0.08Bi_0.06)Te with an ultrahigh zT of 2.7 at 700 K and a record high device zT of 1.41 in the temperature range of 300-773 K was synthesized and investigated. The ultrahigh zT is attributed to the extremely low lattice thermal conductivity induced by strong electron-phonon (EP) interactions as revealed by the experimentally observed Kohn anomaly, through inelastic neutron scattering (INS) measurements. First-principles calculations further demonstrate that the remarkable EP interaction arises from the Fermi surface nesting featured in a one-dimensional (double-walled) topology. Our finding unravels the ultrahigh-zT mechanism in GeTe-based materials, serving as an inspiring guide toward high thermoelectric performance.

Original language	English
Pages (from-to)	1904-1915
Number of pages	12
Journal	Energy and Environmental Science
Volume	17
Issue number	5
DOIs	https://doi.org/10.1039/d3ee04187e
State	Published - 27 Jan 2024

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Ranganayakulu, V. K., Wang, T. H., Chen, C. L., Huang, A., Ma, M. H., Wu, C. M., Tsai, W. H., Hung, T. L., Ou, M. N., Jeng, H. T., Lee, C. H., Chen, K. H., Li, W. H., Brod, M. K., Snyder, G. J., & Chen, Y. Y. (2024). Ultrahigh zT from strong electron-phonon interactions and a low-dimensional Fermi surface. Energy and Environmental Science, 17(5), 1904-1915. https://doi.org/10.1039/d3ee04187e

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abstract = "The outstanding thermoelectric performance of GeTe has attracted significant attention in the research community in recent years. However, many of the underlying physical mechanisms that contribute to GeTe's exceptionally high figure of merit (zT) remain not fully understood. In this study, an Sb-Bi codoped GeTe single crystal (Ge0.86Sb0.08Bi0.06)Te with an ultrahigh zT of 2.7 at 700 K and a record high device zT of 1.41 in the temperature range of 300-773 K was synthesized and investigated. The ultrahigh zT is attributed to the extremely low lattice thermal conductivity induced by strong electron-phonon (EP) interactions as revealed by the experimentally observed Kohn anomaly, through inelastic neutron scattering (INS) measurements. First-principles calculations further demonstrate that the remarkable EP interaction arises from the Fermi surface nesting featured in a one-dimensional (double-walled) topology. Our finding unravels the ultrahigh-zT mechanism in GeTe-based materials, serving as an inspiring guide toward high thermoelectric performance.",

author = "Ranganayakulu, {V. K.} and Wang, {Te Hsien} and Chen, {Cheng Lung} and Angus Huang and Ma, {Ma Hsuan} and Wu, {Chun Min} and Tsai, {Wei Han} and Hung, {Tsu Lien} and Ou, {Min Nan} and Jeng, {Horng Tay} and Lee, {Chih Hao} and Chen, {Kuei Hsien} and Li, {Wen Hsien} and Brod, {Madison K.} and Snyder, {G. Jeffrey} and Chen, {Yang Yuan}",

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AU - Ranganayakulu, V. K.

AU - Wang, Te Hsien

AU - Chen, Cheng Lung

AU - Huang, Angus

AU - Ma, Ma Hsuan

AU - Wu, Chun Min

AU - Tsai, Wei Han

AU - Hung, Tsu Lien

AU - Ou, Min Nan

AU - Jeng, Horng Tay

AU - Lee, Chih Hao

AU - Chen, Kuei Hsien

AU - Li, Wen Hsien

AU - Brod, Madison K.

AU - Snyder, G. Jeffrey

AU - Chen, Yang Yuan

PY - 2024/1/27

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N2 - The outstanding thermoelectric performance of GeTe has attracted significant attention in the research community in recent years. However, many of the underlying physical mechanisms that contribute to GeTe's exceptionally high figure of merit (zT) remain not fully understood. In this study, an Sb-Bi codoped GeTe single crystal (Ge0.86Sb0.08Bi0.06)Te with an ultrahigh zT of 2.7 at 700 K and a record high device zT of 1.41 in the temperature range of 300-773 K was synthesized and investigated. The ultrahigh zT is attributed to the extremely low lattice thermal conductivity induced by strong electron-phonon (EP) interactions as revealed by the experimentally observed Kohn anomaly, through inelastic neutron scattering (INS) measurements. First-principles calculations further demonstrate that the remarkable EP interaction arises from the Fermi surface nesting featured in a one-dimensional (double-walled) topology. Our finding unravels the ultrahigh-zT mechanism in GeTe-based materials, serving as an inspiring guide toward high thermoelectric performance.

AB - The outstanding thermoelectric performance of GeTe has attracted significant attention in the research community in recent years. However, many of the underlying physical mechanisms that contribute to GeTe's exceptionally high figure of merit (zT) remain not fully understood. In this study, an Sb-Bi codoped GeTe single crystal (Ge0.86Sb0.08Bi0.06)Te with an ultrahigh zT of 2.7 at 700 K and a record high device zT of 1.41 in the temperature range of 300-773 K was synthesized and investigated. The ultrahigh zT is attributed to the extremely low lattice thermal conductivity induced by strong electron-phonon (EP) interactions as revealed by the experimentally observed Kohn anomaly, through inelastic neutron scattering (INS) measurements. First-principles calculations further demonstrate that the remarkable EP interaction arises from the Fermi surface nesting featured in a one-dimensional (double-walled) topology. Our finding unravels the ultrahigh-zT mechanism in GeTe-based materials, serving as an inspiring guide toward high thermoelectric performance.

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Ultrahigh zT from strong electron-phonon interactions and a low-dimensional Fermi surface

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