Strong Phonon–Phonon Interactions Securing Extraordinary Thermoelectric Ge1–xSbxTe with Zn-Alloying-Induced Band Alignment

Hong, Min; Wang, Yuan; Feng, Tianli; Sun, Qiang; Xu, Shengduo; Matsumura, Syo; Pantelides, Sokrates T.; Zou, Jin; Chen, Zhi-Gang

doi:10.1021/jacs.8b12624

Title: Strong Phonon–Phonon Interactions Securing Extraordinary Thermoelectric Ge_1–xSb_xTe with Zn-Alloying-Induced Band Alignment

Journal Article · Fri Dec 28 00:00:00 EST 2018 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.8b12624· OSTI ID:1597920

^[1]; Wang, Yuan ^[2];

^[3]; Sun, Qiang ^[4]; Xu, Shengduo ^[4]; Matsumura, Syo ^[5]; Pantelides, Sokrates T. ^[3];

^[4];

^[1]

University of Southern Queensland, Springfield (Australia); The University of Queensland, Brisbane (Australia)
University of Southern Queensland, Springfield (Australia)
Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
The University of Queensland, Brisbane (Australia)
Kyushu Univ., Fukuoka (Japan)

The ability of substitution atoms to decrease thermal conductivity is usually ascribed to the enhanced phonon-impurity scattering by assuming the original phonon dispersion relations. In this study, we find that 10% SbGe alloying in GeTe modifies the phonon dispersions significantly, closes the acoustic–optical phonon band gap, increases the phonon–phonon scattering rates, and reduces the phonon group velocities. These changes, together with grain boundaries, nanoprecipitates, and planar vacancies, lead to a significant decrease in the lattice thermal conductivity. In addition, an extra 2–6% Zn alloying decreases the energy offset between valence band edges at L and Σ points in Ge_1–xSb_xTe that is found to be induced by the Ge 4s² lone pairs. Since Zn is free of s² lone pair electrons, substituting Ge with Zn atoms can consequently diminish the Ge 4s² lone-pair characters and reduce the energy offset, resulting in two energetically merged valence band maxima. Further, the refined band structures render a power factor up to 40 μW cm^–1 K^–2 in Ge_0.86Sb_0.1Zn_0.04Te. Ultimately, a superhigh zT of 2.2 is achieved. This study clarifies the impacts of high-concentration substitutional atoms on phonon band structure, phonon–phonon scattering rates, and the convergence of electron valence band edges, which could provide guidelines for developing high-performance thermoelectric materials.

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Research Organization:: Vanderbilt Univ., Nashville, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC); Australian Research Council (ARC)

DOE Contract Number:: FG02-09ER46554

OSTI ID:: 1597920

Journal Information:: Journal of the American Chemical Society, Vol. 141, Issue 4; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

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Title: Strong Phonon–Phonon Interactions Securing Extraordinary Thermoelectric Ge1–xSbxTe with Zn-Alloying-Induced Band Alignment

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Title: Strong Phonon–Phonon Interactions Securing Extraordinary Thermoelectric Ge_1–xSb_xTe with Zn-Alloying-Induced Band Alignment