When band convergence is not beneficial for thermoelectrics

Park, Junsoo; Dylla, Maxwell; Xia, Yi; Wood, Max; Snyder, G. Jeffrey; Jain, Anubhav

doi:10.1038/s41467-021-23839-w

Title: When band convergence is not beneficial for thermoelectrics

Journal Article · 07 June 2021 · Nature Communications

DOI: https://doi.org/10.1038/s41467-021-23839-w · OSTI ID:1787114

; Dylla, Maxwell; Xia, Yi; Wood, Max; Snyder, G. Jeffrey;

Abstract Band convergence is considered a clear benefit to thermoelectric performance because it increases the charge carrier concentration for a given Fermi level, which typically enhances charge conductivity while preserving the Seebeck coefficient. However, this advantage hinges on the assumption that interband scattering of carriers is weak or insignificant. With first-principles treatment of electron-phonon scattering in the CaMg ₂ Sb ₂ -CaZn ₂ Sb ₂ Zintl system and full Heusler Sr ₂ SbAu, we demonstrate that the benefit of band convergence can be intrinsically negated by interband scattering depending on the manner in which bands converge. In the Zintl alloy, band convergence does not improve weighted mobility or the density-of-states effective mass. We trace the underlying reason to the fact that the bands converge at a one k-point, which induces strong interband scattering of both the deformation-potential and the polar-optical kinds. The case contrasts with band convergence at distant k-points (as in the full Heusler), which better preserves the single-band scattering behavior thereby successfully leading to improved performance. Therefore, we suggest that band convergence as thermoelectric design principle is best suited to cases in which it occurs at distant k-points.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1787114

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 12; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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