A Chemical Understanding of the Band Convergence in Thermoelectric CoSb 3 Skutterudites: Influence of Electron Population, Local Thermal Expansion, and Bonding Interactions

Hanus, Riley; Guo, Xingyu; Tang, Yinglu; Li, Guodong; Snyder, G. Jeffrey; Zeier, Wolfgang G.

doi:10.1021/acs.chemmater.6b04506

Title: A Chemical Understanding of the Band Convergence in Thermoelectric CoSb ₃ Skutterudites: Influence of Electron Population, Local Thermal Expansion, and Bonding Interactions

Journal Article · Fri Jan 13 00:00:00 EST 2017 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.6b04506· OSTI ID:1347010

Hanus, Riley; Guo, Xingyu; Tang, Yinglu; Li, Guodong; Snyder, G. Jeffrey;

N-Type skutterudites, such as Yb_xCo₄Sb₁₂, have recently been shown to exhibit high valley degeneracy with possible band convergence, explaining the excellent thermoelectric efficiency of these materials. Using a combined theoretical and experimental approach involving temperature-dependent synchrotron diffraction, molecular orbital diagrams, and computational studies, the chemical nature of critical features in the band structure is highlighted. We identify how n-type doping on the filler site induces structural changes that are observed in both the diffraction data and computational results. Additionally, we show how chemical n-type doping slightly alters the electronic band structure, moving the high-valley degeneracy secondary conduction band closer to the primary conduction band and thus inducing band convergence.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

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

OSTI ID:: 1347010

Journal Information:: Chemistry of Materials, Vol. 29, Issue 3; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: ENGLISH

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Title: A Chemical Understanding of the Band Convergence in Thermoelectric CoSb ₃ Skutterudites: Influence of Electron Population, Local Thermal Expansion, and Bonding Interactions