Band structure engineering and thermoelectric properties of charge-compensated filled skutterudites

Shi, Xiaoya; Yang, Jiong; Wu, Lijun; Salvador, James R.; Zhang, Cheng; Villaire, William L.; Haddad, Daad; Yang, Jihui; Zhu, Yimei; Li, Qiang

doi:10.1038/srep14641

Title: Band structure engineering and thermoelectric properties of charge-compensated filled skutterudites

Journal Article · Mon Oct 12 00:00:00 EDT 2015 · Scientific Reports

DOI:https://doi.org/10.1038/srep14641· OSTI ID:1235857

Shi, Xiaoya ^[1]; Yang, Jiong ^[2]; Wu, Lijun ^[1]; Salvador, James R. ^[3]; Zhang, Cheng ^[1]; Villaire, William L. ^[4]; Haddad, Daad ^[3]; Yang, Jihui ^[2]; Zhu, Yimei ^[1]; Li, Qiang ^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States)
Univ. of Washington, Seattle, WA (United States)
General Motors R&D Center, Warren, MI (United States)
General Motor Global Design, Engineering and Product Programs, Warren, MI (United States)

Thermoelectric properties of semiconductors are intimately related to their electronic band structure, which can be engineered via chemical doping. Dopant Ga in the cage-structured skutterudite Co₄Sb₁₂ substitutes Sb sites while occupying the void sites. Combining quantitative scanning transmission electron microscopy and first-principles calculations, we show that Ga dual-site occupancy breaks the symmetry of the Sb-Sb network, splits the deep triply-degenerate conduction bands, and drives them downward to the band edge. The charge-compensating nature of the dual occupancy Ga increases overall filling fraction limit. By imparting this unique band structure feature, and judiciously doping the materials by increasing the Yb content, we promote the Fermi level to a point where carriers are in energetic proximity to these features. Increased participation of these heavier bands in electronic transport leads to increased thermopower and effective mass. Further, the localized distortion from Ga/Sb substitution enhances the phonon scattering to reduce the thermal conductivity effectively.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

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

Grant/Contract Number:: SC00112704

OSTI ID:: 1235857

Report Number(s):: BNL-111606-2015-JA; R&D Project: MA015MACA; KC0201010

Journal Information:: Scientific Reports, Vol. 5, Issue 48; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 34 works

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Thermoelectric transport properties of Ni-, Pd-, and Pt- doped skutterudites with S-filling as charge compensation Tu, Zhikang; Sun, Xin; Li, Xin AIP Advances, Vol. 9, Issue 4 https://doi.org/10.1063/1.5095820	journal	April 2019
Characterization of rattling in relation to thermal conductivity: Ordered half-Heusler semiconductors Feng, Zhenzhen; Fu, Yuhao; Zhang, Yongsheng Physical Review B, Vol. 101, Issue 6 https://doi.org/10.1103/physrevb.101.064301	journal	February 2020
Characterization of rattling in relation to thermal conductivity: ordered half-Heusler semiconductors Feng, Zhenzhen; Fu, Yuhao; Zhang, Yongsheng arXiv https://doi.org/10.48550/arxiv.2001.08029	text	January 2020

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