Achieving band convergence by tuning the bonding ionicity in n‐type Mg 3 Sb 2

Sun, Xin; Li, Xin; Yang, Jiong; Xi, Jinyang; Nelson, Ryky; Ertural, Christina; Dronskowski, Richard; Liu, Weishu; Snyder, Gerald J.; Singh, David J.; Zhang, Wenqing

doi:10.1002/jcc.25822

Title: Achieving band convergence by tuning the bonding ionicity in n‐type Mg ₃ Sb ₂

Journal Article · 19 March 2019 · Journal of Computational Chemistry

DOI: https://doi.org/10.1002/jcc.25822 · OSTI ID:1501950

Sun, Xin ^[1]; Li, Xin ^[1];

^[1]; Xi, Jinyang ^[1]; Nelson, Ryky ^[2]; Ertural, Christina ^[2];

^[2]; Liu, Weishu ^[3];

^[4]; Singh, David J. ^[5]; Zhang, Wenqing ^[6]

Materials Genome Institute Shanghai University No. 99 Shangda Road, Shanghai, 200444 China
Chair of Solid‐State and Quantum Chemistry Institute of Inorganic Chemistry and Jülich‐Aachen Research Alliance (JARA‐HPC), RWTH Aachen University D‐52056 Aachen Germany
Department of Materials Science and Engineering Southern University of Science and Technology No. 1088 Xueyuan Road, Shenzhen Guangdong, 518055 China
Department of Materials Science and Engineering Northwestern University Evanston Illinois 60208
Department of Physics and Astronomy University of Missouri Columbia Missouri 65211
Department of Physics and Shenzhen Institute for Quantum Science &, Technology Southern University of Science and Technology No. 1088 Xueyuan Road, Shenzhen Guangdong, 518055 China

Identifying strategies for beneficial band engineering is crucial for the optimization of thermoelectric (TE) materials. In this study, we demonstrate the beneficial effects of ionic dopants on n‐type Mg ₃ Sb ₂ . Using the band‐resolved projected crystal orbital Hamilton population, the covalent characters of the bonding between Mg atoms at different sites are observed. By partially substituting the Mg at the octahedral sites with more ionic dopants, such as Ca and Yb, the conduction band minimum (CBM) of Mg ₃ Sb ₂ is altered to be more anisotropic with an enhanced band degeneracy of 7. The CBM density of states of doped Mg ₃ Sb ₂ with these dopants is significantly enlarged by band engineering. The improved Seebeck coefficients and power factors, together with the reduced lattice thermal conductivities, imply that the partial introduction of more ionic dopants in Mg ₃ Sb ₂ is a general solution for its n‐type TE performance. © 2019 Wiley Periodicals, Inc.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0019114

OSTI ID:: 1501950

Journal Information:: Journal of Computational Chemistry, Journal Name: Journal of Computational Chemistry Journal Issue: 18 Vol. 40; ISSN 0192-8651

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Achieving band convergence by tuning the bonding ionicity in n‐type Mg ₃ Sb ₂