journal article·2021-02-09

Temperature-Dependent Band Renormalization in CoSb3 Skutterudites Due to Sb-Ring-Related Vibrations

Ziyu Wang, Jinyang Xi, Jinyan Ning, Kai Guo, Bo Duan, Jun Luo, G. Jeffrey Snyder, Jiong Yang, Wenqing Zhang

Chemistry of Materials· Volume 33· Issue 3
Publisher page

Abstract

The temperature-dependent electronic structures in the thermoelectric semiconductor CoSb3 and its Yb-filled counterpart are studied by using the electron–phonon renormalization (EPR) method, considering both lattice expansion and phonon-induced atomic vibrations. The primary direct band gaps at the Γ-point for skutterudites decrease with increasing temperature, largely due to the increase in the energy level at the valance band maximum (VBM). The energy difference between the conduction band minimum (CBM) and second CB also decreases with temperature, inducing band convergence at high temperatures. The phonon vibrations of the Sb rings are responsible for these temperature-dependent electronic structures. Specifically, the four Sb-ring-related Ag phonon mode in CoSb3 plays a decisive role in causing the increase in the VBM with temperature and decrease in the primary band gap. The band convergence at high temperatures is due to the different responses to lattice vibrations of the second CB and the CBM for both systems. Our work sheds light on the relation between chemical bonds and phonon-assisted electronic structures.
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Research context

OpenAlex topics: Advanced Thermoelectric Materials and Devices · Chalcogenide Semiconductor Thin Films · Advanced Semiconductor Detectors and Materials

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Materials Genome Institute, Shanghai University, 99 Shangda Road, Shanghai 200444, China

School of Materials Science and Engineering, Shanghai University, 99 Shangda Road, Shanghai 200444, China

Hubei Key Laboratory of Theory and Application of Advanced Materials Mechanics, Wuhan University of Technology, Wuhan, Hubei 430070, China

Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, United States

Department of Physics and Shenzhen Institute for Quantum Science & Engineering, Southern University of Science and Technology, Shenzhen, Guangdong 518055, China

Guangdong Provincial Key Laboratory of Computational Science and Material Design, and Shenzhen Key Laboratory of Advanced Quantum Functional Materials and Devices, Southern University of Science and Technology, Shenzhen, Guangdong 518055, China

Funding

National Natural Science Foundation of China

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