Volume 21, Issue 9 2411244
Research Article

Thermoelectric Properties of a Light Compound Fe2S2: the Role of Electron Correlation Strengthened Spin-Orbital Coupling

Xincan Wang

Xincan Wang

Center of Quantum Materials and Devices, College of Physics, Chongqing University, Chongqing, 401331 China

Search for more papers by this author
Zizhen Zhou

Corresponding Author

Zizhen Zhou

Center of Quantum Materials and Devices, College of Physics, Chongqing University, Chongqing, 401331 China

E-mail: [email protected]; [email protected]

Search for more papers by this author
Xiaolong Yang

Xiaolong Yang

Center of Quantum Materials and Devices, College of Physics, Chongqing University, Chongqing, 401331 China

Search for more papers by this author
Guang Han

Guang Han

College of Materials Science and Engineering, Chongqing University, Chongqing, 400044 China

Search for more papers by this author
Xu Lu

Xu Lu

Center of Quantum Materials and Devices, College of Physics, Chongqing University, Chongqing, 401331 China

Search for more papers by this author
Guoyu Wang

Guoyu Wang

College of Materials Science and Engineering, Chongqing University, Chongqing, 400044 China

Search for more papers by this author
Xiaoyuan Zhou

Corresponding Author

Xiaoyuan Zhou

Center of Quantum Materials and Devices, College of Physics, Chongqing University, Chongqing, 401331 China

E-mail: [email protected]; [email protected]

Search for more papers by this author
First published: 13 January 2025

Abstract

Spin-orbit coupling (SOC) induced nontrivial bandgap and complex Fermi surface has been considered to be profitable for thermoelectrics, which, however, is generally appreciable only in heavy elements, thereby detrimental to practical application. In this study, the SOC-driven extraordinary thermoelectric performance in a light 2D material Fe₂S₂ is demonstrated via first-principles calculations. The abnormally strong SOC, induced by electron correlation through 3d orbitals polarization, significantly renormalizes the band structures, which opens the bandgap via Fe 3d orbitals inversion, exposes the second conduction valley with weak electron-phonon coupling, and aligns the energy of Fe 3d and S 3p orbitals with divergent momentum in valence band. Such topological band renormalization triggers improvement of both p- and n-type power factors by more than 200%. Combining with the low lattice thermal conductivity caused by lone pair electrons and intense high-order phonon scattering, the peak zT can reach 1.6 and 1.8 for p- and n-type Fe₂S₂ at 400 K, respectively. This work unravels the mechanism of SOC-provoked high zT in electron correlation systems, which inspires the development of high-performance thermoelectric materials without heavy and scarce elements.

Conflict of Interest

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

The full text of this article hosted at iucr.org is unavailable due to technical difficulties.