Spin-orbital coupling effect on power factor in semiconducting transition-metal dichalcogenide monolayers

TL;DR

This study investigates how spin-orbital coupling affects the thermoelectric power factor in semiconducting transition-metal dichalcogenide monolayers, revealing its varying impact on p-type and n-type doping and identifying promising materials.

Contribution

It provides a comprehensive analysis of SOC effects on thermoelectric properties across various TMDC monolayers using first-principles and Boltzmann transport theory, highlighting new insights into doping behaviors.

Findings

SOC reduces p-type power factor significantly.

SOC enhances n-type power factor in WX2 monolayers.

Pt-based TMDCs show highest Seebeck coefficients.

Abstract

The electronic structures and thermoelectric properties of semiconducting transition-metal dichalcogenide monolayers $\mathrm{MX_2}$ (M=Zr, Hf, Mo, W and Pt; X=S, Se and Te) are investigated by combining first-principles and Boltzmann transport theory, including spin-orbital coupling (SOC). It is found that the gap decrease increases from S to Te in each cation group, when the SOC is opened. The spin-orbital splitting has the same trend with gap reducing. Calculated results show that SOC has noteworthy detrimental effect on p-type power factor, while has a negligible influence in n-type doping except W cation group, which can be understood by considering the effects of SOC on the valence and conduction bands. For $\mathrm{WX_2}$ (X=S, Se and Te), the SOC leads to observably enhanced power factor in n-type doping, which can be explained by SOC-induced band degeneracy, namely bands converge. Among all cation groups, Pt cation group shows the highest Seebeck coefficient, which leads to best power factor, if we assume scattering time is fixed. Calculated results show that $\mathrm{MS_2}$ (M=Zr, Hf, Mo, W and Pt) have best p-type power factor for all cation groups, and that $\mathrm{MSe_2}$ (M=Zr and Hf), $\mathrm{WS_2}$ and $\mathrm{MTe_2}$ (M=Mo and Pt) have more wonderful n-type power factor in respective cation group. Therefore, these results may be useful for further theoretical prediction or experimental search of excellent thermoelectric materials from semiconducting transition-metal dichalcogenide monolayers.