Synergy of Rashba and Topological Effects for High-Performance Bismuth-Based Thermoelectrics

Abstract: Band convergence is a key strategy for enhancing thermoelectric (TE) performance. Herein, we demonstrate a promising approach to enhance band convergence through inducing Rashba splitting in topological insulators. Theoretically designed Janus $\beta$-Bi$_2$Se$_2$Te and $\beta$-Bi$_2$Te$_2$Se exhibited inherent topological band inversion and Rashba splitting due to the strong spin-orbit coupling (SOC) with broken inversion symmetry. These characteristics synergistically improve band convergence, leading to a substantially enhanced power factor. Meanwhile, the Janus structural asymmetry suppresses lattice thermal conductivity. Consequently, Janus structures achieve boosted TE performance, especially for $\beta$-Bi$_2$Se$_2$Te, peaking figure of merit ($zT$) of 2.82. This work establishes a new framework for designing Janus topological compounds with high TE performance by the synergistic effect of Rashba splitting and band inversion.