Suppression of intervalley scattering and enhanced phonon anharmonic interactions in 2D Bi2TeSe2: Crystal-field symmetry and band convergence

The electron-phonon (el-ph) and phonon-phonon interactions play a key role in determining electronic and thermal transport properties, respectively, in promising two-dimensional (2D) semiconductor devices. In this study, we investigated el-ph interactions using Wannier-Fourier interpolation method and renormalized phonon scattering considering finite-temperature effects in Bi2TeSe2 monolayer. The results show that the optical phonon modes dominate the carrier scattering, where level repulsion induced by crystal field splitting and spin-orbit coupling (SOC) effect effectively suppresses intervalley scattering, leading to high hole mobility. Moreover, the strong anharmonicity in Bi2TeSe2 monolayer results in the temperature-dependent softening of its optical phonons, along with a corresponding variation in interatomic force constants (IFCs). As a result, the lattice thermal conductivity is remarkably low and exhibits weak temperature dependence. Finally, the predicted dimensionless thermoelectric figure of merit exceeds unity in the range of 200 K–800 K, indicating the potential of Bi2TeSe2 monolayer for thermoelectric applications. This work provides new insights into the elimination of intervalley scattering by crystal field splitting and SOC effects, and paves the way for the evaluation of thermoelectric properties of materials with complex scattering mechanisms and strong anharmonicity.