Significant role of first-principles electron-phonon coupling in the electronic and thermoelectric properties of LiZnAs and ScAgC semiconductors (2506.13675v1)

Abstract: The half-Heusler (hH) compounds are currently considered promising thermoelectric (TE) materials due to their favorable thermopower and electrical conductivity. Accurate estimates of these properties are therefore highly desirable and require a detailed understanding of the microscopic mechanisms that govern transport. To enable such estimations, we carry out comprehensive first-principles computations of one of the primary factors limiting carrier transport, namely the electron-phonon ($e-ph$) interaction, in representative hH semiconductors such as LiZnAs and ScAgC. Our study first investigates the $e-ph$ renormalization of electronic dispersion based on the non-adiabatic Allen-Heine-Cardona theory. We then solve the Boltzmann transport equation (BTE) under multiple relaxation-time approximations (RTAs) to evaluate the carrier transport properties. Phonon-limited electron and hole mobilities are comparatively assessed using the linearized self-energy and momentum RTAs (SERTA and MRTA), and the exact or iterative BTE (IBTE) solutions within $e-ph$ coupling. Electrical transport coefficients for TE performance are also comparatively analyzed under the constant RTA (CRTA), SERTA, and MRTA schemes. The lattice thermal conductivity, determined from phonon-phonon interaction, is further reduced through nanostructuring techniques. The bulk LiZnAs (ScAgC) compound achieves the highest figure of merit ($zT$) of 1.05 (0.78) at 900 K with an electron doping concentration of 10$^{18}$ (10$^{19}$) cm$^{-3}$ under the MRTA scheme. This value significantly increases to 1.53 (1.0) for a 20 nm nanostructured sample. The remarkably high $zT$ achieved through inherently present phonon-induced electron scattering and the grain-boundary effect in semiconductors opens a promising path for discovering highly efficient and accurate hH materials for TE technology.