First-principles calculations of charge carrier mobility and conductivity in bulk semiconductors and two-dimensional materials

Abstract

One of the fundamental properties of semiconductors is their ability to support highly tunable electric currents in the presence of electric fields or carrier concentration gradients. These properties are described by transport coefficients such as electron and hole mobilities. Recently, advances in electronic structure methods for real materials have made it possible to study these properties with predictive accuracy and without resorting to empirical parameters. Here, we review the most recent developments in the area of ab initio calculations of carrier mobilities of semiconductors. In the first part, we offer a brief historical overview of approaches to the calculation of carrier mobilities, and we establish the conceptual framework underlying modern ab initio approaches. We summarize the Boltzmann theory of carrier transport and we discuss its scope of applicability, merits, and limitations in the broader context of many-body Green's function approaches. We discuss recent implementations of the Boltzmann formalism within the context of density functional theory and many-body perturbation theory calculations, placing an emphasis on the key computational challenges and suggested solutions. In the second part, we discuss recent investigations of classic materials such as silicon, diamond, GaAs, GaN, Ga2O3, and lead halide perovskites as well as low-dimensional semiconductors such as graphene, silicene, phosphorene, MoS2, and InSe. We also review recent efforts toward high-throughput calculations of carrier transport. In the last part, we discuss the extension of the methodology to study spintronics and topological materials and we comment on the possibility of incorporating Berry-phase effects and many-body correlations beyond the standard Boltzmann formalism.