First-Principle Calculation of Charge Carrier Mobility in 3D and 2D Hybrid Perovskites

We compute charge carrier mobilities of hybrid perovskite from complex band structure using the Quantum Espresso suite. An effective medium obtained from an appropriate configurational average acquires an imaginary ‘self-energy’ to that related to the mean scattering lifetime. We calculate the self-energy by matching the imaginary part of complex wave vector of the effective medium to that of the real configuration, where the interference effect between neighboring supercells is removed by an absorbing complex potential. The scattering lifetime yields the carrier mobility through Boltzmann transport equation. To allow computation over a sufficiently large supercell, the organic molecules in the hybrid perovskites are represented by an effective Molecular Pseudopotential. We calculate the 3D and 2D hybrid perovskite carrier mobility limited by the orientational disorder of the methylammonium ion and its dependence on temperature and, in the case 2D perovskite, thickness.