Lawrence Berkeley National Laboratory

Here we develop a microscopic approach aimed at the description of a suite of physical effects related to carrier transport in, and the optical properties of, halide perovskites. Our theory is based on the description of the nuclear dynamics to all orders and goes beyond the common assumption of linear electron-phonon coupling in describing the carrier dynamics and band gap characteristics. When combined with first-principles calculations and applied to the prototypical MAPbI₃ system, our theory explains seemingly disparate experimental findings associated with both the charge-carrier mobility and optical absorption properties, including their temperature dependencies. Our findings demonstrate that orbital-overlap fluctuations in the lead-halide structure plays a significant role in determining the optoelectronic features of halide perovskites.