Rapid Decoherence Induced by Light Expansion Suppresses Charge Recombination in Mixed Cation Perovskites: Time-Domain ab Initio Analysis

. We demonstrate that charge carrier lifetime extends by a factor of 1.5 within 1% lattice expansion; the bandgap grows only by 0.04 eV; the electron-phonon coupling increases by 13%; and the decoherence time shortens by 37%. The small bandgap change has negligible influence on recombination times. Lattice expansion enhances atomic fluctuations that lead to the enhancement of electron-phonon coupling and acceleration of decoherence. By creating several high-frequency phonon modes, the lattice expansion shortens the decoherence time further. As a result, rapid decoherence beats an enhanced electron-phonon coupling, playing the dominant role in suppressing the nonradiative electron-hole recombination. The light-induced lattice expansion or strain effects provide a rational route to improve the perovskite photovoltaic and photoelectronic device performance.