Great Influence of Pressure and Isotope Effects on Nonradiative Charge Loss in Hybrid Organic-Inorganic Perovskites.

Abstract

The intrinsic softness of hybrid organic-inorganic perovskites (HOIPs) allows their lattice and optoelectronic performance to be tunable to external pressure. Using nonadiabatic (NA) molecular dynamics, we demonstrate that a mild pressure accelerates hot electron relaxation and suppresses nonradiative electron-hole recombination in CH3NH3PbI3. Both processes are governed by NA coupling, which is enhanced between the electronic states of the quasi-continuous bands while is decreased between the band-edge states by reducing the electron-hole wave function overlap. Hydrogen/deuterium isotope exchange alleviates the pressure-induced NA coupling by increasing lattice rigidity and decreasing wave function overlap, slowing down both the hot electron relaxation and electron-hole recombination processes. The simulated time scales of sub-3 ps for hot electron relaxation and half nanoseconds for recombination agree well with the experiments. The study suggests that the isotope exchange can mitigate the pressure-caused fast losses of hot electrons and further prolong the charge carrier lifetime in HOIPs.