Isotopic Exchange Extends Charge Carrier Lifetime in Metal Lead Perovskites by Quantum Dynamics Simulations

One may expect that isotopic exchange has no influence on charge carrier lifetime and perovskite solar cell performance because isotopic effects do not affect the fundamental electronic structure of materials. Experiments defy this expectation. By performing nonadiabatic (NA) molecular dynamics simulations, we demonstrate that hydrogen and deuterium exchange significantly enhances the excited-state lifetime and stability of CH3NH3PbI3. Replacing lighter hydrogen with heavier deuterium suppresses the collective motions of organic and inorganic components, thus enhancing lattice stiffness and decreasing the NA coupling. Isotopic exchange further reduces NA coupling by localizing electron wave functions for separation of electrons and holes, which beats the extended coherence time, slowing down nonradiative electron–hole recombination from CH3ND3PbI3 to CD3ND3PbI3 with respect to the pristine system. The unchanged fundamental electronic structure together with the prolonged carrier lifetime and enhanced stability rationalize the improvement of the deuterated CH3NH3PbI3 solar cells. Our work provides valuable insights into isotope effects for the design of high-performance perovskite photovoltaic and optoelectronic devices.