Investigating Ultrafast Excited-state Proton Transfer With Nonadiabatic Dynamics Simulations

Photoinduced processes resulting in the transfer of protons and electrons play a vital role in artificial solar energy conversion devices. Therefore a fundamental mechanistic understanding of photoinduced electron/proton transfer processes is essential for improving the efficiency and guiding the design of such devices. In order to obtain detailed insights into the excited-state proton transfer process and the role of the solvent in modulating it, we carry out on-the-fly nonadiabatic dynamics simulations with explicit solvent in a hybrid quantum mechanical/molecular mechanical (QM/MM) framework. The electronic surfaces are generated by a semiempirical implementation of the floating occupation molecular orbital complete active space configuration interaction (FOMO-CASCI) method and the molecular dynamics with quantum transitions (MDQT) surface-hopping method is used to account for nonadiabatic transitions.