Ultrafast Charge Transfer Coupled to Quantum Proton Motion at Molecule/Metal Oxide Interface

Understanding the ultrafast dynamics of photoexcited carriers at semiconductor/molecule interface is essential for improving solar energy conversion efficiency. At such interfaces, hydrogen bond (H-bond) network often formed, and quantum proton motion expected. However, how nuclear effects (NQEs) will influence charge transfer still unknown. By combining two kinds emerging molecular methods ab initio level - path-integral based time-dependent nonadiabatic dynamics, choosing CH3OH/TiO as a prototypical system to study, we find that in H-bond strongly coupled with interface. The hole trapping ability of adsorbed CH3OH molecule then notably enhanced by NQEs, thus, it behaves scavenger on TiO2. It concluded may play critical role enhancing efficiency photoexcitation.