We investigate photoinduced proton-coupled electron transfer (PI-PCET) reaction through a recently developed quasi-diabatic (QD) quantum dynamics propagation scheme. This scheme allows us to use accurate diabatic based dynamics approach with adiabatic electronic calculation for on-the-fly propagation. Here, we investigate PI-PCET non-adiabatic dynamics with Partial Linearized Density Matrix (PLDM) path-integral dynamics and the instantaneous adiabatic electron-proton vibronic basis. Our numerical results demonstrate the importance of treating proton quantum mechanically for an accurate description of PI-PCET dynamics, the role of solvent fluctuation and its impact on proton tunneling, and various reaction regimes that exhibit different kinetic isotope effects. This work opens the possibility for studying PI-PCET reaction in realistic chemical and biological systems through combining accurate diabatic quantum dynamics approach with efficient adiabatic electronic structure calculations.

Enhancing singlet-fission dynamics by suppressing destructive interference between charge-transfer pathways

256th National Meeting (2018)

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