ΔSCF with Subsystem Density Embedding for Efficient Nonadiabatic Molecular Dynamics in Condensed-Phase Systems

Abstract

An approach combining subsystem density embedding with the variational delta self-consistent field is presented, which extends current capabilities for excited-electronic-state calculations. It was applied on full-atomic nonadiabatic dynamics of a solvated diimide system, demonstrating that comparable accuracy can be achieved for this system for the investigated configuration space and with a shorter simulation time than the computationally more expensive conventional Kohn–Sham density functional theory-based method. This opens a new pragmatic technique for efficient simulation of nonadiabatic processes in the condensed phase, in particular, for liquids.