Fully-Integrated Surface Hopping as Quantum Decoherence Correction in Nonadiabatic Dynamics

In this work, we present a fully integrated surface hopping approach for nonadiabatic molecular dynamics simulations in extended atomistic systems. In lieu of conducting on-the-fly hopping processes in multiple surface hopping realizations, within the neglect of back-reaction approximation, it is possible to conduct a full resummation of the population dynamics for indefinite time with modest computational cost. Our method provides a way to sum up all histories of piece-wise coherent evolution of quantum system altered with the wave function collapses, yielding converged population dynamics without the need for multiple trajectories. The method can also be viewed as a way to represent decoherence correction in nonadiabatic dynamics. The performance of the approach is demonstrated by comparing its performance with that of the standard trajectory surface hopping approaches with and without decoherence correction as applied to a spin-boson Hamiltonian model and an atomistic fullerene example.