Flexible Surface Hopping Approach to Model the Crossover from Hopping to Band-like Transport in Organic Crystals.

Abstract

Two distinct pictures are usually evoked when modeling charge transport in organic crystals, that is, band and hopping models, the signature of which is conveyed by a characteristic temperature dependence of mobility. Here, we present a novel flexible surface hopping approach compliant with general Hamiltonians that is able to grasp the crossover from hopping to band-like transport regimes. This approach is applied to solve a one-dimensional mixed quantum-classical model and to calculate the temperature dependence of charge mobility along with the degree of charge spatial localization. It is found that the roles of both local and nonlocal electron-phonon couplings strongly depend on the intrinsic charge localization strength.