Jumping Kinetic Monte Carlo: Fast and Accurate Simulations of Partially Delocalized Charge Transport in Organic Semiconductors.

Abstract

Developing devices using disordered organic semiconductors requires accurate and practical models of charge transport. In these materials, charge transport occurs through partially delocalized states in an intermediate regime between localized hopping and delocalized band conduction. Partial delocalization can increase mobilities by orders of magnitude compared to those with conventional hopping, making it important for the design of materials and devices. Although delocalization, disorder, and polaron formation can be described using delocalized kinetic Monte Carlo (dKMC), it is a computationally expensive method. Here, we develop jumping kinetic Monte Carlo (jKMC), a model that approaches the accuracy of dKMC for modest amounts of delocalization (such as those found in disordered organic semiconductors), with a computational cost comparable to that of conventional hopping. jKMC achieves its computational performance by modeling conduction using identical spherical polarons, yielding a simple delocalization correction to the Marcus hopping rate that allows polarons to jump over their nearest neighbors. jKMC can be used in regimes of partial delocalization inaccessible to dKMC to show that modest delocalization can increase mobilities by as much as 2 orders of magnitude.