Theoretical study of equilibrium and nonequilibrium exciton dynamics in disordered semiconductors

Abstract

We develop a temperature-dependent theory for singlet exciton hopping transport in disordered semiconductors. It draws on the transport level concept within a F\"orster transfer model and bridges the gap in describing the transition from equilibrium to nonequilibrium time-dependent spectral diffusion. We test the validity range of the developed model using kinetic Monte Carlo simulations and find agreement over a broad range of temperatures. It reproduces the scaling of the diffusion length and spectral shift with the dimensionless disorder parameter and describes in a unified manner the transition from equilibrium to nonequilibrium transport regime. We find that the diffusion length in the nonequilibrium regime does not scale with the the third power of the F\"orster radius. The developed theory provides a powerful tool for interpreting time-resolved and steady state spectroscopy experiments in a variety of disordered materials, including organic semiconductors and colloidal quantum dots.