Global Equilibrium and Non-Equilibrium Theory of Hopping Exciton Transport in Disordered Semiconductors

TL;DR

This paper introduces a temperature-dependent theory for exciton hopping in disordered semiconductors, bridging equilibrium and non-equilibrium regimes, validated by simulations, and applicable to spectroscopy analysis.

Contribution

It presents a novel unified model for exciton transport that captures the transition from equilibrium to non-equilibrium states in disordered semiconductors.

Findings

The model agrees with kinetic Monte Carlo simulations across temperatures.

Diffusion length scaling differs from the third power of the F"orster radius in non-equilibrium.

The theory aids interpretation of spectroscopy in organic semiconductors and quantum dots.

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 non-equilibrium 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 non-equilibrium transport regime. We find that the diffusion length in the non-equilibrium 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.