Nonequilibrium dynamics of localized and delocalized excitons in colloidal quantum dot solids

TL;DR

This paper investigates how microscopic disorder affects the nonequilibrium exciton dynamics in colloidal quantum dot solids, linking microscopic processes to macroscopic optoelectronic properties through a theoretical model.

Contribution

It introduces a theoretical framework for understanding exciton dynamics in disordered QD solids, highlighting the impact of disorder on relaxation processes and spectral signatures.

Findings

Disorder promotes nonequilibrium relaxation dynamics.

Signatures of nonequilibrium effects appear in time-dependent spectra.

Microscopic exciton behavior relates to macroscopic emission properties.

Abstract

Self-assembled quantum dot (QD) solids are a highly tunable class of materials with a wide range of applications in solid-state electronics and optoelectronic devices. In this perspective, we highlight how the presence of microscopic disorder in these materials can influence their macroscopic optoelectronic properties. Specifically, we consider the dynamics of excitons in energetically disordered QD solids using a theoretical model framework for both localized and delocalized excitonic regimes. In both cases, we emphasize the tendency of energetic disorder to promote nonequilibrium relaxation dynamics and discuss how the signatures of these nonequilibrium effects manifest in time-dependent spectral measurements. Moreover, we describe the connection between the microscopic dynamics of excitons within the material and the measurement of material specific parameters, such as emission linewidth broadening and energetic dissipation rate.