Exciton diffusion and halo effects in monolayer semiconductors

TL;DR

This study directly observes exciton diffusion in monolayer WS2, revealing nonlinear behavior, density-dependent diffusion coefficients, and halo formation due to Auger recombination and memory effects, advancing understanding of exciton dynamics.

Contribution

It provides the first direct measurement of exciton diffusion and halo formation in monolayer WS2, highlighting nonlinear effects and the role of Auger recombination.

Findings

Diffusion coefficient increases from 0.3 to over 30 cm²/s with exciton density.

Formation of long-lived halo shapes at high excitation densities.

Auger recombination explains the increase in diffusion and halo effects.

Abstract

We directly monitor exciton propagation in freestanding and SiO2-supported WS2 monolayers through spatially- and time-resolved micro-photoluminescence under ambient conditions. We find highly nonlinear behavior with characteristic, qualitative changes in the spatial profiles of the exciton emission and an effective diffusion coefficient increasing from 0.3 to more than 30 cm2/s, depending on the injected exciton density. Solving the diffusion equation while accounting for Auger recombination allows us to identify and quantitatively understand the main origin of the increase in the observed diffusion coefficient. At elevated excitation densities, the initial Gaussian distribution of the excitons evolves into long-lived halo shapes with micrometer-scale diameter, indicating additional memory effects in the exciton dynamics.