Exciton Diffusion and Halo Effects in Monolayer Semiconductors

We directly monitor exciton propagation in freestanding and SiO2-supported WS2 monolayers through spatially and time-resolved microphotoluminescence under ambient conditions. We find a 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 cm(2)/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 mu m-scale diameter, indicating additional memory effects in the exciton dynamics.