Ultrafast Control of the Dimensionality of Exciton-Exciton Annihilation in Atomically Thin Black Phosphorus

Abstract

Using microtransient absorption spectroscopy, we show that the dynamical form of exciton-exciton annihilation in atomically thin black phosphorous can be made to switch between time varying 1D scattering and time-independent 2D scattering. At low carrier densities, anisotropy drives the 1D behavior, but as the photoexcitation density approaches the exciton saturation limit, the 2D nature of exciton-exciton scattering takes over. Furthermore, lowering the temperature provides a handle on the ultrafast timescale at which the 1D to 2D transition occurs. We understand our results quantitatively using a diffusion based model of exciton-exciton scattering.