Ultrafast Spatial Hole Burning Dynamics in Monolayer WS2: Insights from Time-resolved Photoluminescence Spectroscopy

TL;DR

This study reveals ultrafast nonlinear excitonic transport dynamics in monolayer WS2, driven by exciton-exciton interactions, defect trapping, and photo-oxidation, with implications for excitonic device control.

Contribution

It provides the first detailed experimental and theoretical analysis of ultrafast excitonic diffusion and nonlinear effects in monolayer WS2 under intense optical excitation.

Findings

Ultrafast spatial hole burning observed in excitonic emission.

Exciton-exciton annihilation and defect trapping govern transport dynamics.

Diffusion model accurately reproduces experimental observations.

Abstract

The transport of excitons lies at the heart of excitonic devices. Probing, understanding, and manipulating excitonic transport represents a critical step prior to their technological applications. In this work, we report experimental studies on the ultrafast nonlinear transport of excitons in monolayer WS2. Under intense optical pumping, we observed an ultrafast spatial hole burning effect in the excitonic emission profile, followed by a re-brightening at even higher pumping density. By means of time- and spatially-resolved photoluminescence imaging spectroscopy, we revealed the underlying mechanism responsible for these nontrivial excitonic diffusion dynamics. Our results demonstrate that the combined effects of ultrafast exciton-exciton annihilation, efficient hole trapping by intrinsic sulfur vacancy defects, and laser-induced photo-oxidation govern the evolution of exciton transport under strong optical excitation. The observed dynamics are in excellent agreement with our diffusion model simulations, providing new insights into the nonlinear excitonic transport behaviors as well as their optical control mechanism in two-dimensional semiconductors.