Band-Edge Carrier Trapping Limits Light Emission in WSe$_2$

TL;DR

This study investigates how band-edge carrier traps in WSe$_2$ monolayers limit light emission, revealing a linear relationship between photoluminescence lifetime and intensity, and emphasizing trap control for improved optoelectronic performance.

Contribution

It provides a comprehensive analysis of over 200 monolayers, linking carrier traps to emission efficiency, and demonstrates the impact of photooxidation on nonradiative decay pathways.

Findings

Photoluminescence lifetime correlates linearly with emission intensity.

Photooxidation induces band-edge carrier traps that reduce emission.

Controlling traps is key to enhancing light emission in WSe$_2$.

Abstract

Monolayers of transition metal dichalcogenides (TMDs) exhibit bright photoluminescence, a desirable property for light-emitting diodes and single-photon emitters. Because the emission intensity is heavily influenced by factors such as defect density and oxidation, it is critical to understand how they affect photoluminescence efficiency. However, due to the time-consuming process of identifying individual monolayers, studies of high-quality exfoliated TMDs have been limited to only a few samples. Here, we present an investigation of excited-state lifetimes and spectra for over 200 WSe$_2$ exfoliated monolayers at room temperature. We find a linear correlation between photoluminescence lifetime and intensity across hundreds of monolayers and within individual monolayers. Results from intentional photooxidation experiments indicate that this correlation is due to photoinduced band-edge carrier traps, which introduce a nonradiative decay pathway that competes with exciton emission. Our work highlights the importance of controlling such traps, as they are the primary limitation of bright photoluminescence.