All-Optical Reversible Manipulation of Exciton and Trion Emissions in Monolayer WS₂

Monolayer transition metal dichalcogenides (TMDs) are direct gap semiconductors with promising applications in diverse optoelectronic devices. To improve devices' performance, recent investigations have been systematically focused on the tuning of their optical properties. However, an all-optical approach with the reversible feature is still a challenge. Here we demonstrate the tunability of the photoluminescence (PL) properties of monolayer WS₂ via laser irradiation. The broad-range and continuous modulation of PL intensity, as well as the conversion between neutral and charged excitons have been readily and reversibly achieved by only switching the two laser power densities. We attribute the reversible manipulation to the laser-assisted adsorption and desorption of gas molecules, which will deplete or release free electrons from the surface of WS₂ and thus modify its PL properties. This all-optical manipulation, with advantages of reversibility, quantitative control, and high spatial resolution, suggests promising applications of TMDs monolayers in optoelectronic and nanophotonic applications, such as erasable optical data storage, micropatterning, and display.