Spatially Selective Enhancement of Photoluminescence in MoS₂ by Exciton-Mediated Adsorption and Defect Passivation

Monolayers of transition-metal dichalcogenides (TMDs) are promising components for flexible optoelectronic devices because of their direct band gap and atomically thin nature. The photoluminescence (PL) from these materials is often strongly suppressed by nonradiative recombination mediated by midgap defect states. Here, we demonstrate up to a 200-fold increase in PL intensity from monolayer MoS₂ synthesized by chemical vapor deposition (CVD) by controlled exposure to laser light in the ambient. This spatially resolved passivation treatment is stable in air and vacuum. Regions unexposed to laser light remain dark in fluorescence despite continuous impingement of ambient gas molecules. A wavelength-dependent study confirms that PL brightening is concomitant with exciton generation in the MoS₂; laser light below the optical band gap fails to produce any enhancement in the PL. We highlight the photosensitive nature of the process by successfully brightening with a low-power broadband white light source. We decouple changes in absorption from defect passivation by examining the degree of circularly polarized PL. This measurement, which is independent of exciton generation, confirms that laser brightening reduces the rate of nonradiative recombination in the MoS₂. A series of gas exposure studies demonstrate a clear correlation between PL brightening and the presence of water. We propose that H₂O molecules passivate sulfur vacancies in the CVD-grown MoS₂ but require photogenerated excitons to overcome a large adsorption barrier. This work represents an important step in understanding the passivation of CVD-synthesized TMDs and demonstrates the interplay between adsorption and exciton generation.