In this study, we demonstrate a synergistic enhancement of photoluminescence (PL) in an atomically thin molybdenum disulfide (MoS2) monolayer using a dual-laser-beam-assisted chemical modification method. A continuous-wave (CW) green laser, directed perpendicularly at the MoS2, locally raises the temperature and induces the formation of sulfur (S) vacancies, resulting in a significant increase in PL intensity. Subsequently, a UV nanosecond laser beam laterally illuminates the area above the MoS2 layer, breaking chlorine molecules and introducing chlorine radicals without damaging the sample. This process further enhances the PL in the region previously affected by S vacancies. The binding energy of chlorine atoms to S-vacancy sites is greater than that to the pristine MoS2 surface, facilitating more effective p-type doping. The stronger interaction at the defect sites created by the CW laser contributes to the observed synergistic PL enhancement. Our approach presents a novel method for precise and spatially selective chemical doping in two-dimensional (2D) van der Waals (vdW) materials.
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