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Transition metal dichalcogenides (TMDs) represent an entire new class ofsemiconducting 2D materials with exciting properties. Defects in 2D TMDs cancrucially affect their physical and chemical properties. However,characterization of the presence and spatial distribution of defects is limitedeither in throughput or in resolution. Here, we demonstrate large area mappingof reactive sulfur-deficient defects in 2D-TMDs coupling single-moleculelocalization microscopy with fluorescence labeling using thiol chemistry. Ourmethod, reminiscent of PAINT strategies, relies on the specific binding byreversible physisorption of fluorescent probes to sulfur-vacancies via a thiolgroup and their intermittent emission to apply localization of the labeleddefects with a precision down to 15 nm. Tuning the distance between thefluorophore and the docking thiol site allows us to control F\"oster ResonanceEnergy Transfer (FRET) process and reveal large structural defects such asgrain boundaries and line defects, due to the local irregular latticestructure. Our methodology provides a simple and fast alternative forlarge-scale mapping of non-radiative defects in 2D materials and paves the wayfor in-situ and spatially resolved monitoring of the interaction betweenchemical agent and the defects in 2D materials that has general implicationsfor defect engineering in aqueous condition.

Super-resolved optical mapping of reactive sulfur-vacancy in 2D transition metal dichalcogenides