atomically thin 2D layered materials, such as monolayer transition metal dichalcogenides (TMDs), [5][6][7][8] hexagonal boron nitride (hBN). [9,10] and gallium selenide, [11] are attractive alternative hosts to overcome such fundamental limitations of bulk counterparts.Following the initial reports on single photon emitters observed in naturally occurring defects in as-grown and as-exfoliated 2D TMDs, [5][6][7][8] various strain and crystal defect engineering approaches have been developed to deterministically generate these quantum emitters. While local strain introduced by nano-pillars/ holes or nano-indents commonly results in single photon emitters in a variety of 2D materials including hBN, WS 2 , WSe 2 , and MoSe 2 , [12][13][14][15][16][17] creation of point defects by ion [10,18] and electron [9,19] beam irradiation has proved to be a viable route to inducing similar quantum emitters. Further, direct writing of quantum emitter arrays on monolayer MoS 2 with precisely controlled positions has been demonstrated using a focused helium ion beam. [20][21][22] Chalcogen vacancies (V X , X = S/Se), which are commonly present in TMDs, are known to introduce in-gap states. [23][24][25][26] Studies on helium-ion treated MoS 2 (Refs. [18,(20)(21)(22)27,28]) found that transitions involving such in-gap states can be optically bright and yield anti-bunched photons at sufficiently low-density defects. However, emission peaks commonly attributed to chalcogen vacancies in other TMDs are often broad (FWHM > 100 meV), lacking typical features of quantum emitters. [26,29,30] Defect engineering of atomically thin semiconducting crystals is an attractive route to developing single-photon sources and valleytronic devices. For these applications, defects with well-defined optical characteristics need to be generated in a precisely controlled manner. However, defect-induced optical features are often complicated by the presence of multiple defect species, hindering the identification of their structural origin. Here, we report systematic generation of optically active atomic defects in monolayer MoS 2 , WS 2 , MoSe 2 , and WSe 2 via proton-beam irradiation. Defect-induced emissions are found to occur ≈100 to 200 meV below the neutral exciton peak, showing typical characteristics of localized excitons such as saturation at high-excitation rates and long lifetime. Using scanning transmission electron microscopy, it is shown that freshly created chalcogen vacancies are responsible for the localized exciton emission. Density functional theory and ab initio GW plus Bethe-Salpeter-equation calculations reveal that the observed emission can be attributed to transitions involving defect levels of chalcogen vacancy and the valence band edge state.