Quantum Dots in Transition Metal Dichalcogenides Induced by Atomic-Scale Deformations

Single-photon emission from monolayer transition metal dichalcogenides requires the existence of localized, atom-like states within the extended material. Here, we predict from first-principles the existence of quantum dots around atomic-scale protrusions, which result from substrate roughness or particles trapped between layers. Using density functional theory, we find such deformations to give rise to local membrane stretching and curvature, which lead to the emergence of gap states. Having enhanced outer-surface localization, they are prone to mixing with states pertaining to chalcogen vacancies and adsorbates. If the deformation is sharp, the conduction band minimum furthermore assumes atomic and valley-mixed character, potentially enabling quantum light emission. When such structural defects are arranged in an array, the new states couple to form energetically separated sub-bands, holding promise for intriguing superlattice dynamics. All of the observed features are shown to be closely linked to elastic, deformation-induced intra- and intervalley scattering processes.