Localized Intervalley Defect Excitons as Single-Photon Emitters in WSe2

Single-photon emitters play a key role in present and emerging quantum technologies. Several recent measurements have established monolayer WSe2 as a promising candidate for a reliable single-photon source. The origin and underlying microscopic processes have remained, however, largely elusive. We present a multiscale tight-binding simulation for the optical spectra of WSe2 under nonuniform strain and in the presence of point defects employing the Bethe-Salpeter equation. Strain locally shifts excitonic energy levels into the band gap where they overlap with localized intragap defect states. The resulting hybridization allows for efficient filling and subsequent radiative decay of the defect states. We identify intervalley defect excitonic states as the likely candidate for antibunched single-photon emission. This proposed scenario is shown to account for a large variety of experimental observations including brightness, radiative transition rates, the variation of the excitonic energy with applied magnetic and electric fields as well as the variation of the polarization of the emitted photon with the magnetic field.