Orbitally resolved single-photon emission from an individual atomic vacancy center in a semiconductor

Atomically confined spins are emerging as active components in quantum optoelectronic devices such as quantum bits and sensors. However, interrogating single spins at atomic length-scales remains a sizeable challenge, limited by diffraction in conventional optics. Here we show that the highly-local excitation provided by injecting energetic charge carriers from the atomically sharp probe of a scanning tunneling microscope can trigger single-photon emission from individual atomic vacancy centers in a layered semiconductor. With an effective spatial resolution of <1 nm, we show that the captured light closely mirrors the orbital symmetry of the bound-state wavefunction of the vacancy center while photon correlation measurements confirm single-photon emission, as reflected in clear photon anti-bunching signatures. Our results constitute an important step toward the realization of an electrically addressable single-atom quantum light source and solid-state spinphoton interface, addressed at the atomic-scale.