Atomic-Scale Dynamics Probed by Photon Correlations

Light absorption and emission have their origins in fast atomic-scale phenomena. To characterize these basic steps (e.g., in photosynthesis, luminescence, and quantum optics), it is necessary to access picosecond temporal and picometer spatial scales simultaneously. In this Perspective, we describe how state-of-the-art picosecond photon correlation spectroscopy combined with luminescence induced at the atomic scale with a scanning tunneling microscope (STM) enables such studies. We outline recent STM-induced luminescence work on single-photon emitters and the dynamics of excitons, charges, molecules, and atoms as well as several prospective experiments concerning light-matter interactions at the nanoscale. We also describe future strategies for measuring and rationalizing ultrafast phenomena at the nanoscale.