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Photon statistics is a powerful tool for characterizing the emission dynamicsof nanoscopic systems and their photophysics. Recent advances that combinecorrelation spectroscopy with scanning tunneling microscopy-inducedluminescence (STML) have allowed measuring the emission dynamics fromindividual molecules and defects demonstrating their nature as single photonemitters. The application of correlation spectroscopy to the analysis of thedynamics of a well-characterized adsorbate system in ultrahigh vacuum remainedto be shown. Here we combine single photon time correlations with STML tomeasure the dynamics of individual $H_2$ molecules between a gold tip and aAu(111) surface. An adsorbed $H_2$ molecule performs recurrent excursions belowthe tip apex. We use the fact that the presence of the $H_2$ molecule in thejunction modifies plasmon emission to study the adsorbate dynamics. Using the$H_2$ molecule as a chopper for STM-induced optical emission intensity wedemonstrate bunching in the plasmonic photon train in a single measurement oversix orders of magnitude in the time domain (from microseconds to seconds) thattakes only a few seconds. Our findings illustrate the power of using photonstatistics to measure the diffusion dynamics of adsorbates with STML.

A single hydrogen molecule as an intensity chopper in an electrically-driven plasmonic nanocavity