Light emission probing quantum shot noise and charge fluctuations at a biased molecular junction

The emission of plasmonic light from a single C(60) molecule on Cu(111) is probed in a scanning tunneling microscope from the weak-coupling, tunneling range to strong coupling of the molecule to the electrodes at contact. At positive sample voltage the photon yield decreases owing to shot-noise suppression in an increasingly transparent quantum contact. At reversed bias an unexpected nonlinear increase occurs. First-principles transport calculations reveal that ultrafast charge fluctuations on the molecule give rise to additional noise at optical frequencies beyond the shot noise of the current that is injected to the tip.