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The scanning-tunneling-microscope-induced luminescence emerges recently as anincisive tool to measure the molecular properties down to the single-moleculelevel. The rapid experimental progress is far ahead of the theoretical effortto understand the observed phenomena. Such incompetence leads to a significantdifficulty in quantitatively assigning the observed feature of the fluorescencespectrum to the structure and dynamics of a single molecule. This letter isdevoted to reveal the microscopic origin of the molecular excitation viainelastic scattering of the tunneling electrons in scanning tunnelingmicroscope. The current theory explains the observed large photon countingasymmetry between the molecular luminescence intensity at positive and negativebias voltage.

Microscopic origin of molecule excitation via inelastic electron scattering in scanning tunneling microscope