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The electronic excitation of molecules triggers diverse phenomena such asluminescence and photovoltaic effects, which are the bases of variousenergy-converting devices. Understanding and control of the excitations at thesingle-molecule level are long standing targets, however, they have beenhampered by the limited spatial resolution in optical probing techniques. Herewe investigate the electronic excitation of a single molecule withsub-molecular precision using a localised plasmon at the tip apex of a scanningtunnelling microscope (STM) as an excitation probe. Coherent energy transferbetween the plasmon and molecular excitons is discovered when the plasmon islocated in the proximity of isolated molecules, which is corroborated by atheoretical analysis. The polarised plasmonic field enables selectiveexcitation of an electronic transition between anisotropic frontier molecularorbitals. Our findings have established the foundation of a novelsingle-molecule spectroscopy with STM, providing an integrated platform forreal-space investigation of localised excited states.

Orbital-selective single molecule excitation and spectroscopy based on plasmon-exciton coupling