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The molecular dark state participates in many important photon-inducedprocesses, yet is typically beyond the optical-spectroscopic measurement due tothe forbidden transition dictated by the selection rule. In this work, wepropose to use the scanning tunneling microscope (STM) as an incisive tool todirectly profile the dark-state transition density of a single molecule, takingadvantage of the localized static electronic field near the metal tip. Thedetection of dark state is achieved by measuring the fluorescence from a higherbright state to the ground state with assistant optical pumping. The currentproposal shall bring new methodology to study the single-molecule properties inthe electro-optical devices and the light-assisted biological processes.

Directly profiling the dark-state transition density via scanning tunneling microscope