Fano description of single-hydrocarbon fluorescence excited by a scanning tunneling microscope

Abstract

The detection of fluorescence with submolecular resolution enables the exploration of spatially varying photon yields and vibronic properties at the single-molecule level. By placing individual polycyclic aromatic hydrocarbon molecules into the plasmon cavity formed by the tip of a scanning tunneling microscope and a NaCl-covered Ag(111) surface, molecular light emission spectra are obtained that unravel vibrational progression. In addition, light spectra unveil a signature of the molecule even when the tunneling current is injected well separated from the molecular emitter. This signature exhibits a distance-dependent Fano profile that reflects the subtle interplay between inelastic tunneling electrons, the molecular exciton and localized plasmons in at-distance as well as on-molecule fluorescence. The presented findings open the path to luminescence of a different class of molecules than investigated before and contribute to the understanding of single-molecule luminescence at surfaces in a unified picture.

24 pages, 4 figures

References in corpus (4)

• Orbital-selective single molecule excitation and spectroscopy based on plasmon-exciton coupling
• Electrically-driven vibronic spectroscopy with sub-molecular resolution
• Narrow-line single-molecule transducer between electronic circuits and surface plasmons
• Bright electroluminescence from single graphene nanoribbon junctions

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• Microscopic origin of molecule excitation via inelastic electron scattering in scanning tunneling microscope
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• Selectively addressing plasmonic modes and excitonic states in a nanocavity hosting a quantum emitter