Fluorescence from a single-molecule probe directly attached to a plasmonic STM tip

Niklas Friedrich (), Anna Rosławska, Xabier Arrieta, Katharina Kaiser, Michelangelo Romeo, Eric Moal, Fabrice Scheurer, Javier Aizpurua, Andrei G. Borisov, Tomáš Neuman () and Guillaume Schull ()
Additional contact information
Niklas Friedrich: CIC nanoGUNE-BRTA
Anna Rosławska: Université de Strasbourg, CNRS, IPCMS
Xabier Arrieta: CSIC-UPV/EHU
Katharina Kaiser: Université de Strasbourg, CNRS, IPCMS
Michelangelo Romeo: Université de Strasbourg, CNRS, IPCMS
Eric Moal: Institut des Sciences Moléculaires d’Orsay
Fabrice Scheurer: Université de Strasbourg, CNRS, IPCMS
Javier Aizpurua: Donostia International Physics Center
Andrei G. Borisov: Institut des Sciences Moléculaires d’Orsay
Tomáš Neuman: Institut des Sciences Moléculaires d’Orsay
Guillaume Schull: Université de Strasbourg, CNRS, IPCMS

Nature Communications, 2024, vol. 15, issue 1, 1-8

Abstract: Abstract The scanning tunneling microscope (STM) provides access to atomic-scale properties of a conductive sample. While single-molecule tip functionalization has become a standard procedure, fluorescent molecular probes remained absent from the available tool set. Here, the plasmonic tip of an STM is functionalized with a single fluorescent molecule and is scanned on a plasmonic substrate. The tunneling current flowing through the tip-molecule-substrate junction generates a narrow-line emission of light corresponding to the fluorescence of the negatively charged molecule suspended at the apex of the tip, i.e., the emission of the excited molecular anion. The fluorescence of this molecular probe is recorded for tip-substrate nanocavities featuring different plasmonic resonances, for different tip-substrate distances and applied bias voltages, and on different substrates. We demonstrate that the width of the emission peak can be used as a probe of the exciton-plasmon coupling strength and that the energy of the emitted photons is governed by the molecule interactions with its environment. Additionally, we theoretically elucidate why the direct contact of the suspended molecule with the metallic tip does not totally quench the radiative emission of the molecule.

Date: 2024
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DOI: 10.1038/s41467-024-53707-2

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