Gating Single-Molecule Fluorescence with Electrons

Tip-enhanced photoluminescence (TEPL) measurements are performed with subnanometer spatial resolution on individual molecules decoupled from a metallic substrate by a thin NaCl layer. TEPL spectra reveal progressive fluorescence quenching with decreasing tip-molecule distance when electrons tunneling from the tip of a scanning tunneling microscope are injected at resonance with the molecular states. Rate equations based on a many-body model reveal that the luminescence quenching is due to a progressive population inversion between the ground neutral (S_{0}) and the ground charge (D_{0}^{-}) states of the molecule occurring when the current is raised. We demonstrate that the bias voltage and the lateral tip position can be used to gate the molecular emission. Our approach can be applied to any molecular system, providing unprecedented control over the fluorescence of a single molecule.

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Publication Details

Journal
Physical Review Letters
Published
2024-10-08
DOI
https://doi.org/10.1103/physrevlett.133.156902
Citations
7
Primary Topic
Molecular Junctions and Nanostructures
Type
article
Field-Weighted Citation Impact
1.46

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article

Gating Single-Molecule Fluorescence with Electrons

Katharina Kaiser, Song Jiang, Michelangelo Romeo, Fabrice Scheurer et al.
7 citations
Physical Review Letters
Molecular Junctions and Nanostructures
1.46
article

Gating Single-Molecule Fluorescence with Electrons

Katharina Kaiser, Song Jiang, Michelangelo Romeo, Fabrice Scheurer, Anna Rosławska, Guillaume Schull
article en
7 citations

Abstract

Tip-enhanced photoluminescence (TEPL) measurements are performed with subnanometer spatial resolution on individual molecules decoupled from a metallic substrate by a thin NaCl layer. TEPL spectra reveal progressive fluorescence quenching with decreasing tip-molecule distance when electrons tunneling from the tip of a scanning tunneling microscope are injected at resonance with the molecular states. Rate equations based on a many-body model reveal that the luminescence quenching is due to a progressive population inversion between the ground neutral (S_{0}) and the ground charge (D_{0}^{-}) states of the molecule occurring when the current is raised. We demonstrate that the bias voltage and the lateral tip position can be used to gate the molecular emission. Our approach can be applied to any molecular system, providing unprecedented control over the fluorescence of a single molecule.

Physical Review LettersVol. 133(15)
Max Planck Institute for Solid State Research (DE), Université de Strasbourg (FR), University of Göttingen (DE)
European Commission, Deutsche Forschungsgemeinschaft, Agence Nationale de la Recherche, Institut National de la Santé et de la Recherche Médicale, Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung, Université de Strasbourg, Centre National de la Recherche Scientifique, Horizon 2020 Framework Programme, H2020 European Research Council
Openalex Percentile: Top 17%
Molecular Junctions and Nanostructures
1.46
DOIOpen Access PDFOpenAlex
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Gating Single-Molecule Fluorescence with Electrons — Katharina Kaiser, Song Jiang, et al. · Physical Review Letters (2024) | TGRS Research Map | TGRS