Gating single-molecule fluorescence with electrons
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arXiv
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| Main Authors: | , , , , |
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| Format: | Preprint |
| Published: |
2024
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| _version_ | 1866910368605929472 |
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| author | Kaiser, Katharina Romeo, Michelangelo Scheurer, Fabrice Schull, Guillaume Rosławska, Anna |
| author_facet | Kaiser, Katharina Romeo, Michelangelo Scheurer, Fabrice Schull, Guillaume Rosławska, Anna |
| contents | Tip-enhanced photoluminescence (TEPL) measurements are performed with sub-nanometer 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 both the bias voltage and the atomic-scale lateral position of the tip can be used to gate the molecular emission. Our approach can in principle be applied to any molecular system, providing unprecedented control over the fluorescence of a single molecule. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2403_10410 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Gating single-molecule fluorescence with electrons Kaiser, Katharina Romeo, Michelangelo Scheurer, Fabrice Schull, Guillaume Rosławska, Anna Mesoscale and Nanoscale Physics Tip-enhanced photoluminescence (TEPL) measurements are performed with sub-nanometer 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 both the bias voltage and the atomic-scale lateral position of the tip can be used to gate the molecular emission. Our approach can in principle be applied to any molecular system, providing unprecedented control over the fluorescence of a single molecule. |
| title | Gating single-molecule fluorescence with electrons |
| topic | Mesoscale and Nanoscale Physics |
| url | https://arxiv.org/abs/2403.10410 |