Gating single-molecule fluorescence with electrons

Fuente: arXiv
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Main Authors: Kaiser, Katharina, Romeo, Michelangelo, Scheurer, Fabrice, Schull, Guillaume, Rosławska, Anna
Format: Preprint
Published: 2024
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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