1. Mapping Lamb, Stark, and Purcell Effects at a Chromophore-Picocavity Junction with Hyper-Resolved Fluorescence Microscopy
- Author
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Rosławska, Anna, Neuman, Tomáš, Doppagne, Benjamin, Borisov, Andrei G., Romeo, Michelangelo, Scheurer, Fabrice, Aizpurua, Javier, Schull, Guillaume, Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS), Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS)-Matériaux et Nanosciences Grand-Est (MNGE), Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Institut National de la Santé et de la Recherche Médicale (INSERM)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Réseau nanophotonique et optique, Université de Strasbourg (UNISTRA)-Université de Haute-Alsace (UHA) Mulhouse - Colmar (Université de Haute-Alsace (UHA))-Centre National de la Recherche Scientifique (CNRS)-Université de Strasbourg (UNISTRA)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences Moléculaires d'Orsay (ISMO), Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS), University of the Basque Country/Euskal Herriko Unibertsitatea (UPV/EHU), schull, guillaume, European Research Council, European Commission, Agence Nationale de la Recherche (France), Energy Frontier Research Centers (US), Ministerio de Ciencia, Innovación y Universidades (España), Agencia Estatal de Investigación (España), and Eusko Jaurlaritza
- Subjects
[PHYS]Physics [physics] ,Physics::Biological Physics ,Condensed Matter - Mesoscale and Nanoscale Physics ,Physics ,QC1-999 ,Mesoscale and Nanoscale Physics (cond-mat.mes-hall) ,Physics::Atomic and Molecular Clusters ,FOS: Physical sciences ,General Physics and Astronomy ,Physics::Chemical Physics ,[PHYS] Physics [physics] - Abstract
The interactions of the excited states of a single chromophore with static and dynamic electric fields spatially varying at the atomic scale are investigated in a joint experimental and theoretical effort. In this configuration, the spatial extension of the fields confined at the apex of a scanning tunneling microscope tip is smaller than that of the molecular exciton, a property used to generate fluorescence maps of the chromophore with intramolecular resolution. Theoretical simulations of the electrostatic and electrodynamic interactions occurring at the picocavity junction formed by the chromophore, the tip, and the substrate reveal the key role played by subtle variations of Purcell, Lamb, and Stark effects. They also demonstrate that hyper-resolved fluorescence maps of the line shift and linewidth of the excitonic emission can be understood as images of the static charge redistribution upon electronic excitation of the molecule and as the distribution of the dynamical charge oscillation associated with the molecular exciton, respectively., This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation program (Grant Agreement No. 771850) and the European Union’s Horizon 2020 research and innovation program under the Marie Skłodowska-Curie Grant Agreement No. 894434. The Labex NIE (Contract No. ANR-11-LABX-0058_NIE), the International Center for Frontier Research in Chemistry (FRC), the Spanish Ministry of Science (Project No. PID2019–107432 GB-I00), and the Department of Education of the Basque Government (Project No. IT116419) are acknowledged for financial support.
- Published
- 2022