Journal
PHYSICAL REVIEW X
Volume 12, Issue 1, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevX.12.011012
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Funding
- European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program [771850]
- European Union's Horizon 2020 research and innovation program under the Marie Sklodowska-Curie Grant [894434]
- Labex NIE [ANR-11-LABX-0058_NIE]
- International Center for Frontier Research in Chemistry (FRC)
- Spanish Ministry of Science [PID2019-107432 GB-I00]
- Department of Education of the Basque Government [IT1164-19]
- Marie Curie Actions (MSCA) [894434] Funding Source: Marie Curie Actions (MSCA)
- European Research Council (ERC) [771850] Funding Source: European Research Council (ERC)
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Experimental and theoretical investigation of the interactions between excited states of a single chromophore and static and dynamic electric fields varying at the atomic scale. The fluorescence maps of the chromophore with intramolecular resolution reveal the static charge redistribution and dynamic charge oscillation associated with the molecular exciton.
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.
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