Mapping Lamb, Stark and Purcell effects at a chromophore-picocavity junction with hyper-resolved fluorescence microscopy

Anna Roslawska; Tomáš Neuman; Benjamin Doppagne; Andrei G. Borisov; Michelangelo Romeo; Fabrice Scheurer; Javier Aizpurua; Guillaume Schull

arXiv · 2107.01072

Mapping Lamb, Stark and Purcell effects at a chromophore-picocavity junction with hyper-resolved fluorescence microscopy

Anna Roslawska·Tomáš Neuman·Benjamin Doppagne·Andrei G. Borisov·Michelangelo Romeo·Fabrice Scheurer·Javier Aizpurua·Guillaume Schull

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Abstract

The interactions between the excited states of a single chromophore with static and dynamic electric fields confined to a plasmonic cavity of picometer dimensions are investigated in a joint experimental and theoretical effort. In this configuration, the spatial extensions of the confined fields are smaller than the one of the molecular exciton, a property that is used to generate fluorescence maps of the chromophores with intra-molecular resolution. Theoretical simulations of the electrostatic and electrodynamic interactions occurring at the chromophore-picocavity junction are able to reproduce and interpret these hyper-resolved fluorescence maps, and reveal the key role played by subtle variations of Purcell, Lamb and Stark effects at the chromophore-picocavity junction.

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Anna Roslawska, Tomáš Neuman, Benjamin Doppagne, Andrei G. Borisov, Michelangelo Romeo, Fabrice Scheurer, Javier Aizpurua, Guillaume Schull. 2021-07-02. Mapping Lamb, Stark and Purcell effects at a chromophore-picocavity junction with hyper-resolved fluorescence microscopy. https://arxiv.org/abs/2107.01072

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