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      Light Interaction with Photonic and Plasmonic Resonances

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          Single-molecule strong coupling at room temperature in plasmonic nanocavities

          Emitters placed in an optical cavity experience an environment that changes their coupling to light. In the weak-coupling regime light extraction is enhanced, but more profound effects emerge in the single-molecule strong-coupling regime where mixed light-matter states form1,2. Individual two-level emitters in such cavities become non-linear for single photons, forming key building blocks for quantum information systems as well as ultra-low power switches and lasers3–6. Such cavity quantum electrodynamics has until now been the preserve of low temperatures and complex fabrication, severely compromising their use5,7,8. Here, by scaling the cavity volume below 40 nm3 and using host-guest chemistry to align 1-10 protectively-isolated methylene-blue molecules, we reach the strong-coupling regime at room temperature and in ambient conditions. Dispersion curves from >50 plasmonic nanocavities display characteristic anticrossings, with Rabi frequencies of 300 meV for 10 molecules decreasing to 90 meV for single molecules, matching quantitative models. Statistical analysis of vibrational spectroscopy time-series and dark-field scattering spectra provide evidence of single-molecule strong coupling. This dressing of molecules with light can modify photochemistry, opening up the exploration of complex natural processes such as photosynthesis9 and pathways towards manipulation of chemical bonds10.
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            Nonlinear plasmonics

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              Enhancement and Quenching of Single-Molecule Fluorescence

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                Author and article information

                Journal
                Laser & Photonics Reviews
                Laser & Photonics Reviews
                Wiley
                18638880
                May 2018
                May 2018
                April 17 2018
                : 12
                : 5
                : 1700113
                Affiliations
                [1 ]LP2N; Institut d'Optique Graduate School; CNRS; Univ. Bordeaux; 33400 Talence France
                [2 ]Laboratoire Charles Fabry; Institut d'Optique Graduate School; CNRS; Université Paris-Saclay; 91127 Palaiseau Cedex France
                Article
                10.1002/lpor.201700113
                fd98aadf-1424-4c32-a342-f0031db807d7
                © 2018

                http://doi.wiley.com/10.1002/tdm_license_1.1

                http://onlinelibrary.wiley.com/termsAndConditions#vor

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