Cooperative bi-exponential decay of dye emission coupled via plasmons

Bi-exponential decay of dye fluorescence near the surface of plasmonic metamaterials and core-shell nanoparticles is shown to be an intrinsic property of the coupled system. Indeed, the Dicke, cooperative states involve two groups of transitions: super-radiant, from the most excited to the ground st...

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Bibliographic Details
Published in:Scientific reports 2018-06, Vol.8 (1), p.9508-12, Article 9508
Main Authors: Lyvers, David P, Moazzezi, Mojtaba, de Silva, Vashista C, Brown, Dean P, Urbas, Augustine M, Rostovtsev, Yuri V, Drachev, Vladimir P
Format: Article
Language:English
Subjects:
Dyes
Nanoparticles
Silicon dioxide
Silver
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Summary:Bi-exponential decay of dye fluorescence near the surface of plasmonic metamaterials and core-shell nanoparticles is shown to be an intrinsic property of the coupled system. Indeed, the Dicke, cooperative states involve two groups of transitions: super-radiant, from the most excited to the ground states and sub-radiant, which cannot reach the ground state. The relaxation in the sub-radiant system occurs mainly due to the interaction with the plasmon modes. Our theory shows that the relaxation leads to the population of the sub-radiant states by dephasing the super-radiant Dicke states giving rise to the bi-exponential decay in agreement with the experiments. We use a set of metamaterial samples consisting of gratings of paired silver nanostrips coated with Rh800 dye molecules, having resonances in the same spectral range. The bi-exponential decay is demonstrated for Au\SiO \ATTO655 core-shell nanoparticles as well, which persists even when averaging over a broad range of the coupling parameter.
ISSN:2045-2322
2045-2322
DOI:10.1038/s41598-018-27901-4