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Coupling of molecular emitters and plasmonic cavities beyond the point-dipole approximation

AuthorsNeuman, Tomáš; Esteban, Ruben; Casanova, David; García-Vidal, F. J.; Aizpurua, Javier CSIC ORCID
KeywordsSingle-molecule spectroscopy
Point-dipole approximation
Quantum nano-optics
Plasmon−exciton coupling
Quantum chemistry
Issue Date2018
PublisherAmerican Chemical Society
CitationNano Letters 18(4): 2358-2364 (2018)
AbstractAs the size of a molecular emitter becomes comparable to the dimensions of a nearby optical resonator, the standard approach that considers the emitter to be a point-like dipole breaks down. By adoption of a quantum description of the electronic transitions of organic molecular emitters, coupled to a plasmonic electromagnetic field, we are able to accurately calculate the position-dependent coupling strength between a plasmon and an emitter. The spatial distribution of excitonic and photonic quantum states is found to be a key aspect in determining the dynamics of molecular emission in ultrasmall cavities both in the weak and strong coupling regimes. Moreover, we show that the extreme localization of plasmonic fields leads to the selection rule breaking of molecular excitations.
Identifiersdoi: 10.1021/acs.nanolett.7b05297
e-issn: 1530-6992
issn: 1530-6984
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