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

AuthorsNeuman, Tomáš; Esteban, Ruben; Casanova, David; García-Vidal, F. J.; Aizpurua, Javier
Issue Date2018
CitationCEN 2018
AbstractIn state-of-the-art plasmonic cavities the localization of electromagnetic fields reaches down to a couple of nm3, which is a scale comparable to the size of molecular emitters placed inside them. In such a situation, the approximation of the molecule as a structureless point-like dipole breaks down. Here we address the coupling of localized cavity plasmons with a molecular exciton beyond the point-dipole approximation. To that end we adopt a quantum chemical description of the molecular electronic transitions that we combine with a quantum-optical model that describes the quantized plasmonic fields. We calculate the spatially dependent coupling strength between the plasmon and the molecular exciton, revealing that the spatial extent of the electronic transition density of the molecular exciton plays a key role in determining the dynamics of the molecular excited state interacting with the plasmonic cavity in both the weak (Purcell effect) and the strong-coupling (Rabi oscillations) regimes. The spatial dependence of the plasmon-exciton coupling strength predicted by the model nicely reproduces experimental results in literature. Furthermore we show that the extreme field localization in plasmonic cavities can lead to breaking of optical selection rules, making the otherwise dark excitonic transitions in molecules accessible to light. Our findings are thus of importance in nanoscale optical spectroscopy or for optical manipulation of chemical properties of single molecules.
DescriptionResumen del trabajo presentado a la Spanish Conference on Nanophotonics (Conferencia Española de Nanofotónica-CEN), celebrada en Donostia-San Sebastián (España) del 3 al 5 de octubre de 2018.
Appears in Collections:(CFM) Comunicaciones congresos
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