Hybrid materials formed by plasmonic nanostructures and J-aggregates provide a unique combination of highly localized and enhanced electromagnetic field in metal constituent with large oscillator strength and extremely narrow exciton band of the organic component. The coherent coupling of localized plasmons of the multispiked gold nanoparticles (nanostars) and excitons of JC1 dye J-aggregates results in a Rabi splitting reaching 260 meV. Importantly, broad absorption features of nanostars extending over a visible and near-infrared spectral range allowed us to demonstrate double Rabi splitting resulting from the simultaneous coherent coupling between plasmons of the nanostars and excitons of J-aggregates of two different cyanine dyes.
Hybrid materials formed by plasmonic nanostructures and J-aggregates provide a unique combination of localized and enhanced electro-magnetic field in metal constituent with large oscillator strength and extremely narrow exciton band of the organic component. The coherent coupling of the plasmons of the multi-spiked gold nanostars and the excitons of JC1 dye J-aggregates results in a Rabi splitting reaching 260 meV. Importantly, broad absorption features of nanostars extending over a visible and near-infrared spectral range allowed us to demonstrate double Rabi splitting resulting from the simultaneous coherent coupling between plasmons of the nanostars and excitons of J-aggregates of two different dyes. INTRODUCTIONJ-aggregates of the organic dyes are of significant interest for the development of an advanced photonic technologies thanks to their ability to delocalize and migrate the excitonic energy over a large number of the aggregated dye molecules [1]. The hybridization of the electronic states in strongly coupled hybrid nanosystems consisting of plasmonic nanostructures and J-aggregates results in an intriguing quantum electrodynamics phenomena such as Rabi splitting, which manifests itself in the appearance of double-peaked feature in their transmission or absorption spectra [2]. In the strong coupling regime, the value of Rabi splitting depends on the oscillator strength of the exciton as well as on the increase in the local density of the electromagnetic modes and field enhancement both provided by the noble metal nanostructures. To date, Rabi splitting arising from coherent coupling between electronic polarizations of the plasmonic systems and the molecular excitons in J-aggregates of cyanine dyes has been demonstrated for a variety of metal constituents, such as Au, Ag, and Au/Ag colloidal nanoparticles [3, 4], core-shell Au and Ag nanoparticles [5,6], Ag films [7], spherical nanovoids in Au films [8], Au nanoshells [9], Au nanorods, [10,11] and arrays of Ag nanodisks [12]. Among different plasmonic nanostructures, multispiked gold nanoparticles with a star-like shape [13][14][15][16] are particularly interesting for the development of the photonic devices and sensors based on the strong coupling phenomenon. These nanoparticles consist of a near-spherical core with typically 5 to 8 arms [17], whose sharp tips give rise to the strong spatial confinement of the electromagnetic field at their ends, with the enhancement factors similar to those in the metallic nanoshell dimers [18,19]. The coexistence of different plasmon resonances resulting from the hybridization of the core and the individual tips results in the increased number of the localized plasmonic modes [18,20] (as compared to the spherical nanoparticles or nanorods) available for the coherent interaction with quantum emitters. Moreover, the hybridization of plasmons localized at the core and the tips of the stars results in the increased effective dipole moment of the tip plasmons and the enlarged cross-section for plasmon excitation [18]. In th...
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