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We demonstrate an ultrafast manipulation of the Rabi splitting energy Ω(R) in a metal-molecular aggregate hybrid nanostructure. Femtosecond excitation drastically alters the optical properties of a model system formed by coating a gold nanoslit array with a thin J-aggregated dye layer. Controlled and reversible transient switching from strong (Ω(R) ≃ 55 meV) to weak (Ω(R) ≈ 0) coupling on a sub-ps time scale is directly evidenced by mapping the nonequilibrium dispersion relations of the coupled excitations. Such a strong, externally controllable coupling of excitons and surface plasmon polaritons is of considerable interest for ultrafast all-optical switching applications in nanoscale plasmonic circuits.

We report on the interplay between strong coupling and radiative damping of strongly coupled excitons (Xs) and surface plasmon polaritons (SPPs) in a hybrid system made of J-aggregates and metal nanostructures. The optical response of the system is probed at the field level by angle-resolved spectral interferometry. We show that two different energy transfer channels coexist: coherent resonant dipole-dipole interaction and an incoherent exchange due to the spontaneous emissions of a photon by one emitter and its subsequent reabsorption by another. The interplay between both pathways results in a pronounced modification of the radiative damping due to the formation of super- and subradiant polariton states. This is confirmed by probing the ultrafast nonlinear response of the polariton system and explained within a coupled oscillator model. Such a strong modification of the radiative damping opens up interesting directions in coherent active plasmonics.

We report on the observation of optical Stark effects in J-aggregate-metal hybrid nanostructures exhibiting strong exciton-surface-plasmon-polariton coupling. For redshifted nonresonant excitation, pump-probe spectra show short-lived dispersive line shapes of the exciton-surface-plasmon-polariton coupled modes caused by a pump-induced Stark shift of the polariton resonances. For larger coupling strengths, the sign of the Stark shift is reversed by a transient reduction in normal mode splitting. Our studies demonstrate an approach to coherently control and largely enhance optical Stark effects in strongly coupled hybrid systems. This may be useful for applications in ultrafast all-optical switching.

The anisotropic plasmons properties of black phosphorus allow for realizing direction-dependent plasmonics devices. Here, we theoretically investigated the hybridization between graphene surface plasmons (GSP) and anisotropic black phosphorus localized surface plasmons (BPLSP) in the strong coupling regime. By dynamically adjusting the Fermi level of graphene, we show that the strong coherent GSP-BPLSP coupling can be achieved in both armchair and zigzag directions, which is attributed to the anisotropic black phosphorus with different in-plane effective electron masses along the two crystal axes. The strong coupling is quantitatively described by calculating the dispersion of the hybrid modes using a coupled oscillator model. Mode splitting energy of 26.5 meV and 19 meV are determined for the GSP-BPLSP hybridization along armchair and zigzag direction, respectively. We also find that the coupling strength can be strongly affected by the distance between graphene sheet and black phosphorus nanoribbons. Our work may provide the building blocks to construct future highly compact anisotropic plasmonics devices based on two-dimensional materials at infrared and terahertz frequencies.