Signatures of strong coupling on nanoparticles: Revealing absorption anticrossing by tuning the dielectric environment

Abstract: Strongly coupled plasmon-exciton systems offer promising applications in nanooptics. The classification of the coupling regime is currently debated both from experimental and theoretical perspectives. We present a method to unambiguously identify strong coupling in plasmon-exciton core-shell nanoparticles by measuring true absorption spectra of the system. We investigate the coupling of excitons in J-aggregates to the localized surface plasmon polaritons on gold nanospheres and nanorods by fine-tuning the plasmon resonance via layer-by-layer deposition of polyelectrolytes. While both structures show a characteristic anticrossing in extinction and scattering experiments, the careful assessment of the systems' light absorption reveals that strong coupling of the plasmon to the exciton is only present in the nanorod system. In a phenomenological model of two classical coupled oscillators, intermediate coupling strengths split up only the resonance frequency of the light-driven oscillator, while the other one still dissipates energy at its original frequency. Only in the strong-coupling limit, both oscillators split up the frequencies at which they dissipate energy, qualitatively explaining our experimental finding.