Rabi Splitting in Photoluminescence Spectra of Hybrid Systems of Gold Nanorods and J-Aggregates

We experimentally and theoretically investigate the interactions between localized plasmons in gold nanorods and excitons in J-aggregates under ambient conditions. Thanks to our sample preparation procedure we are able to track a clear anticrossing behavior of the hybridized modes not only in the extinction but also in the photoluminescence (PL) spectra of this hybrid system. Notably, while previous studies often found the PL signal to be dominated by a single mode (emission from so-called lower polariton branch), here we follow the evolution of the two PL peaks as the plasmon energy is detuned from the excitonic resonance. Both the extinction and PL results are in good agreement with the theoretical predictions obtained for a model that assumes two interacting modes with a ratio between the coupling strength and the plasmonic losses close to 0.4, indicative of the strong coupling regime with a significant Rabi splitting estimated to be ∼200 meV. The evolution of the PL line shape as the plasmon is detuned depends on the illumination wavelength, which we attribute to an incoherent excitation given by decay processes in either the metallic rods or the J-aggregates.