Plexcitonic Optical Chirality: Strong Exciton-Plasmon Coupling in Chiral J-Aggregate-Metal Nanoparticle Complexes.

Abstract

Understanding the unique characteristics of plexcitons, hybridized states resulting from the strong coupling between plasmons and excitons, is vital for both fundamental studies and practical applications in nano-optics. However, the research of plexcitons from the perspective of chiral optics has been rarely reported. Here, we experimentally investigate the optical chirality of plexcitonic systems consisting of composite metal nanoparticles and chiral J-aggregates in the strong coupling regime. Mode splitting and anticrossing behavior are observed in both the circular dichroism (CD) and extinction spectra of the hybrid nanosystems. A large mode splitting (at zero detuning) of up to 136 meV/214 meV in CD/extinction measurements confirms that the systems attain the strong coupling regime. This phenomenon indicates that the formation of plexcitons modifies not only the extinction but also the optical chirality of the hybrid systems. We develop a quasistatic theory to elucidate the chiral optical responses of hybrid systems. Furthermore, we propose and justify a criterion of strong plasmon-exciton interaction: the mode splitting in the CD spectra (at zero detuning) is larger than half of that in the extinction spectra. Our findings give a chiral perspective on the study of strong plasmon-exciton coupling and have potential applications in the chiral optical field.