Resonance Coupling in Silicon Nanosphere-J-Aggregate Heterostructures

Due to their optical magnetic and electric resonances associated with the high refractive index, dielectric silicon nanoparticles have been explored as novel nanocavities that are excellent candidates for enhancing various light matter interactions at the nanoscale. Here, from both of theoretical and experimental aspects, we explored resonance coupling between excitons and magnetic/electric resonances in heterostructures composed of the silicon nanoparticle coated with a molecular J-aggregate shell. The resonance coupling was originated from coherent energy transfer between the exciton and magnetic/electric modes, which was manifested by quenching dips on the scattering spectrum due to formation of hybrid modes. The influences of various parameters, including the molecular oscillation strength, molecular absorption line width, molecular shell thickness, refractive index of the surrounding environment, and separation between the core and shell, on the resonance coupling behaviors were scrutinized. In particular, the resonance coupling can approach the strong coupling regime by choosing appropriate molecular parameters, where an anticrossing behavior with a mode splitting of 100 meV was observed on the energy diagram. Most interestingly, the hybrid modes in such dielectric heterostructure can exhibit unidirectional light scattering behaviors, which cannot be achieved by those in plexcitonic nanoparticle composed of a metal nanoparticle core and a molecular shell.