Plasmonic nanostructures for shrinking structured light to access forbidden transitions

Plasmonic nanostructures have considerable applicability in light–matter interactions owing to their capacity for strong field confinement and enhancement. Nanogap structures allow us to tailor electric field distributions at the nanoscale, bridging the differences in size and shape of atomic and light structures. In this study, we demonstrated that a plasmonic tetramer structure can squeeze structured light into a nanoscale area, in which a strong field gradient allows access to forbidden transitions. Numerical simulations showed that the gold tetramer structure on a glass substrate possesses a plasmonic eigenmode, which forms structured light with a quadrupole profile in the nanogap region at the center of the tetramer. The top–down technique employed using electron-beam lithography allows us to produce a gap size of approximately 50 nm, which supports plasmonic resonance in the near-infrared regime. In addition, we demonstrated an array architecture in which a collective lattice resonance enhances the intensity of the quadrupole field in multiple lattice units. This study highlights the possibility of accessing multipolar transitions in a combined system of structured light and plasmonic nanostructures. Our findings may lead to new platforms for spectroscopy, sensing, and light sources that take advantage of the full electronic spectrum of an emitter.