Multipole Superradiance from Densely Assembled Metallic Nanoparticles

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Abstract

The collective phenomenon of localized surface plasmons (LSPs) in a high-density collection of interacting metallic nanoparticles (NPs) is a crucial issue in various research fields such as optical physics, photochemistry, and biological science. Here, we report the dark-field measurement of the chemically controlled optical response of LSPs in densely assembled collection of a vast number of gold NPs on a microsphere (AuNP-covered bead). Remarkably, AuNP-covered beads exhibit plasmonic superradiance depending on sizes of binder molecules, where the giant spectral broadening more than 400 meV and significant enhancement of scattering have been observed. Furthermore, self-consistent theoretical analysis has also revealed that multipole collective modes contribute to the superradiance, leading to the enhancement by 2 orders of magnitude in both the far-field scattering and the localized fields of broadband light. The results obtained provide an innovative design principle for solar energy conversion and optical biosensors with incoherent light.

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