Multipolar second harmonic generation from planar arrays of Au nanoparticles

We demonstrate optical Second Harmonic Generation (SHG) in planar arrays of cylindrical Au nanoparticles arranged in periodic and deterministic aperiodic geometries. In order to understand the respective roles of near-field plasmonic coupling and long-range photonic interactions on the SHG signal, we systematically vary the interparticle separation from 60 nm to distances comparable to the incident pump wavelength. Using polarization-resolved measurements under femtosecond pumping, we demonstrate multipolar SHG signal largely tunable by the array geometry. Moreover, we show that the SHG signal intensity is maximized by arranging Au nanoparticles in aperiodic spiral arrays. The possibility to engineer multipolar SHG in planar arrays of metallic nanoparticles paves the way to the development of novel optical elements for nanophotonics, such as nonlinear optical sensors, compact frequency converters, optical mixers, and broadband harmonic generators on a chip.