Metallic and dielectric nanoparticles (NPs) have synergistic electromagnetic properties but their positioning into morphologically defined hybrid arrays with novel optical properties still poses significant challenges. A template-guided self-assembly strategy is introduced for the positioning of metallic and dielectric NPs at pre-defined lattice sites. The chemical assembly approach facilitates the fabrication of clusters of metallic NPs with interparticle separations of only a few nanometers in a landscape of dielectric NPs positioned hundreds of nanometers apart. This approach is used to generate two-dimensional interdigitated arrays of 250 nm diameter TiO2 NPs and clusters of electromagnetically strongly coupled 60 nm Au NPs. The morphology-dependent near- and far-field responses of the resulting multiscale optoplasmonic arrays are analyzed in detail. Elastic and inelastic scattering spectroscopy in combination with electromagnetic simulations reveal that optoplasmonic arrays sustain delocalized photonic–plasmonic modes that achieve a cascaded E-field enhancement in the gap junctions of the Au NP clusters and simultaneously increase the E-field intensity throughout the entire array.
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