Centimeter-Scale Superlattices of Three-Dimensionally Orientated Plasmonic Dimers with Highly Tunable Collective Properties

The precise organization and orientation of plasmonic molecules on substrates is crucial to their application in functional devices but still remains a grand challenge. This article describes a bottom-up strategy to efficiently fabricate centimeter-scale superlattices of three-dimensionally oriented plasmonic dimers with highly tunable collective optical properties on substrates. The in-plane (i.e., X–Y plane) and out-of-plane (i.e., along Z-axis) orientation of the constituent plasmonic dimers can be precisely controlled by a combination of directional capillary force and supporting polymer film. Our experimental measurements and numerical simulations show that the macroscopic dimer superlattices exhibit polarization-dependent plasmon Fano resonances in air and multimodal surface lattice resonances with high quality factors in a homogeneous medium, owing to the high positional and orientational ordering of the subunits. Our strategy enables the fabrication of complex plasmonic nanostructures with precise configurations for advanced plasmonic devices such as plasmon nanolasing and metamaterials.