Designer Metasurfaces via Nanocube Assembly at the Air-Water Interface.

The advent of metasurfaces has revolutionized the design of optical instruments, and recent advancements in fabrication techniques are further accelerating their practical applications. However, conventional top-down fabrication of intricate nanostructures proves to be expensive and time-consuming, posing challenges for large-scale production. Here, we propose a cost-effective bottom-up approach to create nanostructure arrays with arbitrarily complex meta-atoms displaying single nanoparticle lateral resolution over submillimeter areas, minimizing the need for advanced and high-cost nanofabrication equipment. By utilizing air/water interface assembly, we transfer nanoparticles onto templated polydimethylsiloxane (PDMS) irrespective of nanopattern density, shape, or size. We demonstrate the robust assembly of nanocubes into meta-atoms with diverse configurations generally unachievable by conventional methods, including U, L, cross, S, T, gammadion, split-ring resonators, and Pancharatnam-Berry metasurfaces with designer optical functionalities. We also show nanocube epitaxy at near ambient temperature to transform the meta-atoms into complex continuous nanostructures that can be swiftly transferred from PDMS to various substrates via contact printing. Our approach potentially offers a large-scale manufacturing alternative to top-down fabrication for metal nanostructuring, unlocking possibilities in the realm of nanophotonics.