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.