Scalable and controlled self-assembly of aluminum-based random plasmonic metasurfaces

Subwavelength metal-dielectric plasmonic metasurfaces enable light management beyond the diffraction limit. However, a costeffective and reliable fabrication method for such structures remains a major challenge hindering their full exploitation. Here, we propose a simple yet powerful manufacturing route for plasmonic metasurfaces based on a bottom-up approach. The fabricated metasurfaces consist of a dense distribution of randomly oriented nanoscale scatterers composed of aluminum (Al) nanohole-disk pairs, which exhibit angle-independent scattering that is tunable across the entire visible spectrum. The macroscopic response of the metasurfaces is controlled via the properties of an isolated Al nanohole-disk pair at the nanoscale. In addition, the optical field confinement at the scatterers and their random distribution of sizes result in a strongly enhanced Raman signal that enables broadly tunable excitation using a single substrate. This unique combination of a reliable and lithography-free methodology with the use of aluminum permits the exploitation of the full potential of random plasmonic metasurfaces for diagnostics and coloration.