Origin of extrinsic chirality in metasurfaces and nanoholes fabricated by nanosphere lithography

Nanosphere lithography is a cost- and time-efficient tool for the fabrication of various nanostructured materials. Multiple steps of metal layer deposition at different oblique angles were shown to produce complex asymmetric and chiral shapes. Here, we investigate samples in which polystyrene nanospheres are covered by Ag or combination of Ag and Au at a single step (under 45 deg). In this way, we obtain metasurfaces with asymmetric shells, with a nanohole array formed due to the shadowing effect. We investigate chiro-optical properties of four samples by exciting them in the 700-1000 nm range, at angles of incidence from -45deg to +45deg; we report on dissymmetry in the total extinction between left and right circularly polarized excitation gext, which follows the rules of extrinsic chirality. We then resolve the transmission of Ag metasurface in terms of hyperspectral Stokes parameters, and we connect the S3 parameter with gext. Finally, we characterize nanohole arrays obtained from the same samples when the nanospheres are removed; we further perform electromagnetic simulations to gain insight into the "egg" shaped nanohole.