Demonstration of extrinsic chirality in self-assembled asymmetric plasmonic metasurfaces and nanohole arrays.

Chirality, the lack of mirror symmetry, can be mimicked in nanophotonics and plasmonics by breaking the symmetry in light-nanostructure interaction. Here we report on versatile use of nanosphere lithography for the fabrication of low-cost metasurfaces, which exhibit broadband handedness- and angle-dependent extinction in the near-infrared range, thus offering extrinsic chiro-optical behavior. We measure wavelength and angle dependence of the extinction for four samples. Two samples are made of polystyrene nanospheres asymmetrically covered by silver and gold in one case and silver only in the other case, with a nanohole array at the bottom. The other two samples are nanohole arrays, obtained after the nanosphere removal from the first two samples. Rich extrinsic chiral features are governed by different chiro-optical mechanisms in the three-dimensional plasmonic semi-shells and planar nanohole arrays. We also measure Stokes parameters in the same wavelength and incidence angle range and show that the transmitted fields follow the extrinsic chirality features of the extinction dissymmetry. We further study the influences of the nanostructured shapes and in-plane orientations on the intrinsic vs extrinsic chirality. The nanoholes are modelled as oval shapes in metal, showing good agreement with the experiments. We thus confirm that nanosphere lithography can provide different geometries for chiral light manipulation at the nanoscale, with the possibility to extend functionalities with optimized oval shapes and combination of constituent metals.