Plasmonic hole arrays with extreme optical chirality in linear and nonlinear regimes

Metamaterials with high optical activity (OA) and circular dichroism (CD) are desired for various prospective applications ranging from circular light polarizing to enhanced chiral sensing and biosensing. Modern techniques allow fabricating subwavelength arrays of holes of complex chiral shapes that exhibit extreme optical chirality: their OA and CD take the whole range of possible values in the visible. In order to understand the nature of extreme chirality, we performed the electromagnetic finite difference time domain simulations for the hole shapes resolved by atomic force microscopy. The analysis of the simulation data allowed us to develop an analytical chiral coupled-mode model that nicely fits the results and explains the extreme chirality as determined by the Fano-type transmission resonance due to the interference of a weak background channel and a resonant plasmon channel. The model shows critical importance of the dissipation losses, the hole shape symmetry and chirality. In a planar 2D-chiral hole array, the mirror asymmetry can be induced by the difference of dielectric materials adjacent to the array sides and even their weak deviation results in remarkably strong OA and CD. We note that such deviations can arise due to the dielectric nonlinearity and discuss how 2D-chiral metamaterials in symmetric environment can acquire optical chirality due to the nonlinear symmetry breaking.