Circular dichroism spectra of naturally occurring molecules and also of synthetic chiral arrangements of plasmonic particles often exhibit characteristic bisignate shapes. Such spectra consist of peaks next to dips (or vice versa) and result from the superposition of signals originating from many individual chiral objects oriented randomly in solution. Here we show that by first aligning and then toggling the orientation of DNA-origami-scaffolded nanoparticle helices attached to a substrate, we are able to reversibly switch the optical response between two distinct circular dichroism spectra corresponding to either perpendicular or parallel helix orientation with respect to the light beam. The observed directional circular dichroism of our switchable plasmonic material is in good agreement with predictions based on dipole approximation theory. Such dynamic metamaterials introduce functionality into soft matter-based optical devices and may enable novel data storage schemes or signal modulators.

Surface plasmon enhanced second harmonic generation in gold grating slabs was investigated. The efficiency is analyzed with respect to the phase matching at the fundamental and the second harmonic frequencies. A classical electromagnetic model was developed under the weak nonlinearity approximation and solved by the finite element method. The measured zeroth order transmitted second harmonic intensity was found to be in quantitative agreement with numerical results. It is shown experimentally and numerically that proper phase matching at both frequencies improves the second harmonic efficiency.

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