We present a new electromagnetic phenomenon-the asymmetric second-harmonic generation from planar chiral structures. The effect consists in distinguishing the handedness of a chiral material by rotating the sample in an experiment involving solely linearly polarized light. This phenomenon originates in the surface plasmon resonance of chiral gold nanostructures, where homodyne interference of anisotropic and chiral electric and/or magnetic multipoles appears to play an important role.

In high definition mapping of the plasmonic patterns on the surfaces of nanostructures, the diffraction limit of light remains an important obstacle. Here we demonstrate that this diffraction limit can be completely circumvented. We show that upon illuminating nanostructures made of nickel and palladium, the resulting surface-plasmon pattern is imprinted on the structures themselves; the hotspots (regions of local field enhancement) are decorated with overgrowths, allowing for their subsequent imaging with scanning-probe techniques. The resulting resolution of plasmon pattern imaging is correspondingly improved.

Abstract:In optics, chirality is typically associated with circularly polarized light. Here we present a novel way to detect the handedness of chiral materials with linearly polarized light. We performed Second Harmonic Generation (SHG) microscopy on G-shaped planar chiral nanostructures made of gold. The SHG response originates in distinctive hotspots, whose arrangement is dependent of the handedness. These results uncover new directions for studying chirality in artificial materials.

Novel ways to detect the handedness in chiral optical metamaterials by means of the second harmonic generation (SHG) process have recently been proposed. However, the precise origin of the SHG emission has yet to be unambiguously established. In this paper, we present computational simulations of both the electric currents and the electromagnetic fields in chiral planar metamaterials, at the fundamental frequency (FF), and discuss the implications of our results on the characteristics of experimentally measured SHG. In particular, we show that the results of our numerical simulations are in good agreement with the experimental mapping of SHG sources. Thus, the SHG in these metamaterials can be attributed to a strong local enhancement of the electromagnetic fields at the FF, which depends on the particular structure of the patterned metamaterial.

Chirality effects in optical second harmonic generation (SHG) are studied in periodic planar arrays of gold G-shaped nanostructures. We show that G-shaped structures of different handedness demonstrate different SHG efficiency for the left and right circular polarizations, as well as the opposite directions of the SHG polarization plane rotation. The observed effects are interpreted as the appearance of chirality in the SHG response which allows clear distinguishing of two enantiomers.

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Recently, a great amount of research has been triggered by the prediction, formulated by Pendry and co-authors, that novel and enhanced nonlinear optical phenomena could be observed in metamaterials.[l] This prediction is based on the fact that, in metamaterials, local field enhancements can have a dramatic influence over the optical properties of the material.