Chiro-optical signals from chiral molecules/structures are inherently weak. In particular, enhancing the circular-dichroism (CD) effect (different absorption of left or right circularly polarized light) in the non-linear optical (NLO) signal from chiral molecular materials is challenging and imperative since it is advantageous in various areas, from biomedical sciences to miniaturized photonic devices. Here we suggest and realize for the first time an approach to enhance the CD effect taking advantage of the NLO effects resonantly enhanced in the nonlinear chiral organic micro-resonators. These R- and S-type resonators in the form of micro-spheres are prepared by the self-assembly technique from the corresponding axially chiral enantiomeric molecules, namely R- and S-4-[2,2′-diethoxy-6′-(4-formylphenyl)-[1,1′-binaphthalen]-6-yl]benzaldehyde in CHCl₃/MeOH mixtures. Each enantiomeric micro-sphere, upon optical pumping, acts as a whispering gallery mode (WGM) resonator as the photo-luminescence (PL) is excited in a single- or in a two-photon regime. We show that the NLO-CD effect and the two-photon absorption (TPA) in the case of micro-spheres are at least twice as high as compared to a continuous film of the same effective thickness. This is due to pronounced field localization effects in micro-spheres with high Q-factor, which increases the photon residence time (τ_P) in a chiral medium and thus strengthens the light–matter interaction. Finite-difference time-domain (FDTD) numerical calculations confirm a strong light localization near the boundary of the micro-spheres.

Circular dichroism in optical second harmonic generation (CD-SHG) is studied in planar symmetrical arrays of G-shaped and mirror-G-shaped nanostructures. Anisotropic CD-SHG measurements demonstrate a strong dependence of the value and the sign of the CD effect on the angle of incidence of the fundamental radiation. We show that both dipole and higher order multipole components of the second order susceptibility are responsible for the CD response from G-shaped nanostructures.

Chiral planar metamaterials are known for their possibility to show strong nonlinear optical effects such as second harmonic generation (SHG) circular dichroism or asymmetric SHG. The underlying mechanisms are commonly discussed in terms of local field effects and formation of localized SHG sources (so called “hotspots”) that are sensitive to the shape and size of meta-atoms. Nevertheless, a full characterization of the polarization state of the nonlinear optical radiation from the hotspots has not been performed until now. Here we present the results of the polarization-resolved second harmonic generation microscopy studies of planar chiral G-shaped metamaterials. We demonstrate that the SHG radiation coming from the hotspots that are localized within a single meta-atom is partially polarized; moreover, the SHG polarization state reveals the chirality of the structure. The observed effects are attributed to the induced plasmonic current oscillations at the fundamental frequency along with the local field distribution.