Strong chiroptical effects recently reported result from the interaction of light with chiral plasmonic nanostructures. Such nanostructures can be used to enhance the chiroptical response of chiral molecules and could also significantly increase the enantiomeric excess of direct asymmetric synthesis and catalysis. Moreover, in optical metamaterials, chirality leads to negative refractive index and all the promising applications thereof. In this Progress Report, we highlight four different strategies which have been used to achieve giant chiroptical effects in chiral nanostructures. These strategies consecutively highlight the importance of chirality in the nanostructures (for linear and nonlinear chiroptical effects), in the experimental setup and in the light itself. Because, in the future, manipulating chirality will play an important role, we present two examples of chiral switches. Whereas in the first one, switching the chirality of incoming light causes a reversal of the handedness in the nanostructures, in the second one, switching the handedness of the nanostructures causes a reversal in the chirality of outgoing light.

Throughout the 19th and 20th century, chirality has mostly been associated with chemistry. However, while chirality can be very useful for understanding molecules, molecules are not well suited for understanding chirality. Indeed, the size of atoms, the length of molecular bonds and the orientations of orbitals cannot be varied at will. It is therefore difficult to study the emergence and evolution of chirality in molecules, as a function of geometrical parameters. By contrast, chiral metal nanostructures offer an unprecedented flexibility of design. Modern nanofabrication allows chiral metal nanoparticles to tune the geometric and optical chirality parameters, which are key for properties such as negative refractive index and superchiral light. Chiral meta/nano‐materials are promising for numerous technological applications, such as chiral molecular sensing, separation and synthesis, super‐resolution imaging, nanorobotics, and ultra‐thin broadband optical components for chiral light. This review covers some of the fundamentals and highlights recent trends. We begin by discussing linear chiroptical effects. We then survey the design of modern chiral materials. Next, the emergence and use of chirality parameters are summarized. In the following part, we cover the properties of nonlinear chiroptical materials. Finally, in the conclusion section, we point out current limitations and future directions of development.

We discuss the linear dispersive properties of finite one-dimensional photonic band-gap structures. We introduce the concept of a complex effective index for structures of finite length, derived from a generalized dispersion equation that identically satisfies the Kramers-Kronig relations. We then address the conditions necessary for optimal, phase-matched, resonant second harmonic generation. The combination of enhanced density of modes, field localization, and exact phase matching near the band edge conspire to yield conversion efficiencies orders of magnitude higher than quasi-phase-matched structures of similar lengths. We also discuss an unusual and interesting effect: counterpropagating waves can simultaneously travel with different phase velocities, pointing to the existence of two dispersion relations for structures of finite length.

We numerically demonstrate negative refraction of the Poynting vector and sub-wavelength focusing in the visible part of the spectrum using a transparent multilayer, metallo-dielectric photonic band gap structure. Our results reveal that in the wavelength regime of interest evanescent waves are not transmitted by the structure, and that the main underlying physical mechanisms for sub-wavelength focusing are resonance tunneling, field localization, and propagation effects. These structures offer several advantages: tunability and high transmittance (50% or better) across the visible and near IR ranges; large object-image distances, with image planes located beyond the range where the evanescent waves have decayed. From a practical point of view, our findings point to a simpler way to fabricate a material that exhibits negative refraction and maintains high transparency across a broad wavelength range. Transparent metallo-dielectric stacks also provide an opportunity to expand the exploration of wave propagation phenomena in metals, both in the linear and nonlinear regimes.

Here we report the experimental observation of circular dichroism in the second-harmonic field (800-400 nm conversion) generated by self-organized gold nanowire arrays with subwavelength periodicity (160 nm). Such circular dichroism, raised by a nonlinear optical extrinsic chirality, is the evident signature of the sample morphology. It arises from the curvature of the self-assembled wires, producing a lack of symmetry at oblique incidence. The results were compared, both in the optical linear and nonlinear regime, with a reference sample composed of straight wires. Despite the weak extrinsic optical chirality of our samples (not observable by our optical linear measurements), high visibility (more than 50%) was obtained in the second-harmonic generated field.

The present investigation is concerned with the study of pulsed second-harmonic generation under conditions of phase and group velocity mismatch, and generally low conversion efficiencies and pump intensities. In positive-index, nonmetallic materials, we generally find qualitative agreement with previous reports regarding the presence of a double-peaked second harmonic signal, which comprises a pulse that walks off and propagates at the nominal group velocity one expects at the second-harmonic frequency, and a second pulse that is "captured" and propagates under the pump pulse. We find that the origin of the double-peaked structure resides in a phase-locking mechanism that characterizes not only second-harmonic generation, but also chi((3)) processes and third-harmonic generation. The phase-locking mechanism that we describe occurs for arbitrarily small pump intensities, and so it is not a soliton effect, which usually relies on a threshold mechanism, although multicolor solitons display similar phase locking characteristics. Thus, in second harmonic generation a phase-matched component is always generated, even under conditions of material phase mismatch: This component is anomalous, because the material does not allow energy exchange between the pump and the second-harmonic beam. On the other hand, if the material is phase matched, phase locking and phase matching are indistinguishable, and the conversion process becomes efficient. We also report a similar phase-locking phenomenon in negative index materials. A spectral analysis of the pump and the generated signals reveals that the phase-locking phenomenon causes the forward moving, phase-locked second-harmonic pulse to experience the same negative index as the pump pulse, even though the index of refraction at the second-harmonic frequency is positive. Our analysis further shows that the reflected second-harmonic pulse generated at the interface and the forward-moving, phase-locked pulse appear to be part of the same pulse initially generated at the surface, part of which is immediately back-reflected, while the rest becomes trapped and dragged along by the pump pulse. These pulses thus constitute twin pulses generated at the interface, having the same negative wave vector, but propagating in opposite directions. Almost any break of the longitudinal symmetry, even an exceedingly small chi((2)) discontinuity, releases the trapped pulse which then propagates in the backward direction. These dynamics are indicative of very rich and intricate interactions that characterize ultrashort pulse propagation phenomena

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We demonstrate significant enhancement of second-order nonlinear interactions in a one-dimensional semiconductor Bragg mirror operating as a photonic band gap structure. The enhancement comes from a simultaneous availability of a high density of states, thanks to high field localization, and the improvement of effective coherent length near the photonic band edge.