We present a theoretical approach to the study of second- and third-harmonic generation from metallic structures and nanocavities filled with a nonlinear material in the ultrashort pulse regime. We model the metal as a two-component medium, using the hydrodynamic model to describe free electrons and Lorentz oscillators to account for core electron contributions to both the linear dielectric constant and harmonic generation. The active nonlinear medium that may fill a metallic nanocavity, or be positioned between metallic layers in a stack, is also modeled using Lorentz oscillators and surface phenomena due to symmetry breaking are taken into account. We study the effects of incident TE- and TM-polarized fields and show that a simple reexamination of the basic equations reveals additional, exploitable dynamical features of nonlinear frequency conversion in plasmonic nanostructures.

We experimentally demonstrate efficient third harmonic generation from an indium tin oxide nanofilm (λ/42 thick) on a glass substrate for a pump wavelength of 1.4 μm. A conversion efficiency of 3.3 × 10⁻⁶ is achieved by exploiting the field enhancement properties of the epsilon-near-zero mode with an enhancement factor of 200. This nanoscale frequency conversion method is applicable to other plasmonic materials and reststrahlen materials in proximity of the longitudinal optical phonon frequencies.

We show an alternative path to efficient second- and third-harmonic generation in proximity of the zero crossing points of the dielectric permittivity in conjunction with low absorption. Under these circumstances, any material, either natural or artificial, will show similar degrees of field enhancement followed by strong harmonic generation, without resorting to any resonant mechanism. The results presented in this paper provide a general demonstration of the potential that the zero-crossing-point condition holds for nonlinear optical phenomena. We investigate a generic Lorentz medium and demonstrate that a singularity-driven enhancement of the electric field may be achieved even in extremely thin layers of material. We also discuss the role of nonlinear surface sources in a realistic scenario where a 20-nm layer of CaF2 is excited at 21 $\mu${}m, where $\epsilon${} $\sim${} 0. Finally, we show similar behavior in an artificial composite material that includes absorbing dyes in the visible range, provide a general tool for the improvement of harmonic generation using the $\epsilon${} $\sim${} 0 condition, and illustrate that this singularity-driven enhancement of the field lowers the thresholds for a plethora of nonlinear optical phenomena.

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.

We investigate local-field enhancement phenomena in subwavelength, $\epsilon${}-near-zero (ENZ) slabs that do not exploit Fabry-P\'erot resonances. In particular, we study the linear response of engineered metamaterial slabs of finite thickness based on plasmonic nanoshells that show an ENZ band in the visible range, and naturally occurring materials (e.g., SiO${}_{2}$) that also display ENZ properties, under oblique, TM-polarized plane-wave incidence. We then introduce active gain material in engineered metamaterial slabs that adds peculiar spectral and angular features to transmission, reflection, and absorption properties, and leads to a further local-field enhancement. These findings are supported by two theoretical studies: First, a simple interface between two semi-infinite media, namely free space and a generic ENZ medium; then, an ENZ slab of finite thickness, with the aim of understanding the system's behavior when varying the ENZ properties as well as the incident angle. For either case we report three distinct physical conditions for which we explain spectral and angular features that might result in strong field enhancement. The gain-assisted metamaterial implementation has the potential of triggering and enhancing low-threshold nonlinear phenomena thanks to the large local fields found at specific frequency and angular bands.

Nonlinear light sources are central to a myriad of applications, driving a quest for their miniaturisation down to the nanoscale. In this quest, nonlinear metasurfaces hold a great promise, as they enhance nonlinear effects through their resonant photonic environment and high refractive index, such as in high-index dielectric metasurfaces. However, despite the sub-diffractive operation of dielectric metasurfaces at the fundamental wave, this condition is not fulfilled for the nonlinearly generated harmonic waves, thereby all nonlinear metasurfaces to date emit multiple diffractive beams. Here, we demonstrate the enhanced single-beam second- and third-harmonic generation in a metasurface of crystalline transition-metal-dichalcogenide material, offering the highest refractive index. We show that the interplay between the resonances of the metasurface allows for tuning of the unidirectional second-harmonic radiation in forward or backward direction, not possible in any bulk nonlinear crystal. Our results open new opportunities for metasurface-based nonlinear light-sources, including nonlinear mirrors and entangled-photon generation.