Nonlinear Metasurfaces: A Paradigm Shift in Nonlinear Optics

Abstract: Frequency conversion processes, such as second- and third-harmonic generation, are one of the most common effects in nonlinear optics which offer many opportunities for photonics, chemistry, material science, characterization, and biosensing. Given the inherently weak nonlinear response of natural materials, one typically relies on optically large samples and complex phase-matching techniques to achieve nonlinear effects. A direct translation of these approaches to small dimensions, however, is extremely challenging, because nonlinear effects locally comparable to the linear response cannot be induced without reaching extremely high light intensities leading to the material breakdown. For this reason, the quest to synthesize novel materials with enhanced optical nonlinearities at moderate input intensities is very active nowadays. In the last decade, several approaches to engineering the nonlinear properties of artificial materials, metamaterials, and metasurfaces have been introduced. Here, we review the current state of the art in the field of small-scale nonlinear optics, with special emphasis on high-harmonic generation from ultrathin metasurfaces, including those based on plasmonic and high-index dielectric resonators, as well as semiconductor-loaded plasmonic metasurfaces. We discuss the role of specific electromagnetic field configurations for efficient harmonic generation, including magnetic dipole, Fano resonance, and anapole ones. We also discuss the most recent advances in controlling the phase front profiles of generated nonlinear waves enabled by nonlinear metasurfaces consisting of nanoresonators with judiciously tailored shapes. Finally, we compare viable approaches to enhance nonlinearities without phase matching constraints in ultrathin metasurfaces, and offer a perspective and outlook on the future development of this exciting field.