Resonant Chiral Effects in Nonlinear Dielectric Metasurfaces

We study the resonant enhancement of linear and nonlinear chiroptical effects in planar silicon metasurfaces with an in-plane asymmetry supporting multipolar Mie resonances and quasi-bound states in the continuum (quasi-BICs). We demonstrate theoretically and observe in experiment the pronounced linear circular dichroism at the quasi-BIC resonances originating from the interaction of modes with the substrate. We further find that both local field enhancement and third-harmonic signal are large for Mie resonances and some quasi-BIC modes due to the critical coupling. We demonstrate experimentally a strong nonlinear chiroptical response associated with high efficiency of the third-harmonic generation and large nonlinear circular dichroism varying from +0.918 ± 0.049 to −0.771 ± 0.004 for the samples with different asymmetries. We reveal the nonreciprocal nature of nonlinear chirality governed by the microscopic symmetry of nonlinearities and macroscopic symmetries of the meta-atom and metasurface lattice. We believe our results suggest a general strategy for engineering nonlinear chiroptical response in dielectric resonant metasurfaces

Observation of Enhanced Generation of a Fifth Harmonic from Halide Perovskite Nonlocal Metasurfaces

Lead halide perovskites are widely employed in photonic and light-emitting devices because of their rich optoelectronic properties and simplicity of fabrication based on low-cost flexible technologies. Perovskite bulk crystals and films demonstrate outstanding nonlinear characteristics with large optical nonlinearities exceeding the nonlinear susceptibilities of conventional semiconductor materials by several orders of magnitude. One of the promising approaches for further enhancement of the nonlinear response of perovskites as dielectric photonic materials is to employ optical resonances of structured surfaces, or metasurfaces. Nonlocal metasurfaces supporting lattice modes over many unit cells provide a new approach to both spatial and spectral control of light fields, and they may deliver improved characteristics of nonlinear effects for a wide range of applications associated with broadband excitation of multiple high-quality resonances. Here we report on the first observation of enhanced fifth harmonic generation in MAPbBr3 halide perovskite nonlocal metasurfaces driven by high-quality resonances at the generated harmonic wavelength in the visible frequency range. The demonstrated enhancement is about 2 orders of magnitude compared to an unpatterned MAPbBr3 film of the same thickness, and is broadband by virtue of the excitation of multiple resonant modes in the highly nonlocal regime. Our work suggests a novel approach for achieving parametric processes in resonant dielectric structures with high efficiency