Leveraging Plasmonic Nanocavity Arrays Forming Metasurfaces to Boost Second Harmonic Generation Due to Surface Effects

ABSTRACT Plasmonic metasurfaces have emerged as a promising platform for enhancing a range of nonlinear optical processes, offering compact geometry and flexibility in light manipulation. Second‐order nonlinear processes, like second harmonic generation (SHG), typically require non‐centrosymmetric crystals to be realized. Here, we experimentally demonstrate enhanced SHG response by using a gold nanocavity array forming a plasmonic metasurface absorber where titanium dioxide (TiO 2 ), a centrosymmetric dielectric material, with subwavelength thickness, is deposited in the realized nanogaps. While such a dielectric material has an extremely low second‐order nonlinear susceptibility, we observe 10 5 ‐fold boosting in the nonlinear SHG process mainly due to the surface nonlinear susceptibility of the gold metal, aided by the significant electric field enhancement that occurs in the nanogaps due to the formed nanocavity resonance. The experimental results obtained are theoretically explained with extensive and rigorous nonlinear simulations that consider all the bulk and surface linear and nonlinear material properties. The presented robust harmonic generation from an ultrathin plasmonic metasurface can be used in nonlinear and quantum integrated photonic applications.