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

TL;DR

This paper demonstrates a 105-fold enhancement in second harmonic generation using a plasmonic nanocavity array with a thin TiO2 layer, leveraging surface effects and nanocavity resonance.

Contribution

It introduces a novel plasmonic metasurface design that significantly boosts SHG through surface nonlinear susceptibility and electric field enhancement.

Findings

105-fold increase in SHG response observed.

Surface nonlinear susceptibility of gold contributes to enhancement.

Theoretical simulations confirm experimental results.

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 (TiO2), a centrosymmetric dielectric material, with subwavelength thickness is deposited in the realized nanogaps. While such dielectric material has an extremely low second order nonlinear susceptibility, we observe 105-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.