A comparative analysis of surface and bulk contributions to second-harmonic generation in centrosymmetric nanoparticles.

Second-harmonic generation (SHG) from nanoparticles made of centrosymmetric materials provides an effective tool to characterize many important properties of photonic structures at the subwavelength scale. Here we study the relative contribution of surface and bulk effects to SHG for plasmonic and dielectric nanostructures made of centrosymmetric materials in both dispersive and non-dispersive regimes. Our calculations of the far-fields generated by the nonlinear surface and bulk currents reveal that the size of the nanoparticle strongly influences the amount and relative contributions of the surface and bulk SHG effects. Importantly, our study reveals that, whereas for plasmonic nanoparticles the surface contribution is always dominant, the bulk and surface SHG effects can become comparable for dielectric nanoparticles, and thus they both should be taken into account when analyzing nonlinear optical properties of all-dielectric nanostructures.