A Novel Hierarchical Nanostructure for Enhanced Optical Nonlinearity Based on Scattering Mechanism.

Surface modification of nonlinear optical materials (NOMs) is widely applied to fabricate diverse photonic devices, such as frequency combs, modulators, and all-optical switches. In this work, a double-layer nanostructure with heterogeneous nanoparticles (NPs) is proposed to achieve enhanced third-order optical nonlinearity of NOMs. The mechanism of modified optical nonlinearity is elucidated to be the scattering-induced energy transfer between adjacent NPs layers. Based on the LiNbO3 platform, as a typical example, double layers of embedded Cu and Ag NPs are synthesized by sequential ion implantation, demonstrating twofold magnitude of near-infrared enhancement factor and modulation depth in comparison with a single layer of Cu NPs. With the elastic collision model and thermolysis theory being considered, the shift of the localized surface plasmon resonance (LSPR) peak reveals the formation mechanism of the double-layer nanostructure. Utilizing the enhanced optical nonlinearity of LiNbO3 as modulators, a Q-switched mode-locked waveguide laser at 1 µm is achieved with shorter pulse duration. It suggests potential applications to improve the performance of nonlinear photonic devices by using double-layer metallic nanostructures.