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Abstract Integration of nanoscale photonic and plasmonic components on Si substrates is a critical step toward Si‐based integrated nanophotonic devices. In this work, a set of unique complex 3D metamaterials with intercalated nanolayered and nanopillar structures with tunable plasmonic and optical properties on Si substrates is designed. More specifically, the 3D metamaterials combine metal (Au) nanopillars and alternating metal‐nitride (Au‐TiN and Au‐TaN) nanolayers, epitaxially grown on Si substrates. The ultrafine Au nanopillars (d≈ 3 nm) continuously grow throughout all the nanolayers with high epitaxial quality. Novel optical properties, such as highly anisotropic optical property, high absorbance covering the entire visible spectrum regime, and hyperbolic property in the visible regime, are demonstrated. Furthermore, a waveguide based on a silicon nitride (Si₃N₄) ridge with a multilayer structure is successfully fabricated. The demonstration of 3D nanoscale metamaterial design integrated on Si opens up a new route toward tunable metamaterials nanostructure designs with versatile material selection for various optical components in Si integrated photonics. 

Abstract Photonic integrated circuits require various optical materials with versatile optical properties and easy on‐chip device integration. To address such needs, a well‐designed nanoscale metal‐oxide metamaterial, that is, plasmonic Au nanoparticles embedded in nonlinear LiNbO₃(LNO) matrix, is demonstrated with tailorable optical response. Specifically, epitaxial and single‐domain LNO thin films with tailored Au nanoparticle morphologies (i.e., various nanoparticle sizes and densities), are grown by a pulsed laser deposition method. The optical measurement presents obvious surface plasmon resonance and dramatically varied complex dielectric function because of the embedded Au nanoparticles, and its response can be well tailored by varying the size and density of Au nanoparticles. An optical waveguide structure based on the thin film stacks of a‐Si on SiO₂/Au‐LNO is fabricated and exhibits low optical dispersion with an optimized evanescent field staying in the LNO‐Au active layer. The hybrid Au‐LNO metamaterial thin films provide a novel platform for tunable optical materials and their future on‐chip integrations in photonic‐based integrated circuits.