Metal-free plasmonic metamaterials with wide-range tunable optical properties are highly desired for various components in future integrated optical devices. Designing a ceramic–ceramic hybrid metamaterial has been theoretically proposed as a solution to this critical optical material demand. However, the processing of such all-ceramic metamaterials is challenging due to difficulties in integrating two very dissimilar ceramic phases as one hybrid system. In this work, an oxide-nitride hybrid metamaterial combining two highly dissimilar ceramic phases, i.e., semiconducting weak ferromagnetic NiO nanorods and conductive plasmonic TiN matrix, has been successfully integrated as a unique vertically aligned nanocomposite form. Highly anisotropic optical properties such as hyperbolic dispersions and strong magneto-optical coupling have been demonstrated under room temperature. The novel functionalities presented show the strong potentials of this new ceramic–ceramic hybrid thin film platform and its future applications in next-generation nanophotonics and magneto-optical integrated devices without the lossy metallic components.

Magneto‐optical (MO) coupling incorporates photon‐induced change of magnetic polarization that can be adopted in ultrafast switching, optical isolators, mode convertors, and optical data storage components for advanced optical integrated circuits. However, integrating plasmonic, magnetic, and dielectric properties in one single material system poses challenges since one natural material can hardly possess all these functionalities. Here, co‐deposition of a three‐phase heterostructure composed of a durable conductive nitride matrix with embedded core–shell vertically aligned nanopillars, is demonstrated. The unique coupling between ferromagnetic NiO core and atomically sharp plasmonic Au shell enables strong MO activity out‐of‐plane at room temperature. Further, a template growth process is applied, which significantly enhances the ordering of the nanopillar array. The ordered nanostructure offers two schemes of spin polarization which result in stronger antisymmetry of Kerr rotation. The presented complex hybrid metamaterial platform with strong magnetic and optical anisotropies is promising for tunable and modulated all‐optical‐based nanodevices.

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Materials with magneto-optic coupling properties are highly coveted for their potential applications ranging from spintronics and optical switches to sensors. In this work, a new, three-phase Au–Fe–La0.5Sr0.5FeO3 (LSFO) hybrid material grown in a vertically aligned nanocomposite (VAN) form has been demonstrated. This three-phase hybrid material combines the strong ferromagnetic properties of Fe and the strong plasmonic properties of Au and the dielectric nature of the LSFO matrix. More interestingly, the immiscible Au and Fe phases form Au-encapsulated Fe nanopillars, embedded in the LSFO matrix. Multifunctionalities including anisotropic optical dielectric properties, plasmonic properties, magnetic anisotropy, and room-temperature magneto-optic Kerr effect coupling are demonstrated. The single-step growth method to grow the immiscible two-metal nanostructures (i.e., Au and Fe) in the complex hybrid material form opens exciting new potential opportunities for future three-phase VAN systems with more versatile metal selections.

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