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Self-assembly processes provide the means to achieve scalable and versatilemetamaterials by "bottom-up" fabrication. Despite their enormous potential,especially as a platform for energy materials, self-assembled metamaterials areoften limited to single phase systems, and complex multi-phase metamaterialshave scarcely been explored.We propose a new approach based on sequentialself-assembly that enables the formation of a two-phase metamaterial composedof a disordered network metamaterial with embedded nanoparticles. Takingadvantage of both the high-spatial and high-energy resolution of electronenergy loss spectroscopy, we observe inhomogeneous localization of light in thenetwork, concurrent with dipolar and higher-order localized surface plasmonmodes in the nanoparticles. Moreover, we demonstrate that the coupling strengthdeviates from the interaction of two classical dipoles when entering the strongcoupling regime. The observed energy exchange between two phases in thiscomplex metamaterial, realized solely through self-assembly, implies thepossibility to exploit these disordered systems for plasmon-enhanced catalysis.

Sequential Self-Assembly for Scalable Fabrication of Disordered Two-Phase Metamaterials