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Percolated Plasmonic Superlattices of Nanospheres with 1 nm‐Level Gap as High‐Index Metamaterials

Nanophotonics relies on precise control of refractive index (RI) which can be designed with metamaterials. Plasmonic superstructures of nanoparticles (NPs) can suggest a versatile way of tuning RI. However, the plasmonic effects in the superstructures demand 1 nm‐level exquisite control over the interparticle gap, which is challenging in a sub‐wavelength NPs. Thus far, a large‐area demonstration has been mostly discouraged. Here, heteroligand AuNPs are prepared, which are stable in oil but become Janus particles at the oil–water interface, called “adaptive Janus particles.” NPs are bound at the interface and assembled into 2D arrays over square centimeters as toluene evaporates, which distinctively exhibits the RI tunability. In visible and NIR light, the 2D superstructures exhibit the highest‐ever RI (≈7.8) with varying the size and interparticle gap of NPs, which is successfully explained by a plasmonic percolation model. Furthermore, fully solution‐processable 2D plasmonic superstructures are proved to be advantageous in flexible photonic devices such as distributed Bragg reflectors.