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Common materials show a limited range of refractive indices over the visible and infrared wavelengths, and their values are not easily tunable once the material is chosen. Here, self-assembled metal nanoparticle arrays are proposed as an effective optical material with a large range of possible refractive indices that are nearly dispersionless over broad wavelength ranges. The material can be potentially fabricated over a large curved surface, and the resulting index is even more tunable by various postprocessing methods, such as material substitution or mechanical stretching. We achieve the highest refractive index of 5.0 at resonance in the visible, exceeding 4.2 over a broadband wavelength regime out of resonance. The key differences from previous studies of self-assembled metal particle arrays are the consideration of the diamagnetic effect and the careful choice of the ligands, which determine the gaps between particles. The sensitivity of the effective index to the size and material of the gap regio...

Multilevel hierarchical platforms that combine nano- and microstructures have been intensively explored to mimic superior properties found in nature. However, unless directly replicated from biological samples, desirable multiscale structures have been challenging to efficiently produce to date. Departing from conventional wafer-based technology, new and efficient techniques suitable for fabricating bioinspired structures are highly desired to produce three-dimensional architectures even on nonplanar substrates. Here, we report a facile approach to realize functional nanostructures on uneven microstructured platforms via scalable optical fabrication techniques. The ultrathin form (∼3 μm) of a phase grating composed of poly(vinyl alcohol) makes the material physically flexible and enables full-conformal contact with rough surfaces. The near-field optical effect can be identically generated on highly curved surfaces as a result of superior conformality. Densely packed nanodots with submicron periodicity are uniformly formed on microlens arrays with a radius of curvature that is as low as ∼28 μm. Increasing the size of the gratings causes the production area to be successfully expanded by up to 16 in(2). The "nano-on-micro" structures mimicking real compound eyes are transferred to flexible and stretchable substrates by sequential imprinting, facilitating multifunctional optical films applicable to antireflective diffusers for large-area sheet-illumination displays.

Plasmonics allow localization of an electromagnetic (EM) field into nanoscale "hotspots", a feature that is of technological significance due to potential applications related to spectroscopic sensing and nanofocusing. In relation to this, many researchers have sought to fabricate metallic nanostructures with sharp edges, as they provide much higher EM field enhancement compared with rounded structures. However, a fabrication method satisfying stringent requirements for the efficient EM field enhancement including three-dimensionality, vertical orientation, large-area fabrication, and tunability of structural features, which are of practical importance for efficient plasmonic light enhancement at hotspots, has yet to be achieved. Herein, we fabricate large-area, vertically aligned three-dimensional plasmonic tip (i.e., nanofunnel) arrays with unprecedented flexibility in the control of the structural features by directional photofluidization lithography. Using this approach, the structural features of nanofunnel tips including the sharpness, shape, and orientation were precisely controlled in a scalable and deterministic manner. The effects of the structural features of the nanofunnel on the EM field enhancement were systematically investigated and analyzed, and the optimum tip features for maximum EM field enhancement were thereupon identified. The suggested nanofabrication technique and resulting structures will be of practical importance in spectroscopic and nanophotonic applications.

Highly ordered metallic nanostructures have attracted an increasing interest in nanoscale electronics, photonics, and spectroscopic imaging. However, methods typically used for fabricating metallic nanostructures, such as direct writing and template-based nanolithography, have low throughput and are, moreover, limited to specific fabricated shapes such as holes, lines, and prisms, respectively. Herein, we demonstrate directional photofluidization lithography (DPL) as a new method to address the aforementioned problems of current nanolithography. The key idea of DPL is the use of photoreconfigurable polymer arrays to be molded in metallic nanostructures instead of conventional colloids or cross-linked polymer arrays. The photoreconfiguration of polymers by directional photofluidization allows unprecedented control over the sizes and shapes of metallic nanostructures. Besides the capability for precise control of structural features, DPL ensures scalable, parallel, and cost-effective processing, highly compatible with high-throughput fabrication. Therefore, DPL can expand not only the potential for specific metallic nanostructure applications but also large-scale innovative nanolithography.