Soft Plasmonic Assemblies Exhibiting Unnaturally High Refractive Index

The increases in refractive indices (n) of materials are crucial for transformative optical technologies. With the progress of monolithic lithography, large advances have been achieved with several semiconductors, including silicon, germanium, and gallium arsenide, which generally provide higher n of ∼4.0 compared to those of other elements. Nevertheless, above this upper limit of naturally available n, the range of light–matter interactions could be unprecedentedly expanded, which in turn enriches the possible applications. Here, we present a soft self-assembly of polyhedral Au colloids as a promising method to achieve unnaturally high n values. The interfacial assembly of Au nanocubes provides n of 6.4 at the resonant wavelength (near-infrared) and 4.5 in the off-resonant regimes (mid-infrared), which have not been previously reached. The soft self-assembly of polyhedral Au colloids can be a versatile and highly effective route for the fabrication of optical metamaterials with unnaturally high n values

Practical Limits of Achieving Artificial Magnetism and Effective Optical Medium by Using Self-Assembly of Metallic Colloidal Clusters

The self-assembly of metallic colloidal clusters (so called plasmonic metamolecules) has been viewed as a versatile, but highly effective approach for the materialization of the metamaterials exhibiting artificial magnetism at optical frequencies (including visible and near infrared (NIR) regimes). Indeed, several proofs of concepts of plasmonic metamolecules have been successfully demonstrated in both theoretical and experimental ways. Nevertheless, this self-assembly strategy has barely been used and still remains an underutilized method. For example, the self-assembly and optical utilization of the plasmonic metamolecules have been limited to the discrete unit of the structure; the materialization of effective optical medium made of plasmonic metamolecules is highly challenging. In this work, we theoretically exploited the practical limits of self-assembly technology for the fabrication of optical magnetic metamaterials

Achieving Optical Refractive Index of 10-Plus by Colloidal Self-Assembly

This study demonstrates the developments of self-assembled optical metasurfaces to overcome inherent limitations in polarization density (P) within natural materials, which hinder achieving high refractive indices (n) at optical frequencies. The Maxwellian macroscopic description establishes a link between P and n, revealing a static limit in natural materials, restricting n to approximately 4.0 at optical frequencies. Optical metasurfaces, utilizing metallic colloids on a deep-subwavelength scale, offer a solution by unnaturally enhancing n through electric dipolar (ED) resonances. Self-assembly enables the creation of nanometer-scale metallic gaps between metallic nanoparticles (NPs), paving the way for achieving exceptionally high n at optical frequencies. This study focuses on assembling polyhedral gold (Au) NPs into a closely packed monolayer by rationally designing the polymeric ligand to balance attractive and repulsive forces, in that polymeric brush-mediated self-assembly of the close-packed Au NP monolayer is robustly achieved over a large-area. The resulting monolayer of Au nanospheres (NSs), nanooctahedras (NOs), and nanocubes (NCs) exhibits high macroscopic integrity and crystallinity, sufficiently enough for pushing n to record-high regimes. The study underlies the significance of capacitive coupling in achieving an unnaturally high n and explores fine-tuning Au NC size to optimize this coupling. The achieved n of 10.12 at optical frequencies stands as a benchmark, highlighting the potential of polyhedral Au NPs in advancing optical metasurfaces

Petal-Inspired Diffractive Grating on a Wavy Surface: Deterministic Fabrications and Applications to Colorizations and LED Devices

Interestingly, the petals of flowering plants display unique hierarchical structures, in which surface relief gratings (SRGs) are conformably coated on a curved surface with a large radius of curvature (hereafter referred to as wavy surface). However, systematic studies on the interplay between the diffractive modes and the wavy surface have not yet been reported, due to the absence of deterministic nanofabrication methods capable of generating combinatorially diverse SRGs on a wavy surface. Here, by taking advantage of the recently developed nanofabrication composed of evaporative assembly and photofluidic holography inscription, we were able to achieve (i) combinatorially diverse petal-inspired SRGs with controlled curvatures, periodicities, and dimensionalities, and (ii) systematic optical studies of the relevant diffraction modes. Furthermore, the unique diffraction modes of the petal-inspired SRGs were found to be useful for the enhancement of the outcoupling efficiency of an organic light emitting diode (OLED). Thus, our systematic analysis of the interplay between the diffractive modes and the petal-inspired SRGs provides a basis for making more informed decisions in the design of petal-inspired diffractive grating and its applications to optoelectronics

Ultralow-Loss Substrate for Nanophotonic Dark-Field Microscopy

For the colloidal nanophotonic structures, a transmission electron microscope (TEM) grid has been widely used as a substrate of dark-field microscopy because a nanometer-scale feature can be effectively determined by TEM imaging following dark-field microscopic studies. However, an optically lossy carbon layer has been implemented in conventional TEM grids. A broadband scattering from the edges of the TEM grid further restricted an accessible signal-to-noise ratio. Herein, we demonstrate that the freely suspended, ultrathin, and wide-scale transparent nanomembrane can address such challenges. We developed a 1 mm by 600 μm scale and 20 nm thick poly­(vinyl formal) nanomembrane, whose area is around 180 times wider than a conventional TEM grid, so that the possible broadband scattering at the edges of the grid was effectively excluded. Also, such nanomembranes can be formed without the assistance of carbon support; allowing us to achieve the highest signal-to-background ratio of scattering among other substrates