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

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