Direct Three-Dimensional Observation of the Plasmonic Near-Fields of a Nanoparticle with Circular Dichroism.

Characterizing the spatial distribution of the electromagnetic fields of a plasmonic nanoparticle is crucial for exploiting its strong light-matter interaction for optoelectronic and catalytic applications. However, observing the near-fields in three dimensions with a high spatial resolution is still challenging. To realize efficient three-dimensional (3D) nanoscale mapping of the plasmonic fields of nanoparticles with complex shapes, this work established autoencoder-embedded electron energy loss spectroscopy (EELS) tomography.

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) and high refractive indices (n) within naturally occurring materials. The Maxwellian macroscopic description establishes a link between P and n, revealing a static limit in natural materials, restricting n to ≈4.0 at optical frequencies.

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A general guiding principle for colloidal crystallization is to tame the attractive enthalpy such that it slightly overwhelms the repulsive interaction. As-synthesized colloids are generally designed to retain a strong repulsive potential for the high stability of suspensions, encoding appropriate attractive potentials into colloids has been key to their crystallization. Despite the myriad of interparticle attractions for colloidal crystallization, the van der Waals (vdW) force remains unexplored.

Strain and crystallographic identification of the helically concaved gap surfaces of chiral nanoparticles.

Identifying the three-dimensional (3D) crystal plane and strain-field distributions of nanocrystals is essential for optical, catalytic, and electronic applications. However, it remains a challenge to image concave surfaces of nanoparticles. Here, we develop a methodology for visualizing the 3D information of chiral gold nanoparticles ≈ 200 nm in size with concave gap structures by Bragg coherent X-ray diffraction imaging.

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.

Enantioselective sensing by collective circular dichroism.

Quantitative determination and in situ monitoring of molecular chirality at extremely low concentrations is still challenging with simple optics because of the molecular-scale mismatch with the incident light wavelength. Advances in spectroscopy and nanophotonics have successfully lowered the detection limit in enantioselective sensing, as it can bring the microscopic chiral characteristics of molecules into the macroscopic scale or squeeze the chiral light into the subwavelength scale. Conventional nanophotonic approaches depend mainly on the optical helicity density by localized resonances within an individual structure, such as localized surface plasmon resonances (LSPRs) or dielectric Mie resonances.

DNA as grabbers and steerers of quantum emitters.

The chemically synthesizable quantum emitters such as quantum dots (QDs), fluorescent nanodiamonds (FNDs), and organic fluorescent dyes can be integrated with an easy-to-craft quantum nanophotonic device, which would be readily developed by non-lithographic solution process. As a representative example, the solution dipping or casting of such soft quantum emitters on a flat metal layer and subsequent drop-casting of plasmonic nanoparticles can afford the quantum emitter-coupled plasmonic nanocavity (referred to as a nanoparticle-on-mirror (NPoM) cavity), allowing us for exploiting various quantum mechanical behaviors of light-matter interactions such as quantum electrodynamics (QED), strong coupling (e.g.

DNA Origami Guided Self-Assembly of Plasmonic Polymers with Robust Long-Range Plasmonic Resonance.

Plasmonic polymers consisting of metallic nanoparticles (NPs) are able to squeeze light into the deep-subwavelength space and transfer along a highly confined nanoscale path in long range. DNA nanotechnology, particularly benefiting from the molecular programmability of DNA origami, has provided otherwise nearly impossible platforms for constructing plasmonic nanoparticle polymers with designer configurations and nanoscale gaps. Here, we design and assemble a DNA origami hashtag tile that is able to polymerize into one-dimensional chains with high rigidity.

Exploiting Colloidal Metamaterials for Achieving Unnatural Optical Refractions.

The scaling down of meta-atoms or metamolecules (collectively denoted as metaunits) is a long-lasting issue from the time when the concept of metamaterials was first suggested. According to the effective medium theory, which is the foundational concept of metamaterials, the structural sizes of meta-units should be much smaller than the working wavelengths (e.g.

DNA Base Pair Stacking Crystallization of Gold Colloids.

We describe a DNA base pair (bp) stacking driven 3D crystallization of 70-80 nm gold nanospheres (Au NSs) into a large-area, face-centered-cubic (FCC) lattice. Although great advances have been achieved over the past decade, DNA nanoparticle (NP) crystallization has relied solely on the base complementary binding. This limits the accessible crystal size particularly for the larger and heavier Au NPs (>50 nm).

Bioinspired Toolkit Based on Intermolecular Encoder toward Evolutionary 4D Chiral Plasmonic Materials.

Over the last two decades, nanophotonics, including plasmonics and metamaterials, have promised compelling opportunities for exotic control over light-matter interactions. The strong chiral light-matter interaction is a representative example. Three-dimensional (3D) chirality has existed naturally only in organic molecules and bio-organisms, but a negligible chiroptic effect was attained with these naturally occurring materials because of their small absorption cross sections.

Magnetic Plasmon Networks Programmed by Molecular Self-Assembly.

Nanoscale manipulation of magnetic fields has been a long-term pursuit in plasmonics and metamaterials, as it can enable a range of appealing optical properties, such as high-sensitivity circular dichroism, directional scattering, and low-refractive-index materials. Inspired by the natural magnetism of aromatic molecules, the cyclic ring cluster of plasmonic nanoparticles (NPs) has been suggested as a promising architecture with induced unnatural magnetism, especially at visible frequencies. However, it remains challenging to assemble plasmonic NPs into complex networks exhibiting strong visible magnetism.

Photofluidic Near-Field Mapping of Electric-Field Resonance in Plasmonic Metasurface Assembled with Gold Nanoparticles.

We present a near-field mapping of electric fields from the individual superspherical and ultrasmooth gold nanoparticles (AuNPs) and artificially assembled AuNP nanostructures by measuring the reconfiguration of an azobenzene-containing polymer(azo-polymer) film. Various configurations of AuNPs and the azo-polymer were studied with atomic force microscopy measurements and calculations. The interference was systematically studied with AuNP dimers of various gap distances and different embedding depth in the polymer film.

Assembly of "3D" plasmonic clusters by "2D" AFM nanomanipulation of highly uniform and smooth gold nanospheres.

Atomic force microscopy (AFM) nanomanipulation has been viewed as a deterministic method for the assembly of plasmonic metamolecules because it enables unprecedented engineering of clusters with exquisite control over particle number and geometry. Nevertheless, the dimensionality of plasmonic metamolecules via AFM nanomanipulation is limited to 2D, so as to restrict the design space of available artificial electromagnetisms. Here, we show that "2D" nanomanipulation of the AFM tip can be used to assemble "3D" plasmonic metamolecules in a versatile and deterministic way by dribbling highly spherical and smooth gold nanospheres (NSs) on a nanohole template rather than on a flat surface.

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.