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Organizing the colloidal particles into 3D superstructures is a promising strategy for fabricating functional metamaterials with novel optical, electric, and catalytic properties. The rich surface properties of the colloidal particles provide many ways to manipulate their assembly behavior. Emulsion droplets are ideal microspaces for confining colloidal self-assembly, offering many advantages such as versatility, scalability, and controllability over size, shape, and composition. In this review, we first introduce recently developed strategies for the emulsion-confined assembly of colloidal particles into 3D superstructures by manipulating the interfacial properties of the emulsion droplets and colloidal particles, then demonstrate the novel collective properties of the assembled superstructures and highlight some of their unique optical and catalytic properties and applications in bioimaging, diagnosis, drug delivery, and therapy.

Expensive instruments and complicated data processing are often required to discriminate solvents with similar structures and properties. Colorimetric sensors with high selectivity, low cost, and good portability are highly desirable to simplify such detection tasks. Herein, we report the fabrication of a photonic crystal sensor based on the self-assembled resorcinol formaldehyde (RF) hollow spheres to realize colorimetric sensing of polar solvents, including homologs and isomers based on the saturated diffusion time. The diffusion of solvent molecules through the photonic crystal film exhibits a unique three-step diffusion profile accompanied by a dynamic color change, as determined by the physicochemical properties of the solvent molecules and their interactions with the polymer shells, making it possible to accurately identify the solvent type based on the dynamic reflection spectra or visual perception. With its superior selectivity and sensitivity, this single-component colorimetric sensor represents a straightforward tool for convenient solvent detection and identification.

Morphological and magnetic anisotropy can be combined in colloidal assembly to create unconventional secondary structures. We show here that magnetite nanorods interact along a critical angle, depending on their aspect ratios and assemble into body-centered tetragonal colloidal crystals. Under a magnetic field, size-dependent attractive and repulsive domains develop on the ends and center of the nanorods, respectively. Our joint experiment-computational multiscale study demonstrates the presence of a critical angle in the attractive domain, which defines the equilibrium bonding states of interacting rods and leads to the formation of non–close-packed yet hard-contact tetragonal crystals. Small-angle x-ray scattering measurement attributes the perfect tetragonal phase to the slow assembly kinetics. The crystals exhibit brilliant structural colors, which can be actively tuned by changing the magnetic field direction. These highly ordered frameworks and well-defined three-dimensional nanochannels may offer new opportunities for manipulating nanoscale chemical transformation, mass transportation, and wave propagation.

Responsive chromic materials are highly desirable in the fields of displays, anti-counterfeiting, and camouflage, but their advanced applications are usually limited by the unrealized delicate and independent tunability of their three intrinsic attributes of color. This work achieves the separate, continuous, and reversible modulation of structural color brightness and hue with an aqueous suspension of dual-responsive Fe 3 O 4 @polyvinylpyrrolidone (PVP)@poly( N -isopropyl acrylamide) (PNIPAM) flexible photonic nanochains. The underlying modulation mechanism of color brightness was experimentally and numerically deciphered by analyzing the morphological responses to stimuli. When an increasing magnetic field was applied, the random worm-like flexible photonic nanochains gradually orientated along the field direction, due to the dominant magnetic dipole interaction over the thermal motion, lengthening the orientation segment length up to the whole of the nanochains. Consequently, the suspension displays increased color brightness (characterized by diffraction intensity). Meanwhile, the color hue (characterized by diffraction frequency) could be controlled by temperature, due to the volume changes of the interparticle PNIPAM. The achieved diverse color modulation advances the next-generation responsive chromic materials and enriches the basic understanding of the color tuning mechanisms. With versatile and facile color tunability and shape patterning, the developed responsive chromic liquid promises tomore »have attractive potential in full-color displays and in adaptive camouflages.« less

Over the last three decades, photonic crystals (PhCs) have attracted intense interests thanks to their broad potential applications in optics and photonics. Generally, these structures can be fabricated via either “top-down” lithographic or “bottom-up” self-assembly approaches. The self-assembly approaches have attracted particular attention due to their low cost, simple fabrication processes, relative convenience of scaling up, and the ease of creating complex structures with nanometer precision. The self-assembled colloidal crystals (CCs), which are good candidates for PhCs, have offered unprecedented opportunities for photonics, optics, optoelectronics, sensing, energy harvesting, environmental remediation, pigments, and many other applications. The creation of high-quality CCs and their mass fabrication over large areas are the critical limiting factors for real-world applications. This paper reviews the state-of-the-art techniques in the self-assembly of colloidal particles for the fabrication of large-area high-quality CCs and CCs with unique symmetries. The first part of this review summarizes the types of defects commonly encountered in the fabrication process and their effects on the optical properties of the resultant CCs. Next, the mechanisms of the formation of cracks/defects are discussed, and a range of versatile fabrication methods to create large-area crack/defect-free two-dimensional and three-dimensional CCs are described. Meanwhile, we also shed light onmore »both the advantages and limitations of these advanced approaches developed to fabricate high-quality CCs. The self-assembly routes and achievements in the fabrication of CCs with the ability to open a complete photonic bandgap, such as cubic diamond and pyrochlore structure CCs, are discussed as well. Then emerging applications of large-area high-quality CCs and unique photonic structures enabled by the advanced self-assembly methods are illustrated. At the end of this review, we outlook the future approaches in the fabrication of perfect CCs and highlight their novel real-world applications.« less