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Icosahedral colloidal clusters are a new class of spherical colloidal crystals. This cluster allows for potentially superior optical properties in comparison to conventional onion-like colloidal su...

Colloidal assembly in emulsion drops provides fundamental tools for studying optimum particle arrangement under spherical confinement and practical means for producing photonic microparticles. Recent progress has revealed that energetically favored cluster configurations are different from conventional supraballs, which could enhance optical performance. This paper reviews state-of-the-art emulsion-templated colloidal clusters, and particularly focuses on recently reported novel structures such as icosahedral, decahedral, and single-crystalline face-centered cubic (fcc) clusters. We classify the clusters according to the number of component particles as small (N < O(102)), medium (O(102) ≤ N ≤ O(104)), and large (N ≥ O(105)). For each size of clusters, we discuss the detailed structures, mechanisms of cluster formation, and optical properties and potential applications. Finally, we outline current challenges and questions that require further investigation.

Colloidal particles with a repulsive interparticle potential spontaneously form crystalline lattices, which are used as a motif for photonic materials. It is difficult to predict the crystal arrangement in spherical volume as lattices are incompatible with a spherical surface. Here, the optimum arrangement of charged colloids is experimentally investigated by encapsulating them in double-emulsion drops. Under conditions of strong interparticle repulsion, the colloidal crystal rapidly grows from the surface toward the center of the microcapsule, forming an onion-like arrangement. By contrast, for weak repulsion, crystallites slowly grow and fuse through rearrangement to form a single-crystal phase. Single-crystal structure is energetically favorable even for strong repulsion. Nevertheless, a high energy barrier to colloidal rearrangement kinetically arrests the onion-like structure formed by heterogeneous nucleation. Unlike the isotropic onion-shaped product, the anisotropic single-crystal-containing microcapsules selectively display-at certain orientations but not others-one of the distinct colors from the various crystal planes.

Colloidal crystallization is analogous to the crystallization in bulk atomic systems in various aspects, which has been explored as a model system. However, a real-time probing of the phenomenon still remains challenging. Here, a levitation system for a study of colloidal crystallization is demonstrated. Colloidal particles in a levitated droplet are gradually concentrated by isotropic evaporation of water from the surface of the droplet, resulting in crystallization. The structural change of the colloidal array during crystallization is investigated by simultaneously measuring the volume and reflectance spectra of the droplet. The crystal nucleates from the surface of the droplet at which the volume fraction exceeds the threshold and then the growth proceeds. The crystal growth behavior depends on the initial concentrations of colloidal particles and salts which determine the overall direction of crystal growth and interparticle spacing, respectively. The results show that a levitating bulk droplet has a great potential as a tool for in situ investigation of colloidal crystallization.