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                            We demonstrate the preparation of colloidal crystals at nematic liquid crystal–air interfaces by simultaneous photopolymerization and assembly. Polymer colloids are produced by polymerization-induced phase separation of 2-hydroxyethyl methacrylate in the non-reactive liquid crystal (LC) 4-cyano-4′-pentylbiphenyl (5CB) using an open-cell setup. Colloids adsorbed to the nematic 5CB–air interface form non-close-packed hexagonal crystals that cover the entire interface area. We examine the mechanism of growth and assembly for the preparation of LC-templated interfacial colloidal superstructures. 
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