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Cracks and defects, which could result in lower reflectivity and larger full width at half maximum (FWHM), are the major obstacles for obtaining highly ordered structures of colloidal crystals (CCs). The high-quality CCs with high reflectivity (more than 90%) and 9.2 nm narrow FWHM have been successfully fabricated using a fixed proportion of a soft matter system composed of silica particles (SPs), polyethylene glycol diacrylate (PEGDA), and ethanol. The influences of refractivity difference, volume fractions, and particle dimension on FWHM were illuminated. Firstly, we clarified the influences of the planar interface and the bending interface on the self-assembly. The CCs had been successfully fabricated on the planar interface and presented unfavorable results on the bending interface. Secondly, a hard sphere system consisting of SPs, PEGDA, and ethanol was established, and the entropy-driven phase transition mechanism of a polydisperse system was expounded. The FWHM and reflectivity of CCs showed an increasing trend with increasing temperature. Consequently, high-quality CCs were obtained by adjusting temperatures (ordered structure formed at 90 °C and solidified at 0 °C) based on the surface phase rule of the system. We acquired a profound understanding of the principle and process of self-assembly, which is significant for preparation and application of CCs such as optical filters.

Entropy-Induced Self-Assembly of Colloidal Crystals with High Reflectivity and Narrow Reflection Bandwidth