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Structural color arises from geometric diffraction; it has potential applications in optical materials because it is more resistant to environmental degradation than coloration mechanisms that are of chemical origin. Structural color can be produced from self-assembled films of colloidal size particles. While the relationship between the crystal structure and structural color reflection peak wavelength is well studied, the connection between assembly quality and the degree of reflective structural color is less understood. Here, we study this connection by investigating the structural color reflection peak intensity and width as a function of defect density and film thickness using a combined experimental and computational approach. Polystyrene microspheres are self-assembled into defective colloidal crystals via solvent evaporation. Colloidal crystal growth via sedimentation is simulated with molecular dynamics, and the reflection spectra of simulated structures are calculated by using the finite-difference time-domain algorithm. We examine the impact of commonly observed defect types (vacancies, stacking fault tetrahedra, planar faults, and microcracks) on structural color peak intensity. We find that the reduction in peak intensity scales with increased defect density. The reduction is less sensitive to the type of defect than to its volume. In addition, the reflectance of structural color increases as a function of the crystal thickness, until a plateau is reached at thicknesses greater than about 9.0 μm. The maximum reflection is 78.8 ± 0.9%; this value is significantly less than the 100% reflectivity predicted for a fully crystalline, defect-free material. Furthermore, we find that colloidal crystal films with small quantities of defects may be approximated as multilayer reflective materials. These findings can guide the design of optical materials with variable structural color intensity.

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Self-assembled colloidal crystals can exhibit structural colors, a phenomenon of intense reflection within a range of wavelengths caused by constructive interference. Such diffraction effects are most intense for highly uniform crystals; however, in practice, colloidal crystals may include particles of irregular size, which can reduce the quality of the crystal. Despite its importance in realizing high-quality structural colors, a quantitative relationship between particles of irregular size, crystal quality, and the resultant structural color response remains unclear. This study systematically and quantitatively investigates the effect of adding particles of irregular size on the microstructural quality and structural color reflectivity of colloidal crystals formed by evaporative self-assembly via experiment and simulation. We examine two sizes of irregular particlesthose which are 1.9 times larger and 0.4 times smaller than the host crystal. We find that small irregular particles are more detrimental to surface crystal quality and structural color reflectivity than large irregular particles. When incorporated with 10% volume fraction of irregularly sized particles, the reflectivity of crystal films with large (small) irregularly sized particles decreases by 18.4 ± 5.6% (27.5 ± 5.8%), and a measure of surface crystal quality derived from Fourier analysis of scanning electron microscopy images reduces by 40.0 ± 4.5% (48.8 ± 6.0%). By modeling colloidal films incorporated with irregular particles via molecular dynamics simulation and computing the reflection spectra of the modeled crystals via the finite-difference time-domain method, we find that the peak reflectivity of the assembled structures increases monotonically with overall crystallinity, and that overall crystallinity is correlated with the volume fraction of incorporated irregular particles. The quantitative relationships developed in this study can be applied to predict the level of irregularly sized particles that can be tolerated in colloidal films before significant degradation in crystal quality and reflectivity occurs.

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