Frustrated crystallization kinetics in marginally mismatched binary self-assembly driven by depletion interactions

We investigate two-dimensional crystal assemblies formed by a binary mixture of colloidal particles with a size ratio of 0.88 and driven by short-ranged depletion interactions. Our experiments show that the orientational order of the assembly decreases with an increasing fraction of impurity particles, reaching up to 18% reduction in a 1 : 1 binary mixture compared to a monodisperse suspension. We observe slower growth rate and arrested dynamics in the binary mixture, whereas the monodisperse sample follows a two-step nucleation and growth mechanism. We performed molecular dynamics simulations to calculate the minimum energy states for different size ratios and number ratios of the binary mixture. The simulation results predict a compromised translational order but sustained orientational order in a binary mixture with a size ratio as high as 0.88. From the combined experimental and numerical results, we conclude that the disordered assemblies found in a binary mixture originate from the frustration in assembly kinetics rather than topological frustration when there is a marginal mismatch between the two particle sizes.