Shape and Interaction Decoupling for Colloidal Pre-Assembly

Creating materials with a structural hierarchy that is independently controllable at a range of scales requires breaking naturally occurring hierarchies. Breaking natural hierarchies is possible if building block attributes can be decoupled from the structure of pre-assembled, mesoscale building blocks that form the next level in the structural hierarchy. Here, we show that pre-assembled colloidal structures achieving geometric and interaction decoupling can be prepared in emulsions of silica superballs, which are cubic-like particles with rounded edges. We show that, for clusters of up to nine particles, colloidal superballs pack consistently like spheres, despite the presence of shape anisotropy and facets in the cubic-like particles. We compare our results with clusters prepared with magnetic superballs and find good qualitative agreement, suggesting that the cluster geometries are solely determined by the shape of the constituent particles. Our findings demonstrate that highly shape-anisotropic building blocks, under suitable conditions, can be pre-assembled into structures that are not found in bulk, thereby achieving a decoupling that can be further exploited for hierarchical materials development.