Magnetic Coupling in Colloidal Clusters for Hierarchical Self-Assembly

[Image: see text] Manipulating the way in which colloidal particles self-organize is a central challenge in the design of functional soft materials. Meeting this challenge requires the use of building blocks that interact with one another in a highly specific manner. Their fabrication, however, is limited by the complexity of the available synthesis procedures. Here, we demonstrate that, starting from experimentally available magnetic colloids, we can create a variety of complex building blocks suitable for hierarchical self-organization through a simple scalable process. Using computer simulations, we compress spherical and cubic magnetic colloids in spherical confinement, and investigate their suitability to form small clusters with reproducible structural and magnetic properties. We find that, while the structure of these clusters is highly reproducible, their magnetic character depends on the particle shape. Only spherical particles have the rotational degrees of freedom to produce consistent magnetic configurations, whereas cubic particles frustrate the minimization of the cluster energy, resulting in various magnetic configurations. To highlight their potential for self-assembly, we demonstrate that already clusters of three magnetic particles form highly nontrivial Archimedean lattices, namely, staggered kagome, bounce, and honeycomb, when focusing on different aspects of the same monolayer structure. The work presented here offers a conceptually different way to design materials by utilizing preassembled magnetic building blocks that can readily self-organize into complex structures.