Directed Self‐Assembly Pathways of Active Colloidal Clusters

Despite the mounting interest in synthetic active particles, too little is known about their assembly into higher‐order clusters. Here, mixing bare silica particles with Janus particles that are self‐propelled in electric fields, we assemble rotating chiral clusters of various sorts, their structures consisting of active particles wrapped around central “hub” particles. These clusters self‐assemble from the competition between standard energetic interactions and the need to be stable as the clusters rotate when the energy source is turned on, and fall apart when the energy input is off. This allows one to guide the formation of intended clusters, as the final structure depends notably on the sequence of steps in which the clusters form.