The process of crystallization is difficult to observe for transported, out-of-equilibrium systems, as the continuous energy injection increases activity and competes with ordering. In emerging fields such as microfluidics and active matter, the formation of long-range order is often frustrated by the presence of hydrodynamics. Here we show that a population of colloidal rollers assembled by magnetic fields into large-scale propelling carpets can form perfect crystalline materials upon suitable balance between magnetism and hydrodynamics. We demonstrate a field-tunable annealing protocol based on a controlled colloidal flow above the carpet that enables complete crystallization after a few seconds of propulsion. The structural transition from a disordered to a crystalline carpet phase is captured via spatial and temporal correlation functions. Our findings unveil a novel pathway to magnetically anneal clusters of propelling particles, bridging driven systems with crystallization and freezing in material science.

The realization of micromotors able to dock and transport microscopic objects in a fluid medium has direct applications toward the delivery of drugs and chemicals in small channels and pores, and the realization of functional wireless microrobots in lab-on-a-chip technology. A simple and general method to tow microscopic particles in water by using remotely controllable light-activated hematite microdockers is demonstrated. These anisotropic ferromagnetic particles can be synthesized in bulk and present the remarkable ability to be activated by light while independently manipulated via external fields. The photoactivation process induces a phoretic flow capable to attract cargos toward the surface of the propellers, while a rotating magnetic field is used to transport the composite particles to any location of the experimental platform. The method allows the assembling of small colloidal clusters of various sizes, composed by a skeleton of mobile magnetic dockers, which cooperatively keep, transport, and release the microscopic cargos. The possibility to easily reconfigure in situ the location of the docker above the cargo is demonstrated, which enables optimize transport and cargo release operations.

SignificanceCollections of polar active particles have been unable to form stable and long-living structures due to the presence of self-propulsion. We solve this timely issue by introducing the concept of “active doping” and show that a few light-activated apolar, i.e., non–self-propelling, units can be used to rapidly trigger the formation of solid clusters and gels composed of passive colloidal particles. Our active doping can be used to assemble disparate microscopic objects, including synthetic or biological ones, paving the way toward the extension of fundamental concepts of gel and glass formation to active out-of-equilibrium systems.

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