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Magnetically-guided colloidal assembly has proven to be a versatile method for building hierarchical particle assemblies. This review describes the dipolar interactions that govern superparamagnetic colloids in time-varying magnetic fields, and how such interactions have guided colloidal assembly into materials with increasing complexity that display novel dynamics. The assembly process is driven by magnetic dipole–dipole interactions, whose strength can be tuned to be attractive or repulsive. Generally, these interactions are directional in static external magnetic fields. More recently, time-varying magnetic fields have been utilized to generate dipolar interactions that vary in both time and space, allowing particle interactions to be tuned from anisotropic to isotropic. These interactions guide the dynamics of hierarchical assemblies of 1-D chains, 2-D networks, and 2-D clusters in both static and time-varying fields. Specifically, unlinked and chemically-linked colloidal chains exhibit complex dynamics, such as fragmentation, buckling, coiling, and wagging phenomena. 2-D networks exhibit controlled porosity and interesting coarsening dynamics. Finally, 2-D clusters have shown to be an ideal model system for exploring phenomena related to statistical thermodynamics. This review provides recent advances in this fast-growing field with a focus on its scientific potential. 

Phase separation processes are widely utilized to assemble complex fluids into novel materials. These separation processes can be thermodynamically driven due to changes in concentration, pressure, or temperature. Phase separation can also be induced with external stimuli, such as magnetic fields, resulting in novel nonequilibrium systems. However, how external stimuli influence the transition pathways between phases has not been explored in detail. Here, we describe the phase separation dynamics of superparamagnetic colloids in time-varying magnetic fields. An initially homogeneous colloidal suspension can transition from a continuous colloidal phase with voids to discrete colloidal clusters, through a bicontinuous phase formed via spinodal decomposition. The type of transition depends on the particle concentration and magnitude of the applied magnetic field. The spatiotemporal evolution of the microstructure during the nucleation and growth period is quantified by analyzing the morphology using Minkowski functionals. The characteristic length of the colloidal systems was determined to correlate with system variables such as magnetic field strength, particle concentration, and time in a power-law scaling relationship. Understanding the interplay between particle concentration and applied magnetic field allows for better control of the phases observed in these magnetically tunable colloidal systems.