Multidirectional colloidal assembly in concurrent electric and magnetic fields

Dipolar interactions between nano- and micron sized colloids lead to their assembly into domains with well-defined local order. The particles with a single dipole induced by an external field assemble into linear chains and clusters. However, to achieve the formation of multidirectionally organized nano- or microassemblies with tunable physical characteristics, more sophisticated interaction tools are needed. Here we demonstrate that such complex interactions can be introduced in the form of two independent, non-interacting dipoles (double-dipoles) within a microparticle. We show how this can be achieved by the simultaneous application of alternating current (AC)-electric field and uniform magnetic field to dispersions of superparamagnetic microspheres. Depending on their timing and intensity, concurrent electric and magnetic fields lead to the formation of bidirectional particle chains, colloidal networks, and discrete crystals. We investigate the mechanistic details of the assembly process, and identify and classify the non-equilibrium states formed. The morphologies of different experimental states are in excellent correlation with our theoretical predictions based on Brownian dynamics simulations combined with a structural analysis based on local energy parameters. This novel methodology of introducing and interpreting double-dipolar particle interactions may assist in the assembly of colloidal coatings, dynamically reconfigurable particle networks, and bidirectional active structures.