High-Density and Well-Aligned Hierarchical Structures of Colloids Assembled under Orthogonal Magnetic and Electric Fields

Colloids can be used either as model systems for directed assembly or as the necessary building blocks for making functional materials. Previous work primarily focused on assembling colloids under a single external field, where controlling particle-particle interactions is limited. This work presents results under a combination of electric and magnetic fields. When these two fields are orthogonally applied, we can independently tune the magnitude and direction of the dipolar attraction and repulsion between the particles. As a result, we obtain well-aligned, highly dense, but individually separated linear chains at intermediate particle concentrations. Both the inter- and intrachain spacings can be tuned by adjusting the particle concentration and relative strengths of both fields. At high particle concentrations and by tuning the electric field frequency, the individual microspheres can assemble into colloidal oligomers such as trimers, tetramers, heptamers, and nonamers in response to the electric field due to the synergy between dipolar and electrohydrodynamic interactions. These oligomers, in turn, serve as building blocks for making hierarchical structures with finer architectures upon superimposing a one-dimensional (1D) magnetic field. In addition to experiments, Monte Carlo (MC) simulations have been performed on colloids confined near the electrode, interacting through a Stockmayer-like potential. They faithfully reproduce key observations in the experiments. Our work demonstrates the potential of using orthogonal electric and magnetic fields to assemble diversified types of highly aligned structures for applications in high-strength composites, optical materials, or structured battery electrodes.