Phase transformations can be difficult to characterize at the microscopic level due to the inability to directly observe individual atomic motions. Model colloidal systems, by contrast, permit the direct observation of individual particle dynamics and of collective rearrangements, which allows for real-space characterization of phase transitions. Here, we study a quasi-two-dimensional, binary colloidal alloy that exhibits liquid–solid and solid–solid phase transitions, focusing on the kinetics of a diffusionless transformation between two crystal phases. Experiments are conducted on a monolayer of magnetic and nonmagnetic spheres suspended in a thin layer of ferrofluid and exposed to a tunable magnetic field. A theoretical model of hard spheres with point dipoles at their centers is used to guide the choice of experimental parameters and characterize the underlying materials physics. When the applied field is normal to the fluid layer, a checkerboard crystal forms; when the angle between the field and the normal is sufficiently large, a striped crystal assembles. As the field is slowly tilted away from the normal, we find that the transformation pathway between the two phases depends strongly on crystal orientation, field strength, and degree of confinement of the monolayer. In some cases, the pathway occurs by smooth magnetostrictive shear, while in others it involves the sudden formation of martensitic plates.

Electromagnetic fields can generate orientation-dependent, long range interactions between colloidal components that direct their assembly into highly ordered structures, such as small ordered clusters, chains, and large crystalline lattices. While much effort has been devoted to exploring the assembly of spherical colloids, few reports have investigated the directed assembly of non-spherical particles with Janus or patchy morphologies. Here, we use photolithographic techniques to fabricate a wide range of anisotropically shaped patchy particles and follow their assembly in liquid suspensions under the influence of electric and magnetic fields. We analyze the assembly of several types of patchy particles across a range of field parameters and fluid compositions, and report a number of distinct, well-ordered, assembly architectures including cylindrical, prismatic, and staggered chains. The structures assembled from anisotropic patchy components provide a glimpse into the range of architectures that can be created by combining field directed assembly with rationally designed particles. By using numerical simulations to model the electric and magnetic field interactions between these particles, we interpret the results of the assembly process and explain how they can be controlled by the position of the metal facet, the frequency (for AC fields), or magnetic susceptibility of the medium. The resulting structures, and similar ones produced through the field-directed assembly of patchy anisotropic particles, can possess unique electrical and optical properties and may have potential applications in a number of future technology applications such as microactuators, metamaterials and multiferroic materials.

We demonstrate a magnetic technique for assembling bidisperse and tridisperse colloidal particle fluids into a variety of complex structures with dimensionality ranging from 0-D (rings) to 1-D (chains) to 2-D (tiles). Compared with prior work on bidisperse particles that are commensurate in size, here we explore the assembly of different sized particles, and we show that due to packing constraints, new particle structures can be realized experimentally. Extending these experiments to a tridisperse system, we demonstrate that at low concentrations the smallest particle does not change the underlying crystal structures of the bidisperse system; however, it can assist in the formation of crystallite structures that were not stable in a bidisperse system. Additionally, we discovered that the smallest particle mimics the role of the ferrofluid, by shifting the locations in phase space where the bidisperse crystal structures can be experimentally obtained. Finally, we demonstrate that 3-particle crystal structures can be tuned by varying the strength of the external field, which is not possible in a 2-particle system.Keywords: colloidal particles; diamagnetic; dipole−dipole interaction; ferrofluid; magnetic assembly; paramagnetic; tunable

We present theoretical, numerical, and experimental analyses on the non-linear dynamic behavior of superparamagnetic beads exposed to a periodic array of micro-magnets and an external rotating field. The agreement between theoretical and experimental results revealed that non-linear magnetic forcing dynamics are responsible for transitions between phase-locked orbits, sub-harmonic orbits, and closed orbits, representing different mobility regimes of colloidal beads. These results suggest that the non-linear behavior can be exploited to construct a novel colloidal separation device that can achieve effectively infinite separation resolution for different types of beads, by exploiting minor differences in their bead's properties. We also identify a unique set of initial conditions, which we denote the “devil's gate” which can be used to expeditiously identify the full range of mobility for a given bead type.

The assembly of complex structures out of simple colloidal building blocks is of practical interest for building materials with unique optical properties (for example photonic crystals1 and DNA biosensors2) and is of fundamental importance in improving our understanding of self-assembly processes occurring on molecular to macroscopic length scales3, 4, 5. Here we demonstrate a self-assembly principle that is capable of organizing a diverse set of colloidal particles into highly reproducible, rotationally symmetric arrangements. The structures are assembled using the magnetostatic interaction between effectively diamagnetic and paramagnetic particles within a magnetized ferrofluid. The resulting multipolar geometries resemble electrostatic charge configurations such as axial quadrupoles (‘Saturn rings’), axial octupoles (‘flowers’), linear quadrupoles (poles) and mixed multipole arrangements (‘two tone’), which represent just a few examples of the type of structure that can be built using this technique.

This work is motivated by the unexpected experimental observation that field gradients can control the alignment of nonmagnetic nanorods immersed inside magnetic fluids. In the presence of local field gradients, nanorods were observed to align perpendicular to the external field at low field strengths, but parallel to the external field at high field strengths. The switching behavior results from the competition between a preference to align with the external field (orientational potential energy) and preference to move into regions of minimum magnetic field (positional potential energy). A theoretical model is developed to explain this experimental behavior by investigating the statistics of nanorod alignment as a function of both the external uniform magnetic field strength and the local magnetic field variation above a periodic array of micromagnets. Computational phase diagrams are developed which indicate that the relative population of nanorods in parallel and perpendicular states can be adjusted through several control parameters. However, an energy barrier to rotation was discovered to influence the rate kinetics and restrict the utility of this assembly technique to nanorods which are slightly shorter than the micromagnet length. Experimental results concerning the orientation of nanorods inside magnetic fluid are also presented and shown to be in strong agreement with the theoretical work.

Magnetic separation is part of a vast subject dealing with manipulation of colloidal particles on the basis of their magnetic as well as other types of properties. This paper will review some physical fundamentals of this subject and summarize models of magnetic separation and manipulation that have been developed mostly over the last 30 years. Recent work focusing on the use of micro-systems in separation, manipulation and assembly of non-magnetic colloidal particles in magnetic fluids will be emphasized.

We introduce a method for transporting colloidal particles, large molecules, cells, and other materials across surfaces and for assembling them into highly regular patterns. In this method, nonmagnetic materials are manipulated by a fluid dispersion of magnetic nanoparticles. Manipulation of materials is guided by a program of magnetic information stored in a substrate. Dynamic control over the motion of nonmagnetic particles can be achieved by reprogramming the substrate magnetization on the fly. The unexpectedly large degree of control over particle motion can be used to manipulate large ensembles of particles in parallel, potentially with local control over particle trajectory.