Pattern formation of dipolar colloids in rotating fields: layering and synchronization

We report Brownian dynamics (BD) simulation and theoretical results for a system of spherical colloidal particles with permanent dipole moments in a rotating magnetic field. Performing simulations at a fixed packing fraction and dipole coupling parameter, we construct a full non-equilibrium phase diagram as a function of the driving frequency (omega(0)) and field strength (B-0). This diagram contains both synchronized states, where the individual particles follow the field with (on average) constant phase difference, and asynchronous states. The synchronization is accompanied by layer formation, i.e., by spatial symmetry-breaking, similar to systems of induced dipoles in rotating fields. In the permanent dipole case, however, too large omega(0) yields a breakdown of layering, supplemented by complex changes of the single-particle rotational dynamics from synchronous to asynchronous behavior. We show that the limit frequencies omega(c) can be well described as a bifurcation in the nonlinear equation of motion of a single-particle rotating in a viscous medium. Finally, we present a simple density functional theory, which describes the emergence of layers in perfectly synchronized states as an equilibrium phase transition.