Low temperature structural transitions in dipolar hard spheres: the influence on magnetic properties

We investigate the structural chain-to-ring transition at low temperature in a gas of dipolar hard spheres (DRS). Due to the weakening of entropic contribution, ring formation becomes noticeable when the effective dipole-dipole magnetic interaction increases, It results in the redistribution of particles from usually observed flexible chains into flexible rings. The concentration (rho) of DI-IS plays a crucial part in this transition: at a very low rho only chains and rings are observed, whereas even a slight increase of the volume fraction leads to the formation of branched or defect structures. As a result, the fraction of DHS aggregated in defect-free rings turns out to be a non-monotonic function of rho. The average ring size is found to be a slower increasing function of rho when compared Lo that of chains. Both theory and computer simulations confirm the dramatic influence of the ring formation on the rho-dependence of the initial magnetic susceptibility (chi) when the temperature decreases. The rings clue to their zero total dipole moment are irresponsive to a weak magnetic field and drive to the strong decrease of the initial magnetic susceptibility. (C) 2014 Elsevier B.V. All rights reserved.

Temperature-induced structural transitions in self-assembling magnetic nanocolloids

With the help of a unique combination of density functional theory and computer simulations, we discover two possible scenarios, depending on concentration, for the hierarchical self-assembly of magnetic nanoparticles on cooling. We show that typically considered low temperature clusters, i.e. defect-free chains and rings, merge into more complex branched structures through only three types of defects: four-way X junctions, three-way Y junctions and two-way Z junctions. Our accurate calculations reveal the predominance of weakly magnetically responsive rings cross-linked by X defects at the lowest temperatures. We thus provide a strategy to fine-tune magnetic and thermodynamic responses of magnetic nanocolloids to be used in medical and microfluidics applications.