No Arabic abstract
We report that binary dispersions of like-charged colloidal particles with large charge asymmetry but similar size exhibit phase separation into crystal and fluid phases under very low salt conditions. This is unexpected because the effective colloid-colloid pair interactions are accurately described by a Yukawa model which is stable to demixing. We show that colloid-ion interactions provide an energetic driving force for phase separation, which is initiated by crystallization of one species.
A theoretical study of the structure formation observed very recently [Phys. Rev. Lett. 90, 128303 (2003)] in binary colloids is presented. In our model solely the dipole-dipole interaction of the particles is considered, electrohidrodynamic effects are excluded. Based on molecular dynamics simulations and analytic calculations we show that the total concentration of the particles, the relative concentration and the relative dipole moment of the components determine the structure of the colloid. At low concentrations the kinetic aggregation of particles results in fractal structures which show a crossover behavior when increasing the concentration. At high concentration various lattice structures are obtained in a good agreement with experiments.
As a generic model system of an asymmetric binary fluid mixture, hexadecane dissolved in carbon dioxide is considered, using a coarse-grained bead-spring model for the short polymer, and a simple spherical particle with Lennard-Jones interactions for the carbon dioxide molecules. In previous work, it has been shown that this model reproduces the real phase diagram reasonable well, and also the initial stages of spinodal decomposition in the bulk following a sudden expansion of the system could be studied. Using the parallelized simulation package ESPResSo on a multiprocessor supercomputer, phase separation of thin fluid films confined between parallel walls that are repulsive for both types of molecules are simulated in a rather large system (1356 x 1356 x 67.8 A^3, corresponding to about 3.2 million atoms). Following the sudden system expansion, a complicated interplay between phase separation in the directions perpendicular and parallel to the walls is found: in the early stages the hexadecane molecules accumulate mostly in the center of the slit pore, but as the coarsening of the structure in the parallel direction proceeds, the inhomogeneity in the perpendicular direction gets much reduced. Studying then the structure factors and correlation functions at fixed distances from the wall, the densities are essentially not conserved at these distances, and hence the behavior differs strongly from spinodal decomposition in the bulk. Some of the characteristic lengths show a nonmonotonic variation with time, and simple coarsening described by power-law growth is only observed if the domain sizes are much larger than the film thickness.
Phase separation of binary fluids quenched by contact with cold external walls is considered. Navier-Stokes, convection-diffusion, and energy equations are solved by lattice Boltzmann method coupled with finite-difference schemes. At high viscosity, different morphologies are observed by varying the thermal diffusivity. In the range of thermal diffusivities with domains growing parallel to the walls, temperature and phase separation fronts propagate towards the inner of the system with power-law behavior. At low viscosity hydrodynamics favors rounded shapes, and complex patterns with different lengthscales appear. Off-symmetrical systems behave similarly but with more ordered configurations.
Materials undergoing both phase separation and chemical reactions (defined here as all processes that change particle type or number) form an important class of non-equilibrium systems. Examples range from suspensions of self-propelled bacteria with birth-death dynamics, to bio-molecular condensates, or membraneless organelles, within cells. In contrast to their passive counterparts, such systems have conserved and non-conserved dynamics that do not, in general, derive from a shared free energy. This mismatch breaks time-reversal symmetry and leads to new types of dynamical competition that are absent in or near equilibrium. We construct a canonical scalar field theory to describe such systems, with conserved and non-conserved dynamics obeying Model B and Model A respectively (in the Hohenberg-Halperin classification), chosen such that the two free energies involved are incompatible. The resulting minimal model is shown to capture the various phenomenologies reported previously for more complicated models with the same physical ingredients, including microphase separation, limit cycles and droplet splitting. We find a low-dimensional subspace of parameters for which time-reversal symmetry is accidentally recovered, and show that here the dynamics of the order parameter field (but not its conserved current) is exactly the same as an equilibrium system in which microphase separation is caused by long-range attractive interactions.
We present a numerical study of the phase behavior of repulsively interacting active polar particles that align their active velocities nematically. The amplitude of the active velocity, and the noise in its orientational alignment control the active nature of the system. At high values of orientational noise, the structural fluid undergoes a continuous nematic-isotropic transition in active orientation. This transition is well separated from an active phase separation, characterized by the formation of high density hexatic clusters, observed at lower noise strengths. With increasing activity, the system undergoes a re-entrant fluid-phase separation-fluid transition. The phase coexistence at low activity can be understood in terms of motility induced phase separation. In contrast, the re-melting of hexatic clusters, and the collective motion at low orientational noise are dominated by flocking behavior. At high activity, sliding and jamming of polar sub-clusters, formation of grain boundaries, lane formation, and subsequent fragmentation of the polar patches mediate remelting.