Phase separation dynamics in a symmetric binary mixture of ultrasoft particles.

Phase separation plays a key role in determining the self-assembly of biological and soft-matter systems. In biological systems, liquid-liquid phase separation inside a cell leads to the formation of various macromolecular aggregates. The interaction among these aggregates is soft, i.e., they can significantly overlap at a small energy cost. From a computer simulation point of view, these complex macromolecular aggregates are generally modeled by soft particles. The effective interaction between two particles is defined via the generalized exponential model of index n, with n = 4. Here, using molecular dynamics simulations, we study the phase separation dynamics of a size-symmetric binary mixture of ultrasoft particles. We find that when the mixture is quenched to a temperature below the critical temperature, the two components spontaneously start to separate. Domains of the two components form, and the equal-time order parameter reveals that the domain sizes grow with time in a power-law manner with an exponent of 1/3, which is consistent with the Lifshitz-Slyozov law for conserved systems. Furthermore, the static structure factor shows a power-law decay with an exponent of 4, consistent with the Porod law.

On the yielding of a point-defect-rich model crystal under shear: insights from molecular dynamics simulations.

In real crystals and at finite temperatures point defects are inevitable. Under shear their dynamics severely influence the mechanical properties of these crystals, giving rise to non-linear effects, such as ductility. In an effort to elucidate the complex behavior of crystals under plastic deformation it is crucial to explore and to understand the interplay between the timescale related to the equilibrium point-defect diffusion and the shear-induced timescale. Based on extensive non-equilibrium molecular dynamics simulations we present a detailed investigation on the yielding behavior of cluster crystals, an archetypical model for a defect-rich crystal: in such a system clusters of overlapping particles occupy the lattice sites of a regular (FCC) structure. In equilibrium particles diffuse via site-to-site hopping while maintaining the crystalline structure intact. We investigate these cluster crystals at a fixed density and at different temperatures where the system remains in the FCC structure: temperature allows us to vary the diffusion timescale appropriately. We then expose the crystal to shear, thereby choosing shear rates which cover timescales that are both higher and lower than the equilibrium diffusion timescales. We investigate the macroscopic and microscopic response of our cluster crystal to shear and find that the yielding scenario of such a system does not rely on the diffusion of the particles - it is rather related to the plastic deformation of the underlying crystalline structure. The local bond order parameters and the measurement of local angles between neighboring clusters confirm the cooperative movement of the clusters close to the yield point. Performing complementary, related simulations for an FCC crystal formed by harshly repulsive particles reveals similarities in the yielding behavior between both systems. Still we find that the diffusion of particles does influence characteristic features in the cluster crystal, such as a less prominent increase of order parameters close to the yield point. Our simulations provide for the first time an insight into the role of the diffusion of defects in the yielding behavior of a defect-rich crystal under shear. These observations will thus be helpful in the development of theories for the plastic deformation of defect-rich crystals.

Flow heterogeneities in supercooled liquids and glasses under shear.

Using extensive nonequilibrium molecular dynamics simulations, we investigate a glass-forming binary Lennard-Jones mixture under shear. Both supercooled liquids and glasses are considered. Our focus is on the characterization of inhomogeneous flow patterns such as shear bands that appear as a transient response to the external shear. For the supercooled liquids, we analyze the crossover from Newtonian to non-Newtonian behavior with increasing shear rate γ[over ̇]. Above a critical shear rate γ[over ̇]_{c} where a non-Newtonian response sets in, the transient dynamics are associated with the occurrence of short-lived vertical shear bands, i.e., bands of high mobility that form perpendicular to the flow direction. In the glass states, long-lived horizontal shear bands, i.e., bands of high mobility parallel to the flow direction, are observed in addition to vertical ones. The systems with shear bands are characterized in terms of mobility maps, stress-strain relations, mean-squared displacements, and (local) potential energies. The initial formation of a horizontal shear band provides an efficient stress release, corresponds to a local minimum of the potential energy, and is followed by a slow broadening of the band towards the homogeneously flowing fluid in the steady state. Whether a horizontal or a vertical shear band forms cannot be predicted from the initial undeformed sample. Furthermore, we show that with increasing system size, the probability for the occurrence of horizontal shear bands increases.

Steady-state rheology and structure of soft hybrid mixtures of liquid crystals and magnetic nanoparticles.

Using non-equilibrium molecular dynamics simulations, we study the rheology of a model hybrid mixture of liquid crystals (LCs) and dipolar soft spheres (DSS) representing magnetic nanoparticles. The bulk isotropic LC-DSS mixture is sheared with different shear rates using Lees-Edwards periodic boundary conditions. The steady-state rheological properties and the effect of the shear on the microstructure of the mixture are studied for different strengths of the dipolar coupling, λ, among the DSS. We find that at large shear rates, the mixture shows a shear-thinning behavior for all considered values of λ. At low and intermediate values of λ, a crossover from Newtonian to non-Newtonian behavior is observed as the rate of applied shear is increased. In contrast, for large values of λ, such a crossover is not observed within the range of shear rates considered. Also, the extent of the non-Newtonian regime increases as λ is increased. These features can be understood via the shear-induced changes of the microstructure. In particular, the LCs display a shear-induced isotropic-to-nematic transition at large shear rates with a shear-rate dependent degree of nematic ordering. The DSS show a shear-induced nematic ordering only for large values of λ, where the particles self-assemble into chains. Moreover, at large λ and low shear rates, our simulations indicate that the DSS form ferromagnetic domains.

Non-monotonic response of a sheared magnetic liquid crystal to a continuously increasing external field.

Utilizing molecular dynamics simulations, we report a nonmonotonic dependence of the shear stress on the strength of a continuously increasing (i.e., time-varying) external magnetic field (H) in a liquid-crystalline mixture of magnetic and nonmagnetic anisotropic particles. We relate the origin of this nonmonotonicity of the transient dynamics to the competing effects of particle alignment along the shear-induced direction, on the one hand, and the magnetic field direction, on the other hand. To isolate the role of these competing effects, we consider a two-component mixture composed of particles with effectively identical steric interactions, where the orientations of a small fraction, i.e., the magnetic ones, are coupled to the external magnetic field. By increasing H from zero, the orientations of the magnetic particles show a Fréederickz-like transition and eventually start deviating from the shear-induced orientation, leading to an increase in shear stress. Upon further increase of H, a demixing of the magnetic particles from the nonmagnetic ones occurs, which leads to a drop in shear stress, hence creating a nonmonotonic response to H. Unlike the equilibrium demixing phenomena reported in previous studies, the demixing observed here is neither due to size-polydispersity nor due to a wall-induced nematic transition. Based on a simplified Onsager analysis, we rather argue that it occurs solely due to packing entropy of particles with different shear- or magnetic-field-induced orientations.

Anomalous transport of magnetic colloids in a liquid crystal-magnetic colloid mixture.

We report an extensive molecular dynamics study on the translational dynamics of a hybrid system composed of dipolar soft spheres (DSS), representing ferromagnetic particles, suspended in a liquid crystal (LC) matrix. We observe that the LC matrix strongly modifies the dynamics of the DSS. In the isotropic regime, the DSS show a crossover from subdiffusive to normal diffusive behavior at long times, with an increase of the subdiffusive regime as the dipolar coupling strength is increased. In the nematic regime, the LC matrix, due to the collective reorientation of LC particles, imposes a cylindrical confinement on the DSS chains. This leads to a diffusive dynamics of DSS along the nematic director and a subdiffusive dynamics (with an exponent of ∼0.5) in the perpendicular direction. The confinement provided by the LC matrix is also reflected by the oscillatory behavior of the components of the velocity autocorrelation function of the DSS in the nematic phase.

Non-Porod behavior in systems with rough morphologies.

Many experiments yield multi-scale morphologies which are smooth on some length scales and fractal on others. Accurate statements about morphological properties, e.g., roughness exponent, fractal dimension, domain size, interfacial width, etc. are obtained from the correlation function and structure factor. In this paper, we present structure factor data for two systems: (a) droplet-in-droplet morphologies of double-phase-separating mixtures; and (b) ground-state morphologies in dilute anti-ferromagnets. An important characteristic of the scattering data is a non-Porod tail, which is associated with scattering off rough domains and interfaces.

Ground-state morphologies in the random-field Ising model: scaling properties and non-Porod behavior.

We use a computationally efficient graph-cut method (GCM) to obtain the ground-state morphologies (at zero temperature) of the random-field Ising model in d=2,3. The GCM enables us to obtain comprehensive numerical results on large-scale systems. We analyze the morphologies by computing correlation functions and structure factors. These quantities enable us to precisely evaluate characteristic properties, e.g., domain sizes, scaling functions, roughness exponents, fractal dimensions, etc.