No Arabic abstract
Recent studies of dynamic self-assembly in ferromagnetic colloids suspended in liquid-air or liquid-liquid interfaces revealed a rich variety of dynamic structures ranging from linear snakes to axisymmetric asters, which exhibit novel morphology of the magnetic ordering accompanied by large-scale hydrodynamic flows. Based on controlled experiments and first principle theory, we argue that the transition from snakes to asters is governed by the viscosity of the suspending liquid where less viscous liquids favor snakes and more viscous, asters. By obtaining analytic solutions of the time-averaged Navier-Stokes equations, we gain insights into the role of mean hydrodynamic flows and an overall balance of forces governing the self-assembly. Our results illustrate that the viscosity can be used to control the outcome of the dynamic self-assembly in magnetic colloidal suspensions.
We study DNA self-assembly and DNA computation using a coarse-grained DNA model within the directional dynamic bonding framework {[}C. Svaneborg, Comp. Phys. Comm. 183, 1793 (2012){]}. In our model, a single nucleotide or domain is represented by a single interaction site. Complementary sites can reversibly hybridize and dehybridize during a simulation. This bond dynamics induces a dynamics of the angular and dihedral bonds, that model the collective effects of chemical structure on the hybridization dynamics. We use the DNA model to perform simulations of the self-assembly kinetics of DNA tetrahedra, an icosahedron, as well as strand displacement operations used in DNA computation.
The Dynamic Monte Carlo (DMC) method is an established molecular simulation technique for the analysis of the dynamics in colloidal suspensions. An excellent alternative to Brownian Dynamics or Molecular Dynamics simulation, DMC is applicable to systems of spherical and/or anisotropic particles and to equilibrium or out-of-equilibrium processes. In this work, we present a theoretical and methodological framework to extend DMC to the study of heterogeneous systems, where the presence of an interface between coexisting phases introduces an additional element of complexity in determining the dynamic properties. In particular, we simulate a Lennard-Jones fluid at the liquid-vapor equilibrium and determine the diffusion coefficients in the bulk of each phase and across the interface. To test the validity of our DMC results, we also perform Brownian Dynamics simulations and unveil an excellent quantitative agreement between the two simulation techniques.
Dense particulate suspensions can not only increase their viscosity and shear thicken under external forcing, but also jam into a solid-like state that is fully reversible when the force is removed. An impact on the surface of a dense suspension can trigger this jamming process by generating a shear front that propagates into the bulk of the system. Tracking and visualizing such a front is difficult because suspensions are optically opaque and the front can propagate as fast as several meters per second. Recently, high-speed ultrasound imaging has been used to overcome this problem and extract two-dimensional sections of the flow field associated with jamming front propagation. Here we extend this method to reconstruct the three-dimensional flow field. This enables us to investigate the evolution of jamming fronts for which axisymmetry cannot be assumed, such as impact at angles tilted away from the normal to the free surface of the suspension. We find that sufficiently far from solid boundaries the resulting flow field is approximately identical to that generated by normal impact, but rotated and aligned with the angle of impact. However, once the front approaches the solid boundary at the bottom of the container, it generates a squeeze flow that deforms the front profile and causes jamming to proceed in a non-axisymmetric manner.
Dynamic particle-scale numerical simulations are used to show that the shear thickening observed in dense colloidal, or Brownian, suspensions is of a similar nature to that observed in non-colloidal suspensions, i.e., a stress-induced transition from a flow of lubricated near-contacting particles to a flow of a frictionally contacting network of particles. Abrupt (or discontinuous) shear thickening is found to be a geometric rather than hydrodynamic phenomenon; it stems from the strong sensitivity of the jamming volume fraction to the nature of contact forces between suspended particles. The thickening obtained in a colloidal suspension of purely hard frictional spheres is qualitatively similar to experimental observations. However, the agreement cannot be made quantitative with only hydrodynamics, frictional contacts and Brownian forces. Therefore the role of a short-range repulsive potential mimicking the stabilization of actual suspensions on the thickening is studied. The effects of Brownian and repulsive forces on the onset stress can be combined in an additive manner. The simulations including Brownian and stabilizing forces show excellent agreement with experimental data for the viscosity $eta$ and the second normal stress difference $N_2$.
An experimental system has been found recently, a coagulated CaCO3 suspension system, which shows very variable yield behaviour depending upon how it is tested and, specifically, at what rate it is sheared. At Peclet numbers Pe > 1 it behaves as a simple Herschel Bulkley liquid, whereas at Pe < 1 highly non-monotonic flow curves are seen. In controlled stress testing it shows hysteresis and shear banding and in the usual type of stress scan, used to measure flow curves in controlled stress mode routinely, it can show very erratic and irreproducible behaviour. All of these features will be attributed here to a dependence of the solid phase, or, yield stress, on the prevailing rate of shear at the yield point. Stress growth curves obtained from step strain-rate testing showed that this rate-dependence was a consequence of Peclet number dependent strain softening. At very low Pe, yield was cooperative and the yield strain was order-one, whereas as Pe approached unity, the yield strain reduced to that needed to break interparticle bonds, causing the yield stress to be greatly reduced. It is suspected that rate-dependent yield could well be the rule rather than the exception for cohesive suspensions more generally. If so, then the Herschel-Bulkley equation can usefully be generalized to read (in simple shear). The proposition that rate-dependent yield might be general for cohesive suspensions is amenable to critical experimental testing by a range of means and along lines suggested.