Microscopic basis for pattern formation and anomalous transport in two-dimensional active gels

Active gels are a class of biologically-relevant material containing embedded agents that spontaneously generate forces acting on a sparse filament network. In vitro experiments of protein filaments and molecular motors have revealed a range of non- equilibrium pattern formation resulting from motor motion along filament tracks, and there are a number of hydrodynamic models purporting to describe such systems. Here we present results of extensive simulations designed to elucidate the microscopic basis underpinning macroscopic flow in active gels. Our numerical scheme includes thermal fluctuations in filament positions, excluded volume interactions, and filament elasticity in the form of bending and stretching modes. Motors are represented individually as bipolar springs governed by rate-based rules for attachment, detachment and unidirectional motion of motor heads along the filament contour. We systematically vary motor density and speed, and uncover parameter regions corresponding to unusual statics and dynamics which overlap but do not coincide. The anomalous statics arise at high motor densities and take the form of end-bound localized filament bundles for rapid motors, and extended clusters exhibiting enhanced small-wavenumber density fluctuations and power-law cluster-size distributions for slow, processive motors. Anomalous dynamics arise for slow, processive motors over a range of motor densities, and are most evident as superdiffusive mass transport, which we argue is the consequence of a form of effective self-propulsion resulting from the polar coupling between motors and filaments.Comment: 14 pages, 17 figures. Minor clarifications and updated/additional references. To appear in Soft Matte

Translational and rotational friction on a colloidal rod near a wall

We present particulate simulation results for translational and rotational friction components of a shish-kebab model of a colloidal rod with aspect ratio (length over diameter) $L/D = 10$ in the presence of a planar hard wall. Hydrodynamic interactions between rod and wall cause an overall enhancement of the friction tensor components. We find that the friction enhancements to reasonable approximation scale inversely linear with the closest distance $d$ between the rod surface and the wall, for $d$ in the range between $D/8$ and $L$. The dependence of the wall-induced friction on the angle $\theta$ between the long axis of the rod and the normal to the wall is studied and fitted with simple polynomials in $\cos \theta$.Comment: 8 pages, 8 figure

Mesoscale modeling of the rheology of pressure sensitive adhesives through inclusion of transient forces

For optimal application, pressure-sensitive adhesives must have rheological properties in between those of a viscoplastic solid and those of a viscoelastic liquid. Such adhesives can be produced by emulsion polymerisation, resulting in latex particles which are dispersed in water and contain long-chain acrylic polymers. When the emulsion is dried, the latex particles coalesce and an adhesive film is formed. The rheological properties of the dried samples are believed to be dominated by the interface regions between the original latex particles, but the relation between rheology and latex particle properties is poorly understood. In this paper we show that it is possible to describe the bulk rheology of a pressure-sensitive adhesive by means of a mesoscale simulation model. To reach experimental time and length scales, each latex particle is represented by just one simulated particle. The model is subjected to oscillatory shear flow and extensional flow. Simple order of magnitude estimates of the model parameters already lead to semi-quantitative agreement with experimental results. We show that inclusion of transient forces in the model, i.e. forces with memory of previous configurations, is essential to correctly predict the linear and nonlinear properties.Comment: 29 pages, 8 figure

Force calculation on walls and embedded particles in multiparticle collision dynamics simulations

Colloidal solutions posses a wide range of time and length scales, so that it is unfeasible to keep track of all of them within a single simulation. As a consequence some form of coarse-graining must be applied. In this work we use the Multi-Particle Collision Dynamics scheme. We describe a particular implementation of no-slip boundary conditions upon a solid surface, capable of providing correct force s on the solid bypassing the calculation of the velocity profile or the stre ss tensor in the fluid near the surface. As an application we measure the friction on a spherical particle, when it is placed in a bulk fluid and when it is confined in a slit. We show that the implementation of the no-slip boundary conditions leads to an enhanced Ensko g friction, which can be understood analytically. Because of the long-range nature of hydrodynamic interactions, the Stokes friction obtained from the simulations is sensitive of the simulation box size. We address this topic for the slit geometry, showing that that the dependence on the system size differs very much from what is expected in a 3D system, where periodic boundary conditions are used in all directions.Comment: To appear in Physical Review

Systematic coarse-graining of the dynamics of entangled polymer melts: the road from chemistry to rheology

For optimal processing and design of entangled polymeric materials it is important to establish a rigorous link between the detailed molecular composition of the polymer and the viscoelastic properties of the macroscopic melt. We review current and past computer simulation techniques and critically assess their ability to provide such a link between chemistry and rheology. We distinguish between two classes of coarse-graining levels, which we term coarse-grained molecular dynamics (CGMD) and coarse-grained stochastic dynamics (CGSD). In CGMD the coarse-grained beads are still relatively hard, thus automatically preventing bond crossing. This also implies an upper limit on the number of atoms that can be lumped together and therefore on the longest chain lengths that can be studied. To reach a higher degree of coarse-graining, in CGSD many more atoms are lumped together, leading to relatively soft beads. In that case friction and stochastic forces dominate the interactions, and actions must be undertaken to prevent bond crossing. We also review alternative methods that make use of the tube model of polymer dynamics, by obtaining the entanglement characteristics through a primitive path analysis and by simulation of a primitive chain network. We finally review super-coarse-grained methods in which an entire polymer is represented by a single particle, and comment on ways to include memory effects and transient forces.Comment: Topical review, 31 pages, 10 figure

Dynamic Response of Block Copolymer Wormlike Micelles to Shear Flow

The linear and non-linear dynamic response to an oscillatory shear flow of giant wormlike micelles consisting of Pb-Peo block copolymers is studied by means of Fourier transform rheology. Experiments are performed in the vicinity of the isotropic-nematic phase transition concentration, where the location of isotropic-nematic phase transition lines is determined independently. Strong shear-thinning behaviour is observed due to critical slowing down of orientational diffusion as a result of the vicinity of the isotropic- nematic spinodal. This severe shear-thinning behaviour is shown to result in gradient shear banding. Time-resolved Small angle neutron scattering experiments are used to obtain insight in the microscopic phenomena that underly the observed rheological response. An equation of motion for the order-parameter tensor and an expression of the stress tensor in terms of the order-parameter tensor are used to interpret the experimental data, both in the linear and non-linear regime. Scaling of the dynamic behaviour of the orientational order parameter and the stress is found when critical slowing down due to the vicinity of the isotropic-nematic spinodal is accounted for.Comment: Accepted by J. Phys.: Condens. Matter, CODEF II Special Issue. 20 pages, 9 figure

Dynamic Response of Block Copolymer Wormlike Micelles to Shear Flow

The linear and non-linear dynamic response to an oscillatory shear flow of giant wormlike micelles consisting of Pb-Peo block copolymers is studied by means of Fourier transform rheology. Experiments are performed in the vicinity of the isotropic-nematic phase transition concentration, where the location of isotropic-nematic phase transition lines is determined independently. Strong shear-thinning behaviour is observed due to critical slowing down of orientational diffusion as a result of the vicinity of the isotropic- nematic spinodal. This severe shear-thinning behaviour is shown to result in gradient shear banding. Time-resolved Small angle neutron scattering experiments are used to obtain insight in the microscopic phenomena that underly the observed rheological response. An equation of motion for the order-parameter tensor and an expression of the stress tensor in terms of the order-parameter tensor are used to interpret the experimental data, both in the linear and non-linear regime. Scaling of the dynamic behaviour of the orientational order parameter and the stress is found when critical slowing down due to the vicinity of the isotropic-nematic spinodal is accounted for.Comment: Accepted by J. Phys.: Condens. Matter, CODEF II Special Issue. 20 pages, 9 figure