123 research outputs found
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) 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
between the rod surface and the wall, for in the range between and
. The dependence of the wall-induced friction on the angle between
the long axis of the rod and the normal to the wall is studied and fitted with
simple polynomials in .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
Interfaces between a saturated aqueous urea solution and crystalline urea:A molecular dynamics study
General weak segregation theory with an application to monodisperse semi-flexible diblock copolymers
A general theory has been developed for a polydisperse semi-flexible multi-block copolymer melt. Using the Bawendi-Freed approach to model semi-flexible chains, an expression for the Landau free energy is derived in the weak segregation regime, which includes density and orientation order-parameters. The orientation order-parameter is described in the smectic phase and in more complicated structures, such as the hexagonal phase. The Landau free energy contains contributions of two kinds of interactions. The first kind is the Flory-Huggins interaction, which describes the incompatibility of chemically different blocks and may induce microphase separation. The second kind is the Maier-Saupe interaction, which may induce nematic ordering. In the framework of the weak segregation limit, the Landau theory allows us to predict phase structures in the melt as a function of the composition, persistence length, and the strength of the Flory-Huggins and Maier-Saupe interaction. The general theory is applied to a simple system of monodisperse semi-flexible diblock copolymers. In several phase diagrams, a number of possible phase structures are predicted, such as the bcc, hexagonal, smectic-A, smectic-C, and nematic phase. The influence of the Maier-Saupe interaction on the microphase structure is thoroughly discussed.</p
Non-monotonic Soret coefficients of aqueous LiCl solutions with varying concentrations
We investigate the thermodiffusive properties of aqueous solutions of lithium chloride, using thermal diffusion forced Rayleigh scattering in a concentration range of 0.5-2 mole per kg of solvent and a temperature range of 5 to 45 °C. All solutions exhibit non-monotonic variations of the Soret coefficient ST with a concentration exhibiting a minimum at about one mole per kg of solvent. The depth of the minimum decreases with increasing temperature and shifts slightly towards higher concentrations. We compare the experimental data with published data and apply a recent model based on overlapping hydration shells. Additionally, we calculate the ratio of the phenomenological Onsager coefficients using our experimental results and published data to calculate the thermodynamic factor. Simple linear, quadratic and exponential functions can be used to describe this ratio accurately, and together with the thermodynamic factors, the experimental Soret coefficients can be reproduced. The main conclusion from this analysis is that the minimum of the Soret coefficients results from a maximum in the thermodynamic factor, which appears itself at concentrations far below the experimental concentrations. Only after multiplication by the (negative) monotonous Onsager ratio does the minimum move into the experimental concentration window.</p
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
- …