We report an investigation of the equilibrium and dynamic properties of polyelectrolyte solutions confined between platinum surfaces with a dynamic Surface Force Apparatus. The polyelectrolyte adsorbs on the surfaces in a dense compact layer bearing a surface charge in good agreement with the theoretical predictions. The flow of the solution on this charged adsorbed layer is probed over four decades of spatial scales and one decade of frequency by dynamic measurements. At distances larger than the hundredth of nanometers, the flow of the viscoelastic solution is well described by a partial slip boundary condition. We show that the wall slip is quantitatively described by an interfacial friction coefficient, according to the original Navier's formulation, and not by a slip length. At smaller distance the partial slip model overestimates the solution mobility, and we observe the presence of a low viscosity layer coating the surfaces. The viscosity and thickness of this boundary layer are directly resolved, and found to be independent on shear-rate, frequency, and confinement. We discuss the thickness of the low viscosity layer in terms of the structural length of the semi-dilute solution and the Debye length screening the adsorbed layer charge.
The structure and dynamics of a range of polystyrene sulphonate comb polyelectrolytes with well defined chain architectures were examined with static light scattering, dynamic light scattering, small angle neutron/X-ray scattering, particle tracking microrheology and diffusing wave spectroscopy. The chains adopted extended cylindrical conformations in dilute solutions. In semi-dilute solutions a universal behaviour was found for the correlation length (X) on the monomer concentration (c), X=(3.0/b)c^-0.47, independent of the comb architecture (b is the monomer size). The high frequency viscoel…
The modification of the boundary condition for polyelectrolyte adsorption on charged surface with short-ranged interaction is investigated under two regimes. For weakly charged Gaussian polymer in which the short-ranged attraction dominates, the boundary condition is the same as that of the neutral polymer adsorption. For highly charged polymer (compressed state) in which the electrostatic interaction dominates, the linear relationship (electrostatic boundary condition) between the surface monomer density and the surface charge density needs to be modified.
In this paper we study swimming of a model organism, the so-called Taylor's swimming sheet, in a viscoelastic fluid close to a solid boundary. This situation comprises natural habitats of many swimming microorganisms, and while previous investigations have considered the effects of both swimming next to a boundary and swimming in a viscoelastic fluid, seldom have both effects been considered simultaneously. We re-visit the small wave amplitude result obtained by Elfring and Lauga (Gwynn J. Elfring and Eric Lauga, in Saverio E. Spagnolie, editor, Complex Fluids in Biological Systems, Springer N…
We present mesoscopic DPD-simulations of polyelectrolyte electrophoresis in confined nanogeometries, for varying salt concentration and surface slip conditions. Special attention is given to the influence of electroosmotic flow (EOF) on the migration of the polyelectrolyte. The effective polyelectrolyte mobility is found to depend strongly on the boundary properties, i.e., the slip length and the width of the electric double layer. Analytic expressions for the electroosmotic mobility and the total mobility are derived which are in good agreement with the numerical results. The relevant quantit…
For a tailored functionalization of cellulose based papers, the interaction between paper fibers and functional additives have to be understood. Planar cellulose surfaces present a suitable model system for studying the binding of additives. In this work, polyelectrolyte multilayers (PEMs) as model surfaces are prepared by alternating dip coating of the negatively charged cellulose derivate carboxymethyl cellulose and a polycation, either PDADMAC or chitosan. The varied parameters of the PEM formation are the polyelectrolyte concentrations and pH (pH=2-6). Both PEM systems exhibit an exponenti…
The behavior of a polyelectrolyte adsorbed on a charged substrate of high-dielectric constant is studied by both Monte-Carlo simulation and analytical methods. It is found that in a low enough ionic strength medium, the adsorption transition is first-order where the substrate surface charge still keeps repulsive. The monomer density at the adsorbed surface is identified as the order parameter. It follows a linear relation with substrate surface charge density because of the electrostatic boundary condition at the charged surface. During the transition, the adsorption layer thickness remains fi…
Most biological fluids are viscoelastic, meaning that they have elastic properties in addition to the dissipative properties found in Newtonian fluids. Computational models can help us understand viscoelastic flow, but are often limited in how they deal with complex flow geometries and suspended particles. Here, we present a lattice Boltzmann solver for Oldroyd-B fluids that can handle arbitrarily-shaped fixed and moving boundary conditions, which makes it ideally suited for the simulation of confined colloidal suspensions. We validate our method using several standard rheological setups, and …
To elucidate the key factor for the quantitative prediction of the shear-thickening in suspensions in viscoelastic fluids, direct numerical simulations of many-particle suspensions in a multi-mode Oldroyd-B fluid are performed using the smoothed profile method. Suspension flow under simple shear flow is solved under periodic boundary conditions by using Lees--Edwards boundary conditions for particle dynamics and a time-dependent oblique coordinate system that evolves with mean shear flow for fluid dynamics. Semi-dilute many-particle suspensions up to a particle volume fraction of 0.1 are inves…
The actin cytoskeleton of adherent tissue cells often condenses into filament bundles contracted by myosin motors, so-called stress fibers, which play a crucial role in the mechanical interaction of cells with their environment. Stress fibers are usually attached to their environment at the endpoints, but possibly also along their whole length. We introduce a theoretical model for such contractile filament bundles which combines passive viscoelasticity with active contractility. The model equations are solved analytically for two different types of boundary conditions. A free boundary correspo…
The electric double layer (EDL) that forms at the interface between a polyelectrolyte gel and a salt bath is studied using asymptotic and numerical methods. Specifically, matched asymptotic expansions, based on the smallness of the Debye length relative to the typical gel dimensions, are used to construct solutions of the governing equations and derive electroneutral models with consistent jump conditions across the gel-bath interface. A general approach for solving the equations of incompressible nonlinear elasticity in a curved boundary layer is developed and used to resolve the gel mechanic…
We present experimental evidence of global viscoelastic flow transitions in 2:1, 8:1 and 32:1 planar contractions under inertia-less conditions. Light sheet visualization and laser Doppler velocimetry techniques are used to probe spatial structure and time scales associated with the onset of these instabilities. The results are reported in terms of critical Weissenberg numbers characterizing the fluid flow rates. For a given contraction ratio and polymer fluid, a two-dimensional, steady flow with converging streamlines transitions to a two-dimensional pattern with diverging streamlines beyond …
Using a dynamic Surface Force Apparatus, we demonstrate that the notion of slip length used to describe the boundary flow of simple liquids, is not appropriate for viscoelastic liquids. Rather, the appropriate description lies in the original Navier's partial slip boundary condition, formulated in terms of an interfacial friction coefficient. We establish an exact analytical expression to extract the interfacial friction coefficient from oscillatory drainage forces between a sphere and a plane, suitable for dynamic SFA or Atomic Force Microscopy non-contact measurements. We use this model to i…
The linear (Winkler) foundation is a simple model widely used for decades to account for the surface response of elastic bodies. It models the response as purely local, linear, and perpendicular to the surface. We extend this model to the case where the foundation is made of a structured material such as a polymer network, which has characteristic scales of length and time. We use the two-fluid model of viscoelastic structured materials to treat a film of finite thickness, supported on a rigid solid and subjected to a concentrated normal force at its free surface. We obtain the foundation modu…
Finite difference method in prolate spheroidal coordinates for freely suspended spheroidal particles in linear flows of viscous and viscoelastic fluids
We investigated the viscoelastic properties of colloid-polymer mixtures at intermediate colloid volume fraction and varying polymer concentrations, thereby tuning the attractive interactions. Within the examined range of polymer concentrations, the samples ranged from fluids to gels. Already in the liquid phase the viscoelastic properties significantly changed when approaching the gelation boundary, indicating the formation of clusters and transient networks. This is supported by an increasing correlation length of the density fluctuations, observed by static light scattering and microscopy. A…
The spreading of liquid drops on soft substrates is extremely slow, owing to strong viscoelastic dissipation inside the solid. A detailed understanding of the spreading dynamics has remained elusive, partly owing to the difficulty in quantifying the strong viscoelastic deformations below the contact line that determine the shape of moving wetting ridges. Here we present direct experimental visualisations of the dynamic wetting ridge, complemented with measurements of the liquid contact angle. It is observed that the wetting ridge exhibits a rotation that follows exactly the dynamic liquid cont…
We find three types of steady solutions and remarkable flow pattern transitions between them in a two-dimensional wavy-walled channel for low to moderate Reynolds (Re) and Weissenberg (Wi) numbers using direct numerical simulations with spectral element method. The solutions are called "convective", "transition", and "elastic" in ascending order of Wi. In the convective region in the Re-Wi parameter space, the convective effect and the pressure gradient balance on average. As Wi increases, the elastic effect becomes suddenly comparable and the first transition sets in. Through the transition, …
In order to investigate the rheological properties of viscoelastic fluids by mesoscopic hydrodynamics methods, we develop a multi-particle collision dynamics (MPC) model for a fluid of harmonic dumbbells. The algorithm consists of alternating streaming and collision steps. The advantage of the harmonic interactions is that the integration of the equations of motion in the streaming step can be performed analytically. Therefore, the algorithm is computationally as efficient as the original MPC algorithm for Newtonian fluids. The collision step is the same as in the original MPC method. All part…
We study shear banding flows in models of wormlike micelles or polymer solutions, and explore the effects of different boundary conditions for the viscoelastic stress. These are needed because the equations of motion are inherently non-local and include ``diffusive'' or square-gradient terms. Using the diffusive Johnson-Segalman model and a variant of the Rolie-Poly model for entangled micelles or polymer solutions, we study the interplay between different boundary conditions and the intrinsic stress gradient imposed by the flow geometry. We consider prescribed gradient (Neumann) or value (Dir…
