SearcharxivSearch

arXiv subjects

P. D. Olmsted

Publications and source records attributed to P. D. Olmsted.

16 recordsLinked to original sources

Perspectives on the viscoelasticity and flow behavior of entangled linear and branched polymers

We briefly review the recent advances in the rheology of entangled polymers and identify emerging research trends and outstanding challenges, especially with respect to branched polymers. Emphasis is placed on the role of well-characterized model systems, as well as the synergy of synthesis-characterization, rheometry and modeling/simulations. The theoretical framework for understanding the observed linear and nonlinear rheological phenomena is the tube model which is critically assessed in view of its successes and shortcomings, whereas alternative approaches are briefly discussed. Finally, intriguing experimental findings and controversial issues that merit consistent explanation, such as shear banding instabilities, multiple stress overshoots in transient simple shear and enhanced steady-state elongational viscosity in polymer solutions, are discussed, whereas future directions such as branch point dynamics and anisotropic monomeric friction are outlined.

cond-mat.soft

Dynamics of an asymmetric bilayer lipid membrane in a viscous solvent

Bilayer lipid membranes (BLMs) are an essential component of many biological systems, forming a functional barrier between the cell and the surrounding environment. When the membrane relaxes from a structural perturbation, the dynamics of the relaxation depends on the bilayer structure. We present a model of a BLM in a viscous solvent, including an explicit description of a 'thick' membrane, where the fluctuations in the thickness of a monolayer leaflet are coupled to changes in the lipid density within that monolayer. We find dispersion relations describing three intuitive forms of bilayer motion, including a mode describing motion of the intermonolayer surface not noted previously in the literature. Two intrinsic length scales emerge that help characterise the dynamics; the well known Saffman-Delbruck length and another, $\ell_r$, resulting from the intermonolayer friction. The framework also allows for asymmetry in the BLM parameters between the monolayer leaflets, which is found to couple dynamic modes of bilayer motion.

cond-mat.soft

Transient shear banding in entangled polymers: a study using the Rolie-Poly model

Spatially inhomogeneous shear flow occurs in entangled polymer solutions, both as steady state shear banding and transiently after a large step strain or during start up to a steady uniform shear rate. Steady state shear banding is a hallmark of models with a non-monotonic constitutive relation between total shear stress and applied shear rate, but transient banding is sometimes seen in fluids that do not shear band at steady state. We model this behavior using the diffusive Rolie-Poly model in a Newtonian solvent, whose constitutive behavior can be monotonic or non-monotonic depending on the degree of convected constraint release (CCR). We study monotonic constitutive behaviour. Linear stability analysis of start up to a sufficiently high shear rate shows that spatial fluctuations are unstable at early times. There is a strong correlation between this instability and the negative slope of the (time dependent) constitutive curve. If the time integral of the most unstable eigenvalue is sufficiently large then the system exhibits transient shear bands that later vanish in steady state. We show how perturbations, due to fluctuations or the inhomogeneous stresses, can trigger this instability. This transient behavior is similar to recent observations in entangled polymer solutions

cond-mat.soft

Adams and Olmsted Reply to comment on article "A non-monotonic constitutive model is not necessary to obtain shear banding phenomena in entangled polymer solution" [Phys. Rev. Lett. 102, 067801 (2009), arXiv:0805.0679]

Wang [Phys. Rev. Lett. 103, 219801 (2009)] makes the following points about our Letter [Phys. Rev. Lett. 102, 067801 (2009), arXiv:0805.0679]: (1) He infers that, "contrary to its title, shear banding emerged from monotonic curves only if there was a stress gradient", and he points out that nonquiescent relaxation was found (experimentally) after step strain in geometries without a stress gradient. (2) He disagrees with the values of the parameters we used. (3) In some recent experiments the flow was homogeneous after cessation of step strain, and only subsequently developed nonquiescent macroscopic motion. We only showed step strains that developed an inhomogeneity before cessation of flow. In this reply we address these points.

cond-mat.soft

Statistical mechanics far from equilibrium: prediction and test for a sheared system

We report the complete statistical treatment of a system of particles interacting via Newtonian forces in continuous boundary-driven flow, far from equilibrium. By numerically time-stepping the force-balance equations of a model fluid we measure occupancies and transition rates in simulation. The high-shear-rate simulation data verify the invariant quantities predicted by our statistical theory, thus demonstrating that a class of non-equilibrium steady states of matter, namely sheared complex fluids, is amenable to statistical treatment from first principles.

cond-mat.stat-mech

Two-dimensional perturbations in a scalar model for shear banding

We present an analytical study of a toy model for shear banding, without normal stresses, which uses a piecewise linear approximation to the flow curve (shear stress as a function of shear rate). This model exhibits multiple stationary states, one of which is linearly stable against general two-dimensional perturbations. This is in contrast to analogous results for the Johnson-Segalman model, which includes normal stresses, and which has been reported to be linearly unstable for general two-dimensional perturbations. This strongly suggests that the linear instabilities found in the Johnson-Segalman can be attributed to normal stress effects.

cond-mat.soft

A non-monotonic constitutive model is not necessary to obtain shear banding phenomena in entangled polymer solutions

In 1975 Doi and Edwards predicted that entangled polymer melts and solutions can have a constitutive instability, signified by a decreasing stress for shear rates greater than the inverse of the reptation time. Experiments did not support this, and more sophisticated theories incorporated Marrucci's idea (1996) of removing constraints by advection; this produced a monotonically increasing stress and thus stable constitutive behavior. Recent experiments have suggested that entangled polymer solutions may possess a constitutive instability after all, and have led some workers to question the validity of existing constitutive models. In this Letter we use a simple modern constitutive model for entangled polymers, the non-stretching Rolie-Poly model with an added solvent viscosity, and show that (1) instability and shear banding is captured within this simple class of models; (2) shear banding phenomena is observable for weakly stable fluids in flow geometries that impose a sufficiently inhomogeneous total shear stress; (3) transient phenomena can possess inhomogeneities that resemble shear banding, even for weakly stable fluids. Many of these results are model-independent.

cond-mat.soft

Validation of the Jarzynski relation for a system with strong thermal coupling: an isothermal ideal gas model

We revisit the paradigm of an ideal gas under isothermal conditions. A moving piston performs work on an ideal gas in a container that is strongly coupled to a heat reservoir. The thermal coupling is modelled by stochastic scattering at the boundaries. In contrast to recent studies of an adiabatic ideal gas with a piston [R.C. Lua and A.Y. Grosberg, \textit{J. Phys. Chem. B} 109, 6805 (2005); I. Bena et al., \textit{Europhys. Lett.} 71, 879 (2005)], container and piston stay in contact with the heat bath during the work process. Under this condition the heat reservoir as well as the system depend on the work parameter $λ$ and microscopic reversibility is broken for a moving piston. Our model is thus not included in the class of systems for which the non-equilibrium work theorem has been derived rigorously either by Hamiltonian [C. Jarzynski, \textit{J. Stat. Mech.} P09005 (2004)] or stochastic methods [G.E. Crooks, \textit{J. Stat. Phys.} 90, 1481 (1998)]. Nevertheless the validity of the non-equilibrium work theorem is confirmed both numerically for a wide range of parameter values and analytically in the limit of a very fast moving piston, i.e. in the far non-equilibrium regime.

cond-mat.stat-mech

The interplay between boundary conditions and flow geometries in shear banding: hysteresis, band configurations, and surface transitions

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 (Dirichlet) of the viscoelastic stress tensor at the boundary, as well as mixed boundary conditions in which an anchoring strength competes with the gradient contribution to the stress dynamics. We find that hysteresis during shear rate sweeps is suppressed if the boundary conditions favor the state that is induced by the sweep. For example, if the boundaries favor the high shear rate phase then hysteresis is suppressed at the low shear rate edges of the stress plateau. If the boundaries favor the low shear rate state, then the high shear rate band can lie in the center of the flow cell, leading to a three-band configuration. Sufficiently strong stress gradients due to curved flow geometries, such as that of cylindrical Couette flow, can convert this to a two-band state by forcing the high shear rate phase against the wall of higher stress, and can suppress the hysteresis loop observed during a shear rate sweep.

cond-mat.soft

Equilibrium Onions?

We demonstrate the possibility of a stable equilibrium multi-lamellar (``onion'') phase in pure lamellar systems (no excess solvent) due to a sufficiently negative Gaussian curvature modulus. The onion phase is stabilized by non-linear elastic moduli coupled to a polydisperse size distribution (Apollonian packing) to allow space-filling without appreciable elastic distortion. This model is compared to experiments on copolymer-decorated lamellar surfactant systems, with reasonable qualitative agreement.

cond-mat.soft

Timescales in shear banding of wormlike micelles

We show the existence of three well defined time scales in the dynamics of wormlike micelles after a step between two shear rates on the stress plateau. These time scales are compatible with the presence of a structured interface between bands of different viscosities and correspond to the isotropic band destabilization during the stress overshoot, reconstruction of the interface after the overshoot and travel of a fully formed interface. The last stage can be used to estimate a stress diffusion coefficient.

cond-mat.mtrl-sci

Instability of Myelin Tubes under Dehydration: deswelling of layered cylindrical structures

We report experimental observations of an undulational instability of myelin figures. Motivated by this, we examine theoretically the deformation and possible instability of concentric, cylindrical, multi-lamellar membrane structures. Under conditions of osmotic stress (swelling or dehydration), we find a stable, deformed state in which the layer deformation is given by δR ~ r^{\sqrt{B_A/(hB)}}, where B_A is the area compression modulus, B is the inter-layer compression modulus, and h is the repeat distance of layers. Also, above a finite threshold of dehydration (or osmotic stress), we find that the system becomes unstable to undulations, first with a characteristic wavelength of order \sqrt{xi d_0}, where xi is the standard smectic penetration depth and d_0 is the thickness of dehydrated region.

cond-mat.soft

A Minimal Model for Vorticity and Gradient Banding in Complex Fluids

A general phenomenological reaction-diffusion model for flow-induced phase transitions in complex fluids is presented. The model consists of an equation of motion for a nonconserved composition variable, coupled to a Newtonian stress relations for the reactant and product species. Multivalued reaction terms allow for different homogeneous phases to coexist with each other, resulting in banded composition and shear rate profiles. The one-dimensional equation of motion is evolved from a random initial state to its final steady-state. We find that the system chooses banded states over homogeneous states, depending on the shape of the stress constitutive curve and the magnitude of the diffusion coefficient. Banding in the flow gradient direction under shear rate control is observed for shear-thinning transitions, while banding in the vorticity direction under stress control is observed for shear-thickening transitions.

cond-mat.soft

Matched asymptotic solutions for the steady banded flow of the diffusive Johnson-Segalman model in various geometries

We present analytic solutions for steady flow of the Johnson-Segalman (JS) model with a diffusion term in various geometries and under controlled strain rate conditions, using matched asymptotic expansions. The diffusion term represents a singular perturbation that lifts the continuous degeneracy of stable, banded, steady states present in the absence of diffusion. We show that the stable steady flow solutions in Poiseuille and cylindrical Couette geometries always have two bands. For Couette flow and small curvature, two different banded solutions are possible, differing by the spatial sequence of the two bands.

cond-mat.soft

The Johnson-Segalman model with a diffusion term in Couette flow

We study the Johnson-Segalman (JS) model as a paradigm for some complex fluids which are observed to phase separate, or ``shear-band'' in flow. We analyze the behavior of this model in cylindrical Couette flow and demonstrate the history dependence inherent in the local JS model. We add a simple gradient term to the stress dynamics and demonstrate how this term breaks the degeneracy of the local model and prescribes a much smaller (discrete, rather than continuous) set of banded steady state solutions. We investigate some of the effects of the curvature of Couette flow on the observable steady state behavior and kinetics, and discuss some of the implications for metastability.

cond-mat.soft

Microscopic Viscoelasticity: Shear Moduli of Soft Materials Determined from Thermal Fluctuations

We describe a high-resolution, high-bandwidth technique for determining the local viscoelasticity of soft materials such as polymer gels. Loss and storage shear moduli are determined from the power spectra of thermal fluctuations of embedded micron-sized probe particles, observed with an interferometric microscope. This provides a passive, small-amplitude measurement of rheological properties over a much broader frequency range than previously accessible to microrheology. We study both F-actin biopolymer solutions and polyacrylamide (PAAm) gels, as model semiflexible and flexible systems, respectively. We observe high-frequency omega^(3/4) scaling of the shear modulus in F-actin solutions, in contrast to omega^(1/2) scaling for PAAm.

cond-mat.soft