NMR velocimetry studies of the steady-shear rheology of a concentrated hard-sphere colloidal system

NMR velocimetry has been used to observe the steady-shear rheological behaviour of a concentrated suspension of hard-sphere like 370 nm diameter PMMA core-shell latex particles at the volume fraction Φ = 0.46, the liquid core of the spheres rendering possible NMR observation of the particles themselves. Rheological measurements in a cone-and-plate geometry indicate that when aged (i.e. left at rest for two weeks), the material exhibits yield stress behaviour at very low shear rates. For shear rates greater than 1 s ^{- 1} a transition to liquid-like behaviour was observed, leading to a rejuvenated fluid state which exhibits shear-thinning behaviour over a wide range of shear rates. A similar yield stress behaviour was reflected in NMR velocimetry measurements in a Couette geometry, where the solid-to liquid transition could be clearly observed. Under steady-state flow, the fluid state inside the radius at which yield stress was observed, exhibited shear-thinning behaviour with a power law exponent n slowly approaching unity with increasing shear rate. This behaviour has some similarities with a model of Derec et al. in which aging and rejuvenation effects compete. Substantial wall slip was observed both at the inner and at the outer wall, an effect which disappeared as the shear rate was increased. No radial particle migration from the high-shear region at the inner wall was observed.     

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 relation 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. Received 1 April 2001 and Received in final form 16 June 2001     

Effect of tangential interface motion on the viscous instability in fluid flow past flexible surfaces

The stability of linear shear flow of a Newtonian fluid past a flexible membrane is analysed in the limit of low Reynolds number as well as in the intermediate Reynolds number regime for two different membrane models. The objective of this paper is to demonstrate the importance of tangential motion in the membrane on the stability characteristics of the shear flow. The first model assumes the wall to be a “spring-backed” plate membrane, and the displacement of the wall is phenomenologically related in a linear manner to the change in the fluid stresses at the wall. In the second model, the membrane is assumed to be a two-dimensional compressible viscoelastic sheet of infinitesimal thickness, in which the constitutive relation for the shear stress contains an elastic part that depends on the local displacement field and a viscous component that depends on the local velocity in the membrane. The stability characteristics of the laminar flow in the limit of low are crucially dependent on the tangential motion in the membrane wall. In both cases, the flow is stable in the low Reynolds number limit in the absence of tangential motion in the membrane. However, the presence of tangential motion in the membrane destabilises the shear flow even in the absence of fluid inertia. In this case, the non-dimensional velocity (Λ_t) required for unstable fluctuations is proportional to the wavenumber k ( Λ _t∼k) in the plate membrane type of wall while it scales as k² in the viscoelastic membrane type of wall ( Λ _t∼k ²) in the limit k→ 0. The results of the low Reynolds number analysis are extended numerically to the intermediate Reynolds number regime for the case of a viscoelastic membrane. The numerical results show that for a given set of wall parameters, the flow is unstable only in a finite range of Reynolds number, and it is stable in the limit of large Reynolds number. Received 8 November 2000 and Received in final form 20 March 2001     

Self-healing slip pulses and the friction of gelatin gels

We present an extensive experimental study and scaling analysis of friction of gelatin gels on glass. At low driving velocities, sliding occurs via propagation of periodic self-healing slip pulses whose velocity is limited by collective diffusion of the gel network. Healing can be attributed to a frictional instability occurring at the slip velocity V = V _c. For V > V _c, sliding is homogeneous and friction is ruled by the shear-thinning rheology of an interfacial layer of thickness of order the (nanometric) mesh size, containing a solution of polymer chain ends hanging from the network. In spite of its high degree of confinement, the rheology of this system does not differ qualitatively from known bulk ones. The observed ageing of the static friction threshold reveals the slow increase of adhesive bonding between chain ends and glass. Such structural ageing is compatible with the existence of a velocity-weakening regime at velocities smaller than V _c, hence with the existence of the healing instability. Received: 7 March 2003 / Accepted: 2 May 2003 / Published online: 11 June 2003 RID="b" ID="b"e-mail: ronsin@gps.jussieu.fr     

Ultrasound velocimetry in a shear-thickening wormlike micellar solution: Evidence for the coexistence of radial and vorticity shear bands

We carried out pointwise local velocity measurements on 40 mM cetylpyridinium chloride-sodium salicylate (CPyCl-NaSal) wormlike micellar solution using high-frequency ultrasound velocimetry in a Couette shear cell. The studied wormlike solution exhibits Newtonian, shear-thinning and shear-thickening rheological behavior in a stress-controlled environment. Previous rheology, flow visualization and small-angle light/neutron scattering experiments in the shear-thickening regime of this system showed the presence of stress-driven alternating transparent and turbid rings or vorticity bands along the axis of the Couette geometry. Through local velocity measurements we observe a homogeneous flow inside the 1mm gap of the Couette cell in the shear-thinning (stress-plateau) region. Only when the solution is sheared beyond the critical shear stress (shear-thickening regime) in a stress-controlled experiment, we observe inhomogeneous flow characterized by radial or velocity gradient shear bands with a highly sheared band near the rotor and a weakly sheared band near the stator of the Couette geometry. Furthermore, fast measurements performed in the shear-thickening regime to capture the temporal evolution of local velocities indicate coexistence of both radial and vorticity shear bands. However the same measurements carried out in shear rate controlled mode of the rheometer do not show such rheological complexity.     

Probing the strange quark condensate by di-electrons from φ-meson decays in heavy-ion collisions at SIS energies

QCD sum rules predict that the change of the strange quark condensate 〈ˉss〉 in hadron matter at finite baryon density causes a shift of the peak position of the di-electron spectra from φ-meson decays. Due to the expansion of hadron matter in heavy-ion collisions, the φ peak suffers a smearing governed by the interval of density in the expanding fireball, which appears as an effective broadening of the di-electron spectrum in the φ region. The emerging broadening is sensitive to the in-medium change of 〈ˉss〉. This allows to probe directly in-medium modifications of 〈ˉss〉 via di-electron spectra in heavy-ion collisions at SIS energies with HADES. Received: 22 November 2002 / Accepted: 30 January 2003 / Published online: 29 April 2003     

Dynamical properties of the slithering-snake algorithm: A numerical test of the activated-reptation hypothesis

Correlations in the motion of reptating polymers in a melt are investigated by means of Monte Carlo simulations of the three-dimensional slithering-snake version of the bond-fluctuation model. Surprisingly, the slithering-snake dynamics becomes inconsistent with classical reptation predictions at high chain overlap (created either by chain length N or by the volume fraction φ of occupied lattice sites), where the relaxation times increase much faster than expected. This is due to the anomalous curvilinear diffusion in a finite time window whose upper bound (N) is set by the density of chain ends φ/N. Density fluctuations created by passing chain ends allow a reference polymer to break out of the local cage of immobile obstacles created by neighboring chains. The dynamics of dense solutions of “snakes” at t ≪ is identical to that of a benchmark system where all chains but one are frozen. We demonstrate that the subdiffusive dynamical regime is caused by the slow creeping of a chain out of its correlation hole. Our results are in good qualitative agreement with the activated-reptation scheme proposed recently by Semenov and Rubinstein (Eur. Phys. J. B, 1 (1998) 87). Additionally, we briefly comment on the relevance of local relaxation pathways within a slithering-snake scheme. Our preliminary results suggest that a judicious choice of the ratio of local to slithering-snake moves is crucial to equilibrate a melt of long chains efficiently. Received: 18 December 2002 / Accepted: 3 April 2003 / Published online: 12 May 2003 RID="a" ID="a"e-mail: jwittmer@dpm.univ-lyon1.fr RID="b" ID="b"Current address: University of Illinois at Urbana-Champaign.     

Anomalous elasticity of an ordered lamellar liquid foam

We investigate experimentally the linear viscoelastic properties of a lamellar liquid foam as a function of the cell size and spatial organisation. The system consists of multilamellar vesicles generated by a simple shear flow on a lyotropic lamellar phase. The vesicles can be prepared either in an amorphous or a spatially ordered state. Their size is easily tunable in the range R = 0.5-15 μm. Whereas the shear modulus of the amorphous lamellar foam is alike that of usual liquid foams or concentrated emulsions and scales linearly with 1/R, the elastic modulus of the ordered foam is almost independent of the cell size. This result --probably the first describing the elasticity of an ordered foam-like system-- remains unexplained. Received 7 August 2000     

Rheology and aging: A simple approach

We introduce a rheological model to describe the low-frequency mechanical properties of systems near a fluid/paste transition. We propose a Landau-like expansion for the vicinity of this transition, treating the stress relaxation rate as an order parameter. This leads to a formally simple model that allows us to describe the interplay between aging and non-linearities in the mechanical response of the system. We focus here on systems prepared by fluidification under a strong shear, on which mechanical measurments are performed (oscillatory rheology, stress relaxation, response to a steady shear rate), after a waiting time during which the system evolves on its own. Received 14 June 2000     

Viscosity minimum in bimodal concentrated suspensions under shear

We study a model of concentrated suspensions under shear in two dimensions. Interactions between suspended particles are dominated by direct-contact viscoelastic forces and the particles are neutrally bouyant. The bimodal suspensions consist of a variable proportion between large and small droplets, with a fixed global suspended fraction. Going beyond the assumptions of the classical theory of Farris (R.J. Farris, Trans. Soc. Rheol. 12, 281 (1968)), we discuss a shear viscosity minimum, as a function of the small-to-large-particle ratio, in shear geometries imposed by external body forces and boundaries. Within a linear-response scheme, we find the dependence of the viscosity minimum on the imposed shear and the microscopic drop friction parameters. We also discuss the viscosity minimum under dynamically imposed shear applied by boundaries. We find a reduction of macroscopic viscosity with the increase of the microscopic friction parameters that is understood using a simple two-drop model. Our simulation results are qualitatively consistent with recent experiments in concentrated bimodal emulsions with a highly viscous or rigid suspended component. Received 28 June 2002 RID="a" ID="a"e-mail: ernesto@pion.ivic.ve     

Monte-Carlo simulation of transient gel formation and break-up during reversible aggregation

Monte-Carlo simulations of reversible aggregation on a cubic lattice were done by introducing a finite probability (P) of nearest neighbours to form a bond. Depending on the volume fraction of occupied sites (φ) and P we observed different phenomena by monitoring as a function of time the space filling and the distribution of the aggregates and the gel fraction. At smaller values of P the system develops into an equilibrium distribution of aggregates of which the average size increases with increasing φ until above a critical value the system percolates. At larger values of P the system phase separates into two phases with different densities. Above a critical value of φ the system percolates during a finite time. The life time of the gel and the maximum gel fraction were studied as a function of P. Received 1st March 2001 and Received in final form 24 April 2001     

Yielding and flow in adhesive and nonadhesive concentrated emulsions

The nonlinear rheological response of soft glassy materials is addressed experimentally by focusing on concentrated emulsions where interdroplet attraction is tuned through varying the surfactant content. Velocity profiles are recorded using ultrasonic velocimetry simultaneously to global rheological data in the Couette geometry. Our data show that nonadhesive and adhesive emulsions have radically different flow behaviors in the vicinity of yielding: while the flow remains homogeneous in the nonadhesive emulsion and the Herschel-Bulkley model for a yield stress fluid describes the data very accurately, the adhesive system displays shear localization and does not follow a simple constitutive equation, suggesting that the mechanisms involved in yielding transitions are not universal.     

Universal properties of lamellar systems under weak shear

We have observed that different lamellar phases (thermotropic, lyotropic of surfactants or blockcopolymers) share the same rheological properties = A(T)σ^m, m = 1.67±0.1, independently of their chemical nature, in a range of shear rates , shear stresses σ, and temperatures T, where the flow is stationary. It is argued that the key phenomenon is the appearance of screw dislocations whose glide under an applied shear counterbalances plastically the applied vorticity, and stabilizes the layers, whose slip past each other is thus made more feasible. The theory, which makes use in other respects of the high-temperature creep model in solids, reproduces correctly the power law behavior and the values of A(T). Received 18 April 2001 and Received in final form 25 October 2001     

Noise correlations in shear flows

We consider the effects of a shear on velocity fluctuations in a flow. The shear gives rise to a transient amplification that not only influences the amplitude of perturbations but also their time correlations. We show that, in the presence of white noise, time correlations of transversal velocity components are exponential and that correlations of the longitudinal components are exponential with an algebraic prefactor. Cross correlations between transversal and downstream components are strongly asymmetric and provide a clear indication of non-normal amplification. We suggest experimental tests of our predictions. Received 26 February 2002 / Received in final form 11 March 2003 Published online 20 June 2003 RID="a" ID="a"e-mail: bruno.eckhardt@physik.uni-marburg.de RID="b" ID="b"Also at: Jawaharlal Nehru Centre for Advanced Scientific Research, Bangalore, India     

Production of φ mesons in near-threshold πN and NN reactions

We analyze the production of φ mesons in πN and NN reactions in the near-threshold region, using throughout the conventional “non-strange” dynamics based on such processes which are allowed by the non-ideal ω-φ mixing. We show that the occurrence of the direct φNN interaction may show up in different unpolarized and polarization observables in πN→Nφ reactions. We find a strong non-trivial difference between observables in the reactions pp→ppφ and pn→pnφ caused by the different role of the spin singlet and triplet states in the entrance channel. A series of predictions for the experimental study of this effect is presented. Received: 27 January 2000     

Echo tracer dispersion in flows of polymer solutions through porous media: A tool for detecting weak permeability heterogeneities?

Tracer dispersion in Newtonian and shear-thinning fluids (scleroglucan-water polymer solutions) flowing through single and double porosity grain packings has been studied experimentally using both classical transmission dispersion and echo dispersion (in the latter, the concentration variation front is pumped back through a detector at the inlet after penetrating for a chosen distance into the sample). Transmission dispersion increases markedly in both types of samples with the shear thinning index of the fluid at all Péclet numbers (except when molecular diffusion is dominant). Echo and transmission experiments give nearly identical dispersivity values for Newtonian fluids while echo dispersivity is lower than transmission for shear thinning ones. The normalized dispersivity difference has same order of magnitude for single and double porosity samples and increases with the shear thinning exponent α (by a factor of 2 between α = 0.35 and α = 0.60). This difference may be due to heterogeneities inducing permeability variations of small amplitude over distances of the order of the sample section : their influence on tracer dispersion is partly reversible with respect to a change of the flow direction and is only detectable if it is amplified by the shear-thinning properties of the fluid. Received 19 September 2001     

Random inelasticity and velocity fluctuations in a driven granular gas

We analyze the deviations from Maxwell-Boltzmann statistics found in recent experiments studying velocity distributions in two-dimensional granular gases driven into a non-equilibrium stationary state by a strong vertical vibration. We show that in its simplest version, the “stochastic thermostat” model of heated inelastic hard spheres, contrary to what has been hitherto stated, is incompatible with the experimental data, although predicting a reminiscent high-velocity stretched-exponential behavior with an exponent 3/2. The experimental observations lead to refine a recently proposed random restitution coefficient model. Very good agreement is then found with experimental velocity distributions within this framework, which appears self-consistent and further provides relevant probes to investigate the universality of the velocity statistics. Received: 27 May 2002 / Accepted: 6 May 2003 / Published online: 27 May 2003 RID="a" ID="a"e-mail: Alain.Barrat@th.u-psud.fr     

Robust propagation direction of stresses in a minimal granular packing

By employing the adaptive network simulation method, we demonstrate that the ensemble-averaged stress caused by a local force for packings of frictionless rigid beads is concentrated along rays whose slope is consistent with unity: forces propagate along lines at 45 degrees to the horizontal or vertical. This slope is shown to be independent of polydispersity or the degree to which the system is sheared. Further confirmation of this result comes from fitting the components of the stress tensor to the null stress “constitutive equation”. The magnitude of the response is also shown to fall off with the -1/2 power of distance. We argue that our findings are a natural consequence of a system that preserves its volume under small perturbations. Received 30 April 2001 and Received in final form 16 August 2001     

On the current status of OZI violation in πN and pp reactions

The available data on ω and φ production from πN and pp collisions are reanalyzed with respect to an OZI rule violation on the basis of transition matrix elements. The data are found to be compatible with a constant ratio R , which however, deviates substantially from the SU(3) prediction based on the present knowledge of the φ-ω mixing angle. Received: 5 July 1999 / Revised version: 20 October 1999