Statistics of tumbling of a single polymer molecule in shear flow

We present experimental results on statistics of polymer orientation angles relative to the shear plane and tumbling times in shear flow with thermal noise. The strong deviation of the probability distribution functions (PDFs) of the orientation angles from Gaussian PDFs was observed in good accord with theory. A universal exponential PDF tail for the tumbling times and its predicted scaling with Wi (that is, the dimensionless shear rate normalized by the polymer relaxation time) are also tested experimentally against numerics. The scaling relations of PDF widths for both angles as a function of Wi are verified and compared with numerics.     

Measurement of diffusion in the presence of shear flow

We demonstrate here a method whereby molecular diffusion coefficients may be measured in the presence of the deformational flow field of a rheo-NMR cell. The method, which uses a repetitive CPMG train of rf pulses interspersed with magnetic field gradient pulses, allows the anisotropic diffusion spectrum to be directly probed. We focus on the cylindrical Couette cell, for which the radial, tangential, and axial directions correspond to the hydrodynamic velocity gradient, velocity, and vorticity directions. While ideal Couette flow does not perturb the vorticity direction, it does perturb diffusion measurements for the velocity gradient direction, and to a lesser extent, the velocity direction. We show that with closely spaced gradient pulses operating in a flow-compensating mode, there exists a diffusion limit below which one cannot measure, that scales as T(2)gamma(4), where gamma is the shear rate and T the gradient pulse repetition period. For a typical rheo-NMR cell, and for the more challenging velocity gradient direction, diffusion rates above 10(-12) m(2) s(-1) can be accurately measured (to 1% error) at shear rates up to 3s(-1). We demonstrate the use of the method in measuring the diffusion spectrum of a lyotropic lamellar phase under shear.     

Polymer solutions in co-rotating Taylor-Couette flow without vorticity

We present experimental results of the flow of dilute and semi-dilute polymer solutions in co-rotating Taylor-Couette cylinders. The experimental set-up consists of a modified Mars II rheometer (Thermo Scientific) with two drive units that are mounted opposite each other. The rotational velocities of the inner and outer cylinders are chosen in a way such that the angular velocity has a 1/r profile and the flow is free of vorticity, but the direction of elongation is not constant, but rotates with the flow. Our particle image velocimetry (PIV) measurements show that for polymer solutions without shear thinning the flow is indeed free of vorticity and is equal to a stagnation point flow at a given position and a given instant in time. In contrast, torque measurements reveal that the stresses are identical to the stresses that are present in a plane shear flow. Thus, we find that for polymer solutions a flow with vorticity and a constant direction of elongation is equal to a flow without vorticity in which the direction of elongation is rotating. Finally, we show that for shear thinning solutions the flow velocity becomes non-monotonic through the gap and resembles a pluglike profile which is known from the Poiseuille flow.     

Cyclic motion of a grafted polymer under shear flow

The long-time dynamics of a single end-tethered chain under shear flow are studied using molecular and Brownian dynamics simulations of a flexible polymer. As observed in previous experiments with tethered DNA [Phys. Rev. Lett. 84, 4769 (2000)], under a flow sheared at constant rate the chain performs a cyclic motion. But, contrary to what has been previously suggested, a well-defined characteristic period exists and it is clearly revealed in the cross spectra of the chain extension along flow and gradient directions. The main cycling time scales like the time needed to stretch the polymer by convection, being about 10 times the relaxation time of the chain in flow. This coherent recursive motion introduces long memory in the fluid and suggests resonance effects under periodic external forcing.     

Effect of magnetic fields on out-of-plane orientations of nematic liquid crystalline polymers under simple shear flow

The effect of magnetic fields on out-of-plane orientations of liquid crystalline polymers (LCPs) under simple shear flows is numerically analyzed using the Doi–Hess equation. The evolution equation for the probability distribution function of the LCP molecules is directly solved without any approximation closure. The initial director is parallel to the vorticity direction. Two cases of the magnetic fields are considered (1) the magnetic field parallel to the flow direction, and (2) the magnetic field parallel to the velocity gradient direction. For both cases a log-rolling orientation state is detected at low shear rates. However, the director is quickly aligned along the direction of magnetic fields because of the deformation of molecules. The field affects on the scalar order parameter rather than the major orientation direction for the magnetic field parallel to the flow direction. On the other hand regarding the magnetic field along the vorticity gradient direction, the effect of the magnetic field is more remarkable on the major orientation in comparison with the effect on the scalar order parameter. Also it is be found that the order parameter is increased obviously with increasing the magnetic fields. It is an efficient way to improve the performance of LCP materials.     

Vacillating breathing and tumbling of vesicles under shear flow

The dynamics of vesicles under a shear flow are analyzed analytically in the small deformation regime. We derive two coupled nonlinear equations which describe the vesicle orientation in the flow and its shape evolution. A new type of motion is found, namely, a "vacillating-breathing" mode: the vesicle orientation undergoes an oscillation around the flow direction, while the shape executes breathing dynamics. This solution coexists with tumbling. Moreover, we provide an explicit expression for the tumbling threshold. A rheological law for a dilute vesicle suspension is outlined.     

Dynamics of two trapped Brownian particles: Shear-induced cross-correlations

The dynamics of two Brownian particles trapped by two neighboring harmonic potentials in a linear shear flow is investigated. The positional correlation functions in this system are calculated analytically and analyzed as a function of the shear rate and the trap distance. Shear-induced cross-correlations between particle fluctuations along orthogonal directions in the shear plane are found. They are linear in the shear rate, asymmetric in time, and occur for one particle as well as between both particles. Moreover, the shear rate enters as a quadratic correction to the well-known correlations of random displacements along parallel spatial directions. The correlation functions depend on the orientation of the connection vector between the potential minima with respect to the flow direction. As a consequence, the inter-particle cross-correlations between orthogonal fluctuations can have zero, one or two local extrema as a function of time. Possible experiments for detecting these predicted correlations are described.     

Accurate statistics of a flexible polymer chain in shear flow

We present exact and analytically accurate results for the problem of a flexible polymer chain in shear flow. Under such a flow the polymer tumbles, and the probability distribution of the tumbling times tau of the polymer decays exponentially as approximately exp(-alphatau/tau_{0}) (where tau_{0} is the longest relaxation time). We show that for a Rouse chain this nontrivial constant alpha can be calculated in the limit of a large Weissenberg number (high shear rate) and is in excellent agreement with our simulation result of alpha approximately 0.324. We also derive exactly the distribution functions for the length and the orientational angles of the end-to-end vector R of the polymer.     

Undulation instability under shear: A model to explain the different orientations of a lamellar phase under shear?

We study the effects of a dilation on a sheared smectic A phase. Through a linear analysis, we show that undulation may grow in the direction of the flow and of the vorticity as found in previous works. At higher shear rates, we evidence that the undulation along the flow disappears whereas it persists in the vorticity direction. We determine the stable or unstable zone as a function of the shear rate and of the lamellar spacing. This allows us to draw a theoretical shear diagram of the instability. Finally we compare our results with the orientations found experimentally in a lyotropic lamellar phase under shear. Our diagram describes qualitatively and quantitatively the transition observed at high shear rate. Received 18 October 1999     

Kayaking and wagging of rods in shear flow

For the first time, we have simulated the periodic collective orientational motions performed by rigid liquid-crystalline polymers with large aspect ratio in the nematic state in shear flow. In order to be able to do so, we developed a new, event-driven Brownian dynamics technique. We present the results of simulations of rods with aspect ratios L/d ranging from 20 to 60 at volume fractions phi given by Lphi/d = 3.5 and 4.5. By studying the path of the director, i.e., the average direction of the rods, we observe kayaking, wagging, flow aligning, and log-rolling type of orbits, depending on the parameters of the simulation and the initial orientation. We find that the tumbling periods depend on Lphi/d and the shear rate but not on the type of motion. Our simulation results qualitatively confirm theoretical predictions and are in good agreement with the experimental measurements of tumbling times of fd viruses.     

Large-eddy simulation of impinging jets with embedded azimuthal vortices

We have carried out large-eddy simulations of an impinging jet with embedded azimuthal vortices, a model of the wake of a helicopter hovering in ground effect. The azimuthal vortices are generated by sinusoidal forcing of the velocity at the jet exit. They strengthen while they are advected towards the ground; when they are close to the solid surface, a layer of opposite-sign vorticity is formed at the wall, and lifted up to form a secondary vortex that interacts with the primary one. Regions of reversed flow are caused by the strong, localised, adverse pressure gradient. After this interaction, the primary vortices begin to decay, mostly due to the Reynolds shear stresses, which contribute to the turbulent diffusion of vorticity term in the budget of the phase-averaged azimuthal vorticity. This mechanism is extremely robust, and plays the most important role in the vortex decay even if no turbulence is initially present in the jet, or if the no-slip condition is removed. A three-dimensional instability also plays a role: removing it leads to slower decay. Our results also point out some challenges for turbulence models for the unsteady Reynolds-averaged Navier–Stokes equations.     

Analysis of membrane tank-tread of nonspherical capsules and red blood cells

We present an analysis of membrane motion of deformable capsules and red blood cells suspended in a linear shear flow and undergoing swinging and tumbling motions using three-dimensional numerical simulations. This study is motivated by the theory of the shape-preserving cells which predicts that the direction of the membrane rotation depends on the cell orientation and reverses at every 45° inclination angle of the cell major axis with respect to the external flow direction. By considering large deformation of capsules and red blood cells, here we investigate how the shape oscillation affects the time dependence and the direction reversal of the membrane rotation. We find that the membrane tank-tread is highly time-dependent in nature and synchronized with the time-dependent deformation. The maximum and minimum of the tank-tread velocity occur at and near the minimum and maximum deformation, respectively. For the swinging capsules and red blood cells, the direction of the membrane rotation is always along the direction of the external fluid rotation; however, a direction reversal occurs during the tumbling motion in which case the membrane rotates in the direction of the external fluid rotation when the major axis is mostly in the extensional quadrant of the shear flow, and in the opposite direction when it is mostly in the compressional quadrant. Unlike the theory which predicts the direction reversal at every 45° inclination angle irrespective of the control parameters, namely, the capillary number, viscosity ratio, and asphericity, we find that the angle at which the direction reversal occurs depends on these parameters. In particular, if the tumbling motion occurs by decreasing the capillary number, the membrane rotation is in the direction of the external flow rotation in the entire extensional quadrant, but in the opposite direction in the compressional quadrant, irrespective of the specific values of the capillary number. If the tumbling motion occurs by increasing the viscosity ratio and asphericity, the angle at which the direction reversal occurs depends on the specific values of these two parameters. The spatial variation of the tank-tread velocity also is analyzed and attributed to the straining motion of the external flow.      

Dynamics of viscous vesicles in shear flow

The dynamics of giant lipid vesicles under shear flow is experimentally investigated. Consistent with previous theoretical and numerical studies, two flow regimes are identified depending on the viscosity ratio between the interior and the exterior of the vesicle, and its reduced volume or excess surface. At low viscosity ratios, a tank-treading motion of the membrane takes place, the vesicle assuming a constant orientation with respect to the flow direction. At higher viscosity ratios, a tumbling motion is observed in which the whole vesicle rotates with a periodically modulated velocity. When the shear rate increases, this tumbling motion becomes increasingly sensitive to vesicle deformation due to the elongational component of the flow and significant deviations from simpler models are observed. A good characterization of these various flow regimes is essential for the validation of analytical and numerical models, and to relate microscopic dynamics to macroscopic rheology of suspensions of deformable particles, such as blood.     

Wetting of phospholipid membranes on hydrophilic surfaces - Concepts towards self-healing membranes

We report on the wetting behavior of phospholipid membranes on solid surfaces immersed in aqueous solution. Using fluorescence microscopy, the spreading velocity of fluid bilayers advancing from a lipid source is investigated. The kinetic spreading coefficient was measured as a function of temperature for pure DMPC membranes and as a function of charge density and cholesterol content for binary membranes. A theoretical model for the membrane flow is presented, which takes into account the liquid crystalline bilayer architecture of the lipid membrane. The spreading power results from the membrane-solid VdW interaction and is dissipated in hydrodynamic shear flow as well as by inter-monolayer friction within the bilayer. The frictional drag causes a dynamic tension gradient in the spreading membrane, which is manifested by a single exponential decay of the fluorescence intensity profile along the spreading direction. Obstacles are shown to act as pinning centers deforming the advancing line interface. However, no depinning was observed, since the centers are circumflown without abrupt relaxation. Received 6 November 1998     

Confined cubic blue phases under shear

We study the behaviour of confined cubic blue phases under shear flow via lattice Boltzmann simulations. We focus on the two experimentally observed phases, blue phase I and blue phase II. The disclination network of blue phase II continuously breaks and reforms under shear, leading to an oscillatory stress response in time. The oscillations are only regular for very thin samples. For thicker samples, the shear leads to a 'stick-slip' motion of part of the network along the vorticity direction. Blue phase I responds very differently: its defect network undergoes seemingly chaotic rearrangements under shear, irrespective of system size.     

Shear-thickening transition in surfactant solutions: New experimental features from rheology and flow birefringence

We report on the shear-thickening transition observed in dilute aqueous solutions of cetyltrimethylammonium tosylate (CTAT) at concentrations . We have re-examined the kinetics of the shear-thickening transition using start-up experiments at rates above the critical shear rate . Using simple well-defined protocols, we have found that the transient mechanical response depends dramatically on the thermal and on the shear histories. Using the same protocols, flow birefringence experiments were carried out. The gap of a Couette cell containing the sheared solution has been visualized between crossed polarizers in steady shear conditions, as well as in start-up experiments. We show that the birefringent shear-induced phase starts from the inner cylinder and grows along the velocity gradient direction, as in a shear banding situation. However, around we have not observed a regime of phase coexistence (isotropic and birefringent). Received 11 November 1999     

A new approach to visualizing spectral density functions and deriving motional correlation time distributions: applications to an alpha-helix-forming peptide and to a well-folded protein

A new approach to visualizing spectral densities and analyzing NMR relaxation data has been developed. By plotting the spectral density function, J(omega), as F(omega)=2 omega J(omega) on the log-log scale, the distribution of motional correlation times can be easily visualized. F(omega) is calculated from experimental data using a multi-Lorentzian expansion that is insensitive to the number of Lorentzians used and allows contributions from overall tumbling and internal motions to be separated without explicitly determining values for correlation times and their weighting coefficients. To demonstrate the approach, (15)N and (13)C NMR relaxation data have been analyzed for backbone NH and C(alpha)H groups in an alpha-helix-forming peptide 17mer and in a well-folded 138-residue protein, and the functions F(omega) have been calculated and deconvoluted for contributions from overall tumbling and internal motions. Overall tumbling correlation time distribution maxima yield essentially the same overall correlation times obtained using the Lipari-Szabo model and other standard NMR relaxation data analyses. Internal motional correlational times for NH and C(alpha)H bond motions fall in the range from 100 ps to about 1 ns. Slower overall molecular tumbling leads to better separation of internal motional correlation time distributions from those of overall tumbling. The usefulness of the approach rests in its ability to visualize spectral densities and to define and separate frequency distributions for molecular motions.     

Sample-to-sample torque fluctuations in a system of coaxial randomly charged surfaces

The stress propagation in a concentrated attractive colloidal suspension under shear is studied using numerical simulations. The spatial correlations of the intercolloidal stress field are studied and an inertia-like tensor is defined in order to characterize the anisotropic nature of the stress field. It is shown that the colloids remain in a liquid order, the intercolloidal stress is strongly anisotropic. A transition under flow is observed: during a transient regime at low deformation, the stress propagates along the compression direction of the shear, whereas at larger deformations, the stress is organized into layers parallel to the (flow, vorticity) plane.     

Semiflexible polymers in shear flow

The dynamics of semiflexible polymers under the influence of shear flow is studied analytically. Power laws are derived for various conformational and dynamical quantities which are in agreement with experimental findings. In particular, the tumbling motion is analyzed and expressions are provided for the probability distributions of the orientation angles and the tumbling time. The calculations explain the similarities in the behavior of flexible and semiflexible polymers as well as free-draining and nondraining systems.     

Spatiotemporal dynamics of shear induced bands en route to rheochaos

We show experimentally that the route to rheochaos in shear rate relaxation measurements is via Type-III intermittency and mixed mode oscillations in the shear-thinning wormlike micellar system of cetyltrimethylammonium tosylate in the presence of salt sodium chloride. Depolarised small angle light scattering measurements performed during flow show that scattered intensity temporally follows the shear rate/stress dynamics and portrays the crucial role played by nematic ordering. Direct visualization of the gap of the Couette cell, illuminated by an unpolarised laser sheet, in the (vorticity, velocity gradient) plane shows that the spatiotemporal dynamics of the shear induced structures is closely related to the temporal behaviour of shear rate/stress fluctuations.