Accelerated Stokesian Dynamics Research Articles

Parallel accelerated Stokesian dynamics with Brownian motion

We present scalable algorithms to simulate large-scale stochastic particle systems amenable for modeling dense colloidal suspensions, glasses and gels. To handle the large number of particles and consequent many-body interactions present in such systems, we leverage an Accelerated Stokesian Dynamics (ASD) approach, for which we developed parallel algorithms in a distributed memory architecture. We present parallelization of the sparse near-field (including singular lubrication) interactions, and of the matrix-free many-body far-field interactions, along with a strategy for communicating and mapping the distributed data structures between the near- and far field. Scaling to up to tens of thousands of processors for a million particles is demonstrated. In addition, we propose a novel algorithm to efficiently simulate correlated Brownian motion with hydrodynamic interactions. The original Accelerated Stokesian Dynamics approach requires the separate computation of far-field and near-field Brownian forces. Recent advancements propose computation of a far-field velocity using positive spectral Ewald decomposition. We present an alternative approach for calculating the far-field Brownian velocity by implementing the fluctuating force coupling method and embedding it using a nested scheme into ASD. This straightforward and flexible approach reduces the computational time of the Brownian far-field force construction from O(NlogN)1+|α| to O(NlogN).

Ewald sum for hydrodynamic interactions of rigid spherical microswimmers.

We derive the Ewald sum decomposition of the grand mobility tensor which captures the hydrodynamic interactions in an infinite suspension of rigid spherical microswimmers. The grand mobility tensor connects the motion of an individual swimmer to the active and passive forces and torques acting on all the swimmers, and it is calculated based on a minimal microswimmer model incorporating the swimmers' finite body size. Our results have direct applications to the Stokesian dynamics simulations of an infinite suspension of rigid-bodied microswimmers. They also provide a platform to develop more advanced methods such as particle-mesh-Ewald-sum and accelerated Stokesian dynamics simulations.

Short- and long-time diffusion and dynamic scaling in suspensions of charged colloidal particles.

We report on a comprehensive theory-simulation-experimental study of collective and self-diffusion in concentrated suspensions of charge-stabilized colloidal spheres. In theory and simulation, the spheres are assumed to interact directly by a hard-core plus screened Coulomb effective pair potential. The intermediate scattering function, fc(q, t), is calculated by elaborate accelerated Stokesian dynamics (ASD) simulations for Brownian systems where many-particle hydrodynamic interactions (HIs) are fully accounted for, using a novel extrapolation scheme to a macroscopically large system size valid for all correlation times. The study spans the correlation time range from the colloidal short-time to the long-time regime. Additionally, Brownian Dynamics (BD) simulation and mode-coupling theory (MCT) results of fc(q, t) are generated where HIs are neglected. Using these results, the influence of HIs on collective and self-diffusion and the accuracy of the MCT method are quantified. It is shown that HIs enhance collective and self-diffusion at intermediate and long times. At short times self-diffusion, and for wavenumbers outside the structure factor peak region also collective diffusion, are slowed down by HIs. MCT significantly overestimates the slowing influence of dynamic particle caging. The dynamic scattering functions obtained in the ASD simulations are in overall good agreement with our dynamic light scattering (DLS) results for a concentration series of charged silica spheres in an organic solvent mixture, in the experimental time window and wavenumber range. From the simulation data for the time derivative of the width function associated with fc(q, t), there is indication of long-time exponential decay of fc(q, t), for wavenumbers around the location of the static structure factor principal peak. The experimental scattering functions in the probed time range are consistent with a time-wavenumber factorization scaling behavior of fc(q, t) that was first reported by Segrè and Pusey [Phys. Rev. Lett. 77, 771 (1996)] for suspensions of hard spheres. Our BD simulation and MCT results predict a significant violation of exact factorization scaling which, however, is approximately restored according to the ASD results when HIs are accounted for, consistent with the experimental findings for fc(q, t). Our study of collective diffusion is amended by simulation and theoretical results for the self-intermediate scattering function, fs(q, t), and its non-Gaussian parameter α2(t) and for the particle mean squared displacement W(t) and its time derivative. Since self-diffusion properties are not assessed in standard DLS measurements, a method to deduce W(t) approximately from fc(q, t) is theoretically validated.

Normal modes of weak colloidal gels.

The normal modes and relaxation rates of weak colloidal gels are investigated in calculations using different models of the hydrodynamic interactions between suspended particles. The relaxation spectrum is computed for freely draining, Rotne-Prager-Yamakawa, and accelerated Stokesian dynamics approximations of the hydrodynamic mobility in a normal mode analysis of a harmonic network representing several colloidal gels. We find that the density of states and spatial structure of the normal modes are fundamentally altered by long-ranged hydrodynamic coupling among the particles. Short-ranged coupling due to hydrodynamic lubrication affects only the relaxation rates of short-wavelength modes. Hydrodynamic models accounting for long-ranged coupling exhibit a microscopic relaxation rate for each normal mode, λ that scales as l^{-2}, where l is the spatial correlation length of the normal mode. For the freely draining approximation, which neglects long-ranged coupling, the microscopic relaxation rate scales as l^{-γ}, where γ varies between three and two with increasing particle volume fraction. A simple phenomenological model of the internal elastic response to normal mode fluctuations is developed, which shows that long-ranged hydrodynamic interactions play a central role in the viscoelasticity of the gel network. Dynamic simulations of hard spheres that gel in response to short-ranged depletion attractions are used to test the applicability of the density of states predictions. For particle concentrations up to 30% by volume, the power law decay of the relaxation modulus in simulations accounting for long-ranged hydrodynamic interactions agrees with predictions generated by the density of states of the corresponding harmonic networks as well as experimental measurements. For higher volume fractions, excluded volume interactions dominate the stress response, and the prediction from the harmonic network density of states fails. Analogous to the Zimm model in polymer physics, our results indicate that long-ranged hydrodynamic interactions play a crucial role in determining the microscopic dynamics and macroscopic properties of weak colloidal gels.

Nonlinear rheology of colloidal suspensions probed by oscillatory shear

The nonlinear stress and microstructural response of a colloidal hard sphere suspension undergoing medium and large amplitude oscillatory simple shear have been studied using Accelerated Stokesian dynamics. The goal is to understand how nonlinearity arises and to link the structural effects to the resulting suspension stress. The imposed shear is given by the time-dependent rate γ̇(t)=γ̇0eiαt. Most results are shown for a hard-sphere suspension at a particle volume fraction ϕ=0.4. These are freely flowing conditions far from either glassy or jammed conditions, but the concept of the particle cage from glass dynamics is used. The cage is defined here in a statistical manner as the surface of elevated nearest neighbor probability, a sphere at contact for equilibrium. The cage concept is used in interpreting the microstructural deformation: For sufficiently small strain amplitude γ0, the cage deforms negligibly due to flow and the suspension remains in the linear response regime, but this is found to require γ0<0.01 at ϕ=0.4, as shown by a spectral decomposition of the microstructure in time, which discriminates rigorously between linear and nonlinear deformation. At larger γ0, termed medium amplitude and large amplitude in other studies, the material response is nonlinear. To preface the large amplitude oscillatory shear analysis, we use linear viscoelasticity theory to compare stress fluctuations at equilibrium to results obtained at finite Péclet number Pe and small γ0, as well as available experimental data and theoretical predictions; Pe=6πηγ̇0a3/kT is the ratio of hydrodynamic to Brownian forces, where η is the viscosity of the suspending liquid, γ̇0 is the shear rate amplitude, a is the particle radius, k is the Boltzmann constant, and T is the absolute temperature. The shear stress σxy and the normal stress differences N1 and N2 are analyzed under oscillatory shear at amplitudes 0.01≤γ0≤3.6 for a range of Pe. (The frequency α is related to Pe through γ̇0=αγ0 and the nondimensional frequency is given by the Deborah number De=Pe/γ0=6πηαa3/kT.) Pipkin diagrams are shown for σxy, N1 and N2. When hydrodynamic forces dominate the flow of the suspension, the complex viscosity |η*| has a nonmonotonic dependence on γ0, and Fourier-transform rheology shows the nonlinearity of the stress response to be maximized at an intermediate strain amplitude that depends on Pe. The elastic and viscous behavior of the suspension, as determined by a Chebyshev polynomial decomposition, is distinctly different for small and large Pe. The influence of the microstructure on the normal stress differences is discussed, noting that N1 is significant only when angular distortion of the microstructure is present, whereas N2 is formed with an accumulation of pair correlation at contact even at low oscillation amplitude.

Unsteady shear flows of colloidal hard-sphere suspensions by dynamic simulation

The rheology during the start-up and cessation of simple shear flow has been investigated for near hard-sphere colloidal suspensions. Simulations augmented by theoretical analysis are used to determine how the non-Newtonian stress development and relaxation depend on the microstructure. Accelerated Stokesian dynamics (ASD) and Brownian dynamics (BD) simulations are used for 0.05 ≤ Pe ≤ 500 in concentrated freely flowing suspensions; the Peclet number defining the ratio of shear to thermal motion is P e = 3 π η γ a 3 / k T with η the suspending fluid viscosity, γ the shear rate, and kT the thermal energy. Theoretical predictions based on the Smoluchowski equation for dilute suspensions are made, and these are primarily used for comparison with results from BD simulations in which hydrodynamic interactions are neglected. For suspensions with hydrodynamics, simulations by ASD are used to probe start-up and flow cessation over a large range of Pe; these studies focus on solid volume fraction ϕ = 0.4, with...

Pair mobility functions for rigid spheres in concentrated colloidal dispersions: Stresslet and straining motion couplings.

Accurate modeling of particle interactions arising from hydrodynamic, entropic, and other microscopic forces is essential to understanding and predicting particle motion and suspension behavior in complex and biological fluids. The long-range nature of hydrodynamic interactions can be particularly challenging to capture. In dilute dispersions, pair-level interactions are sufficient and can be modeled in detail by analytical relations derived by Jeffrey and Onishi [J. Fluid Mech. 139, 261-290 (1984)] and Jeffrey [Phys. Fluids A 4, 16-29 (1992)]. In more concentrated dispersions, analytical modeling of many-body hydrodynamic interactions quickly becomes intractable, leading to the development of simplified models. These include mean-field approaches that smear out particle-scale structure and essentially assume that long-range hydrodynamic interactions are screened by crowding, as particle mobility decays at high concentrations. Toward the development of an accurate and simplified model for the hydrodynamic interactions in concentrated suspensions, we recently computed a set of effective pair of hydrodynamic functions coupling particle motion to a hydrodynamic force and torque at volume fractions up to 50% utilizing accelerated Stokesian dynamics and a fast stochastic sampling technique [Zia et al., J. Chem. Phys. 143, 224901 (2015)]. We showed that the hydrodynamic mobility in suspensions of colloidal spheres is not screened, and the power law decay of the hydrodynamic functions persists at all concentrations studied. In the present work, we extend these mobility functions to include the couplings of particle motion and straining flow to the hydrodynamic stresslet. The couplings computed in these two articles constitute a set of orthogonal coupling functions that can be utilized to compute equilibrium properties in suspensions at arbitrary concentration and are readily applied to solve many-body hydrodynamic interactions analytically.

Active microrheology of colloidal suspensions: Simulation and microstructural theory

Discrete particle simulations by accelerated Stokesian dynamics (ASD) and a microstructural theory are applied to study the structure and viscosity of hard-sphere Brownian suspensions in active microrheology (MR). The work considers moderate to dense suspensions, from near to far from equilibrium conditions. The microscopic theory explicitly considers many-body hydrodynamic interactions in active MR and is compared with the results of ASD simulations, which include detailed near- and far-field hydrodynamic interactions. We consider probe and bath particles which are spherical and of the same radius a. Two conditions of moving the probe sphere are considered: These apply constant force (CF) and constant velocity (CV), which approximately model magnetic bead and optical tweezer experiments, respectively. The structure is quantified using the probability distribution of colloidal particles around the probe, Pb|p(r)=ng(r), giving the probability of finding a bath particle centered at a vector position r relative to a moving probe particle instantaneously centered at the origin; n is the bath particles number density, and is related to the suspension solid volume fraction, ϕ, by n=3ϕ/4πa3. The pair distribution function for the bath particles relative to the probe, g(r), is computed as a solution to the pair Smoluchowski equation (SE) for 0.2≤ϕ≤0.50, and a range of Péclet numbers, describing the ratio of external force on the probe to thermal forces and defined as Pef=Fexta/(kbT) and PeU=6πηUexta2/(kbT) for CF and CV conditions, respectively. Results of simulation and theory demonstrate that a wake zone depleted of bath particles behind the moving probe forms at large Péclet numbers, while a boundary-layer accumulation develops upstream and near the probe. The wake length saturates at Pef≫1 for CF, while it continuously grows with PeU in CV. This contrast in behavior is related to the dispersion in the motion of the probe under CF conditions, while CV motion has no dispersion; the dispersion is a direct result of many-body nonthermal interactions. This effect is incorporated in the theory as a force-induced diffusion flux in pair SE. We also demonstrate that, despite this difference of structure in the two methods of moving the probe, the probability distribution of particles near the probe is primarily set by the Péclet number, for both CF and CV conditions, in agreement with dilute theories; as a consequence, similar values for apparent viscosity are found for the CF and CV conditions. Using the microscopic theory, the structural anisotropy and Brownian viscosity near equilibrium are shown to be quantitatively similar in both CF and CV motions, which is in contrast with the dilute theory which predicts larger distortions and Brownian viscosities in CV, by a factor of two relative to CF MR. This difference relative to dilute theory arises due to the determining role of many-body interactions associated with the underlying equilibrium structure in the semidilute to concentrated regime.

Shear and normal stress measurements in non-Brownian monodisperse and bidisperse suspensions

There was an error in data reduction, resulting in incorrect values for the normal stress differences $N_1$ and $N_2$ shown in Figs. 7-10, and the corrected figures are shown here. In particular, the algebraic sign of $N_1$ is changed, as are the relative magnitudes of $N_1$ and $N_2$. The negative values of $N_1$ for these non-shear-thickening suspensions are larger in magnitude than those reported by other workers, but both $N_1$ and $N_2$ are in general agreement with the accelerated Stokesian Dynamics calculations of Sierou and Brady [1].

Pair mobility functions for rigid spheres in concentrated colloidal dispersions: Force, torque, translation, and rotation.

The formulation of detailed models for the dynamics of condensed soft matter including colloidal suspensions and other complex fluids requires accurate description of the physical forces between microstructural constituents. In dilute suspensions, pair-level interactions are sufficient to capture hydrodynamic, interparticle, and thermodynamic forces. In dense suspensions, many-body interactions must be considered. Prior analytical approaches to capturing such interactions such as mean-field approaches replace detailed interactions with averaged approximations. However, long-range coupling and effects of concentration on local structure, which may play an important role in, e.g., phase transitions, are smeared out in such approaches. An alternative to such approximations is the detailed modeling of hydrodynamic interactions utilizing precise couplings between moments of the hydrodynamic traction on a suspended particle and the motion of that or other suspended particles. For two isolated spheres, a set of these functions was calculated by Jeffrey and Onishi [J. Fluid Mech. 139, 261-290 (1984)] and Jeffrey [J. Phys. Fluids 4, 16-29 (1992)]. Along with pioneering work by Batchelor, these are the touchstone for low-Reynolds-number hydrodynamic interactions and have been applied directly in the solution of many important problems related to the dynamics of dilute colloidal dispersions [G. K. Batchelor and J. T. Green, J. Fluid Mech. 56, 375-400 (1972) and G. K. Batchelor, J. Fluid Mech. 74, 1-29 (1976)]. Toward extension of these functions to concentrated systems, here we present a new stochastic sampling technique to rapidly calculate an analogous set of mobility functions describing the hydrodynamic interactions between two hard spheres immersed in a suspension of arbitrary concentration, utilizing accelerated Stokesian dynamics simulations. These mobility functions provide precise, radially dependent couplings of hydrodynamic force and torque to particle translation and rotation, for arbitrary colloid volume fraction ϕ. The pair mobilities (describing entrainment of one particle by the disturbance flow created by another) decay slowly with separation distance: as 1/r, for volume fractions 0.05 ≤ ϕ ≤ 0.5. For the relative mobility, we find an initially rapid growth as a pair separates, followed by a slow, 1/r growth. Up to ϕ ≤ 0.4, the relative mobility does not reached the far-field value even beyond separations of many particle sizes. In the case of ϕ = 0.5, the far-field asymptote is reached but only at a separation of eight radii and after a slow 1/r growth. At these higher concentrations, the coefficients also reveal liquid-like structural effects on pair mobility at close separations. These results confirm that long-range many-body hydrodynamic interactions are an essential part of the dynamics of concentrated systems and that care must be taken when applying renormalization schemes.

Spectral Ewald Acceleration of Stokesian Dynamics for polydisperse suspensions

In this work we develop the Spectral Ewald Accelerated Stokesian Dynamics (SEASD), a novel computational method for dynamic simulations of polydisperse colloidal suspensions with full hydrodynamic interactions. SEASD is based on the framework of Stokesian Dynamics (SD) with extension to compressible solvents, and uses the Spectral Ewald (SE) method [Lindbo and Tornberg (2010) [29]] for the wave-space mobility computation. To meet the performance requirement of dynamic simulations, we use Graphic Processing Units (GPU) to evaluate the suspension mobility, and achieve an order of magnitude speedup compared to a CPU implementation. For further speedup, we develop a novel far-field block-diagonal preconditioner to reduce the far-field evaluations in the iterative solver, and SEASD-nf, a polydisperse extension of the mean-field Brownian approximation of Banchio and Brady (2003) [39]. We extensively discuss implementation and parameter selection strategies in SEASD, and demonstrate the spectral accuracy in the mobility evaluation and the overall O(Nlog⁡N) computation scaling. We present three computational examples to further validate SEASD and SEASD-nf in monodisperse and bidisperse suspensions: the short-time transport properties, the equilibrium osmotic pressure and viscoelastic moduli, and the steady shear Brownian rheology. Our validation results show that the agreement between SEASD and SEASD-nf is satisfactory over a wide range of parameters, and also provide significant insight into the dynamics of polydisperse colloidal suspensions.

Dynamics in dense hard-sphere colloidal suspensions

The dynamic behavior of a hard-sphere colloidal suspension was studied by x-ray photon correlation spectroscopy and small-angle x-ray scattering over a wide range of particle volume fractions. The short-time mobility of the particles was found to be smaller than that of free particles even at relatively low concentrations, showing the importance of indirect hydrodynamic interactions. Hydrodynamic functions were derived from the data, and for moderate particle volume fractions (Φ≤ 0.40) there is good agreement with earlier many-body theory calculations by Beenakker and Mazur [Physica A 120, 349 (1984)]. Important discrepancies appear at higher concentrations, above Φ≈ 0.40, where the hydrodynamic effects are overestimated by the Beenakker-Mazur theory, but predicted accurately by an accelerated Stokesian dynamics algorithm developed by Banchio and Brady [J. Chem. Phys. 118, 10323 (2003)]. For the relaxation rates, good agreement was also found between the experimental data and a scaling form predicted by the mode coupling theory. In the high concentration range, with the fluid suspensions approaching the glass transition, the long-time diffusion coefficient was compared with the short-time collective diffusion coefficient to verify a scaling relation previously proposed by Segrè and Pusey [Phys. Rev. Lett. 77, 771 (1996)]. We discuss our results in view of previous experimental attempts to validate this scaling law [L. Lurio et al., Phys. Rev. Lett. 84, 785 (2000)].

Effect of repulsive interactions on structure and rheology of sheared colloidal dispersions

A previously developed Smoluchowski theory for concentrated hard-sphere suspensions in shear flow is extended to study structure and rheology of colloidal suspensions with soft repulsive interactions. Accelerated Stokesian Dynamics simulations are carried out to provide insight and to enable direct comparison with theoretical predictions. The effect of extended range repulsive interactions is studied by considering repulsive interactions with different steepness, using identical potentials in simulation and theory, for varying shear rates characterized in dimensionless form as 0.1 ≤ Pe ≤ 100; here, Pe = 6πηa3/kbT is the ratio of hydrodynamic to Brownian forces and η is the fluid viscosity, is the shear rate, a is the particle radius and kbT is the thermal energy. Examples of predicted microstructures and the equivalent simulated results for hard-sphere suspensions at ϕ = 0.40 are also presented for comparison. The predicted pair distribution function is in good agreement with simulations before the onset of a shear-induced ordering transition in simulations of the soft colloids. The calculations of shear viscosity based on the predicted microstructure were also in general agreement with simulation results. The role of hydrodynamic interactions on flow-induced structures is discussed in the context of the proposed theory.

Short-time rheology and diffusion in suspensions of Yukawa-type colloidal particles

A comprehensive study is presented on the short-time dynamics in suspensions of charged colloidal spheres. The explored parameter space covers the major part of the fluid-state regime, with colloid concentrations extending up to the freezing transition. The particles are assumed to interact directly by a hard-core plus screened Coulomb potential, and indirectly by solvent-mediated hydrodynamic interactions. By comparison with accurate accelerated Stokesian Dynamics (ASD) simulations of the hydrodynamic function H(q), and the high-frequency viscosity η(∞), we investigate the accuracy of two fast and easy-to-implement analytical schemes. The first scheme, referred to as the pairwise additive (PA) scheme, uses exact two-body hydrodynamic mobility tensors. It is in good agreement with the ASD simulations of H(q) and η(∞), for smaller volume fractions up to about 10% and 20%, respectively. The second scheme is a hybrid method combining the virtues of the δγ scheme by Beenakker and Mazur with those of the PA scheme. It leads to predictions in good agreement with the simulation data, for all considered concentrations, combining thus precision with computational efficiency. The hybrid method is used to test the accuracy of a generalized Stokes-Einstein (GSE) relation proposed by Kholodenko and Douglas, showing its severe violation in low salinity systems. For hard spheres, however, this GSE relation applies decently well.

The hydrodynamics of confined dispersions

AbstractA method is proposed for computing the low-Reynolds-number hydrodynamic forces on particles comprising a suspension confined by two parallel, no-slip walls. This is constructed via the two-dimensional analogue of Hasimoto’s solution (J. Fluid Mech., vol. 5, 1959, pp. 317–328) for a periodic array of point forces in a viscous, incompressible fluid, and, like Hasimoto, the summation of interactions is accelerated by substitution and superposition of ‘Ewald-like’ forcing. This method is akin to the accelerated Stokesian dynamics technique (J. Fluid Mech., vol. 448, 2001, pp. 115–146) and models the suspension dynamics with log–linear computational scaling. The effectiveness of this approach is demonstrated with a calculation of the high-frequency dynamic viscosity of a colloidal dispersion as function of volume fraction and channel width. Similarly, the short-time self-diffusivity for and the sedimentation rate of spherical particles in a confined suspension are determined. The results demonstrate the influence of confining geometry on the transport of small particles, which is becoming increasingly important for micro- and biofluidics.

Anisotropic diffusion in confined colloidal dispersions: The evanescent diffusivity

We employ an analogy to traditional dynamic light scattering to describe the inhomogeneous and anisotropic diffusion of colloid particles near a solid boundary measured via evanescent wave dynamic light scattering. Following this approach, we generate new expressions for the short-time self- and collective diffusivities of colloidal dispersions with arbitrary volume fraction. We use these expressions in combination with accelerated Stokesian dynamics simulations to calculate the diffusivities in the limit of large and small scattering wave numbers for evanescent penetration depths ranging from four particle radii to one-fifth of a particle radius and volume fractions from 10% to 40%. We show that at high volume fractions, and larger penetration depths, the boundaries have little effect on the dynamics of the suspension parallel to the wall since, to a first approximation, the boundary acts hydrodynamically much as another nearby particle. However, near and normal to the wall, the diffusivity shows a strong dependence on penetration depth for all volume fractions. This is due to the lubrication interactions between the particles and the boundary as the particle moves relative to the wall. These results are novel and comprehensive with respect to the range of penetration depth and volume fraction and provide a complete determination of the effect of hydrodynamic interactions on colloidal diffusion adjacent to a rigid boundary.

Multi-scale calculation of settling speed of coarse particles by accelerated Stokesian dynamics without adjustable parameter

The calculation of settling speed of coarse particles is firstly addressed, with accelerated Stokesian dynamics without adjustable parameters, in which far field force acting on the particle instead of particle velocity is chosen as dependent variables to consider inter-particle hydrodynamic interactions. The sedimentation of a simple cubic array of spherical particles is simulated and compared to the results available to verify and validate the numerical code and computational scheme. The improved method keeps the same computational cost of the order O(N log N) as usual accelerated Stokesian dynamics does. Then, more realistic random suspension sedimentation is investigated with the help of Mont Carlo method. The computational results agree well with experimental fitting. Finally, the sedimentation of finer cohesive particle, which is often observed in estuary environment, is presented as a further application in coastal engineering.

Ordering transition and structural evolution under shear in Brownian suspensions

Shear-induced ordering is known to occur in sheared suspensions. The range of parameters for which this order occurs is probed here by simulation of monodisperse Brownian hard-sphere suspensions using accelerated Stokesian Dynamics. The simulations are performed for particle volume fractions of 0.47≤ϕ≤0.57 at Peclet numbers of 1≤Pe=6πηγa3/kT≤104, where η is the suspending fluid viscosity, γ is the imposed shear rate, a is the sphere radius, and kT is the thermal energy. At Pe≥10, when particle volume fraction is above ϕ≈0.50, the suspensions undergo ordering over extended periods at the onset of flow, with remarkable reduction in the shear viscosity and self-diffusivity. The thixotropic response is a result of microstructural ordering, which is characterized both by the real space pair distribution function and its Fourier transform, the static structure factor. Both show that the particles tend to flow in chains with hexagonal packing in the plane normal to the flow. An order parameter is formulated to...

Structural dependent drag force and orientation prediction for small fractal aggregates

Aggregates settle in viscous fluids in specific directions depending on their morphology. We investigated the settling behavior of fractal aggregates with D f = 1.85 in fluids using the Accelerated Stokesian Dynamics method. The results have been compared with experimental data. A simple equation is proposed which gives the drag force in dependence on the radius of gyration r gyr , the projection area A p and the aggregate orientation during settling. This equation reproduces the data from ASD within ± 10 % for Re <1. Additionally, a new algorithm has been developed which allows a prediction of the orientation of such fractal aggregates provided that they have time enough to orient in the fluid. Moreover, the drag force acting on them can be predicted in a narrow range (maximum error 15%). This algorithm allows a very fast evaluation of the orienting behavior with small deviations.

Short-time transport properties in dense suspensions: From neutral to charge-stabilized colloidal spheres

We present a detailed study of short-time dynamic properties in concentrated suspensions of charge-stabilized and of neutral colloidal spheres. The particles in many of these systems are subject to significant many-body hydrodynamic interactions. A recently developed accelerated Stokesian dynamics (ASD) simulation method is used to calculate hydrodynamic functions, wave-number-dependent collective diffusion coefficients, self-diffusion and sedimentation coefficients, and high-frequency limiting viscosities. The dynamic properties are discussed in dependence on the particle concentration and salt content. Our ASD simulation results are compared with existing theoretical predictions, notably those of the renormalized density fluctuation expansion method of Beenakker and Mazur [Physica A 126, 349 (1984)], and earlier simulation data on hard spheres. The range of applicability and the accuracy of various theoretical expressions for short-time properties are explored through comparison with the simulation data. We analyze, in particular, the validity of generalized Stokes-Einstein relations relating short-time diffusion properties to the high-frequency limiting viscosity, and we point to the distinctly different behavior of de-ionized charge-stabilized systems in comparison to hard spheres.