Microrheology of colloidal dispersions: Shape matters

We consider a “probe” particle translating at constant velocity through an otherwise quiescent dispersion of colloidal “bath” particles, as a model for particle-tracking microrheology experiments in the active (nonlinear) regime. The probe is a body of revolution with major and minor semiaxes a and b, respectively, and the bath particles are spheres of radii b. The probe's shape is such that when its major or minor axis is the axis of revolution the excluded-volume, or contact, surface between the probe and a bath particle is a prolate or oblate spheroid, respectively. The moving probe drives the microstructure of the dispersion out of equilibrium; counteracting this is the Brownian diffusion of the bath particles. For a prolate or oblate probe translating along its symmetry axis, we calculate the nonequilibrium microstructure to first order in the volume fraction of bath particles and over the entire range of the Péclet number (Pe), neglecting hydrodynamic interactions. Here, Pe is defined as the non-dimensional velocity of the probe. The microstructure is employed to calculate the average external force on the probe, from which one can infer a “microviscosity” of the dispersion via Stokes drag law. The microviscosity is computed as a function of the aspect ratio of the probe, â=a/b, thereby delineating the role of the probe's shape. For a prolate probe, regardless of the value of â, the microviscosity monotonically decreases, or “velocity thins,” from a Newtonian plateau at small Pe until a second Newtonian plateau is reached as Pe-->[infinity]. After appropriate scaling, we demonstrate this behavior to be in agreement with microrheology studies using spherical probes [Squires and Brady, “A simple paradigm for active and nonlinear microrheology,” Phys. Fluids 17(7), 073101 (2005)] and conventional (macro-)rheological investigations [Bergenholtz et al., “The non-Newtonian rheology of dilute colloidal suspensions,” J. Fluid. Mech. 456, 239–275 (2002)]. For an oblate probe, the microviscosity again transitions between two Newtonian plateaus: for â3.52 the microviscosity at small Pe is less than at large Pe, which suggests it “velocity thickens” as Pe is increased. This anomalous velocity thickening—due entirely to the probe shape—highlights the care needed when designing microrheology experiments with non-spherical probes

On the bulk viscosity of suspensions

The bulk viscosity of a suspension relates the deviation of the trace of the macroscopic or averaged stress from its equilibrium value to the average rate of expansion. For a suspension the equilibrium macroscopic stress is the sum of the fluid pressure and the osmotic pressure of the suspended particles. An average rate of expansion drives the suspension microstructure out of equilibrium and is resisted by the thermal motion of the particles. Expressions are given to compute the bulk viscosity for all concentrations and all expansion rates and shown to be completely analogous to the well-known formulae for the deviatoric macroscopic stress, which are used, for example, to compute the shear viscosity. The effect of rigid spherical particles on the bulk viscosity is determined to second order in volume fraction and to leading order in the Péclet number, which is defined as the expansion rate made dimensionless with the Brownian time scale. A repulsive hard-sphere-like interparticle force reduces the hydrodynamic interactions between particles and decreases the bulk viscosity

A new resistance function for two rigid spheres in a uniform compressible low-Reynolds-number flow

The pressure moment of a rigid particle is defined as the trace of the first moment of the surface stress acting on the particle. We calculate the pressure moments of two unequal rigid spheres immersed in a uniform compressible linear flow, using twin multipole expansions and lubrication theory. Following the practice established in previous studies on two-body hydrodynamic interactions at low Reynolds number, the results are expressed in terms of a new (stresslet) resistance function

Dynamics of forced and unforced autophoretic particles

Chemically active, or autophoretic, particles that isotropically emit or absorb solute molecules undergo spontaneous self-propulsion when their activity is increased beyond a critical P\'{e}clet number ($Pe$). Here, we conduct numerical computations, using a spectral-element based method, of a rigid, spherical autophoretic particle in unsteady rectilinear translation. The particle can be freely suspended (or `unforced') or subject to an external force field (or `forced'). The motion of an unforced particle progresses through four regimes as $Pe$ is increased: quiescent, steady, stirring, and chaos. The particle is stationary in the quiescent regime, and the solute profile is isotropic about the particle. At $Pe=4$ the fore-aft symmetry in the solute profile is broken, resulting in its steady self-propulsion. Our computations indicate that the self-propulsion speed scales linearly with $Pe-4$ near the onset of self-propulsion, as has been predicted in previous studies. A further increase in $Pe$ gives rise to the stirring regime at $Pe\approx27$, where the fluid undergoes recirculation, while the particle remains essentially stationary. As $Pe$ is increased even further, the particle dynamics are marked by chaotic oscillations at $Pe\approx55$ and higher, which we characterize in terms of the mean square displacement and velocity autocorrelation of the particle. Our results for an autophoretic particle under a weak external force are in good agreement with recent asymptotic predictions (Saha, Yariv, and Schnitzer, J. Fluid Mech., vol. 916, A47, 2021). Additionally, we demonstrate that the strength and temporal scheduling of the external force may be tuned to modulate the chaotic dynamics at large $Pe$.Comment: 21 pages, 13 figure

Non-Brownian diffusion and chaotic rheology of autophoretic disks

The dynamics of a two dimensional autophoretic disk is quantified as a minimal model for the chaotic trajectories undertaken by active droplets. Via direct numerical simulations, we show that the mean-square displacement of the disk in a quiescent fluid is linear at long times. Surprisingly, however, this apparently diffusive behavior is non-Brownian, owing to strong cross-correlations in the displacement tensor. The effect of a shear flow field on the chaotic motion of a 2D autophoretic disk is examined. Here, the stresslet on the disk is chaotic for weak shear flows; a dilute suspension of such disks would exhibit a chaotic shear rheology. This chaotic rheology is quenched first into a periodic state and ultimately a steady state as the flow strength is increased

Spontaneous locomotion of a symmetric squirmer

The squirmer is a popular model to analyse the fluid mechanics of a self-propelled object, such as a micro-organism. We demonstrate that some fore-aft symmetric squirmers can spontaneously self-propel above a critical Reynolds number. Specifically, we numerically study the effects of inertia on axisymmetric squirmers characterised by a 'quadrupolar' fore-aft symmetric distribution of surface-slip velocity; under creeping-flow conditions, such squirmers generate a pure stresslet flow, the stresslet sign classifying the squirmer as either a 'pusher' or 'puller.' Assuming axial symmetry, and over the examined range of the Reynolds number $Re$ (defined based upon the magnitude of the quadrupolar squirming), we find that spontaneous symmetry breaking occurs in the puller case above $Re \approx 14.3$, with steady swimming emerging at the threshold via a supercritical pitchfork bifurcation, beyond which the swimming speed grows monotonically with $Re$

Single particle motion in colloidal dispersions: a simple model for active and nonlinear microrheology

The motion of a single Brownian probe particle subjected to a constant external body force and immersed in a dispersion of colloidal particles is studied with a view to providing a simple model for particle tracking microrheology experiments in the active and nonlinear regime. The non-equilibrium configuration of particles induced by the motion of the probe is calculated to first order in the volume fraction of colloidal particles over the entire range of Pe, accounting for hydrodynamic and excluded volume interactions between the probe and dispersion particles. Here, Pe is the dimensionless external force on the probe, or Péclet number, and is a characteristic measure of the degree to which the equilibrium microstructure of the dispersion is distorted. For small Pe, the microstructure (in a reference frame moving with the probe) is primarily dictated by Brownian diffusion and is approximately fore–aft symmetric about the direction of the external force. In the large Pe limit, advection is dominant except in a thin boundary layer in the compressive region of the flow where it is balanced by Brownian diffusion, leading to a highly non-equilibrium microstructure. The computed microstructure is employed to calculate the average translational velocity of the probe, from which the ‘microviscosity’ of the dispersion may be inferred via application of Stokes drag law. For small departures from equilibrium (Pe), the microviscosity ‘force-thins’ proportional to $\hbox{\it Pe}^2$ from its Newtonian low-force plateau. For particles with long-range excluded volume interactions, force-thinning persists until a terminal Newtonian plateau is reached in the limit $\hbox{\it Pe}\,{\rightarrow}\,\infty$. In the case of particles with very short-range excluded volume interactions, the force-thinning ceases at $\hbox{\it Pe}\,{\sim}\, O(1)$, at which point the microviscosity attains a minimum value. Beyond $\hbox{\it Pe}\,{\sim}\, O(1)$, the microstructural boundary layer coincides with the lubrication range of hydrodynamic interactions causing the microviscosity to enter a continuous ‘force-thickening’ regime. The qualitative picture of the microviscosity variation with Pe is in good agreement with theoretical and computational investigations on the ‘macroviscosity’ of sheared colloidal dispersions, and, after appropriate scaling, we are able to make a direct quantitative comparison. This suggests that active tracking microrheology is a valuable tool with which to explore the rich nonlinear rheology of complex fluids