Obituary for Stefan U. Egelhaaf
This is a tribute to honor Stefan U. Egelhaaf (1963-2023), a pioneer in experimental soft condensed matter physics.
cond-mat.soft↗
arXiv subjects
W. C. K. Poon
Publications and source records attributed to W. C. K. Poon.
Rheology of Polydisperse non-Spherical Graphite Particles Suspended in Mineral Oil
We study the role of filler concentration and microphysics on the rheology of polydisperse flake-graphite particles suspended in Newtonian mineral oil. Under steady shear, our samples exhibit shear thinning and yielding behaviour is observed for volume fractions $ϕ> 0.18$. Time-temperature superposition was observed using an Arrhenius-type horizontal shift factor, giving a flow activation energy that is dependent on the graphite volume fraction, suggesting concentration-dependent contributions to relaxation processes in the suspensions. The flow curves are fitted by a constraint-based model, indicating that the flow behaviour is controlled by frictional and adhesive contacts, with the model suggesting that the adhesive stress is temperature dependent.
cond-mat.soft↗
Electrostatic inactivation of RNA viruses at air-water and liquid-liquid interfaces
Understanding the interactions between viruses and surfaces or interfaces is important, as they provide the principles underpinning the cleaning and disinfection of contaminated surfaces. Yet, the physics of such interactions is currently poorly understood. For instance, there are longstanding experimental observations suggesting that the presence of air-water interfaces can generically inactivate and kill viruses, yet the mechanism underlying this phenomenon remains unknown. Here we use theory and simulations to show that electrostatics provides one such mechanism, and that this is very general. Thus, we predict that the free energy of an RNA virus should increase by several thousands of $k_BT$ as the virion breaches an air-water interface. We also show that the fate of a virus approaching a generic liquid-liquid interface depends strongly on the detailed balance between interfacial and electrostatic forces, which can be tuned, for instance, by choosing different media to contact a virus-laden respiratory droplet. We propose that these results can be used to design effective strategies for surface disinfection. Intriguingly, tunability requires electrostatic and interfacial forces to scale similarly with viral size, which naturally occurs when charges are arranged in a double-shell distribution as in RNA viruses like influenza and all coronaviruses.
cond-mat.soft↗
The role of friction in the yielding of adhesive non-Brownian suspensions
Yielding behavior is well known in attractive colloidal suspensions. Adhesive non-Brownian suspensions, in which the interparticle bonds are due to finite-size contacts, also show yielding behavior. We use a combination of steady-state, oscillatory and shear-reversal rheology to probe the physical origins of yielding in the latter class of materials, and find that yielding is not simply a matter of breaking adhesive bonds, but involves unjamming from a shear-jammed state in which the micro-structure has adapted to the direction of the applied load. Comparison with a recent constraint-based rheology model shows the importance of friction in determining the yield stress, suggesting novel ways to tune the flow of such suspensions.
cond-mat.soft↗
Competing Time Scales Lead to Oscillations in Shear-Thickening Suspensions
Competing time scales generate novelty. Here, we show that a coupling between the time scales imposed by instrument inertia and the formation of inter-particle frictional contacts in shear-thickening suspensions leads to highly asymmetric shear-rate oscillations. Experiments tuning the presence of oscillations by varying the two time-scales validate our model. The observed oscillations give access to a shear-jamming portion of the flow curve that is forbidden in conventional rheometry. Moreover, the oscillation frequency allows us to quantify an intrinsic relaxation time for particle contacts. The coupling of fast contact network dynamics to a slower system variable should be generic to many other areas of dense suspension flow, with instrument inertia providing a paradigmatic example.
cond-mat.soft↗
A constraint-based approach to granular dispersion rheology
We present a phenomenological model for granular suspension rheology in which particle interactions enter as constraints to relative particle motion. By considering constraints that are formed and released by stress respectively, we derive a range of experimental flow curves in a single treatment and predict singularities in viscosity and yield stress consistent with literature data. Fundamentally, we offer a generic description of suspension flow that is independent of bespoke microphysics.
cond-mat.soft↗
A unified description of the rheology of hard-particle suspensions
The rheology of suspensions of Brownian, or colloidal, particles (diameter $d \lesssim 1$ $μ$m) differs markedly from that of larger grains ($d \gtrsim 50$ $μ$m). Each of these two regimes has been separately studied, but the flow of suspensions with intermediate particle sizes (1 $μ\textrm{m} \lesssim d \lesssim 50$ $μ$m), which occur ubiquitously in applications, remains poorly understood. By measuring the rheology of suspensions of hard spheres with a wide range of sizes, we show experimentally that shear thickening drives the transition from colloidal to granular flow across the intermediate size regime. This insight makes possible a unified description of the (non-inertial) rheology of hard spheres over the full size spectrum. Moreover, we are able to test a new theory of friction-induced shear thickening, showing that our data can be well fitted using expressions derived from it.
cond-mat.soft↗
Creep and flow of glasses: strain response linked to the spatial distribution of dynamical heterogeneities
Mechanical properties are of central importance to materials sciences, in particular if they depend on external stimuli. Here we investigate the rheological response of amorphous solids, namely col- loidal glasses, to external forces. Using confocal microscopy and computer simulations, we establish a quantitative link between the macroscopic creep response and the microscopic single-particle dy- namics. We observe dynamical heterogeneities, namely regions of enhanced mobility, which remain localized in the creep regime, but grow for applied stresses leading to steady flow. These different behaviors are also reflected in the average particle dynamics, quantified by the mean squared dis- placement of the individual particles, and the fraction of active regions. Both microscopic quantities are found to be proportional to the macroscopic strain, despite the non-equilibrium and non-linear conditions during creep and the transient regime prior to steady flow.
cond-mat.soft↗
Filling an emulsion drop with motile bacteria
We have measured the spatial distribution of motile Escherichia coli inside spherical water droplets emulsified in oil. At low cell concentrations, the cell density peaks at the water-oil interface; at increasing concentration, the bulk of each droplet fills up uniformly while the surface peak remains. Simulations and theory show that the bulk density results from a `traffic' of cells leaving the surface layer, increasingly due to cell-cell scattering as the surface coverage rises above $\sim 10\%$. Our findings show similarities with the physics of a rarefied gas in a spherical cavity with attractive walls.
cond-mat.soft↗
Enhanced diffusion of nonswimmers in a three-dimensional bath of motile bacteria
We show, using differential dynamic microscopy, that the diffusivity of non-motile cells in a three-dimensional (3D) population of motile E. coli is enhanced by an amount proportional to the active cell flux. While non-motile mutants without flagella and mutants with paralysed flagella have quite different thermal diffusivities and therefore hydrodynamic radii, their diffusivities are enhanced to the same extent by swimmers in the regime of cell densities explored here. Integrating the advective motion of non-swimmers caused by swimmers with finite persistence-length trajectories predicts our observations to within 2%, indicating that fluid entrainment is not relevant for diffusion enhancement in 3D.
physics.bio-ph↗
Phase separation and rotor self-assembly in active particle suspensions
Adding a non-adsorbing polymer to passive colloids induces an attraction between the particles via the `depletion' mechanism. High enough polymer concentrations lead to phase separation. We combine experiments, theory and simulations to demonstrate that using active colloids (such as motile bacteria) dramatically changes the physics of such mixtures. First, significantly stronger inter-particle attraction is needed to cause phase separation. Secondly, the finite size aggregates formed at lower inter-particle attraction show unidirectional rotation. These micro-rotors demonstrate the self assembly of functional structures using active particles. The angular speed of the rotating clusters scales approximately as the inverse of their size, which may be understood theoretically by assuming that the torques exerted by the outermost bacteria in a cluster add up randomly. Our simulations suggest that both the suppression of phase separation and the self assembly of rotors are generic features of aggregating swimmers, and should therefore occur in a variety of biological and synthetic active particle systems.
cond-mat.soft↗
Wall slip and flow of concentrated hard-sphere colloidal suspensions
We present a comprehensive study of the slip and flow of concentrated colloidal suspensions using cone-plate rheometry and simultaneous confocal imaging. In the colloidal glass regime, for smooth, non-stick walls, the solid nature of the suspension causes a transition in the rheology from Herschel-Bulkley (HB) bulk flow behavior at large stress to a Bingham-like slip behavior at low stress, which is suppressed for sufficient colloid-wall attraction or colloid-scale wall roughness. Visualization shows how the slip-shear transition depends on gap size and the boundary conditions at both walls and that partial slip persist well above the yield stress. A phenomenological model, incorporating the Bingham slip law and HB bulk flow, fully accounts for the behavior. Microscopically, the Bingham law is related to a thin (sub-colloidal) lubrication layer at the wall, giving rise to a characteristic dependence of slip parameters on particle size and concentration. We relate this to the suspension's osmotic pressure and yield stress and also analyze the influence of van der Waals interaction. For the largest concentrations, we observe non-uniform flow around the yield stress, in line with recent work on bulk shear-banding of concentrated pastes. We also describe residual slip in concentrated liquid suspensions, where the vanishing yield stress causes coexistence of (weak) slip and bulk shear flow for all measured rates.
cond-mat.soft↗
Migration of chemotactic bacteria in soft agar: role of gel concentration
We study the migration of chemotactic wild-type Escherichia coli populations in semisolid (soft) agar in the concentration range C = 0.15-0.5% (w/v). For C < 0.35%, expanding bacterial colonies display characteristic chemotactic rings. At C = 0.35%, however, bacteria migrate as broad circular bands rather than sharp rings. These are growth/diffusion waves arising because of suppression of chemotaxis by the agar and have not been previously reported experimentally to our knowledge. For C = 0.4-0.5%, expanding colonies do not span the depth of the agar and develop pronounced front instabilities. The migration front speed is weakly dependent on agar concentration at C < 0.25%, but decreases sharply above this value. We discuss these observations in terms of an extended Keller-Segel model for which we derived novel transport parameter expressions accounting for perturbations of the chemotactic response by collisions with the agar. The model makes it possible to fit the observed front speed decay in the range C = 0.15-0.35%, and its solutions qualitatively reproduce the observed transition from chemotactic to growth/diffusion bands. We discuss the implications of our results for the study of bacteria in porous media and for the design of improved bacteriological chemotaxis assays.
cond-mat.soft↗
Polydispersity Effects in Colloid-Polymer Mixtures
We study phase separation and transient gelation in a mixture consisting of polydisperse colloids and non-adsorbing polymers, where the ratio of the average size of the polymer to that of the colloid is approximately 0.063. Unlike what has been reported previously for mixtures with somewhat lower colloid polydispersity, the addition of polymers does not expand the fluid-solid coexistence region. Instead, we find a region of fluid-solid coexistence which has an approximately constant width but an unexpected re-entrant shape. We detect the presence of a metastable gas-liquid binodal, which gives rise to two-stepped crystallization kinetics that can be rationalized as the effect of fractionation. Finally, we find that the separation into multiple coexisting solid phases at high colloid volume fractions predicted by equilibrium statistical mechanics is kinetically suppressed before the system reaches dynamical arrest.
cond-mat.soft↗
Shear banding and flow-concentration coupling in colloidal glasses
We report experiments on hard sphere colloidal glasses that reveal a type of shear banding hitherto unobserved in soft glasses. We present a scenario that relates this to an instability arising from shear-concentration coupling, a mechanism previously thought unimportant in this class of materials. Below a characteristic shear rate $\dotγ_c$ we observe increasingly non-linear velocity profiles and strongly localized flows. We attribute this trend to very slight concentration gradients (likely to evade direct detection) arising in the unstable flow regime. A simple model accounts for both the observed increase of $\dotγ_c$ with concentration, and the fluctuations observed in the flow.
cond-mat.soft↗
Crystallization of hard-sphere glasses
We study by molecular dynamics the interplay between arrest and crystallization in hard spheres. For state points in the plane of volume fraction ($0.54 \leq phi \leq 0.63$) and polydispersity ($0 \leq s \leq 0.085$), we delineate states that spontaneously crystallize from those that do not. For noncrystallizing (or precrystallization) samples we find isodiffusivity lines consistent with an ideal glass transition at $ϕ_g \approx 0.585$, independent of $s$. Despite this, for $s<0.05$, crystallization occurs at $ϕ> ϕ_g$. This happens on time scales for which the system is aging, and a diffusive regime in the mean square displacement is not reached; by those criteria, the system is a glass. Hence, contrary to a widespread assumption in the colloid literature, the occurrence of spontaneous crystallization within a bulk amorphous state does not prove that this state was an ergodic fluid rather than a glass.
cond-mat.soft↗
Hard Spheres: Crystallization and Glass Formation
Motivated by old experiments on colloidal suspensions, we report molecular dynamics simulations of assemblies of hard spheres, addressing crystallization and glass formation. The simulations cover wide ranges of polydispersity s (standard deviation of the particle size distribution divided by its mean) and particle concentration. No crystallization is observed for s > 0.07. For 0.02 < s < 0.07, we find that increasing the polydispersity at a given concentration slows down crystal nucleation. The main effect here is that polydispersity reduces the supersaturation since it tends to stabilise the fluid but to destabilise the crystal. At a given polydispersity (< 0.07) we find three regimes of nucleation: standard nucleation and growth at concentrations in and slightly above the coexistence region; "spinodal nucleation", where the free energy barrier to nucleation appears to be negligible, at intermediate concentrations; and, at the highest concentrations, a new mechanism, still to be fully understood, which only requires small re-arrangement of the particle positions. The cross-over between the second and third regimes occurs at a concentration, around 58% by volume, where the colloid experiments show a marked change in the nature of the crystals formed and the particle dynamics indicate an "ideal" glass transition.
cond-mat.mtrl-sci↗
Slip and flow of hard-sphere colloidal glasses
We study the flow of concentrated hard-sphere colloidal suspensions along smooth, non-stick walls using cone-plate rheometry and simultaneous confocal microscopy. In the glass regime, the global flow shows a transition from Herschel-Bulkley behavior at large shear rate to a characteristic Bingham slip response at small rates, absent for ergodic colloidal fluids. Imaging reveals both the `solid' microstructure during full slip and the local nature of the `slip to shear' transition. Both the local and global flow are described by a phenomenological model, and the associated Bingham slip parameters exhibit characteristic scaling with size and concentration of the hard spheres.
cond-mat.soft↗