We report rheological measurements of a noncolloidal particle suspension in a Newtonian solvent at 40% solid volume fraction. An anomalous, frequency-dependent complex viscosity is found under oscillatory shear (OS) flow, whereas a constant dynamic viscosity is found under the same shear rates in steady shear (SS) flow. We show that this contradiction arises from the underlying microstructural difference between OS and SS, mediated by weak interparticle forces. Discrete element simulations of proxy particle suspensions confirm this hypothesis and reveal an adhesion-induced, shear thinning mechanism with a -1/5 slope, only in OS, in agreement with experiments.
Recent experiments report that slowly-sheared noncolloidal particle suspensions can exhibit unexpected rate($ω$)-dependent complex viscosities in oscillatory shear, despite a constant relative viscosity in steady shear. Using a minimal hydrodynamic model, we show that a weak interparticle attraction reproduces this behavior. At volume fractions $ϕ=20\sim50$%, the complex viscosities in both experiments and simulations display power-law reductions in shear, with a $ϕ$-dependent exponent maximum at $ϕ=40$%, resulting from the interplay between hydrodynamic, collision and adhesive interactions. F…
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 rhe…
We investigate the impact of nanoparticle roughness on the phase behaviour of suspensions in models of calcium carbonate nanoparticles. We use a Derjaguin approach that incorporates roughness effects and interactions between the nanoparticles modelled with a combination of DLVO forces and hydration forces, derived using experimental data and atomistic molecular dynamics simulations, respectively. Roughness effects, such as atomic steps or terraces appearing in mineral surfaces result in very different effective inter-nanoparticle potentials. Using stochastic Langevin Dynamics computer simulati…
Acoustic modulation of shear thickening transition in dense adhesive suspensions
ENSL, CNRS, Laboratoire de Physique（法国国家科学研究中心里昂高等师范学院物理实验室）；Holcim Innovation Center（豪瑞创新中心）；Department of Polymer Engineering, IPC, University of Minho（米尼奥大学高分子工程系）
The dynamics of an adhesive two-dimensional vesicle doublet under various flow conditions is investigated numerically using a high-order, adaptive-in-time boundary integral method. In a quiescent flow, two nearby vesicles move slowly towards each other under the adhesive potential, pushing out fluid between them to form a vesicle doublet at equilibrium. A lubrication analysis on such draining of a thin film gives the dependencies of draining time on adhesion strength and separation distance that are in good agreement with numerical results. In a planar extensional flow we find a stable vesicle…
We show that a suspension of non-Brownian calcite particles in glycerol-water mixtures can be tuned continuously from being a yield-stress suspension to a shear-thickening suspension--without a measurable yield stress--by the addition of various surfactants. We interpret our results within a recent theoretical framework that models the rheological effects of stress-dependent constraints on inter-particle motion. Bare calcite particle suspensions are found to have finite yield stresses. In these suspensions, frictional contacts that constrain inter-particle sliding form at an infinitesimal appl…
Recent studies have highlighted that oscillatory and time-dependent shear flows might help increase flowability of dense suspensions. While most focus has been on cross-flows we here study a simple two-dimensional suspensions where we apply simultaneously oscillatory and stationary shear along the same direction. We first show that the viscosities in this set-up significantly decrease with an increasing magnitude of the oscillations, contrary to previous claims. The decrease can be attributed to the large decrease in the number of contacts and an altered microstructure as the magnitude of the …
Oscillatory shear has been widely used to study the rheological properties of suspensions under unsteady shear. Furthermore, recent works have shown that oscillatory flows can improve the flowability of dense suspensions. While most studies have been done under constant volume we here study oscillatory shear flows of a two-dimensional suspensions using a normal pressure-controlled set-up. To characterise the rheology, we introduce both a complex macroscopic friction coefficient $μ^{*}$, following the convention of the complex viscosity $η^{*}$, and a shear-rate averaged viscous number $J'$. Th…
We report direct measurements of spatially resolved surface stresses of a dense suspension during large amplitude oscillatory shear (LAOS) in the discontinuous shear thickening regime using boundary stress microscopy. Consistent with previous studies, bulk rheology shows a dramatic increase in the complex viscosity above a frequency-dependent critical strain. We find that the viscosity increase is coincident with that appearance of large heterogeneous boundary stresses, indicative of the formation of transient solid-like phases (SLPs) on spatial scales large compared to the particle size. The …
We study the rheological response of dense suspensions of elliptical particles, with an aspect ratio equal to 3, under oscillatory shear flows and imposed pressure by numerical simulations. Like for the isotropic particles, we find that the oscillatory shear flows respect the Cox-Merz rule at large oscillatory strains but differ at low strains, with a lower viscosity than the steady shear and higher shear jamming packing fractions. However, unlike the isotropic cases (i.e., discs and spheres), frictionless ellipses get dynamically arrested in their initial orientational configuration at small …
Using the method of Brownian dynamics, we investigate the dynamic properties of a 2d suspension of active disks at high Péclet numbers using active microrheology. In our simulations the tracer particle is driven either by a constant or an oscillatory external force. In the first case, we find that the mobility of the tracer initially appreciably decreases with the external force and then becomes approximately constant for larger forces. For an oscillatory driving force we find that the dynamic mobility shows a quite complex behavior -- it displays a highly nonlinear behavior on both the amplit…
Using a combination of theory, experiment and simulation we investigate the nonlinear response of dense colloidal suspensions to large amplitude oscillatory shear flow. The time-dependent stress response is calculated using a recently developed schematic mode-coupling-type theory describing colloidal suspensions under externally applied flow. For finite strain amplitudes the theory generates a nonlinear response, characterized by significant higher harmonic contributions. An important feature of the theory is the prediction of an ideal glass transition at sufficiently strong coupling, which is…
Particle-based simulations of discontinuous shear thickening (DST) and shear jamming (SJ) suspensions are used to study the role of stress-activated constraints, with an emphasis on resistance to gear-like rolling. Rolling friction decreases the volume fraction required for DST and SJ, in quantitative agreement with real-life suspensions with adhesive surface chemistries and "rough" particle shapes. It sets a distinct structure of the frictional force network compared to only sliding friction, and from a dynamical perspective leads to an increase in the velocity correlation length, in part res…
Dense non-Brownian suspensions including both the hydrodynamic interactions and the frictional contacts between particles are numerically studied under simple and oscillatory shears in terms of the lattice Boltzmann method. We successfully reproduce the discontinuous shear thickening (DST) under a simple shear for bulk three-dimensional systems. For our simulation of an oscillatory shear in a quasi-two-dimensional system, we measure the mechanical response when we reduce the strain amplitude after the initial oscillations with a larger strain amplitude. Here, we find the existence of the shear…
The rheological properties of capillary suspensions, suspensions with small amounts of an added immiscible fluid, are dramatically altered with the addition of the secondary fluid. We investigate a capillary suspension to determine how the network ages and restructures at rest and under applied external shear deformation. The present work uses calcium carbonate suspended in silicone oil (11 % solids) with added water as a model system. Aging of capillary suspensions and their response to applied oscillatory shear is distinctly different from particulate gels dominated by the van der Waals forc…
Surface effects are generally prevailing in confined colloidal systems. Here we report on dispersed nanoparticles close to a fluid membrane. Exact results regarding the static organization are derived for a dilute solution of non-adhesive colloids. It is shown that thermal fluctuations of the membrane broaden the density profile, but on average colloids are neither accumulated nor depleted near the surface. The radial correlation function is also evaluated, from which we obtain the effective pair-potential between colloids. This entropically-driven interaction shares many similarities with the…
We present here a microscopic study of the effect of shear on a dense purely repulsive colloidal suspension. We use Multispeckle Diffusing Wave Spectroscopy to monitor the transient motions of colloidal particles after being submitted to an oscillatory strain. This technique proves efficient to record the time evolution of the relaxation times distribution. After a high oscillatory shear, we show that this distribution displays a full aging behavior. Oppositely, when a moderate shear is applied the distribution is modified in a non trivial way. Whereas high shear is able to erase all the sampl…
Of all current detection techniques with nanometer resolution, only X-ray microscopy allows imaging nanoparticles in suspension. Can it also be used to investigate structural dynamics? When studying response to mechanical stimuli, the challenge lies in applying them with precision comparable to spatial resolution. In the first shear experiments performed in an X-ray microscope, we accomplished this by inserting a piezo actuator driven shear cell into the focal plane of a scanning transmission X-ray microscope (STXM). Thus shear-induced reorganization of magnetite nanoparticle aggregates could …
Stress induced yielding/fluidization in disordered solids, characterized by irreversibility and enhanced dissipation, is important for a wide range of industrial and geological processes. Although, such phenomena in thermal systems have been extensively studied, they remain poorly understood for granular solids. Here, using oscillatory shear rheology and in-situ optical imaging, we study energy dissipation in a dense granular suspension of adhesive particles that forms yield stress solids far below the isotropic jamming point obtained in the limit of hard-sphere repulsion. We find interesting …
For optimal application, pressure-sensitive adhesives must have rheological properties in between those of a viscoplastic solid and those of a viscoelastic liquid. Such adhesives can be produced by emulsion polymerisation, resulting in latex particles which are dispersed in water and contain long-chain acrylic polymers. When the emulsion is dried, the latex particles coalesce and an adhesive film is formed. The rheological properties of the dried samples are believed to be dominated by the interface regions between the original latex particles, but the relation between rheology and latex parti…
Magnetorheological fluids (MRF) are suspensions of magnetic particles that solidify in the presence of magnetic fields due to the particles forming chains along field lines. The magnetic forces between particles dominate the solidification process and determine the yield stress of the material. Here, we investigate how reversible chemical links between particles influence MRF yield stress and stiffness through rheological testing in flow and oscillation mode. First, we functionalize particles with phosphonate groups that are expected to link through hydrogen bonding and find that this MRF exhi…
Collections of non-Brownian particles suspended in a viscous fluid and subjected to oscillatory shear at very low Reynolds number have recently been shown to exhibit a remarkable dynamical phase transition separating reversible from irreversible behaviour as the strain amplitude or volume fraction are increased. We present a simple model for this phenomenon, based on which we argue that this transition lies in the universality class of the conserved DP models or, equivalently, the Manna model. This leads to predictions for the scaling behaviour of a large number of experimental observables. No…
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, i…
We show that particle roughness leads to changes in the number, shape and resulting capillary force of liquid bridges in capillary suspensions. We created fluorescently labeled, raspberry-like particles with varying roughness by electrostatically adsorbing silica nanoparticles with sizes between 40 nm and 250 nm on silica microparticles. Rougher particles require more liquid to fill the surface asperities before they form pendular bridges, resulting in smaller and weaker bridges. In a system where the effective bridge volume is adjusted, higher particle roughness leads to less clustered networ…
In a recent work, Wyss, {\it et.al.} [Phys. Rev. Lett., {\bf 98}, 238303 (2007)] have noted a property of `soft solids' under oscillatory shear, the so-called strain-rate frequency superposition (SRFS). We extend this study to the case of soft solids under large-amplitude oscillatory shear (LAOS). We show results from LAOS studies in a monodisperse hydrogel suspension, an aqueous gel, and a biopolymer suspension, and show that constant strain-rate frequency sweep measurements with soft solids can be superimposed onto master curves for higher harmonic moduli, with the {\it same} shift factors a…
We experimentally investigate shear thickening in dense granular suspensions under oscillatory shear. Directly imaging the suspension-air interface, we observe dilation beyond a critical strain $γ_c$ and the end of shear thickening as the maximum confining stress is reached and the contact line moves. Analyzing the shear profile, we extract the viscosity contributions due to hydrodynamics $η_μ$, dilation $η_c$ and sedimentation $η_g$. While $η_g$ governs the shear thinning regime, $η_μ$ and $η_c$ together determine the shear thickening behavior. As the suspending liquid's viscosity varies from…
The onset of thermal convection in a horizontal layer of a colloidal suspension is investigated in terms of a continuum model for binary-fluid mixtures where the viscosity depends on the local concentration of colloidal particles. With an increasing difference between the viscosity at the warmer and the colder boundary the threshold of convection is reduced in the range of positive values of the separation ratio psi with the onset of stationary convection as well as in the range of negative values of psi with an oscillatory Hopf bifurcation. Additionally the convection rolls are shifted downwa…
We study the motion of radially driven fluid-immersed particles in a novel Hele-Shaw cell with open boundaries. The initially uniform suspension forms a striped pattern within a specific range of horizontal oscillation frequencies and for sufficiently large amplitudes. We observe that the initial coarsening dynamics of the stripes gradually slows down and the pattern reaches a steady state after a few minutes. The distance between the stripes in the steady state exhibits an exponentially saturating increase with increased oscillation amplitude or frequency. The width of the stripes decreases a…
Optical tweezers (OTs) can detect pico-Newton range forces operating on a colloidal particle trapped in a medium and have been successfully utilized to investigate complex systems with internal structures. Laponite clay particles in an aqueous medium self-assemble to form microscopic networks over time as electrostatic interactions between the particles gradually evolve in a physical aging process. We investigate the forced movements of an optically trapped micron-sized colloidal probe particle, suspended in an aging Laponite suspension, as the underlying Laponite microstructures gradually dev…
We show that Hertzian particle contacts are the underlying cause of the as-yet-unexplained noninteger power laws in weakly nonlinear rheology. In the medium amplitude oscillatory shear (MAOS) region, the cubic scaling of the leading order nonlinear shear stress ($σ_\mathrm{3} \sim γ_\mathrm{0}^{m_\mathrm{3}}$, $m_\mathrm{3}=3$) is the standard expectation. Expanding on the work by Natalia et al. [J. Rheol. 64 625-635 (2020)], we report an extensive data set of noncubical, noninteger power law scalings $m_\mathrm{3}$ for particle suspensions in two immiscible fluids with a capillary attractive …
In periodically sheared suspensions there is a dynamical phase transition characterized by a critical strain amplitude $γ_c$ between an absorbing state where particle trajectories are reversible and an active state where trajectories are chaotic and diffusive. Repulsive non-hydrodynamic interactions between "colliding" particles' surfaces have been proposed as a source of this broken time reversal symmetry. A simple toy model called Random Organization qualitatively reproduces the dynamical features of this transition. Random Organization and other absorbing state models exhibit hyperuniformit…
Strong effects of the Faraday instability on suspensions of rodlike colloidal particles are reported through measurements of the critical acceleration and of the surface wave amplitude. We show that the transition to parametrically excited surface waves displays discontinuous and hysteretic features. This subcritical behaviour is attributed to the shear-thinning properties of our colloidal suspensions thanks to a phenomenological model based on rheological data under large amplitude oscillatory shear. Birefringence measurements provide direct evidence that Faraday waves induce local nematic or…
Repeated/cyclic shearing can drive amorphous solids to a steady-state encoding a memory of the applied strain amplitude. However, recent experiments find that the effect of such memory formation on the mechanical properties of the bulk material is rather weak. Here we study the memory effect in a yield stress solid formed by a dense suspension of cornstarch particles in paraffin oil. Under cyclic shear, the system evolves towards a steady-state showing training-induced strain stiffening and plasticity. A readout reveals that the system encodes a strong memory of the training amplitude as indic…
From suspensions to porous multilayers: microstructure formation and particle packing in drying colloidal films
Helmholtz Institute Erlangen-Nürnberg for Renewable Energy (IET-2), Forschungszentrum Jülich（于利希研究中心埃尔朗根-纽伦堡亥姆霍兹可再生能源研究所（IET-2））；Friedrich-Alexander-Universität Erlangen-Nürnberg（埃尔朗根-纽伦堡弗里德里希·亚历山大大学）
In this work the ageing dynamics of soft solids of aqueous suspension of laponite has been investigated under the oscillatory stress field. We observed that at small stresses elastic and viscous moduli showed a steady rise with the elastic modulus increasing at a faster rate than the viscous modulus. However at higher stresses both the moduli underwent a sudden rise by several orders of magnitude with the onset of rise getting shifted to a higher age for a larger shear stress. We believe that the observed behavior is due to interaction of barrier height distribution of the potential energy wel…
Self-propelled microorganisms, such as unicellular algae or bacteria, swim along their director relative to the fluid velocity. Under a steady shear flow the director rotates in close orbit, a periodic structure that is preserved under an oscillatory shear flow. If the shear flow is subjected to small fluctuations produced by small irregularities in the microchannel or by other swimmers nearby, the director dynamics becomes stochastic. Numerical integration of the swimmer motion shows that there is stochastic resonance: The displacement in the vorticity direction is maximized for a finite nois…
The linear and nonlinear rheological behavior of two rod-like particle suspensions as a function of concentration is studied using small amplitude oscillatory shear, steady shear and capillary breakup extensional rheometry. The rod-like suspensions are composed of fd virus and its mutant fdY21M, which are perfectly monodisperse, with a length on the order of 900 nm. The particles are semi flexible yet differ in their persistence length. The effect of stiffness on the rheological behavior in both, shear and extensional flow, is investigated experimentally. The linear viscoelastic shear data is …
Hypothesis: While the mechanical disruption of microscopic structures in complex fluids by large shear flows has been studied extensively, the effects of applied strains on the dielectric properties of macromolecular aggregates has received far less attention. Simultaneous rheology and dielectric experiments can be employed to study the dynamics of sheared colloidal suspensions over spatiotemporal scales spanning several decades. Experiments: Using a precision impedance analyzer, we study the dielectric behavior of strongly sheared aqueous suspensions of thermoreversible hydrogel poly(N-isopro…
Dense suspensions tend to shear jam at large packing fractions. However, it has recently been shown that various oscillation protocols can unjam as well as reduce viscosity and dissipation. In this numerical work, we ask ourselves what is the optimum shear protocol in terms of dissipation. We show that many cruising protocols' dissipation are similar to shear protocols with a steady primary shear and superimposed cross oscillations, even though the latter's viscosity reduction is more considerable. Furthermore, we find that alternating between primary and perpendicular oscillations yields a mu…
We investigate the nonequilibrium behavior of dense, plastic-crystalline suspensions of mildly anisotropic colloidal hard dumbbells under the action of an oscillatory shear field by employing Brownian dynamics computer simulations. In particular, we extend previous investigations, where we uncovered novel nonequilibrium phase transitions, to other aspect ratios and to a larger nonequilibrium parameter space, that is, a wider range of strains and shear frequencies. We compare and discuss selected results in the context of novel scattering and rheological experiments. Both simulations and experi…
Thermoresponsive poly(N-isopropylacrylamide) (PNIPAM) particles of a nearly constant swelling ratio and with polydispersity indices (PDIs) varying over a wide range (7.4% - 48.9%) are synthesized to study the effects of polydispersity on the dynamics of suspensions of soft PNIPAM colloidal particles. The PNIPAM particles are characterized using dynamic light scattering (DLS) and scanning electron microscopy (SEM). The zero shear viscosity ($η_{0}$) data of these colloidal suspensions, estimated from rheometric experiments as a function of the effective volume fraction $ϕ_{eff}$ of the suspensi…
Using high-speed confocal microscopy, we measure the particle positions in a colloidal suspension under large amplitude oscillatory shear. Using the particle positions we quantify the in situ anisotropy of the pair-correlation function -- a measure of the Brownian stress. From these data, we find two distinct types of responses as the system crosses over from equilibrium to far-from-equilibrium states. The first is a nonlinear amplitude saturation that arises from shear-induced advection, while the second is a linear frequency saturation due to competition between suspension relaxation and she…
We examine microstructural and mechanical changes which occur during oscillatory shear flow and reformation after flow cessation of an intermediate volume fraction colloidal gel using rheometry and Brownian Dynamics (BD) simulations. A model depletion colloid-polymer mixture is used, comprising of a hard sphere colloidal suspension with the addition of non-adsorbing linear polymer chains. Results reveal three distinct regimes depending on the strain amplitude of oscillatory shear. Large shear strain amplitudes fully break the structure which results into a more homogenous and stronger gel afte…
We report on the response of a yield stress material, namely a colloidal gel made of attractive carbon black particles, submitted to large amplitude oscillatory shear stress (LAOStress). At a constant stress amplitude well below its apparent yield stress, the gel displays fatigue and progressively turns from an elastic solid to a viscous fluid. The time-resolved analysis of the strain response, of the Fourier spectrum, and of Lissajous plots allows one to define two different timescales $τ_w<τ_f$ associated with the yielding and fluidization of the gel. Coupling rheology to ultrasonic imaging …
