It is well known that jammed soft materials will flow if sheared above their yield stress - think mayonnaise spread on bread - but a complete microscopic description of this seemingly sim- ple process has yet to emerge. What remains elusive is a microscopic framework that explains the macroscopic flow, derived from a 3-D spatially resolved analysis of the dynamics of the droplets or particles that compose the soft material. By combining confocal-rheology experiments on compressed emulsions and numerical simulations, we unravel that the primary microscopic mechanisms for flow are strongly influenced by the rate of the imposed deformation. When shearing fast, small coordinated clusters of droplets move collectively as in a conga line, while at low rates the flow emerges from bursts of droplet rearrangements, correlated over large domains. These regions exhibit complex spatio-temporal correlation patterns that reflect the long range elasticity embedded in the jammed material. These results identify the three-dimensional structure of microscopic rearrangements within sheared soft solids, revealing that the characteristic shape and dynamics of these structures are strongly determined by the rate of the external shear.
Jammed matter is by definition impenetrable to light, rendering the characterization of the 3D geometry difficult. Confocal microscopy of a dyed, refractive index matched emulsion nevertheless allows one to image the jammed system. Here we explain the origin of the mechanism of enhanced fluorescence at the contacts of jammed emulsion droplets in terms of a blue-shifted fluorescence emission band due to the change in the polarity of the interfacial environment. We then use this information to determine the contact network in the emulsion, which models a frictionless jammed system. This enables …
We study dense and highly polydisperse emulsions at droplet volume fractions ϕ>= 0.65. We apply oscillatory shear and observe droplet motion using confocal microscopy. The presence of droplets with sizes several times the mean size dramatically changes the motion of smaller droplets. Both affine and nonaffine droplet motions are observed, with the more nonaffine motion exhibited by the smaller droplets which are pushed around by the larger droplets. Droplet motions are correlated over length scales from one to four times the mean droplet diameter, with larger length scales corresponding to hig…
Using confocal microscopy we investigate the effect of attraction on the packing of polydisperse emulsions under gravity. We find that the distributions of neighbors, coordination number, and local packing fraction as a function of attraction are captured by recently proposed geometrical modeling and statistical mechanics approaches to granular matter. This extends the range of applicability of these tools to polydisperse, attractive jammed packings. Furthermore, the dependence of packing density and average coordination number on the strength of attraction provides the first experimental test…
A thermodynamic formulation of jammed matter is reviewed. Experiments and simulations of compressed emulsions and granular materials are then used to provide a foundation for the thermodynamics.
The micromechanics of a variety of systems experiencing a structural arrest due to their high density could be unified by a thermodynamic framework governing their approach to 'jammed' configurations. The mechanism of supporting an applied stress through the microstructure of these highly packed materials is important in inferring the features responsible for the inhomogeneous stress transmission and testing the universality for all jammed matter. In this paper we present a novel method for measuring the force distribution within the bulk of a compressed emulsion system using confocal microsco…
Porous materials possess numerous useful functions because of their high surface area and ability to modulate the transport of heat, mass, fluids, and electromagnetic waves. Unlike highly ordered structures, disordered porous structures offer the advantages of ease of fabrication and high fault tolerance. Bicontinuous interfacially jammed emulsion gels (bijels) are kinetically trapped disordered biphasic materials that can be converted to porous materials with tunable features. Current methods of bijel fabrication result in domains that are micrometers or larger, and non-uniform in size, limit…
We study long range density fluctuations (hyperuniformity) in two-dimensional jammed packings of bidisperse droplets. Taking advantage of microfluidics, we systematically span a large range of size and concentration ratios of the two droplet populations. We identify various defects increasing long range density fluctuations mainly due to organization of local particle environment. By choosing an appropriate bidispersity, we fabricate materials with a high level of hyperuniformity. Interesting transparency properties of these optimized materials are established based on numerical simulations.
We study the Poiseuille flow of a soft-glassy material above the jamming point, where the material flows like a complex fluid with Herschel- Bulkley rheology. Microscopic plastic rearrangements and the emergence of their spatial correlations induce cooperativity flow behavior whose effect is pronounced in presence of confinement. With the help of lattice Boltzmann numerical simulations of confined dense emulsions, we explore the role of geometrical roughness in providing activation of plastic events close to the boundaries. We probe also the spatial configuration of the fluidity field, a conti…
We perform computational studies of jammed particle packings in two dimensions undergoing isotropic compression using the well-characterized soft particle (SP) model and the deformable particle (DP) model that we developed for compressed bubbles and emulsions. In the SP model, circular particles are allowed to overlap, generating purely repulsive forces. In the DP model, particles minimize their perimeter, while deforming at fixed area to avoid overlap during compression. We directly compare the structural and mechanical properties of jammed particle packings generated using the SP and DP mode…
We study the bulk and shear elastic properties of barely-compressed, "athermal" emulsions and find that the rigidity of the jammed solid fails at remarkably large critical osmotic pressures. The minuscule yield strain and similarly small Brownian particle displacement of solid emulsions close to this transition suggests that this catastrophic failure corresponds to a plastic-entropic instability: the solid becomes too soft and weak to resist the thermal agitation of the droplets that compose it and fails. We propose a modified Lindemann stability criterion to describe this transition and deriv…
Soft, amorphous solids such as tissues, foams, and emulsions are composed of deformable particles. However, the effect of single-particle deformability on the collective behavior of soft solids is still poorly understood. We perform numerical simulations of two-dimensional jammed packings of explicitly deformable particles to study the mechanical response of model soft solids. We find that jammed packings of deformable particles with excess shape degrees of freedom possess low-frequency quartic vibrational modes that stabilize the packings even though they possess fewer interparticle contacts …
We discuss the linear and non-linear rheology of concentrated (sub)microscale emulsions, amorphous disordered solids composed of repulsive and deformable soft colloidal spheres. Based on recent results from simulation and theory, we derive quantitative predictions for the dependences of the elastic shear modulus and the yield stress on the droplet volume fraction. The remarkable agreement with experiments we observe supports the scenario that the repulsive glass and the jammed state can be clearly identified in the rheology of soft spheres at finite temperature while crossing continuously from…
We demonstrate that the elasticity of jammed solids is nonlocal. By forcing frictionless soft sphere packings at varying wavelength, we directly access their transverse and longitudinal compliances without resorting to curve fitting. The observed wavelength dependence of the compliances is incompatible with classical (local) elasticity, and hence quantifies the amplitude of nonlocal effects. Three distinct length scales, two of which diverge, control the amplitude of both nonlocal effects and fluctuations about the mean response. Our results identify new, more accurate constitutive relations f…
We determine the linear viscoelastic response of jammed packings of athermal repulsive viscous spheres, a model for emulsions, wet foams, and soft colloidal suspensions. We numerically measure the complex shear modulus, a fundamental characterization of the response, and demonstrate that low frequency response displays dynamic critical scaling near unjamming. Viscoelastic shear response is governed by the relaxational eigenmodes of a packing. We use scaling arguments to explain the distribution of eigenrates, which develops a divergence at unjamming. We then derive the critical exponents chara…
Force chains, which are quasi-linear self-organised structures carrying large stresses, are ubiquitous in jammed amorphous materials, such as granular materials, foams, emulsions or even assemblies of cells. Predicting where they will form upon mechanical deformation is crucial in order to describe the physical properties of such materials, but remains an open question. Here we demonstrate that graph neural networks (GNN) can accurately infer the location of these force chains in frictionless materials from the local structure prior to deformation, without receiving any information about the i…
The shear response of soft solids can be modeled with linear elasticity, provided the forcing is slow and weak. Both of these approximations must break down when the material loses rigidity, such as in foams and emulsions at their (un)jamming point -- suggesting that the window of linear elastic response near jamming is exceedingly narrow. Yet precisely when and how this breakdown occurs remains unclear. To answer these questions, we perform computer simulations of stress relaxation and shear startup experiments in athermal soft sphere packings, the canonical model for jamming. By systematical…
The postulate of the existence of a jamming phase diagram (Liu and Nagel, Nature 396, 21 EP (1998aa)) provides a theoretical basis for the classification of a wide range of amorphous solids (colloidal, molecular and emulsion glasses, colloidal and polymer gels, foams and granular matter) on the basis of whether these materials are in the jammed or unjammed state. Whilst such simple classification is appealing, it fails to capture that the criterion of rigidity of such amorphous solids may be defined with respect to a particular deformation orientation or mode (i.e. shear, extrusion, consolidat…
The current microscopic picture of plasticity in amorphous materials assumes local failure events to produce displacement fields complying with linear elasticity. Indeed, the flow properties of nonaffine systems such as foams, emulsions and granular materials close to jamming, that produce a fluctuating displacement fields when failing, are still controversial. Here we show, via a thorough numerical investigation of jammed materials, that nonaffinity induces a critical scaling of the flow properties dictated by the distance to the jamming point. We rationalize this critical behavior introducin…
Amorphous glassy materials of diverse nature -- concentrated emulsions, granular materials, pastes, molecular glasses -- display complex flow properties, intermediate between solid and liquid, which are at the root of their use in many applications. A classical feature, well documented yet not really understood, is the very non-linear nature of the flow rule relating stresses and strain rates. Using a microfluidic velocimetry technique, we characterize the flow of thin layers of concentrated emulsions, confined in gaps of different thicknesses by surfaces of different roughness. Beyond the cla…
We present examples of bicontinuous interfacially jammed emulsion gels ("bijels") with a designed gradient in the channel size along the sample. These samples are created by quenching binary fluids which have a gradient in particle concentration along the sample, since the channel size is determined by the local particle concentration. A gradient in local particle concentration is achieved using a two-stage loading process, with different particle volume fractions in each stage. Confocal microscopy and image analysis were used to quantitatively measure the channel size of the bijels. Bijels wi…
Solids deform and fluids flow, but soft glassy materials, such as emulsions, foams, suspensions, and pastes, exhibit an intricate mix of solid and liquid-like behavior. While much progress has been made to understand their elastic (small strain) and flow (infinite strain) properties, such understanding is lacking for the softening and yielding phenomena that connect these asymptotic regimes. Here we present a comprehensive framework for softening and yielding of soft glassy materials, based on extensive numerical simulations of oscillatory rheological tests, and show that two distinct scenario…
In this work, we study the deformation behavior of thin films of various soft glassy materials that are simultaneously subjected to two creep flow fields, rotational shear flow by applying torque and elongational flow by applying normal force. The generic behavior under the combined fields is investigated in different soft glassy materials with diverse microstructure such as: hair gel, emulsion paint, shaving foam and clay suspension. Increase in strength of one stress component while keeping the other constant, not only leads to an expected enhanced deformation in its own direction, but also …
