Using non-equilibrium molecular dynamics simulations we study the yielding behaviour of a model cluster crystal formed by ultrasoft particles under shear. We investigate the evolution of stress as a function of strain for different shear rates, $\dotγ$, and temperatures. The stress-strain relation displays a pronounced maximum at the yielding point; the height of this maximum, $σ_\text{p}$, increases via a power law with an increasing shear range and tends to saturate to a finite value if the limit shear rate goes to zero (at least within the considered temperature range). Interestingly, this behaviour can be captured by the Herschel-Bulkley type model which, for a given temperature, allows us to predict a static yield stress $σ^{0}_\text{p}$ (in the shear rate tending to zero limit), a characteristic timescale $τ_\text{c}$, and the exponent $α$ of the above-mentioned power-law decay of the $σ_\text{p}$ at high shear rates. Furthermore, for different temperatures, the $σ_\text{p}$ can be scaled as functions of $\dotγ$ onto a single master curve when scaled by corresponding $τ_\text{c}$ and $σ_\text{p}^{0}$. Moreover, for a given shear rate, $σ_\text{p}$ displays a logarithmic dependence on temperature. Again, the $σ_\text{p}{-}T$ curves for different shear rates can be scaled on a single logarithmic master curve when scaled by a corresponding fitting parameters.
Blends of multicyclic and linear polymers under biaxial elongational flow were analyzed using coarse-grained molecular dynamics simulations. The multicyclic/linear blends displayed overshoot in the normal stress difference at the start-up of biaxial elongational flow. This overshoot was steeper for multicyclic/linear blends than for our previously reported monocyclic/linear blends [T. Murashima, K. Hagita, and T. Kawakatsu, Macromolecules, 2021, 54, 7210]. Investigation of the origin of the overshoot in the multicyclic/linear blends revealed a different mechanism than that previously observed …
A Force-Level Theory of the Rheology of Entangled Rod and Chain Polymer Liquids. II. Perturbed Reptation, Stress Overshoot, Emergent Convective Constraint Release and Steady State Flow
The mechanical non-linear response of dense Brownian suspensions of polymer gel particles is studied experimentally and by means of numerical simulations. It is shown that the response to the application of a constant shear rate depends on the previous history of the suspension. When the flow starts from a suspension at rest, it exhibits an elastic response followed by a stress overshoot and then a plastic flow regime. Conversely, after flow reversal, the stress overshoot does not occur, and the apparent elastic modulus is reduced while numerical simulations reveal that the anisotropy of the l…
We study theoretically the yielding of sheared amorphous materials as a function of increasing levels of initial sample annealing prior to shear, in three widely used constitutive models and three widely studied annealing protocols. In thermal systems we find a gradual progression, with increasing annealing, from smoothly "ductile" yielding, in which the sample remains homogeneous, to abruptly "brittle" yielding, in which it becomes strongly shear banded. This progression arises from an increase with annealing in the size of an overshoot in the underlying stress-strain curve for homogeneous sh…
Understanding the origin of the unique rheological properties of wheat gluten, the protein fraction of wheat grain, is crucial in bread-making processes and questions scientists since polymeric glutenins. To better understand the respective role of the different classes of proteins in the supramolecular structure of gluten and its link to the material properties, we investigate here concentrated dispersions of gluten proteins in water with a fixed total protein concentration but variable composition in gliadin and glutenin. Linear viscoelasticity measurements show a gradual increase of the vis…
We formulate a microscopic, force-level, activated dynamics-based statistical-mechanical theory for the continuous startup nonlinear shear-rheology of ultra-dense glass-forming hard-sphere fluids and colloidal suspensions in the context of the ECNLE approach. Activated structural relaxation is described as a coupled local-nonlocal event involving caging and longer-range collective elasticity which controls the characteristic stress relaxation time. Theoretical predictions for the deformation-induced mobility enhancement, onset of relaxation acceleration at low values of stress, strain, or shea…
Soft glassy materials such as mayonnaise, wet clays, or dense microgels display under external shear a solid-to-liquid transition. Such a shear-induced transition is often associated with a non-monotonic stress response, in the form of a stress maximum referred to as "stress overshoot". This ubiquitous phenomenon is characterized by the coordinates of the maximum in terms of stress $σ_\text{M}$ and strain $γ_\text{M}$ that both increase as weak power laws of the applied shear rate. Here we rationalize such power-law scalings using a continuum model that predicts two different regimes in the li…
Viscosity overshoot of entangled polymer melts has been observed under shear flow and uniaxial elongational flow, but has never been observed under biaxial elongational flow. We confirmed the presence of viscosity overshoot under biaxial elongational flows observed in a mixed system of ring and linear polymers expressed by coarse-grained molecular dynamics simulations. The overshoot was found to be more pronounced in weakly entangled melts. Furthermore, the threshold strain rate $\dot{\varepsilon}_{\rm th}$ distinguishing linear and nonlinear behaviors was found to be dependent on the linear c…
We investigate dilation-induced surface deformations in a Discontinuous Shear Thickening (DST) suspension to determine the relationship between dilation and stresses in DST. Video is taken at two observation points on the surface of the suspension in a rheometer while shear and normal stresses are measured. A roughened surface of the suspension is observed as particles poke through the liquid-air interface, corresponding to dilation. Dilation events are found to be intermittent and localized spatially. Shear and normal stresses also fluctuate between high- and low-stress states, and dilation i…
Focusing on simulated polymer glasses well below the glass transition, we confirm the validity and the efficiency of the recently proposed simple-average expression $G(t) = μ_A - h(t)$ for the computational determination of the shear stress relaxation modulus $G(t)$. Here, $μ_A = G(0)$ characterizes the affine shear transformation of the system at $t=0$ and $h(t)$ the mean-square displacement of the instantaneous shear stress as a function of time $t$. This relation is seen to be particulary useful for systems with quenched or sluggish transient shear stresses which necessarily arise below the…
We present new general relationships among the material properties of an isotropic material kept in homogeneous stress conditions with hydrostatic pressure and plane shear. The derivation is not limited to the proximity of the zero shear-stress and -strain condition, which allows us to identify the relationship between adiabatic and isothermal shear compliances (inverse of the moduli of rigidity) along with new links, among others, between isobaric and isochoric shear thermal expansion coefficients, heat capacities at constant stress and constant shear strain. Such relationships are important …
Simulations are used to study the steady shear rheology of dense suspensions of frictional particles exhibiting discontinuous shear thickening and shear jamming, in which finite-range cohesive interactions result in a yield stress. We develop a constitutive model that combines yielding behavior and shear thinning at low stress with the frictional shear thickening at high stresses, in good agreement with the simulation results. This work shows that there is a distinct difference between solids below the yield stress and in the shear-jammed state, as the two occur at widely separated stress leve…
In soft amorphous materials, shear cessation after large shear deformation leads to structures having residual shear stress. The origin of these states and the distribution of the local shear stresses within the material is not well understood, despite its importance for the change in material properties and consequent applications. In this work, we use molecular dynamics simulations of a model dense non-Brownian soft amorphous material to probe the non-trivial relaxation process towards a residual stress state. We find that, similar to thermal glasses, an increase in shear rate prior to the s…
The transition between shear-flowing and shear-arrested states of frictional granular matter is studied using constant-stress discrete element simulations. By subjecting a dilute system of frictional grains to a constant external shear stress and pressure, friction-dependent critical shear stress and density are clearly identified with both exhibiting a crossover between low and high friction. The critical shear stress bifurcates two nonequilibrium steady states: (i) steady state shear flow characterized by a constant deformation rate, and (ii) shear arrest characterized by temporally decaying…
Yield stress materials fail when the imposed stress crosses a critical threshold. A well-known dynamical response to the applied stress is the phenomenon of creep where the cumulative deformation grows sublinearly with time, prior to failure or arrest. Using extensive molecular dynamics simulations, we study such response for a model amorphous system, in the athermal limit, and probe how the annealing history of the initial state determines the observed behaviour to an applied shear stress. Further, we analyze the microscopic dynamics in the vicinity of the yield threshold, using large systems…
We observe a novel type of shear banding in the rheology of thixotropic yield-stress fluids that is due to the coupling of both non-locality and thixotropy. The latter is known to lead to shear banding even in homogeneous stress fields, but the bands observed in the presence of non-local effects appear different as the shear rate varies continuously over the shear band. Here, we introduce a simple non-local model for the shear banding (NL-SB), and we implement it for the analysis of micron-scale rheo-MRI velocimetry measurements of a milk microgel suspension in a cone-and-plate geometry. The p…
Many dense particulate suspensions show a stress induced transformation from a liquid-like state to a solid-like shear jammed (SJ) state. However, the underlying particle-scale dynamics leading to such striking, reversible transition of the bulk remains unknown. Here, we study transient stress relaxation behaviour of SJ states formed by a well-characterized dense suspension under a step strain perturbation. We observe a strongly non-exponential relaxation that develops a sharp discontinuous stress drop at short time for high enough peak-stress values. High resolution boundary imaging and norma…
Normal stresses in complex fluids lead to new flow phenomena because they can be comparable to or even larger than the shear stress itself. In addition, they are of paramount importance for formulating and testing constitutive equations for predicting non-viscometric flow behavior. Very little attention has so far been paid to the normal stresses of yield stress fluids, mainly because they are very difficult to measure. We report the first systematic study of the first and second normal stress differences, N1 (>0) and N2 (<0), in both continuous and oscillatory shear of three model yield stres…
