We theoretically investigate glass transition behaviors of the glassy graphene in a wide range of temperature, where this amorphous graphene is described as a hard-sphere fluid. The dynamic arrest of a particle is assumingly caused by interactions with its nearest neighbors and surrounding fluid particles. The assumption allows us to analyze roles of local and collective particle mobility. We calculate the temperature dependence of structural relaxation time and dynamic shear modulus, the dynamic fragility, and the glass transition temperature. In addition, correlations between these physical quantities are comprehensively discussed. Our theoretical calculations agree quantitatively well with recent simulations and Dyre's shoving model.
We study shear banding in soft glassy materials subject to a large amplitude oscillatory shear flow (LAOS). By numerical simulations of the widely used soft glassy rheology model, supplemented by more general physical arguments, we demonstrate strong banding over an extensive range of amplitudes and frequencies of the imposed shear rate $\dotγ(t)=\dotγ_0\cos(ωt)$, even in materials that do not permit banding as their steady state response to a steady imposed shear flow $\dotγ=\dotγ_0=$const. Highly counterintuitively, banding persists in LAOS even in the limit of zero frequency $ω\to 0$, where…
We study theoretically the dynamics of soft glassy materials during the process of stress relaxation following the rapid imposition of a shear strain. By detailed numerical simulations of a mesoscopic soft glassy rheology model and three different simplified continuum fluidity models, we show that a dramatic shear localisation instability arises, in which the strain field suddenly becomes heterogeneous within the sample, accompanied by a precipitous drop in the stress. Remarkably, this instability can arise at extremely long delay times after the strain was applied, due to the long-term memory…
In a recent letter, Govaert et al. examined the relationship between strain hardening modulus $G_r$ and flow stress $σ_{flow}$ for five different glassy polymers. In each case, results for $G_r$ at different strain rates or different temperatures were linearly related to the flow stress. They suggested that this linear relation was inconsistent with simulations. Data from previous publications and new results are presented to show that simulations also yield a linear relation between modulus and flow stress. Possible explanations for the change in the ratio of modulus to flow stress with tempe…
We study theoretically shear banding in soft glassy materials subject to large amplitude time-periodic shear flows, considering separately the protocols of large amplitude oscillatory shear strain, large amplitude square or triangular or sawtooth strain rate, and large amplitude oscillatory shear stress. In each case, we find shear banding to be an important part of the material's flow response for a broad range of values of the frequency $ω$ and amplitude of the imposed oscillation. Crucially, and highly counterintuitively, in the glass phase this persists even to the lowest frequencies acces…
We study the dynamics of a tagged particle in a glassy system under shear. The recently developed integration through transients approach based on mode coupling theory, is continued to arrive at the equations for the tagged particle correlators and the mean squared displacements. The equations are solved numerically for a two dimensional system, including a nonlinear stability analysis of the glass solution, the so called beta-analysis. We perform Brownian Dynamics simulations in 2-D and compare with theory. After switch on, transient glassy correlation functions show strong fingerprints of th…
Soft Glassy Materials, Non Linear Rheology, Lattice Kinetic models, frustrated phase separation} We present numerical simulations based on a Boltzmann kinetic model with competing interactions, aimed at characterizating the rheological properties of soft-glassy materials. The lattice kinetic model is shown to reproduce typical signatures of driven soft-glassy flows in confined geometries, such as Herschel-Bulkley rheology, shear-banding and histeresys. This lends further credit to the present lattice kinetic model as a valuable tool for the theoretical/computational investigation of the rheolo…
Many soft materials, including foams, dense emulsions, micro gel bead suspensions, star polymers, dense packing of surfactant onion micelles, and textured morphologies of liquid crystals, share the basic "glassy" features of structural disorder and metastability. These in turn give rise to several notable features in the low frequency shear rheology (deformation and flow properties) of these materials: in particular, the existence of a yield stress below which the material behaves like a solid, and above which it flows like a liquid. In the last decade, intense experimental activity has also r…
Shear Unfreezing Explains Yielding, Plasticity and Neck Initiation of Glassy Polymers
School of Physics, Beihang University（北京航空航天大学物理学院）；Wenzhou Institute, University of Chinese Academy of Sciences（中国科学院大学温州研究院）；Peng Huanwu Collaborative Center for Research and Education, Beihang University（北京航空航天大学彭恒武科教协同中心）
In this study, we numerically investigated the mechanical responses and trajectories of frictional granular particles under oscillatory shear in the reversible phase where particle trajectories form closed loops below the yielding point. When the friction coefficient is small, the storage modulus exhibits softening, and the loss modulus remains finite in the quasi-static limit. As the friction coefficient increases, the softening and residual loss modulus are suppressed. The storage and loss moduli satisfy scaling laws if they are plotted as functions of the areas of the loop trajectories divi…
Using molecular dynamics simulation of a standard coarse-grained polymer glass model we investigate by means of the stress-fluctuation formalism the shear modulus $μ$ as a function of temperature $T$ and sampling time $Δt$. While the ensemble-averaged modulus $μ(T)$ is found to decrease continuously for all $Δt$ sampled, its standard deviation $δμ(T)$ is non-monotonous with a striking peak at the glass transition. Confirming the effective time-translational invariance of our systems, $μ(Δt)$ can be understood using a weighted integral over the shear-stress relaxation modulus $G(t)$. While the …
The shear modulus of jammed frictional granular materials with the harmonic repulsive interaction under an oscillatory shear is numerically investigated. It is confirmed that the storage modulus, the real part of the shear modulus, for frictional grains with sufficiently small strain amplitude $γ_0$ discontinuously emerges at the jamming transition point. The storage modulus for small $γ_0$ differs from that of frictionless grains even in the zero friction limit, while they are almost identical with each other for sufficiently large $γ_0$, where the transition becomes continuous. The stress-st…
We study the Couette flow of a quasi-2d soft-glassy material in a Hele-Shaw geometry. The material is chosen to be above the jamming point, where a yield stress $σ_Y$ emerges, below which the material deforms elastically and above which it flows like a complex fluid according to a Herschel-Bulkley (HB) rheology. Simultaneously, the effect of the confining plates is modelled as an effective linear friction law, while the walls aside the Hele-Shaw cell are sufficiently close to each other to allow visible cooperativity effects in the velocity profiles (Goyon et al., Nature 454, 84-87 (2008)). Th…
Yield stress fluids display a rich rheological phenomenology. Beyond the defining existence of a yield stress in the steady state flow curve, this includes in many materials rather flat viscoelastic spectra over many decades of frequency in small amplitude oscillatory shear; slow stress relaxation following the sudden imposition of a small shear strain; stress overshoot in shear startup; logarithmic or sublinear power law creep following the imposition of a shear stress below the yield stress; creep followed by yielding after the imposition of a shear stress above the yield stress; richly feat…
We consider the adiabatic evolution of glassy states under external perturbations. Although the formalism we use is very general, we focus here on infinite-dimensional hard spheres where an exact analysis is possible. We consider perturbations of the boundary, i.e. compression or (volume preserving) shear-strain, and we compute the response of glassy states to such perturbations: pressure and shear-stress. We find that both quantities overshoot before the glass state becomes unstable at a spinodal point where it melts into a liquid (or yields). We also estimate the yield stress of the glass. F…
A multi-component lattice Boltzmann model recently introduced (R. Benzi et al. Phys. Rev. Lett 102, 026002 (2009)) to describe some dynamical behaviors of soft-flowing materials is theoretically analyzed. Equilibrium and transport properties are derived within the framework of a continuum free-energy formulation, and checked against numerical simulations. Due to the competition between short-range inter-species repulsion and mid-range intra-species attraction, the model is shown to give rise to a very rich configurational dynamics of the density field, exhibiting numerous features of soft-flow…
From a theoretical study of the mechanical response of jammed materials comprising frictionless and overdamped particles under oscillatory shear, we find that the material becomes soft, and the loss modulus remains finite even in an absorbing state where any irreversible plastic deformation does not exist. The trajectories of the particles in this region exhibit hysteresis loops. We succeed in clarifying the origin of the softening of the material and the residual loss modulus with the aid of Fourier analysis. We also clarify the roles of the yielding point in the softening to distinguish the …
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 study the transient start-up dynamics of a fluidity model which captures the rheological behavior of aging soft glassy materials, in a rectilinear shear flow upon application of step shear rate. We observe that when the steady state flow curve is non-monotonic the system shows transient and/or apparent steady state shear banding in close qualitative agreement with experimental observations. Due to a competetion between aging and rejuvenation during the start up, we show that there is an apparent steady state banding at large times even for shear rates such that the steady state flow curve a…
We study the emergence of critical dynamics in the steady shear rheology of fluidized soft glassy materials. Within a mesoscale elasto-plastic model accounting for a shear band instability, we show how an additional noise can induce a transition from phase separated to homogeneous flow, accompanied by critical-like fluctuations of the macroscopic shear rate. Both macroscopic quantities and fluctuations exhibit power law behaviors in the vicinity of this transition, consistent with previous experimental findings on vibrated granular media. Altogether, our results suggest a generic scenario for …
The temperature dependence of the high-frequency shear modulus measured in the kHz range is compared to the mean-squared displacement measured in the nanosecond range for the two van der Waals bonded glass-forming liquids cumene and 5PPE. This provides an experimental test for the assumption connecting two versions of the shoving model for the non-Arrhenius temperature dependence of the relaxation time in glass formers. The two versions of the model are also tested directly and both are shown to work well for these liquids.
We present an integrated experimental and quantitative theoretical study of the mechanics of self-crosslinked, neutral, repulsive pNIPAM microgel suspensions over concentration (c) range spanning the fluid, glassy and putative "soft jammed" regimes. In the glassy regime we measure a linear elastic dynamic shear modulus over 3 decades which follows an apparent power law concentration dependence G'~$c^{5.64}$, followed by a sharp crossover to a nearly linear growth at high concentrations. We formulate a theoretical approach to address all three regimes within a single conceptual Brownian dynamic…
We numerically study the linear response of two-dimensional frictional granular materials under oscillatory shear. The storage modulus $G'$ and the loss modulus $G''$ in the zero strain rate limit depend on the initial strain amplitude of the oscillatory shear before measurement. The shear jammed state (satisfying $G'>0$) can be observed at an amplitude greater than a critical initial strain amplitude. The fragile state is defined by the emergence of liquid-like and solid-like states depending on the form of the initial shear. In this state, the observed $G'$ after the reduction of the strain …
Many amorphous glassy materials exhibit complex spatio-temporal mechanical response and rheology, characterized by an intermittent stress-strain response and a fluctuating velocity profile. Under quasistatic and athermal deformation protocols this heterogeneous plastic flow was shown to be composed of plastic events of various sizes. In this paper, through numerical study of a 2D LJ amorphous solid, we generalize the study of the heterogeneous dynamics of glassy materials to the finite shear-rate and temperature case. The global mechanical response obtained through the use of Molecular Dynamic…
We study hidden scale invariance in the glassy phase of the Kob-Andersen binary Lennard-Jones system. After cooling below the glass transition, we generate a so-called isomorph from the fluctuations of potential energy and virial in the NVT ensemble -- a set of density, temperature pairs for which structure and dynamics are identical when expressed in appropriate reduced units. To access dynamical features we shear the system using the SLLOD algorithm coupled with Lees-Edwards boundary conditions, and study the statistics of stress fluctuations and the particle displacements transverse to the …
We study the viscoelastic response of amorphous polymers using theory and simulations. By accounting for internal stresses and considering instantaneous normal modes (INMs) within athermal non-affine theory, we make parameter-free predictions of the dynamic viscoelastic moduli obtained in coarse-grained simulations of polymer glasses at non-zero temperatures. The theoretical results show very good correspondence with rheology data collected from molecular dynamics simulations over five orders of magnitude in frequency, with some instabilities that accumulate in the low-frequency part on approa…
Shear modulus of frictionless granular materials near the jamming transition under oscillatory shear is numerically investigated. It is found that the shear modulus $G$ satisfies a scaling law to interpolate between $G \sim (ϕ- ϕ_J)^{1/2}$ and $G \sim γ_0^{-1/2}(ϕ-ϕ_J)$ for a linear spring model of the elastic interaction between contacting grains, where $ϕ$, $ϕ_J$, and $γ_0$ are, respectively, the volume fraction of grains, the fraction at the jamming point, and the amplitude of the oscillatory shear. The linear relation between the shear modulus and $ϕ- ϕ_J$ can be understood by slip avalanc…
We study the response to shear deformations of packings of long spherocylindrical particles that interact via frictional forces with friction coefficient $μ$. The packings are produced and deformed with the help of molecular dynamics simulations combined with minimization techniques performed on a GPU. We calculate the linear shear modulus $g_\infty$, which is orders of magnitude larger than the modulus $g_0$ in the corresponding frictionless system. The motion of the particles responsible for these large frictional forces is governed by and increases with the length $\ell$ of the spherocylind…
The nonlinear rheology of a soft glassy material is captured by its constitutive relation, shear stress vs shear rate, which is most generally obtained by sweeping up or down the shear rate over a finite temporal window. For a huge amount of complex fluids, the up and down sweeps do not superimpose and define a rheological hysteresis loop. By means of extensive rheometry coupled to time-resolved velocimetry, we unravel the local scenario involved in rheological hysteresis for various types of well-studied soft materials. We introduce two observables that quantify the hysteresis in macroscopic …
The shear stress relaxation modulus $G(t)$ may be determined from the shear stress $τ(t)$ after switching on a tiny step strain $γ$ or by inverse Fourier transformation of the storage modulus $G^{\prime}(ω)$ or the loss modulus $G^{\prime\prime}(ω)$ obtained in a standard oscillatory shear experiment at angular frequency $ω$. It is widely assumed that $G(t)$ is equivalent in general to the equilibrium stress autocorrelation function $C(t) = βV \langle δτ(t) δτ(0)\rangle$ which may be readily computed in computer simulations ($β$ being the inverse temperature and $V$ the volume). Focusing on is…
We point out that the instantaneous shear modulus of the shoving model for the non-Arrhenius temperature dependence of viscous liquids' relaxation time is the experimentally accessible high-frequency plateau modulus, not the idealized instantaneous affine shear modulus that cannot be measured. Data for a large selection of metallic glasses are compared to three different versions of the shoving model. The original shear-modulus based version shows a slight correlation to the Poisson ratio, which is eliminated by the energy-landscape formulation of the model in which the bulk modulus plays a mi…
We examine how the distribution of contour lengths and the high-stretch stiffening of individual chain segments affect the macroscopic shear modulus of flexible polymer gels, using a 2D numerical model, in which polymer segments form a triangular network and disorder is introduced by varying their contour lengths. We show that in the relevant parameter range: (i) the non-affine contribution to the shear modulus is negligible, i.e. the Born approximation is satisfactory; (ii) the shear modulus is dominated by the contribution originating from equilibrium chain tensions. Moreover, mechanical equ…
We present a linearized shear-transformation-zone (STZ) theory of glassy dynamics in which the internal STZ transition rates are characterized by a broad distribution of activation barriers. For slowly aging or fully aged systems, the main features of the barrier-height distribution are determined by the effective temperature and other near-equilibrium properties of the configurational degrees of freedom. Our theory accounts for the wide range of relaxation rates observed in both structural glasses and soft glassy materials such as colloidal suspensions. We find that the frequency dependent lo…
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 …
Although glassy relaxation is typically associated with disorder, here we report on a new type of glassy dynamics relating to dislocations within 2-D crystals of colloidal dimers. Previous studies have demonstrated that dislocation motion in dimer crystals is restricted by certain particle orientations. Here, we drag an optically trapped particle through such dimer crystals, creating dislocations. We find a two-stage relaxation response where initially dislocations glide until encountering particles that cage their motion. Subsequent relaxation occurs logarithmically slowly through a second pr…
The problem of effective shear and bulk moduli, of an effective Poison's ratio and of an effective dielectric response in microcomposites of the ferroelastic-dielectric type was studied by us recently. Recently one of us, M. Hudak, studied static mechanical properties of the EVA material theoretically and experimentally. We extend our mentioned study of mechanical response of microcomposites of the type ferrolastics - dielectrics to study of Young modulus and shear wave velocity.
Translational dynamics of two-dimensional glass forming fluids is strongly influenced by soft, long-wavelength fluctuations first recognized by D. Mermin and H. Wagner. As a result of these fluctuations, characteristic features of glassy dynamics, such as plateaus in the mean squared displacement and the self-intermediate scattering function, are absent in two dimensions. In contrast, Mermin-Wagner fluctuations do not influence orientational relaxation and well developed plateaus are observed in orientational correlation functions. It has been suggested that by monitoring translational motion …
Emergent odd viscoelasticity in chiral soft glassy materials
University of Göttingen（哥廷根大学）；Ecole Polytechnique de l’Université de Nantes, LTeN, U6607, Nantes Université（南特大学理工学院，LTeN，U6607）；King’s College London（伦敦国王学院）
Using molecular simulations and theory, we develop an explicit mapping of the contribution of molecular relaxation modes in glassy thermosets to the shear modulus, where the relaxations were tuned by altering the polarity of side groups. Specifically, motions at the domain, segmental, monomer, and atomic levels are taken from molecular dynamics snapshots and directly linked with the viscoelasticity through a framework based in the lattice dynamics of amorphous solids. This unique approach provides direct insight into the roles of chemical groups in the stress response, including the timescale …
The high frequency (instantaneous) shear modulus of three-dimensional Yukawa systems is evaluated in a wide parameter range, from the very weakly coupled gaseous state to the strongly coupled fluid at the crystallization point (Yukwa melt). This allows us to quantify how shear rigidity develops with increasing coupling and inter-particle correlations. The radial distribution functions (RDFs) needed to calculate the excess shear modulus have been obtained from extensive molecular dynamics (MD) simulations. MD results demonstrate that fluid RDFs appear quasi-universal on the curves parallel to t…
