By using fluid-kinetic simulations of confined and concentrated emulsion droplets, we investigate the nature of space non-homogeneity in soft-glassy dynamics and provide quantitative measurements of the statistical features of plastic events in the proximity of the yield-stress threshold. Above the yield stress, our results show the existence of a finite stress correlation scale, which can be mapped directly onto the {\it cooperativity scale}, recently introduced in the literature to capture non-local effects in the soft-glassy dynamics. In this regime, the emergence of a separate boundary (wall) rheology with higher fluidity than the bulk, is highlighted in terms of near-wall spontaneous segregation of plastic events. Near the yield stress, where the cooperative scale cannot be estimated with sufficient accuracy, the system shows a clear increase of the stress correlation scale, whereas plastic events exhibit intermittent clustering in time, with no preferential spatial location. A quantitative measurement of the space-time correlation associated with the motion of the interface of the droplets is key to spot the long-range amorphous order at the yield stress threshold.
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 beha…
We compare the slow dynamics of irreversible gels, colloidal gels, glasses and spin glasses by analyzing the behavior of the so called non-linear dynamical susceptibility, a quantity usually introduced to quantitatively characterize the dynamical heterogeneities. In glasses this quantity typically grows with the time, reaches a maximum and then decreases at large time, due to the transient nature of dynamical heterogeneities and to the absence of a diverging static correlation length. We have recently shown that in irreversible gels the dynamical susceptibility is instead an increasing functio…
In this talk I will present a complete theory for the behaviour of large-scale dynamical heterogeneities in glasses. Following the work arXiv:1001.1746 I will show that we can write a (physically motivated) simple stochastic differential equation that is potentially able to explain the behaviour of large scale dynamical heterogeneities in glasses. It turns out that this behaviour is in the same universality class of the dynamics near the endpoint of a metastable phase in a disordered system, as far as reparametrization invariant quantities are concerned. Therefore Large scale dynamical heterog…
Sheared multi-component bulk metallic glasses are characterized by both chemical and structural disorder that define their properties. We investigate the behavior of the local, microstructural elastic modulus across the plastic yielding transition in six Ni-based multi-component glasses, that are characterized by compositional features commonly associated with solid solution formability. We find that elastic modulus fluctuations display consistent percolation characteristics pointing towards universal behavior across chemical compositions and overall yielding sharpness characteristics. Elastic…
Using extensive non-equilibrium molecular dynamics simulations, we investigate a glassforming binary Lennard-Jones mixture under shear. Both supercooled liquids and glasses are considered. Our focus is on the characterization of inhomogeneous flow patterns such as shear bands that appear as a transient response to the external shear. For the supercooled liquids, we analyze the crossover from Newtonian to non-Newtonian behavior with increasing shear rate $\dotγ$. Above a critical shear rate $\dotγ_c$ where a non-Newtonian response sets in, the transient dynamics are associated with the occurren…
By comparing the response to external strains in metallic glasses and in Lenard-Jones glasses we find a quantitative universality of the fundamental plastic instabilities in the athermal, quasistatic limit. Microscopically these two types of glasses are as different as one can imagine, the latter being determined by binary interactions, whereas the former by multiple interactions due to the effect of the electron gas that cannot be disregarded. In spite of this enormous difference the plastic instability is the same saddle-node bifurcation. As a result the statistics of stress and energy drops…
Volume and enthalpy relaxation of glasses after a sudden temperature change has been extensively studied since Kovacs seminal work. One observes an asymmetric approach to equilibrium upon cooling versus heating and, more counter-intuitively, the expansion gap paradox, i.e. a dependence on the initial temperature of the effective relaxation time even close to equilibrium when heating. Here we show that a distinguishable-particles lattice model can capture both the asymmetry and the expansion gap. We quantitatively characterize the energetic states of the particles configurations using a physica…
In a recent paper [S. Mandal et al., Phys. Rev. E 88, 022129 (2013)] the nature of spatial correlations of plasticity in hard sphere glasses was addressed both via computer simulations and in experiments. It was found that the experimentally obtained correlations obey a power law whereas the correlations from simulations are better fitted by an exponential decay. We here provide direct evidence--- via simulations of a hard sphere glass in 2D---that this discrepancy is a consequence of the finite system size in the 3D simulations. By extending the study to a 2D soft disk model at zero temperatu…
By considering the low-frequency vibrational modes of amorphous solids, Manning and Liu [Phys. Rev. Lett. 107, 108302 (2011)] showed that a population of "soft spots" can be identified that are intimately related to plasticity at zero temperature under quasistatic shear. In this work we track individual soft spots with time in a two-dimensional sheared thermal Lennard Jones glass at temperatures ranging from deep in the glassy regime to above the glass transition temperature. We show that the lifetimes of individual soft spots are correlated with the timescale for structural relaxation. We add…
The slow flow of amorphous solids exhibits striking heterogeneities: swift localised particle rearrangements take place in the midst of a more or less homogeneously deforming medium. Recently, experimental as well as numerical work has revealed spatial correlations between these flow heterogeneities. Here, we use molecular dynamics (MD) simulations to characterise the rearrangements and systematically probe their correlations both in time and in space. In particular, these correlations display a four-fold azimuthal symmetry characteristic of shear stress redistribution in an elastic medium and…
We use an analogue of nanoindentation on a colloidal glass to elucidate the incipient plastic deformation of glasses. By tracking the motion of the individual particles in three dimensions, we visualize the strain field and glass structure during the emerging deformation. At the onset of flow, we observe a power-law distribution of strain indicating strongly correlated deformation, and reflecting a critical state of the glass. At later stages, the strain acquires a Gaussian distribution, indicating that plastic events become uncorrelated. Investigation of the glass structure using both static …
In this paper we focus on the mechanical properties of oligomeric glasses (waxes), employing a microscopic model that provides, via numerical simulations, information about the shear modulus of such materials, the failure mechanism via plastic instabilities and about the geometric responses of the oligomers themselves to a mechanical load. We present a microscopic theory that explains the numerically observed phenomena, including an exact theory of the shear modulus and of the plastic instabilities, both local and system spanning. In addition we present a model to explain the geometric changes…
At temperatures well below their glass transition, the deformation properties of bulk metallic glasses are characterised by a sharp transition from elasticity to plasticity, a reproducible yield stress, and an approximately linear decrease of this stress with increasing temperature. In the present work it shown that when the well known properties of the under-cooled liquid regime, in terms of the underlying potential energy landscape, are assumed to be also valid at low temperature, a simple thermal activation model is able to reproduce the observed onset of macro-scopic yield. At these temper…
The plastic deformation of amorphous solids is mediated by localized shear transformations involving small groups of particles rearranging irreversibly in an elastic background. We introduce and compare three different computational methods to extract the size and orientation of these shear transformations in simulations of a two-dimensional (2D) athermal model glass under simple shear. We find that the shear angles are broadly distributed around the macroscopic shear direction, with a more or less Gaussian distribution with a standard deviation of around 20 $\bullet$ about the direction of ma…
We study the effect of physical aging on the mechanical properties of a model polymer glass using molecular dynamics simulations. The creep compliance is determined simultaneously with the structural relaxation under a constant uniaxial load below yield at constant temperature. The model successfully captures universal features found experimentally in polymer glasses, including signatures of mechanical rejuvenation. We analyze microscopic relaxation timescales and show that they exhibit the same aging characteristics as the macroscopic creep compliance. In addition, our model indicates that th…
The dynamical arrest of gels is the consequence of a well defined structural phase transition, leading to the formation of a spanning cluster of bonded particles. The dynamical glass transition, instead, is not accompanied by any clear structural signature. Nevertheless, both transitions are characterized by the emergence of dynamical heterogeneities. Reviewing recent results from numerical simulations, we discuss the behavior of dynamical heterogeneities in different systems and show that a clear connection with the structure exists in the case of gels. The emerging picture may be also releva…
We show that quasi localized low-frequency modes in the vibrational spectrum can be used to construct soft spots, or regions vulnerable to rearrangement, which serve as a universal tool for the identification of flow defects in solids. We show that soft spots not only encode spatial information, via their location, but also directional information, via directors for particles within each soft spot. Single crystals with isolated dislocations exhibit low-frequency phonon modes that localize at the core, and their polarization pattern predicts the motion of atoms during elementary dislocation gli…
Simulations are used to examine the microscopic origins of strain hardening in polymer glasses. While stress-strain curves for a wide range of temperature can be fit to the functional form predicted by entropic network models, many other results are fundamentally inconsistent with the physical picture underlying these models. Stresses are too large to be entropic and have the wrong trend with temperature. The most dramatic hardening at large strains reflects increases in energy as chains are pulled taut between entanglements rather than a change in entropy. A weak entropic stress is only obser…
In amorphous solids at finite temperatures the particles follow chaotic trajectories which, at temperatures sufficiently lower than the glass transition, are trapped in "cages". Averaging their positions for times shorter than the diffusion time, one can define a time-averaged configuration. Under strain or stress, these {\em average} configurations undergo sharp plastic instabilities. In athermal glasses the understanding of plastic instabilities is furnished by the Hessian matrix, its eigenvalues and eigenfunctions. Here we propose an uplifting of Hessian methods to thermal glasses, with the…
Plastic deformation in amorphous solids is known to be carried by stress-induced localized rearrangements of a few tens of particles, accompanied by the conversion of elastic energy to heat. Despite their central role in determining how glasses yield and break, the search for a simple and generally applicable definition of the precursors of those plastic rearrangements -- the so-called shear transformation zones (STZs) -- is still ongoing. Here we present a simple definition of STZs -- based solely on the harmonic approximation of a glass' energy. We explain why and demonstrate directly that o…
The presence of strong local fluctuations -- dynamical heterogeneities -- has been observed near the glass transitions of a wide variety of materials. Here we explore the possible presence of universality in those fluctuations. We compare the statistical properties of fluctuations obtained from numerical simulations of four different glass-forming systems: two polymer systems and two particle systems. We find strong evidence for universality, both in the qualitative behavior of the fluctuations and in the remarkable agreement of the scaling functions describing them.
Dynamical heterogeneities -- strong fluctuations near the glass transition -- are believed to be crucial to explain much of the glass transition phenomenology. One possible hypothesis for their origin is that they emerge from soft (Goldstone) modes associated with a broken continuous symmetry under time reparametrizations. To test this hypothesis, we use numerical simulation data from four glass-forming models to construct coarse grained observables that probe the dynamical heterogeneity, and decompose the fluctuations of these observables into two transverse components associated with the pos…
When strained beyond the linear regime, soft colloidal glasses yield to steady-state plastic flow in a way that is similar to the deformation of conventional amorphous solids. Due to the much larger size of the colloidal particles with respect to the atoms comprising an amorphous solid, colloidal glasses allow to obtain microscopic insight into the nature of the yielding transition, as we illustrate here combining experiments, atomistic simulations, and mesoscopic modeling. Our results unanimously show growing clusters of non-affine deformation percolating at yielding. In agreement with percol…
Plastic instabilities in amorphous materials are often studied using idealized models of binary mixtures that do not capture accurately molecular interactions and bonding present in real glasses. Here we study atomic scale plastic instabilities in a three dimensional molecular dynamics model of silica glass under quasi-static shear. We identify two distinct types of elementary plastic events, one is a standard quasi-localized atomic rearrangement while the second is a bond breaking event that is absent in simplified models of fragile glass formers. Our results show that both plastic events can…
Beijing Normal University（北京师范大学）；Université Grenoble Alpes, CNRS, LIPhy（格勒诺布尔阿尔卑斯大学，法国国家科学研究中心，LIPhy）；University of Montpellier and CNRS（蒙彼利埃大学和法国国家科学研究中心）
We present the relaxation dynamics of glass-forming glycerol mixed with 1.1 nm sized polyhedral oligomeric silsesquioxane (POSS) molecules using dielectric spectroscopy (DS) and two different neutron scattering (NS) techniques. Both, the reorientational dynamics as measured by DS and the density fluctuations detected by NS reveal a broadening of the alpha relaxation when POSS molecules are added. Moreover, we find a significant slowing down of the alpha-relaxation time. These effects are in accord with the heterogeneity scenario considered for the dynamics of glasses and supercooled liquids. T…
Many amorphous materials show spatially heterogenous dynamics, as different regions of the same system relax at different rates. Such a signature, known as Dynamic Heterogeneity, has been crucial to understand the jamming transition in simple model systems and, currently, is considered very promising to characterize more complex fluids of industrial and biological relevance. Unfortunately, measurements of dynamic heterogeneities typically require sophysticated experimental set-ups and are performed by few specialized groups. It is now possible to quantitatively characterize the relaxation proc…
In metallic glasses a clear correlation had been established between plasticity or ductility with the Poisson ratio and alternatively the ratio of the elastic bulk modulus to the shear modulus, K/G. Such a correlation between these two macroscopic mechanical properties is intriguing and is challenging to explain from the dynamics on a microscopic level. Such a microscopic explanation is provided in this paper.
X-ray photon correlation is used to probe the slow dynamics of the glass-former B2O3 across the glass transition. In the undercooled liquid phase the decay times of the measured correlation functions are consistent with visible light scattering results and independent of the incoming flux; in the glass they are instead temperature independent and show a definite dependence on the X-ray flux. This dependence can be exploited to obtain information on the volume occupied by the atoms that move in the glass following an absorption event. The length scale derived in this way, of the order of the na…
Mode coupling theory (MCT) has had notable successes in addressing the rheology of hard-sphere colloidal glasses, and also soft colloidal glasses such as star-polymers. Here, we explore the properties of a recently developed MCT-based schematic constitutive equation under idealized experimental protocols involving single and then double step strains. We find strong deviations from expectations based on factorable, BKZ-type constitutive models. Specifically, a nonvanishing stress remains long after the application of two equal and opposite step strains; this residual stress is a signature of pl…
Reversible switching of the complex network dynamics of proteins is mimicked in selected network glasses and compacted small carbohydrate molecules. Protein transitions occur on long time scales ~ us -ms, evocative of the exponentially large viscosities found in glass-forming supercooled liquids just above the glass transition; in searching for mechanisms for reversibly slowed "geared activation", Kauzmann was led from proteins to glasses. I show here that selected network glasses and small carbohydrate molecules can be used to model such transitions, and elucidate in particular some universal…
Large dilatational hyperelasticity of glasses en route to cavitation failure
Weizmann Institute of Science（魏茨曼科学研究所）；University of Amsterdam（阿姆斯特丹大学）；CNRS, ESPCI Paris, Université PSL, Sorbonne Université, Université Paris Cité（法国国家科学研究中心、巴黎高等物理化工学院、巴黎文理研究大学、索邦大学、巴黎西岱大学）
Molecular dynamics computer simulations of a binary Lennard-Jones glass under shear are presented. The mechanical response of glassy states having different thermal histories is investigated by imposing a wide range of external shear rates, at different temperatures. The stress-strain relations exhibit an overshoot at a strain of around 0.1, marking the yielding of the glass sample and the onset of plastic flow. The amplitude of the overshoot shows a logarithmic behavior with respect to a dimensionless variable, given by the age of the sample times the shear rate. Dynamical heterogeneities hav…
As approaching the glass transition, particle motion in liquids becomes highly heterogeneous and regions with virtually no mobility coexist with liquid-like domains. This complex dynamics is believed to be responsible for different phenomena including non-exponential relaxation and the breakdown of Stokes-Einstein relation. Understanding the relationships between dynamical heterogeneities and local structure in metallic liquids and glasses is a major scientific challenge. Here we use classical molecular dynamics simulations to study the atomic dynamics and microscopic structure of $\mbox{Cu}_{…
Simulations are used to examine the microscopic origins of strain hardening in polymer glasses. While traditional entropic network models can be fit to the total stress, their underlying assumptions are inconsistent with simulation results. There is a substantial energetic contribution to the stress that rises rapidly as segments between entanglements are pulled taut. The thermal component of stress is less sensitive to entanglements, mostly irreversible, and directly related to the rate of local plastic arrangements. Entangled and unentangled chains show the same strain hardening when plotted…
Using molecular dynamics simulation with an angle-dependent Lennard-Jones potential, we study orientational glass with quadrupolar symmetry in mixtures of elliptic particles and circular impurities in two dimensions. With a mild aspect ratio ($=1.2$) and a mild size ratio ($=1.2$), we realize a plastic crystal at relatively high temperature $T$. With further lowering $T$, we find a structural phase transition for very small impurity concentration $c$ and pinned disordered orientations for not small $c$. The ellipses are anchored by the impurities in the planar alignment. With increasing $c$, t…
Glasses exhibit a liquid-like structure but a solid-like rheological response with plastic deformations only occurring beyond yielding. Thus, predicting the rheological behavior from the microscopic structure is difficult, but important for materials science. Here, we consider colloidal suspensions and propose to supplement the static structural information with the local dynamics, namely the rearrangement and breaking of the cage of neighbors. This is quantified by the mean squared nonaffine displacement and the number of particles that remain nearest neighbors for a long time, i.e. long-live…
Frictional granular matter is shown to be fundamentally different in its plastic responses to external strains from generic glasses and amorphous solids without friction. While regular glasses exhibit plastic instabilities due to a vanishing of a real eigenvalue of the Hessian matrix, frictional granular materials can exhibit a previously unnoticed additional mechanism for instabilities, i.e. the appearance of a pair of complex eigenvalues leading to oscillatory exponential growth of perturbations which are tamed by dynamical nonlinearities. This fundamental difference appears crucial for the …
We show that in monomeric supercooled liquids and glasses that are plastically flowing at a constant shear stress $σ$ while being deformed with strain rate $\dotε$, the microscopic structural relaxation time $τ_{\rm str}$ is given by the universal relation $σ/G_\infty\dotε$ with $G_\infty$ a modulus. This equality holds for all rheological regimes from temperatures above the glass transition all the way to the athermal limit, and arises from the competing effects of elastic loading and viscous dissipation. In macromolecular (polymeric) glasses, however, the stress decouples from this relaxatio…
Raman spectroscopy is a useful experimental tool to investigate local deformation and structural changes in SiO$_2$-based glasses. Using a semi-classical modelling of Raman spectra in large samples of silica glasses, we show in this paper that shear plastic flow affects the Raman measurement in the upper part of the spectrum. We relate these changes to structural modifications, as well as a detailed analysis of the vibration modes computed in the same frequency range. These results opens the door to in situ monitoring of plastic damage in silica-based structures.
We present results from microscopic mode coupling theory generalized to colloidal dispersions under shear in an integration-through-transients formalism. Stress-strain curves in start-up shear, flow curves, and normal stresses are calculated with the equilibrium static structure factor as only input. Hard spheres close to their glass transition are considered, as are hard spheres with a short-ranged square-well attraction at their attraction dominated glass transition. The consequences of steric packing and physical bond formation on the linear elastic response, the stress release during yield…
Recent progresses in the description of glassy relaxation and ageing are reviewed for the wide class of network-forming materials such as $GeO_2$, Ge$_x$Se$_{1-x}$, silicates (SiO$_2$-Na$_2$O) or borates (B$_2$O$_3$-Li$_2$O), all of them having an important usefulness in domestic, geological or optoelectronic applications. A brief introduction of the glass transition phenomenology is given, together with the salient features that are revealed both from theory and experiments. Standard experimental methods used for the characterization of the slowing down of the dynamics are reviewed. We then d…
In the three-dimensional Heisenberg spin glass in a random field we study the properties of the inherent structures that are obtained by an instantaneous cooling from infinite temperature. For not too large field the density of states $g(ω)$ develops localized soft {\em plastic} modes and reaches zero as $ω^4$ (for large fiels a gap appears). When we perturb the system adding a force along the softest mode one reaches very similar minima of the energy, separated by small barriers, that appear to be good candidates for classical two-level systems.
The usefulness of glasses, and particularly of metallic glasses, in technological applications is often limited by their toughness, which is defined as the area under the stress vs. strain curve before plastic yielding. Recently toughness was found to increase significantly by the addition of small concentrations of foreign atoms that act as pinning centers. We model this phenomenon at zero temperature and quasi-static straining with randomly positioned particles that participate in the elastic deformation but are pinned in the non-affine return to mechanical equilibrium. We find a very strong…
While perfect crystals may exhibit a purely elastic response to shear all the way to yielding, the response of amorphous solids is punctuated by plastic events. The prevalence of this plasticity depends on the number of particles $N$ of the system, with the average strain interval before the first plastic event, $\overline{Δγ}$, scaling like $N^α$ with $α$ negative: larger samples are more susceptible to plasticity due to more numerous disorder-induced soft spots. In this paper we examine this scaling relation in ultra-stable glasses prepared with the Swap Monte Carlo algorithm, with regard to…
Understanding the fracture toughness of glasses is of prime importance for science and technology. We study it here using extensive atomistic simulations in which the interaction potential, glass transition cooling rate and loading geometry are systematically varied, mimicking a broad range of experimentally accessible properties. Glasses' nonequilibrium mechanical disorder is quantified through $A_{\rm g}$, the dimensionless prefactor of the universal spectrum of nonphononic excitations, which measures the abundance of soft glassy defects that affect plastic deformability. We show that while …
We have employed molecular dynamics simulations based on the TIP4P/2005 water model to investigate the local structural, dynamical, and dielectric properties of the two recently reported body-centered-cubic and face-centered-cubic plastic crystal phases of water. Our results reveal significant differences in the local orientational structure and rotational dynamics of water molecules for the two polymorphs. The probability distributions of trigonal and tetrahedral order parameters exhibit a multi-modal structure, implying the existence of significant local orientational heterogeneities, partic…
We report observations of unusal \emph{first} plastic events in silica and metallic glasses in the shear startup regime at applied strain two orders of magnitude smaller than yield strain. The (non-Affine) particle displacement field during these events have complex real space structure with multiple disconnected cores of high displacement appearing at the \emph{same} applied strain under athermal quasistatic simple shear deformation, and identified by a ``cell based cluster analysis'' method. By monitoring the stress relaxation during the first plastic event by Langevin dynamics simulation, w…
