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Jamming is a geometric phase transition occurring in dense particle systems in the absence of temperature. We use computer simulations to analyze the effect of thermal fluctuations on several signatures of the transition. We show that scaling laws for bulk and shear moduli only become relevant when thermal fluctuations are extremely small, and propose their relative ratio as a quantitative signature of jamming criticality. Despite the nonequilibrium nature of the transition, we find that thermally induced fluctuations and mechanical responses obey equilibrium fluctuation-dissipation relations near jamming, provided the appropriate fluctuating component of the particle displacements is analyzed. This shows that mechanical moduli can be directly measured from particle positions in mechanically unperturbed packings, and suggests that the definition of a "nonequilibrium index" is unnecessary for amorphous materials. We find that fluctuations of particle displacements are spatially correlated, and define a transverse and a longitudinal correlation length scale which both diverge as the jamming transition is approached. We analyze the frozen component of density fluctuations and find that it displays signatures of nearly hyperuniform behavior at large length scales. This demonstrates that hyperuniformity in jammed packings is unrelated to a vanishing compressibility and explains why it appears remarkably robust against temperature and density variations. Differently from jamming criticality, obstacles preventing the observation of hyperuniformity in colloidal systems do not originate from thermal fluctuations.

We combine computer simulations and analytical theory to investigate the glassy dynamics in dense assemblies of athermal particles evolving under the sole influence of self-propulsion. Our simulations reveal that when the persistence time of the self-propulsion is increased, the local structure becomes more pronounced, whereas the long-time dynamics first accelerates and then slows down. We explain these surprising findings by constructing a nonequilibrium microscopic theory that yields nontrivial predictions for the glassy dynamics. These predictions are in qualitative agreement with the simulations and reveal the importance of steady-state correlations of the local velocities to the nonequilibrium dynamics of dense self-propelled particles.

We use large scale computer simulations and finite-size scaling analysis to study the shear rheology of dense three-dimensional suspensions of frictionless non-Brownian particles in the vicinity of the jamming transition. We perform simulations of soft repulsive particles at constant shear rate, constant pressure, and finite system size and carefully study the asymptotic limits of large system sizes and infinitely hard particle repulsion. We first focus on the asymptotic behavior of the shear viscosity in the hard particle limit. By measuring the viscosity increase over about 5 orders of magnitude, we are able to confirm its asymptotic power law divergence close to the jamming transition. However, a precise determination of the critical density and critical exponent is difficult due to the "multiscaling" behavior of the viscosity. Additionally, finite-size scaling analysis suggests that this divergence is accompanied by a growing correlation length scale, which also diverges algebraically. Finally, we study the effect of particle softness and propose a natural extension of the standard granular rheology, which we test against our simulation data. Close to the jamming transition, this "soft granular rheology" offers a detailed description of the nonlinear rheology of soft particles, which differs from earlier empirical scaling forms.

We introduce a kinetic Monte Carlo model for self-propelled hard disks to capture with minimal ingredients the interplay between thermal fluctuations, excluded volume, and self-propulsion in large assemblies of active particles. We analyze in detail the resulting (density, self-propulsion) nonequilibrium phase diagram over a broad range of parameters. We find that purely repulsive hard disks spontaneously aggregate into fractal clusters as self-propulsion is increased and rationalize the evolution of the average cluster size by developing a kinetic model of reversible aggregation. As density is increased, the nonequilibrium clusters percolate to form a ramified structure reminiscent of a physical gel. We show that the addition of a finite amount of noise is needed to trigger a nonequilibrium phase separation, showing that demixing in active Brownian particles results from a delicate balance between noise, interparticle interactions, and self-propulsion. We show that self-propulsion has a profound influence on the dynamics of the active fluid. We find that the diffusion constant has a nonmonotonic behavior as self-propulsion is increased at finite density and that activity produces strong deviations from Fickian diffusion that persist over large time scales and length scales, suggesting that systems of active particles generically behave as dynamically heterogeneous systems.

We study the relaxation dynamics of a binary Lennard-Jones liquid in the presence of an amorphous wall generated from equilibrium particle configurations. In qualitative agreement with the results presented by Kob et al. [Nat. Phys. 8, 164 (2012).] for a liquid of harmonic spheres, we find that our binary mixture shows a saturation of the dynamical length scale close to the mode-coupling temperature T(c). Furthermore we show that, due to the broken symmetry imposed by the wall, signatures of an additional change in dynamics become apparent at a temperature well above T(c). We provide evidence that this modification in the relaxation dynamics occurs at a recently proposed dynamical crossover temperature T(s) > T(c), which is related to the breakdown of the Stokes-Einstein relation. We find that this dynamical crossover at T(s) is also observed for the harmonic spheres as well as a WCA liquid, showing that it may be a general feature of glass-forming systems.

The yield stress is a defining feature of amorphous materials which is difficult to analyze theoretically, because it stems from the strongly nonlinear response of an arrested solid to an applied deformation. Mode-coupling theory predicts the flow curves of materials undergoing a glass transition and thus offers predictions for the yield stress of amorphous solids. We use this approach to analyze several classes of disordered solids, using simple models of hard-sphere glasses, soft glasses, and metallic glasses for which the mode-coupling predictions can be directly compared to the outcome of numerical measurements. The theory correctly describes the emergence of a yield stress of entropic nature in hard-sphere glasses, and its rapid growth as density approaches random close packing at qualitative level. By contrast, the emergence of solid behavior in soft and metallic glasses, which originates from direct particle interactions is not well described by the theory. We show that similar shortcomings arise in the description of the caging dynamics of the glass phase at rest. We discuss the range of applicability of mode-coupling theory to understand the yield stress and nonlinear rheology of amorphous materials.

We analyze numerically thermal fluctuations of the static overlap between equilibrium configurations in a glass-forming liquid approaching the glass transition. We find that the emergence of slow dynamics near the onset temperature correlates with the development of non-Gaussian probability distributions of overlap fluctuations, measured using both annealed and quenched definitions. Below a critical temperature, a thermodynamic field conjugate to the overlap induces a first-order phase transition, whose existence we numerically demonstrate in the annealed case. These results establish that the approach to the glass transition is accompanied by profound changes in the nature of thermodynamic fluctuations, deconstructing the view that glassy dynamics occurs with little structural evolution.

We present a comprehensive theoretical study of finite-size effects in the relaxation dynamics of glass-forming liquids. Our analysis is motivated by recent theoretical progress regarding the understanding of relevant correlation length scales in liquids approaching the glass transition. We obtain predictions both from general theoretical arguments and from a variety of specific perspectives: mode-coupling theory, kinetically constrained and defect models, and random first-order transition theory. In the last approach, we predict in particular a nonmonotonic evolution of finite-size effects across the mode-coupling crossover due to the competition between mode-coupling and activated relaxation. We study the role of competing relaxation mechanisms in giving rise to nonmonotonic finite-size effects by devising a kinetically constrained model where the proximity to the mode-coupling singularity can be continuously tuned by changing the lattice topology. We use our theoretical findings to interpret the results of extensive molecular dynamics studies of four model liquids with distinct structures and kinetic fragilities. While the less fragile model only displays modest finite-size effects, we find a more significant size dependence evolving with temperature for more fragile models, such as Lennard-Jones particles and soft spheres. Finally, for a binary mixture of harmonic spheres we observe the predicted nonmonotonic temperature evolution of finite-size effects near the fitted mode-coupling singularity, suggesting that the crossover from mode-coupling to activated dynamics is more pronounced for this model. Finally, we discuss the close connection between our results and the recent report of a nonmonotonic temperature evolution of a dynamic length scale near the mode-coupling crossover in harmonic spheres.

We perform molecular dynamics simulations to characterize the occurrence of inhomogeneous shear flows in soft jammed materials. We use rough walls to impose a simple shear flow and study the athermal motion of jammed assemblies of soft particles in two spatial dimensions, both for purely repulsive interactions and in the presence of an additional short-range attraction of varying strength. In steady state, pronounced flow inhomogeneities emerge for all systems when the shear rate becomes small. Deviations from linear flow are stronger in magnitude and become very long lived when the strength of the attraction increases, but differ from permanent shear bands. Flow inhomogeneities occur in a stress window bounded by the dynamic and static yield stress values. Attractive forces enhance the flow heterogeneities because they accelerate stress relaxation, thus effectively moving the system closer to the yield stress regime where inhomogeneities are most pronounced. The present scenario for understanding the effect of particle adhesion on shear localization, which is based on detailed molecular dynamics simulations with realistic particle interactions, differs qualitatively from previous qualitative explanations and ad hoc theoretical modeling., (© 2012 American Physical Society)

We use a random pinning procedure to study amorphous order in two glassy spin models. On increasing the concentration of pinned spins at constant temperature, we find a sharp crossover (but no thermodynamic phase transition) from bulk relaxation to localization in a single state. At low temperatures, both models exhibit scaling behavior. We discuss the growing length and time scales associated with amorphous order, and the fraction of pinned spins required to localize the system in a single state. These results, obtained for finite dimensional interacting models, provide a theoretical scenario for the effect of random pinning that differs qualitatively from previous approaches based either on mean-field, mode-coupling, or renormalization group treatments., (© 2012 American Physical Society)

We analyze static point-to-set correlations in glass-forming liquids. The generic idea is to freeze the position of a set of particles in an equilibrium configuration and to perform sampling in the presence of this additional constraint. Qualitatively different geometries for the confining set of particles are considered and a detailed comparison of resulting static and dynamic correlation functions is performed. Our results reveal the existence of static spatial correlations not detected by conventional two-body correlators, which appear to be decoupled from, and shorter-ranged than, dynamical length scales characterizing dynamic heterogeneity. We find that the dynamics slows down dramatically under confinement, which suggests new ways to investigate the glass transition. Our results indicate that the geometry in which particles are randomly pinned is the best candidate to study static correlations., (© 2012 American Physical Society)

We develop a microscopic theory to analyze the phase behavior and compute correlation functions of dense assemblies of soft repulsive particles both at finite temperature, as in colloidal materials, and at vanishing temperature, a situation relevant for granular materials and emulsions. We use a mean-field statistical mechanical approach which combines elements of liquid state theory to replica calculations to obtain quantitative predictions for the location of phase boundaries, macroscopic thermodynamic properties, and microstructure of the system. We focus, in particular, on the derivation of scaling properties emerging in the vicinity of the jamming transition occurring at large density and zero temperature. The new predictions we obtain for pair correlation functions near contact are tested using computer simulations. Our work also clarifies the conceptual nature of the jamming transition and its relation to the phenomenon of the glass transition observed in atomic liquids.

We use theory and simulations to investigate the existence of amorphous glassy states in ultrasoft colloids. We combine the hypernetted chain approximation with mode-coupling theory to study the dynamic phase diagram of soft repulsive spheres interacting with a Hertzian potential, focusing on low temperatures and large densities. At constant temperature, we find that an amorphous glassy state is entered upon compression, as in colloidal hard spheres, but the glass unexpectedly melts when density increases further. We attribute this reentrant fluid-glass transition to particle softness and correlate this behavior to previously reported anomalies in soft systems, thus emphasizing its generality. The predicted fluid-glass-fluid sequence is confirmed numerically.

In its common implementation, the mode-coupling theory of the glass transition predicts the time evolution of the intermediate scattering functions in viscous liquids on the sole basis of the structural information encoded in two-point density correlations. We provide a critical test of this property and show that the theory fails to describe the strong differences of dynamical behavior seen in two model liquids characterized by very similar pair-correlation functions. Because we use "exact" static information provided by numerical simulations, our results are a direct indication that some important information about the dynamics of viscous liquids is not captured by pair correlations and is thus not described by the mode-coupling theory, even in the temperature regime where the theory is usually applied.

We study the nonequilibrium aging dynamics in a system of quasihard spheres at large density by means of computer simulations. We find that, after a sudden quench to large density, the relaxation time initially increases exponentially with the age of the system. After a surprisingly large crossover time, the system enters the asymptotic aging regime characterized by a nearly linear increase in the relaxation time with age. In this aging regime, single-particle motion is strongly non-fickian, with a mean-squared displacement increasing subdiffusively, associated with broad non-gaussian tails in the distribution of particle displacements. We find that the system ages through temporally intermittent relaxation events, and a detailed finite-size analysis of these collective dynamic fluctuations reveals that these events are not spanning the entire system, but remain spatially localized.

We use computer simulations to study the dynamics of a physical gel at high densities where gelation and the glass transition interfere. We report and provide detailed physical understanding of complex relaxation patterns for time-correlation functions which generically decay in a three-step process. For certain combinations of parameters we find logarithmic decays of the correlators and subdiffusive particle motion.

We combine the hypernetted chain approximation of liquid state theory with the mode-coupling theory of the glass transition to analyze the structure and dynamics of soft spheres interacting via harmonic repulsion. We determine the locus of the fluid-glass dynamic transition in a temperature--volume fraction phase diagram. The zero-temperature (hard-sphere) glass transition influences the dynamics at finite temperatures in its vicinity. This directly implies a form of dynamic scaling for both the average relaxation time and dynamic susceptibilities quantifying dynamic heterogeneity. We discuss several qualitative disagreements between theory and existing simulations at equilibrium. Our theoretical results are, however, very similar to numerical results for the driven athermal dynamics of repulsive spheres, suggesting that "mean-field" mode-coupling approaches might be good starting points to describe these nonequilibrium dynamics.

We use computer simulations to study the glass transition of dense fluids made of polydisperse repulsive spheres. For hard particles, we vary the volume fraction, phi , and use compressible particles to explore finite temperatures, T>0 . In the hard sphere limit, our dynamic data show evidence of an avoided mode-coupling singularity near phi(MCT) is approximately 0.592; they are consistent with a divergence of equilibrium relaxation times occurring at phi(0) is approximately 0.635, but they leave open the existence of a finite temperature singularity for compressible spheres at volume fraction phi>phi(0). Using direct measurements and a scaling procedure, we estimate the equilibrium equation of state for the hard sphere metastable fluid up to phi(0), where pressure remains finite, suggesting that phi(0) corresponds to an ideal glass transition. We use nonequilibrium protocols to explore glassy states above phi(0) and establish the existence of multiple equations of state for the unequilibrated glass of hard spheres, all diverging at different densities in the range phi in [0.642, 0.664]. Glassiness thus results in the existence of a continuum of densities where jamming transitions can occur.

Dynamic heterogeneity in glass formers has been related to their static structure using the concept of dynamic propensity. We reexamine this relationship by analyzing dynamical fluctuations in two atomistic glass formers and two theoretical models. We introduce quantitative statistical indicators which show that the dynamics of individual particles cannot be predicted on the basis of the propensity or by any structural indicator. However, the spatial structure of the propensity field does have predictive power for the spatial correlations associated with dynamic heterogeneity. Our results suggest that the quest for a connection between the static and dynamic properties of glass formers at the particle level is in vain, but they demonstrate that such a connection does exist on larger length scales.

We implement a standard Monte Carlo algorithm to study the slow, equilibrium dynamics of a silica melt in a wide temperature regime, from 6100K down to 2750K . We find that the average dynamical behavior of the system is in quantitative agreement with results obtained from molecular dynamics simulations, at least in the long-time regime corresponding to the alpha -relaxation. By contrast, the strong thermal vibrations related to the boson peak present at short times in molecular dynamics are efficiently suppressed by the Monte Carlo algorithm. This allows us to reconsider silica dynamics in the context of mode-coupling theory, because several shortcomings of the theory were previously attributed to thermal vibrations. A mode-coupling theory analysis of our data is qualitatively correct, but quantitative tests of the theory fail, raising doubts about the very existence of an avoided singularity in this system. We discuss the emergence of dynamic heterogeneity and report detailed measurements of a decoupling between translational diffusion and structural relaxation, and of a growing four-point dynamic susceptibility. Dynamic heterogeneity appears to be less pronounced than in more fragile glass-forming models, but not of a qualitatively different nature.

We suggest the emergence of spatially correlated dynamics in slowly compacting dense granular media by analyzing analytically and numerically multipoint correlation functions in a simple particle model characterized by slow nonequilibrium dynamics. We show that the logarithmically slow dynamics at large times is accompanied by spatially extended dynamic structures that resemble the ones observed in glass-forming liquids and dense colloidal suspensions. This suggests that dynamic heterogeneity is another key common feature present in very different jamming materials.

We study static and dynamic spatial correlations in a two-dimensional spin model with four-body plaquette interactions and standard Glauber dynamics by means of analytic arguments and Monte Carlo simulations. We study in detail the dynamical behavior which becomes glassy at low temperatures, due to the emergence of effective kinetic constraints in a dual representation where spins are mapped to plaquette variables. We study the interplay between nontrivial static correlations of the spins and the dynamic "four-point" correlations usually studied in the context of supercooled liquids. We show that slow dynamics is spatially heterogeneous due to the presence of diverging length scales and scaling, as is also found in kinetically constrained models. This analogy is illustrated by a comparative study of a froth model where the kinetic constraints are imposed.

We compute analytically and numerically the four-point correlation function that characterizes nontrivial cooperative dynamics in glassy systems within several models of glasses: elastoplastic deformations, mode-coupling theory (MCT), collectively rearranging regions (CRR's), diffusing defects, and kinetically constrained models (KCM's). Some features of the four-point susceptibility chi(4) (t) are expected to be universal: at short times we expect a power-law increase in time as t(4) due to ballistic motion (t(2) if the dynamics is Brownian) followed by an elastic regime (most relevant deep in the glass phase) characterized by a t or sqrt[t] growth, depending on whether phonons are propagative or diffusive. We find in both the beta and early alpha regime that chi(4) approximately t(mu), where mu is directly related to the mechanism responsible for relaxation. This regime ends when a maximum of chi(4) is reached at a time t= t(*) of the order of the relaxation time of the system. This maximum is followed by a fast decay to zero at large times. The height of the maximum also follows a power law chi(4) (t(*)) approximately t(*lambda). The value of the exponents mu and lambda allows one to distinguish between different mechanisms. For example, freely diffusing defects in d=3 lead to mu=2 and lambda=1 , whereas the CRR scenario rather predicts either mu=1 or a logarithmic behavior depending on the nature of the nucleation events and a logarithmic behavior of chi(4) (t(*)) . MCT leads to mu=b and lambda=1/gamma , where b and gamma are the standard MCT exponents. We compare our theoretical results with numerical simulations on a Lennard-Jones and a soft-sphere system. Within the limited time scales accessible to numerical simulations, we find that the exponent mu is rather small, mu<1 , with a value in reasonable agreement with the MCT predictions, but not with the prediction of simple diffusive defect models, KCM's with noncooperative defects, and CRR's. Experimental and numerical determination of chi(4) (t) for longer time scales and lower temperatures would yield highly valuable information on the glass formation mechanism.

We derive a dynamic field theory for a kinetically constrained model, based on the Fredrickson-Andersen model, which we expect to describe the properties of an Arrhenius (strong) supercooled liquid at the coarse-grained level. We study this field theory using the renormalization group. For mesoscopic length and time scales, and for space dimension d>/=2 , the behavior of the model is governed by a zero-temperature dynamical critical point in the directed percolation universality class. We argue that in d=1 its behavior is that of compact directed percolation. We perform detailed numerical simulations of the corresponding Fredrickson-Andersen model on the lattice in various dimensions, and find reasonable quantitative agreement with the field theory predictions.

We numerically obtain a quantitative demonstration that development of spatial correlations of mobility as temperature is lowered is responsible for the "decoupling" of transport properties of supercooled liquids. This result further demonstrates the necessity of a spatial description of the glass formation and therefore seriously challenges a number of popular alternative theoretical descriptions.

We show that the various crossovers between dynamical regimes observed in experiments and simulations of supercooled liquids can be explained in simple terms from the existence and statistical properties of dynamical heterogeneities. We confirm that dynamic heterogeneity is responsible for the slowing down of glass formers at temperatures well above the dynamic singularity Tc predicted by mode-coupling theory. Our results imply that activated processes govern the long-time dynamics even in the temperature regime where they are neglected by mode-coupling theory. We show that alternative interpretations based on topographic properties of the potential energy landscape are inefficient ways of describing simple physical features which are naturally accounted for within our approach. We show in particular that the reported links between mode coupling and landscape singularities do not exist.

We investigate the relation between two-time multispin correlation and response functions in the nonequilibrium critical dynamics of Ising models in d=1 and d=2 spatial dimensions. In these nonequilibrium situations, the fluctuation-dissipation theorem (FDT) is not satisfied. We find FDT "violations" qualitatively similar to those reported in various glassy materials, but quantitatively dependent on the chosen observable, in contrast to the results obtained in infinite-range glass models. Nevertheless, all FDT violations can be understood by considering separately the contributions from large wave vectors, which are at quasiequilibrium and obey the FDT, and from small wave vectors where a generalized FDT holds with a nontrivial fluctuation-dissipation ratio X infinity. In d=1, we get X(infinity)=1/2 for spin observables, which measure the orientation of domains, while X(infinity)=0 for observables that are sensitive to the domain-wall motion. Numerical simulations in d=2 reveal a unique X infinity approximately equal 0.34 for all observables. Measurement protocols for X infinity are discussed in detail. Our results suggest that the definition of an effective temperature T(eff)=T/X(infinity) for large length scales is generically possible in nonequilibrium critical dynamics.