arXiv subjects

Ludovic Berthier

Publications and source records attributed to Ludovic Berthier.

At least 181 records · Page 10Linked to original sources

arXiv2009

Jamming transitions in amorphous packings of frictionless spheres occur over a continuous range of volume fractions

We numerically produce fully amorphous assemblies of frictionless spheres in three dimensions and study the jamming transition these packings undergo at large volume fractions. We specify four protocols yielding a critical value for the jamming volume fraction which is sharply defined in the limit of large system size, but is different for each protocol. Thus, we directly establish the existence of a continuous range of volume fraction where nonequilibrium jamming transitions occur. However, these jamming transitions share the same critical behaviour. Our results suggest that, even in the absence of partial crystalline ordering, a unique location of a random close packing does not exist, and that volume fraction alone is not sufficient to describe the properties of jammed states.

cond-mat.stat-mech↗

arXiv2009

Nonperturbative effect of attractive forces in viscous liquids

We study the role of the attractive intermolecular forces in the viscous regime of a simple glass-forming liquid by using computer simulations. To this end, we compare the structure and the dynamics of a standard Lennard-Jones glass-forming liquid model with and without the attractive tail of the interaction potentials. The viscous slowing down of the two systems are found to be quantitatively and qualitatively different over a broad density range, whereas the static pair correlations remain close. The common assumption that the behaviour of dense nonassociated liquids is determined by the short-ranged repulsive part of the intermolecular potentials dramatically breaks down for the relaxation in the viscous liquid regime.

cond-mat.stat-mech↗

arXiv2009

Probing the equilibrium dynamics of colloidal hard spheres above the mode-coupling glass transition

We use dynamic light scattering and computer simulations to study equilibrium dynamics and dynamic heterogeneity in concentrated suspensions of colloidal hard spheres. Our study covers an unprecedented density range and spans seven decades in structural relaxation time, $\ta$, including equilibrium easurements above $ϕ_{\rm c}$, the location of the glass transition deduced from fitting our data to mode-coupling theory. Instead of falling out of equilibrium, the system remains ergodic above $ϕ_{\rm c}$ and enters a new dynamical regime where $\ta$ increases with a functional form that was not anticipated by previous experiments, while the amplitude of dynamic heterogeneity grows slower than a power law with $\ta$, as found in molecular glass-formers close to the glass transition.

cond-mat.soft↗

arXiv2009

Compressing nearly hard sphere fluids increases glass fragility

We use molecular dynamics to investigate the glass transition occurring at large volume fraction, phi, and low temperature, T, in assemblies of soft repulsive particles. We find that equilibrium dynamics in the (phi, T) plane obey a form of dynamic scaling in the proximity of a critical point at T=0 and phi=phi_0, which should correspond to the ideal glass transition of hard spheres. This glass point, `point G', is distinct from athermal jamming thresholds. A remarkable consequence of scaling behaviour is that the dynamics at fixed phi passes smoothly from that of a strong glass to that of a very fragile glass as phi increases beyond phi_0. Correlations between fragility and various physical properties are explored.

cond-mat.stat-mech↗

arXiv2009

Dynamic light scattering measurements in the activated regime of dense colloidal hard spheres

We use dynamic light scattering and numerical simulations to study the approach to equilibrium and the equilibrium dynamics of systems of colloidal hard spheres over a broad range of density, from dilute systems up to very concentrated suspensions undergoing glassy dynamics. We discuss several experimental issues (sedimentation, thermal control, non-equilibrium aging effects, dynamic heterogeneity) arising when very large relaxation times are measured. When analyzed over more than seven decades in time, we find that the equilibrium relaxation time, tau_alpha, of our system is described by the algebraic divergence predicted by mode-coupling theory over a window of about three decades. At higher density, tau_alpha increases exponentially with distance to a critical volume fraction phi_0 which is much larger than the mode-coupling singularity. This is reminiscent of the behavior of molecular glass-formers in the activated regime. We compare these results to previous work, carefully discussing crystallization and size polydispersity effects. Our results suggest the absence of a genuine algebraic divergence of tau_alpha in colloidal hard spheres.

cond-mat.soft↗

arXiv2009

The glass transition of dense fluids of hard and compressible spheres

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} ~ 0.592, they are consistent with a divergence of equilibrium relaxation times occurring at phi_0 ~ 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 new 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 non-equilibrium 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.

cond-mat.stat-mech↗

arXiv2008

Static and dynamic properties of a reversible gel

We study a microscopically realistic model of a physical gel and use computer simulations to investigate its static and dynamic properties at thermal equilibrium. The phase diagram comprises a sol phase, a coexistence region ending at a critical point, a gelation line, and an equilibrium gel phase unrelated to phase separation. The global structure of the gel is homogeneous, but the stress is supported by a fractal network. Gelation results in a dramatic slowing down of the dynamics, which can be used to locate the transition, which otherwise shows no structural signatures. Moreover, the equilibrium gel dynamics is highly heterogeneous as a result of the presence of particle families with different mobilities. An analysis of gel dynamics in terms of mobile and arrested particles allows us to elucidate several differences between the dynamics of equilibrium gels and that of glass-formers.

cond-mat.soft↗

arXiv2008

On the relaxation dynamics of glass-forming systems: Insights from computer simulations

We discuss the relaxation dynamics of a simple lattice gas model for glass-forming systems and show that with increasing density of particles this dynamics slows down very quickly. By monitoring the trajectory of tagged particles we find that their motion is very heterogeneous in space and time, leading to regions in space in which there is a fast dynamics and others in which it is slow. We determine how the geometric properties of these quickly relaxing regions depend on density and time. Motivated by this heterogeneous hopping dynamics, we use a simple model, a variant of a continuous time random walk, to characterize the relaxation dynamics. In particular we find from this model that for large displacements the self part of the van Hove function shows an exponential tail, in agreement with recent findings from experiments and simulations of glass-forming systems.

cond-mat.soft↗

arXiv2008

A random walk description of the heterogeneous glassy dynamics of attracting colloids

We study the heterogeneous dynamics of attractive colloidal particles close to the gel transition using confocal microscopy experiments combined with a theoretical statistical analysis. We focus on single particle dynamics and show that the self part of the van Hove distribution function is not the Gaussian expected for a Fickian process, but that it reflects instead the existence, at any given time, of colloids with widely different mobilities. Our confocal microscopy measurements can be described well by a simple analytical model based on a conventional continuous time random walk picture, as already found in several other glassy materials. In particular, the theory successfully accounts for the presence of broad tails in the van Hove distributions that exhibit exponential, rather than Gaussian, decay at large distance.

cond-mat.soft↗

arXiv2007

Spatial correlations in the dynamics of glassforming liquids: Experimental determination of their temperature dependence

We use recently introduced three-point dynamic susceptibilities to obtain an experimental determination of the temperature evolution of the number of molecules, N_corr, that are dynamically correlated during the structural relaxation of supercooled liquids. We first discuss in detail the physical content of three-point functions that relate the sensitivity of the averaged two-time dynamics to external control parameters (such as temperature or density), as well as their connection to the more standard four-point dynamic susceptibility associated with dynamical heterogeneities. We then demonstrate that these functions can be experimentally determined with a good precision. We gather available data to obtain the temperature dependence of N_corr for a large number of supercooled liquids over a wide range of relaxation timescales from the glass transition up to the onset of slow dynamics. We find that N_corr systematically grows when approaching the glass transition. It does so in a modest manner close to the glass transition, which is consistent with an activation-based picture of the dynamics in glassforming materials. For higher temperatures, there appears to be a regime where N_corr behaves as a power-law of the relaxation time. Finally, we find that the dynamic response to density, while being smaller than the dynamic response to temperature, behaves similarly, in agreement with theoretical expectations.

cond-mat.stat-mech↗

arXiv2007

Structure and dynamics in glass-formers: predictability at large length scales

Dynamic heterogeneity in glass-formers has been related to their static structure using the concept of dynamic propensity. We re-examine 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, nor 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 static and dynamic properties of glass-formers at the particle level is vain, but they demonstrate that such connection does exist on larger length scales.

cond-mat.stat-mech↗

arXiv2007

Universal nature of particle displacements close to glass and jamming transitions

We examine the structure of the distribution of single particle displacements (van-Hove function) in a broad class of materials close to glass and jamming transitions. In a wide time window comprising structural relaxation, van-Hove functions reflect the coexistence of slow and fast particles (dynamic heterogeneity). The tails of the distributions exhibit exponential, rather than Gaussian, decay. We argue that this behavior is universal in glassy materials and should be considered the analog, in space, of the stretched exponential decay of time correlation functions. We introduce a dynamical model that describes quantitatively numerical and experimental data in supercooled liquids, colloidal hard spheres and granular materials. The tails of the distributions directly explain the decoupling between translational diffusion and structural relaxation observed in glassy materials.

cond-mat.stat-mech↗

arXiv2007

Amorphous silica modeled with truncated and screened Coulomb interactions: A molecular dynamics simulation study

We show that finite-range alternatives to the standard long-range BKS pair potential for silica might be used in molecular dynamics simulations. We study two such models that can be efficiently simulated since no Ewald summation is required. We first consider the Wolf method, where the Coulomb interactions are truncated at a cutoff distance r_c such that the requirement of charge neutrality holds. Various static and dynamic quantities are computed and compared to results from simulations using Ewald summations. We find very good agreement for r_c ~ 10 Angstroms. For lower values of r_c, the long--range structure is affected which is accompanied by a slight acceleration of dynamic properties. In a second approach, the Coulomb interaction is replaced by an effective Yukawa interaction with two new parameters determined by a force fitting procedure. The same trend as for the Wolf method is seen. However, slightly larger cutoffs have to be used in order to obtain the same accuracy with respect to static and dynamic quantities as for the Wolf method.

cond-mat.stat-mech↗

arXiv2007

Revisiting the slow dynamics of a silica melt using Monte Carlo simulations

We implement a standard Monte Carlo algorithm to study the slow, equilibrium dynamics of a silica melt in a wide temperature regime, from 6100 K down to 2750 K. We find that the average dynamical behaviour 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.

cond-mat.dis-nn↗

arXiv2007

Non-equilibrium dynamics of spin facilitated glass models

We consider the dynamics of spin facilitated models of glasses in the non-equilibrium aging regime following a sudden quench from high to low temperatures. We briefly review known results obtained for the broad class of kinetically constrained models, and then present new results for the behaviour of the one-spin facilitated Fredrickson-Andersen and East models in various spatial dimensions. The time evolution of one-time quantities, such as the energy density, and the detailed properties of two-time correlation and response functions are studied using a combination of theoretical approaches, including exact mappings of master operators and reductions to integrable quantum spin chains, field theory and renormalization group, and independent interval and timescale separation methods. The resulting analytical predictions are confirmed by means of detailed numerical simulations. The models we consider are characterized by trivial static properties, with no finite temperature singularities, but they nevertheless display a surprising variety of dynamic behaviour during aging, which can be directly related to the existence and growth in time of dynamic lengthscales. Well-behaved fluctuation-dissipation ratios can be defined for these models, and we study their properties in detail. We confirm in particular the existence of negative fluctuation-dissipation ratios for a large number of observables. Our results suggest that well-defined violations of fluctuation-dissipation relations, of a purely dynamic origin and unrelated to the thermodynamic concept of effective temperatures, could in general be present in non-equilibrium glassy materials.

cond-mat.stat-mech↗

arXiv2007

Heterogeneous diffusion in a reversible gel

We introduce a microscopically realistic model of a physical gel and use computer simulations to study its static and dynamic properties at thermal equilibrium. The phase diagram comprises a sol phase, a coexistence region ending at a critical point, a gelation line determined by geometric percolation, and an equilibrium gel phase unrelated to phase separation. The global structure of the gel is homogeneous, but the stress is supported by a fractal network. The gel dynamics is highly heterogeneous and we propose a theoretical model to quantitatively describe dynamic heterogeneity in gels. We elucidate several differences between the dynamics of gels and that of glass-formers.

cond-mat.soft↗

arXiv2007

The slow dynamics of glassy materials: Insights from computer simulations

The physics of glasses can be studied from many viewpoints, from material scientists interested in the development of new materials to statistical physicists inventing new theoretical tools to deal with disordered systems. In these lectures I described a variety of physical phenomena observed in actual glassy materials, from disordered magnetic systems to soft gels. Despite the very large gap between experimental and numerical time windows, I showed that computer simulations represent an efficient theoretical tool which can shed light on the microscopic origins of glassy dynamics.

cond-mat.stat-mech↗

arXiv2007

Spontaneous and induced dynamic fluctuations in glass-formers I: General results and dependence on ensemble and dynamics

We study theoretically and numerically a family of multi-point dynamic susceptibilities that quantify the strength and characteristic lengthscales of dynamic heterogeneities in glass-forming materials. We use general theoretical arguments (fluctuation-dissipation relations and symmetries of relevant dynamical field theories) to relate the sensitivity of averaged two-time correlators to temperature and density to spontaneous fluctuations of the local dynamics. Our theoretical results are then compared to molecular dynamics simulations of the Newtonian, Brownian and Monte-Carlo dynamics of two representative glass-forming liquids, a fragile binary Lennard-Jones mixture and a model for the strong glass-former silica. We justify in detail the claim made in [Science 310, 1797 (2005)], that the temperature dependence of correlation functions allows one to extract useful information on dynamic lengthscales in glassy systems. We also discuss some subtle issues associated to the choice of microscopic dynamics and of statistical ensemble through conserved quantities, which are found to play an important role in determining dynamic correlations.

cond-mat.stat-mech↗