arXiv subjects

Luca Cipelletti

Publications and source records attributed to Luca Cipelletti.

At least 55 records · Page 3Linked to original sources

arXiv2010

Ultra-long range correlations of the dynamics of jammed soft matter

We use Photon Correlation Imaging, a recently introduced space-resolved dynamic light scattering method, to investigate the spatial correlation of the dynamics of a variety of jammed and glassy soft materials. Strikingly, we find that in deeply jammed soft materials spatial correlations of the dynamics are quite generally ultra-long ranged, extending up to the system size, orders of magnitude larger than any relevant structural length scale, such as the particle size, or the mesh size for colloidal gel systems. This has to be contrasted with the case of molecular, colloidal and granular ``supercooled'' fluids, where spatial correlations of the dynamics extend over a few particles at most. Our findings suggest that ultra long range spatial correlations in the dynamics of a system are directly related to the origin of elasticity. While solid-like systems with entropic elasticity exhibit very moderate correlations, systems with enthalpic elasticity exhibit ultra-long range correlations due to the effective transmission of strains throughout the contact network.

cond-mat.soft↗

arXiv2010

Subdiffusion and intermittent dynamic fluctuations in the aging regime of concentrated hard spheres

We study the nonequilibrium aging dynamics in a system of quasi-hard 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 linear increase of the relaxation time with age. In this aging regime, single particle motion is strongly non-Fickian, with a mean-squared displacement increasing subdiffusively, associated to 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.

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

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

Resolving long-range spatial correlations in jammed colloidal systems using photon correlation imaging

We introduce a new dynamic light scattering method, termed photon correlation imaging, which enables us to resolve the dynamics of soft matter in space and time. We demonstrate photon correlation imaging by investigating the slow dynamics of a quasi two-dimensional coarsening foam made of highly packed, deformable bubbles and a rigid gel network formed by dilute, attractive colloidal particles. We find the dynamics of both systems to be determined by intermittent rearrangement events. For the foam, the rearrangements extend over a few bubbles, but a small dynamical correlation is observed up to macroscopic length scales. For the gel, dynamical correlations extend up to the system size. These results indicate that dynamical correlations can be extremely long-ranged in jammed systems and point to the key role of mechanical properties in determining their nature.

cond-mat.soft↗

arXiv2008

Direct-space investigation of the ultraslow ballistic dynamics of a soft glass

We use light microscopy to investigate the aging dynamics of a glass made of closely packed soft spheres, following a rapid transition from a fluid to a solid-like state. By measuring time-resolved, coarse-grained displacements fields, we identify two classes of dynamical events, corresponding to reversible and irreversible rearrangements, respectively. The reversible events are due to the small, experimentally unavoidable fluctuations of the temperature imposed to the sample, leading to transient thermal expansions and contractions that cause shear deformations. The irreversible events are plastic rearrangements, induced by the repeated shear cycles. We show that the displacement due to the irreversible rearrangements grows linearly with time, both on average and at a local level. The velocity associated with this ballistic motion decreases exponentially with sample age, accounting for the observed slowing down of the dynamics. The displacement field due to the irreversible rearrangements has a vortex-like structure and is spatially correlated over surprisingly long distances.

cond-mat.soft↗

arXiv2008

Unexpected drop of dynamical heterogeneities in colloidal suspensions approaching the jamming transition

As the glass (in molecular fluids\cite{Donth}) or the jamming (in colloids and grains\cite{LiuNature1998}) transitions are approached, the dynamics slow down dramatically with no marked structural changes. Dynamical heterogeneity (DH) plays a crucial role: structural relaxation occurs through correlated rearrangements of particle ``blobs'' of size $ξ$\cite{WeeksScience2000,DauchotPRL2005,Glotzer,Ediger}. On approaching these transitions, $ξ$ grows in glass-formers\cite{Glotzer,Ediger}, colloids\cite{WeeksScience2000,BerthierScience2005}, and driven granular materials\cite{KeysNaturePhys2007} alike, strengthening the analogies between the glass and the jamming transitions. However, little is known yet on the behavior of DH very close to dynamical arrest. Here, we measure in colloids the maximum of a ``dynamical susceptibility'', $χ^*$, whose growth is usually associated to that of $ξ$\cite{LacevicPRE}. $χ^*$ initially increases with volume fraction $ϕ$, as in\cite{KeysNaturePhys2007}, but strikingly drops dramatically very close to jamming. We show that this unexpected behavior results from the competition between the growth of $ξ$ and the reduced particle displacements associated with rearrangements in very dense suspensions, unveiling a richer-than-expected scenario.

cond-mat.soft↗

arXiv2007

Investigation of $q$-dependent dynamical heterogeneity in a colloidal gel by x-ray photon correlation spectroscopy

We use time-resolved X-Photon Correlation Spectroscopy to investigate the slow dynamics of colloidal gels made of moderately attractive carbon black particles. We show that the slow dynamics is temporally heterogeneous and quantify its fluctuations by measuring the variance $χ$ of the instantaneous intensity correlation function. The amplitude of dynamical fluctuations has a non-monotonic dependence on scattering vector $q$, in stark contrast with recent experiments on strongly attractive colloidal gels [Duri and Cipelletti, \textit{Europhys. Lett.} \textbf{76}, 972 (2006)]. We propose a simple scaling argument for the $q$-dependence of fluctuations in glassy systems that rationalizes these findings.

cond-mat.soft↗

arXiv2007

Adaptive Speckle Imaging Interferometry: a new technique for the analysis of microstructure dynamics, drying processes and coating formation

We describe an extension of multi-speckle diffusing wave spectroscopy adapted to follow the non-stationary microscopic dynamics in drying films and coatings in a very reactive way and with a high dynamic range. We call this technique "Adaptive Speckle Imaging Interferometry". We introduce an efficient tool, the inter-image distance, to evaluate the speckle dynamics, and the concept of "speckle rate" (SR, in Hz) to quantify this dynamics. The adaptive algorithm plots a simple kinetics, the time evolution of the SR, providing a non-invasive characterization of drying phenomena. A new commercial instrument, called HORUS(R), based on ASII and specialized in the analysis of film formation and drying processes is presented.

cond-mat.soft↗

arXiv2006

Origin of the slow dynamics and the aging of a soft glass

We study by light microscopy a soft glass consisting of a compact arrangement of polydisperse elastic spheres. We show that its slow and non-stationary dynamics results from the unavoidable small fluctuations of temperature, which induce intermittent local mechanical shear in the sample, because of thermal expansion and contraction. Temperature-induced shear provokes both reversible and irreversible rearrangements whose amplitude decreases with time, leading to an exponential slowing down of the dynamics with sample age.

cond-mat.soft↗

arXiv2006

Length scale dependence of dynamical heterogeneity in a colloidal fractal gel

We use time-resolved dynamic light scattering to investigate the slow dynamics of a colloidal gel. The final decay of the average intensity autocorrelation function is well described by $g\_2(q,τ)-1 \sim \exp[-(τ/τ\_\mathrm{f})^p]$, with $τ\_\mathrm{f} \sim q^{-1}$ and $p$ decreasing from 1.5 to 1 with increasing $q$. We show that the dynamics is not due to a continuous ballistic process, as proposed in previous works, but rather to rare, intermittent rearrangements. We quantify the dynamical fluctuations resulting from intermittency by means of the variance $χ(τ,q)$ of the instantaneous autocorrelation function, the analogous of the dynamical susceptibility $χ\_4$ studied in glass formers. The amplitude of $χ$ is found to grow linearly with $q$. We propose a simple --yet general-- model of intermittent dynamics that accounts for the $q$ dependence of both the average correlation functions and $χ$.

cond-mat.soft↗

arXiv2006

The Role of Solid Friction in the Sedimentation of Strongly Attractive Colloidal Gels

We study experimentally and theoretically the sedimentation of gels made of strongly aggregated colloidal particles, focussing on the long time behavior, when mechanical equilibrium is asymptotically reached. The asymptotic gel height is found to vary linearly with the initial height, a finding in stark contrast with a recent study on similar gels [Manley \textit{et al.} 2005 \textit{Phys. Rev. Lett.} \textbf{94} 218302]. We show that the asymptotic compaction results from the balance between gravity pull, network elasticity, and solid friction between the gel and the container walls. Based on these ingredients, we propose a simple model to account for the dependence of the height loss on the initial height and volume fraction. As a result of our analysis, we show that the static friction coefficient between the gel and the container walls strongly depends on volume fraction: the higher the volume fraction, the weaker the solid friction. This nonintuitive behavior is explained using simple scaling arguments.

cond-mat.soft↗

arXiv2005

Direct experimental evidence of a growing length scale accompanying the glass transition

Understanding glass formation is a challenge because the existence of a true glass state, distinct from liquid and solid, remains elusive: Glasses are liquids that have become too viscous to flow. An old idea, as yet unproven experimentally, is that the dynamics becomes sluggish as the glass transition approaches because increasingly larger regions of the material have to move simultaneously to allow flow. We introduce new multipoint dynamical susceptibilities to estimate quantitatively the size of these regions and provide direct experimental evidence that the glass formation of molecular liquids and colloidal suspensions is accompanied by growing dynamic correlation length scales.

cond-mat.stat-mech↗

arXiv2005

Time Resolved Correlation measurements of temporally heterogeneous dynamics

Time Resolved Correlation (TRC) is a recently introduced light scattering technique that allows to detect and quantify dynamic heterogeneities. The technique is based on the analysis of the temporal evolution of the speckle pattern generated by the light scattered by a sample, which is quantified by $c\_I(t,τ)$, the degree of correlation between speckle images recorded at time $t$ and $t+τ$. Heterogeneous dynamics results in significant fluctuations of $c\_I(t,τ)$ with time $t$. We describe how to optimize TRC measurements and how to detect and avoid possible artifacts. The statistical properties of the fluctuations of $c\_I$ are analyzed by studying their variance, probability distribution function, and time autocorrelation function. We show that these quantities are affected by a noise contribution due to the finite number $N$ of detected speckles. We propose and demonstrate a method to correct for the noise contribution, based on a $N\to \infty$ extrapolation scheme. Examples from both homogeneous and heterogeneous dynamics are provided. Connections with recent numerical and analytical works on heterogeneous glassy dynamics are briefly discussed.

cond-mat.soft↗

arXiv2005

Aging and ultra-slow equilibration in concentrated colloidal hard spheres

We study the dynamic behaviour of concentrated colloidal hard spheres using Time Resolved Correlation, a light scattering technique that can detect the slow evolution of the dynamics in out-of-equilibrium systems. Surprisingly, equilibrium is reached a very long time after sample initialization, the non-stationary regime lasting up to three orders of magnitude more than the relaxation time of the system. Before reaching equilibrium, the system displays unusual aging behaviour. The intermediate scattering function decays faster than exponentially and its relaxation time evolves non-monotonically with sample age.

cond-mat.soft↗

arXiv2005

Slow dynamics in glassy soft matter

Measuring, characterizing and modelling the slow dynamics of glassy soft matter is a great challenge, with an impact that ranges from industrial applications to fundamental issues in modern statistical physics, such as the glass transition and the description of out-of-equilibrium systems. Although our understanding of these phenomena is still far from complete, recent simulations and novel theoretical approaches and experimental methods have shed new light on the dynamics of soft glassy materials. In this paper, we review the work of the last few years, with an emphasis on experiments in four distinct and yet related areas: the existence of two different glass states (attractive and repulsive), the dynamics of systems very far from equilibrium, the effect of an external perturbation on glassy materials, and dynamical heterogeneity.

cond-mat.soft↗

arXiv2004

Intrinsic aging and effective viscosity in the slow dynamics of a soft glass with tunable elasticity

We investigate by rheology and light scattering the influence of the elastic modulus, $G_0$, on the slow dynamics and the aging of a soft glass. We show that the slow dynamics and the aging can be entirely described by the evolution of an effective viscosity, $η_{eff}$, defined as the characteristic time measured in a stress relaxation experiment times $G_0$. At all time, $η_{eff}$ is found to be independent of $G_0$, of elastic perturbations, and of the rate at which the sample is quenched in the glassy phase. We propose a simple model that links $η_{eff}$ to the internal stress built up at the fluid-to-solid transition.

cond-mat.soft↗

arXiv2004

Fluctations and noise in time-resolved light scattering experiments : measuring temporally heterogeneous dynamics

We use Time Resolved Correlation (TRC), a recently introduced light scattering method, to study the dynamics of a variety of jammed, or glassy, soft materials. The output of a TRC experiment is cI(t,tau), the time series of the degree of correlation between the speckle patterns generated by the light scattered at time t and t+tau. We characterize the fluctuations of cI by calculating their Probability Density Function, their variance as a function of the lag tau, and their time autocorrelation function. The comparison between these quantities for a Brownian sample and for jammed materials indicate unambiguously that the slow dynamics measured in soft glasses is temporally heterogeneous. The analogies with recent experimental, numerical and theoretical work on temporal heterogeneity in the glassy dynamics are briefly discussed.

cond-mat.soft↗