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We report the existence of capillary waves propagating along the boundary between miscible co-flowing fluids. We unveil that the interplay between transient interfacial stresses and confinement drives the progressive transition from the well-known inertial regime, characterized by a wavenumber independent of frequency, $k\sim\omega^{0}$, to an unexpected capillary-wave scaling, $k\sim\omega^{2/3}$. This allows us to measure the effective interfacial tension between miscible fluids and its rapid decay on time scales never probed so far, which we rationalize with a model going beyond square gradient theories., Comment: 20 pages, 11 figures

Colloidal Solids (COLIS) is a state-of-the-art light scattering setup developed for experiments onboard the International Space Station (ISS). COLIS allows for probing the structure and dynamics of soft matter systems on a wide range of length scales, from a few nm to tens of microns, and on time scales from 100 ns to tens of hours. In addition to conventional static and dynamic light scattering, COLIS includes depolarized dynamic light scattering, a small-angle camera, photon correlation imaging, and optical manipulation of thermosensitive samples through an auxiliary near-infrared laser beam, thereby providing a unique platform for probing soft matter systems. We demonstrate COLIS through ground tests on standard Brownian suspensions, and on protein, colloidal glasses, and gel systems similar to those to be used in future ISS experiments.

We present a novel dynamic light scattering setup to probe, with time and space resolution, the microscopic dynamics of soft matter systems confined within millimeter-sized spherical drops. By using an ad-hoc optical layout, we tackle the challenges raised by refraction effects due to the unconventional shape of the samples. We first validate the setup by investigating the dynamics of a suspension of Brownian particles. The dynamics measured at different positions in the drop, and hence different scattering angles, are found to be in excellent agreement with those obtained for the same sample in a conventional light scattering setup. We then demonstrate the setup capabilities by investigating a bead made of a polymer hydrogel undergoing swelling. The gel microscopic dynamics exhibit a space dependence that strongly varies with time elapsed since the beginning of swelling. Initially, the dynamics in the periphery of the bead are much faster than in the core, indicative of non-uniform swelling. As the swelling proceeds, the dynamics slow down and become more spatially homogeneous. By comparing the experimental results to numerical and analytical calculations for the dynamics of a homogeneous, purely elastic sphere undergoing swelling, we establish that the mean square displacement of the gel strands deviates from the affine motion inferred from the macroscopic deformation, evolving from fast diffusive-like dynamics at the onset of swelling to slower, yet supradiffusive, rearrangements at later stages.

Concentrated colloidal suspensions and emulsions are amorphous soft solids, widespread in technological and industrial applications and studied as model systems in physics and material sciences. They are easily fluidized by applying a mechanical stress, undergoing a yielding transition that still lacks a unified description. Here, we investigate yielding in three classes of repulsive soft solids, using analytical and numerical modelling and experiments probing the microscopic dynamics and mechanical response under oscillatory shear. We find that at the microscopic level yielding consists in a transition between two distinct dynamical states, which we rationalize by proposing a lattice model with dynamical coupling between neighboring sites, leading to a unified state diagram for yielding. Leveraging the analogy with Wan der Waals's phase diagram for real gases, we show that distance from a critical point plays a major role in the emergence of first-order-like vs second-order-like features in yielding, thereby reconciling previously contrasting observations on the nature of the transition., Comment: 23 pages, 5 figures

Multiple speckle diffusing wave spectroscopy (MSDWS) can be applied to measure spatially heterogeneous mechanical behavior in soft solids, with high sensitivity to deformation and both spatial and temporal resolution. In this paper, we discuss the mathematical approach behind the quantification of the deformation rate from MSDWS data and provide guidelines for optimizing the selection of experimental parameters in measurements. After validating the method in extensional tests on an elastomer, we provide an example of the potentiality of MSDWS by measuring the spatial distribution of the deformation rate during shear debonding of adhesive tapes. We quantitatively characterize the deformation rate distribution related to shearing and peeling under loading. A highly heterogeneous deformation rate distribution is observed, and time-dependent measurements reveal an increase in deformation localization hundreds of seconds before full debonding. This behavior, previously predicted by theory and simulation, is here demonstrated experimentally for the first time.

Mucus is a biological gel covering the surface of several tissues and insuring key biological functions, including as a protective barrier against dehydration, pathogens penetration, or gastric acids. Mucus biological functioning requires a finely tuned balance between solid-like and fluid-like mechanical response, insured by reversible bonds between mucins, the glycoproteins that form the gel. In living organisms, mucus is subject to various kinds of mechanical stresses, e.g. due to osmosis, bacterial penetration, coughing and gastric peristalsis. However, our knowledge of the effects of stress on mucus is still rudimentary and mostly limited to macroscopic rheological measurements, with no insight into the relevant microscopic mechanisms. Here, we run mechanical tests simultaneously to measurements of the microscopic dynamics of pig gastric mucus. Strikingly, we find that a modest shear stress, within the macroscopic rheological linear regime, dramatically enhances mucus reorganization at the microscopic level, as signalled by a transient acceleration of the microscopic dynamics, by up to two orders of magnitude. We rationalize these findings by proposing a simple yet general model for the dynamics of physical gels under strain and validate its assumptions through numerical simulations of spring networks. These results shed new light on the rearrangement dynamics of mucus at the microscopic scale, with potential implications in phenomena ranging from mucus clearance to bacterial and drug penetration., Comment: To appear in PNAS

We investigate the delayed rupture of biopolymer gels under a constant shear load by simultaneous dynamic light scattering and rheology measurements. We unveil the crucial role of normal stresses built up during gelation: all samples that eventually fracture self-weaken during the gelation process, as revealed by a partial relaxation of the normal stress concomitant to a burst of microscopic plastic rearrangements. Upon applying a shear stress, weakened gels exhibit in the creep regime distinctive signatures in their microscopic dynamics, which anticipate macroscopic fracture by up to thousands of seconds. The dynamics in fracturing gels are faster than those of non-fracturing gels and exhibit large spatio-temporal fluctuations. A spatially localized region with significant plasticity eventually nucleates, expands progressively, and finally invades the whole sample triggering macroscopic failure., Comment: accepted for publication in Physical Review Letters

We exploit the deformation of drops spinning in a denser background fluid to investigate the effective interfacial tension (EIT) between miscible molecular fluids. We find that for sufficiently low interfacial tension, spinning drops develop dumbbell shapes, with two large heads connected by a thinner central body. We show that this shape depends not only on the density and viscosity contrast between the drop and background fluids, but also on the fluid molecular structure, and hence on the stresses developing at their interface due to different molecular interaction. We systematically investigate the dynamics of dumbbell-shaped drops of water-glycerol mixtures spinning in a pure glycerol reservoir. By developing a model for the deformation based on the balance of the shear stress opposing the deformation, the imposed normal stress on the drop and an effective interfacial tension, we exploit the time evolution of the drop shape to measure the EIT. Our results show that the EIT in water-glycerol systems is orders of magnitude lower than that reported in previous experimental measurements, and in excellent agreement with values calculated via the phase field model proposed in [Phys. Rev. X 6, 041057, 2016]., Comment: 11 pages, 6 figures

The mechanical properties of soft matter are of great importance in countless applications, in addition of being an active field of academic research. Given the relative ease with which soft materials can be deformed, their non-linear behavior is of particular relevance. Large loads eventually result in material failure. In this Perspective article, we discuss recent work aiming at detecting precursors of failure by scrutinizing the microscopic structure and dynamics of soft systems under various conditions of loading. In particular, we show that the microscopic dynamics is a powerful indicator of the ultimate fate of soft materials, capable of unveiling precursors of failure up to thousands of seconds before any macroscopic sign of weakening., Comment: 12 pages, 7 figures

We report on the extensional dynamics of spinning drops in miscible and immiscible background fluids following a rotation speed jump. Two radically different behaviours are observed. Drops in immiscible environments relax exponentially to their equilibrium shape, with a relaxation time that does not depend on the centrifugal forcing. We find an excellent quantitative agreement with the relaxation time predicted for quasi-spherical drops by Stone and Bush (Q. Appl. Math. 54, 551 (1996)), while other models proposed in the literature fail to capture our data. By contrast, drops immersed in a miscible background fluid do not relax to a steady shape: they elongate indefinitely, their length following a power-law $l(t)\sim t^{\frac{2}{5}}$ in very good agreement with the dynamics predicted by Lister and Stone (J. Fluid Mech. 317, 275 (1996)) for inviscid drops. Our results strongly suggest that low compositional gradients in miscible fluids do not give rise to an effective interfacial tension measurable by spinning drop tensiometry., Comment: 31 pages, 6 figures

Cells and tissues have the remarkable ability to actively generate the forces required to change their shape. This active mechanical behavior is largely mediated by the actin cytoskeleton, a crosslinked network of actin filaments that is contracted by myosin motors. Experiments and active gel theories have established that the length scale over which gel contraction occurs is governed by a balance between molecular motor activity and crosslink density. By contrast, the dynamics that govern the contractile activity of the cytoskeleton remain poorly understood. Here we investigate the microscopic dynamics of reconstituted actin-myosin networks using simultaneous real-space video microscopy and Fourier-space dynamic light scattering. Light scattering reveals rich and unanticipated microscopic dynamics that evolve with sample age. We uncover two dynamical precursors that precede macroscopic gel contraction. One is characterized by a progressive acceleration of stress-induced rearrangements, while the other consists of sudden rearrangements that depend on network adhesion to the boundaries and are highly heterogeneous. Our findings reveal an intriguing analogy between self-driven rupture and collapse of active gels to the delayed rupture of passive gels under external loads.

We discuss in two companion papers (arXiv:1802.03737 and the present manuscript) how Fourier-space measurements may be coupled to rheological tests in order to elucidate the relationship between mechanical properties and microscopic dynamics in soft matter. In this second companion paper, we focus on Differential Dynamic Microscopy (DDM) under shear. We highlight the analogies and the differences with Dynamic Light Scattering coupled to rheology, providing a theoretical approach and practical guidelines to separate the contributions to DDM arising from the affine and the non-affine part of the microscopic displacement field. We show that in DDM under shear the coherence of the illuminating source plays a key role, determining the effective sample thickness that is probed. Our theoretical analysis is validated by experiments on 2D samples and 3D gels., Comment: This is a companion paper to the manuscript arXiv:1802.03737

Material failure is ubiquitous, with implications from geology to everyday life and material science. It often involves sudden, unpredictable events, with little or no macroscopically detectable precursors. A deeper understanding of the microscopic mechanisms eventually leading to failure is clearly required, but experiments remain scarce. Here, we show that the microscopic dynamics of a colloidal gel, a model network-forming system, exhibit dramatic changes that precede its macroscopic failure by thousands of seconds. Using an original setup coupling light scattering and rheology, we simultaneously measure the macroscopic deformation and the microscopic dynamics of the gel, while applying a constant shear stress. We show that the network failure is preceded by qualitative and quantitative changes of the dynamics, from reversible particle displacements to a burst of irreversible plastic rearrangements.

Power law rheology is of widespread occurrence in complex materials that are characterized by the presence of a very broad range of microstructural length and time scales. Although phenomenological models able to reproduce the observed rheological features exist, in general a well-established connection with the microscopic origin of this mechanical behavior is still missing. As a model system, this work focuses on a fractal colloidal gel. We thoroughly characterize the linear power law rheology of the sample and its age dependence. We show that at all sample ages and for a variety of rheological tests the gel linear viscoelasticity is very accurately described by a Fractional Maxwell (FM) model, characterized by a power law behavior. Thanks to a unique set-up that couples small-angle static and dynamic light scattering to rheological measurements, we demonstrate that the power law rheology observed in the linear regime originates from reversible non-affine rearrangements and discuss the possible relationship between the FM model and the microscopic structure of the gel.

Understanding the microscopic origin of the rheological behavior of soft matter is a long-lasting endeavour. While early efforts concentrated mainly on the relationship between rheology and structure, current research focuses on the role of microscopic dynamics. We present in two companion papers a thorough discussion of how Fourier space-based methods may be coupled to rheology to shed light on the relationship between the microscopic dynamics and the mechanical response of soft systems. In this first companion paper, we report a theoretical, numerical and experimental investigation of dynamic light scattering coupled to rheology. While in ideal solids and simple viscous fluids the displacement field under a shear deformation is purely affine, additional non-affine displacements arise in many situations of great interest, for example in elastically heterogeneous materials or due to plastic rearrangements. We show how affine and non-affine displacements can be separately resolved by dynamic light scattering, and discuss in detail the effect of several non-idealities in typical experiments., Comment: 13 pages, 7 figures. First paper of a series of two companion papers. The second companion paper will be posted shortly

Hydrodynamic instabilities in miscible fluids are ubiquitous, from natural phenomena up to geological scales, to industrial and technological applications, where they represent the only way to control and promote mixing at low Reynolds numbers, well below the transition from laminar to turbulent flow. As for immiscible fluids, the onset of hydrodynamic instabilities in miscible fluids is directly related to the physics of their interfaces. The focus of this review is therefore on the general mechanisms driving the growth of disturbances at the boundary between miscible fluids, under a variety of forcing conditions. In the absence of a regularizing mechanism, these disturbances would grow indefinitely. For immiscible fluids, interfacial tension provides such a regularizing mechanism, because of the energy cost associated to the creation of new interface by a growing disturbance. For miscible fluids, however, the very existence of interfacial stresses that mimic an effective surface tension is debated. Other mechanisms, however, may also be relevant, such as viscous dissipation. We shall review the stabilizing mechanisms that control the most common hydrodynamic instabilities, highlighting those cases for which the lack of an effective interfacial tension poses deep conceptual problems in the mathematical formulation of a linear stability analysis. Finally, we provide a short overview on the ongoing research on the effective, out of equilibrium interfacial tension between miscible fluids., Comment: 9 figures

We explore the glassy dynamics of soft colloids using microgels and charged particles interacting by steric and screened Coulomb interactions, respectively. In the supercooled regime, the structural relaxation time $\tau_\alpha$ of both systems grows steeply with volume fraction, reminiscent of the behavior of colloidal hard spheres. Computer simulations confirm that the growth of $\tau_\alpha$ on approaching the glass transition is independent of particle softness. By contrast, softness becomes relevant at very large packing fractions when the system falls out of equilibrium. In this non-equilibrium regime, $\tau_\alpha$ depends surprisingly weakly on packing fraction and time correlation functions exhibit a compressed exponential decay consistent with stress-driven relaxation. The transition to this novel regime coincides with the onset of an anomalous decrease of local order with increasing density typical of ultrasoft systems. We propose that these peculiar dynamics results from the combination of the non-equilibrium aging dynamics expected in the glassy state and the tendency of colloids interacting through soft potentials to refluidize at high packing fractions., Comment: 6 pages, 4 figures + Supplemental Material (5 pages, 5 figures)

We investigate how the microstructure of a colloidal polycrystal influences its linear viscoelasticity. We use thermosensitive copolymer micelles that arrange in water in a cubic crystalline lattice, yielding a colloidal polycrystal. The polycrystal is doped with a small amount of nanoparticles, of size comparable to that of the micelles, which behave as impurities and thus partially segregate in the grain boundaries. We show that the shear elastic modulus only depends on the packing of the micelles and does not vary neither with the presence of nanoparticles nor with the crystal microstructure. By contrast, we find that the loss modulus is strongly affected by the presence of nanoparticles. A comparison between rheology data and small-angle neutron scattering data suggests that the loss modulus is dictated by the total amount of nanoparticles in the grain boundaries, which in turn depends on the sample microstructure.

We explore the influence of particle softness and internal structure on both the bulk and interfacial rheological properties of colloidal suspensions. We probe bulk stresses by conventional rheology, by measuring the flow curves, shear stress vs strain rate, for suspensions of soft, deformable microgel particles and suspensions of near hard-sphere-like silica particles. A similar behavior is seen for both kind of particles in suspensions at concentrations up to the random close packing volume fraction, in agreement with recent theoretical predictions for sub-micron colloids. Transient interfacial stresses are measured by analyzing the patterns formed by the interface between the suspensions and their own solvent, due to a generalized Saffman-Taylor hydrodynamic instability. At odd with the bulk behavior, we find that microgels and hard particle suspensions exhibit vastly different interfacial stress properties. We propose that this surprising behavior results mainly from the difference in particle internal structure (polymeric network for microgels vs compact solid for the silica particles), rather than softness alone., Comment: 20 pages, 8 figures

Taylor dispersion analysis is an increasingly popular characterization method that measures the diffusion coefficient, and hence the hydrodynamic radius, of (bio)polymers, nanoparticles or even small molecules. In this work, we describe an extension to current data analysis schemes that allows size polydispersity to be quantified for an arbitrary sample, thereby significantly enhancing the potentiality of Taylor dispersion analysis. The method is based on a cumulant development similar to that used for the analysis of dynamic light scattering data. Specific challenges posed by the cumulant analysis of Taylor dispersion data are discussed, and practical ways to address them are proposed. We successfully test this new method by analyzing both simulated and experimental data for solutions of moderately polydisperse polymers and polymer mixtures., Comment: 41 pages (including Supporting Information), 5 figures (+ 7 figs. in the Supporting Information)

We study the fingering instability of the interface between two miscible fluids, a colloidal suspension and its own solvent. The temporal evolution of the interface in a Hele-Shaw cell is found to be governed by the competition between the non-linear viscosity of the suspension and an off-equilibrium, effective surface tension $\Gamma_e$. By studying suspensions in a wide range of volume fractions, $\Phi_\mathrm{C}$, we show that $\Gamma_e \sim \Phi_\mathrm{C}^2$, in agreement with Korteweg's theory for miscible fluids. The surface tension exhibits an anomalous increase with particle size, which we account for using entropy arguments., Comment: 5 pages, 5 figures + supplementary material

We use confocal microscopy and time-resolved light scattering to investigate plasticity in a col- loidal polycrystal, following the evolution of the network of grain boundaries as the sample is submitted to thousands of shear deformation cycles. The grain boundary motion is found to be ballistic, with a velocity distribution function exhibiting non-trivial power law tails. The shear- induced dynamics initially slow down, similarly to the aging of the spontaneous dynamics in glassy materials, but eventually reach a steady state. Surprisingly, the cross-over time between the ini- tial aging regime and the steady state decreases with increasing probed length scale, hinting at a hierarchical organization of the grain boundary dynamics., Comment: main paper + supplementary materials

We investigate the dynamics of alginate gels, an important class of biopolymer-based viscoelastic materials, by combining mechanical tests and non-conventional, time-resolved light scattering methods. Two relaxation modes are observed upon applying a compressive or shear stress. Dynamic light scattering and diffusive wave spectroscopy measurements reveal that these modes are associated with discontinuous rearrangement events that restructure the gel network via anomalous, non-diffusive microscopic dynamics. We show that these dynamics are due to both thermal activation and internal stress stored during gelation and propose a scenario where a hierarchy of cross-links with different life times is responsible for the observed complex behavior. Measurements at various temperatures and sample ages are presented to support this scenario., Comment: To appear in Soft Matter

The constituents of soft matter systems such as colloidal suspensions, emulsions, polymers, and biological tissues undergo microscopic random motion, due to thermal energy. They may also experience drift motion correlated over mesoscopic or macroscopic length scales, \textit{e.g.} in response to an internal or applied stress or during flow. We present a new method for measuring simultaneously both the microscopic motion and the mesoscopic or macroscopic drift. The method is based on the analysis of spatio-temporal cross-correlation functions of speckle patterns taken in an imaging configuration. The method is tested on a translating Brownian suspension and a sheared colloidal glass.

We describe a light scattering apparatus based on a novel optical scheme covering the scattering angle range $0.5\dg \le \theta \le 25\dg$, an intermediate regime at the frontier between wide angle and small angle setups that is difficult to access by existing instruments. Our apparatus uses standard, readily available optomechanical components. Thanks to the use of a charge-coupled device detector, both static and dynamic light scattering can be performed simultaneously at several scattering angles. We demonstrate the capabilities of our apparatus by measuring the scattering profile of a variety of samples and the Brownian dynamics of a dilute colloidal suspension.

We investigate by scattering techniques the structure of water-based soft composite materials comprising a crystal made of Pluronic block-copolymer micelles arranged in a face-centered cubic lattice and a small amount (at most 2% by volume) of silica nanoparticles, of size comparable to that of the micelles. The copolymer is thermosensitive: it is hydrophilic and fully dissolved in water at low temperature (T ~ 0{\deg}C), and self-assembles into micelles at room temperature, where the block-copolymer is amphiphilic. We use contrast matching small-angle neuron scattering experiments to probe independently the structure of the nanoparticles and that of the polymer. We find that the nanoparticles do not perturb the crystalline order. In addition, a structure peak is measured for the silica nanoparticles dispersed in the polycrystalline samples. This implies that the samples are spatially heterogeneous and comprise, without macroscopic phase separation, silica-poor and silica-rich regions. We show that the nanoparticle concentration in the silica-rich regions is about tenfold the average concentration. These regions are grain boundaries between crystallites, where nanoparticles concentrate, as shown by static light scattering and by light microscopy imaging of the samples. We show that the temperature rate at which the sample is prepared strongly influence the segregation of the nanoparticles in the grain-boundaries., Comment: accepted for publication in Langmuir

We study the crystallization of a colloidal model system in presence of secondary nanoparticles acting as impurities. Using confocal microscopy, we show that the nanoparticles segregate in the grain boundaries of the colloidal polycrystal. We demonstrate that the texture of the polycrystal can be tuned by varying independently the nanoparticle volume fraction and the crystallization rate, and quantify our findings using standard models for the nucleation and growth of crystalline materials. Remarkably, we find that the efficiency of the segregation of the nanoparticles in the grain-boundaries is determined solely by the typical size of the crystalline grains., Comment: accepted for publication in Soft Matter

We study the sedimentation of colloidal gels by using a combination of light scattering, polarimetry and video imaging. The asymptotic concentration profiles $\varphi(z,t\rightarrow \infty)$ exhibit remarkable scaling properties: profiles for gels prepared at different initial volume fractions and particle interactions can be superimposed onto a single master curve by using suitable reduced variables. We show theoretically that this behavior stems from a power law dependence of the compressive elastic modulus \textit{vs} $\varphi$, which we directly test experimentally. The sedimentation kinetics comprises an initial latency stage, followed by a rapid collapse where the gel height $h$ decreases at constant velocity, and a final compaction stage characterized by a stretched exponential relaxation of $h$ towards a plateau. Analogies and differences with previous works are briefly discussed., Comment: This is an author-created, un-copyedited version of an article accepted for publication in Journal of Physics Condensed Matter. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it. The definitive publisher-authenticated version will be available online

We use a combination of original light scattering techniques and particles with unique optical properties to investigate the behavior of suspensions of attractive colloids under gravitational stress, following over time the concentration profile, the velocity profile, and the microscopic dynamics. During the compression regime, the sedimentation velocity grows nearly linearly with height, implying that the gel settling may be fully described by a (time-dependent) strain rate. We find that the microscopic dynamics exhibit remarkable scaling properties when time is normalized by strain rate, showing that the gel microscopic restructuring is dominated by its macroscopic deformation., Comment: Physical Review Letters (2011) xxxx

Concentrated colloidal suspensions are a well-tested model system which has a glass transition. Colloids are suspensions of small solid particles in a liquid, and exhibit glassy behavior when the particle concentration is high; the particles are roughly analogous to individual molecules in a traditional glass. Because the particle size can be large (100 nm - 1000 nm), these samples can be studied with a variety of optical techniques including microscopy and dynamic light scattering. Here we review the phenomena associated with the colloidal glass transition, and in particular discuss observations of spatial and temporally heterogeneous dynamics within colloidal samples near the glass transition. Although this Chapter focuses primarily on results from hard-sphere-like colloidal particles, we also discuss other colloidal systems with attractive or soft repulsive interactions., Comment: Chapter of "Dynamical heterogeneities in glasses, colloids, and granular media", Eds.: L. Berthier, G. Biroli, J-P Bouchaud, L. Cipelletti and W. van Saarloos (Oxford University Press, to appear), more info at http://w3.lcvn.univ-montp2.fr/~lucacip/DH_book.htm

Foams are ideal model systems to study stress-driven dynamics, as stress-imbalances within the system are continuously generated by the coarsening process, which unlike thermal fluctuations, can be conveniently quantified by optical means. However, the high turbidity of foams generally hinders the detailed study of the temporal and spatial distribution of rearrangement events, such that definite assessments regarding their contribution to the overall dynamics could not be made so far. In this paper, we use novel light scattering techniques to measure the frequency and position of events within a large sample volume. As recently reported (A. S. Gittings and D. J. Durian, Phys. Rev. E, 2008, 78, 066313), we find that the foam dynamics is determined by two distinct processes: intermittent bubble rearrangements of finite duration and a spatially homogeneous quasicontinuous process. Our experiments show that the convolution of these two processes determines the age-dependence of the mean dynamics, such that relations between intermittent rearrangements and coarsening process can not be established by considering means. By contrast the use of the recently introduced photon correlation imaging technique (A. Duri, D. A. Sessoms, V. Trappe, and L. Cipelletti, Phys. Rev. Lett., 2009, 102, 085702) enables us to assess that the event frequency is directly determined by the strain-rate imposed by the coarsening process. Surprisingly, we also find that, although the distribution of successive events in time is consistent with a random process, the spatial distribution of successive events is not random: rearrangements are more likely to occur within a recently rearranged zone. This implies that a topological rearrangement is likely to lead to an unstable configuration, such that a small amount of coarsening-induced strain is sufficient to trigger another event.

Brambilla, et al. Reply: van Megen and Williams (vMW) question our recent claim that dense colloidal hard spheres enter at large volume fraction \phi a dynamical regime not observed in earlier work and not described by the mode-coupling theory (MCT) of the glass transition., Comment: Reply to a comment by van Megen and Williams

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., Comment: To appear in Soft Matter

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., Comment: 11 pages; 10 figs

We investigate dynamical heterogeneities in the collective relaxation of a concentrated microgel system, for which the packing fraction can be conveniently varied by changing the temperature. The packing fraction dependent mechanical properties are characterised by a fluid-solid transition, where the system properties switch from a viscous to an elastic low-frequency behaviour. Approaching this transition from below, we find that the range of spatial correlations in the dynamics increases. Beyond this transition, the spatial correlation range reaches a maximum, extending over the entire observable system size of approximately 5 mm. Increasing the packing fraction even further leads to a second transition, which is characterised by the development of large zones of lower and higher dynamical activity that are well separated from each other; the range of correlation decreases at this point. This striking non-monotonic dependence of the spatial correlation length on volume fraction is reminiscent of the behaviour recently observed at the jamming/rigidity transition in granular systems (Lechenault et al. 2008). We identify this second transition as the transition to 'squeezed' states, where the constituents of the system start to exert direct contact forces on each other, such that the dynamics becomes increasingly determined by imbalanced stresses. Evidence of this transition is also found in the frequency dependence of the storage and loss moduli, which become increasingly coupled as direct friction between the particles starts to contribute to the dissipative losses within the system. To our knowledge, our data provide the first observation of a qualitative change in dynamical heterogeneity as the dynamics switch from purely thermally-driven to stress-driven., Comment: 19 pages, 8 figures. Latest version corrects errors in the indication of the concentration of microgel systems and the equation for the temperature dependence of the particle radius

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., Comment: 16 pages; 12 figures

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., Comment: Published version (Phys. Rev. Lett. 102, 085702 (2009)) The Dynamical Activity Mapsprovided as Supplementary Online Material are also available on http://w3.lcvn.univ-montp2.fr/~lucacip/dam/movies.htm

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., Comment: 10 pages, 7 figures, submitted to PRE

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 $\phi_{\rm c}$, 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 $\phi_{\rm c}$ 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., Comment: 4 pages, 3 figures, published in PRL 102 085703 (2009)

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 $\xi$\cite{WeeksScience2000,DauchotPRL2005,Glotzer,Ediger}. On approaching these transitions, $\xi$ 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'', $\chi^*$, whose growth is usually associated to that of $\xi$\cite{LacevicPRE}. $\chi^*$ initially increases with volume fraction $\phi$, 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 $\xi$ and the reduced particle displacements associated with rearrangements in very dense suspensions, unveiling a richer-than-expected scenario., Comment: 1st version originally submitted to Nature Physics. See the Nature Physics website fro the final, published version

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., Comment: 11 pages, 4 figures

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 $\chi$ 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., Comment: Final version published in PRE