arXiv subjects

Luca Cipelletti

Publications and source records attributed to Luca Cipelletti.

At least 37 records · Page 2Linked to original sources

arXiv2017

Hydrodynamic instabilities in miscible fluids

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.

cond-mat.soft↗

arXiv2017

The glass transition of soft colloids

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 $τ_α$ of both systems grows steeply with volume fraction, reminiscent of the behavior of colloidal hard spheres. Computer simulations confirm that the growth of $τ_α$ 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, $τ_α$ 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.

cond-mat.soft↗

arXiv2015

Viscoelasticity of colloidal polycrystals doped with impurities

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.

cond-mat.soft↗

arXiv2014

Bulk and interfacial stresses in suspensions of soft and hard colloids

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.

cond-mat.soft↗

arXiv2014

Plasticity of a colloidal polycrystal under cyclic shear

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.

cond-mat.soft↗

arXiv2014

Polydispersity analysis of Taylor dispersion data: the cumulant method

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.

cond-mat.soft↗

arXiv2013

Off-equilibrium surface tension in colloidal suspensions

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 $Γ_e$. By studying suspensions in a wide range of volume fractions, $Φ_\mathrm{C}$, we show that $Γ_e \sim Φ_\mathrm{C}^2$, 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.

cond-mat.soft↗

arXiv2013

Hierarchical cross-linking in physical alginate gels: a rheological and dynamic light scattering investigation

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.

cond-mat.soft↗

arXiv2013

Simultaneous measurement of the microscopic dynamics and the mesoscopic displacement field in soft systems by speckle imaging

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.

cond-mat.soft↗

arXiv2012

Multiangle static and dynamic light scattering in the intermediate scattering angle range

We describe a light scattering apparatus based on a novel optical scheme covering the scattering angle range $0.5\dg \le θ\le 25\dg$, 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.

physics.optics↗

arXiv2012

Structure of nanoparticles embedded in micellar polycrystals

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°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.

cond-mat.soft↗

arXiv2012

Grain refinement and partitioning of impurities in the grain boundaries of a colloidal polycrystal

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.

cond-mat.soft↗

arXiv2012

Equilibrium concentration profiles and sedimentation kinetics of colloidal gels under gravitational stress

We study the sedimentation of colloidal gels by using a combination of light scattering, polarimetry and video imaging. The asymptotic concentration profiles $φ(z,t\rightarrow \infty)$ 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} $φ$, 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.

cond-mat.soft↗

arXiv2011

Multiple dynamic regimes in concentrated microgel systems

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.

cond-mat.soft↗

arXiv2011

Highly nonlinear dynamics in a slowly sedimenting colloidal gel

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.

cond-mat.soft↗

arXiv2010

Glassy dynamics and dynamical heterogeneity in colloids

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.

cond-mat.soft↗

arXiv2010

Unexpected spatial distribution of bubble rearrangements in coarsening foams

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.

cond-mat.soft↗

arXiv2010

Brambilla, et al. Reply

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

cond-mat.soft↗