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.Comment: Physical Review Letters (2011) xxx

What buoyancy really is. A generalized Archimedes' principle for sedimentation and ultracentrifugation

Particle settling is a pervasive process in nature, and centrifugation is a versatile separation technique. Yet, the results of settling and ultracentrifugation experiments often appear to contradict the very law on which they are based: Archimedes' principle - arguably, the oldest physical law. The purpose of this paper is delving into the very roots of the concept of buoyancy by means of a combined experimental-theoretical study on sedimentation profiles in colloidal mixtures. Our analysis shows that the standard Archimedes' principle is only a limiting approximation, valid for mesoscopic particles settling in a molecular fluid, and we provide a general expression for the actual buoyancy force. This "Generalized Archimedes' Principle" accounts for unexpected effects, such as denser particles floating on top of a lighter fluid, which in fact we observe in our experiments

Short-time self-diffusion in binary colloidal suspensions

The Brownian dynamics of a colloidal particle is consistently modified by the presence in the solvent of other particles of comparable size, whose effects on the particle diffusion coefficient cannot be attributed to a change of the effective solvent viscosity. So far, despite their impact on subjects ranging from microrheology to phoretic transport in crowded environments, a detailed experimental survey of these effects is still lacking. By exploiting the peculiar properties of fluorinated colloidal particle, we have performed an extensive dynamic light scattering (DLS) investigation of short-time self-diffusion in binary colloidal mixtures, focusing on systems where one of the two species (the “tracer” particles) is very diluted compared to the other one (the “host” particles). From the dependence on the host concentration of the DLS correlation function, we have obtained the first-order correction h s 1 s to the tracer single-particle diffusion coefficient, varying the tracer-to-host size ratio q in the range 0.2 ≤ q ≤ 2. Our results support the functional relation of h s 1 s on q proposed to account for the theoretical and numerical results for hard-sphere mixtures. However, h s 1 s seems to have a weaker dependence on the size ratio than theoretically predicted, possibly because of an imperfect matching of the suspensions we used for an ideal hard-sphere mixture. This may be due to the presence of a stabilizing surfactant layer on the particle surface that, although very thin, has significant effects on hydrodynamic lubrication forces

Heterogeneity Governs 3D-Cultures of Clinically Relevant Microbial Communities

The intrinsic heterogeneity of bacterial niches should be retained in in vitrocultures to represent the complex microbial ecology. As a case study,mucin-containing hydrogels -CF-Mu3Gel - are generated by diffusion-inducedgelation, bioinspired on cystic fibrosis (CF) mucus, and a microbial nichechallenging current therapeutic strategies. At breathing frequency, CF-Mu3Gelexhibits aG′andG′′equal to 24 and 3.2 Pa, respectively. Notably, CF-Mu3Gelexhibits structural gradients with a gradual reduction of oxygen tensionacross its thickness (280–194μmol L−1). Over the culture period, a steepdecline in oxygen concentration occurs just a few millimeters below theair–mucus interface in CF-Mu3Gel, similar to those of CF airway mucus.Importantly, the distinctive features of CF-Mu3Gel significantly influencebacterial organization and antimicrobial tolerance in mono- and co-cultures ofStaphylococcus aureusandPseudomonas aeruginosathat standard culturesare unable to emulate. The antimicrobial susceptibility determined inCF-Mu3Gel corroborates the mismatch on the efficacy of antimicrobialtreatment between planktonically cultured bacteria and those in patients.With this example-based research, new light is shed on the understanding ofhow the substrate influences microbial behavior, paving the way for improvedfundamental microbiology studies and more effective drug testing anddevelopment

Relaxation in aging thermoreversible gels: The role of thermal history

The fast setting of gels originating from an arrested phase separation leads to solid structures that incorporate a substantial amount of frozen-in stresses. Using a colloidal system made of particles whose interactions can accurately be tuned with temperature and exploiting Photon Correlation Imaging (PCI), an optical correlation technique blending the powers of scattering and imaging, we show that the relaxation of these internal stresses, which occurs through a cascade of microscopic restructuring events, is strongly influenced by the thermal history of the sample. By changing with a temperature jump the interparticle interactions in an already set gel, we specifically show that gels formed by a deep quench within the coexistence region store a lot of residual stress. This stress quickly relaxes when the interparticle attractions are weakened by decreasing temperature. Conversely, the relaxation of stresses accumulated in gels obtained by a shallower quench comes to a halt by a temperature jump that hardens the gel structure. The evidence we collected may provide useful hints about tempering and annealing processes in disordered solids. This journal i

Phase Behavior and Microscopic Dynamics of a Thermosensitive Gel-Forming Polymer

Soft adaptive networks like polymer gels are almost ideal candidates as surrogates for the extracellular matrix, more so when their rheo-mechanical properties can be carefully tuned by temperature. Using both dynamic light scattering and photon correlation imaging, we have investigated the phase behavior and the microscopic dynamics of a thermoresponsive network, Mebiol Gel, extensively and effectively used as a three-dimensional scaffold for cell growth. In the dilute limit, Mebiol displays a temperature-driven association process characterized by a significant increase of the molecular weight, which is not accompanied, however, by a concurrent increase of the aggregate size. This peculiar behavior is consistent with numerical simulations of a simpler but structurally homologous block-copolymer system. By increasing concentration and approaching gelation, the polymer solution progressively attains the structure of a percolating network, as witnessed by the logarithmic decay of the intensity correlation functions extending over many time decades, a relaxation behavior that is found well within the gel phase too. No evidence of a discontinuous transition to a fully arrested gel phase is, however, detectable in the microscopic dynamics

A heavy intruder in a locally-shaken granular solid

We experimentally investigate the gravitational-driven motion of a heavy object inside a vertical 2D assembly of identical, plastic cylinders arranged in a regular, triangular lattice. The bottom of the assembly is in contact with a rough plate whose horizontal, sinusoidal motion induces the formation of shear bands in the granular solid, aligned with the edges of the lattice. The intruder sinks when the width of the shear band is as large as its size and halts once the regular configuration of the grains is recovered. The resulting vertical motion of the intruder is random and intermittent, as in disordered granular or colloidal systems near jamming, with alternate flows and blockades. We show, in analogy with earthquakes, that the relation between the size and the duration of the flowing events follows a power-law with an exponent larger than one, and that the statistics of their size is compatible with the Gutenberg-Richter law. We also show that the probability density function of times between flowing events is similar to the Omori law governing the distribution of aftershock sequences following large earthquakes. Finally, the analysis of the velocity fluctuations of the intruder points to a transition from a strong to a weak contact network in the ordered granular assembly, similar to the transition from jammed to fragile states in disordered systems

Compressive yield stress of depletion gels from stationary centrifugation profiles

We have investigated the stationary sedimentation profiles of colloidal gels obtained by an arrested phase-separation process driven by depletion forces, which have been compressed either by natural gravity or by a centrifugal acceleration ranging between 6g and 2300g. Our measurements show that the gel rheological properties display a drastic change when the gel particle volume fraction exceeds a value φc , which barely depends on the strength of the interparticle attractive forces that consolidate the network. In particular, the gel compressive yield stress , which increases as for , displays a diverging behaviour for , with an asymptotic value that is close to the random close packing value for hard spheres. The evidence we obtained suggests that basically coincides with the liquid (colloid-rich) branch of the metastable coexistence curve, rather than with the lower (and φ-dependent) values expected for an attractive glass line penetrating inside the coexistence region

Colloidal Swarms Can Settle Faster than Isolated Particles: Enhanced Sedimentation near Phase Separation

By experimenting on model colloids where depletion forces can be carefully tuned and quantified, we show that attractive interactions consistently "promote" particle settling, so much that the sedimentation velocity of a moderately concentrated dispersion can even exceed its single-particle value. At larger particle volume fraction φ, however, hydrodynamic hindrance eventually takes over. Hence, v(φ) actually displays a nonmonotonic trend that may threaten the stability of the settling front to thermal perturbations. Finally, by discussing a representative case, we show that these results are relevant to the investigation of protein association effects by ultracentrifugation