The aging dynamics of colloidal suspensions of Laponite, a synthetic clay, is investigated using dynamic light stattering (DLS) and viscometry after a quench into the glassy phase. DLS allows to follow the diffusion of Laponite particles and reveals that there are two modes of relaxation. The fast mode corresponds to a rapid diffusion of particles within "cages" formed by the neighboring particles. The slow mode corresponds to escape from the cages: its average relaxation time increases exponentially fast with the age of the glass. In addition, the slow mode has a broad distribution of relaxation times, its distribution becoming larger as the system ages. Measuring the concomitant increase of viscosity as the system ages, we can relate the slowing down of the particle dynamics to the viscosity.
We study the nonlinear rheological behavior and the microscopic particle dynamics for a colloidal glass, to see whether recently developed models for driven glassy systems can be applied to predict the rheology. Qualitatively, all the findings predicted by the models can be retrieved in our system. Notably, the viscosity decreases strongly with the shear rate. Since it is difficult to predict non-Newtonian viscosities of colloidal systems due to long-ranged hydrodynamic interactions, this shows the promise of this approach for predicting flow behavior. In addition, the measurements allow us to relate the microscopic diffusion dynamics to the macroscopic viscosity of the system.
In this study, the mobility of nanoparticles in mucus and similar hydrogels as model systems was assessed to elucidate the link between microscopic diffusion behavior and macroscopic penetration of such gels. Differences in particle adhesion to mucus components were strongly dependent on particle coating. Particles coated with 2 kDa PEG exhibited a decreased adhesion to mucus components, whereas chitosan strongly increased the adhesion. Despite such mucoinert properties of PEG, magnetic nanoparticles of both coatings did not penetrate through native respiratory mucus, resisting high magnetic forces (even for several hours). However, model hydrogels were, indeed, penetrated by both particles in dependency of particle coating, obeying the theory of particle mobility in an external force field. Comparison of penetration data with cryogenic scanning EM images of mucus and the applied model systems suggested particularly high rigidity of the mucin scaffold and a broad pore size distribution in mucus as reasons for the observed particle immobilization. Active probing of the rigidity of mucus and model gels with optical tweezers was used in this context to confirm such properties of mucus on the microscale, thus presenting the missing link between micro-and macroscopical observations. Because of high heterogeneity in the size of the voids and pores in mucus, on small scales, particle mobility will depend on adhesive or inert properties. However, particle translocation over distances larger than a few micrometers is restricted by highly rigid structures within the mucus mesh.forced penetration | pulmonary drug delivery | cryoelectronmicroscopy
We present a direct experimental measurement of an effective temperature in a colloidal glass of laponite, using a micrometric bead as a thermometer. The nonequilibrium fluctuation-dissipation relation, in the particular form of a modified Einstein relation, is investigated with diffusion and mobility measurements of the bead embedded in the glass. We observe an unusual nonmonotonic behavior of the effective temperature: starting from the bath temperature, it is found to increase up to a maximum value, and then decrease back, as the system ages. We show that the observed deviation from the Einstein relation is related to the relaxation times previously measured in dynamic light scattering experiments.
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