Microstructure and rheology of soft particle glasses
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Soft particle glasses like microgels and compressed emulsions are densely packed, disordered suspensions of deformable particles. Quantitative relationships among the constituent properties and the macroscopic properties of the suspension are determined for their customized design as rheological additives. The microscopic origin of their macroscopic properties is also determined. Advanced characterization techniques like Large Amplitude Oscillatory Shear (LAOS) and microrheology are studied to use them efficiently to characterize these materials. Their microstructure and rheology are investigated through theory, simulations and experiments. Soft particle glasses are used as rheological additives in many applications including coatings, solid inks and textured food and cosmetic products but their formulation is largely empirical. A quantitative connection between their formulation and rheology is critical to enable their rational design. Their microstructure will lead to the microscopic origin of some unique properties in common with other soft crowded materials like intracellular cytoplasm and clays. These are complex fluids and require novel techniques to characterize them. A study of these techniques is essential to efficiently interpret the observations in terms of their macroscopic properties and the microscopic dynamics involved. Particle scale simulations of steady and oscillatory shear flow are developed to predict the nonlinear rheology and microstructure of these glasses. The origin of yielding is determined as escape of particles from their cages giving rise to a shear induced diffusion. Microrheology is studied by developing simulations of a probe particle being pulled at a constant force and the rheological information from microrheology is quantitatively connected to that from bulk rheological measurements. Soft particle glasses develop internal stresses when quenched to a solid state by flow cessation during processing. Experiments are performed to characterize and a priori predict these stresses. Simulations are used to determine the particle scale mechanisms involved in the stress relaxation on flow cessation and the microstructural origin of internal stresses. A pairwise interaction theory is developed for quiescent glasses to quantitatively predict their microstructure and elastic properties. The theory is then extended to sheared glasses to quantitatively predict their nonlinear rheology. The implementation of the pairwise theories is computationally much faster than the full three-dimensional simulations.