A micromechanical model to predict the flow of soft particle glasses

JR Seth and L Mohan and C Locatelli-Champagne and M Cloitre and RT Bonnecaze, NATURE MATERIALS, 10, 838-843 (2011).

DOI: 10.1038/NMAT3119

Soft particle glasses form a broad family of materials made of deformable particles, as diverse as microgels(1), emulsion droplets(2), star polymers(3), block copolymer micelles and proteins(4), which are jammed at volume fractions where they are in contact and interact via soft elastic repulsions. Despite a great variety of particle elasticity, soft glasses have many generic features in common. They behave like weak elastic solids at rest but flow very much like liquids above the yield stress. This unique feature is exploited to process high-performance coatings, solid inks, ceramic pastes, textured food and personal care products. Much of the understanding of these materials at volume fractions relevant in applications is empirical, and a theory connecting macroscopic flow behaviour to microstructure and particle properties remains a formidable challenge. Here we propose a micromechanical three- dimensional model that quantitatively predicts the nonlinear rheology of soft particle glasses. The shear stress and the normal stress differences depend on both the dynamic pair distribution function and the solvent-mediated EHD interactions among the deformed particles. The predictions, which have no adjustable parameters, are successfully validated with experiments on concentrated emulsions and polyelectrolyte microgel pastes, highlighting the universality of the flow properties of soft glasses. These results provide a framework for designing new soft additives with a desired rheological response.

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