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A micromechanical model to predict the flow of soft particle glasses

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Abstract

Soft particle glasses form a broad family of materials made of deformable particles, as diverse as microgels1, emulsion droplets2, star polymers3, block copolymer micelles and proteins4, 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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Figure 1: Structure and interactions of a model soft glass.
Figure 2: Computed shear stress and first and second normal stress differences of model soft glasses.
Figure 3: Microstructure of sheared soft particle glasses.
Figure 4: Universal constitutive laws for shear stress and normal stress differences from simulated data.
Figure 5: Universal scaling of shear stress and first normal stress difference experimental data.

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Acknowledgements

We are grateful to D. Vlassopoulos for a critical reading of the manuscript. This work was supported by the NoE European Network Sofcomp, the CNRS (PICS 4176), the Petroleum Research Fund (ACS PRF #41236-AC9), and the National Science Foundation (CBET 0854420).

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J.R.S, L.M. and R.T.B. conceived the model, developed the simulations and analysed the results. C.L. and M.C. conceived and conducted the experiments and analysed the results. M.C. and R.T.B. interpreted and synthesized the results and wrote the paper. J.R.S., L.M. and C.L. provided editorial comments on the paper.

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Correspondence to Michel Cloitre.

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The authors declare no competing financial interests.

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Seth, J., Mohan, L., Locatelli-Champagne, C. et al. A micromechanical model to predict the flow of soft particle glasses. Nature Mater 10, 838–843 (2011). https://doi.org/10.1038/nmat3119

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