Abstract

We present an experimental investigation of the solid–fluid transition in a yield stress shear thinning physical gel (Carbopol® 940) under shear. Upon a gradual increase of the external forcing, we observe three distinct deformation regimes: an elastic solid-like regime (characterized by a linear stress–strain dependence), a solid–fluid phase coexistence regime (characterized by a competition between destruction and reformation of the gel), and a purely viscous regime (characterized by a power law stress-rate of strain dependence). The competition between destruction and reformation of the gel is investigated via both systematic measurements of the dynamic elastic moduli (as a function of stress, the amplitude, and temperature) and unsteady flow ramps. The transition from solid behavior to fluid behavior displays a clear hysteresis upon increasing and decreasing values of the external forcing. We find that the deformation power corresponding to the hysteresis region scales linearly with the rate at which the material is being forced (the degree of flow unsteadiness). In the asymptotic limit of small forcing rates, our results agree well with previous steady state investigations of the yielding transition. Based on these experimental findings, we suggest an analogy between the solid–fluid transition and a first-order phase transition, e.g., the magnetization of a ferro-magnet where irreversibility and hysteresis emerge as a consequence of a phase coexistence regime. In order to get further insight into the solid–fluid transition, our experimental findings are complemented by a simple kinetic model that qualitatively describes the structural hysteresis observed in our rheological experiments. The model is fairly well validated against oscillatory flow data by a partial reconstruction of the Pipkin space of the material’s response and its nonlinear spectral behavior.

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