Thixotropy is a phenomenon related to time dependent change in viscosity in the presence or absence of flow. The yield stress, on the other hand, represents the minimum value of stress above which steady flow can be sustained. In addition, the yield stress of a material may also change as a function of time. Both these characteristic features in a material strongly influence the steady state flow curve of the same. This study aims to understand the interrelation between thixotropy, yield stress, and their relation with the flow curve. In this regard, we study five thixotropic materials that show yield stress. The relaxation time of all the five systems shows power-law dependence on aging time with behaviors ranging from weaker than linear, linear to stronger than linear. Furthermore, the elastic modulus and yield stress have been observed to be constant for some systems while time dependent for the others. We also analyze the experimental behavior through a viscoelastic thixotropic structural kinetic model that predicts the observed experimental behavior of constant as well as time-dependent yield stress quite well. These findings indicate that a nonmonotonic steady-state flow curve in a structural kinetic formalism necessarily leads to time-dependent yield stress, while constant yield stress is predicted by a monotonic steady-state flow curve with stress plateau in the limit of low shear rates. The present work, therefore, shows that thixotropic materials may exhibit either monotonic or nonmonotonic flow curves. Consequently, thixotropic materials may show no yield stress, constant yield stress, or time-dependent yield stress.
Chocolate is known to undergo solid–liquid transition upon an increase in temperature as well as under application of deformation field. Upon sudden reduction in temperature from a molten state (or thermal rejuvenation), the rheological properties of chocolate evolve as a function of time under isothermal conditions, a behavior reminiscent of physical aging in polymeric glasses. Then again, subsequent to cessation of shear flow (or mechanical rejuvenation), chocolate shows temporal evolution of the rheological properties, a behavior similar to physical aging in soft glassy materials. In this work, we evaluate three rheological properties—dynamic moduli, relaxation time spectrum, and characteristic relaxation time of chocolate—and compare their evolution after thermal as well as mechanical rejuvenation. We observe that the evolution of the rheological properties subsequent to mechanical rejuvenation is distinctly different from that of thermal rejuvenation, wherein the evolution is more gradual in the former case. On the one hand, this work provides unique insights into how shear affects the rheological behavior of chocolate. On the other hand, this work clearly suggests that chocolate explores different sections of the energy landscape after mechanical rejuvenation compared to that of thermal rejuvenation.
While undergoing gelation transition, a material passes through a distinctive state called the critical gel state. In the neighborhood of this critical gel state, how viscosity, equilibrium modulus, and relaxation times evolve are correlated by scaling relations, and their universality has been validated for materials undergoing the sol - gel transition. In this work, we extend this approach for the gel - sol transition of a thermoresponsive polymeric system of aqueous Poly(vinyl alcohol) (PVOH) gel that passes through the critical state upon increasing temperature. We observe that, in the neighborhood of the critical gel state, the equilibrium modulus and viscosity demonstrate a power law dependence on the relative distance from the critical state in terms of normalized temperature. Furthermore, the relaxation times in the gel and the sol state shows symmetric power law divergence near the critical state. The corresponding critical power law exponents and the dynamic critical exponents computed at the critical gel - sol transition state validate the scaling and hyperscaling relations originally proposed for the critical sol - gel transition very well. Remarkably, the dependence of complex viscosity on frequency at different temperatures shows a comprehensive master curve irrespective of the temperature ramp rate independently in the gel and the sol state. Since sol - gel as well as the gel - sol transitions are opposite to each other, the applicability of the scaling relations validated in this work suggests broader symmetry associated with how the structure evolves around the critical state irrespective of the direction.
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