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Register a new userNonlinear mechanics of colloidal gels: creep, fatigue and shear-induced yielding
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Colloidal gels are formed through the aggregation of attractive particles, whose size ranges from 10~nm to a few micrometers, suspended in a liquid. Such gels are ubiquitous in everyday life applications, from food products to paints or construction materials, in particular thanks to their ability to easily yield, i.e., to turn from a solid to a liquid under the application of a weak external load. Understanding and controlling the mechanical response of colloidal gels is therefore of prime importance. Depending on the details of the system, however, the resulting gel networks present different microstructural organisations that may lead to widely different mechanical responses. This raises important challenges in fully characterizing yielding and in uncovering the mechanisms of nonlinear response in colloidal gels. In this paper, we distinguish between two classes of colloidal gels showing respectively reversible yielding, where the gel network reforms upon load release, and irreversible yielding, where the network is fully destroyed through fractures and phase separation. This broad, empirical distinction is achieved through rheology and local experiments at a mesoscopic scale, intermediate between the network characteristic size and the sample size. We further discuss how the observables derived from creep and fatigue experiments may be modelled to predict yielding and highlight open questions and future research directions in the domain.
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We examine microstructural and mechanical changes which occur during oscillatory shear flow and reformation after flow cessation of an intermediate volume fraction colloidal gel using rheometry and Brownian Dynamics (BD) simulations. A model depletion colloid-polymer mixture is used, comprising of a hard sphere colloidal suspension with the addition of non-adsorbing linear polymer chains. Results reveal three distinct regimes depending on the strain amplitude of oscillatory shear. Large shear strain amplitudes fully break the structure which results into a more homogenous and stronger gel after flow cessation. Intermediate strain amplitudes densify the clusters and lead to highly heterogeneous and weak gels. Shearing the gel to even lower strain amplitudes creates a less heterogonous stronger solid. These three regimes of shearing are connected to the microscopic shear-induced structural heterogeneity. A comparison with steady shear flow reveals that the latter does not produce structural heterogeneities as large as oscillatory shear. Therefore oscillatory shear is a much more efficient way of tuning the mechanical properties of colloidal gels. Moreover, colloidal gels presheared at large strain amplitudes exhibit a distinct nonlinear response characterized largely by a single yielding process while in those presheared at lower rates a two step yield process is promoted due to the creation of highly heterogeneous structures.
The rheological response, in particular the non-linear response, to oscillatory shear is experimentally investigated in colloidal glasses. The glasses are highly concentrated binary hard-sphere mixtures with relatively large size disparities. For a size ratio of 0.2, a strong reduction of the normalized elastic moduli, the yield strain and stress and, for some samples, even melting of the glass to a fluid is observed upon addition of the second species. This is attributed to the more efficient packing, as indicated by the shift of random close packing to larger total volume fractions. This leads to an increase in free volume which favours cage deformations and hence a loosening of the cage. Cage deformations are also favoured by the structural heterogeneity introduced by the second species. For a limited parameter range, we furthermore found indications of two-step yielding, as has been reported previously for attractive glasses. In samples containing spheres with more comparable sizes, namely a size ratio of 0.38, the cage seems less distorted and structural heterogeneities on larger length scales seem to become important. The limited structural changes are reflected in only a small reduction of the moduli, yield strain and stress.
Rigidity percolation (RP) occurs when mechanical stability emerges in disordered networks as constraints or components are added. Here we discuss RP with structural correlations, an effect ignored in classical theories albeit relevant to many liquid-to-amorphous-solid transitions, such as colloidal gelation, which are due to attractive interactions and aggregation. Using a lattice model, we show that structural correlations shift RP to lower volume fractions. Through molecular dynamics simulations, we show that increasing attraction in colloidal gelation increases structural correlation and thus lowers the RP transition, agreeing with experiments. Hence colloidal gelation can be understood as a RP transition, but occurs at volume fractions far below values predicted by the classical RP, due to attractive interactions which induce structural correlation.
From soft polymeric gels to hardened cement paste, amorphous solids under constant load exhibit a pronounced time-dependent deformation called creep. The microscopic mechanism of such a phenomenon is poorly understood and constitutes a significant challenge in densely packed and chemically reactive granular systems. Both features are prominently present in hydrating cement pastes composed of calcium silicate hydrate (C-S-H) nanoparticles, whose packing density increases as a function of time, while cements hydration is taking place. Performing nano-indentation tests and porosity measurements on a large collection of samples at various hydration degrees, we show that the creep response of hydrating cement paste is mainly controlled by the inter-particle distance, and results from slippage between (C-S-H) nanoparticles. Our findings, which pave the way for the design of concrete with improved creep resistance, provide a unique insight into the microscopic mechanism underpinning the creep response in aging granular materials.
We present numerical results for the breakup of a pair of colloidal particles enveloped by a droplet under shear flow. The smoothed profile method is used to accurately account for the hydrodynamic interactions between particles due to the host fluid. We observe that the critical capillary number, $Ca_{rm B}$, at which droplets breakup depends on a velocity ratio, $E$, defined as the ratio of the boundary shift velocity (that restores the droplet shape to a sphere) to the diffusive flux velocity in units of the particle radius $a$. For $E < 10$, $Ca_{B}$ is independent of $E$, as is consistent with the regime studied by Taylor. When $E > 10$, $Ca_{B}$ behaves as $Ca_{rm B} = 2E^{-1}$, which confirms Karam and Bellingers hypothesis. As a consequence, droplet break up will occur when the time scale of droplet deformation $dot{gamma}^{-1}$ is smaller than the diffusive time scale $t_{D} equiv a^{2}/Ltau$ in units of $a$, where $L$ is the diffusion constant and $tau$ is the 2nd order coefficient of the Ginzburg-Landau type free energy of the binary mixture. We emphasize that the breakup of droplet dispersed particles is not only governed by a balance of forces. We find that velocity competition is one of the important contributing factor.
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