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Register a new userCorrelated rigidity percolation and colloidal gels
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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.
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Rheological measurements of model colloidal gels reveal that large variations in the shear moduli as colloidal volume-fraction changes are not reflected by simple structural parameters such as the coordination number, which remains almost a constant. We resolve this apparent contradiction by conducting a normal mode analysis of experimentally measured bond networks of the gels. We find that structural heterogeneity of the gels, which leads to floppy modes and a nonaffine-affine crossover as frequency increases, evolves as a function of the volume fraction and is key to understand the frequency dependent elasticity. Without any free parameters, we achieve good qualitative agreement with the measured mechanical response. Furthermore, we achieve universal collapse of the shear moduli through a phenomenological spring-dashpot model that accounts for the interplay between fluid viscosity, particle dissipation, and contributions from the affine and non-affine network deformation.
Rigidity percolation (RP) is the emergence of mechanical stability in networks. Motivated by the experimentally observed fractal nature of materials like colloidal gels and disordered fiber networks, we study RP in a fractal network. Specifically, we calculate the critical packing fractions of site-diluted lattices of Sierpinski gaskets (SGs) with varying degrees of fractal iteration. Our results suggest that although the correlation length exponent and fractal dimension of the RP of these lattices are identical to that of the regular triangular lattice, the critical volume fraction is dramatically lower due to the fractal nature of the network. Furthermore, we develop a simplified model for an SG lattice based on the fragility analysis of a single SG. This simplified model provides an upper bound for the critical packing fractions of the full fractal lattice, and this upper bound is strictly obeyed by the disorder averaged RP threshold of the fractal lattices. Our results characterize rigidity in ultra-low-density fractal networks.
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.
We study a lattice model of attractive colloids. It is exactly solvable on sparse random graphs. As the pressure and temperature are varied it reproduces many characteristic phenomena of liquids, glasses and colloidal systems such as ideal gel formation, liquid-glass phase coexistence, jamming, or the reentrance of the glass transition.
We sandwich a colloidal gel between two parallel plates and induce a radial flow by lifting the upper plate at a constant velocity. Two distinct scenarios result from such a tensile test: ($i$) stable flows during which the gel undergoes a tensile deformation without yielding, and ($ii$) unstable flows characterized by the radial growth of air fingers into the gel. We show that the unstable regime occurs beyond a critical energy input, independent of the gels macroscopic yield stress. This implies a local fluidization of the gel at the tip of the growing fingers and results in the most unstable wavelength of the patterns exhibiting the characteristic scalings of the classical viscous fingering instability. Our work provides a quantitative criterion for the onset of fingering in colloidal gels based on a local shear-induced yielding, in agreement with the delayed failure framework.
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