More Like this

1. Rheological implications of embedded active matter in colloidal gels

   https://doi.org/10.1039/c9sm01496a  

   Szakasits, Megan E.; Saud, Keara T.; Mao, Xiaoming; Solomon, Michael J. (October 2019, Soft Matter)

   null (Ed.)

   Colloidal gels represent an important class of soft matter, in which networks formed due to strong, short-range interactions display solid-like mechanical properties, such as a finite low-frequency elastic modulus. Here we examine the effect of embedded active colloids on the linear viscoelastic moduli of fractal cluster colloidal gels. We find that the autonomous, out-of-equilibrium dynamics of active colloids incorporated into the colloidal network decreases gel elasticity, in contrast to observed stiffening effects of myosin motors in actin networks. Fractal cluster gels are formed by the well-known mechanism of aggregating polystyrene colloids through addition of divalent electrolyte. Active Janus particles with a platinum hemisphere are created from the same polystyrene colloids and homogeneously embedded in the gels at dilute concentration at the time of aggregation. Upon addition of hydrogen peroxide – a fuel that drives the diffusiophoretic motion of the embedded Janus particles – the microdynamics and mechanical rheology change in proportion to the concentration of hydrogen peroxide and the number of active colloids. We propose a theoretical explanation of this effect in which the decrease in modulus is mediated by active motion-induced softening of the inter-particle attraction. Furthermore, we characterize the failure of the fluctuation–dissipation theorem in the active gels by identifying a discrepancy between the frequency-dependent macroscopic viscoelastic moduli and the values predicted by microrheology from measurement of the gel microdynamics. These findings support efforts to engineer gels for autonomous function by tuning the microscopic dynamics of embedded active particles. Such reconfigurable gels, with multi-state mechanical properties, could find application in materials such as paints and coatings, pharmaceuticals, self-healing materials, and soft robotics. 

   more » « less
2. Stress–stress correlations reveal force chains in gels

   https://doi.org/10.1063/5.0131473  

   Vinutha, H A; Diaz_Ruiz, Fabiola_Doraly; Mao, Xiaoming; Chakraborty, Bulbul; Del_Gado, Emanuela (March 2023, The Journal of Chemical Physics)

   We investigate the spatial correlations of microscopic stresses in soft particulate gels using 2D and 3D numerical simulations. We use a recently developed theoretical framework predicting the analytical form of stress–stress correlations in amorphous assemblies of athermal grains that acquire rigidity under an external load. These correlations exhibit a pinch-point singularity in Fourier space. This leads to long-range correlations and strong anisotropy in real space, which are at the origin of force-chains in granular solids. Our analysis of the model particulate gels at low particle volume fractions demonstrates that stress–stress correlations in these soft materials have characteristics very similar to those in granular solids and can be used to identify force chains. We show that the stress–stress correlations can distinguish floppy from rigid gel networks and that the intensity patterns reflect changes in shear moduli and network topology, due to the emergence of rigid structures during solidification. 

   more » « less
3. A basic model for the nonlinear rheology of bijels

   https://doi.org/10.1122/8.0000914  

   Ching, Herman; Mohraz, Ali (January 2025, Journal of Rheology)

   We examine the rheology of bicontinuous interfacially jammed emulsion gels (bijels) beyond the limit of linear viscoelasticity and propose a simple model that connects bijel rheology to anticipated microstructural changes in the continuous particle-laden interface. The basic elements of our model are constructed from a linear stress relaxation experiment, which suggests glasslike rheology mediated by α (out-of-cage) and β (in-cage) particle dynamics along the interface in this limit. Extending to medium amplitude oscillatory shear experiments then reveals signatures of nonlinearity, which we rationalize as the combined effect of shear-induced dilation of the interface and its simultaneous recompaction by interfacial tension, as well as potential buckling along portions of the interface under compression. Informed by these observations, we present a double Maxwell model with sigmoidal nonlinearities introduced to account for how interfacial dilation and recompaction affect the intercage particle dynamics (α relaxation) along the interface and buckling. This simple model successfully captures the general features of nonlinear rheology in bijels, indicating that their linear-to-nonlinear transition is associated with loss of compaction along the dilated and buckling along the compacted regions of the interface. Our results shed initial light on the microstructural origins of nonlinear rheology in bijels and the reconfigurability afforded in these systems by the balance of glassy particle dynamics and interfacial recompaction under shear deformation. 

   more » « less
4. Topological origins of yielding in short-ranged weakly attractive colloidal gels

   https://doi.org/10.1063/5.0123096  

   Mangal, Deepak; Nabizadeh, Mohammad; Jamali, Safa (January 2023, The Journal of Chemical Physics)

   Yielding of the particulate network in colloidal gels under applied deformation is accompanied by various microstructural changes, including rearrangement, bond rupture, anisotropy, and reformation of secondary structures. While much work has been done to understand the physical underpinnings of yielding in colloidal gels, its topological origins remain poorly understood. Here, employing a series of tools from network science, we characterize the bonds using their orientation and network centrality. We find that bonds with higher centralities in the network are ruptured the most at all applied deformation rates. This suggests that a network analysis of the particulate structure can be used to predict the failure points in colloidal gels a priori. 

   more » « less
5. Microscopic dynamics underlying the stress relaxation of arrested soft materials

   https://doi.org/10.1073/pnas.2201566119  

   Song, Jake; Zhang, Qingteng; de Quesada, Felipe; Rizvi, Mehedi H.; Tracy, Joseph B.; Ilavsky, Jan; Narayanan, Suresh; Del Gado, Emanuela; Leheny, Robert L.; Holten-Andersen, Niels; et al (July 2022, Proceedings of the National Academy of Sciences)

   Arrested soft materials such as gels and glasses exhibit a slow stress relaxation with a broad distribution of relaxation times in response to linear mechanical perturbations. Although this macroscopic stress relaxation is an essential feature in the application of arrested systems as structural materials, consumer products, foods, and biological materials, the microscopic origins of this relaxation remain poorly understood. Here, we elucidate the microscopic dynamics underlying the stress relaxation of such arrested soft materials under both quiescent and mechanically perturbed conditions through X-ray photon correlation spectroscopy. By studying the dynamics of a model associative gel system that undergoes dynamical arrest in the absence of aging effects, we show that the mean stress relaxation time measured from linear rheometry is directly correlated to the quiescent superdiffusive dynamics of the microscopic clusters, which are governed by a buildup of internal stresses during arrest. We also show that perturbing the system via small mechanical deformations can result in large intermittent fluctuations in the form of avalanches, which give rise to a broad non-Gaussian spectrum of relaxation modes at short times that is observed in stress relaxation measurements. These findings suggest that the linear viscoelastic stress relaxation in arrested soft materials may be governed by nonlinear phenomena involving an interplay of internal stress relaxations and perturbation-induced intermittent avalanches. 

   more » « less