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Ali Mohraz

Publications and source records attributed to Ali Mohraz.

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Rheology and Dynamic Arrest in Colloidal Depletion Gels Mediated by Surface Brush Density

We use the density of surface-grafted polymers as a geometry-preserving control parameter for tuning the rheology of colloidal depletion gels. Reducing brush density accelerates gelation and produces gels with higher plateau storage modulus and yield stress. This mechanical enhancement is not accompanied by increased local densification; low-brush networks exhibit lower average contact number and reduced spatial heterogeneity while displaying stronger elastic responses than their high-brush counterparts. Our findings demonstrate a reduced coordination threshold to form elastic nodes in the low-brush gel network. In addition, low-brush gels relax more slowly, accumulate less creep deformation, and exhibit lower effective noise temperatures within the Soft Glassy Rheology framework. These results establish surface-brush density as an experimentally accessible control parameter for colloidal depletion gel rheology with coupled changes in effective attraction, network architecture, and contact kinematics.

cond-mat.soft

Size matters more than packing in bimodal colloidal gel compositions

Colloidal gels are frequently modeled as monodisperse particle networks, although practical formulations commonly contain particles with multiple characteristic sizes. Here, we use large-scale, hydrodynamically resolved simulations of colloidal depletion gels to isolate the effects of particle size and local packing in bimodal systems with a small-to-large size ratio of 1:2. Increasing the large-particle fraction introduces new heterotypic angular motifs and substantially increases the fraction of bonds participating in tetrahedral structures, with a maximum at intermediate composition. However, these additional rigid motifs do not reorganize into larger or more highly connected tetrahedral aggregates. The mean coordination and characteristic aggregate size remain nearly composition independent. By contrast, the void and cluster-size distributions coarsen systematically as the large-particle fraction increases. These mesoscale distributions largely collapse when normalized by a composition-dependent particle length scale, indicating that changes in composition primarily rescale gel architecture rather than producing distinct rigid-network topologies. An elastic modulus estimated using Cauchy-Born theory similarly follows this effective length scale more closely than the abundance of local tetrahedral motifs. These results show that, for moderate size disparity, particle size controls the structural scale and predicted mechanical response of bimodal colloidal gels more strongly than enhanced local packing.

cond-mat.soft

Bimodal colloids highlight the structural mirror of rigidity percolation and yielding

In metastable particulate gels, it is tempting to believe that the dynamic similarities between the fluid-to-solid non-linear phase transition of rigidity percolation and the solid-to-fluid transition that occurs during yielding represent mirror images of the same continuous process. Even though these behaviors are clearly dynamically similar, their multi-scale nature makes it difficult to determine if they could also follow a unified structural pathway. We know from model monodisperse colloidal gels that both yielding and the elastic modulus seem to be heavily influenced by a small subset of topologically distinct singly-connected bridges linking mesoscale features. Here we use particle simulations to examine the participation of different classes of particle-level bonds and their contributions to the bulk mechanical response. We find that rigidity is disproportionately supported by singly connected intercluster bridges, whereas yielding localizes at bonds with high edge-betweenness centrality (EBC); strikingly, these independently identified populations substantially overlap and perform comparable mechanical roles. Bimodality exposes this correspondence by concentrating large-particle contacts in both populations, thereby providing a compositional label for the common backbone. Thus, rigidity and yielding are opposing mechanical manifestations of the same mesoscale structure: the intercluster bottlenecks that establish rigidity are also the sites at which rigidity is preferentially lost.

cond-mat.soft

Brush-mediated angular constraints reshape structure, rigidity, and percolation in colloidal depletion gels

Colloidal gels, like many other soft and disordered solids derive their mechanical properties not only from the strength of interparticle attraction, but also from the symmetry of the forces that constrain particle motion. While non-central interactions are known to profoundly alter rigidity and elasticity, they are typically introduced through particle anisotropy, surface roughness, or patchy interactions, obscuring their independent role. Here we demonstrate a minimal and geometry-preserving route to emergent non-central forces in colloidal gels by reducing the density of surface-grafted polymer brushes. At low brush density, partial brush interpenetration introduces an effective angular bending rigidity at particle contacts, despite fully isotropic particle geometry. This emergent constraint suppresses local densification, stabilizes low-coordination networks, and produces highly ramified gel structures with enhanced elasticity. Combining experiments, simulations, and mean-field theory, we show that these non-central constraints reorganize structure and mechanics across length scales, shifting gelation boundaries and increasing the elastic modulus by nearly a factor of three. Our results establish surface brush density as a generic control parameter for programming interaction symmetry in soft particulate matter, with implications for rigidity, percolation, and mechanical design in disordered systems.

cond-mat.soft