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

Abstract: 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.