Rheological implications of embedded active matter in colloidal gels

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.