Micro–macro-discrepancies in nonlinear microrheology: I. Quantifying mechanisms in a suspension of Brownian ellipsoids

Abstract

Active and nonlinear microrheology experiments involve a colloidal probe that is forced to move within a material, with the goal of recovering the nonlinear rheological response properties of the material. Various mechanisms cause discrepancies between the nonlinear rheology measured microrheologically and macroscopically, including direct probe–bath collisions, the Lagrangian unsteadiness experienced by the material elements, and the spatially inhomogeneous and rheologically mixed strain field set up around the probe. Here, we perform computational nonlinear microrheology experiments, in which a colloidal probe translates through a dilute suspension of Brownian ellipsoids, whose results we compare against analogous computational experiments on the macroscopic shear rheology of the same model material. The quantitative impact of each of the mechanisms for micro–macro-discrepancy can thus be computed directly, with additional computational experiments performed where the processes in question are ‘turned off’. We show that all three discrepancy mechanisms impact the microrheological measurement quantitatively, and that none can be neglected. This motivates a search for microrheological probes whose geometry or forcing is optimized to minimize these impacts, which we present in a companion article.