Viscoelasticity of non-colloidal hydrogel particle suspensions at the liquid-solid transition

Suspensions of soft particles transition from a viscous fluid to a soft material upon increases in phase volume. The criteria defining the transition to this jammed state are difficult to define due to the porous and deformable nature of soft particles. Here, we characterise the rheology of aqueous suspensions of industrially relevant non-colloidal, polydisperse, frictional agarose microgels and evaluate shear and viscoelastic behaviour across a range of phase volumes from the dilute regime to the highly concentrated regime. In order to model the viscoelastic response of suspensions without free fitting parameters, the random close packing volume fraction (φrcp) and the particle modulus are determined, respectively, from particle size distribution measurements and direct measurements of reduced elastic modulus of individual particles (Erp) using Atomic Force Microscopy. It is found that at φrcp, previously shown to correspond to divergence of the viscosity, also corresponds to the suspension transition from a viscous to viscoelastic fluid. However, the transition to a jammed solid-like state (φj) occurs at phase volumes exceeding this value (i.e. φj > φrcp). The suspension modulus and its sudden growth at φj are well-predicted by the Evans and Lips model that incorporates the Erp of the hydrogel particles. This rheological behaviour showing a dual transition is reminiscent of two families of systems: (i) colloidal suspensions and (ii) frictional-adhesive non-colloidal suspensions. However, it does not strictly follow either case. We propose that the width of the transition region is dictated by frictional contact, particle size distribution and particle modulus, and plan to further probe this in future work.