Single Hydrogel Particle Mechanics and Dynamics Studied by Combining Capillary Micromechanics with Osmotic Compression

Hydrogels can exhibit a remarkably complex response to external stimuli and show rich mechanical behavior. Previous studies of the mechanics of hydrogel particles have generally focused on their static, rather than dynamic, response, as traditional methods for measuring single particle response at the microscopic scale cannot readily measure time-dependent mechanics. Here, we study both the static and the time-dependent response of a single batch of polyacrylamide (PAAm) particles by combining direct contact forces, applied by using Capillary Micromechanics, a method where particles are deformed in a tapered capillary, and osmotic forces are applied by a high molecular weight dextran solution. We found higher values of the static compressive and shear elastic moduli for particles exposed to dextran, as compared to water ($K_{\mathrm{Dex}}\approx 63$ kPa vs. $K_{\mathrm{water}}\approx 36$ kPa, and $G_{\mathrm{Dex}}\approx 16$ kPa vs. $G_{\mathrm{water}}\approx 7$ kPa), which we accounted for, theoretically, as being the result of the increased internal polymer concentration. For the dynamic response, we observed surprising behavior, not readily explained by poroelastic theories. The particles exposed to dextran solutions deformed more slowly under applied external forces than did those suspended in water (${\tau }_{\mathrm{Dex}}\approx 90$ s vs. ${\tau }_{\mathrm{water}}\approx 15$ s). The theoretical expectation was the opposite. However, we could account for this behaviour by considering the diffusion of dextran molecules in the surrounding solution, which we found to dominate the compression dynamics of our hydrogel particles suspended in dextran solutions.