Figure 3.

Rheology of Granular Hydrogels. Frequency sweeps from 10 Hz to 0.01 Hz at 1 % amplitude for (A) guest-host microspheres and fragmented gels and (B) host-host microspheres and fragmented gels. All gels demonstrate viscoelastic behavior over the frequency range. Strain sweep from 100 % shear strain to 0.01 % shear strain for (C) guest-host microspheres (blue, circle) and fragmented gels (orange, circle) and (D) host-host microspheres (blue, triangle) and fragmented gels (orange, triangle). (E) Storage modulus at 1 Hz for guest-host and host-host microspheres and fragmented gels. Cyclic strain alternating between low (1 %) and high (500 %) strain over 60 seconds for (F) guest-host and (G) host-host gels. The high strain region is indicated by a grey overlay. (H) The recovery (G’/G’₀) of the initial and final storage modulus in the cyclic strain experiment (F, G). (I, J) Shear-thinning was identified in both the microsphere and fragmented microgels via a unidirectional shear rate sweep. The solid lines indicate the linear regression at the zero-frequency limit. The curvature was determined to be due to the time-dependent nature of reconstruction within the material. Yielding was not observed as determined by the yield strain rate in the oscillatory strain sweeps (Figure 3C, D, Supplementary Figure 1). (K) The calculated yield stress from the unidirectional shear rate sweeps and the oscillatory shear strain sweeps comparison. All groups fall within the 1:1 correlation except for the microspheres which are still within the two-fold range. For all panels, significance between means of three or more groups determined by one-way ANOVA, p < 0.05 with Tukey’s post-hoc pairwise comparisons. ** = p < 0.01, *** = p < 0.001, **** = p < 0.0001.