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Register a new userUsing patchy particles to prevent local rearrangements in models of non-equilibrium colloidal gels
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Simple models based on isotropic interparticle attractions often fail to capture experimentally observed structures of colloidal gels formed through spinodal decomposition and subsequent arrest: the resulting gels are typically denser and less branched than their experimental counterparts. Here we simulate gels formed from soft particles with directional attractions (patchy particles), designed to inhibit lateral particle rearrangement after aggregation. We directly compare simulated structures with experimental colloidal gels made using soft attractive microgel particles, by employing a skeletonization method that reconstructs the 3-dimensional backbone from experiment or simulation. We show that including directional attractions with sufficient valency leads to strongly branched structures compared to isotropic models. Furthermore, combining isotropic and directional attractions provides additional control over aggregation kinetics and gel structure. Our results show that the inhibition of lateral particle rearrangements strongly affects the gel topology, and is an important effect to consider in computational models of colloidal gels.
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We image local structural rearrangements in soft colloidal glasses under small periodic perturbations induced by thermal cycling. Local structural entropy $S_{2}$ positively correlates with observed rearrangements in colloidal glasses. The high $S_{2}$ values of the rearranging clusters in glasses indicate that fragile regions in glasses are structurally less correlated, similar to structural defects in crystalline solids. Slow-evolving high $S_{2}$ spots are capable of predicting local rearrangements long before the relaxations occur, while fluctuation-created high $S_{2}$ spots best correlate with local deformations right before the rearrangement events. Local free volumes are also found to correlate with particle rearrangements at extreme values, although the ability to identify relaxation sites is substantially lower than $S_{2}$. Our experiments provide an efficient structural identifier for the fragile regions in glasses, and highlight the important role of structural correlations in the physics of glasses.
This paper has been temporarily withdrawn by the authors. We have recently found that noise in the experiments is at the origin of the supposed back-and-forth motion which is discussed in the first version of the paper. As a consequence, figs 4 and 5 as well as their discussion are incorrect. Figure 1 and the general trend of fig. 2 are still valid. At this time, we are uncertain whether or not the short time behavior of cI, shown in fig. 3, is affected by measurement noise. We are working on a new version of the paper, using new techniques that allow us to correct for the experimental noise.
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