Network physics of attractive colloidal gels: Resilience, Rigidity, and Phase Diagram

TL;DR

This paper uses network science to analyze the structure and elasticity of attractive colloidal gels, revealing how rigidity emerges from fractal clusters and establishing a phase diagram based on network resilience.

Contribution

It introduces a novel network-based approach to characterize colloidal gel networks and quantitatively relate their structure to elasticity and phase behavior.

Findings

Elasticity correlates with network resilience.

A phase diagram with a clear solid-liquid boundary was experimentally validated.

Cluster networks reveal the physical features of gels at different attraction levels.

Abstract

Attractive colloidal gels exhibit solid-like behavior at vanishingly small fractions of solids, owing to ramified space-spanning networks that form due to particle-particle interactions. These networks give the gel its rigidity, and as the attraction between the particles grows, so does the elasticity of the colloidal network formed. The emergence of this rigidity can be described through a mean field approach; nonetheless, fundamental understanding of how rigidity varies in gels of different attraction strengths is lacking. Moreover, recovering an accurate gelation phase diagram based on the system's variables have been an extremely challenging task. Understanding the nature of these fractal clusters, and how rigidity emerges from their connections is key to controlling and designing gels with desirable properties. Here, we employ well-established concepts of network science to interrogate and characterize the network of colloidal gels. We construct a particle-level network, having all the spatial coordinates of colloids with different attraction levels, and also identify polydisperse rigid fractal clusters using a Gaussian Mixture Model, to form a coarse-grained cluster network that distinctly shows main physical features of the colloidal gels. A simple mass-spring model then is used to recover quantitatively the elasticity of colloidal gels from these cluster networks. Interrogating the resilience of these gel networks show that the elasticity of a gel (a dynamic property) is directly correlated to its cluster network's resilience (a static measure). Finally, we use the resilience investigations to devise [and experimentally validate] a fully resolved phase diagram for colloidal gelation, with a clear solid-liquid phase boundary using a single volume fraction of particles well beyond this phase boundary.