Gelation and Phase Separation of Attractive Colloids

TitleGelation and Phase Separation of Attractive Colloids
Publication TypeThesis
Year of Publication2008
AuthorsLu, Peter J.
UniversityHarvard University
Thesis TypePhD

I present several scientific and technical contributions in this thesis. I demonstrate that the gelation of spherical particles with isotropic, short-range attractive interactions is initiated by spinodal decomposition, a thermodynamic instability that triggers the formation of clusters that span and dynamically arrest to create a gel. This simple, universal gelation picture does not depend on microscopic system-specific details---thus broadly describing any particle system with short-range attractions---and suggests that gelation, often considered a purely kinetic phenomenon, is in fact a direct consequence of equilibrium liquid-gas phase separation. I also demonstrate that spherical particles with isotropic attractive interactions exhibit a stable phase---a fluid of particle clusters---that persists on experimental timescales even in the absence of any long-range Coulombic charge repulsion; this contrasts some expectations based on simulation and theory. I describe a new capability I created by integrating accelerated image processing software that I wrote into a high-speed confocal microscope system that I developed: active target-locking, the ability to follow freely-moving complex objects within a microscope sample, even as they change size, shape, and orientation---in real time. Finally, I report continuous, month-long observations of near-critical spinodal decomposition of colloids with isotropic attractions, aboard the International Space Station. I also include detailed descriptions, with examples and illustrations, of the tools and techniques that I have developed to produce these results.

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Peter J. Lu  |  Harvard University  |  Cambridge, MA 02138 USA |