Dynamical heterogeneity (DH) has been observed in many systems approaching the glass or jamming transition. Whether DH has a structural origin is under heated debate. To provide a deeper understanding, in this thesis I investigate the microscopic dynamics in weakly attractive colloidal systems by confocal fluorescence microscopy. The van Hove density-density correlation function is applied to our systems. Separable fast and slow populations emerge in the self part (svH), while the distinct part shows a strong signature of DH close to the gel transition. At intermediate time, svH shows a purely exponential tail, mainly arising from the fast population. I show that this broad tail is a direct consequence of the occurrence of rare large jumps that are statistically distributed. The slow population tends to form a space-spanning backbone, and its mean squared displacement close to the gel transition exhibits a plateau, whose height is consistent with the range of attraction, suggesting a bonding mechanism for the dynamical arrest. I further examine various quantities characterizing local structure and local dynamics and a strong correlation is identified between them. Subsequently, I develop order parameters for quantifying amorphous structure and apply them to our systems. I find that attractive colloidal systems exhibit higher order under higher attraction tension, while hard spheres become more ordered under higher compression. Finally, I investigate the effect of the range of attraction on the structure and dynamics of attractive colloidal systems. I observe that the system with shorter range of attraction forms a denser and more heterogeneous structure. Meanwhile, I observe an even stronger dynamical heterogeneity. These observations provide further evidence of a connection between structural heterogeneity and dynamical heterogeneity in these systems, providing guidance for a theoretical description of the dynamical arrest as well as the relaxation mechanisms upon gelation and its relation to solidification in glasses. / In order to do all of this, I first implemented full 3D subpixel resolution localization of particles and improved particle tracking algorithms tailored for the sorts of heterogenous dynamics these systems exhibit, that otherwise confounds existing methods such that the very relaxation mechanisms would be missed. This allows us to obtain unprecedented precision in positions of all of the particles and complete tracking, both of which are essential for correctly determining system properties that depend on measured particle dynamics.
| Identifer | oai:union.ndltd.org:LACETR/oai:collectionscanada.gc.ca:QMM.115677 |
| Date | January 2008 |
| Creators | Gao, Yongxiang. |
| Publisher | McGill University |
| Source Sets | Library and Archives Canada ETDs Repository / Centre d'archives des thèses électroniques de Bibliothèque et Archives Canada |
| Language | English |
| Detected Language | English |
| Type | Electronic Thesis or Dissertation |
| Format | application/pdf |
| Coverage | Doctor of Philosophy (Department of Physics.) |
| Rights | All items in eScholarship@McGill are protected by copyright with all rights reserved unless otherwise indicated. |
| Relation | alephsysno: 003133033, proquestno: AAINR66298, Theses scanned by UMI/ProQuest. |
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