Towards a bottom-up understanding of self-assembly and gelation in colloidal and biomolecular systems

Alessio Zaccone (Technical University Munich)

Self-assembly of macromolecules via non-covalent physical bonding often implies that the binding energy between two molecules is on the order of a few kTs. Therefore, widely used paradigms employed in colloidal science such as diffusion-limited irreversible aggregation are not applicable because thermal breakup of bonds is important and it may induce significant restructuring inside a cluster, besides affecting the self-assembly kinetics. The restructuring process may lead to different self-assembly morphologies (micelles, filaments, compact aggregates etc).

We recently develop a new approach which describes self-assembly via diffusion-controlled transport of nanoparticles/molecules in solution crucially allowing for spontaneous thermal bond-breakup. The framework has been successfully applied to self-assembly and gelation of thermoresponsive polymers in water (in both core-shell colloidal and block-copolymer form) to obtain information about the effective bonding interaction which is otherwise not accessible, in combination with light scattering and neutron scattering experiments. Application of this framework to protein self-assembly allows us to relate the aggregate morphology and polymorphism to intermolecular interaction parameters.

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