Significant progress has been made in the field of living/controlled polymerizations over the past decades. The advance in living/controlled polymerizations has enabled the design and tailoring of structurally well-defined macromolecules with complex architectures. Polymers with complex molecular architectures often exhibit properties that are distinct from their linear counterparts. This dissertation aims to exploit the unique properties of rationally designed complex polymer structures to address the challenges related to the preparation of polymeric and hybrid nanostructures, as well as to explore and fundamentally understand the morphology or properties of new macromolecular architecture. The studies presented in this dissertation addressed the challenges (e.g., poor size uniformity, limited accessible compositions) in the formation of polymeric or hybrid nanostructured materials based on the self-assembled polymer micelle approach via rational design of complex spherical star polymer architectures with tailor-made compositions and functionalities through living/controlled polymerizations, as well as investigated the morphology and self-assembly behavior of a newly designed cyclic brush copolymer grafted with P3HT as the side chains. The novel and robust star macromolecular templating strategy developed in this study will open the access to a wide range of structurally and functionally well-defined polymeric and hybrid nanostructured materials with tailor-made compositions and shapes. The findings presented in the work will provide fundamental insights or practical strategies for rational design of polymers with complex macromolecular architectures via living/controlled polymerizations.
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