Recent developments in kinetically controlled supramolecular polymerization permit control of the size (i.e., length and area) of self-assembled nanostructures. However, control of molecular self-assembly at a level comparable with organic synthetic chemistry and the achievement of structural complexity at a hierarchy larger than the molecular level remain challenging. This study focuses on controlling the aspect ratio of supramolecular nanosheets. A systematic understanding of the relationship between the monomer structure and the self-assembly energy landscape has derived a new monomer capable of forming supramolecular nanosheets. With this monomer in hand, the aspect ratio of a supramolecular nanosheet is demonstrated that it can be controlled by modulating intermolecular interactions in two dimensions.
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