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Supramolecular double-stranded Archimedean spirals and concentric toroids

Norihiko Sasaki, Mathijs F. J. Mabesoone, Jun Kikkawa, Tomoya Fukui, Nobutaka Shioya, Takafumi Shimoaka, , Hideaki Takagi, Rie Haruki, , , , ,
Nature Communications , Volume 11, pp 1-9; doi:10.1038/s41467-020-17356-5

Abstract: Connecting molecular-level phenomena to larger scales and, ultimately, to sophisticated molecular systems that resemble living systems remains a considerable challenge in supramolecular chemistry. To this end, molecular self-assembly at higher hierarchical levels has to be understood and controlled. Here, we report unusual self-assembled structures formed from a simple porphyrin derivative. Unexpectedly, this formed a one-dimensional (1D) supramolecular polymer that coiled to give an Archimedean spiral. Our analysis of the supramolecular polymerization by using mass-balance models suggested that the Archimedean spiral is formed at high concentrations of the monomer, whereas other aggregation types might form at low concentrations. Gratifyingly, we discovered that our porphyrin-based monomer formed supramolecular concentric toroids at low concentrations. Moreover, a mechanistic insight into the self-assembly process permitted a controlled synthesis of these concentric toroids. This study both illustrates the richness of self-assembled structures at higher levels of hierarchy and demonstrates a topological effect in noncovalent synthesis.
Keywords: models / porphyrin / Structures / concentrations / spiral / monomer / Supramolecular / Archimedean / concentric toroids

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