TY - JOUR
T1 - Supramolecular double-stranded Archimedean spirals and concentric toroids
AU - Sasaki, Norihiko
AU - Mabesoone, Mathijs F.J.
AU - Kikkawa, Jun
AU - Fukui, Tomoya
AU - Shioya, Nobutaka
AU - Shimoaka, Takafumi
AU - Hasegawa, Takeshi
AU - Takagi, Hideaki
AU - Haruki, Rie
AU - Shimizu, Nobutaka
AU - Adachi, Shin ichi
AU - Meijer, E. W.
AU - Takeuchi, Masayuki
AU - Sugiyasu, Kazunori
N1 - Funding Information:
This research was supported by KAKENHI (JP15H05483 and JP19K05592 for K.S.), Scientific Research on Innovative Areas “Soft crystals: science and photofunctions of flexible response systems with high order” (H2004682 for K.S.), “π-System figuration: control of electron and structural dynamism for innovative functions” (JP26102009 for M.T.), and the Nanotechnology Network Project from the Ministry of Education, Culture, Sports, Science and Technology, Japan. The SAXS measurements were performed at the Photon Factory of High Energy Accelerator Research Organization (Approval numbers 2018P010). M.F.J.M. and E.W.M. acknowledge financial support from NWO (TOP-PUNT Grant 10018944) and the Dutch Ministry of Education, Culture, and Science (Gravitation program 024.001.035).
Publisher Copyright:
© 2020, The Author(s).
PY - 2020/12/1
Y1 - 2020/12/1
N2 - 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.
AB - 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.
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U2 - 10.1038/s41467-020-17356-5
DO - 10.1038/s41467-020-17356-5
M3 - Article
C2 - 32681045
AN - SCOPUS:85088108845
VL - 11
JO - Nature Communications
JF - Nature Communications
SN - 2041-1723
IS - 1
M1 - 3578
ER -