Kinetic Control over Pathway Complexity in Supramolecular Polymerization through Modulating the Energy Landscape by Rational Molecular Design |
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Authors: | Dr Soichiro Ogi Tomoya Fukui Melinda L Jue Prof Dr Masayuki Takeuchi Dr Kazunori Sugiyasu |
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Institution: | 1. Organic Materials Group, Polymer Materials Unit, National Institute for Materials Science (NIMS), 1‐2‐1 Sengen, Tsukuba, Ibaraki 305‐0047 (Japan);2. Department of Materials Science and Engineering, Graduate School of Pure and Applied Sciences, University of Tsukuba, 1‐1‐1 Tennodai, Tsukuba, Ibaraki 305‐8577 (Japan) |
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Abstract: | Far‐from‐equilibrium thermodynamic systems that are established as a consequence of coupled equilibria are the origin of the complex behavior of biological systems. Therefore, research in supramolecular chemistry has recently been shifting emphasis from a thermodynamic standpoint to a kinetic one; however, control over the complex kinetic processes is still in its infancy. Herein, we report our attempt to control the time evolution of supramolecular assembly in a process in which the supramolecular assembly transforms from a J‐aggregate to an H‐aggregate over time. The transformation proceeds through a delicate interplay of these two aggregation pathways. We have succeeded in modulating the energy landscape of the respective aggregates by a rational molecular design. On the basis of this understanding of the energy landscape, programming of the time evolution was achieved through adjusting the balance between the coupled equilibria. |
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Keywords: | pathway complexity porphyrins supramolecular polymerization systems chemistry time evolution |
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