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Ogi, Soichiro; Fukui, Tomoya; Jue, Melinda L.; Takeuchi, Masayuki; Sugiyasu, Kazunori
Angewandte Chemie (International ed.), December 22, 2014, Volume: 53, Issue: 52Journal Article
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. Finding the right balance: The energy landscape of a supramolecular polymerization in which the supramolecular assembly transforms from a J‐aggregate to an H‐aggregate over time has been modulated by a rational molecular design. Based on this, kinetic control over pathway complexity was achieved through adjusting the balance between the coupled equilibria.
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