Kinetic control over pathway complexity in supramolecular polymerization through modulating the energy landscape by rational molecular design

Soichiro Ogi, Tomoya Fukui, Melinda L. Jue, Masayuki Takeuchi, Kazunori Sugiyasu

Research output: Contribution to journalArticlepeer-review

104 Citations (Scopus)

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.

Original languageEnglish
Pages (from-to)14363-14367
Number of pages5
JournalAngewandte Chemie - International Edition
Volume53
Issue number52
DOIs
Publication statusPublished - 2014 Dec 22
Externally publishedYes

Keywords

  • Pathway complexity
  • Porphyrins
  • Supramolecular polymerization
  • Systems chemistry
  • Time evolution

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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