Utilizing redox-chemistry to elucidate the nature of exciton transitions in supramolecular dye nanotubes

D. M. Eisele, C. W. Cone, E. A. Bloemsma, S. M. Vlaming, C. G. F. van der Kwaak, R. J. Silbey, M. G. Bawendi, J. Knoester*, J. P. Rabe, D. A. Vanden Bout

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

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Abstract

Supramolecular assemblies that interact with light have recently garnered much interest as well-defined nanoscale materials for electronic excitation energy collection and transport. However, to control such complex systems it is essential to understand how their various parts interact and whether these interactions result in coherently shared excited states (excitons) or in diffusive energy transport between them. Here, we address this by studying a model system consisting of two concentric cylindrical dye aggregates in a light-harvesting nanotube. Through selective chemistry we are able to unambiguously determine the supramolecular origin of the observed excitonic transitions. These results required the development of a new theoretical model of the supramolecular structure of the assembly. Our results demonstrate that the two cylinders of the nanotube have distinct spectral responses and are best described as two separate, weakly coupled excitonic systems. Understanding such interactions is critical to the control of energy transfer on a molecular scale, a goal in various applications ranging from artificial photosynthesis to molecular electronics.

Original languageEnglish
Pages (from-to)655-662
Number of pages8
JournalNature Chemistry
Volume4
Issue number8
DOIs
Publication statusPublished - Aug-2012

Keywords

  • ENERGY-TRANSFER
  • MOLECULAR NANOTUBES
  • MICROSCOPIC MODEL
  • NANOSCALE SYSTEMS
  • CARBOCYANINE DYE
  • CHIRAL STACKS
  • J-AGGREGATE
  • DYNAMICS
  • LIGHT
  • FLUORESCENCE

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