Robust excitons inhabit soft supramolecular nanotubes

Dörthe M. Eisele, Dylan H. Arias, Xiaofeng Fu, Erik A. Bloemsma, Colby P. Steiner, Russell A. Jensen, Patrick Rebentrost, Holger Eisele, Andrei Tokmakoff, Seth Lloyd, Keith A. Nelson, Daniela Nicastro, Jasper Knoester, Moungi G. Bawendi

Research output: Contribution to journalArticle

59 Scopus citations

Abstract

Nature's highly efficient light-harvesting antennae, such as those found in green sulfur bacteria, consist of supramolecular building blocks that self-assemble into a hierarchy of close-packed structures. In an effort to mimic the fundamental processes that govern nature's efficient systems, it is important to elucidate the role of each level of hierarchy: from molecule, to supramolecular building block, to close-packed building blocks. Here, we study the impact of hierarchical structure. We present a model system that mirrors nature's complexity: cylinders self-assembled from cyanine-dye molecules. Our work reveals that even though close-packing may alter the cylinders' soft mesoscopic structure, robust delocalized excitons are retained: Internal order and strong excitation-transfer interactions-prerequisites for efficient energy transport-are both maintained. Our results suggest that the cylindrical geometry strongly favors robust excitons; it presents a rational design that is potentially key to nature's high efficiency, allowing construction of efficient lightharvesting devices even from soft, supramolecular materials.

Original languageEnglish (US)
Pages (from-to)E3367-E3375
JournalProceedings of the National Academy of Sciences of the United States of America
Volume111
Issue number33
DOIs
StatePublished - Aug 19 2014

Keywords

  • Exciton theory
  • Light-harvesting antennae systems
  • Photosynthesis
  • Self-assembled excitonic nanoscale systems
  • Supramolecular assembly

ASJC Scopus subject areas

  • General

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    Eisele, D. M., Arias, D. H., Fu, X., Bloemsma, E. A., Steiner, C. P., Jensen, R. A., Rebentrost, P., Eisele, H., Tokmakoff, A., Lloyd, S., Nelson, K. A., Nicastro, D., Knoester, J., & Bawendi, M. G. (2014). Robust excitons inhabit soft supramolecular nanotubes. Proceedings of the National Academy of Sciences of the United States of America, 111(33), E3367-E3375. https://doi.org/10.1073/pnas.1408342111