Robust excitons inhabit soft supramolecular nanotubes.

نویسندگان

  • 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
چکیده

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 light-harvesting devices even from soft, supramolecular materials.

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عنوان ژورنال:
  • Proceedings of the National Academy of Sciences of the United States of America

دوره 111 33  شماره 

صفحات  -

تاریخ انتشار 2014