Robust excitons inhabit soft supramolecular nanotubes

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...

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Bibliographic Details
Main Authors: Rebentrost, Frank Patrick, Lloyd, Seth, Nelson, Keith Adam, Bawendi, Moungi G., Eisele, Dorthe M., Arias, Dylan H., Fu, Xiaofeng, Bloemsma, Erik A., Steiner, Colby P., Jensen, Russell A., Eisele, Holger, Tokmakoff, Andrei, Nicastro, Daniela, Knoester, Jasper
Other Authors: Massachusetts Institute of Technology. Department of Chemistry
Format: Article
Language:en_US
Published: National Academy of Sciences (U.S.) 2015
Online Access:http://hdl.handle.net/1721.1/93791
https://orcid.org/0000-0003-2220-4365
https://orcid.org/0000-0003-2358-6967
https://orcid.org/0000-0002-2067-6716
https://orcid.org/0000-0001-7804-5418
https://orcid.org/0000-0002-6728-8163
Description
Summary: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.