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...
Main Authors: | , , , , , , , , , , , , , |
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Other Authors: | |
Format: | Article |
Language: | en_US |
Published: |
National Academy of Sciences (U.S.)
2015
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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 |
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. |
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