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 language | English (US) |
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Pages (from-to) | E3367-E3375 |
Journal | Proceedings of the National Academy of Sciences of the United States of America |
Volume | 111 |
Issue number | 33 |
DOIs | |
State | Published - Aug 19 2014 |
Keywords
- Exciton theory
- Light-harvesting antennae systems
- Photosynthesis
- Self-assembled excitonic nanoscale systems
- Supramolecular assembly
ASJC Scopus subject areas
- General