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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| Format: | Article |
| Language: | en_US |
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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 |
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| author | 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 |
| author2 | Massachusetts Institute of Technology. Department of Chemistry |
| author_facet | Massachusetts Institute of Technology. Department of Chemistry 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 |
| author_sort | Rebentrost, Frank Patrick |
| collection | MIT |
| description | 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. |
| first_indexed | 2024-09-23T15:44:19Z |
| format | Article |
| id | mit-1721.1/93791 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T15:44:19Z |
| publishDate | 2015 |
| publisher | National Academy of Sciences (U.S.) |
| record_format | dspace |
| spelling | mit-1721.1/937912022-10-02T03:44:53Z Robust excitons inhabit soft supramolecular nanotubes 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 Massachusetts Institute of Technology. Department of Chemistry Massachusetts Institute of Technology. Department of Mechanical Engineering Massachusetts Institute of Technology. Research Laboratory of Electronics Rebentrost, Frank Patrick Lloyd, Seth Nelson, Keith Adam Bawendi, Moungi G. Eisele, Dorthe M. Arias, Dylan H. Steiner, Colby P. Jensen, Russell A. 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. United States. Dept. of Energy. Office of Basic Energy Sciences (Energy Frontiers Research Center. Grant DE-SC0001088) United States. Dept. of Energy. Center for Excitonics Alexander von Humboldt-Stiftung (Feodor Lynen Research Fellowship) National Science Foundation (U.S.). Graduate Research Fellowship Program United States. Defense Advanced Research Projects Agency 2015-02-05T18:18:08Z 2015-02-05T18:18:08Z 2014-08 2013-12 Article http://purl.org/eprint/type/JournalArticle 0027-8424 1091-6490 http://hdl.handle.net/1721.1/93791 Eisele, Dorthe M., Dylan H. Arias, Xiaofeng Fu, Erik A. Bloemsma, Colby P. Steiner, Russell A. Jensen, Patrick Rebentrost, et al. “Robust Excitons Inhabit Soft Supramolecular Nanotubes.” Proceedings of the National Academy of Sciences 111, no. 33 (August 4, 2014): E3367–E3375. 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 en_US http://dx.doi.org/10.1073/pnas.1408342111 Proceedings of the National Academy of Sciences of the United States of America Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use. application/pdf National Academy of Sciences (U.S.) National Academy of Sciences (U.S.) |
| spellingShingle | 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 Robust excitons inhabit soft supramolecular nanotubes |
| title | Robust excitons inhabit soft supramolecular nanotubes |
| title_full | Robust excitons inhabit soft supramolecular nanotubes |
| title_fullStr | Robust excitons inhabit soft supramolecular nanotubes |
| title_full_unstemmed | Robust excitons inhabit soft supramolecular nanotubes |
| title_short | Robust excitons inhabit soft supramolecular nanotubes |
| title_sort | robust excitons inhabit soft supramolecular nanotubes |
| url | 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 |
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