Room-Temperature Micron-Scale Exciton Migration in a Stabilized Emissive Molecular Aggregate
We report 1.6 ± 1 μm exciton transport in self-assembled supramolecular light-harvesting nanotubes (LHNs) assembled from amphiphillic cyanine dyes. We stabilize LHNs in a sucrose glass matrix, greatly reducing light and oxidative damage and allowing the observation of exciton–exciton annihilation si...
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| Format: | Article |
| Language: | en_US |
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American Chemical Society
2018
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| Online Access: | http://hdl.handle.net/1721.1/113346 https://orcid.org/0000-0003-1192-4746 https://orcid.org/0000-0002-2710-5545 https://orcid.org/0000-0002-9371-6109 https://orcid.org/0000-0003-2220-4365 https://orcid.org/0000-0002-6728-8163 |
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| author | Eisele, Dörthe M. Caram, Justin R Doria, Sandra Freyria, Francesca Sinclair, Timothy Scott Bawendi, Moungi G Rebentrost, Frank Lloyd, Seth |
| author2 | Massachusetts Institute of Technology. Department of Chemistry |
| author_facet | Massachusetts Institute of Technology. Department of Chemistry Eisele, Dörthe M. Caram, Justin R Doria, Sandra Freyria, Francesca Sinclair, Timothy Scott Bawendi, Moungi G Rebentrost, Frank Lloyd, Seth |
| author_sort | Eisele, Dörthe M. |
| collection | MIT |
| description | We report 1.6 ± 1 μm exciton transport in self-assembled supramolecular light-harvesting nanotubes (LHNs) assembled from amphiphillic cyanine dyes. We stabilize LHNs in a sucrose glass matrix, greatly reducing light and oxidative damage and allowing the observation of exciton–exciton annihilation signatures under weak excitation flux. Fitting to a one-dimensional diffusion model, we find an average exciton diffusion constant of 55 ± 20 cm2/s, among the highest measured for an organic system. We develop a simple model that uses cryogenic measurements of static and dynamic energetic disorder to estimate a diffusion constant of 32 cm2/s, in agreement with experiment. We ascribe large exciton diffusion lengths to low static and dynamic energetic disorder in LHNs. We argue that matrix-stabilized LHNS represent an excellent model system to study coherent excitonic transport.
Keywords: coherent exciton; exciton; exciton delocalization; exciton diffusion; J-aggregate; molecular aggregate |
| first_indexed | 2024-09-23T14:13:43Z |
| format | Article |
| id | mit-1721.1/113346 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T14:13:43Z |
| publishDate | 2018 |
| publisher | American Chemical Society |
| record_format | dspace |
| spelling | mit-1721.1/1133462022-09-28T19:20:53Z Room-Temperature Micron-Scale Exciton Migration in a Stabilized Emissive Molecular Aggregate Eisele, Dörthe M. Caram, Justin R Doria, Sandra Freyria, Francesca Sinclair, Timothy Scott Bawendi, Moungi G Rebentrost, Frank Lloyd, Seth Massachusetts Institute of Technology. Department of Chemistry Massachusetts Institute of Technology. Department of Mechanical Engineering Caram, Justin R Doria, Sandra Freyria, Francesca Sinclair, Timothy Scott Bawendi, Moungi G Rebentrost, Frank Lloyd, Seth We report 1.6 ± 1 μm exciton transport in self-assembled supramolecular light-harvesting nanotubes (LHNs) assembled from amphiphillic cyanine dyes. We stabilize LHNs in a sucrose glass matrix, greatly reducing light and oxidative damage and allowing the observation of exciton–exciton annihilation signatures under weak excitation flux. Fitting to a one-dimensional diffusion model, we find an average exciton diffusion constant of 55 ± 20 cm2/s, among the highest measured for an organic system. We develop a simple model that uses cryogenic measurements of static and dynamic energetic disorder to estimate a diffusion constant of 32 cm2/s, in agreement with experiment. We ascribe large exciton diffusion lengths to low static and dynamic energetic disorder in LHNs. We argue that matrix-stabilized LHNS represent an excellent model system to study coherent excitonic transport. Keywords: coherent exciton; exciton; exciton delocalization; exciton diffusion; J-aggregate; molecular aggregate Eni-MIT Solar Frontiers Center United States. Department of Energy. Center for Excitonics (Grant DE-SC0001088) 2018-01-30T15:58:02Z 2018-01-30T15:58:02Z 2016-09 2016-06 Article http://purl.org/eprint/type/JournalArticle 1530-6984 1530-6992 http://hdl.handle.net/1721.1/113346 Caram, Justin R., et al. “Room-Temperature Micron-Scale Exciton Migration in a Stabilized Emissive Molecular Aggregate.” Nano Letters, vol. 16, no. 11, Nov. 2016, pp. 6808–15. © 2016 American Chemical Society https://orcid.org/0000-0003-1192-4746 https://orcid.org/0000-0002-2710-5545 https://orcid.org/0000-0002-9371-6109 https://orcid.org/0000-0003-2220-4365 https://orcid.org/0000-0002-6728-8163 en_US http://dx.doi.org/10.1021/acs.nanolett.6b02529 Nano Letters 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 American Chemical Society Other univ. web domain |
| spellingShingle | Eisele, Dörthe M. Caram, Justin R Doria, Sandra Freyria, Francesca Sinclair, Timothy Scott Bawendi, Moungi G Rebentrost, Frank Lloyd, Seth Room-Temperature Micron-Scale Exciton Migration in a Stabilized Emissive Molecular Aggregate |
| title | Room-Temperature Micron-Scale Exciton Migration in a Stabilized Emissive Molecular Aggregate |
| title_full | Room-Temperature Micron-Scale Exciton Migration in a Stabilized Emissive Molecular Aggregate |
| title_fullStr | Room-Temperature Micron-Scale Exciton Migration in a Stabilized Emissive Molecular Aggregate |
| title_full_unstemmed | Room-Temperature Micron-Scale Exciton Migration in a Stabilized Emissive Molecular Aggregate |
| title_short | Room-Temperature Micron-Scale Exciton Migration in a Stabilized Emissive Molecular Aggregate |
| title_sort | room temperature micron scale exciton migration in a stabilized emissive molecular aggregate |
| url | http://hdl.handle.net/1721.1/113346 https://orcid.org/0000-0003-1192-4746 https://orcid.org/0000-0002-2710-5545 https://orcid.org/0000-0002-9371-6109 https://orcid.org/0000-0003-2220-4365 https://orcid.org/0000-0002-6728-8163 |
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