How two-dimensional brick layer J-aggregates differ from linear ones: Excitonic properties and line broadening mechanisms
We study the excitonic coupling and homogeneous spectral line width of brick layer J-aggregate films. We begin by analysing the structural information revealed by the two-exciton states probed in two-dimensional spectra. Our first main result is that the relation between the excitonic couplings and...
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| Format: | Article |
| Language: | en_US |
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American Institute of Physics (AIP)
2017
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| Online Access: | http://hdl.handle.net/1721.1/110490 https://orcid.org/0000-0001-7804-5418 https://orcid.org/0000-0001-7616-7809 |
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| author | Duan, Hong-Guang Knoester, Jasper Dijkstra, Arend Gerrit Nelson, Keith Adam Cao, Jianshu |
| author2 | Massachusetts Institute of Technology. Department of Chemistry |
| author_facet | Massachusetts Institute of Technology. Department of Chemistry Duan, Hong-Guang Knoester, Jasper Dijkstra, Arend Gerrit Nelson, Keith Adam Cao, Jianshu |
| author_sort | Duan, Hong-Guang |
| collection | MIT |
| description | We study the excitonic coupling and homogeneous spectral line width of brick layer J-aggregate films. We begin by analysing the structural information revealed by the two-exciton states probed in two-dimensional spectra. Our first main result is that the relation between the excitonic couplings and the spectral shift in a two-dimensional structure is different (larger shift for the same nearest neighbour coupling) from that in a one-dimensional structure, which leads to an estimation of dipolar coupling in two-dimensional lattices. We next investigate the mechanisms of homogeneous broadening—population relaxation and pure dephasing—and evaluate their relative importance in linear and two-dimensional aggregates. Our second main result is that pure dephasing dominates the line width in two-dimensional systems up to a crossover temperature, which explains the linear temperature dependence of the homogeneous line width. This is directly related to the decreased density of states at the band edge when compared with linear aggregates, thus reducing the contribution of population relaxation to dephasing. Pump-probe experiments are suggested to directly measure the lifetime of the bright state and can therefore support the proposed model. |
| first_indexed | 2024-09-23T13:34:54Z |
| format | Article |
| id | mit-1721.1/110490 |
| institution | Massachusetts Institute of Technology |
| language | en_US |
| last_indexed | 2024-09-23T13:34:54Z |
| publishDate | 2017 |
| publisher | American Institute of Physics (AIP) |
| record_format | dspace |
| spelling | mit-1721.1/1104902022-10-01T15:50:53Z How two-dimensional brick layer J-aggregates differ from linear ones: Excitonic properties and line broadening mechanisms Duan, Hong-Guang Knoester, Jasper Dijkstra, Arend Gerrit Nelson, Keith Adam Cao, Jianshu Massachusetts Institute of Technology. Department of Chemistry Dijkstra, Arend Gerrit Nelson, Keith Adam Cao, Jianshu We study the excitonic coupling and homogeneous spectral line width of brick layer J-aggregate films. We begin by analysing the structural information revealed by the two-exciton states probed in two-dimensional spectra. Our first main result is that the relation between the excitonic couplings and the spectral shift in a two-dimensional structure is different (larger shift for the same nearest neighbour coupling) from that in a one-dimensional structure, which leads to an estimation of dipolar coupling in two-dimensional lattices. We next investigate the mechanisms of homogeneous broadening—population relaxation and pure dephasing—and evaluate their relative importance in linear and two-dimensional aggregates. Our second main result is that pure dephasing dominates the line width in two-dimensional systems up to a crossover temperature, which explains the linear temperature dependence of the homogeneous line width. This is directly related to the decreased density of states at the band edge when compared with linear aggregates, thus reducing the contribution of population relaxation to dephasing. Pump-probe experiments are suggested to directly measure the lifetime of the bright state and can therefore support the proposed model. United States. Dept. of Energy. Center for Excitonics (Award DE-SC0001088) National Science Foundation (U.S.) (Grant CHE-1112825) 2017-07-06T15:33:09Z 2017-07-06T15:33:09Z 2016-04 2015-09 Article http://purl.org/eprint/type/JournalArticle 0021-9606 1089-7690 http://hdl.handle.net/1721.1/110490 Dijkstra, Arend G. et al. “How Two-Dimensional Brick Layer J-Aggregates Differ from Linear Ones: Excitonic Properties and Line Broadening Mechanisms.” The Journal of Chemical Physics 144.13 (2016): 134310. © 2016 AIP Publishing https://orcid.org/0000-0001-7804-5418 https://orcid.org/0000-0001-7616-7809 en_US http://dx.doi.org/10.1063/1.4944980 The Journal of Chemical Physics 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 Institute of Physics (AIP) MIT web domain |
| spellingShingle | Duan, Hong-Guang Knoester, Jasper Dijkstra, Arend Gerrit Nelson, Keith Adam Cao, Jianshu How two-dimensional brick layer J-aggregates differ from linear ones: Excitonic properties and line broadening mechanisms |
| title | How two-dimensional brick layer J-aggregates differ from linear ones: Excitonic properties and line broadening mechanisms |
| title_full | How two-dimensional brick layer J-aggregates differ from linear ones: Excitonic properties and line broadening mechanisms |
| title_fullStr | How two-dimensional brick layer J-aggregates differ from linear ones: Excitonic properties and line broadening mechanisms |
| title_full_unstemmed | How two-dimensional brick layer J-aggregates differ from linear ones: Excitonic properties and line broadening mechanisms |
| title_short | How two-dimensional brick layer J-aggregates differ from linear ones: Excitonic properties and line broadening mechanisms |
| title_sort | how two dimensional brick layer j aggregates differ from linear ones excitonic properties and line broadening mechanisms |
| url | http://hdl.handle.net/1721.1/110490 https://orcid.org/0000-0001-7804-5418 https://orcid.org/0000-0001-7616-7809 |
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