Anisotropic Singlet Fission in Single Crystalline Hexacene
Summary: Singlet fission is known to improve solar energy utilization by circumventing the Shockley-Queisser limit. The two essential steps of singlet fission are the formation of a correlated triplet pair and its subsequent quantum decoherence. However, the mechanisms of the triplet pair formation...
| Main Authors: | , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Elsevier
2019-09-01
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| Series: | iScience |
| Online Access: | http://www.sciencedirect.com/science/article/pii/S2589004219303323 |
| _version_ | 1818152346299924480 |
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| author | Dezheng Sun Gang-Hua Deng Bolei Xu Enshi Xu Xia Li Yajing Wu Yuqin Qian Yu Zhong Colin Nuckolls Avetik R. Harutyunyan Hai-Lung Dai Gugang Chen Hanning Chen Yi Rao |
| author_facet | Dezheng Sun Gang-Hua Deng Bolei Xu Enshi Xu Xia Li Yajing Wu Yuqin Qian Yu Zhong Colin Nuckolls Avetik R. Harutyunyan Hai-Lung Dai Gugang Chen Hanning Chen Yi Rao |
| author_sort | Dezheng Sun |
| collection | DOAJ |
| description | Summary: Singlet fission is known to improve solar energy utilization by circumventing the Shockley-Queisser limit. The two essential steps of singlet fission are the formation of a correlated triplet pair and its subsequent quantum decoherence. However, the mechanisms of the triplet pair formation and decoherence still remain elusive. Here we examined both essential steps in single crystalline hexacene and discovered remarkable anisotropy of the overall singlet fission rate along different crystal axes. Since the triplet pair formation emerges on the same timescale along both crystal axes, the quantum decoherence is likely responsible for the directional anisotropy. The distinct quantum decoherence rates are ascribed to the notable difference on their associated energy loss according to the Redfield quantum dissipation theory. Our hybrid experimental/theoretical framework will not only further our understanding of singlet fission, but also shed light on the systematic design of new materials for the third-generation solar cells. : Spectroscopy; Theoretical Photophysics; Quantum Phenomena Subject Areas: Spectroscopy, Theoretical Photophysics, Quantum Phenomena |
| first_indexed | 2024-12-11T13:53:15Z |
| format | Article |
| id | doaj.art-69d0db3f0d764bd8bd4bb65dfaed2a59 |
| institution | Directory Open Access Journal |
| issn | 2589-0042 |
| language | English |
| last_indexed | 2024-12-11T13:53:15Z |
| publishDate | 2019-09-01 |
| publisher | Elsevier |
| record_format | Article |
| series | iScience |
| spelling | doaj.art-69d0db3f0d764bd8bd4bb65dfaed2a592022-12-22T01:04:11ZengElsevieriScience2589-00422019-09-011910791089Anisotropic Singlet Fission in Single Crystalline HexaceneDezheng Sun0Gang-Hua Deng1Bolei Xu2Enshi Xu3Xia Li4Yajing Wu5Yuqin Qian6Yu Zhong7Colin Nuckolls8Avetik R. Harutyunyan9Hai-Lung Dai10Gugang Chen11Hanning Chen12Yi Rao13Department of Physics, Columbia University, New York, NY 10027, USADepartment of Chemistry and Biochemistry, Utah State University, Logan, UT 84322, USADepartment of Chemistry, Temple University, Philadelphia, PA 19122, USADepartment of Chemistry, George Washington University, Washington, DC 20052, USADepartment of Chemistry and Biochemistry, Utah State University, Logan, UT 84322, USADepartment of Chemistry, Temple University, Philadelphia, PA 19122, USADepartment of Chemistry and Biochemistry, Utah State University, Logan, UT 84322, USADepartment of Chemistry, Columbia University, New York, NY 10027, USADepartment of Chemistry, Columbia University, New York, NY 10027, USAHonda Research Institute USA, Inc., San Jose, CA 95134, USADepartment of Chemistry, Temple University, Philadelphia, PA 19122, USAHonda Research Institute USA, Inc., San Jose, CA 95134, USA; Corresponding authorDepartment of Chemistry, George Washington University, Washington, DC 20052, USA; Corresponding authorDepartment of Chemistry and Biochemistry, Utah State University, Logan, UT 84322, USA; Corresponding authorSummary: Singlet fission is known to improve solar energy utilization by circumventing the Shockley-Queisser limit. The two essential steps of singlet fission are the formation of a correlated triplet pair and its subsequent quantum decoherence. However, the mechanisms of the triplet pair formation and decoherence still remain elusive. Here we examined both essential steps in single crystalline hexacene and discovered remarkable anisotropy of the overall singlet fission rate along different crystal axes. Since the triplet pair formation emerges on the same timescale along both crystal axes, the quantum decoherence is likely responsible for the directional anisotropy. The distinct quantum decoherence rates are ascribed to the notable difference on their associated energy loss according to the Redfield quantum dissipation theory. Our hybrid experimental/theoretical framework will not only further our understanding of singlet fission, but also shed light on the systematic design of new materials for the third-generation solar cells. : Spectroscopy; Theoretical Photophysics; Quantum Phenomena Subject Areas: Spectroscopy, Theoretical Photophysics, Quantum Phenomenahttp://www.sciencedirect.com/science/article/pii/S2589004219303323 |
| spellingShingle | Dezheng Sun Gang-Hua Deng Bolei Xu Enshi Xu Xia Li Yajing Wu Yuqin Qian Yu Zhong Colin Nuckolls Avetik R. Harutyunyan Hai-Lung Dai Gugang Chen Hanning Chen Yi Rao Anisotropic Singlet Fission in Single Crystalline Hexacene iScience |
| title | Anisotropic Singlet Fission in Single Crystalline Hexacene |
| title_full | Anisotropic Singlet Fission in Single Crystalline Hexacene |
| title_fullStr | Anisotropic Singlet Fission in Single Crystalline Hexacene |
| title_full_unstemmed | Anisotropic Singlet Fission in Single Crystalline Hexacene |
| title_short | Anisotropic Singlet Fission in Single Crystalline Hexacene |
| title_sort | anisotropic singlet fission in single crystalline hexacene |
| url | http://www.sciencedirect.com/science/article/pii/S2589004219303323 |
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