Dynamics of the triplet-pair state reveals the likely coexistence of coherent and incoherent singlet fission in crystalline hexacene
書誌事項
- 公開日
- 2016-12-05
- 資源種別
- journal article
- 権利情報
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- http://www.springer.com/tdm
- DOI
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- 10.1038/nchem.2665
- 公開者
- Springer Science and Business Media LLC
この論文をさがす
説明
The absorption of a photon usually creates a singlet exciton (S1) in molecular systems, but in some cases S1 may split into two triplets (2×T1) in a process called singlet fission. Singlet fission is believed to proceed through the correlated triplet-pair 1(TT) state. Here, we probe the 1(TT) state in crystalline hexacene using time-resolved photoemission and transient absorption spectroscopies. We find a distinctive 1(TT) state, which decays to 2×T1 with a time constant of 270 fs. However, the decay of S1 and the formation of 1(TT) occur on different timescales of 180 fs and <50 fs, respectively. Theoretical analysis suggests that, in addition to an incoherent S1→1(TT) rate process responsible for the 180 fs timescale, S1 may couple coherently to a vibronically excited 1(TT) on ultrafast timescales (<50 fs). The coexistence of coherent and incoherent singlet fission may also reconcile different experimental observations in other acenes.
収録刊行物
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- Nature Chemistry
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Nature Chemistry 9 (4), 341-346, 2016-12-05
Springer Science and Business Media LLC