期刊
NATURE CHEMISTRY
卷 9, 期 4, 页码 341-346出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.2665
关键词
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资金
- US Department of Energy [DE-SC0014563]
- US National Science Foundation [DMR 1321405]
- Honda Research Institute, USA
- Belgian National Fund for Scientific Research (FRS-FNRS)
- Invited Professor Fellowship, FNRS, Belgium
- U.S. Department of Energy (DOE) [DE-SC0014563] Funding Source: U.S. Department of Energy (DOE)
- Grants-in-Aid for Scientific Research [15K21719, 26105011, 26105001, 15K05374] Funding Source: KAKEN
The absorption of a photon usually creates a singlet exciton (S-1) in molecular systems, but in some cases S-1 may split into two triplets (2xT(1)) in a process called singlet fission. Singlet fission is believed to proceed through the correlated tripletpair (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 2xT(1) with a time constant of 270 fs. However, the decay of S-1 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 S-1 ->(1)(TT) rate process responsible for the 180 fs timescale, S-1 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.
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