Dynamics of the triplet-pair state reveals the likely coexistence of coherent and incoherent singlet fission in crystalline hexacene

Nicholas R. Monahan, Dezheng Sun, Hiroyuki Tamura, Kristopher W. Williams, Bolei Xu, Yu Zhong, Bharat Kumar, Colin Nuckolls, Avetik R. Harutyunyan, Gugang Chen, Hai Lung Dai, David Beljonne, Yi Rao, X. Y. Zhu

    研究成果: Article査読

    104 被引用数 (Scopus)

    抄録

    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 S11(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.

    本文言語English
    ページ(範囲)341-346
    ページ数6
    ジャーナルNature Chemistry
    9
    4
    DOI
    出版ステータスPublished - 2017 4 1

    ASJC Scopus subject areas

    • 化学 (全般)
    • 化学工学(全般)

    フィンガープリント

    「Dynamics of the triplet-pair state reveals the likely coexistence of coherent and incoherent singlet fission in crystalline hexacene」の研究トピックを掘り下げます。これらがまとまってユニークなフィンガープリントを構成します。

    引用スタイル