Quantitative Sequential Photoenergy Conversion Process from Singlet Fission to Intermolecular Two-Electron Transfers Utilizing Tetracene Dimer,ACS Energy Letters

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Quantitative Sequential Photoenergy Conversion Process from Singlet Fission to Intermolecular Two-Electron Transfers Utilizing Tetracene Dimer
ACS Energy Letters ( IF 19.3 ) Pub Date : 2018-11-20 00:00:00 , DOI: 10.1021/acsenergylett.8b01964
Shunta Nakamura ₁ , Hayato Sakai ₁ , Hiroki Nagashima ₂ , Yasuhiro Kobori _{2,

3} , Nikolai V. Tkachenko ₄ , Taku Hasobe ₁

Affiliation

Singlet fission (SF) theoretically enables the performance of the sequential photoenergy conversion process starting from the singlet state and leading to electron transfer (ET) with the radical ion pair quantum yield approaching 200%. Additionally, the long lifetime of the triplet state opens the possibility for an intermolecular ET process in a diffusion-limited reaction. However, the quantitative two-electron transfer process through SF has yet to be reported. Herein we demonstrate the quantitative sequential process involving SF and leading to intermolecular two-electron transfers using 2,2′-biphenyl-bridged tetracene dimer (Tet-BP-Tet: SF and electron donor) and chloranil (Ch: electron acceptor). The high-yield and long-lived individual triplet excited states of Tet-BP-Tet by SF (Φ_T = 175 ± 5% and τ_T = 0.29 ms) resulted in the quantitative two-electron transfer process (Φ_ET = 173 ± 5%) with Ch in benzonitrile.

中文翻译：

从四重态裂变到分子间两电子转移的四序定量光能转化过程，利用四烯二聚体

从理论上讲，单峰裂变（SF）使顺序光能转换过程的性能得以实现，从单峰态开始并导致电子转移（ET），自由基离子对的量子产率接近200％。另外，三重态的长寿命为扩散受限的反应提供了分子间ET过程的可能性。然而，尚未报道过通过SF进行的定量双电子转移过程。在本文中，我们证明了涉及SF并导致分子间两电子转移的定量顺序过程，使用2,2'-联苯桥联的并四苯二聚体（Tet-BP-Tet：SF和电子供体）和邻苯二甲腈（Ch：电子受体）。由SF（Φ高收率和长寿命的个体三重激发态的Tet-BP-四环素的_Ť = 175±5％和τ_Ť = 0.29毫秒）得到定量双电子转移过程（Φ _ET与CH IN苄腈= 173±5％）。

更新日期：2018-11-20

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