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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Substituent Effects on Singlet Exciton Fission in Polycrystalline Thin Films of Cyano-Substituted Diaryltetracenes
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Substituent Effects on Singlet Exciton Fission in Polycrystalline Thin Films of Cyano-Substituted Diaryltetracenes

机译：氰基取代的二芳基二芳基晶薄膜单晶体激子裂变的取代基

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摘要

Cyano-substituted tetracenes (5,11-dicyano-6,12-diphenyltetracene, Tet) undergo exoergic singlet fission (SF), a spin-allowed photophysical process that generates a pair of triplet excitons from one singlet exciton. To elucidate substituent effects on SF, we have measured the SF dynamics and triplet yields of thin films, formed by Tet bearing hydrogen (H), methyl (Me), fluoro (F), and trimethylsilyl (TMS) substituents on the p-phenyl positions and on the 3 and 9 positions of the tetracene core, by time-resolved spectroscopy in the vis-NIR and IR regions. The H-, Me-, and F-Tet display strong intramolecular electronic coupling (pi-pi distances <4 angstrom), and SF gives high triplet exciton yields up to 200% (quantitative). In addition, a charge-transfer state mediates SF in F-Tet films, while H-Tet and Me-Tet show no evidence for such a state. Correlations between the SF yields and the crystal structure show that chromophore slippage along both their short and long axes allows efficient SF and that a large degree of pi contact between the chromophores is not necessary for rapid and efficient SF in the solid state. As expected, the large interchromophore distance in TMS-Tet (>4 angstrom) reduces its SF triplet yield to about 60%.
机译：氰基取代的四丙烯（5,11-二氰-6,12-二苯基核，TET）经历exoergic态裂缝（SF），旋转允许的光学药物方法，从一个单态激子产生一对三重态激子。为了阐明对SF的取代基效应，我们已经测量了通过TET含氢（H），甲基（ME），氟（F）和三甲基甲硅烷基（TMS）取代基在对苯基上形成的薄膜的SF动力学和三重态产量在Vis-nir和IR区域中通过时间分辨的光谱检查，四核的位置和3和9位。 H-，ME-和F-TET显示强的分子内电子耦合（PI-PI距离<4埃），SF提供高度三重态激子的产量，高达200％（定量）。此外，电荷转移状态在F-TET薄膜中介导SF，而H-Tet和Me-Tet则显示出这样的状态的证据。 SF产率和晶体结构之间的相关性表明，沿着它们的短轴和长轴的发色团滑动允许有效的SF，并且发色团之间的大程度的PI接触是在固态中快速高效的SF不需要的。如所预期的，TMS-TET（> 4埃）中的大型间运动距离降低了其SF三重态产率至约60％。

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