Transport of Spin-Entangled Triplet Excitons Generated by Singlet Fission,The Journal of Physical Chemistry Letters

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Transport of Spin-Entangled Triplet Excitons Generated by Singlet Fission
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2018-11-07 00:00:00 , DOI: 10.1021/acs.jpclett.8b02944
Yan Wan _{1,

2} , Gary P. Wiederrecht ₃ , Richard D. Schaller _{3,

4} , Justin C. Johnson ₅ , Libai Huang ₂

Affiliation

Singlet fission provides a promising route for overcoming the Shockley–Queisser limit in solar cells using organic materials. Despite singlet fission dynamics having been extensively investigated, the transport of the various intermediates in relation to the singlet and triplet states is largely unknown. Here we employ temperature-dependent ultrafast transient absorption microscopy to image the transport of singlet fission intermediates in single crystals of tetracene. These measurements suggest a mobile singlet fission intermediate state at low temperatures, with a diffusion constant of 36 cm²s^–1 at 5 K, approaching that for the free singlet excitons, which we attribute to the spin-entangled correlated triplet pair state ¹[TT]. These results indicate that ¹[TT] could transport with a similar mechanism as the bright singlet excitons, which has important implications in designing materials for singlet fission and spintronic applications.

中文翻译：

单重态裂变产生的自旋纠缠三重态激子的输运

单线态裂变为克服使用有机材料的太阳能电池中的Shockley–Queisser限制提供了一条有希望的途径。尽管已经对单线态裂变动力学进行了广泛研究，但关于单线态和三线态的各种中间产物的传输仍是未知的。在这里，我们采用依赖温度的超快速瞬态吸收显微镜来成像并四苯单晶中单重态裂变中间体的传输。这些测量结果表明，在低温下，移动单线态裂变处于中间态，在5 K下的扩散常数为36 cm ² s ^–1，接近于自由单线态激子的扩散常数，我们将其归因于自旋纠缠的相关三重态对态¹ [ TT]。这些结果表明¹ [TT]可以通过与明亮单重态激子相似的机理进行传输，这对于设计用于单重态裂变和自旋电子学应用的材料具有重要意义。

更新日期：2018-11-07

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