并四苯晶体中单重态fission产生的关联三重态之间的磁偶极相互作用
Magnetic dipolar interaction between correlated triplets created by singlet fission in tetracene crystals
摘要：
单重态裂变（SF）可以通过将有机半导体中的一个光激发的单重态激子（S1）分裂成两个三重态（2 T1）来潜在地打破单结太阳能电池中的肖克利-奎塞尔效率极限。暗多激子（ME）态已经被提出作为连接S1到2 T1的中间体。然而，这种ME状态的确切性质，特别是双激发三胞胎如何相互作用，仍然难以捉摸。在这里，我们报告了一个定量研究SF诱导的相关三重态在并四苯晶体中的磁偶极相互作用，通过监测量子拍相关的ME子能级在室温下。观察到通过调谐外部磁场而接近的ME子能级的共振被避免，这与考虑~ 0.008 GHz的磁偶极相互作用的理论预测一致。我们的工作为量化有机材料中的磁偶极相互作用铺平了道路，并标志着朝着理解ME状态的基础物理学迈出了重要一步。
英文摘要：
Singlet fission (SF) can potentially break the Shockley-Queisser efficiency limit in single-junction solar cells by splitting one photo-excited singlet exciton (S1) into two triplets (2T1) in organic semiconductors. A dark multi-exciton (ME) state has been proposed as the intermediate connecting S1 to 2T1. However, the exact nature of this ME state, especially how the doubly-excited triplets interact, remains elusive. Here, we report a quantitative study on the magnetic dipolar interaction between SF-induced correlated triplets in tetracene crystals by monitoring quantum beats relevant to the ME sublevels at room temperature. The resonances of ME sublevels approached by tuning an external magnetic field are observed to be avoided, which agrees well with the theoretical predictions considering a magnetic dipolar interaction of ~ 0.008 GHz. Our work paves a way to quantify the magnetic dipolar interaction in organic materials and marks an important step towards understanding the underlying physics of the ME state.
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