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轨道分辨的单态裂变观测。

Orbital-resolved observation of singlet fission.

机构信息

Department of Physical Chemistry, Fritz Haber Institute of the Max Planck Society, Berlin, Germany.

CELIA, University of Bordeaux-CNRS-CEA, Bordeaux, France.

出版信息

Nature. 2023 Apr;616(7956):275-279. doi: 10.1038/s41586-023-05814-1. Epub 2023 Apr 12.

DOI:10.1038/s41586-023-05814-1
PMID:37045918
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10097594/
Abstract

Singlet fission may boost photovoltaic efficiency by transforming a singlet exciton into two triplet excitons and thereby doubling the number of excited charge carriers. The primary step of singlet fission is the ultrafast creation of the correlated triplet pair. Whereas several mechanisms have been proposed to explain this step, none has emerged as a consensus. The challenge lies in tracking the transient excitonic states. Here we use time- and angle-resolved photoemission spectroscopy to observe the primary step of singlet fission in crystalline pentacene. Our results indicate a charge-transfer mediated mechanism with a hybridization of Frenkel and charge-transfer states in the lowest bright singlet exciton. We gained intimate knowledge about the localization and the orbital character of the exciton wave functions recorded in momentum maps. This allowed us to directly compare the localization of singlet and bitriplet excitons and decompose energetically overlapping states on the basis of their orbital character. Orbital- and localization-resolved many-body dynamics promise deep insights into the mechanics governing molecular systems and topological materials.

摘要

单重态裂变可以通过将单重态激子转化为两个三重态激子来提高光伏效率，从而使激发电荷载流子的数量增加一倍。单重态裂变的主要步骤是超快地产生关联的三重态对。尽管已经提出了几种机制来解释这一步骤，但没有一种机制成为共识。挑战在于跟踪瞬态激子态。在这里，我们使用时间和角度分辨光电子能谱来观察晶体戊烯中单重态裂变的主要步骤。我们的结果表明，在最低亮单重激子中，存在电荷转移介导的机制，其中存在 Frenkel 和电荷转移态的杂化。我们深入了解了动量图谱中记录的激子波函数的局域化和轨道特征。这使我们能够直接比较单重态和双三重态激子的局域化，并根据轨道特征对能量重叠态进行分解。轨道和局域分辨的多体动力学有望深入了解控制分子系统和拓扑材料的力学。

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