Kim Juno, Teo Hao Ting, Hong Yongseok, Oh Juwon, Kim Hyungjun, Chi Chunyan, Kim Dongho
Department of Chemistry, Spectroscopy Laboratory for Functional π-Electronic Systems, Yonsei University, 03722, Seoul, Korea.
Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore, Singapore.
Angew Chem Int Ed Engl. 2020 Nov 16;59(47):20956-20964. doi: 10.1002/anie.202008533. Epub 2020 Aug 20.
Singlet fission in organic semiconducting materials has attracted great attention for the potential application in photovoltaic devices. Research interests have been concentrated on identifying working mechanisms of coherent SF processes in crystalline solids as ultrafast SF is hailed for efficient multiexciton generation. However, as long lifetime of multiexcitonic triplet pair in amorphous solids facilitates the decorrelation process for triplet exciton extractions, a precise examination of incoherent SF processes is demanded in delicate model systems to represent heterogeneous structures. Heterogeneous coupling and energetics for SF were developed in our oligoacene dendrimers, which mimic complicated SF dynamics in amorphous solids. SF dynamics in dendritic structures was thoroughly investigated by time-resolved spectroscopic techniques and quantum chemical calculations in respect of the relative orientation/distance between chromophores and though-bond/-space interactions.
有机半导体材料中的单线态裂变因其在光伏器件中的潜在应用而备受关注。研究兴趣主要集中在确定晶体固体中相干单线态裂变过程的工作机制，因为超快单线态裂变被认为可实现高效的多激子产生。然而，由于非晶态固体中多激子三重态对的长寿命促进了三重态激子提取的去相关过程，因此需要在精细的模型系统中精确研究非相干单线态裂变过程，以表征异质结构。我们在寡并苯树枝状聚合物中开发了单线态裂变的异质耦合和能量学，该聚合物模拟了非晶态固体中复杂的单线态裂变动力学。通过时间分辨光谱技术和量子化学计算，从发色团之间的相对取向/距离以及通过键/空间相互作用方面，对树枝状结构中的单线态裂变动力学进行了深入研究。
