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Soluble Diphenylhexatriene Dimers for Intramolecular Singlet Fission with High Triplet Energy
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-01-22 , DOI: 10.1021/jacs.2c12060 Oliver Millington 1, 2 , Stephanie Montanaro 1 , Anastasia Leventis 1 , Ashish Sharma 2 , Simon A Dowland 2 , Nipun Sawhney 2 , Kealan J Fallon 1, 2 , Weixuan Zeng 1 , Daniel G Congrave 1 , Andrew J Musser 3 , Akshay Rao 2 , Hugo Bronstein 1, 2
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-01-22 , DOI: 10.1021/jacs.2c12060 Oliver Millington 1, 2 , Stephanie Montanaro 1 , Anastasia Leventis 1 , Ashish Sharma 2 , Simon A Dowland 2 , Nipun Sawhney 2 , Kealan J Fallon 1, 2 , Weixuan Zeng 1 , Daniel G Congrave 1 , Andrew J Musser 3 , Akshay Rao 2 , Hugo Bronstein 1, 2
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Intramolecular singlet fission (iSF) facilitates single-molecule exciton multiplication, converting an excited singlet state to a pair of triplet states within a single molecule. A critical parameter in determining the feasibility of SF-enhanced photovoltaic designs is the triplet energy; many existing iSF materials have triplet energies too low for efficient transfer to silicon via a photon multiplier scheme. In this work, a series of six novel dimers based upon the high-triplet-energy, SF-active chromophore, 1,6-diphenyl-1,3,5-hexatriene (DPH) [E(T1) ∼ 1.5 eV], were designed, synthesized, and characterized. Transient absorption spectroscopy and fluorescence lifetime studies reveal that five of the dimers display iSF activity, with time constants for singlet fission varying between 7 ± 2 ps and 2.2 ± 0.2 ns and a high triplet yield of 163 ± 63% in the best-performing dimer. A strong dependence of the rate of fission on the coupling geometry is demonstrated. For optimized iSF behavior, close spatial proximity and minimal through-bond communication are found to be crucial for balancing the rate of SF against the reverse recombination process.
中文翻译：
可溶性二苯基六三烯二聚体用于具有高三线态能量的分子内单线态裂变
分子内单线态裂变 (iSF) 促进单分子激子倍增，将单个分子内的激发单线态转换为一对三线态。确定SF增强型光伏设计可行性的一个关键参数是三线态能量；许多现有的 iSF 材料的三线态能量太低，无法通过光子倍增器方案有效转移到硅。在这项工作中，一系列基于高三线态能量、SF 活性发色团 1,6-二苯基-1,3,5-己三烯 (DPH) [ E (T 1 ) ∼ 1.5 eV] 的新型二聚体，进行了设计、合成和表征。瞬态吸收光谱和荧光寿命研究表明，其中五个二聚体表现出 iSF 活性，单线裂变的时间常数在 7 ± 2 ps 和 2.2 ± 0.2 ns 之间变化，并且性能最佳的二聚体的三线态产率为 163 ± 63% 。证明了裂变速率对耦合几何形状的强烈依赖性。对于优化的 iSF 行为，紧密的空间接近性和最小的键合通信被发现对于平衡 SF 速率与反向重组过程至关重要。
更新日期：2023-01-22
中文翻译：
可溶性二苯基六三烯二聚体用于具有高三线态能量的分子内单线态裂变
分子内单线态裂变 (iSF) 促进单分子激子倍增，将单个分子内的激发单线态转换为一对三线态。确定SF增强型光伏设计可行性的一个关键参数是三线态能量；许多现有的 iSF 材料的三线态能量太低，无法通过光子倍增器方案有效转移到硅。在这项工作中，一系列基于高三线态能量、SF 活性发色团 1,6-二苯基-1,3,5-己三烯 (DPH) [ E (T 1 ) ∼ 1.5 eV] 的新型二聚体，进行了设计、合成和表征。瞬态吸收光谱和荧光寿命研究表明，其中五个二聚体表现出 iSF 活性，单线裂变的时间常数在 7 ± 2 ps 和 2.2 ± 0.2 ns 之间变化，并且性能最佳的二聚体的三线态产率为 163 ± 63% 。证明了裂变速率对耦合几何形状的强烈依赖性。对于优化的 iSF 行为，紧密的空间接近性和最小的键合通信被发现对于平衡 SF 速率与反向重组过程至关重要。
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