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Triplet Transfer Mediates Triplet Pair Separation during Singlet Fission in 6,13‐Bis(triisopropylsilylethynyl)‐Pentacene
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2017-10-20 , DOI: 10.1002/adfm.201703929 Christopher Grieco 1 , Grayson S. Doucette 2, 3 , Jason M. Munro 3, 4 , Eric R. Kennehan 1 , Youngmin Lee 5 , Adam Rimshaw 1 , Marcia M. Payne 6 , Nichole Wonderling 4 , John E. Anthony 6 , Ismaila Dabo 3, 4 , Enrique D. Gomez 4, 5 , John B. Asbury 1, 2
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2017-10-20 , DOI: 10.1002/adfm.201703929 Christopher Grieco 1 , Grayson S. Doucette 2, 3 , Jason M. Munro 3, 4 , Eric R. Kennehan 1 , Youngmin Lee 5 , Adam Rimshaw 1 , Marcia M. Payne 6 , Nichole Wonderling 4 , John E. Anthony 6 , Ismaila Dabo 3, 4 , Enrique D. Gomez 4, 5 , John B. Asbury 1, 2
Affiliation
Triplet population dynamics of solution cast films of isolated polymorphs of 6,13‐bis(triisopropylsilylethynyl) pentacene (TIPS‐Pn) provide quantitative experimental evidence that triplet excitation energy transfer is the dominant mechanism for correlated triplet pair (CTP) separation during singlet fission. Variations in CTP separation rates are compared for polymorphs of TIPS‐Pn with their triplet diffusion characteristics that are controlled by their crystal structures. Since triplet energy transfer is a spin‐forbidden process requiring direct wavefunction overlap, simple calculations of electron and hole transfer integrals are used to predict how molecular packing arrangements would influence triplet transfer rates. The transfer integrals reveal how differences in the packing arrangements affect electronic interactions between pairs of TIPS‐Pn molecules, which are correlated with the relative rates of CTP separation in the polymorphs. These findings suggest that relatively simple computations in conjunction with measurements of molecular packing structures may be used as screening tools to predict a priori whether new types of singlet fission sensitizers have the potential to undergo fast separation of CTP states to form multiplied triplets.
中文翻译:
三重态转移在6,13-双(三异丙基甲硅烷基乙炔基)-并四烯的单重态裂变过程中介导三重态对的分离
6,13-双(三异丙基甲硅烷基乙炔基)并五苯(TIPS-Pn)多晶型物的溶液流延膜的三重态种群动力学提供了定量实验证据,表明三重态激发能转移是单重态裂变过程中相关三重态对(CTP)分离的主要机制。比较了TIPS-Pn的多晶型物的CTP分离速率的变化,其三重态扩散特性受其晶体结构控制。由于三重态能量转移是自旋禁止过程,需要直接的波函数重叠,因此,通过简单的电子和空穴转移积分计算可预测分子堆积结构将如何影响三重态转移速率。转移积分揭示了排列方式的差异如何影响成对的TIPS-Pn分子之间的电子相互作用,这与多晶型物中CTP分离的相对速率相关。这些发现表明,与分子堆积结构的测量相结合的相对简单的计算可以用作筛选工具,以先验地预测新型单线态裂变敏化剂是否具有快速经历CTP状态分离形成三重态的潜力。
更新日期:2017-10-20
中文翻译:
三重态转移在6,13-双(三异丙基甲硅烷基乙炔基)-并四烯的单重态裂变过程中介导三重态对的分离
6,13-双(三异丙基甲硅烷基乙炔基)并五苯(TIPS-Pn)多晶型物的溶液流延膜的三重态种群动力学提供了定量实验证据,表明三重态激发能转移是单重态裂变过程中相关三重态对(CTP)分离的主要机制。比较了TIPS-Pn的多晶型物的CTP分离速率的变化,其三重态扩散特性受其晶体结构控制。由于三重态能量转移是自旋禁止过程,需要直接的波函数重叠,因此,通过简单的电子和空穴转移积分计算可预测分子堆积结构将如何影响三重态转移速率。转移积分揭示了排列方式的差异如何影响成对的TIPS-Pn分子之间的电子相互作用,这与多晶型物中CTP分离的相对速率相关。这些发现表明,与分子堆积结构的测量相结合的相对简单的计算可以用作筛选工具,以先验地预测新型单线态裂变敏化剂是否具有快速经历CTP状态分离形成三重态的潜力。