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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Theoretical Engineering of Singlet Fission Kinetics in Perylene Bisimide Dimer with Chromophore Rotation
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Theoretical Engineering of Singlet Fission Kinetics in Perylene Bisimide Dimer with Chromophore Rotation

机译：发色团旋转的Pernene Bisimide二聚体中单裂变动力学的理论工程

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摘要

We investigated the potential of chromophore’s rotations to tune singlet fission (SF) kinetics in perylene bisimide (PBI) dimers in addition to relative horizontal displacements. The total number of 250 PBI dimers (five displacements along the long and short axis of PBI, respectively, and ten rotation angle changes from parallel to perpendicular alignment) was examined. Ground-state energies showed that dimer formation is favored in all orientations with some differences in interaction strength. Time-dependent density functional theory predicted S_(1) and T_(1) excitons’ energy, and the thermodynamic feasibility of SF process was judged by the energy difference between a S_(1) exciton and twice of T_(1) excitons. In addition, we also estimated the relative rate of multiexciton generation step by the three-state kinetic model with the results of restricted active space employing double spin-flip. Nine promising orientations including two parallel PBI dimers and seven twisted ones were discussed. Wave function composition analysis showed that SF occurs mainly through the superexchange mechanism in various twisted PBI dimers, but the direct two-electron and coherent pathway could be operative at the particular positions. Quantum chemical simulations suggested the rotation as an effective tool to tune SF efficiency in PBI dimers, which is helpful to substantiate more efficient SF material.
机译：除相对水平位移外，我们还研究了生色团旋转对苝-双酰亚胺（PBI）二聚体中单线态裂变（SF）动力学的调节作用。检测了250个PBI二聚体的总数（分别沿PBI长轴和短轴的五个位移，以及十个从平行到垂直排列的旋转角度变化）。基态能量表明，在所有方向上都有利于二聚体的形成，但相互作用强度有所不同。含时密度泛函理论预测了S_1和T_1激子的能量，并通过S_1激子和两个T_1激子的能量差来判断SF过程的热力学可行性。此外，我们还利用三态动力学模型估计了多激子产生的相对速率，并利用双自旋翻转的有限活动空间结果进行了计算。讨论了九种有希望的取向，包括两个平行的PBI二聚体和七个扭曲的PBI二聚体。波函数组成分析表明，SF主要通过各种扭曲的PBI二聚体中的超交换机制发生，但在特定位置，直接双电子相干路径可能起作用。量子化学模拟表明，旋转是调节PBI二聚体中SF效率的有效工具，这有助于证实更有效的SF材料。

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