论文标题
五重奏形成和交换波动:随机共振在单线裂变中的作用
Quintet formation and exchange fluctuations: The role of stochastic resonance in singlet fission
论文作者
论文摘要
Singlet Pission描述了一个Singlet Icciton的两种三胞胎激子的自旋产生。在文献中已经建立了Spin-2(五重奏)三重态作为单线裂变产物的存在,而对五重奏组的控制是将单线裂变应用于光伏和量子信息的重要一步。但是,尚未建立五重奏形成的确定机制,这使得很难设计材料以进行最佳的五重奏形成。在这里,我们概述了一种机制,其中三个间距交换耦合波动驱动快速有效的五重奏组形成。与传统的观点相反,我们表明,尽管交换耦合,五重奏人口仍可能出现。我们在两个构象自由度中评估了这种五重奏形成机制的性能,并将五重能动态与单线裂变分子的材料特性相关联。
Singlet fission describes the spin-conserving production of two triplet excitons from one singlet exciton. The existence of a spin-2 (quintet) triplet-pair state as a product of singlet fission is well established in the literature, and control of quintet formation is an important step towards applying singlet fission in photovoltaics and quantum information. However, a definitive mechanism for quintet formation is yet to be established, which makes it difficult to design materials for optimal quintet formation. Here we outline a mechanism in which inter-triplet exchange coupling fluctuations drive fast and efficient quintet formation. In contrast with conventional wisdom, we show that quintet population can arise despite strong exchange coupling. We evaluate the performance of this quintet formation mechanism in two regimes of conformational freedom, and relate quintet dynamics to material properties of singlet fission molecules.