Diradical Character View of Singlet Fission
Diradical Character View of Singlet Fission
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DOI：
10.1021/jz2015346
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发表时间：
2012-01-19
影响因子：
5.7
通讯作者：
Nakano, Masayoshi
中科院分区：
文献类型：
--
作者：
Minami, Takuya;Nakano, Masayoshi
给出了激发能差与单重态裂变的可行性条件，它们是多重双自由基特征y（i）[定义为LUNO（=最低轨道）+ i（i = 0，1，.）的函数，其中0 j）]使用线性H-4全构型相互作用模型。发现适合单重态裂变的双自由基特征位于y（0）> 0.10的区域，但y（0）与y（1）相似，而具有低/中双自由基特征的双自由基和多自由基化合物，如开壳层单重态多环芳烃，其能量效率在y（0）较小的情况下更好。这些发现表明，多重双自由基特征是探索有效单重态裂变的分子系统的有效指标。
The feasibility conditions of singlet fission on the excitation energy differences are revealed as functions of the multiple diradical characters y(i) [defined by the occupation numbers of the LUNO (= Lowest Unoccupied Natural Orbital) + i (i = 0, 1, ...), where 0 j)] using the linear H-4 full configuration interaction model. The diradical characters suited for singlet fission are found to lie in the region with y(0) > 0.10 except for y(0) similar to y(1), though its energy efficiency is better in case of smaller y(0), to which diradical and multiradical compounds with low/intermediate diradical characters such as open-shell singlet polycyclic aromatic hydrocarbons belong. These findings indicate that the multiple diradical character is an effective indicator for exploring Molecular systems for efficient singlet fission.