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首页> 外文期刊>Journal of the American Chemical Society >Large Second-Order Optical Nonlinearities in Open-Shell Chromophores. Planar Metal Complexes and Organic Radical Ion Aggregates
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Large Second-Order Optical Nonlinearities in Open-Shell Chromophores. Planar Metal Complexes and Organic Radical Ion Aggregates

机译：开壳发色团中的大二阶光学非线性。平面金属络合物和有机自由基离子聚集体

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摘要

Attempts to discover molecular chromophores with large hyperpolarizabilities have largely focused on closed-shell organic species. This contribution explores the use of sum over states (SOS) perturbation theory and the computationally efficient intermediate neglect of differential overlap (INDO) model Hamiltonian, combined with single configuration interaction (SCI) techniques, to calculate frequency-dependent quadratic molecular hyperpolarizabilities of both coordination complexes and organic radical ion chromophore aggregates having open-shell doublet ground state electronic structures. The correct evaluation of the lowest-lying excited states has been tested by comparison with experimental optical spectra. In the cases considered here, the INDO/SCI-SOS method provides both a good description of linear optical transitions and an adequate prediction of second-order nonlinearity. It is seen that the larger secondrorder nonlinearities of systems having open-shell electronic states, as compared to those having analogous closed-shell structures, are a consequence of accessible lower-lying charge-transfer excited electronic states. The INDO/SCI-SOS model is attractive for designing new, highly efficient open-shell second-order nonlinear optical chromophores.
机译：发现具有大超极化能力的分子发色团的尝试主要集中在封闭壳有机物种上。这项贡献探索了状态总和（SOS）扰动理论的使用和差分重叠（INDO）模型哈密顿量的高效计算中性忽略，结合单配置相互作用（SCI）技术，计算了两个配位的频率相关的二次分子超极化率配合物和有机自由基离子发色团聚集体，具有开壳双峰基态电子结构。通过与实验光谱比较，测试了对最低激发态的正确评估。在这里考虑的情况下，INDO / SCI-SOS方法既可以很好地描述线性光学跃迁，又可以提供对二阶非线性的充分预测。可以看出，与具有类似的闭壳结构的系统相比，具有开壳电子状态的系统具有更大的二阶非线性，是可接近的低层电荷转移激发电子状态的结果。 INDO / SCI-SOS模型对于设计新型高效的开壳二阶非线性光学生色团很有吸引力。

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