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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Predicting the Frequency Dispersion of Electronic Hyperpolarizabilities on the Basis of Absorption Data and Thomas-Kuhn Sum Rules
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Predicting the Frequency Dispersion of Electronic Hyperpolarizabilities on the Basis of Absorption Data and Thomas-Kuhn Sum Rules

机译：基于吸收数据和Thomas-Kuhn Sum规则预测电子超极化的频率色散

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摘要

Successfully predicting the frequency dispersion of electronic hyperpolarizabilities is an unresolved challenge in materials science and electronic structure theory. We show that the generalized Thomas-Kuhn sum rules, combined with linear absorption data and measured hyperpolarizability at one or two frequencies, may be used to predict the entire frequency-dependent electronic hyperpolarizability spectrum. This treatment includes two- and three-level contributions that arise from the lowest two or three excited electronic, state manifolds, enabling us to describe the unusual observed frequency dispersion of the dynamic hyperpolarizability in high oscillator strength M-PZn chromophores, where (porphinato)zinc(II) (PZn) and metal(II)polypyridyl (M) units are connected via an ethyne unit that aligns the high oscillator strength transition dipoles of these components in a head-to-tail arrangement. We show that some of these structures can possess very similar linear absorption spectra yet manifest dramatically different frequency-dependent hyperpolarizabilities, because of three-level contributions that result from excited state-to-excited state transition dipoles among charge polarized states. Importantly, this approach provides a quantitative scheme to use linear optical absorption spectra and very limited individual hyperpolarizability measurements to predict the entire frequency-dependent nonlinear optical response.
机译：成功预测电子超极化率的频率色散是材料科学和电子结构理论中尚未解决的挑战。我们表明，广义的Thomas-Kuhn总和规则，结合线性吸收数据和在一个或两个频率上测得的超极化率，可用于预测整个频率相关的电子超极化率谱。这种处理包括由最低的两个或三个受激电子状态流形产生的两级和三级贡献，使我们能够描述在高振荡器强度M-PZn发色团中动态超极化的异常观察到的频散，其中（porphinato）锌（II）（PZn）和金属（II）聚吡啶（M）单元通过乙炔单元连接，该乙炔单元以头到尾的方式对齐这些组件的高振荡器强度跃迁偶极子。我们表明，由于电荷极化态之间从激发态到激发态跃迁偶极子的三能级贡献，这些结构中的某些可以具有非常相似的线性吸收光谱，但表现出明显不同的频率依赖性超极化率。重要的是，这种方法提供了使用线性光学吸收光谱和非常有限的单个超极化率测量值来预测整个与频率相关的非线性光学响应的​​定量方案。

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