Molecular Simulations and Design Group , Max Planck Institute for Dynamics of Complex Technical Systems , Sandtorstrasse 1 , 39106 Magdeburg , Germany.
Chemistry Department , Pohang University of Science and Technology , Namgu, Pohang 790-784 , Korea.
J Phys Chem A. 2019 Oct 31;123(43):9321-9327. doi: 10.1021/acs.jpca.9b05039. Epub 2019 Oct 21.
This work demonstrates the feasibility and applicability of the theory of extended multiphonon electron transitions for the description of nonlinear optical properties of polymethine dyes using quantum chemistry and model calculations. The transformation of a strong one-photon absorption band in dye monomers to a weak two-photon absorption band is rationalized from the electron-nuclear resonance condition. The power law fitting of the results of quantum chemical computations of nonlinear optical properties allows the predicting of the shift of the corresponding Egorov-like resonance curve to the shortest dye in the vinylogous series of dye monomers. The results presented provide an insight and guide for the rational molecular design and application of polymethine dyes.
本工作通过量子化学和模型计算，证明了扩展多声子电子跃迁理论用于描述聚甲川染料非线性光学性质的可行性和适用性。从电子-核共振条件出发，将染料单体中强的单光子吸收带转化为弱的双光子吸收带。非线性光学性质的量子化学计算结果的幂律拟合允许预测相应的 Egorov 类共振曲线在乙烯基取代的染料单体系列中最短染料上的位移。所提出的结果为聚甲川染料的合理分子设计和应用提供了深入的了解和指导。
