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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >QTAIM-Based Scheme for Describing the Linear and Nonlinear Optical Susceptibilities of Molecular Crystals Composed of Molecules with Complex Shapes
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QTAIM-Based Scheme for Describing the Linear and Nonlinear Optical Susceptibilities of Molecular Crystals Composed of Molecules with Complex Shapes

机译：基于QTAIM的描述具有复杂形状的分子组成的分子晶体的线性和非线性光学敏感性的方案

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The Quantum Theory of Atoms in Molecules (QTAIM) to distribute the molecular polarizability tensors over submolecular sites is employed to improve the prediction of local field tensors of molecular crystals and therefore of their linear and second-order nonlinear optical susceptibilities. This extension of the two-step multiscale procedure is intended to better describe crystals built of molecules having complex shapes. When combined with a simple charge embedding approach to account for the crystal field effects on the molecular (hyper)polarizabilities, this QTAIM local field theory (Q-LFT) approach is efficient to predict the x((1))) and x((2)) tensor components. Moreover, it does not require substantial computational resources because the largest calculations are performed on the individual molecules. This is illustrated by considering derivatives of (S)-2-(alpha-methylbenzylamino)-S-nitropyridine (MBANP) as well as 2-methyl-4-nitroanline (MNA), which is a prototypical push pull pi-conjugated compound. In the latter case, the use of the Q-LFT only:leads to minor differences in the?) and x((2)) tensor components with respect to the standard approach where the polarizability is equipartitioned. In the case of the MBANP derivatives, the Q-LFT scheme leads to systematic decrease of the linear and nonlinear optical responses. This generally improves the agreement between the calculated and experimental refractive indices and second-order nonlinear optical susceptibilities. Indeed, the standard partitioning scheme leads to an overestimation of the phenyl out-of-plane polarization component and therefore of the refractive indices. The x((2)) variations among the MBANP derivatives have further been analyzed in terms of molecular geometry, crystal polarizing field, and crystal packing.
机译：利用分子中的原子量子理论（QTAIM）将分子极化率张量分布在亚分子位点上，以改善对分子晶体局部场张量的预测，从而改善其线性和二阶非线性光学磁化率。两步多尺度程序的这种扩展旨在更好地描述由具有复杂形状的分子构建的晶体。当与简单的电荷嵌入方法结合以考虑晶体场对分子（超）极化率的影响时，这种QTAIM局域理论（Q-LFT）方法可有效预测x（（1）））和x（（ 2））张量分量。而且，由于最大的计算是对单个分子进行的，因此不需要大量的计算资源。考虑到（S）-2-（α-甲基苄氨基）-S-硝基吡啶（MBANP）的衍生物以及2-甲基-4-硝基苯胺（MNA），这是典型的推挽式π-共轭化合物，对此进行了说明。在后一种情况下，仅使用Q-LFT：相对于极化率均分的标准方法，会导致？）和x（（2））张量分量的微小差异。在MBANP衍生物的情况下，Q-LFT方案导致线性和非线性光学响应的​​系统减小。这通常会提高计算出的折射率和实验折射率与二阶非线性光学磁化率之间的一致性。实际上，标准分配方案导致对苯基面外极化分量的高估，因此导致对折射率的高估。 MBANP衍生物之间的x（（2））变化已进一步进行了分子几何学，晶体极化场和晶体堆积方面的分析。

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