arXiv 2008.130492020-08-29physics.optics

高温下平面八极分子非线性光学的纳米有序化

Nanoscale ordering of planar octupolar molecules for nonlinear optics at higher temperatures

Michał Jarema, Antoni C. Mituś, Joseph Zyss

摘要：

我们开发的方案在低浓度限制的平面内系统的小平面八极分子的取向有序，在室温下的非线性光学（NLO）的应用程序的目标。八极子与外电场相互作用，分子间相互作用忽略不计。简单的几何力学模型被用来分析在非常弱的极化极限，足以检索的NLO信号，由于NLO探测器和测量链的高灵敏度的取向顺序。讨论了两种情况。首先，八极极化场是由点电荷系统赋予的;该设置受到机械强度和介电击穿极限所施加的与细胞相关的约束。非常弱的八极顺序的基准TATB分子示出出现在氦气温度。第二种情况解决了偶极八极分子与电偶极成分的小混合物。它需要一个强大的领域制度，成为有效的氮气温度范围。在高温（弱相互作用）极限形式主义的非线性磁化率系数矩阵的估计。我们认为，适度的修改系统，如，八极尺寸的增加，伴随着偶极辅助八极化，可以将极化温度增加到氮气温度以上。

英文摘要：

We develop scenarios for orientational ordering of an in-plane system of small flat octupolar molecules at the low-concentration limit, aiming towards nonlinear-optical (NLO) applications at room temperatures. The octupoles interact with external electric poling fields and intermolecular interactions are neglected. Simple statistical-mechanics models are used to analyze the orientational order in the very weak poling limit, sufficient for retrieving the NLO signals owing to the high sensitivity of NLO detectors and measurement chains. Two scenarios are discussed. Firstly, the octupolar poling field is imparted by a system of point charges; the setup is subject to cell-related constraints imposed by mechanical strength and dielectric breakdown limit. The very weak octupolar order of benchmarking TATB molecules is shown to emerge at Helium temperatures. The second scenario addresses the dipoling of octupolar molecules with a small admixture of electric dipolar component. It requires a strong field regime to become effective at Nitrogen temperature range. An estimation of the nonlinear susceptibility coefficient matrix for both scenarios is done in the high-temperature (weak interaction) limit formalism. We argue that moderate modifications of the system like, e.g., an increase of the size of the octupole, accompanied by dipole-assisted octupoling, can increase the poling temperature above Nitrogen temperatures.

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