Multipolar molecules and multipolar fields: probing and controlling the tensorial nature of nonlinear molecular media
Multipolar molecules and multipolar fields: probing and controlling the tensorial nature of nonlinear molecular media
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DOI：
10.1364/josab.15.000257
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发表时间：
1998-01-01
影响因子：
1.9
通讯作者：
Zyss, J
中科院分区：
文献类型：
--
作者：
Brasselet, S;Zyss, J
在二次非线性光学的背景下，通过对偶极分子和八极分子的推广，介绍了一类一般的多极分子。适当的不可约张量形式允许我们定义与相应场张量分量耦合的旋转不变分子特征，从而使我们能够解释各种相干和非相干过程，如谐波光（超瑞利）散射，电极化介质中的相干二次谐波产生，以及最近提出的光学极化方案。根据该模型分析了溶液中的调和光散射实验（针对某些多极分子）和光学极化实验（在分散红1-甲基丙烯酸甲酯薄膜中）。一个广义的张量置换引理允许非线性光-物质相互作用在统计介质中以紧凑的旋转不变表达式浓缩：分子敏感性和读写场极化张量共同驱动这些相互作用的主要张量对称性特征被清楚地揭示出来。(C) 1998美国光学学会。
A general class of multipolar molecules is introduced in the context of quadratic nonlinear optics by way of extension of the more specific cases of dipolar and octupolar molecules. An adequate irreducible tensor formalism permits us to define rotationally invariant molecular features that couple to corresponding field tensor components, thereby enabling us to account for a variety of coherent and noncoherent processes such as harmonic light (hyper-Rayleigh) scattering, coherent second-harmonic generation in electrically poled media, and the recently proposed optical poling scheme. Experiments in both harmonic light scattering in solution (for some multipolar molecules) and optical poling (in Disperse Red 1-methyl methacrylate thin films) are analyzed in light of this model. A general tensorial permutation lemma of broad validity allows nonlinear light-matter interactions to be condensed in a statistical medium in compact rotationally invariant expressions: The main tensorial symmetry features for both molecular susceptibility and read-write field polarization tensors that jointly drive these interactions are clearly revealed. (C) 1998 Optical Society of America.