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Towards highly efficient nonlinear optical chromophores: molecular engineering of octupolar molecules

机译：迈向高效的非线性光学发色团：八极分子的分子工程

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摘要

Octupolar molecules are of particular interest in the field of nonlinear optics due to their potentially large two or three-dimensional quadratic nonlinearities. In order to design molecules combining enhanced first hyperpolarizabilities and excellent transparency, we have implemented an original strategy based upon adequate functionalization of an orthogonalized biphenyl core. We have designed novel 3-dimensional all-organic octupoles of D_2d symmetry and investigated their optical nonlinearities by performing harmonic light scattering experiments in solution. By grafting four electron-donating and/or electron withdrawing substituents on the central biphenyl unit, large molecular nonlinearities (β) have been achieved while maintaining full transparency in the visible range. Molecules displaying larger nonlinearities and better transparency than pNA have been obtained. Molecular optimization has been further pursued via tethering elongated conjugated spikes on the central biphenyl core and taking advantage of multidimensional charge transfer leading to 3D-octupolar molecules disp1aying both larger nonlinearity and broader transparency than DRl (up to β_xy = l45 x l0~-30 esu with λ_max = 400 nm).
机译：由于八极分子可能具有较大的二维或三维二次非线性，因此在非线性光学领域特别受关注。为了设计结合了增强的第一超极化性和出色的透明性的分子，我们基于正交化联苯核的适当功能化，实施了一种原始策略。我们设计了新颖的D_2d对称3维全有机八极体，并通过在溶液中进行谐波散射实验研究了它们的光学非线性。通过在中心联苯单元上接枝四个供电子和/或吸电子取代基，在保持可见范围内的完全透明性的同时，实现了大分子非线性（β）。已经获得了比pNA具有更大的非线性和更好的透明度的分子。通过在中心联苯核心上束缚细长的共轭尖峰并利用多维电荷转移导致3D-八极分子比DR1具有更大的非线性和更宽的透明度（高达β_xy= l45 x l0〜-30 esu）来进一步追求分子优化λ_max= 400 nm）。

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