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Theory guided design and molecular engineering of organic materials for enhanced second-order nonlinear optical properties.

机译：理论指导有机材料的设计和分子工程，以增强二阶非线性光学特性。

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The last two decades of research in the field of organic 2nd-order nonlinear optical (electro-optic) materials has led to a deeper understanding of salient fundamental processes. Detailed definitions of critical structure-property relationships have led to the realization of new materials displaying dramatically enhanced properties. Despite the many recent advances, some critical problems remain unsolved. Although molecular nonlinearities (beta) have increased dramatically, bulk nonlinearity values (r33) have not increased in proportion. The major impediment to the resolution of this shortcoming is the difficulty faced in overcoming limited electric field induced molecular ordering caused by inter-molecular electrostatic interactions. Through the use of sophisticated statistical and quantum mechanical modeling, materials were designed which circumvented such detrimental molecular interactions. In the case of chromophore doped multichromophore dendrimers, these interactions were actually harnessed to enhance electric field induced dipolar order. As a result of this rational, theory guided design approach to novel electro-optic materials, unprecedented r33 (>300 pm/V) was demonstrated. Design, synthesis, and detailed characterization of these new materials is presented within this dissertation. Fundamental research toward molecular structure engineering as well as a new approach to optimization of molecular hyperpolarizability is presented as well.
机译：在有机二阶非线性光学（电光）材料领域的最后二十年研究使人们对基本的基本过程有了更深入的了解。关键结构-属性关系的详细定义导致显示出性能显着增强的新材料的实现。尽管最近取得了许多进步，但一些关键问题仍未解决。尽管分子非线性（β）急剧增加，但本体非线性值（r33）却没有按比例增加。解决该缺点的主要障碍是克服由分子间静电相互作用引起的有限电场诱导的分子有序化所面临的困难。通过使用复杂的统计和量子力学建模，设计了可避免此类有害分子相互作用的材料。在生色团掺杂的多生色团树状聚合物的情况下，实际上利用这些相互作用来增强电场诱导的偶极顺序。由于这种合理的，理论指导的新颖电光材料设计方法，结果证明了空前的r33（> 300 pm / V）。本文介绍了这些新材料的设计，合成和详细表征。还介绍了分子结构工程的基础研究以及优化分子超极化性的新方法。

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