级联效应对二阶超极化率贡献上界的量子力学模型
A quantum mechanical model of the upper bounds of the cascading contribution to the second hyperpolarizability
摘要：
两个分子之间的二阶非线性的微观级联已经被提出来产生增强的三阶分子非线性光学响应。在这篇文章中，我们研究了两分子级联的第二超极化率，并表明它永远不会超过一个具有相同电子数的两分子系统的单分子的基本限制。当适当考虑分子间相互作用时，我们发现级联效应对二阶超极化率的贡献消失了。虽然级联永远不会导致比单个分子更大的非线性光学响应，但它提供了替代的分子设计配置，用于创建具有大的三阶折射率的材料，这些材料可能难以设计成单个分子。
英文摘要：
Microscopic cascading of second-order nonlinearities between two molecules has been proposed to yield an enhanced third-order molecular nonlinear-optical response. In this contribution, we investigate the two-molecule cascaded second hyperpolarizability and show that it will never exceed the fundamental limit of a single molecule with the same number of electrons as the two-molecule system. We show the apparent divergence behavior of the cascading contribution to the second hyperpolarizability vanishes when properly taking into account the intermolecular interactions. Although cascading can never lead to a larger nonlinear-optical response than a single molecule, it provides alternative molecular design configurations for creating materials with large third-order susceptibilities that may be difficult to design into a single molecule.
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