Theory of efficient nonlinear optical excitations based on manipulation of quantum interferences

我们已经从理论上研究了提高光子和有机分子（量子点）之间非线性响应效率的方案。我们将重点放在分子与辅助系统耦合的系统上，例如，在半导体微结构中使用一小块金属纳米和腔模式的光学天线。因此，我们开发了一种方法，在遥远的腔中创造量子点之间的纠缠态。此外，考虑到由光学天线和分子（量子点）组成的耦合系统，我们揭示了增强非线性光激发的条件。所有的结果都可以通过考虑整个系统组成元素之间的量子干涉来解释。此外，将量子主方程与离散偶极子近似方法相结合，提出了在特定系统假设下的非线性响应计算方案。

We have theoretically studied schemes improving efficiencies of nonlinear responses between photons and organic molecules (quantum dots). We focus on the system where the molecules are coupled with auxiliary systems, e.g., optical antenna using a small piece of metal nanometers and cavity mode in the semiconductor microstructure. As a result, we developed a method to create an entangled state between quantum dots in distant cavities. Besides, considering coupled systems that consists of optical antenna and molecules (quantum dots), we revealed the conditions to enhance nonlinear optical excitations. All of the results can be explained by considering quantum interferences between composition elements of the entire systems. In addition, by combining quantum master equation and the discrete dipole approximation method, a scheme to calculate the nonlinear response on the assumption that specific system was developed.