Wang Kuidong, Seidel Marcus, Nagarajan Kalaivanan, Chervy Thibault, Genet Cyriaque, Ebbesen Thomas
ISIS & icFRC, University of Strasbourg and CNRS, 8 allée Gaspard Monge, Strasbourg, France.
Institute of Quantum Electronics, ETH Zürich, Zürich, Switzerland.
Nat Commun. 2021 Mar 5;12(1):1486. doi: 10.1038/s41467-021-21739-7.
Nonlinear optical responses provide a powerful way to understand the microscopic interactions between laser fields and matter. They are critical for plenty of applications, such as in lasers, integrated photonic circuits, biosensing and medical tools. However, most materials exhibit weak optical nonlinearities or long response times when they interact with intense optical fields. Here, we strongly couple the exciton of cyanine dye J-aggregates to an optical mode of a Fabry-Perot (FP) cavity, and achieve an enhancement of the complex nonlinear refractive index by two orders of magnitude compared with that of the uncoupled condition. Moreover, the coupled system shows an ultrafast response of ~120 fs that we extract from optical cross-correlation measurements. The ultrafast and large enhancement of the optical nonlinar coefficients in this work paves the way for exploring strong coupling effects on various third-order nonlinear optical phenomena and for technological applications.
非线性光学响应为理解激光场与物质之间的微观相互作用提供了一种强有力的方法。它们对于许多应用至关重要，例如在激光器、集成光子电路、生物传感和医疗工具等方面。然而，大多数材料在与强光场相互作用时表现出较弱的光学非线性或较长的响应时间。在此，我们将花菁染料J聚集体的激子与法布里-珀罗（FP）腔的光学模式进行强耦合，并实现了复非线性折射率比未耦合状态下增强两个数量级。此外，耦合系统显示出约120飞秒的超快响应，这是我们从光学互相关测量中提取出来的。这项工作中光学非线性系数的超快和大幅增强为探索各种三阶非线性光学现象的强耦合效应以及技术应用铺平了道路。
