Large optical nonlinearity enhancement under electronic strong coupling

Abstract

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 organic molecules to an optical mode of a Fabry-Perot cavity, and achieve an enhancement of the nonlinear complex 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 nonlinar coefficients in this work paves the way for exploring strong coupling effects on various third-order nonlinear optical phenomena and for technological applications.

31 pages, including Supplementary Material file

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• Femtosecond Photophysics of Molecular Polaritons
• When do molecular polaritons behave like optical filters?
• Real-Space, Real-Time Approach to Quantum-Electrodynamical Time-Dependent Density Functional Theory
• Stochastic Variational Approach to Small Atoms and Molecules Coupled to Quantum Field Modes
• Nonlinear semiclassical spectroscopy of ultrafast molecular polariton dynamics
• Mechanisms of the Intensity Dependent Refractive Index in Ultrastrongly Coupled Organic Cavity Polaritons
• The universal model of strong coupling at the nonlinear parametric resonance in open cavity-QED systems
• Spontaneous Raman Scattering under Vibrational Strong Coupling: The Critical Role of Polariton Spatial Mode Coherence