Manipulating Optical Nonlinearities of Molecular Polaritons by Delocalization

Abstract

Optical nonlinearities - how light-matter interactions are influenced by previous interactions with photons, are key resources in the contemporary photonics toolbox, relevant to quantum gate operations and all-optical switches. Optical nonlinearities of materials are often controlled at the microscopic level by chemical modification, which makes on-the-fly manipulation of such response challenging. Tunability of optical nonlinearities in the mid-IR is even less developed, hindering its applications in chemical sensing or IR photonic circuitry. Here, we report control of vibrational polariton coherent nonlinearities by manipulation of macroscopic parameters such as cavity longitudinal length or molecular concentration. These emergent nonlinearities last for the lifetime of the cavity mode, and subsequently evolve into the response determined by an incoherent population of dark reservoir modes. The observed phenomena arise due to the nonlinear macroscopic polarization stemming from strong coupling between microscopic molecular excitations and a macroscopic photonic cavity mode.

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Cited by in corpus (23)

• Molecular polaritons for controlling chemistry with quantum optics
• Molecular polaritonics: Chemical Dynamics under strong Light-Matter Coupling
• Catalysis by Dark States in Vibropolaritonic Chemistry
• Swinging between shine and shadow: Theoretical advances on thermally-activated vibropolaritonic chemistry (a perspective)
• Untargeted Effects in Organic Exciton-Polariton Transient Spectroscopy: A Cautionary Tale
• Cavity molecular dynamics simulations of vibrational polariton enhanced molecular nonlinear absorption
• Enhanced optical nonlinearities under strong light-matter coupling
• Enhancing vibrational light-matter coupling strength beyond the molecular concentration limit using plasmonic arrays
• Polariton relaxation under vibrational strong coupling: Comparing cavity molecular dynamics simulations against Fermi's golden rule rate
• Generalization of the Tavis-Cummings model for multi-level anharmonic systems
• Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach
• An efficient and flexible approach for computing rovibrational polaritons from first principles
• Semi-empirical Quantum Optics for Mid-Infrared Molecular Nanophotonics
• Nonlinear semiclassical spectroscopy of ultrafast molecular polariton dynamics
• Ultrafast modulation of vibrational polaritons for controlling the quantum field statistics at mid-infrared frequencies
• Ab initio study on the dynamics and spectroscopy of collective rovibrational polaritons
• Interplay between Static and Dynamic Disorder: Contrasting Effects on Dark State Population inside a Cavity
• Theory of Molecular Emission Power Spectra. III. Non-Hermitian Interactions in Multichromophoric Systems Coupled with Polaritons
• Coherent anharmonicity transfer from matter to light in the THz regime
• Coherent nonlinear optical probe for cavity-dressed vibrational mode mixing: Multidimensional double-quantum coherence and photon-echo spectroscopy
• Multimode vibrational coupling across the insulator-to-metal transition in 1T-TaS${}_2$ in THz cavities
• Strong light-matter interaction effects on molecular ensembles
• Linear and nonlinear vibrational excitation driven by molecular polaritons