Two-dimensional Infrared Spectroscopy of vibrational polaritons of molecules in an optical cavity

Abstract

Strong coupling of molecular vibrations to an infrared cavity mode affects their nature by creating dressed polariton states. We show how the single and double vibrational polariton manifolds may be controlled by varying the cavity coupling strength, and probed by a time domain 2DIR technique, Double Quantum Coherence (DQC). Applications are made to the amide-I ($CO$) and amide-II ($CN$) bond vibrations of $N-methylacetamide$ (NMA).

arXiv comment16 pages, 6 figures, 1 table

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• Theory of Nanoscale Organic Cavities: The Essential Role of Vibration-Photon Dressed States
• Manipulating Optical Nonlinearities of Molecular Polaritons by Delocalization
• Swinging between shine and shadow: Theoretical advances on thermally-activated vibropolaritonic chemistry (a perspective)
• Multi-level quantum Rabi model for anharmonic vibrational polaritons
• Molding Molecular and Material Properties by Strong Light-Matter Coupling
• The Shape of the Electric Dipole Function Determines the Sub-Picosecond Dynamics of Anharmonic Vibrational Polaritons
• Polariton relaxation under vibrational strong coupling: Comparing cavity molecular dynamics simulations against Fermi's golden rule rate
• Photonics and Spectroscopy in Nanojunctions: A Theoretical Insight
• Generalization of the Tavis-Cummings model for multi-level anharmonic systems: insights on the second excitation manifold
• Light-matter hybrid-orbital-based first-principles methods: the influence of the polariton statistics
• Generalization of the Tavis-Cummings model for multi-level anharmonic systems
• Cavity-induced Non-Adiabatic Dynamics and Spectroscopy of Molecular Rovibrational Polaritons studied by Multi-Mode Quantum Models
• 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
• Disentangling collective coupling in vibrational polaritons with double quantum coherence spectroscopy
• Ab initio study on the dynamics and spectroscopy of collective rovibrational polaritons
• Coherent nonlinear optical probe for cavity-dressed vibrational mode mixing: Multidimensional double-quantum coherence and photon-echo spectroscopy
• Density-Functional Tight Binding Meets Maxwell: Unraveling the Mysteries of (Strong) Light-Matter Coupling Efficiently