Rovibrational Polaritons in Gas-Phase Methane
arXiv:2212.13506 · doi:10.1021/jacs.3c00126
Abstract
Polaritonic states arise when a bright optical transition of a molecular ensemble is resonantly matched to an optical cavity mode frequency. Here, we lay the groundwork to study the behavior of polaritons in clean, isolated systems by establishing a new platform for vibrational strong coupling in gas-phase molecules. We access the strong coupling regime in an intracavity cryogenic buffer gas cell optimized for the preparation of simultaneously cold and dense ensembles, and report a proof-of-principle demonstration in gas-phase methane. We strongly cavity-couple individual rovibrational transitions and probe a range of coupling strengths and detunings. We reproduce our findings with classical cavity transmission simulations in the presence of strong intracavity absorbers. This infrastructure provides a new testbed for benchmark studies of cavity-altered chemistry.
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Cited by in corpus (14)
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- Selective Excitation of IR-Inactive Modes via Vibrational Polaritons: Insights from Atomistic Simulations
- A Cavity-Enhanced Spectroscopist's Lens on Molecular Polaritons
- Ab initio study on the dynamics and spectroscopy of collective rovibrational polaritons
- Ehrenfest Modeling of Cavity Vacuum Fluctuations and How to Achieve Emission from a Three-Level Atom
- Direct readout of excited state lifetimes in chlorin chromophores under electronic strong coupling
- Coherent anharmonicity transfer from matter to light in the THz regime
- Polariton-induced Purcell effects via a reduced semiclassical electrodynamics approach
- Spontaneous Raman Scattering under Vibrational Strong Coupling: The Critical Role of Polariton Spatial Mode Coherence