Rovibrational Polaritons in Gas-Phase Methane.

Wright, Adam D; Nelson, Jane C; Weichman, Marissa L

Wright, Adam D; Nelson, Jane C; Weichman, Marissa L.

Afiliación

Wright AD; Department of Chemistry, Princeton University, Princeton, New Jersey 08544, United States.
Nelson JC; Department of Chemistry, Princeton University, Princeton, New Jersey 08544, United States.
Weichman ML; Department of Chemistry, Princeton University, Princeton, New Jersey 08544, United States.

J Am Chem Soc ; 145(10): 5982-5987, 2023 Mar 15.

Article en En | MEDLINE | ID: mdl-36867733

RESUMEN

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 will provide a new testbed for benchmark studies of cavity-altered chemistry.

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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Am Chem Soc Año: 2023 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos

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