Rovibrational Polaritons in Gas-Phase Methane

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

Research output: Contribution to journalArticlepeer-review

22 Scopus citations

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

Original languageEnglish (US)
Pages (from-to)5982-5987
Number of pages6
JournalJournal of the American Chemical Society
Volume145
Issue number10
DOIs
StatePublished - Mar 15 2023

All Science Journal Classification (ASJC) codes

  • General Chemistry
  • Biochemistry
  • Catalysis
  • Colloid and Surface Chemistry

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