English

Rovibrational Polaritons in Gas-Phase Methane

Chemical Physics 2023-10-20 v2 Quantum Physics

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.

Keywords

Cite

@article{arxiv.2212.13506,
  title  = {Rovibrational Polaritons in Gas-Phase Methane},
  author = {Adam D. Wright and Jane C. Nelson and Marissa L. Weichman},
  journal= {arXiv preprint arXiv:2212.13506},
  year   = {2023}
}
R2 v1 2026-06-28T07:53:59.256Z