Work

Influence of Strong Molecular Vibrations on Decoherence of Molecular Polaritons

Year: 2024

Type: article

Abstract: We derive the transition rates, dephasing rates, and Lamb shifts for a system consisting of many molecules collectively coupled to a resonant cavity mode. Using a variational polaron master equation, we show that strong vibrational interactions inherent to molecules give rise to multi-phonon processes and suppress the light-matter coupling. In the strong light-matter coupling limit, multiphonon contributions to the transition and dephasing rates strongly dominate over single-phonon contributions for typical molecular parameters. This leads to novel dependencies of the rates and spectral line widths on the number of molecules in the cavity. We also find that vibrational Lamb shifts can substantially modify the polariton energies in the strong light-matter coupling limit.

Source: ACS Photonics

DOI: 10.1021/acsphotonics.4c01446

Authors: Dominic M. Rouse, Erik M. Gauger, Brendon W. Lovett

Institutions: University of Glasgow, Heriot-Watt University, University of St Andrews

Language: English

Topic: Strong Light-Matter Interactions

Subfield: Atomic and Molecular Physics, and Optics

Field: Physics and Astronomy

Domain: Physical Sciences

Open Access status: hybrid

Estimated APC paid: $4,500

Funders: Leverhulme Trust, University of Glasgow, Engineering and Physical Sciences Research Council