A1 Journal article (refereed)
Polariton response in the presence of Brownian dissipation from molecular vibrations (2021)
Kansanen, K. S. U., Toppari, J. J., & Heikkilä, T. T. (2021). Polariton response in the presence of Brownian dissipation from molecular vibrations. Journal of Chemical Physics, 154(4), Article 044108. https://doi.org/10.1063/5.0036905
JYU authors or editors
Publication details
All authors or editors: Kansanen, Kalle S. U.; Toppari, J. Jussi; Heikkilä, Tero T.
Journal or series: Journal of Chemical Physics
ISSN: 0021-9606
eISSN: 1089-7690
Publication year: 2021
Publication date: 28/01/2021
Volume: 154
Issue number: 4
Article number: 044108
Publisher: American Institute of Physics
Publication country: United States
Publication language: English
DOI: https://doi.org/10.1063/5.0036905
Publication open access: Not open
Publication channel open access:
Publication is parallel published (JYX): https://jyx.jyu.fi/handle/123456789/74020
Web address of parallel published publication (pre-print): https://arxiv.org/abs/2011.03421
Abstract
We study the elastic response of a stationarily driven system of a cavity field strongly coupled with molecular excitons, taking into account the main dissipation channels due to the finite cavity linewidth and molecular vibrations. We show that the frequently used coupled oscillator model fails in describing this response especially due to the non-Lorentzian dissipation of the molecules to their vibrations. Signatures of this failure are the temperature dependent minimum point of the polariton peak splitting, the uneven polariton peak height at the minimum splitting, and the asymmetric shape of the polariton peaks even at the experimentally accessed “zero-detuning” point. Using a rather generic yet representative model of molecular vibrations, we predict the polariton response in various conditions, depending on the temperature, molecular Stokes shift and vibration frequencies, and the size of the Rabi splitting. Our results can be used as a sanity check of the experiments trying to “prove” results originating from strong coupling, such as vacuum-enhanced chemical reaction rate.
Keywords: molecular physics; quantum physics; quasiparticles; polaritons
Free keywords: molecular vibrations
Contributing organizations
Related projects
- Hybrid nanoelectronic systems in and out of the quantum limit
- Heikkilä, Tero
- Research Council of Finland
- Manipulating Chemistry with Vacuum Light Fields
- Toppari, Jussi
- Research Council of Finland
Ministry reporting: Yes
Reporting Year: 2021
JUFO rating: 1