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Fluidic Molecular Dynamics and Energy Relaxation Pathways in Solution-State Electronic Strong Coupling Using a
Soh Kushida1,2, Kuidong Wang1, Marcus Seidel1
1University of Strasbourg, CNRS, ISIS & icFRC, 8 allée Gaspard Monge, 67000 Strasbourg, France.
The Journal of Physical Chemistry Letters
|August 13, 2025
Summary
Strong coupling between light and matter (SC) enables control over molecular dynamics. This study reveals new ultrafast dynamics in liquid-state molecules under electronic strong coupling (ESC), showing faster energy migration than previously observed.
Area of Science:
- Photochemistry
- Physical Chemistry
- Spectroscopy
Background:
- Light-matter strong coupling (SC) offers control over molecular photophysical dynamics.
- Previous studies on ultrafast dynamics under electronic strong coupling (ESC) primarily focused on solid-state molecular samples.
- The influence of hybridized light-matter states on liquid-phase molecular dynamics remained unexplored.
Purpose of the Study:
- To investigate the ultrafast dynamics of liquid-state molecules under electronic strong coupling (ESC) for the first time.
- To explore the impact of hybridized light-matter states on molecular dynamics in the liquid phase.
- To understand the role of SC in controlling photochemical processes in liquids.
Main Methods:
- Transient absorption spectroscopy to probe ultrafast dynamics.
- Resonant optical Kerr-effect (ROKE) spectroscopy to analyze depolarization kinetics.
- Comparison of liquid-state ESC dynamics with and without an optical cavity.
Main Results:
- Observation of a novel fast decay component in liquid-state ESC, absent in non-coupled systems.
- Accelerated depolarization kinetics in liquid-state ESC, indicating faster energy migration.
- Energy migration rates exceeding polariton lifetimes and molecular rotational constants.
Conclusions:
- Electronic strong coupling significantly alters ultrafast molecular dynamics in the liquid phase.
- Hybridized light-matter states facilitate rapid energy migration in liquid systems.
- These findings provide a foundation for designing liquid-state photochemical systems utilizing SC principles.
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