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Excited State Dynamics of CO₂ Reduction Catalyst under Vibrational Strong Coupling.

Tao Jin¹, Sara T Gebre², Christopher J Miller³

¹Department of Physics, Emory University, 1515 Dickey Drive, Northeast, Atlanta, Georgia 30322, United States.

Journal of the American Chemical Society

|October 10, 2025

Summary

Vibrational strong coupling (VSC) did not significantly alter the dynamic Stokes shift of CO modes in a Re(bpy-COOH)(CO)3Cl complex. This study explored polariton effects on molecular excited-state dynamics using transient IR spectroscopy.

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Published on: February 1, 2020

Area of Science:

Physical Chemistry
Spectroscopy
Quantum Optics

Background:

Molecular polaritons, formed by strong coupling between molecular transitions and optical cavities, offer new ways to control chemical dynamics.
Vibrational strong coupling (VSC) is a key phenomenon in manipulating molecular properties via light-matter interactions.

Purpose of the Study:

To investigate the impact of VSC on solvation-induced time-dependent Stokes shifts.
To probe the excited-state dynamics of Re(bpy-COOH)(CO)3Cl (ReC0A) complex under VSC conditions.
To explore polariton dynamics and their influence on molecular processes.

Main Methods:

Transient infrared (IR) transmission spectroscopy.
Angle-resolved time-dependent transmission spectra of vibrational polaritons.
Fabry-Perot microcavity setup.
Time-dependent excited-state absorption modeling.

Main Results:

Distinct infrared polaritonic signatures of the CO dynamical Stokes shift were observed.
Negligible changes in the solvation-induced vibrational dynamic Stokes shift of CO modes were found under VSC.
Perturbed free induction decay was analyzed in relation to polariton dynamics.

Conclusions:

VSC has minimal effect on the solvation-induced dynamic Stokes shift of CO modes in the studied complex.
The experimental setup provides a platform for probing fundamental VSC effects on molecular reactivity and charge transfer.