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State-Selective Polariton to Dark State Relaxation Dynamics
Bo Xiang1, Raphael F Ribeiro2, Liying Chen2
1Materials Science and Engineering Program , University of California, San Diego , La Jolla , California 92093 , United States.
The Journal of Physical Chemistry. A
|July 4, 2019
Summary
Molecular vibrational polaritons show solvent-dependent dynamics. Lower polaritons in low polarity solvents exhibit slower energy transfer to dark modes, suggesting intermediate states, crucial for cavity-modified chemistry.
Area of Science:
- Physical Chemistry
- Chemical Physics
- Spectroscopy
Background:
- Modifying vibrational dynamics is key for controlling chemical reactions and infrared photonic devices.
- Hybridization between cavity modes and molecular vibrations offers a novel approach to manipulate molecular dynamics.
Purpose of the Study:
- Investigate the dynamics of molecular vibrational polaritons across diverse solvent environments.
- Understand how solvent properties influence polariton relaxation pathways and lifetimes.
Main Methods:
- Theoretical study of molecular vibrational polaritons.
- Analysis of polariton dynamics in various solvent polarities.
- Time-resolved spectroscopy simulations.
Main Results:
- Polariton dynamics are significantly affected by solvent polarity.
- Upper polariton (UP) relaxation to dark modes is consistently rapid (<5 ps).
- Lower polariton (LP) in low polarity solvents shows delayed transfer (10-30 ps) to dark modes, with LP lifetime <5 ps, indicating intermediate states.
Conclusions:
- Solvent interactions dictate the relaxation pathways of molecular vibrational polaritons.
- In low polarity solvents, LP energy populates intermediate dark states before decaying.
- This slow decay into intermediate states may explain observed cavity-modified chemistry phenomena.
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