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Cavity-modified Fermi's golden rule rate constants: Beyond the single mode approximation.
Maximlian A C Saller1, Yifan Lai2, Eitan Geva1
1Department of Chemistrty, University of Michigan, Ann Arbor, Michigan 48109, USA.
The Journal of Chemical Physics
|October 20, 2023
Summary
This study shows that coupling a molecular system to multiple cavity modes significantly enhances Fermi
Area of Science:
- Quantum Chemistry
- Chemical Physics
- Spectroscopy
Background:
- Theoretical framework for estimating cavity-modified equilibrium Fermi's golden rule (FGR) rate constants was previously developed for single cavity modes.
- Understanding molecular system-cavity interactions is crucial for controlling chemical reaction rates.
Purpose of the Study:
- To extend the theoretical framework for FGR rate constants to systems coupled to multiple cavity modes.
- To investigate the cumulative effect of multiple cavity modes on FGR rate constants.
- To analyze conditions for maximizing rate enhancement in the Marcus limit.
Main Methods:
- Theoretical modeling of molecular systems coupled to multiple optical cavity modes.
- Extension of equilibrium Fermi's golden rule (FGR) formalism.
- Analysis within the Marcus limit of rate theory.
Main Results:
- The theoretical framework is successfully extended to multiple cavity modes.
- Coupling to multiple cavity modes can enhance FGR rate constants by orders of magnitude compared to single-mode coupling.
- Conditions for maximizing this enhancement in the Marcus limit are identified.
Conclusions:
- Simultaneous coupling to multiple cavity modes offers a significant pathway for enhancing chemical reaction rates.
- The extended theoretical framework provides a tool for designing systems with optimized cavity-enhanced reaction dynamics.
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