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We present numerically exact quantum dynamics simulations using the hierarchical equation of motion approach to investigate the resonance enhancement of chemical reactions due to the vibrational strong coupling (VSC) in polariton chemistry. The results reveal that the cavity mode acts like a “rate-promoting vibrational mode” that enhances the ground state chemical reaction rate constant when the cavity mode frequency matches the vibrational transition frequency. The exact simulation predicts that the VSC-modified rate constant will change quadratically as the light–matter coupling strength increases. When changing the cavity lifetime from the lossy limit to the lossless limit, the numerically exact results predict that there will be a turnover of the rate constant. Based on the numerical observations, we present an analytic rate theory to explain the observed sharp resonance peak of the rate profile when tuning the cavity frequency to match the quantum transition frequency of the vibrational ground state to excited states. This rate theory further explains the origin of the broadening of the rate profile. The analytic rate theory agrees with the numerical results under the golden rule limit and the short cavity lifetime limit. To the best of our knowledge, this is the first analytic theory that is able to explain the sharp resonance behavior of the VSC-modified rate profile when coupling an adiabatic ground state chemical reaction to the cavity. We envision that both the numerical analysis and the analytic theory will offer invaluable theoretical insights into the fundamental mechanism of the VSC-induced rate constant modifications in polariton chemistry.
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Loading short pulses into long lifetime cavities
We demonstrate the loading of very short optical pulses into a high-Q cavity with linewidth much narrower than the pulse frequency envelope. We show that loading into the cavity is significantly enhanced if the pulse is combined with a cw-field, thus altering the pulse frequency profile to better match the cavity profile.
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- Award ID(s):
- 1936345
- PAR ID:
- 10437358
- Date Published:
- Journal Name:
- CLEO: QELS_Fundamental Science 2022
- Page Range / eLocation ID:
- FM5B.3
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript
- Conference Paper:
- https://doi.org/10.1364/CLEO_QELS.2022.FM5B.3
