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Abstract Recent experiments demonstrate polaritons under the vibrational strong coupling (VSC) regime can modify chemical reactivity. Here, we present a complete theory of VSC-modified rate constants when coupling a single molecule to an optical cavity, where the role of photonic mode lifetime is understood. The analytic expression exhibits a sharp resonance behavior, where the maximum rate constant is reached when the cavity frequency matches the vibration frequency. The theory explains why VSC rate constant modification closely resembles the optical spectra of the vibration outside the cavity. Further, we discussed the temperature dependence of the VSC-modified rate constants. The analytic theory agrees well with the numerically exact hierarchical equations of motion (HEOM) simulations for all explored regimes. Finally, we discussed the resonance condition at the normal incidence when considering in-plane momentum inside a Fabry-Pérot cavity.
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Whispering gallery modes of a triatomic photonic molecule
In this paper, we present the results of numerical simulations of the optical spectra of a three-sphere photonic molecule. The configuration of the system was continuously modified from linear to triangular, in-plane with the fundamental mode excited in one of the spheres and perpendicular to it. We found the relative insensitivity of the spectra to the in-plane deviation from the linear arrangement up to about 110°. For larger angles, the spectra show significant modification consisting of the major spectral peaks splitting and shifting. On the contrary, the spectra are quite sensitive to out-of-plane molecule deviation, even at small angles. Thus, the spectra of photonic molecules can be modified by changing the mutual positions of the constituent resonators, which can be useful in reconfigurable photonic devices.
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- Award ID(s):
- 2102249
- PAR ID:
- 10597390
- Publisher / Repository:
- American Institute of Physics
- Date Published:
- Journal Name:
- AIP Advances
- Volume:
- 12
- Issue:
- 11
- ISSN:
- 2158-3226
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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