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Title: Super-reaction: The collective enhancement of a reaction rate by molecular polaritons in the presence of energy fluctuations
Authors: Nguyen, Thanh Phuc
Author's alias: グエン, タンフク
Issue Date: Jul-2021
Publisher: AIP Publishing
Journal title: The Journal of Chemical Physics
Volume: 155
Issue: 1
Thesis number: 014308
Abstract: Recent experiments have demonstrated that molecular polaritons, hybrid states of light and matter formed by the strong coupling between molecular electronic or vibrational excitations and an optical cavity, can substantially modify the physical and chemical properties of molecular systems. Here, we show that by exploiting the collective character of molecular polaritons in conjunction with the effect of polaron decoupling, i.e., the suppression of environmental influence on the polariton, a super-reaction can be realized, involving a collective enhancement of charge or excitation-energy transfer reaction rate in a system of donors all coupled to a common acceptor. This effect is analogous to the phenomenon of super-radiation. Since the polariton is a superposition state of excitations of all the molecules coupled to the cavity, it is vulnerable to the effect of decoherence caused by energy fluctuations in molecular systems. Consequently, in the absence of a strong light–matter interaction, the reaction rate decreases significantly as the number of molecules increases, even if the system starts from the polariton state. By turning on the light–matter interaction, the dynamic behavior of the system changes dramatically, and the reaction rate increases with the number of molecules, as expected for a super-reaction. The underlying mechanism is shown to be the protection of quantum coherence between different donors as the light–matter interaction becomes stronger.
Rights: © 2021 Author(s).
This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This article appeared in Nguyen Thanh Phuc , "Super-reaction: The collective enhancement of a reaction rate by molecular polaritons in the presence of energy fluctuations", J. Chem. Phys. 155, 014308 (2021) and may be found at https://doi.org/10.1063/5.0052226.
The full-text file will be made open to the public on 7 July 2022 in accordance with publisher's 'Terms and Conditions for Self-Archiving'.
URI: http://hdl.handle.net/2433/265503
DOI(Published Version): 10.1063/5.0052226
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