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  Shining Light on the Microscopic Resonant Mechanism Responsible for Cavity-Mediated Chemical Reactivity

Schäfer, C., Flick, J., Ronca, E., Narang, P., & Rubio, A. (2021). Shining Light on the Microscopic Resonant Mechanism Responsible for Cavity-Mediated Chemical Reactivity.

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2104.12429.pdf (Preprint), 12MB
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https://arxiv.org/abs/2104.12429 (Preprint)
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 Creators:
Schäfer, C.1, 2, 3, 4, 5, Author              
Flick, J.6, 7, Author
Ronca, E.8, Author
Narang, P.7, Author
Rubio, A.1, 2, 3, 6, Author              
Affiliations:
1Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
2Center for Free-Electron Laser Science, ou_persistent22              
3The Hamburg Center for Ultrafast Imaging, ou_persistent22              
4Department of Physics, Chalmers University of Technology, ou_persistent22              
5Department of Microtechnology and Nanoscience, MC2, Chalmers University of Technology, ou_persistent22              
6Center for Computational Quantum Physics, Flatiron Institute, New York, ou_persistent22              
7John A. Paulson School of Engineering and Applied Sciences, Harvard University, ou_persistent22              
8Instituto per i Processi Chimico Fisici del CNR (IPCF-CNR), ou_persistent22              

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 Abstract: Strong light-matter interaction in cavity environments has emerged as a promising and general approach to control chemical reactions in a non-intrusive manner. The underlying mechanism that distinguishes between steering, accelerating, or decelerating a chemical reaction has, however, remained thus far largely unclear, hampering progress in this frontier area of research. In this work, we leverage a combination of first-principles techniques, foremost quantum-electrodynamical density functional theory, applied to the recent experimental realization by Thomas et al. [1] to unveil the microscopic mechanism behind the experimentally observed reduced reaction-rate under resonant vibrational strong light-matter coupling. We find that the cavity mode functions as a mediator between different vibrational eigenmodes, transferring vibrational excitation and anharmonicity, correlating vibrations, and ultimately strengthening the chemical bond of interest. Importantly, the resonant feature observed in experiment, theoretically elusive so far, naturally arises in our investigations. Our theoretical predictions in polaritonic chemistry shine new light on cavity induced mechanisms, providing a crucial control strategy in state-of-the-art photocatalysis and energy conversion, pointing the way towards generalized quantum optical control of chemical systems.

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Language(s): eng - English
 Dates: 2021-04-26
 Publication Status: Published online
 Pages: 11
 Publishing info: -
 Table of Contents: -
 Rev. Type: No review
 Identifiers: arXiv: 2104.12429
 Degree: -

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