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  Effect of many modes on self-polarization and photochemical suppression in cavities

Hoffmann, N., Lacombe, L., Rubio, A., & Maitra, N. T. (2020). Effect of many modes on self-polarization and photochemical suppression in cavities. The Journal of Chemical Physics, 153(10): 104103. doi:10.1063/5.0012723.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0005-8A4E-9 Version Permalink: http://hdl.handle.net/21.11116/0000-0007-2D41-E
Genre: Journal Article

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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 J. Chem. Phys. 153, 104103 (2020) and may be found at https://doi.org/10.1063/5.0012723.
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moviemultimode.mp4 (624 KB), moviemultimodewithsp.mp4 (749 KB), moviesinglemode.mp4 (411 KB)
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https://arxiv.org/abs/2001.07330 (Preprint)
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 Creators:
Hoffmann, N.1, 2, 3, Author              
Lacombe, L.1, Author
Rubio, A.2, 3, 4, 5, Author              
Maitra, N. T.1, Author
Affiliations:
1Department of Physics, Rutgers University at Newark, ou_persistent22              
2Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
3Center for Free-Electron Laser Science, ou_persistent22              
4Center for Computational Quantum Physics, Flatiron Institute, ou_persistent22              
5Nano-Bio Spectroscopy Group and ETSF, Universidad del Pas Vasco, ou_persistent22              

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 Abstract: The standard description of cavity-modified molecular reactions typically involves a single (resonant) mode, while in reality, the quantum cavity supports a range of photon modes. Here, we demonstrate that as more photon modes are accounted for, physicochemical phenomena can dramatically change, as illustrated by the cavity-induced suppression of the important and ubiquitous process of proton-coupled electron-transfer. Using a multi-trajectory Ehrenfest treatment for the photon-modes, we find that self-polarization effects become essential, and we introduce the concept of self-polarization-modified Born–Oppenheimer surfaces as a new construct to analyze dynamics. As the number of cavity photon modes increases, the increasing deviation of these surfaces from the cavity-free Born–Oppenheimer surfaces, together with the interplay between photon emission and absorption inside the widening bands of these surfaces, leads to enhanced suppression. The present findings are general and will have implications for the description and control of cavity-driven physical processes of molecules, nanostructures, and solids embedded in cavities.

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Language(s): eng - English
 Dates: 2020-05-042020-08-182020-09-092020-09-14
 Publication Status: Published in print
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 Table of Contents: -
 Rev. Type: Peer
 Identifiers: arXiv: 2001.07330
DOI: 10.1063/5.0012723
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Title: The Journal of Chemical Physics
  Other : J. Chem. Phys.
Source Genre: Journal
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Publ. Info: Woodbury, N.Y. : American Institute of Physics
Pages: - Volume / Issue: 153 (10) Sequence Number: 104103 Start / End Page: - Identifier: ISSN: 0021-9606
CoNE: https://pure.mpg.de/cone/journals/resource/954922836226