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  Cavity-Modulated Proton Transfer Reactions

Pavošević, F., Hammes-Schiffer, S., Rubio, A., & Flick, J. (2022). Cavity-Modulated Proton Transfer Reactions. Journal of the American Chemical Society, 144(11), 4995-5002. doi:10.1021/jacs.1c13201.

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Theoretical background; computational details; estimation of the molecular volume; Rabi-splitting for different electron-photon coupling strengths; energy barrier calculated on HF optimized geometries; energy contributions breakdown; energy barrier dependence on the cavity frequency; Cartesian coordinates of the optimized geometries (PDF); Text file containing python code (TXT)
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https://arxiv.org/abs/2112.02138 (Preprint)
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 Creators:
Pavošević, F.1, Author
Hammes-Schiffer, S.2, Author
Rubio, A.1, 3, 4, 5, Author              
Flick, J.1, Author
Affiliations:
1Center for Computational Quantum Physics, Flatiron Institute, ou_persistent22              
2Department of Chemistry, Yale University, ou_persistent22              
3Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
4Center for Free-Electron Laser Science, ou_persistent22              
5Nano-Bio Spectroscopy Group and European Theoretical Spectroscopy Facility (ETSF), Universidad del Paìs Vasco (UPV/EHU), ou_persistent22              

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 Abstract: Proton transfer is ubiquitous in many fundamental chemical and biological processes, and the ability to modulate and control the proton transfer rate would have a major impact on numerous quantum technological advances. One possibility to modulate the reaction rate of proton transfer processes is given by exploiting the strong light-matter coupling of chemical systems inside optical or nanoplasmonic cavities. In this work, we investigate the proton transfer reactions in the prototype malonaldehyde and Z-3-amino-propenal (aminopropenal) molecules using different quantum electrodynamics methods, in particular, quantum electrodynamics coupled cluster theory and quantum electrodynamical density functional theory. Depending on the cavity mode polarization direction, we show that the optical cavity can increase the reaction energy barrier by 10–20% or decrease the reaction barrier by ∼5%. By using first-principles methods, this work establishes strong light-matter coupling as a viable and practical route to alter and catalyze proton transfer reactions.

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Language(s): eng - English
 Dates: 2021-12-152022-03-102022-03-23
 Publication Status: Published in print
 Pages: 8
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: arXiv: 2112.02138
DOI: 10.1021/jacs.1c13201
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Project name : We acknowledge financial support from the European Research Council (ERC-2015-AdG-694097), Grupos Consolidados (IT1249-19), the Cluster of Excellence ‘CUI: Advanced Imaging of Matter’ of the Deutsche Forschungsgemeinschaft (DFG) - EXC 2056 - project ID 390715994 [...].
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Title: Journal of the American Chemical Society
  Other : JACS
  Abbreviation : J. Am. Chem. Soc.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 144 (11) Sequence Number: - Start / End Page: 4995 - 5002 Identifier: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870