Cavity-Modulated Proton Transfer Reactions

Fabijan Pavosevic, Sharon Hammes-Schiffer, Angel Rubio, Johannes Flick

Research output: Contribution to journalArticlepeer-review

40 Scopus citations

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.

Original languageEnglish (US)
Pages (from-to)4995-5002
Number of pages8
JournalJournal of the American Chemical Society
Volume144
Issue number11
DOIs
StatePublished - Mar 23 2022
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • Catalysis
  • General Chemistry
  • Biochemistry
  • Colloid and Surface Chemistry

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