ChemRxiv
These are preliminary reports that have not been peer-reviewed. They should not be regarded as conclusive, guide clinical practice/health-related behavior, or be reported in news media as established information. For more information, please see our FAQs.
VF_Cat_Kinetic_Model_HIURA_ver1.pdf (579.85 kB)
0/0

A Reaction Kinetic Model for Vacuum-Field Catalysis Based on Vibrational Light-Matter Coupling

preprint
submitted on 07.08.2019 and posted on 07.08.2019 by Hidefumi Hiura, Atef Shalabney

Since conventional catalysts are materials-based, they are effective only for particular chemical reactions. Recent studies suggest that vacuum-field catalysis (or cavity catalysis) based on vibrational light-matter coupling can boost reactions without the above constraint. Herein, we propose a reaction kinetic model for such vacuum-field-catalyzed reactions. Vibrational light-matter coupling is an interaction in which a molecular vibration and infrared (IR) vacuum field are coupled in resonance, consequently creating a pair of Rabi-split vibro-polaritonic states. Our kinetic model hypothesizes that vibrational light-matter coupling reshapes the reaction potential surface, thereby changing its reaction barrier height. We translate such a qualitative picture into two kinds of analytical equations derived from the Arrhenius and Eyring–Polanyi theories: both the equations are obtained as a function of the coupling ratio ΩR/2ω0 of vibro-polaritons (ΩR: Rabi frequency between a pair of vibro-polaritons, ω0: vibrational frequency of reactants), indicating that ΩR/2ω0 is a decisive quantity to define the catalytic activity of vacuum-field catalysis. Our numerical calculation shows that when ΩR/2ω0 ≥ 0.1, reactions may be accelerated by several orders of magnitude. Most importantly, our kinetic model can account well for rate enhancements ranging from ~100 to ~104 observed for vacuum-field-catalyzed reactions. We expect that our findings will bring fresh perspectives not only to chemistry but also to the broad fields of science and technology.

History

Email Address of Submitting Author

h-hiura@bq.jp.nec.com

Institution

System Platform Research Laboratories, NEC Corporation

Country

Japan

ORCID For Submitting Author

0000-0001-7141-7354

Declaration of Conflict of Interest

The authors declare competing financial interest: Hidefumi Hiura is employed and funded by NEC Corporation, whereas the other co-author, Atef Shalabney has no competing financial interest.

Version Notes

This manuscript is version 1.

Exports

Logo branding

Exports