Nature of the physicochemical process in water photolysis uncovered by a computer simulation

Takeshi Kai; Tomohiro Toigawa; Masatoshi Ukai; Kentaro Fujii; Ritsuko Watanabe; Akinari Yokoya

doi:10.1063/5.0149333

Nature of the physicochemical process in water photolysis uncovered by a computer simulation

J Chem Phys. 2023 Apr 28;158(16):164103. doi: 10.1063/5.0149333.

Authors

Takeshi Kai¹, Tomohiro Toigawa¹, Masatoshi Ukai², Kentaro Fujii³, Ritsuko Watanabe³, Akinari Yokoya³

Affiliations

¹ Nuclear Science and Engineering Center, Japan Atomic Energy Agency, 2-4 Shirane Shirakata, Tokai-mura, Naka-gun, Ibaraki 319-1195, Japan.
² Institute of Engineering, Tokyo University of Agriculture and Technology, Koganei-shi, Tokyo 184-8588, Japan.
³ Institute for Quantum Life Science, National Institutes for Quantum Science and Technology, 2-4 Shirane Shirakata, Tokai-mura, Naka-gun, Ibaraki 319-1195, Japan.

PMID: 37102443
DOI: 10.1063/5.0149333

Abstract

In this work, we investigate the physicochemical process of water photolysis to bridge physical and chemical processes by a newly developed first-principles calculation code. The deceleration, thermalization, delocalization, and initial hydration of the extremely low-energy electrons ejected by water photolysis are sequentially tracked in the condensed phase. We show herein the calculated results for these sequential phenomena during 300 fs. Our results indicate that the mechanisms heavily depend on the intermolecular vibration and rotation modes peculiar to water and the momentum transfer between the electrons and the water medium. We suggest that using our results for the delocalized electron distribution will reproduce successive chemical reactions measured by photolysis experiments using a chemical reaction code. We expect our approach to become a powerful technique for various scientific fields related to water photolysis and radiolysis.