Issue 15, 2020

A global ab initio potential energy surface and dynamics of the proton-transfer reaction: OH + D2 → HOD + D

Abstract

We report an accurate full-dimensional potential energy surface (PES) of the anion–molecule system OH3. The PES was constructed by fitting 55 406 ab inito energies from the CCSD(T)/aug-cc-pVTZ level of theory with the fundamental invariant neural network (FI-NN) approach, resulting in an extremely small fitting error of 0.52 meV. Extensive quasiclassical trajectory (QCT) simulations were carried out on the PES to investigate the proton transfer dynamics (OH + D2 → D + HOD). The product D translational energy distribution and angular distribution were calculated and compared with previous experimental measurements, in which reasonably good agreement has been achieved. The angular distribution at a high collision energy exhibits an exclusively forward scattering peak, indicating the direct stripping mechanism at high energies. With the decrease of the collision energy, the reaction shows a predominantly forward scattering feature, with very small sideways and backward scattering amplitudes, revealing combined mechanisms from direct abstraction with a short reaction time and a complex-forming process with a long reaction time.

Graphical abstract: A global ab initio potential energy surface and dynamics of the proton-transfer reaction: OH− + D2 → HOD + D−

Supplementary files

Article information

Article type
Paper
Submitted
08 ⵉⵏⵏ 2020
Accepted
18 ⵎⴰⵕ 2020
First published
25 ⵎⴰⵕ 2020

Phys. Chem. Chem. Phys., 2020,22, 8203-8211

A global ab initio potential energy surface and dynamics of the proton-transfer reaction: OH + D2 → HOD + D

L. Li, B. Fu, X. Yang and D. H. Zhang, Phys. Chem. Chem. Phys., 2020, 22, 8203 DOI: 10.1039/D0CP00107D

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements