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Issue 3, 2016
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A seven-dimensional quantum dynamics study of the dissociative chemisorption of H2O on Cu(111): effects of azimuthal angles and azimuthal angle-averaging

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Abstract

We report the first seven-dimensional quantum dynamics study for the dissociative chemisorption of H2O on Cu(111) using the time-dependent wave-packet approach, based on an accurate nine-dimensional potential energy surface (PES), which is newly developed by neural network fitting to ∼80 000 density functional theory points. This seven-dimensional quantum model allows the examination of the influence of azimuthal angles and also the investigation of the quantitative relationship between the seven-dimensional (7D) dissociation probabilities and those results calculated by the six-dimensional (6D) model with the flat surface approximation. The reactivity strongly depends on the azimuthal rotations due to different barrier heights. Very large differences are seen between the 7D dissociation probabilities and the 6D results with fixed azimuthal angles, at different fixed sites of impact, indicating that the 6D model by neglecting the azimuthal rotation can introduce substantial errors in calculating dissociation probabilities and the 7D quantum dynamics is essential to investigate the dissociation process. A new azimuthal angle-averaging approach is proposed that the 7D dissociation probability can be well reproduced by averaging 6D results over 18 azimuthal angles, in particular in low kinetic energy regions.

Graphical abstract: A seven-dimensional quantum dynamics study of the dissociative chemisorption of H2O on Cu(111): effects of azimuthal angles and azimuthal angle-averaging

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Article information


Submitted
29 Sep 2015
Accepted
25 Nov 2015
First published
25 Nov 2015

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2016,7, 1840-1845
Article type
Edge Article
Author version available

A seven-dimensional quantum dynamics study of the dissociative chemisorption of H2O on Cu(111): effects of azimuthal angles and azimuthal angle-averaging

T. Liu, Z. Zhang, B. Fu, X. Yang and D. H. Zhang, Chem. Sci., 2016, 7, 1840
DOI: 10.1039/C5SC03689E

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