Six-Dimensional Quantum Dynamics of Dissociative Chemisorption

First-principles quantum dynamical theory for the dissociative chemisorption of H2O on rigid Cu(111)

Despite significant progress made in the past decades, it remains extremely challenging to investigate the dissociative chemisorption dynamics of molecular species on surfaces at a full-dimensional quantum mechanical level, in particular for polyatomic-surface reactions. Here we report, to the best of our knowledge, the first full-dimensional quantum dynamics study for the dissociative chemisor...

Quantum theory of dissociative chemisorption on metal surfaces.

Recent theoretical progress in gas-surface reaction dynamics, a field relevant to heterogeneous catalysis, is described. One of the most fundamental reactions, the dissociative chemisorption of H2 on metal surfaces, can now be treated accurately using quantum mechanics. Density functional theory is used to compute the molecule-surface interaction, and the motion of the hydrogen atoms is simulat...

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

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

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 infl...

Quantum dynamics of polyatomic dissociative chemisorption on transition metal surfaces: mode specificity and bond selectivity.

Dissociative chemisorption is the initial and often rate-limiting step in many heterogeneous processes. As a result, an in-depth understanding of the reaction dynamics of such processes is of great importance for the establishment of a predictive model of heterogeneous catalysis. Overwhelming experimental evidence has suggested that these processes have a non-statistical nature and excitations ...