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Updated: Jun 26, 2025

Multiscale Sampling of a Heterogeneous Water/Metal Catalyst Interface using Density Functional Theory and Force-Field Molecular Dynamics
Published on: April 12, 2019
Six-dimensional quantum dynamics of an Eley-Rideal reaction between gaseous and adsorbed hydrogen atoms on Cu(111)
Longlong Xiong1, Liang Zhang1, Bin Zhao2
1Department of Chemical Physics, Key Laboratory of Precision and Intelligent Chemistry, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, University of Science and Technology of China, Hefei, Anhui 230026, China. bjiangch@ustc.edu.cn.
Abstract:
In the form of direct abstraction of a surface adsorbate by a gaseous projectile, the Eley-Rideal (ER) reaction at the gas-surface interface manifests interesting dynamics. Unfortunately, high-dimensional quantum dynamical (QD) studies for ER reactions remain very challenging, which demands a large configuration space and the coordinate transformation of wavefunctions. Here, we report the first six-dimensional (6D) fully coupled quantum scattering method for studying the ER reaction between gas phase H(D) atoms and adsorbed D(H) atoms on a rigid Cu(111) surface. Reaction probabilities and product rovibrational state distributions obtained by this 6D model are found to be quite different from those obtained by reduced-dimensional QD models, demonstrating the high-dimensional nature of the ER reaction. Using two distinct potential energy surfaces (PESs), we further discuss the influence of the PES on the calculated product vibrational and rotational state distributions, in comparison with experimental results. The lateral corrugation and the exothermicity of the PES are found to play a critical role in controlling the energy disposal in the ER reaction.
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