Six-dimensional quantum dynamics of an Eley-Rideal reaction between gaseous and adsorbed hydrogen atoms on Cu(111)

Xiong, Longlong1; Zhang, Liang1; Zhao, Bin2; Jiang, Bin1,3

2024-05-01

10.1039/d3fd00163f

FARADAY DISCUSSIONS   影响因子和分区

1359-6640

1364-5498

["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.","We report the first six-dimensional (6D) fully coupled quantum scattering method for studying the Eley-Rideal reaction between gas phase H(D) atoms and adsorbed D(H) atoms on a rigid Cu(111) surface."]

SCI ; EI

英语

通讯

National Natural Science Foundation of China[2021ZD0303301] ; Innovation Program for Quantum Science and Technology[XDB0450101] ; Strategic Priority Research Program of the Chinese Academy of Sciences["22325304","22073089","22241301"]

Chemistry

Chemistry, Physical

WOS:001224829900001

ROYAL SOC CHEMISTRY

CHEMISTRY

Web of Science

1.Univ Sci & Technol China, Key Lab Surface & Interface Chem & Energy Catalysi, Dept Chem Phys, Key Lab Precis & Intelligent Chem, Hefei 230026, Anhui, Peoples R China
2.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
3.Univ Sci & Technol China, Hefei Natl Lab, Hefei 230088, Peoples R China

Xiong, Longlong,Zhang, Liang,Zhao, Bin,et al. Six-dimensional quantum dynamics of an Eley-Rideal reaction between gaseous and adsorbed hydrogen atoms on Cu(111)[J]. FARADAY DISCUSSIONS,2024.

Xiong, Longlong,Zhang, Liang,Zhao, Bin,&Jiang, Bin.(2024).Six-dimensional quantum dynamics of an Eley-Rideal reaction between gaseous and adsorbed hydrogen atoms on Cu(111).FARADAY DISCUSSIONS.

Xiong, Longlong,et al."Six-dimensional quantum dynamics of an Eley-Rideal reaction between gaseous and adsorbed hydrogen atoms on Cu(111)".FARADAY DISCUSSIONS (2024).