Hydrogen atom scattering on metal surfaces is investigated based on a simplified Newns–Anderson model. Both the nuclear and electronic degrees of freedom are treated quantum mechanically. By partitioning all the surface electronic states as the bath, the hierarchical equations of motion method for the fermionic bath is employed to simulate the scattering dynamics. It is found that, with a reasonable set of parameters, the main features of the recent experimental studies of hydrogen atom scattering on metal surfaces can be reproduced. Vibrational states on the chemisorption state whose energies are close to the incident energy are found to play an important role, and the scattering process is dominated by a single-pass electronic transition forth and back between the diabatic physisorption and chemisorption states. Further study on the effects of the atom-surface coupling strength reveals that, upon increasing the atom-surface coupling strength, the scattering mechanism changes from typical nonadiabatic transitions to dynamics in the electronic friction regime.
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28 July 2023
Research Article|
July 24 2023
Theoretical study of nonadiabatic hydrogen atom scattering dynamics on metal surfaces using the hierarchical equations of motion method
Xiaohan Dan
;
Xiaohan Dan
(Investigation, Methodology, Software, Writing – original draft, Writing – review & editing)
Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences
, Zhongguancun, Beijing 100190, China
and University of Chinese Academy of Sciences
, Beijing 100049, China
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Qiang Shi
Qiang Shi
a)
(Conceptualization, Funding acquisition, Investigation, Methodology, Software, Supervision, Writing – original draft, Writing – review & editing)
Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences
, Zhongguancun, Beijing 100190, China
and University of Chinese Academy of Sciences
, Beijing 100049, China
a)Author to whom correspondence should be addressed: qshi@iccas.ac.cn
Search for other works by this author on:
a)Author to whom correspondence should be addressed: qshi@iccas.ac.cn
J. Chem. Phys. 159, 044101 (2023)
Article history
Received:
April 18 2023
Accepted:
June 30 2023
Citation
Xiaohan Dan, Qiang Shi; Theoretical study of nonadiabatic hydrogen atom scattering dynamics on metal surfaces using the hierarchical equations of motion method. J. Chem. Phys. 28 July 2023; 159 (4): 044101. https://doi.org/10.1063/5.0155172
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