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Mode specificity of water dissociating on Ni(100): An approximate full-dimensional quantum dynamics study

The mode-specific dynamics for the dissociative chemisorption of H2O on rigid Ni(100) is investigated by approximate nine-dimensional (9D) quantum dynamics calculations. The vibrational state-specific 9D dissociation probabilities are obtained by site-averaging the site-specific seven-dimensional re...

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Published in:The Journal of chemical physics 2023-06, Vol.158 (21)
Main Authors: Liu, Tianhui, Fu, Bina, Zhang, Dong H.
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Language:English
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description The mode-specific dynamics for the dissociative chemisorption of H2O on rigid Ni(100) is investigated by approximate nine-dimensional (9D) quantum dynamics calculations. The vibrational state-specific 9D dissociation probabilities are obtained by site-averaging the site-specific seven-dimensional results based on an accurate full-dimensional potential energy surface newly developed by neural network fitting to density functional theory energy points with the revised version of the Perdew, Burke, and Ernzerhof functional. The mode specificity of H2O/Ni(100) is very different from that of H2O/Ni(111) or H2O/Cu(111) whose reactivity enhancement by vibrational excitations is quite efficient. For H2O/Ni(100), it is found that the excitation in the symmetric stretching mode is more efficacious than increasing the translational energy in promoting the reaction, while the excitations in the asymmetric stretching mode and bending mode are less efficacious than the translational energy at low collision energies. These interesting observations can be attributed to the near central-barrier reaction for H2O/Ni(100), as well as large discrepancies between the site-specific mode specificities at different impact sites. The mode-specific dynamics obtained in this study is different from that obtained with the reaction path Hamiltonian approach, indicating the importance of full-dimensional quantum dynamics for gas–surface reactions.
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These interesting observations can be attributed to the near central-barrier reaction for H2O/Ni(100), as well as large discrepancies between the site-specific mode specificities at different impact sites. 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These interesting observations can be attributed to the near central-barrier reaction for H2O/Ni(100), as well as large discrepancies between the site-specific mode specificities at different impact sites. The mode-specific dynamics obtained in this study is different from that obtained with the reaction path Hamiltonian approach, indicating the importance of full-dimensional quantum dynamics for gas–surface reactions.</abstract><cop>United States</cop><pub>American Institute of Physics</pub><pmid>37272570</pmid><doi>10.1063/5.0153538</doi><tpages>7</tpages><orcidid>https://orcid.org/0000-0001-6011-9263</orcidid><orcidid>https://orcid.org/0000-0003-1568-0259</orcidid><orcidid>https://orcid.org/0000-0001-9426-8822</orcidid><oa>free_for_read</oa></addata></record>
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source American Institute of Physics:Jisc Collections:Transitional Journals Agreement 2021-23 (Reading list); AIP_美国物理联合会现刊(与NSTL共建)
subjects Chemisorption
Density functional theory
Excitation
Hamiltonian functions
Neural networks
Physics
Potential energy
Quantum theory
Stretching
Surface reactions
Vibrational states
title Mode specificity of water dissociating on Ni(100): An approximate full-dimensional quantum dynamics study
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