Water dissociating on rigid Ni(100): A quantum dynamics study on a full-dimensional potential energy surface

doi:10.1063/1.5023069

	Water dissociating on rigid Ni(100): A quantum dynamics study on a full-dimensional potential energy surface
	Zhang, Zhaojun ; Zhang, Dong H.1; Fu, Bina 1; Liu, Tianhui ; Chen, Jun ; Shen, Xiangjian
刊名	JOURNAL OF CHEMICAL PHYSICS
	2018-04-14
卷号	148 期号:14
ISSN号	0021-9606
DOI	10.1063/1.5023069
文献子类	Article
英文摘要	We constructed a nine-dimensional (9D) potential energy surface (PES) for the dissociative chemisorption of H2O on a rigid Ni(100) surface using the neural network method based on roughly 110 000 energies obtained from extensive density functional theory (DFT) calculations. The resulting PES is accurate and smooth, based on the small fitting errors and the good agreement between the fitted PES and the direct DFT calculations. Time dependent wave packet calculations also showed that the PES is very well converged with respect to the fitting procedure. The dissociation probabilities of H2O initially in the ground rovibrational state from 9D quantum dynamics calculations are quite different from the site-specific results from the seven-dimensional (7D) calculations, indicating the importance of full-dimensional quantum dynamics to quantitatively characterize this gas-surface reaction. It is found that the validity of the site-averaging approximation with exact potential holds well, where the site-averaging dissociation probability over 15 fixed impact sites obtained from 7D quantum dynamics calculations can accurately approximate the 9D dissociation probability for H2O in the ground rovibrational state. Published by AIP Publishing.
WOS关键词	CHEMICALLY ACCURATE SIMULATION ; GENERALIZED GRADIENT APPROXIMATION ; AUGMENTED-WAVE METHOD ; MODE SPECIFICITY ; METAL-SURFACES ; REACTIVE SCATTERING ; H-2 DISSOCIATION ; BASIS-SET ; CHEMISORPTION ; CU(111)
WOS研究方向	Chemistry ; Physics
语种	英语
出版者	AMER INST PHYSICS
WOS记录号	WOS:000430128600039
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/169162]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Zhang, Dong H.; Fu, Bina
作者单位	1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, Ctr Theoret & Computat Chem, Dalian 116023, Peoples R China
推荐引用方式 GB/T 7714	Zhang, Zhaojun,Zhang, Dong H.,Fu, Bina,et al. Water dissociating on rigid Ni(100): A quantum dynamics study on a full-dimensional potential energy surface[J]. JOURNAL OF CHEMICAL PHYSICS,2018,148(14).
APA	Zhang, Zhaojun,Zhang, Dong H.,Fu, Bina,Liu, Tianhui,Chen, Jun,&Shen, Xiangjian.(2018).Water dissociating on rigid Ni(100): A quantum dynamics study on a full-dimensional potential energy surface.JOURNAL OF CHEMICAL PHYSICS,148(14).
MLA	Zhang, Zhaojun,et al."Water dissociating on rigid Ni(100): A quantum dynamics study on a full-dimensional potential energy surface".JOURNAL OF CHEMICAL PHYSICS 148.14(2018).