A seven-dimensional quantum dynamics study of the dissociative chemisorption of H2O on Cu(111): effects of azimuthal angles and azimuthal angle-averaging

doi:10.1039/c5sc03689e

	A seven-dimensional quantum dynamics study of the dissociative chemisorption of H2O on Cu(111): effects of azimuthal angles and azimuthal angle-averaging
	Liu, Tianhui 1,2,3; Zhang, Zhaojun 2,3; Fu, Bina 2,3; Yang, Xueming 1,2,3; Zhang, Dong H.2,3
刊名	CHEMICAL SCIENCE
	2016
卷号	7 期号:3 页码:1840-1845
ISSN号	2041-6520
DOI	10.1039/c5sc03689e
文献子类	Article
英文摘要	We report the first seven-dimensional quantum dynamics study for the dissociative chemisorption of H2O on Cu(111) using the time-dependent wave-packet approach, based on an accurate nine-dimensional potential energy surface (PES), which is newly developed by neural network fitting to similar to 80 000 density functional theory points. This seven-dimensional quantum model allows the examination of the influence of azimuthal angles and also the investigation of the quantitative relationship between the seven-dimensional (7D) dissociation probabilities and those results calculated by the six-dimensional (6D) model with the flat surface approximation. The reactivity strongly depends on the azimuthal rotations due to different barrier heights. Very large differences are seen between the 7D dissociation probabilities and the 6D results with fixed azimuthal angles, at different fixed sites of impact, indicating that the 6D model by neglecting the azimuthal rotation can introduce substantial errors in calculating dissociation probabilities and the 7D quantum dynamics is essential to investigate the dissociation process. A new azimuthal angle-averaging approach is proposed that the 7D dissociation probability can be well reproduced by averaging 6D results over 18 azimuthal angles, in particular in low kinetic energy regions.
WOS关键词	CHEMICALLY ACCURATE SIMULATION ; SURFACE REACTIVITY ; NI(100) ; H-2 ; METHANE ; ENERGY ; CH4 ; EXCITATION ; ADSORPTION ; SCATTERING
WOS研究方向	Chemistry
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000371021900023
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/171032]
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	Fu, Bina; Zhang, Dong H.
作者单位	1.Univ Sci & Technol China, Dept Chem Phys, Hefei 230026, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China 3.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	Liu, Tianhui,Zhang, Zhaojun,Fu, Bina,et al. A seven-dimensional quantum dynamics study of the dissociative chemisorption of H2O on Cu(111): effects of azimuthal angles and azimuthal angle-averaging[J]. CHEMICAL SCIENCE,2016,7(3):1840-1845.
APA	Liu, Tianhui,Zhang, Zhaojun,Fu, Bina,Yang, Xueming,&Zhang, Dong H..(2016).A seven-dimensional quantum dynamics study of the dissociative chemisorption of H2O on Cu(111): effects of azimuthal angles and azimuthal angle-averaging.CHEMICAL SCIENCE,7(3),1840-1845.
MLA	Liu, Tianhui,et al."A seven-dimensional quantum dynamics study of the dissociative chemisorption of H2O on Cu(111): effects of azimuthal angles and azimuthal angle-averaging".CHEMICAL SCIENCE 7.3(2016):1840-1845.