Mode specificity for the dissociative chemisorption of H2O on Cu(111): a quantum dynamics study on an accurately fitted potential energy surface

doi:10.1039/c6cp00034g

	Mode specificity for the dissociative chemisorption of H2O on Cu(111): a quantum dynamics study on an accurately fitted potential energy surface
	Liu, Tianhui 1,2,3; Zhang, Zhaojun 1,2; Fu, Bina 1,2; Yang, Xueming 1,2,3; Zhang, Dong H.1,2
刊名	PHYSICAL CHEMISTRY CHEMICAL PHYSICS
	2016-03-28
卷号	18 期号:12 页码:8537-8544
ISSN号	1463-9076
DOI	10.1039/c6cp00034g
文献子类	Article
英文摘要	The mode-specific dynamics for the dissociative chemisorption of H2O on Cu(111) is first investigated by seven-dimensional quantum dynamics calculations, based on an accurately fitted potential energy surface (PES) recently developed by neural network fitting to DFT energy points. It is indicated that excitations in all three vibrational modes have a significant impact on reactivity, which are more efficacious than increasing the translational energy in promoting the reaction, with the largest enhancement for the excitation in the asymmetric stretching mode. There is large discrepancy between the six-dimensional reactivities with fixed azimuthal angles and seven-dimensional results, revealing that the 6D "flat surface" model cannot accurately characterize the reaction dynamics. The azimuthal angle-averaging approach is validated for vibrational excited states of the reactant, where the 7D mode-specific probability can be well reproduced by averaging the 6D azimuthal angle-fixed probabilities over 18 angles.
WOS关键词	GENERALIZED GRADIENT APPROXIMATION ; WAVE BASIS-SET ; HYDROGEN-ATOMS ; METAL-SURFACES ; BOND ; MOLECULES ; WATER ; METHANE ; NI(100) ; SELECTIVITY
WOS研究方向	Chemistry ; Physics
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000372249100024
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/170980]
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.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 3.Univ Sci & Technol China, Dept Chem Phys, Hefei 230026, Peoples R China
推荐引用方式 GB/T 7714	Liu, Tianhui,Zhang, Zhaojun,Fu, Bina,et al. Mode specificity for the dissociative chemisorption of H2O on Cu(111): a quantum dynamics study on an accurately fitted potential energy surface[J]. PHYSICAL CHEMISTRY CHEMICAL PHYSICS,2016,18(12):8537-8544.
APA	Liu, Tianhui,Zhang, Zhaojun,Fu, Bina,Yang, Xueming,&Zhang, Dong H..(2016).Mode specificity for the dissociative chemisorption of H2O on Cu(111): a quantum dynamics study on an accurately fitted potential energy surface.PHYSICAL CHEMISTRY CHEMICAL PHYSICS,18(12),8537-8544.
MLA	Liu, Tianhui,et al."Mode specificity for the dissociative chemisorption of H2O on Cu(111): a quantum dynamics study on an accurately fitted potential energy surface".PHYSICAL CHEMISTRY CHEMICAL PHYSICS 18.12(2016):8537-8544.