HCl dissociating on a rigid Au(111) surface: A six-dimensional quantum mechanical study on a new potential energy surface based on the RPBE functional

	HCl dissociating on a rigid Au(111) surface: A six-dimensional quantum mechanical study on a new potential energy surface based on the RPBE functional
	Fu, Bina 1; Liu, Tianhui ; Zhang, Dong H.1
刊名	JOURNAL OF CHEMICAL PHYSICS
	2017-04-28
卷号	146 期号:16
英文摘要	The dissociative chemisorption of HCl on the Au(111) surface has recently been an interesting and important subject, regarding the discrepancy between the theoretical dissociation probabilities and the experimental sticking probabilities. We here constructed an accurate full-dimensional (sixdimensional (6D)) potential energy surface (PES) based on the density functional theory (DFT) with the revised Perdew-Burke-Ernzerhof (RPBE) functional, and performed 6D quantum mechanical (QM) calculations for HCl dissociating on a rigid Au(111) surface. The effects of vibrational excitations, rotational orientations, and site-averaging approximation on the present RPBE PES are investigated. Due to the much higher barrier height obtained on the RPBE PES than on the PW91 PES, the agreement between the present theoretical and experimental results is greatly improved. In particular, at the very low kinetic energy, the QM-RPBE dissociation probability agrees well with the experimental data. However, the computed QM-RPBE reaction probabilities are still markedly different from the experimental values at most of the energy regions. In addition, the QM-RPBE results achieve good agreement with the recent ab initio molecular dynamics calculations based on the RPBE functional at high kinetic energies. Published by AIP Publishing.
WOS标题词	Science & Technology ; Physical Sciences
类目[WOS]	Chemistry, Physical ; Physics, Atomic, Molecular & Chemical
研究领域[WOS]	Chemistry ; Physics
关键词[WOS]	GENERALIZED GRADIENT APPROXIMATION ; CHEMICALLY ACCURATE SIMULATION ; AUGMENTED-WAVE METHOD ; VIBRATIONAL-EXCITATION ; METAL-SURFACES ; DYNAMICS CALCULATIONS ; TRANSLATIONAL ENERGY ; REACTIVE SCATTERING ; H-2 DISSOCIATION ; MODE SPECIFICITY
收录类别	SCI
语种	英语
WOS记录号	WOS:000400625000026
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/151995]
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
作者单位	1.Chinese Acad Sci, 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	Fu, Bina,Liu, Tianhui,Zhang, Dong H.. HCl dissociating on a rigid Au(111) surface: A six-dimensional quantum mechanical study on a new potential energy surface based on the RPBE functional[J]. JOURNAL OF CHEMICAL PHYSICS,2017,146(16).
APA	Fu, Bina,Liu, Tianhui,&Zhang, Dong H..(2017).HCl dissociating on a rigid Au(111) surface: A six-dimensional quantum mechanical study on a new potential energy surface based on the RPBE functional.JOURNAL OF CHEMICAL PHYSICS,146(16).
MLA	Fu, Bina,et al."HCl dissociating on a rigid Au(111) surface: A six-dimensional quantum mechanical study on a new potential energy surface based on the RPBE functional".JOURNAL OF CHEMICAL PHYSICS 146.16(2017).