Lattice effects of surface cell: Multilayer multiconfiguration time-dependent Hartree study on surface scattering of CO/Cu(100)

doi:10.1063/1.4982962

	Lattice effects of surface cell: Multilayer multiconfiguration time-dependent Hartree study on surface scattering of CO/Cu(100)
	Meng, Qingyong 2,3; Meyer, Hans-Dieter 1
刊名	JOURNAL OF CHEMICAL PHYSICS
	2017-05-14
卷号	146
DOI	10.1063/1.4982962
英文摘要	To study the scattering of CO off a movable Cu(100) surface, extensive multilayer multiconfiguration time-dependent Hartree (ML-MCTDH) calculations are performed based on the SAP [R. Marquardt et al., J. Chem. Phys. 132, 074108 (2010)] potential energy surface in conjunction with a recently developed expansion model [Q. Meng and H.-D. Meyer, J. Chem. Phys. 143, 164310 (2015)] for including lattice motion. The surface vibration potential is constructed by a sum of Morse potentials where the parameters are determined by simulating the vibrational energies of a clean Cu(100) surface. Having constructed the total Hamiltonian, extensive dynamical calculations in both time-independent and time-dependent schemes are performed. Two-layer MCTDH (i.e., normal MCTDH) block-improved-relaxations (time-independent scheme) show that increasing the number of included surface vibrational dimensions lets the vibrational energies of CO/Cu(100) decrease for the frustrated translation (T mode), which is of low energy but increase those of the frustrated rotation (R mode) and the CO-Cu stretch (S mode), whose vibrational energies are larger than the energies of the in-plane surface vibrations (similar to 79 cm(-1)). This energy-shifting behavior was predicted and discussed by a simple model in our previous publication [Q. Meng and H.-D. Meyer, J. Chem. Phys. 143, 164310 (2015)]. By the flux analysis of the MCTDH/ML-MCTDH propagated wave packets, we calculated the sticking probabilities for the X + 0D, X + 1D, X + 3D, X + 5D, and X + 15D systems, where "X" stands for the used dimensionality of the CO/rigid-surface system and the second entry denotes the number of surface degrees of freedom included. From these sticking probabilities, the X + 5D/15D calculations predict a slower decrease of sticking with increasing energy as compared to the sticking of the X + 0D/1D/3D calculations. This is because the translational energy of CO is more easily transferred to surface vibrations, when the vibrational dimensionality of the surface is enlarged. Published by AIP Publishing.
语种	英语
WOS记录号	WOS:000401368900018
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/152277]
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.Heidelberg Univ, Theoret Chem, Phys Chem Inst, Neuenheimer Feld 229, D-69120 Heidelberg, Germany 2.Chinese Acad Sci, State Key Lab Mol React Dynam, Dalian Inst Chem Phys, Zhongshan Rd 457, Dalian 116023, Peoples R China 3.Northwestern Polytech Univ, Dept Appl Chem, Youyi West Rd 127, Xian 710072, Peoples R China
推荐引用方式 GB/T 7714	Meng, Qingyong,Meyer, Hans-Dieter. Lattice effects of surface cell: Multilayer multiconfiguration time-dependent Hartree study on surface scattering of CO/Cu(100)[J]. JOURNAL OF CHEMICAL PHYSICS,2017,146.
APA	Meng, Qingyong,&Meyer, Hans-Dieter.(2017).Lattice effects of surface cell: Multilayer multiconfiguration time-dependent Hartree study on surface scattering of CO/Cu(100).JOURNAL OF CHEMICAL PHYSICS,146.
MLA	Meng, Qingyong,et al."Lattice effects of surface cell: Multilayer multiconfiguration time-dependent Hartree study on surface scattering of CO/Cu(100)".JOURNAL OF CHEMICAL PHYSICS 146(2017).