A full-dimensional time-dependent wave packet study of the OH+CO -> H+CO2 reaction

	A full-dimensional time-dependent wave packet study of the OH+CO -> H+CO2 reaction
	Liu, Shu 1,2; Xu, Xin 1,2; Zhang, Dong H.1,2
刊名	theoretical chemistry accounts
	2012
卷号	131 期号:1
关键词	Complex-forming reactions Quantum scattering Reaction resonance Time-dependent wave packet method
英文摘要	full-dimensional time-dependent wave packet calculations were made to study the oh + co -> h + co2 reaction on the lakin-troya-schatz-harding potential energy surface. because of the presence of deep wells supporting long-lived collision complex, one needs to propagate the wave packet up to 450,000 a.u. of time to fully converge the total reaction probabilities. our calculation revealed that the co bond was substantially excited vibrationally in the complex wells, making it necessary to include sufficient co vibration basis functions to yield quantitatively accurate results for the reaction. we calculated the total reaction probabilities from the ground initial state and two vibrationally excited states for the total angular momentum j = 0. the total reaction probability for the ground initial state is quite small in magnitude with many narrow and overlapping resonances due to the small complex-formation reaction probability and small probability for complex decaying into product channel. initial oh vibrational excitation considerably enhances the reactivity because it enhances the probability for complex decaying into product channel, while initial co excitation has little effects on the reactivity. we also calculated the reaction probabilities for a number of j > 0 states by using the centrifugal sudden approximation. by doing some calculations with multiple k-blocks included, we found that the centrifugal sudden approximation can be employed to calculate the rate constant for the reaction rather accurately. the calculated rate constants only agree with experimental measurements qualitatively, suggesting more theoretical studies be carried out for this prototypical complex-formation four-atom reaction.
WOS标题词	science & technology ; physical sciences
类目[WOS]	chemistry, physical
研究领域[WOS]	chemistry
关键词[WOS]	integral cross-sections ; diatom-diatom reactions ; h-2+oh reaction ; oh plus ; co ; complex ; energy ; distributions ; temperature ; kinetics
收录类别	SCI
语种	英语
WOS记录号	WOS:000300213700018
公开日期	2015-11-17
内容类型	期刊论文
源URL	[http://159.226.238.44/handle/321008/142963]
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, 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	Liu, Shu,Xu, Xin,Zhang, Dong H.. A full-dimensional time-dependent wave packet study of the OH+CO -> H+CO2 reaction[J]. theoretical chemistry accounts,2012,131(1).
APA	Liu, Shu,Xu, Xin,&Zhang, Dong H..(2012).A full-dimensional time-dependent wave packet study of the OH+CO -> H+CO2 reaction.theoretical chemistry accounts,131(1).
MLA	Liu, Shu,et al."A full-dimensional time-dependent wave packet study of the OH+CO -> H+CO2 reaction".theoretical chemistry accounts 131.1(2012).