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Effect of antisymmetric C-H stretching excitation on the dynamics of O(D-1) + CH4 -> OH + CH3
Pan, Huilin1; Yang, Jiayue1; Zhang, Dong1; Shuai, Quan1; Dai, Dongxu1,2; Wu, Guorong1,2; Jiang, Bo1; Yang, Xueming1,2
Source PublicationJOURNAL OF CHEMICAL PHYSICS
2014-04-21
DOI10.1063/1.4871135
Volume140Issue:15
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectPhysics, Atomic, Molecular & Chemical
WOS Research AreaPhysics
WOS KeywordDIFFERENTIAL-CROSS-SECTIONS ; POTENTIAL-ENERGY SURFACE ; BOND-SELECTED REACTION ; BIMOLECULAR REACTIONS ; ATOMIC CHLORINE ; AB-INITIO ; BEND-EXCITATION ; MOLECULAR-BEAM ; REDUCED DIMENSIONALITY ; VIBRATIONAL-EXCITATION
AbstractThe effect of antisymmetric C-H stretching excitation of CH4 on the dynamics and reactivity of the O(D-1) + CH4 -> OH + CD3 reaction at the collision energy of 6.10 kcal/mol has been investigated using the crossed-beam and time-sliced velocity map imaging techniques. The antisymmetric C-H stretching mode excited CH4 molecule was prepared by direct infrared excitation. From the measured images of the CH3 products with the infrared laser on and off, the product translational energy and angular distributions were derived for both the ground and vibrationally excited reactions. Experimental results show that the vibrational energy of the antisymmetric stretching excited CH4 reagent is channeled exclusively into the vibrational energy of the OH co-products and, hence, the OH products from the excited-state reaction are about one vibrational quantum hotter than those from the ground-state reaction, and the product angular distributions are barely affected by the vibrational excitation of the CH4 reagent. The reactivity was found to be suppressed by the antisymmetric stretching excitation of CH4 for all observed CH3 vibrational states. The degree of suppression is different for different CH3 vibrational states: the suppression is about 40%-60% for the ground state and the umbrella mode excited CH3 products, while for the CH3 products with one quantum symmetric stretching mode excitation, the suppression is much less pronounced. In consequence, the vibrational state distribution of the CH3 product from the excited-state reaction is considerably different from that of the ground-state reaction. (C) 2014 AIP Publishing LLC.
Language英语
WOS IDWOS:000336045800016
Citation statistics
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/145717
Collection中国科学院大连化学物理研究所
Affiliation1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Liaoning, Peoples R China
2.Univ Sci & Technol China, Synerget Innovat Ctr Quantum Informat & Quantum P, Hefei 230026, Anhui, Peoples R China
Recommended Citation
GB/T 7714
Pan, Huilin,Yang, Jiayue,Zhang, Dong,et al. Effect of antisymmetric C-H stretching excitation on the dynamics of O(D-1) + CH4 -> OH + CH3[J]. JOURNAL OF CHEMICAL PHYSICS,2014,140(15).
APA Pan, Huilin.,Yang, Jiayue.,Zhang, Dong.,Shuai, Quan.,Dai, Dongxu.,...&Yang, Xueming.(2014).Effect of antisymmetric C-H stretching excitation on the dynamics of O(D-1) + CH4 -> OH + CH3.JOURNAL OF CHEMICAL PHYSICS,140(15).
MLA Pan, Huilin,et al."Effect of antisymmetric C-H stretching excitation on the dynamics of O(D-1) + CH4 -> OH + CH3".JOURNAL OF CHEMICAL PHYSICS 140.15(2014).
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