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学科主题: 物理化学
题名: Reactivity Inhibitation by Antisymmetric Stretching Excitation in Dual-mechanism Reaction O(1D)+CH4
作者: Pan HL(潘慧琳) ;  Shuai Q(帅全) ;  Yang JY(杨家岳) ;  Zhang D(张冬) ;  Jiang B(姜波) ;  Dai DX(戴东旭) ;  Yang XM(杨学明)
会议文集: Conference on Molecular Energy Transfer 2011 Book of abstracts
会议名称: International Conference on Molecular Energy Transfer 2011
会议日期: 2011-09-11
出版日期: 2011
会议地点: 牛津
其他题名: CH4的非对称伸缩振动激发对双重机理反应O(1D)+CH4反应性的抑制
通讯作者: 杨学明
出版者: 待补充
出版地: 待补充
合作性质: 墙报
部门归属: 1102
主办者: 英国牛津大学
摘要: Different forms of energy play distinct roles in chemical reactions1. How does the additional vibrational energy of the reactant work along the reaction coordinate? This problem is extremely important in understanding details of reaction dynamics. Accordingly, we performed a series of cross-beam experiments of the dual-mechanism reaction O(1D)+CH4(ν3=0, 1)→OH+CH3, on a newly-built time-sliced ion velocity imaging machine2 at collision energies ranging from 3.23 to 6.70 kcal/mol. One of the reaction products CH3 was state-selectively detected using a (2+1) resonance-enhanced multiphoton ionization(REMPI) technique3. To everyone’s surprise, channels producing , , states of product CH3 were completely depleted by the reactant vibrational excitation, while the / path exposed less depletion. It means the antisymmetric stretching excitation of reactant CH4 not only exhibits no promotion to the reaction, but also restrains the rupture of the excited bond. In other words, it hinders the overall cross section of the title reaction. This finding furthers our understanding of polyatomic reactions, and requires more experimental and theoretical works on corresponding reaction dynamics.
英文摘要: Different forms of energy play distinct roles in chemical reactions1. How does the additional vibrational energy of the reactant work along the reaction coordinate? This problem is extremely important in understanding details of reaction dynamics. Accordingly, we performed a series of cross-beam experiments of the dual-mechanism reaction O(1D)+CH4(ν3=0, 1)→OH+CH3, on a newly-built time-sliced ion velocity imaging machine2 at collision energies ranging from 3.23 to 6.70 kcal/mol. One of the reaction products CH3 was state-selectively detected using a (2+1) resonance-enhanced multiphoton ionization(REMPI) technique3. To everyone’s surprise, channels producing , , states of product CH3 were completely depleted by the reactant vibrational excitation, while the / path exposed less depletion. It means the antisymmetric stretching excitation of reactant CH4 not only exhibits no promotion to the reaction, but also restrains the rupture of the excited bond. In other words, it hinders the overall cross section of the title reaction. This finding furthers our understanding of polyatomic reactions, and requires more experimental and theoretical works on corresponding reaction dynamics.
内容类型: 会议论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/115965
Appears in Collections:中国科学院大连化学物理研究所_会议论文

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Recommended Citation:
Pan HL,Shuai Q,Yang JY,et al. Reactivity Inhibitation by Antisymmetric Stretching Excitation in Dual-mechanism Reaction O(1D)+CH4[C]. 见:International Conference on Molecular Energy Transfer 2011. 牛津. 2011-09-11.
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