Loss of Memory in H + CH4 → H2 + CH3 State-to-State Reactive Scattering.
Loss of Memory in H + CH4 → H2 + CH3 State-to-State Reactive Scattering.
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DOI：
10.1021/jz502525p
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发表时间：
2015-01
期刊：
影响因子：
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通讯作者：
R. Welsch;U. Manthe
中科院分区：
文献类型：
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作者：
R. Welsch;U. Manthe
采用多层多组态含时HARTREE方法和量子过渡态概念，通过精确的全维量子动力学计算，计算了H+CH4→H2+CH3反应的态间反应几率.从甲烷反应物的不同振动和转动状态出发，研究了总角动量为零的反应。结果表明，产物的振动态分布与反应物的初始振荡态基本无关。反应产物仅在甲基伞模式下表现出振动激发。在H2或其他CH3振动中未观察到激发。分析结果，观察到的振动记忆丧失可以用基于过渡态的反应过程的观点来解释。
State-to-state reaction probabilities for the H + CH4→ H2 + CH3 reaction are calculated by accurate full-dimensional quantum dynamics calculations employing the multilayer multiconfigurational time-dependent Hartree approach and the quantum transition-state concept. Reactions starting from different vibrational and rotational states of the methane reactant are investigated for vanishing total angular momentum. The vibrational state distributions of the products are found to be essentially independent of the initial rovibrational state of the reactants. The reaction products only show vibrational excitation in the methyl umbrella mode. No excitation in H2 vibration or another CH3 vibration is observed. Analyzing the results, the observed loss of vibrational memory can be explained by a transition-state-based view of the reaction process.