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Loss of Memory in H + CH4 → H2 + CH3 State-to-State Reactive Scattering

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journal contribution
posted on 17.12.2015, 07:12 by Ralph Welsch, Uwe Manthe
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.