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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >More Protected Vibrational States at the Dissociation Limit of SCCl_2
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More Protected Vibrational States at the Dissociation Limit of SCCl_2

机译：在SCCl_2的解离极限下更多受保护的振动态

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Local vibrational coupling models predict that intramolecular vibrational energy redistribution (IVR) is not completely statistical even at the dissociation limit of polyatomic molecules. Thus states protected from IVR and from rapid dissociation form regular progressions and can be assigned vibrational quantum numbers. We previously observed such regular progressions of states in vibrational spectra of the molecule SCCl_2, but a discrepancy in the density of such states remained between theory and experiment. Here we show that the gap can be closed by observing and assigning additional vibrational transitions above the dissociation limit of SCCl_2, and by carefully analyzing the theoretically expected density of protected states. The newly observed transitions originate from recently assigned and more highly excited vibrational levels in the B? electronic state, connecting to the X? ground state by different Franck?Condon factors. Based on our analysis of Franck?Condon activity, we conclude that theory and experiment agree within measurement uncertainty. Consistency between theory and experiment implies that even more protected states should be observed for larger molecules, leading to nonstatistical dissociation reactions.
机译：局部振动耦合模型预测，即使在多原子分子的解离极限下，分子内振动能量重新分布（IVR）也不完全统计。因此，受IVR保护和免受快速离解的状态会形成规则的过程，并可以分配振动量子数。我们以前在分子SCCl_2的振动光谱中观察到了这种规律的状态演化，但是这种状态的密度在理论和实验之间仍然存在差异。在这里，我们表明，可以通过观察和分配高于SCCl_2的解离极限的其他振动跃迁并仔细分析保护态的理论预期密度，来缩小间隙。新近观察到的跃迁起源于B？中最近分配的和更高激发的振动能级。电子状态，连接到X？基态由不同的Franck？Condon因子决定。根据对弗兰克·康登活性的分析，我们得出结论，理论和实验在测量不确定度内是一致的。理论与实验之间的一致性意味着，对于较大的分子，甚至应观察到更多的保护状态，从而导致非统计解离反应。

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