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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Ultrafast photodissociation dynamics of acetone at 195 nm: I. Initial-state, intermediate, and product temporal evolutions by femtosecond mass-selected multiphoton ionization spectroscopy
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Ultrafast photodissociation dynamics of acetone at 195 nm: I. Initial-state, intermediate, and product temporal evolutions by femtosecond mass-selected multiphoton ionization spectroscopy

机译：丙酮在195 nm处的超快光解动力学：I.飞秒质量选择多光子电离光谱法的初始状态，中间过程和产物时间演化

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摘要

The photodissociation dynamics of the acetone S-2 (n, 3s) Rydberg state excited at 195 nm has been studied by using femtosecond pump-probe mass-selected multiphoton ionization spectroscopy. For the first time, the temporal evolutions of the initial state, intermediates, and methyl products were simultaneously measured and analyzed for this reaction to elucidate the complex dynamics. Two mechanisms were considered: (1) the commonly accepted mechanism in which the primary dissociation occurs on the first triplet-state surface, and (2) the recently proposed mechanism in which the primary dissociation takes place on the first singlet-excited-state surface. Our results and analyses supported the validity of the new mechanism. On the other hand, the conventional mechanism was found to be inadequate to describe the observed dynamics. The temporal evolution of methyl products arising from the secondary dissociation of hot acetyl intermediates exhibited a very complex behavior that can be ascribed to the combination of a nonuniform initial vibrational distribution and the competition between dissociation and slow intramolecular vibrational redistribution.
机译：利用飞秒泵浦探针质量选择多光子电离光谱技术研究了在195 nm激发的丙酮S-2（n，3s）Rydberg态的光解动力学。首次同时测量和分析了初始状态，中间体和甲基产物的时间变化，并分析了该反应，以阐明复杂的动力学过程。考虑了两种机理：（1）在第一三重态表面上发生初级解离的普遍接受的机制，以及（2）在第一单重态激发表面上进行初级解离的最近提出的机理。 。我们的结果和分析支持新机制的有效性。另一方面，发现常规机制不足以描述所观察到的动力学。由热的乙酰基中间体的二次解离产生的甲基产物的时间演化表现出非常复杂的行为，这可归因于初始振动分布不均匀以及解离与分子内缓慢振动再分布之间竞争的结合。

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