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Tracking ultrafast relaxation dynamics of furan by femtosecond photoelectron imaging

机译:飞秒光电子成像跟踪呋喃的超快弛豫动力学

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摘要

Ultrafast internal conversion dynamics of furan has been studied by femtosecond photoelectron imaging (PEI) coupled with photofragmentation (PF) spectroscopy. Photoelectron imaging of single-color multiphoton ionization and two-color pump-probe ionization are obtained and analyzed. Photoelectron bands are assigned to the related states. The time evolution of the photoelectron signal by pump-probe ionization can be well described by a biexponential decay: two rapid relaxation pathways with time constants of similar to 15 fs and 85 (+/- 11) fs. The rapid relaxation is ascribed to the ultrafast internal conversion (IC) from the S-2 state to the vibrationally hot S-1 state. The second relaxation process is attributed to the redistributions and depopulation of secondarily populated high vibronic S-1 state and the formation of alpha-carbene and beta-carbene by H immigration. Additionally, the transient characteristics of the fragment ions are also measured and discussed as a complementary understanding. (C) 2014 Elsevier B.V. All rights reserved.
机译:飞秒光电子成像(PEI)与光碎化(PF)光谱结合研究了呋喃的超快内部转化动力学。获得并分析了单色多光子电离和两色泵浦探针电离的光电子成像。将光电子能带分配给相关状态。光电子信号通过泵浦探针电离的时间演化可以通过双指数衰减来很好地描述:两个快速弛豫路径,其时间常数类似于15 fs和85(+/- 11)fs。快速松弛归因于从S-2状态到振动热S-1状态的超快内部转换(IC)。第二弛豫过程归因于二次填充的高振动S-1状态的重新分布和减少以及H迁移形成的α-卡宾和β-卡宾。此外,还对碎片离子的瞬态特性进行了测量和讨论,以作为补充理解。 (C)2014 Elsevier B.V.保留所有权利。

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