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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Femtosecond Resonance-Enhanced Multiphoton Ionization of Perylene in Hexane. Electronic Excitation of the Radical Cation and Evidence of Hydrogen Abstraction from the Solvent
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Femtosecond Resonance-Enhanced Multiphoton Ionization of Perylene in Hexane. Electronic Excitation of the Radical Cation and Evidence of Hydrogen Abstraction from the Solvent

机译：飞秒共振增强Per烷中Multi的多光子电离。自由基阳离子的电子激发和从溶剂中提取氢的证据

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摘要

We demonstrate that perylene in solution can be highly excited with relatively weak femtosecond radiation via two-photon resonance-enhanced multiphoton ionization and excitation. The femtosecond multiphoton excitation spectra of two different observables are presented for perylene dissolved in hexane. The first of these is the normal S_1 → S_0 fluorescence that arises from relaxation of perylene through the singlet manifold after multiphoton excitation. The second observable is the ion yield that results from multiphoton ionization. A comparison of these two excitation spectra is presented, and their striking similarity indicates that both processes occur via the same initial two-photon resonance in the 500-550 nm region. A mechanism is presented illustrating the predicted excitation and relaxation pathways. The multiphoton-excited emission spectrum of the sample exhibits anomalous emission in the 550-620 nm range. Comparison of this emission with the one-photon-excited emission spectrum of perylene in concentrated sulfuric acid shows that the anomalous emission originates from electronic excitation of cationic species present in sulfuric acid. Previous assignment of emission from perylene dissolved in sulfuric acid to the protonated cation implies that the perylene radical cation in hexane abstracts a hydrogen atom from the solvent on an ultrafast time scale.
机译：我们证明溶液中的per可以通过相对较弱的飞秒辐射通过双光子共振增强的多光子电离和激发而被高度激发。给出了溶解在己烷中的per的两个不同观测值的飞秒多光子激发光谱。第一个是正常的S_1→S_0荧光，该荧光是由于多光子激发后of通过单重态歧管的弛豫而产生的。第二个可观察到的是多光子电离产生的离子产率。给出了这两个激发光谱的比较，它们惊人的相似性表明这两个过程都是通过相同的初始双光子共振在500-550 nm区域发生的。提出了一种机制，说明了预测的激发和弛豫途径。样品的多光子激发发射光谱在550-620 nm范围内显示异常发射。将该发射光谱与浓硫酸中per的单光子激发发射光谱进行比较，表明异常发射源自硫酸中存在的阳离子物种的电子激发。从溶解在硫酸中的per到质子化阳离子的发射的先前分配意味着在己烷中的per自由基阳离子在超快的时间尺度上从溶剂中提取氢原子。

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