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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Femtosecond Multiphoton Ionization Photoelectron Spectroscopy of the S_2 State of Phenol
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Femtosecond Multiphoton Ionization Photoelectron Spectroscopy of the S_2 State of Phenol

机译：飞秒的苯酚S_2状态的多光子电离光电子能谱

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摘要

We investigated the short-lived S_2(~1A_1) state of phenol using two-photon resonance-enhanced photoionization coupled with photoelectron spectroscopy. Spectra were obtained by exciting the S_2 state with femtosecond laser pulses at various wavelengths near 207 nm and ionizing with pulses at 207 or 414 nm. The spectra feature a strong transition to the ground electronic state of the ion (X-tilde) and a very weak transition to the first excited electronic state of the ion (A-tilde). In comparison, ionization via the longer-lived S_1 state using 275 nm pulses generates slightly more A-tilde ions. We interpret the relative intensities of the A-tilde state signals as a reflection of configuration interactions in the intermediate S_2 and S_1 states. Time-delayed ionization experiments, as well as experiments with different laser pulse durations, suggest that the S_2 state has a lifetime between 150 and 350 fs. Ionization via S_1 produces a vibrationally resolved photoelectron spectrum, while ionization via S_2 leads to a highly congested spectrum. The envelope of the latter spectrum extends over more than 1 eV and features a long progression, probably in the 6a vibration. This suggests that the S_2 state has a geometrical structure that is displaced from the ground state along the 6a coordinate. No vibrational structure could be resolved in the A-tilde ion spectrum obtained by ionization via either S_2 or S_1.
机译：我们使用双光子共振增强光电离和光电子能谱研究了苯酚的短寿命S_2（〜1A_1）状态。通过用在207 nm附近的各种波长的飞秒激光脉冲激发S_2状态并用207或414 nm的脉冲电离来获得光谱。光谱的特征是离子向基态电子强跃迁（X波浪），离子向第一激发电子态微弱跃迁（A波浪）。相比之下，使用275 nm脉冲通过寿命更长的S_1状态进行电离会产生更多的A倾斜离子。我们将A波浪状态信号的相对强度解释为中间S_2和S_1状态中配置相互作用的反映。延时电离实验以及具有不同激光脉冲持续时间的实验表明，S_2状态的寿命在150至350 fs之间。通过S_1进行电离会产生振动分解的光电子光谱，而通过S_2进行电离会导致光谱高度拥挤。后一个频谱的包络线延伸超过1 eV，并具有很长的传播时间，可能在6a振动中。这表明S_2状态具有沿着6a坐标从基态偏移的几何结构。在通过S_2或S_1电离获得的A-波浪离子光谱中，无法解析振动结构。

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