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利用纳秒和飞秒激光及飞行时间质谱仪对氮化苯 溶剂分子团簇的多光子电离和离解进行了研究。通过解决实验中的技术难题,实现了在气相条件下实验研究嘧啶与水团簇的多光子电离。首次观测到该团簇的多光子电离质谱,发现电离后形成了质子化团簇系列,通过团簇浓度随激光强度的变化以及理论计算,阐明了团簇内质子转移过程,以及电荷分布和质子转移过程随着团簇尺寸的变化;首次观测到吡啶团簇在飞秒光电离过程中的质子化和非质子化团簇离子共存的现象。非质子化吡啶二聚体离子的存在及高水平下理论计算表明,吡啶分子之间可以形成C -H N氢键,对文献中报道的结果给予了纠正,提供了弱氢键团簇中质子转移的一个极佳范例;首次研究并获得了嘧啶 甲醇以及哒嗪 甲醇氢键团簇的多光子实验研究结果.实验发现团簇经激光电离后只产生质子化产物,并从理论计算得到各种团簇的稳定构型,阐明了团簇发生电离后质子转移反应的过程和机理
The multi-photon ionization and dissociation of the molecular clusters of nitrobenzene solvent were investigated using nanosecond and femtosecond laser and time-of-flight mass spectrometry. By solving the technical problems in the experiment, the experimental study of multiphoton ionization of pyrimidine and water clusters in gas phase has been achieved. For the first time, the multi-photon ionization mass spectrometry of this cluster was observed and it was found that a series of protonated clusters were formed after ionization. Through the variation of cluster concentration with laser intensity and theoretical calculation, the intramolecular proton transfer process as well as the charge distribution and proton The change of cluster size with the change of cluster size was observed for the first time. The coexistence of protonated and unprotonated cluster ions in pyridine ionization was observed for the first time. The existence of non-protonated pyridine dimer ions and theoretical calculations at high levels show that C-HHN hydrogen bonds can be formed between the pyridine molecules, correcting the reported results in the literature, providing proton transfer in weakly hydrogen-bonded clusters For the first time and obtained the pyrimidine methanol and pyridazine methanol hydrogen bonding clusters of multi-photon experimental results show that the cluster generated by laser ionization only protonated products, and calculated from the theoretical group of various groups The stability of the cluster configuration, elucidation of cluster ionization proton transfer reaction process and mechanism