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首页> 外文期刊>The Journal of Chemical Physics >The ejection of triatomic molecular hydrogen ions H_3~+ produced by the interaction of benzene molecules with ultrafast laser pulses
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The ejection of triatomic molecular hydrogen ions H_3~+ produced by the interaction of benzene molecules with ultrafast laser pulses

机译：苯分子与超快激光脉冲相互作用产生的三原子分子氢离子H_3〜+的喷射

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摘要

The ejection process of triatomic molecular hydrogen ions produced by the interaction of benzene with ultrafast laser pulses of moderate strong intensity (～10~(14) W/cm~2) is studied by means of TOF mass spectrometry. The H_3~+ formation can only take place through the rupture of two C–H bonds and the migration of hydrogen atoms within the molecular structure. The H_3~+ fragments are released with high kinetic energy (typically 2–8 eV) and at laser intensities ≥10~(14) W/cm~2, well above that required for the double ionization of benzene, suggesting that its formation is taking place within multiply charged parent ions. The relative ejection efficiency of H_3~+ molecular hydrogen ions with respect to the atomic ones is found to be strongly decreasing as a function of the laser intensity and pulse duration (67–25 fs). It is concluded that the H_3~+ formation is only feasible within parent molecular precursors of relatively low charged states and before significant elongation of their structure takes place, while the higher multiply charged molecular ions preferentially dissociate into H~+ ions. The ejection of H_2~+ ions is also discussed in comparison to the production of H_3~+ and H~+ions. Finally, by recording the mass spectra of two deuterium label isotopes of benzene (1,2-C_6H_4D_2, 1,4-C_6H_4D_2) it is verified that the ejection efficiency of some molecular fragments,such as D_2H~+, DH~+, is dependent on the specific position of hydrogen atoms in the molecular skeleton prior dissociation.
机译：通过TOF质谱研究了苯与中等强度（〜10〜（14）W / cm〜2）的超快激光脉冲相互作用产生的三原子分子氢离子的喷射过程。 H_3〜+的形成只能通过两个C–H键的断裂以及分子结构内氢原子的迁移来实现。 H_3〜+碎片以高动能（通常为2–8 eV）释放，并且激光强度≥10〜（14）W / cm〜2，远高于苯的双电离所需的水平，这表明其形成是发生在多电荷母离子中。发现H_3〜+分子氢离子相对于原子氢离子的相对喷射效率随着激光强度和脉冲持续时间（67–25 fs）的变化而大大降低。结论是，H_3〜+的形成仅在带电状态相对较低的母体分子前体中以及在其结构显着伸长之前才是可行的，而较高的带多重电荷的分子离子优先解离为H〜+离子。与H_3〜+和H〜+离子的产生相比，还讨论了H_2〜+离子的喷射。最后，通过记录两个氘标记的苯的同位素（1,2-C_6H_4D_2，1,4-C_6H_4D_2）的质谱图，验证了某些分子碎片（如D_2H〜+，DH〜+）的喷射效率为取决于解离之前分子骨架中氢原子的具体位置。

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