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首页> 外文期刊>Physical chemistry chemical physics: PCCP >Rapid bond rearrangement in core-excited molecular water
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Rapid bond rearrangement in core-excited molecular water

机译：核心激发分子水中的快速粘合重排

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The angular anisotropy of fragments created in the dissociation of core-electron excited water molecules is studied to probe the correlation between fragmentation channels, kinematics and molecular geometry. We present fragment kinetic measurements for water molecules where the inner-shell oxygen electron is excited to the unoccupied 4a1 and 2b2 valence molecular orbitals. The kinematics of individual fragmentation channels are measured using fully three-dimensional momentum imaging of fragments. The results show that the geometry of the molecule and the kinetic energy of fragments are strongly coupled in the atomisation process. In addition we identify a fragmentation process arising from bond rearrangement evidenced by the H2~+-O~+ ion pair which is accessible for resonant excitation of the 1s electron. In all of the two-body fragmentation processes the dissociation takes place along the potential-energy surface, while atomisation reveals both dissociation along the potential surface and Coulomb explosion. The angular distribution of fragments suggests that the bond rearrangement is very rapid; likely on a sub 10 fs time scale.
机译：研究了在核心 - 电子激发水分子的解离中产生的片段的角度各向异性，以探测碎片通道，运动学和分子几何之间的相关性。我们为水分子呈现片段动力学测量，其中内壳氧电子激发到未占用的4A1和2B2价分子轨道。使用碎片的全三维动量成像来测量单个碎片通道的运动学。结果表明，在雾化过程中，分子的几何形状和片段的动能强烈偶联。此外，我们鉴定了由H2〜+ -O +离子对所证明的粘合重新排列引起的碎片过程，其可用于1S电子的共振激发。在所有双体碎片过程中，解离沿电位 - 能量表面发生，而雾化揭示沿电位表面和库仑爆炸的解离。片段的角度分布表明粘合重排非常迅速;可能在10 fs时间尺度上。

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