论文标题

h $^{+} $+h $^{+} $分离频道的光电和碎片动力学在nh $ _3 $中以直接单光量双电离为单位

Photoelectron and fragmentation dynamics of the H$^{+}$ + H$^{+}$ dissociative channel in NH$_3$ following direct single-photon double ionization

论文作者

Larsen, Kirk A., Rescigno, Thomas N., Severt, Travis, Streeter, Zachary L., Iskandar, Wael, Heck, Saijoscha, Gatton, Averell, Champenois, Elio G., Strom, Richard, Jochim, Bethany, Reedy, Dylan, Call, Demitri, Moshammer, Robert, Dörner, Reinhard, Landers, Allen L., Williams, Joshua B., McCurdy, C. William, Lucchese, Robert R., Ben-Itzhak, Itzik, Slaughter, Daniel S., Weber, Thorsten

论文摘要

我们报告了H $^{+} $+H $^{+} $片段化通道的测量值,直接单光量在61.5 eV时中性NH $ _ {3} $的单光电离,其中两个光电子和两个质子使用3-D Momkum Imamm巧妙地测量了两个光电子和两个质子。我们基于我们的多差配置相互作用计算计算,我们确定了有助于H $^{+} $+H $^{+} $解离的四个dication电子状态。提出了这四种电子状态之间提取的分支比率。在四个dication电子状态中,三个在一致的过程中分离,而第四个则经历了顺序的片段化机制。我们发现证据表明,中性的NH片段或中间NH $^+$离子在RO振动上显着激发。我们还确定了两个光电子之间的相对发射角差异,这是它们在四种不同的疾病状态的能量共享的函数,这与先前对原子靶标的先前观察结果有些相似。

We report measurements on the H$^{+}$ + H$^{+}$ fragmentation channel following direct single-photon double ionization of neutral NH$_{3}$ at 61.5 eV, where the two photoelectrons and two protons are measured in coincidence using 3-D momentum imaging. We identify four dication electronic states that contribute to H$^{+}$ + H$^{+}$ dissociation, based on our multireference configuration-interaction calculations of the dication potential energy surfaces. The extracted branching ratios between these four dication electronic states are presented. Of the four dication electronic states, three dissociate in a concerted process, while the fourth undergoes a sequential fragmentation mechanism. We find evidence that the neutral NH fragment or intermediate NH$^+$ ion is markedly ro-vibrationally excited. We also identify differences in the relative emission angle between the two photoelectrons as a function of their energy sharing for the four different dication states, which bare some similarities to previous observations made on atomic targets.

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