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Dynamics of Three-body Dissociation of Inner-shell Excited Molecules

内壳层激发分子三体解离动力学

基本信息

批准号：
12440169
负责人：
KOYANO Inosuke
金额：
$ 8.06万
依托单位：
Himeji Institute of Technology
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (B)
财政年份：
2000
资助国家：
日本
起止时间：
2000 至 2001
项目状态：
已结题

项目摘要

In this two-year project, we performed three types of detailed experiments on the ionization and dissociation dynamics of inner-shell excited polyatomic olecules. Two sophisticated apparatus were used which we had introduced on the soft X-ray photochemistry beamline of the third-generations ynchrotron radiation facility Spring-8: a very high resolution photoelectron / Auger electron energy analyzer (SCIENTA) and a multicoincidence ion / electron momentum imaging apparatus (3DTOF).In the first experiment, we used only the ion part of the 3DTOF apparatus to study the dissociation dynamics of three- and four-atomic molecules, such as CO_2, N_2O, and BF_3, and succeeded in detecting three and four fragment ions originating from triply- and quadruply-ionized parent molecules, respectively, in coincidence. The study was highlighted by the separate observation of the two components of the Renner-Teller split Cls→π^* and Ols→π^* excited states. Other highlights were the findings of the bond an … More gle difference at the moment of ionic fragmentation between the N_t (terminal) ls→π^* and N_c (central) ls→π^* excited states of N_2O and of the fact that the inner-shall excited BF_3 molecule changes its Structure from planar to trigonometric pyramidal before the Auger emission takes place.In the second type of experiments, both the electron and ion detectors of the 3DTOF apparatus were used to successfully obtain the electron-ion-ion triple coincidence. The photoelectron angular distributions (PADs) of the fixed-in-space CO_2 molecule could be obtained by taking coincidence measurements among CO^+, O^+, and photoelectron, the momenta of the former two determining the direction of the molecular axis in the three-dimensional space. Variation in the PADs with the excitation energy within the Cls→π^* and Ols→π^* resonance peaks has clearly been demonstrated.The third type of experiment was the very high-resolution resonant Auger spectroscopy using SCIENTA, in which a so-called sub-natural linewidth spectroscopy was aimed at. A highlight was the first observation of multimode excitation in the Ols→2b_2 excitation of the H_2O molecule, i.e., The observation of the progression of the bending vibration in addition to that of the symmetric stretching vibration in the Auger final state. Less

在这个为期两年的项目中，我们对内壳层激发多原子分子的电离和解离动力学进行了三种类型的详细实验。使用了我们在第三代同步辐射设施Spring-8的软X射线光化学光束线上引入的两个复杂装置：甚高分辨率光电子/俄歇电子能量分析仪（SCIENTA）和多符合离子/电子动量成像装置（3DTOF）。在第一个实验中，我们只使用3DTOF装置的离子部分来研究三原子和四原子分子，如CO_2，N_2O和BF_3的解离动力学，并成功地同时检测到分别来自三重和四重电离的母分子的三个和四个碎片离子。这项研究的亮点是对伦纳-泰勒分裂的Cls→π^* 和Ols→π^* 激发态的两个分量的单独观察。其他亮点是债券的发现， ...更多信息 N_t之间离子碎裂瞬间的角差在第二类实验中，N_2O的（末端）ls→π^* 和N_c（中心）ls→π^* 激发态以及内激发的BF_3分子在俄歇发射前由平面结构转变为三角锥结构。使用3DTOF装置的电子和离子检测器成功地获得了电子-离子-离子三重符合。通过对CO^+、O^+和光电子之间的动量进行符合测量，可以得到固定在空间中的CO_2分子的光电子角分布（PAD），其中CO^+、O^+和光电子的动量决定了分子轴在三维空间中的方向。在Cls→π^* 和Ols→π^* 共振峰内，PAD随激发能的变化得到了明确的证明。第三类实验是利用SCIENTA进行的超高分辨率共振俄歇光谱，其目的是所谓的亚自然线宽光谱。重点是在H_2O分子的Ols→2b_2激发中首次观察到多模激发，即，在俄歇终态中，除了对称伸缩振动外，还观察到了弯曲振动的发展。少