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Ultrafast Dissociation Dynamics of Inner-Shell Excited Molecules

内壳激发分子的超快解离动力学

基本信息

批准号：
10440178
负责人：
KOYANO Inosuke
金额：
$ 7.94万
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：
1998
资助国家：
日本
起止时间：
1998 至 1999
项目状态：
已结题

项目摘要

Following the proposed plan, we have performed in the present project three types of experiments shown below, placing particular emphasis on the second and third experiments which aim at direct observation of ultrafast nuclear motion in the core-hole state of some simple molecules : (1) measurements of high resolution resonance Auger electron spectra with a cylindrical mirror electron energy analyzer, (2) measurements of wavelength-dependent asymmetry parameter (βvalues) for all fragments from the inner-shell excited CO_2 within an unresolved resonance peak, (3) direct measurements of linear momentum distribution of all fragment ions produced following resonant inner-shell excitation. The last subject included development of a new technique consisting of a time-of-flight measurement using a position-sensitive two-dimensional detectors with delay-line anodes.The most prominent among many successful results is the separate observation of the two Renner-Teller split states as achieved by … More the above-mentioned linear momentum distribution measurements. Each of the C1s^<-1>2π_υ and O1s^<-1>2π_υ core-hole states is predicted to be split into two levels by the vibronic coupling with the bending vibration : one is which the π orbital lies in the bending plane (bent structure) and the other in which it extrudes perpendicularly from the bending plane (linear structure), but these levels have never been observed separately. With the present technique, we could nicely observe one of these levels separately from the other by utilizing vector products of the two momenta corresponding to the two O^+ fragment ions. In this way it has clearly been shown that the molecules just before the dissociation are more bent with the excitation to the former level than with that to the latter level. This is interpreted as reflecting the nuclear motion in the core-excited states towards the equilibrium geometry. This represents the first direct verification of the occurrence of linear and bent structures for the C1s^<-1>2π_υ and O1s^<-1>2π_υ core-hole state (Renner-Teller split pair). Less

按照提议的计划，我们在本项目中进行了如下所示的三种类型的实验，特别强调第二和第三种实验，旨在直接观察一些简单分子的核空穴状态下的超快核运动：（1）使用柱面镜电子能量分析仪测量高分辨率共振俄歇电子能谱，（2）测量波长相关的不对称参数（β值）对于未解析的共振峰内内壳层激发的CO_2的所有碎片，（3）直接测量共振内壳层激发后产生的所有碎片离子的线性动量分布。最后一个主题包括开发一种新技术，该技术包括使用带有延迟线阳极的位置敏感二维探测器进行飞行时间测量。许多成功结果中最突出的是通过上述线性动量分布测量实现的两个 Renner-Teller 分裂态的单独观察。 C1s^<-1>2π_υ 和 O1s^<-1>2π_υ 核孔态中的每一个都被预测通过与弯曲振动的振动耦合而分裂成两个能级：一个是π轨道位于弯曲平面内（弯曲结构），另一个是π轨道从弯曲平面垂直挤出（线性结构），但这些能级从未被单独观察到。利用本技术，我们可以利用与两个 O^+ 碎片离子相对应的两个动量的矢量乘积，很好地分别观察这些能级中的一个能级。通过这种方式，已经清楚地表明，在前一能级的激发下，解离前的分子比在后一能级的激发下更加弯曲。这被解释为反映了核激发态中朝向平衡几何形状的核运动。这代表了对 C1s^<-1>2π_υ 和 O1s^<-1>2π_υ 核孔态（Renner-Teller 分裂对）线性和弯曲结构出现的首次直接验证。较少的