Statistical Spectroscopy of Quantum Chaos State in Vibrationally Highly Excited polyatomic Molecules

高振动激发多原子分子中量子混沌态的统计光谱

基本信息

批准号：
02044038
负责人：
TSUCHIYA Soji
金额：
$ 3.46万
依托单位：
The University of Tokyo
依托单位国家：
日本
项目类别：
Grant-in-Aid for international Scientific Research
财政年份：
1990
资助国家：
日本
起止时间：
1990 至 1991
项目状态：
已结题

项目摘要

This project aims at cooperative experimental and theoretical studies on intramolecular vibrational dynamics of highly excited polyatomic molecules which have been carried out in four laboratories of Tokyo, Cambridge, Grenoble and Paris.1. Vibrational dynamics of highly excited acetylene(1) MIT group proposed a chaotic vibrational dynamics by means of a statistical analysis of level energies of vibrationally highly excited acetylene.(2) Grenoble group claimed an incomplete chaotic dynamics of excited acetylene based on the Fourier analysis of the spectral data obtained by MIT group.(3) Tokyo group observed a dispersed fluorescence spectrum of acetylene in a single rovibronic level to obtain a global feature of the vibrational level structure. They could analyze it in terms of an anharmonic expansion function assuming five normal modes in an energy region up to around 14, 000 cm^<-1>. Beyond this energy, two CH bending, modes (trans and cis) couple each other, so that a local chaotic dy … More namics is realized within these modes. Couplings to other modes occur in another stage approaching a final full chaotic dynamics.(4) Following the above proposal, MIT group confirmed an anharmonic coupling scheme between two CH stretching modes based on the high-resolution SEP spectrum of acetylene.2. Unimolecular dissociation reaction of NO_2(1) Tokyo group succeeded to take a state-selected photofragment (O or NO) excitation spectrum of NO_2. The observed spectrum showed a line structure which indicated the dissociation reaction via highly excited vibrational states of N0_2.(2) The vibrational level structure of excited N0_2 was discussed by Grenoble group, who predicted a chaotic level structure even in the region below the dissociation threshold.3. Structure and dynamics of electronically excited van der Waals complexes(1) Tokyo group predicted the structure of HgAr_2 complex by means of LIF spectroscopy and optical-optical double resonance method.(2) Orsay group discussed the structure of HgAr_2 based on a semi-empirical calculation of the potential surface as well as resonantly enhanced multiple photon ionization method. Less

该项目旨在对高激发态多原子分子的分子内振动动力学进行合作实验和理论研究，该研究已在东京、剑桥、格勒诺布尔和巴黎的四个实验室开展。通过对振动高度激发的乙炔能级能量的统计分析，得出混沌振动动力学。（2）格勒诺布尔小组基于光谱的傅里叶分析，声称激发乙炔的不完全混沌动力学(3)东京小组观察了单个振动电子能级中乙炔的分散荧光光谱，以获得振动能级结构的全局特征，他们可以根据假设五种简正模态的非简谐展开函数对其进行分析。能量区域高达 14, 000 cm^<-1> 超出此能量，两个 CH 弯曲模式（反式和顺式）相互耦合，从而在其中实现局部混沌 dy ... More 纳米学。这些模式与其他模式的耦合发生在接近最终完全混沌动力学的另一个阶段。(4) 根据上述建议，麻省理工学院研究小组基于乙炔的高分辨率 SEP 谱确认了两种 CH 伸缩模式之间的非和谐耦合方案。 NO_2(1)的单分子解离反应东京组成功拍摄了NO_2的状态选择光碎片(O或NO)激发光谱,观察到的光谱显示出表明解离的线结构。 (2)Grenoble小组讨论了激发态N0_2的振动能级结构，预测即使在解离阈值以下的区域也存在混沌能级结构。3．瓦尔斯配合物(1)Tokyo课题组利用LIF光谱和光学-光学双共振法预测了HgAr_2配合物的结构。(2)Orsay课题组基于势面的半经验计算以及共振增强多光子电离法。