Spectroscopic Studies of Transitions to Vibrational Chaotic States of Highly Excited Polyatomic Molecules

高激发多原子分子向振动混沌态转变的光谱研究

• 批准号: 06453027
• 负责人: TSUCHIYA Soji
• 金额: $ 4.67万
• 依托单位: JAPAN WOMEN'S UNIVERSITY
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for General Scientific Research (B)
• 财政年份: 1994
• 资助国家: 日本
• 起止时间: 1994 至 1995
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-06453027/
• 关键词: Molecular Vibrational Dynamics; Chaos; Normal Vibration; Unimolecular Reaction

Dispersed fluorescence spectroscopy has been applied to elucidate the vibrational dynamics of highly excited polyatomic molecules. The major concern of this project is to clarify the mechanism of the transition from the 'regular' to 'chaotic' vibrational dynamics in highly excited polyatomic molecules.The observed vibrational level structure of a highly excited polyatomic molecule was found to be of a hierarchical one owing to the anharmonic resonances among certain vibrational modes. The intermode couplings occurs in a stepwise manner as the vibhrational energy increases towards the vibrational chaotic state in the final stage.It was found that the vibrational spectra of excited acetylene in the ground electronic state reflect the above situation, i.e., the trans-CH bending mode loses its physical ground in a high energy region through a strong coupling with the cis-CH bending mode, and that in a more higher energy region further couplings with CC and CH stretching modes occurs.The conclusion derived above is generalized by observing the spectra of other simple polyatomic molecules in their highly excited states.

色散荧光光谱已被应用于阐明高激发态多原子分子的振动动力学。本项目的主要内容是阐明高激发态多原子分子从“规则”振动动力学到“混沌”振动动力学的转变机制，发现高激发态多原子分子的振动能级结构是一种分级结构，这是由于某些振动模式之间存在非谐共振。在最后阶段，随着振动能量的增加，模间耦合以阶梯方式向振动混沌态发展，发现基态乙炔的振动光谱反映了上述情况，即，trans-CH弯曲模在高能区通过与cis-CH弯曲模的强耦合而失去物理基础，在更高的能区进一步与CC和CH伸缩模耦合，上述结论通过观察其它简单多原子分子的高激发态光谱得到了推广.

项目成果

K. Yamanouchi et al.: "New Scheme for Extracting Molecular Dynamics from Spectra: Case study on Vibrationally Highly Excited Acetylene" Laser Chemistry. 14. 183-190 (1994)

K. Yamanouchi 等人：“从光谱中提取分子动力学的新方案：振动高激发乙炔的案例研究”激光化学。

K. Yamanouchi et al.: "Laser Induced Fluorescence Spectroscopy of the C^1B_2-X^1A_1 Band of Jet-cooled SO_2: Rotational and Vibrational Analyses in the 235-210 nm Region" J. Mol. Structure. 352/353. 541-559 (1995)

K. Yamanouchi 等人：“喷射冷却 SO_2 的 C^1B_2-X^1A_1 带的激光诱导荧光光谱：235-210 nm 区域的旋转和振动分析”J. Mol。

J. Miyawaki et al.: "Feature state assignment and hierarchical and statistical analyses of vibronic level structure of NO_2 in the 16300-25130cm^<-1> region" J. Chem. Phys.101. 4505-4513 (1994)

J. Miyawaki 等人：“NO_2 在 16300-25130cm^<-1> 区域的电子能级结构的特征状态分配和层次统计分析”J. Chem。

K.Yamanouchi,et al.: "Laser Induced Fluorescence Spectroscopy of the C^1B_2-X^2A_1 Band of Jet-cooled SO_2: Rotational and vibrational Analyses in the 235-210 nm Region" J.Mol.Structure. 352/353. 541-559 (1995)

K.Yamanouchi 等人：“喷射冷却 SO_2 的 C^1B_2-X^2A_1 带的激光诱导荧光光谱：235-210 nm 区域的旋转和振动分析”J.Mol.Structure。

S.Tsuchiya: "Intramolecular Dynamics and Unimolecular Reaction. A Case Study of State-selectively Excited Nitrogen Dioxide" Proc. of 6th International Symposium on Advanced Nuclear Energy Research. 87-96 (1995)

S.Tsuchiya：“分子内动力学和单分子反应。状态选择性激发二氧化氮的案例研究”Proc。