STUDY OF REACTION DYNAMICS VIA MEASUREMENTS OF DIFFERENTIAL CROSS SECTIONS DEPENDENT ON ROTATIONAL ANGULAR MOMENTUM POLARIZATION OF REACTION PRODUCTS

通过测量取决于反应产物的旋转角动量极化的微分截面来研究反应动力学

• 批准号: 11640506
• 负责人: FUJIMURA Yo
• 金额: $ 1.86万
• 依托单位: KYOTO UNIVERSITY
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for Scientific Research (C)
• 财政年份: 1999
• 资助国家: 日本
• 起止时间: 1999 至 2000
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-11640506/
• 关键词: Oxygen; Nitrous Oxide; Hydrocarbon; Reaction Dynamics; Doppler Spectroscopy; Vector Correlation; Polarization; Differential Cross Sections; 気相素反応; 偏光ドップラー分光; 回転角運動量; 水分子

Chemical dynamics of elementary gas phase reactions have been studied via Doppler-resolved polarization spectroscopy. By using this technique, differential cross sections can be measured state-resolved manner. Furthermore, this method enables us to measure the polarization of the rotational angular momentum of reaction products.Collision-free diatomic product molecules were probed with high-resolution dye laser excitation and its Doppler-broadened line profiles were analyzed to extract the information of vector properties such as differential cross sections and rotational angular momentum polarization. We investigated the reactions of O(^1D) or O(^3P) atom with some several simple molecules. The followings are the summaries of this study. 1) For O(^1D)+N_2O→NO+NO reaction, the rotational angular momentum of the NO products are isotropic and consistent with the efficient energy randomization within all the degrees of freedom of reaction intermediates leading to apparent statistical rovi … More brational state distribution of NO products despite the absence of a deep potential well. 2) For O(^3P)+RH→OH+R reaction (RH : saturated hydrocarbons), reaction mechanism varies with collision energy and traditional understanding of a simple rebound abstraction mechanism is not universally proper especially in high collision energy. 3) For O(^1D)+RH→OH+R reaction, the suggested two-type mechanisms dependent on the size of RH and rovibrational state of OH products are not largely different in the lifetime of reactive intermediate. Rotational angular momentum vectors of high rotational levels are perpendicular to the scattering plane, that is, C-O-H bending motion exerts the OH rotation. This trend is similar to the O(^1D)+H_2O reaction, where O(^1D) insertion is dominant as in the O(^1D)+RH reaction.To obtain these finding is only enabled by polarization Doppler method. Some of the findings in this study give new understandings Which are opposite to the previous ones based on insufficient state-resolved measurements. The study elucidating elementary bimolecular reactions in this manner is essential for the fundamental understanding of chemical reaction dynamics. Less

基本气相反应的化学动力学已经通过多普勒分辨的极化光谱研究了。通过使用此技术，可以测量差分横截面的状态分辨方式。此外，这种方法使我们能够测量反应产物的旋转角动量的极化。对无碰撞的双原子产物分子进行探测，并分析了高分辨率的染料激光兴奋，其多普勒囊线谱分析以提取矢量特性的信息，例如差异截面和旋转式动量，以提取载体的信息。我们研究了O（^1d）或O（^3p）原子与一些简单分子的反应。以下是本研究的摘要。 1）对于O（^1d）+N_2O→NO+无反应，无产物的旋转角动量是各向同性的，并且与所有反应自由度中间人的有效能量随机化一致，导致明显的统计Rovi…尽管没有深度潜在的潜能，但NO NO NO BRIENATIAL STATICTION ROVINE都会产生明显的统计状态。 2）对于O（^3p）+RH→OH+R反应（RH：饱和碳氢化合物），反应机制随碰撞能量和对简单反弹抽象机制的传统理解而变化，尤其是在高碰撞能量中，尤其是在高碰撞能量上。 3）对于O（^1D）+RH→OH+R反应，建议的两种机制取决于OH产品的RH和Rovinbibrational Sate的大小，在反应性中间体的寿命中并没有很大差异。高旋转水平的旋转角动量向量垂直于散射平面，即C-O-H弯曲运动会施加OH旋转。这种趋势类似于O（^1d）+H_2O反应，其中O（^1d）插入主要像O（^1D）+RH反应中的主流。要获得这些发现仅通过极化多普勒方法启用。这项研究的一些发现给出了与以前基于状态解决的测量不足的新理解相反。以这种方式阐明基本双分子反应的研究对于对化学反应动力学的基本理解至关重要。较少的

项目成果

Hiroshi Tsurumaki: "Sterodynamics of the reactions of O(^3P) with saturated hydrocarbons : The dependences on the collision energy and the structrual features of hydrocarbons"The Journal of Chemical Physics. 112・19. 8338-8346 (2000)

Hiroshi Tsurumaki：“O(^3P) 与饱和烃的反应的立体动力学：对碰撞能量和烃的结构特征的依赖性”化学物理杂志 112・19 (2000)。

Hiroshi Tsurumaki: "Stereodynamics of the reactions of O(^3P) with saturated hydrocarbons : The dependences on the collision energy and the structural features of hydrocarbons"The Journal of Chemical Physics. 112. 8338-8346 (2000)

Hiroshi Tsurumaki：“O(^3P) 与饱和碳氢化合物反应的立体动力学：对碰撞能量和碳氢化合物结构特征的依赖性”化学物理杂志。

Hiroshi Tsurumaki: "Scalar and vector properties of the NO (ν'=0) produced from the reaction O(^1D)+N_2O→NO+NO"The Journal of Chemical Physics. 111. 592-599 (1999)

Hiroshi Tsurumaki：“O(^1D)+N_2O→NO+NO 反应产生的 NO (ν=0) 的标量和矢量性质”化学物理杂志 111. 592-599 (1999)。

Hiroshi Akagi: "Theoretical investigation of the potential energy surfaces for the O(^1D) + N_2O reaction"Chemical Physics Letters. 324. 423-429 (2000)

Hiroshi Akagi：“O(^1D) N_2O 反应势能面的理论研究”《化学物理快报》。

Hiroshi Akagi: "Energy partitioning in two kinds of NO molecules generated from the reaction of O(^1D)with N_2O : Vibrational state distribution of "new" and "old" NO's"The Journal of Chemical Physics. 111. 115-122 (1999)

Hiroshi Akagi：“O(^1D)与 N_2O 反应生成的两种 NO 分子的能量分配：“新”和“旧”NO 的振动状态分布”《化学物理杂志》。