【作者】 李淑娟；

【导师】 石英；

【作者基本信息】 吉林大学 ， 原子与分子物理， 2012， 硕士

【摘要】 要全面掌握一个化学反应的特征，不仅是探索其标量特性，如反应产物的分支比、微分反应截面的分布、反应速率等，还要研究其矢量特性，如速度和角动量与碰撞能之间的关系，反应物和生成物的散射方向等。只有把二者结合起来，才能揭示出反应更多的立体动力学信息。本文中采用QCT方法计算了反应物的振动量子数,碰撞能和同位素效应对Li+H (D) F→LiF+H (D)反应的立体动力学的影响。反应都基于由Aguado等人所构建的AP2势能面上进行的。本文首先，计算了反应体系的标量性质，例如，反应Li+HF→LiF+H的反应几率、总的反应截面、产物转动取向的值p2j’ k随振动量子数变化的影响；其次，分析了4个反应的相应的矢量相关的性质，例如，极角P (θr)及方位角P (φ r)以及空间角P (θ r,φ r)的分布和极化微分反应截面PDDCS的四个分量随相应的反应变量的变化的结果。本文依次计算了： Li+HF反应以振动量子数为变量，Li+DF反应以振动量子数为变量、 Li+DF反应以碰撞能为变量、以氢原子的同位素为变量的Li+H (D)F反应进行计算并分析了每个反应的标量性质和矢量性质。得出结论：反应k-j’的两矢量相关性质的P (θ r)分布显示出产物转动角动量j’强烈地取向于相对速度矢量k，各个变量对其相应反应的P (θ r)分布性质均有影响且对相应反应的P (θr)分布性质的影响程度大小不同；描述k-k’-j’三矢量相关的性质P (φ r)分布，结果表明产物转动角动量j’不仅强烈地取向于y轴而且也有定向于y轴负方向的趋势。同时从结果也可得出各个反应受碰撞能、反应物振动态的改变和氢原子同位素的改变对其P (φ r)的分布性质均产生了影响。建立在中心场模型下的四个反应的极化微分反应截面PDDCS及它的性质受各因素变化的影响反映出产物分子空间散射的定向与取向；最后，反应截面和反应几率受氢原子同位素效应Li+H (D) F→LiF+H (D)反应的影响，二者曲线都呈现出变弱的相同趋势。更多还原

【Abstract】 In order to understand the dynamics of elementary reaction fully, itis important to study not only its scalar properties, but also its vectorproperties. Scalar properties, such as reaction product branch ratio, crosssection distribution, reaction probability. Vector properties, such asvelocities and angular momentum, can be directly related to collisionenergies, reactants and the products scattering direction and so on. Onlyby understanding together above properties can the fullest information ofthe stereodynamics be obtained. In the thesis, Quasi-classical trajectory(QCT) calculations have been employed to study the influence of the reagentvibrational quantum number, collision energy and the isotope effect ofhydrogen atom on the reaction probability ofLi+HF→LiF+H. Reactionsexecuted on the AP2potential energy surface (PES) developed by Aguado etal. First, the text calculated reactions scalar properties. For example,Li+HF→LiF+Hthe reaction probability, the integral cross section andthe product rotational alignments p2j’ kare also calculated thatincreased with vibrational quantum numbers monotonically. At the same time,reactions vector properties also were calculated. Such as angulardistribution of the product, P (θ r),P(φ r),P (θ r, φr)which could reflect thevector correlation and PDDCS have been calculated at every reaction. Thetext calculated: Li+HFand Li+DFreaction change with vibrationalquantum number, Li+DFchanges with collision energy and Li+H (D)Fwiththe isotope effect of hydrogen atom are presented in Fig one by one. Theresult, the distribution of P (θ r)shown that the rotational angular momentumvectors j’ of the products were strongly aligned along the relative velocity direction k, the influence of reactions shows different characters with thevariability reagents. The distribution of P (φ r)which implied a preference forthe left-hand product rotation in planes parallel to that of the scatteringplane and the influence of P(φ r)shows different characters with vibrationalquantum number, collision energy, and the isotope effect of hydrogen atom onthe reactions. Four polarization dependent different cross-sections alsopresented in the center-of-mass frame respectively which properties reflectreveal the alignment and the orientation of the product molecules. Last, theisotope effect of hydrogen atom about Li+HF (D)→LiF+H (D)reactions, thereaction probability and the integral cross section were influenced so large.Meanwhile, they have the same weaken distribution.更多还原