轨道角动量对反应立体动力学的选择性作用

IF 1.5 4区 物理与天体物理 Q3 OPTICS The European Physical Journal D Pub Date : 2023-04-18 DOI:10.1140/epjd/s10053-023-00643-3
Stefano Falcinelli, Marco Parriani, Franco Vecchiocattivi, Fernando Pirani
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引用次数: 0

摘要

本文报道了三种不同化学电离反应的立体动力学控制特性,这是我们最近的研究目标,因为它们参与了等离子体、星际介质、行星大气、火焰和激光中发生的现象的平衡。用现象学方法得到的光势,在试剂的相对构型的整个空间中定义,以准确和内部一致的方式表述了三种不同体系的光势。在本研究中,利用与开壳层原子的特定精细能级和/或与分子试剂的确定取向渐近相关的多维势的一些切割来强调沿选定的反应入口通道的碰撞动力学的关键特征。同样,决定反应立体动力学拓扑结构的基本量也得到了适当的定义,强调了三种情况下微观反应演化的相关变化。许多注意力集中在轨道角动量的选择性上,它在任意选择的碰撞能量下影响每一个碰撞事件。它控制着两种不同反应机制的相对重量。直接反应机制是由短程化学力驱动,通过试剂之间的直接电子转移,促进一个典型的初等氧化反应。间接机制由远程化学力和物理力的结合控制,可以通过试剂之间的虚拟光子交换触发,促进一种光电离过程。获得的结果和强调的差异似乎是许多其他基本过程的普遍兴趣,在这个细节水平上更难以表征。图形抽象
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The selective role of the orbital angular momentum on the reaction stereo-dynamics

This paper reports on the characterization of the stereo-dynamic controlling three different chemi-ionization reactions, recent objective of our study, since they participate to the balance of phenomena occurring in plasma, interstellar medium, planetary atmospheres, flames and lasers. The optical potential, obtained by a phenomenological method and defined in the whole space of the relative configurations of reagents, has been formulated in an accurate and internally consistent way for three different systems. Some cuts of the multidimensional potential, that asymptotically correlate with a specific fine level of the open shell atom and/or with a defined orientation of the molecular reagent, have been exploited in the present study to emphasize crucial features of the collision dynamics along selected entrance channels of the reactions. Consistently, basic quantities determining the topology of the reaction stereo-dynamics have been properly defined, emphasizing in the three cases relevant changes in the microscopic reaction evolution. Much attention focused on the selectivity of the orbital angular momentum, affecting each collision event at any chosen collision energy. It controls the relative weight of two different reaction mechanisms. The direct reaction mechanism is driven by short-range chemical forces, promoting, by direct electron transfer between reagents, a prototypical elementary oxidation reaction. The indirect mechanism, controlled by the combination of long-range chemical and physical forces, can be triggered by a virtual photon exchanged between reagents, promoting a sort of photo-ionization process. Obtained results and emphasized differences appear to be of general interest for many other elementary processes, more difficult to characterize at this level of detail.

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来源期刊
The European Physical Journal D
The European Physical Journal D 物理-物理:原子、分子和化学物理
CiteScore
3.10
自引率
11.10%
发文量
213
审稿时长
3 months
期刊介绍: The European Physical Journal D (EPJ D) presents new and original research results in: Atomic Physics; Molecular Physics and Chemical Physics; Atomic and Molecular Collisions; Clusters and Nanostructures; Plasma Physics; Laser Cooling and Quantum Gas; Nonlinear Dynamics; Optical Physics; Quantum Optics and Quantum Information; Ultraintense and Ultrashort Laser Fields. The range of topics covered in these areas is extensive, from Molecular Interaction and Reactivity to Spectroscopy and Thermodynamics of Clusters, from Atomic Optics to Bose-Einstein Condensation to Femtochemistry.
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