Reaction dynamics of Al+O2→AlO+O studied by the crossed-beam laser-induced fluorescence technique
Reaction dynamics of Al+O2→AlO+O studied by the crossed-beam laser-induced fluorescence technique
复制标题
DOI：
10.1063/1.1591177
复制
发表时间：
2003-08-15
影响因子：
4.4
通讯作者：
Honma, K
中科院分区：
文献类型：
--
作者：
Honma, K
用交叉束技术研究了Al+O-2-->AlO+O反应在6.9 - 25.3kJ/mol五种碰撞能量下的动力学。Al原子束由激光蒸发产生，并与O-2束成直角相交。用激光诱导荧光法检测了AlO（B（2）Sigma（+）-X（2）Sigma（+））跃迁，并测定了转动-振动分布。观察到的旋转和振动分布显示更大的人口在较低的振动和旋转水平比预期的统计。在两个碰撞能量下，还测定了Al（P-2（1/2））和Al（P-2（3/2））两种自旋轨道态的转动分布。在12.2 kJ/mol的碰撞能量下，较高能量的自旋轨道激发态Al（P-2（3/2））显示出较低的反应性，即，大约是基态自旋轨道状态Al（P-2（1/2））的三分之一。然而，这两种状态的转动分布几乎相同。Al（P-2（1/2））和Al（P-2（3/2））的反应性和转动分布在更高的碰撞能量（18.5 kJ/mol）下变得相似。这些结果表明，Al与O-2的反应通过中间络合物进行。两种自旋轨道状态导致复合物，失去初始电子状态的记忆，并提供相同的旋转分布。(C)2003年，美国物理学会。
Dynamics of the reaction, Al+O-2-->AlO+O, was studied by using the crossed-beam technique at five collision energies from 6.9 to 25.3 kJ/mol. The Al atomic beam was generated by laser vaporization and crossed with the O-2 beam at a right angle. The product AlO was detected by laser-induced fluorescence of the AlO(B (2)Sigma(+)-X (2)Sigma(+)) transition and the rotational-vibrational distributions were determined. The observed rotational and vibrational distributions displayed greater populations in lower vibrational and rotational levels than expected statistically. Rotational distributions were also determined for two spin-orbit states of Al, Al(P-2(1/2)) and Al(P-2(3/2)), at two collision energies. At a collision energy of 12.2 kJ/mol, the higher energy spin-orbit excited state, Al(P-2(3/2)), showed lower reactivity, i.e., about one-third of the ground spin-orbit state, Al(P-2(1/2)). However, the rotational distributions for the two states were almost identical. Both the reactivity and rotational distributions for Al(P-2(1/2)) and Al(P-2(3/2)) became similar at a higher collision energy, 18.5 kJ/mol. These results suggest that the reaction of Al with O-2 proceeds via an intermediate complex. Both spin-orbit states lead to the complex, lose memory of the initial electronic state, and provide identical rotational distributions. (C) 2003 American Institute of Physics.