Honma Kenji, Miyashita Kazuki, Matsumoto Yoshiteru
Graduate School of Material Science, University of Hyogo, 3-2-1 Kohto, Kamigori, Hyogo 678-1297, Japan.
J Chem Phys. 2014 Jun 7;140(21):214304. doi: 10.1063/1.4879616.
Oxidation reaction of a gas-phase aluminum atom by a molecular oxygen was studied by a crossed-beam condition at 12.4 kJ/mol of collision energy. A (1+1) resonance-enhanced multiphoton ionization (REMPI) via the D(2)Σ(+)-X(2)Σ(+) transition of AlO was applied to ionize the product. The REMPI spectrum was analyzed to determine rotational state distributions for v = 0-2 of AlO. For several vib-rotational states of AlO, state selected angular and kinetic energy distributions were determined by a time-sliced ion imaging technique for the first time. Kinetic energy distributions were well represented by that taken into account initial energy spreads of collision energy and the population of the spin-orbit levels of the counter product O((3)P(J)) determined previously. All angular distributions showed forward and backward peaks, and the forward peaks were more pronounced than the backward one for the states of low internal energy. The backward peak intensity became comparable to the forward one for the states of high internal energy. These results and the rotational state distributions suggested that the reaction proceeds via an intermediate which has a lifetime comparable to or shorter than its rotational period.
在碰撞能量为12.4 kJ/mol的交叉束条件下,研究了气相铝原子与分子氧的氧化反应。通过AlO的D(2)Σ(+)-X(2)Σ(+)跃迁的(1+1)共振增强多光子电离(REMPI)来电离产物。分析REMPI光谱以确定AlO的v = 0-2的转动状态分布。对于AlO的几个振转状态,首次通过时间切片离子成像技术确定了状态选择的角分布和动能分布。动能分布可以很好地由考虑碰撞能量的初始能量展宽和先前确定的反产物O((3)P(J))的自旋轨道能级的布居来表示。所有角分布都显示出向前和向后的峰,对于低内能状态,向前的峰比向后的峰更明显。对于高内能状态,向后峰的强度变得与向前峰相当。这些结果和转动状态分布表明,该反应通过一个寿命与其转动周期相当或更短的中间体进行。