在高度兴奋的状态中漫游:三原子分子分解的中心原子消除
Zhenxing Li1, Yan-Lin Fu1, Zijie Luo1,2
1State Key Laboratory of Molecular Reaction Dynamics and Dalian Coherent Light Source, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, P. R. China.
概括
分子漫游是一种非常规的反应途径,在SO2光解离的高度兴奋状态下观察到. 这种机制产生更热的硫氧和氧碎片, 挑战传统的最小能量路径假设.
科学领域:
- 化学物理
- 摄影化学
- 反应动力学
背景情况:
- 化学反应通常遵循最小能量路径 (MEP).
- 漫游,偏离MEP,已知在地面和第一个激发状态.
- 在高度兴奋的状态中漫游仍然很大程度上未建立.
研究的目的:
- 在SO2光解的高度激发状态下研究解离路径.
- 确定漫游机制是否发生在高度兴奋的状态.
- 通过不同的解离道产生碎片的特征.
主要方法:
- 在高度激发状态下对SO2进行光解离.
- 分离产品的分析,特别是S{1D}和O{2a1Δg}片段.
- 用光谱鉴定来确定O2的振动状态
主要成果:
- 确定了SO2光解的两个解离途径.
- 一个路径遵循MEP,产生振动较冷的O2{a1Δg).
- 第二个途径,涉及漫游,通过分子内氧抽取产生振动更热的O2 (a1Δg).
结论:
- 漫游动态被证实发生在高度激发的分子光解离状态中.
- 这种漫游机制涉及分子内O抽象和重定向运动.
- 漫游可能是高度兴奋状态分子光解离的常见机制,而不是例外.
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