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成像 O(1D) + CD4 → OD + CD3 反应动力学:探测振动和旋转激发的 CD3 产物。

Imaging the O(1D) + CD4 → OD + CD3 reaction dynamics: probing vibrationally and rotationally excited CD3 products.

机构信息

State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023, People's Republic of China.

出版信息

J Chem Phys. 2012 Dec 14;137(22):224301. doi: 10.1063/1.4767397.

DOI:10.1063/1.4767397
PMID:23248997
Abstract

The dynamics of the O((1)D) + CD(4) → OD + CD(3) reaction has been studied using the crossed molecular beam technique with sliced velocity map imaging. Internally excited CD(3) products were detected using a (2+1) resonance-enhanced multiphoton ionization with state resolution. Dual reaction mechanisms, insertion and abstraction, were only observed for CD(3) products with its umbrella mode (v(2)) excited or in its ground state, while CD(3) products with other vibrational mode excited do not show any evidence of contributions from the abstraction pathway. Experimental results indicate that even though the insertion channel dominates the reaction, the abstraction channel contributes relatively more to vibrationally excited CD(3) products. The state-to-state correlation between the two reaction products, OD and CD(3), was determined for the abstraction channel at different collision energies. In addition, we measured rotationally hot CD(3) products and found that these products are only produced via the insertion channel.

摘要

使用交叉分子束技术和切片速度图成像,研究了 O((1)D) + CD(4) → OD + CD(3) 反应的动力学。通过具有态分辨率的 (2+1) 共振增强多光子电离,检测到内部激发的 CD(3)产物。仅观察到 CD(3)产物的伞式模式(v(2)) 激发或处于基态时存在插入和提取两种反应机制,而处于其他振动模式激发态的 CD(3)产物则没有表现出来自提取途径的任何证据。实验结果表明,尽管插入通道主导反应,但提取通道对振动激发的 CD(3)产物的贡献相对更大。在不同的碰撞能量下,确定了两个反应产物 OD 和 CD(3)之间的态态相关。此外,我们测量了旋转热 CD(3)产物,发现这些产物仅通过插入通道产生。

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