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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >O(~1D) + N_2O Reaction: NO Vibrational and Rotational Distributions
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O(~1D) + N_2O Reaction: NO Vibrational and Rotational Distributions

机译：O（〜1D）+ N_2O反应：NO振动和旋转分布

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摘要

The O(~1D) + N_2O → 2NO(X ~2Π) reaction has been studied in a molecular beam experiment in which O_3 and N_2O were coexpanded. The precursor O(~1D) was prepared by O_3 photodissociation at 266 nm, and the NO(X ~2Π) molecules born from the reaction as the O(~1D) recoiled out of the beam were detected by 1+1 REMPI over the 220?246 nm probe laser wavelength range. The resulting spectrum was simulated to extract rotational and vibrational distributions of the NO(X ~2Π) molecules. The product rotational distribution is found to be characterized by a constant rotational temperature of ≈4500 K for all observed bands, v = 0?9. An inverted vibrational distribution is observed. A consistent explanation of this and previous experimental results is possible if there are two channels for the reaction, one producing a nearly statistical vibrational distribution for low O(~1D)?N_2O relative velocity collisions and a second producing the inverted distribution observed here for high relative velocity collisions. The former might correspond to an insertion/complex-formation reaction, while the latter might correspond to a stripping reaction. Velocity relaxation of the O(~1D) is argued to compete strongly with reaction in most bulb studies, so that these studies see predominantly the nearly statistical distribution. In contrast, the beam experiments do not detect the part of the vibrational distribution produced in low relative velocity reactions because the O(~1D) is not relaxed from its initial velocity before it either reacts or leaves the beam.
机译：在分子束实验中研究了O（〜1D）+ N_2O→2NO（X〜2Π）反应，其中O_3和N_2O共同展开。通过在266 nm处进行O_3光解离制备前体O（〜1D），并通过1 + 1 REMPI在反应过程中检测出从反应中脱出的O（〜1D）分子中产生的NO（X〜2Π）分子。 220？246 nm探针激光波长范围。模拟所得的光谱以提取NO（X〜2Π）分子的旋转和振动分布。发现产物旋转分布的特征在于，对于所有观察到的频带，v = 0？9，恒定的旋转温度为≈4500K。观察到反向振动分布。如果有两个反应通道，则有可能对此反应和先前的实验结果进行一致的解释，一个通道在低O（〜1D）？N_2O相对速度碰撞时产生几乎统计的振动分布，第二个通道在此处观察到反演分布时获得较高的振动分布。相对速度碰撞。前者可能对应于插入/形成复合物的反应，而后者可能对应于汽提反应。在大多数球茎研究中，O（〜1D）的速度弛豫被认为与反应具有很强的竞争性，因此这些研究主要看到了接近统计的分布。相反，由于O（〜1D）在反应或离开光束之前并未从其初始速度放松，因此光束实验无法检测到在相对速度较低的反应中产生的振动分布的一部分。

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