A photochemical model of ozone interference effects in laser detection of tropospheric OH
A photochemical model of ozone interference effects in laser detection of tropospheric OH
复制标题
激光探测对流层OH中臭氧干扰效应的光化学模型
DOI：
10.1029/jd095id10p16427
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发表时间：
1990
影响因子：
--
通讯作者：
D. Crosley
中科院分区：
文献类型：
--
作者：
Gregory P Smith;D. Crosley
通过详细的光化学模型解决了对流层羟基激光诱导荧光检测中激光产生的干扰。这种现象是通过检测激光光解臭氧以及随后 O(1D) 与 H2O 反应形成 OH 而产生的。该方法是描述相关化学反应、碰撞能量转移以及光解和光谱过程的耦合微分方程的直接时间积分，包括对由于输入参数的不确定性造成的限制的评估。目标是利用该模型定量设计·OH检测方法，使得实验结果不需要依赖这样的模型来解释。先前报道的对流层 OH 测量结果似乎受到臭氧干扰效应和监测转变的光饱和的污染。然而，建议的改进可以将问题降低到低于 2×105 OH 分子/cm3 的干扰水平，从而使测量可用于测试快速对流层光化学理论。
Laser-generated interference in the laser-induced fluorescence detection of tropospheric hydroxyl is addressed by a detailed photochemical model. This phenomenon arises through photolysis of ozone by the detection laser and subsequent reaction of O(1D) with H2O to form OH. The approach is direct time integration of the coupled differential equations describing the pertinent chemical reactions, collisional energy transfer, and photolytic and spectroscopic processes, including an assessment of limitations due to uncertainties in the input parameters. The goal is to use the model to quantitatively design OH detection methods so that the experimental results need not rely on such a model for interpretation. Previously reported measurements of tropospheric OH appear to have been contaminated by ozone interference effects and by optical saturation of the monitoring transition. However, suggested improvements can reduce the problem to interference levels below 2×105 OH molecules/cm3, permitting measurements useful for testing theories of fast tropospheric photochemistry.