Microwave observations and modeling of O3, H2O, and HO2 in the mesosphere
Microwave observations and modeling of O3, H2O, and HO2 in the mesosphere
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中间层中 O3、H2O 和 HO2 的微波观测和建模
DOI：
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发表时间：
1994
期刊：
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通讯作者：
D. Muhleman
中科院分区：
文献类型：
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作者：
R. Clancy;B. Sandor;D. Rusch;D. Muhleman
1992年4月10日至12日，在基特峰国家射电天文台（NRAO）获得了HO 2，H218 O和O3的微波（波长为1.2 mm）谱线观测结果。观测到的碰撞线的形状的光谱带宽和分辨率是适当的检索剖面丰度为O3，H2O，和HO 2在平流层上部和中间层（45- 70公里的高度）与20-30%的不确定性。导出的O3廓线比太阳中间层探测器（SME）和平流层气溶胶气体实验（SAGE）II的4月30°N平均廓线显示的中间层臭氧丰度大20-30%，比采用当前光化学速率常数和微波H218 O观测约束的H2O廓线的光化学模式显示的中间层臭氧丰度大60-80%。令人惊讶的是，微波测量产生的中间层HO 2丰度大约是标准模型光化学预测的两倍。由于HOx（OH，HO 2，H）是中层臭氧催化破坏的主要因素，因此模型对HO 2和O3的低估表明模型光化学发生了变化，这与Ox产生和HOx损失率的误差不同。Ox产生的增加和/或HOx损失率的增加被认为是平流层上部/中间层臭氧丰度数据-模型持续不一致的可能来源。基于O_3和HO_2的微波测量结果，我们提出了改变OH和HO_2之间分配的模型速率的建议.特别地，O + HO_2 → OH + O_2反应的速率系数的大幅度降低（60-80%）被证明是唯一能够增加O_3和HO_2的模型丰度的方法.根据微波观测以及光化学模拟对平流层上层/中层臭氧的显著预报不足。
Microwave (wave ∼1.2 mm) spectral line observations of HO2, H218O, and O3 were obtained at the Kitt Peak National Radio Astronomy Observatory (NRAO) on April 10–12, 1992. The spectral bandwidth and resolution of the observed collisional line shapes are appropriate to retrieving profile abundances for O3, H2O, and HO2 in the upper stratosphere and mesosphere (45- to 70-km altitude) with 20–30% uncertainties. The derived profile for O3 exhibits 20–30% larger mesospheric ozone abundances than indicated by the April 30°N average profiles from Solar Mesosphere Explorer (SME) and Stratosphere Aerosol Gas Experiment (SAGE) II and 60–80% larger than a photochemical model employing current photochemical rate constants and an H2O profile constrained by the microwave H218O observations. Surprisingly, the microwave measurement of HO2 yields mesospheric HO2 abundances roughly twice those predicted by the standard model photochemistry. As HOx(OH, HO2, H) is the primary agent for catalytic destruction of ozone in the mesosphere, the model underpredictions of both HO2 and O3 suggest a change in the model photochemistry that is distinct from errors in Ox production and HOx loss rates. Increases in Ox production and/or increases in HOx loss rates have been considered as the likely sources for the persistent data-model disagreement in upper stratospheric/mesospheric ozone abundances. Based on the microwave measurements of O3 and HO2, we propose changes to model rates for partitioning between OH and HO2.Specifically, a large (60–80%) decrease in the rate coefficient for the reaction O + HO2 → OH + O2 is shown to be uniquely capable of increasing model abundances for O3 and HO2, in accordance with the microwave observations as well as the outstanding underprediction of upper stratospheric/mesospheric ozone by photochemical modeling.