Cady-Pereira K E, Shephard M W, Millet D B, Luo M, Wells K C, Xiao Y, Payne V H, Worden J
Atmospheric and Environmental Research, Inc., Lexington, Massachusetts, USA.
Environment Canada, Toronto, Ontario, Canada.
Atmos Chem Phys. 2012 Sep;12(17):8189-8203. doi: 10.5194/acp-12-8189-2012. Epub 2012 Sep 12.
We present a detailed description of the TES methanol (CHOH) retrieval algorithm, along with initial global results showing the seasonal and spatial distribution of methanol in the lower troposphere. The full development of the TES methanol retrieval is described, including microwindow selection, error analysis, and the utilization of a priori and initial guess information provided by the GEOS-Chem chemical transport model. Retrieval simulations and a sensitivity analysis using the developed retrieval strategy show that TES: (i) generally provides less than 1.0 piece of information, (ii) is sensitive in the lower troposphere with peak sensitivity typically occurring between 900-700 hPa (1-3 km) at a vertical resolution of ~5 km, (iii) has a limit of detectability between 0.5 and 1.0 ppbv Representative Volume Mixing Ratio (RVMR) depending on the atmospheric conditions, corresponding roughly to a profile with a maximum concentration of at least 1 to 2 ppbv, and (iv) in a simulation environment has a mean bias of 0.16 ppbv with a standard deviation of 0.34 ppbv. Applying the newly derived TES retrieval globally and comparing the results with corresponding GEOS-Chem output, we find generally consistent large-scale patterns between the two. However, TES often reveals higher methanol concentrations than simulated in the Northern Hemisphere spring, summer and fall. In the Southern Hemisphere, the TES methanol observations indicate a model overestimate over the bulk of South America from December through July, and a model underestimate during the biomass burning season.
我们详细介绍了对流层发射光谱仪(TES)的甲醇(CH₃OH)反演算法,以及展示对流层低层甲醇季节和空间分布的初步全球结果。文中描述了TES甲醇反演的全面发展过程,包括微窗口选择、误差分析以及利用GEOS - Chem化学传输模型提供的先验和初始猜测信息。使用所开发的反演策略进行的反演模拟和敏感性分析表明,TES:(i)通常提供的信息量小于1.0;(ii)在对流层低层较为敏感,在垂直分辨率约为5 km时,峰值敏感性通常出现在约900 - 700 hPa(约1 - 3 km)之间;(iii)根据大气条件,可检测限在0.5至1.0 ppbv代表性体积混合比(RVMR)之间,大致对应于最大浓度至少为1至2 ppbv的廓线;(iv)在模拟环境中,平均偏差为0.16 ppbv,标准偏差为0.34 ppbv。在全球范围内应用新推导的TES反演方法,并将结果与相应的GEOS - Chem输出进行比较,我们发现两者之间总体上存在一致的大尺度模式。然而,在北半球春季、夏季和秋季,TES常常显示出比模拟值更高的甲醇浓度。在南半球,TES甲醇观测结果表明,从12月到7月,模型在南美洲大部分地区高估了甲醇浓度,而在生物质燃烧季节则低估了甲醇浓度。