Springtime transitions of NO2, CO, and O3 over North America: Model evaluation and analysis
Springtime transitions of NO2, CO, and O3 over North America: Model evaluation and analysis
复制标题
DOI：
10.1029/2007jd009632
复制
发表时间：
2008-10-24
影响因子：
4.4
通讯作者：
Edgerton, Eric
中科院分区：
文献类型：
--
作者：
Choi, Yunsoo;Wang, Yuhang;Edgerton, Eric
来自AIRNow和东南气溶胶研究和表征研究网络的地面观测、来自空客在役飞机计划的臭氧和水蒸气测量的飞机观测、臭氧探测仪以及来自全球臭氧绘图实验的遥感测量、总臭氧绘图光谱仪（TOMS）、和平流层气溶胶和气体实验（SAGE）二，2000年2月至5月在北美地区的春季转换的特征O-3及其前体。这些测量提供了一个全面的数据集，以评估的3-D区域化学传输模式（REAM）的性能。应用该模型分析了影响春季微量气体浓度转换和输出的关键因素。全球GEOS-CHEM模式用于提供化学初始和边界条件。一般来说，模式的结果是在对流层中的观测，除了对流层上层的O-3的低偏差，偏差减少向夏季和低纬度。REAM对春季观测到的地表O-3增加速率进行了较好的模拟。地球观测化学对美国东部的估计过高。驱动模式差异的一个关键因素是白天混合深度。在REAM中的浅边界层导致更有效地去除自由基，因此在春天，当初级自由基源相对较小时，光化学的激活较慢。REAM和GEOS-CHEM之间化石燃料氮氧化物排放量自上而下的估计值的比较显示了模型的依赖性。相关的不确定性每月高达20%。取一个赛季的平均值可以减少这种不确定性。虽然对流层柱NO2在大陆上减少，但由于闪电产生的NOx，它在北大西洋西部增加。因此，REAM模式模拟了该地区对流层O-3的显着增加，如TOMS-SAGE II的列数据所示。闪电的影响在模型模拟的氮氧化物排放中也很明显。
Surface observations from AIRNow and Southeastern Aerosol Research and Characterization Study networks, aircraft observations from the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft program, ozonesondes, and remote sensing measurements from Global Ozone Mapping Experiment, Total Ozone Mapping Spectrometer (TOMS), and Stratospheric Aerosol and Gas Experiment (SAGE) II for February-May 2000 over North America are used to characterize the springtime transitions of O-3 and its precursors. These measurements provide a comprehensive data set to evaluate the performance of the 3-D Regional Chemical Transport Model (REAM). The model is then applied to analyze the key factors affecting the springtime transitions of trace gas concentrations and export. The global GEOS-CHEM model is used to provide chemical initial and boundary conditions. Generally, the model results are in good agreement with the observations in the troposphere except for a low bias of upper tropospheric O-3; the bias decreases toward the summer and lower latitudes. The rate of observed surface O-3 increase in spring is simulated well by REAM. It is overestimated by GEOS-CHEM over the eastern United States. A key factor driving the model difference is daytime mixing depth. A shallow boundary layer in REAM leads to more efficient removal of radicals and hence slower activation of photochemistry in spring, when the primary radical source is relatively small. Comparison of top-down estimates of fossil fuel NOx emissions between REAM and GEOS-CHEM shows model dependence. The associated uncertainty is up to 20% on a monthly basis. Averaging over a season reduces this uncertainty. While tropospheric column NO2 decreases over the continent, it increases over the western North Atlantic due to lightning NOx production. Consequently, the REAM model simulates significant increases of tropospheric O-3 over the region as indicated by column data derived from TOMS-SAGE II. Lightning impact is also evident in model-simulated NOx exports.