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Evaluating secondary inorganic aerosols in three dimensions

机译:在三维中评估二级无机气溶胶

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The spatial distribution of aerosols and their chemical composition dictates whether aerosols have a cooling or a warming effect on the climate system. Hence, properly modeling the three-dimensional distribution of aerosols is a crucial step for coherent climate simulations. Since surface measurement networks only give 2-D data, and most satellites supply integrated column information, it is thus important to integrate aircraft measurements in climate model evaluations. In this study, the vertical distribution of secondary inorganic aerosol (i.e., sulfate, ammonium, and nitrate) is evaluated against a collection of 14 AMS flight campaigns and surface measurements from 2000 to 2010 in the USA and Europe. GISS ModelE2 is used with multiple aerosol microphysics (MATRIX, OMA) and thermodynamic (ISORROPIA II, EQSAM) configurations. Our results show that the MATRIX microphysical scheme improves the model performance for sulfate, but that there is a systematic underestimation of ammonium and nitrate over the USA and Europe in all model configurations. In terms of gaseous precursors, nitric acid concentrations are largely underestimated at the surface while overestimated in the higher levels of the model. Heterogeneous reactions on dust surfaces are an important sink for nitric acid, even high in the troposphere. At high altitudes, nitrate formation is calculated to be ammonia limited. The underestimation of ammonium and nitrate in polluted regions is most likely caused by a too simplified treatment of the NH3?∕?NH4+ partitioning which affects the HNO3?∕?NO3? partitioning.
机译:气溶胶及其化学成分的空间分布决定了气溶胶是否对气候系统具有冷却或温暖效果。因此,适当地建模气溶胶的三维分布是用于相干气候模拟的重要步骤。由于表面测量网络仅提供2-D数据,并且大多数卫星提供集成列信息,因此必须在气候模型评估中集成飞机测量值。在该研究中,评估二级无机气溶胶(即硫酸盐,铵和硝酸铵)的垂直分布,从2000年到2010年在美国和欧洲的2000年到2010年收集14个AMS飞行竞选和表面测量。 Giss Modele2与多种气溶胶微生物(矩阵,OMA)和热力学(Isorropia II,EQSAM)配置一起使用。我们的研究结果表明,基质微物理方案提高了硫酸盐的模型性能,但在所有模型配置中,在美国和欧洲的铵和硝酸盐有系统低估。就气体前体而言,硝酸浓度在大部分在表面上大约低估,同时在模型的较高水平中估计。灰尘表面的异质反应是硝酸的重要水槽,甚至在对流层中高。在高海拔地区,计算硝酸盐形成为氨限制。在污染区域中低估铵和硝酸盐很可能是由对NH3的过度简化的治疗引起的NH 3?/θnH4+分区,这会影响HNO3?/?NO3?分区。

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