Implementation of state-of-the-art ternary new-particle formation scheme to the regional chemical transport model PMCAMx-UF in Europe
Implementation of state-of-the-art ternary new-particle formation scheme to the regional chemical transport model PMCAMx-UF in Europe
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DOI：
10.5194/gmd-9-2741-2016
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发表时间：
2016-08-22
影响因子：
5.1
通讯作者：
Riipinen, Ilona
中科院分区：
文献类型：
--
作者：
Baranizadeh, Elham;Murphy, Benjamin N.;Riipinen, Ilona
PMCAMx-UF是一个三维化学输运模式，利用ACDC模拟的H2SO 4-NH3-H2O三元路径的粒子生成速率，对PMCAMx-UF中的粒子生成方案进行了更新。该模型于2008年5月应用于欧洲，在此期间开展了EUCAARI-LONGREX（欧洲气溶胶云气候和空气质量相互作用-远程实验）活动，提供了飞机上气溶胶数浓度的垂直廓线。更新后的模型再现了整个大气柱中大于4 nm的颗粒物在1个数量级内的观测数浓度。考虑到不需要半经验拟合来获得现实的颗粒形成速率，该协议是令人鼓舞的。还用对流层紫外线和可见光辐射传输模式更新了用于修改PMCAMx-UF中光解率廓线的云调整方案。结果表明，尽管新的云调整方案对总粒子数浓度的影响很小，但预测在多云地区附近会有增强的新粒子形成。这是由于云层上方和附近的辐射增强，这反过来又导致硫酸产量增加。还讨论了结果的敏感性，包括从自然源的排放。
The particle formation scheme within PMCAMx-UF, a three-dimensional chemical transport model, was updated with particle formation rates for the ternary H2SO4-NH3-H2O pathway simulated by the Atmospheric Cluster Dynamics Code (ACDC) using quantum chemical input data. The model was applied over Europe for May 2008, during which the EUCAARI-LONGREX (European Aerosol Cloud Climate and Air Quality Interactions-Long-Range Experiment) campaign was carried out, providing aircraft vertical profiles of aerosol number concentrations. The updated model reproduces the observed number concentrations of particles larger than 4 nm within 1 order of magnitude throughout the atmospheric column. This agreement is encouraging considering the fact that no semi-empirical fitting was needed to obtain realistic particle formation rates. The cloud adjustment scheme for modifying the photolysis rate profiles within PMCAMx-UF was also updated with the TUV (Tropospheric Ultraviolet and Visible) radiative-transfer model. Results show that, although the effect of the new cloud adjustment scheme on total number concentrations is small, enhanced new-particle formation is predicted near cloudy regions. This is due to the enhanced radiation above and in the vicinity of the clouds, which in turn leads to higher production of sulfuric acid. The sensitivity of the results to including emissions from natural sources is also discussed.