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Global Modeling of Secondary Organic Aerosol With Organic Nucleation

机译:有机成核的二次有机气溶胶的全球造型

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Organic nucleation has been identified as an important way to form secondary organic aerosol (SOA) and change the number concentration of aerosol and thus its climate effect. A global atmospheric chemistry model is developed to include a comprehensive organic nucleation scheme that includes heteromolecular nucleation of sulfuric acid and organics, neutral pure organic nucleation, and ion‐induced pure organic nucleation. Our model simulation shows reasonable agreement with the seasonal as well as spatial pattern of organic carbon concentration in America, while it fails to predict the seasonal pattern of organic carbon in Europe due to the lack of sharp increases in primary organic aerosol emissions in the winter. Including organic nucleation decreases the bias of the annual average particle number concentration at 54% of the available observation sites and increases the temporal correlation coefficients at 58% of the sites. Ion‐induced pure organic nucleation contributes the most to the total organic nucleation rate, which peaks around 400 hPa in the tropics. Heteromolecular nucleation of sulfuric acid and organics dominates the total organic nucleation rate in the summer and mostly occurs in the lower troposphere. The number concentration of particles formed from organic nucleation (newSOA) in the nucleation and Aitken modes is highest in the tropics, while accumulation mode newSOA is highest in the Northern Hemisphere due to growth as a result of the condensation of sulfate. Three sensitivity experiments suggest that more studies are needed to investigate the formation mechanism of newSOA, so that a more accurate simulation of the spatial and size distribution of newSOA can be developed.
机译:有机成核已被鉴定为形成二次有机气溶胶(SOA)并改变气溶胶的数量浓度,从而确定其气候效应。开发了全局大气化学模型,包括综合有机成核方案,包括硫酸和有机物,中性纯的有机成核和离子诱导的纯有机成核的异形核心。我们的模型仿真显示了美国的季节性以及美国有机碳浓度的空间模式的合理协议,而由于冬季原发性有机气溶胶排放缺乏急剧增加,它未能预测欧洲有机碳的季节性模式。包括有机成核将年平均粒子数浓度的偏差降低54%的可用观察位点,并增加58%的位点的时间相关系数。离子诱导的纯有机成核导致总有机成核速率最大,其在热带地带中达到400 HPA左右。硫酸和有机物的异质成核在夏季占据了总有机成核速率,大部分发生在对流层下方。在核心和Aitken模式中由有机成核(Newsoa)形成的颗粒的数量浓度在热带地区中最高,而纽约半球在北半球的累积模式最高,由于硫酸盐的缩合,北半球是最高的。三种敏感性实验表明,需要更多的研究来研究Newsoa的形成机制,从而可以开发更准确地模拟纽索达的空间和尺寸分布。

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