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A secondary organic aerosol formation model considering successive oxidation aging and kinetic condensation of organic compounds: global scale implications

机译：考虑有机化合物的连续氧化老化和动力学缩合的二级有机气溶胶形成模型：全球规模的意义

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The widely used two-product secondary organic aerosol(SOA) formation model has been extended in this study to consider thevolatility changes of secondary organic gases (SOG) arising from the agingprocess as well as the kinetic condensation of low volatile SOG (LV-SOG). Inaddition to semi-volatile SOG (SV-SOG) with saturation vapor pressure at290 K (C*290) in the range of ~3 ppt–3 ppb and medium-volatile SOG (MV-SOG)with C*290in the range of ~0.3–300 ppb, we add a third componentrepresenting LV-SOG with C*290below ~3 ppt and design a scheme to transfer MV-SOG to SV-SOG andSV-SOG to LV-SOG associated with oxidation aging. This extended SOAformation model has been implemented in a global aerosol model (GEOS-Chem)and the co-condensation of H2SO4 and LV-SOG on pre-existingparticles is explicitly simulated. We show that, over many parts of thecontinents, LV-SOG concentrations are generally a factor of ~2–20higher than those of H2SO4 and the kinetic condensation of LV-SOGsignificantly enhances particle growth rates. Comparisons of the simulatedand observed evolution of particle size distributions at a boreal forestsite (Hyyti?l?, Finland) clearly show that LV-SOG condensation iscritical in order to bring the simulations closer to the observations. Withthe new SOA formation scheme, annual mean SOA mass increases by a factor of2–10 in many parts of the boundary layer and reaches above 0.5 μg m?3in most parts of the main continents, improving the agreement withaerosol mass spectrometer (AMS) SOA measurements. While the new schemegenerally decreases the concentration of condensation nuclei larger than 10 nm by 3–30%in the lower boundary layer as a result of enhanced surfacearea and reduced nucleation rates, it substantially increases theconcentration of cloud condensation nuclei at a water supersaturation ratioof 0.2%, ranging from ~5–20% over a large fraction of oceans andhigh latitude continents to more than 50% over some parts of SouthAmerica, Australia, and Indonesia. Our study highlights the importance forglobal aerosol models to explicitly account for the oxidation aging of SOGsand their contribution to particle growth.
机译：本研究扩展了广泛使用的两产品二次有机气溶胶（SOA）形成模型，以考虑由于老化过程引起的二次有机气体（SOG）的挥发性变化以及低挥发性SOG（LV-SOG）的动态缩合。除了饱和蒸气压为290 K（ C * 290 ）且饱和蒸汽压在〜3 ppt范围内的半挥发性SOG（SV-SOG）之外–3 ppb和中挥发性的SOG（MV-SOG）， C * 290 在〜0.3–300 ppb的范围内，表示LV-SOG的 C * 290 低于〜3 ppt的第三部分，并设计了将MV-SOG转移到SV-SOG和SV-从SOG到LV-SOG伴随着氧化老化。此扩展的SOAformation模型已在全局气溶胶模型（GEOS-Chem）中实施，H 2 SO 4 和LV-SOG在预先存在的粒子上的共冷凝为明确模拟。我们发现，在大陆的许多地方，LV-SOG的浓度通常比H 2 SO 4 高约2-20倍，并且LV的动力学凝聚-SOG显着提高了颗粒的生长速度。比较和观察了北方森林地带（Hyytil ?，芬兰）的粒径分布演变的模拟结果清楚地表明，LV-SOG凝结是至关重要的，以便使模拟更接近观测结果。借助新的SOA形成方案，边界层许多地方的年均SOA质量增加了2-10倍，并且在主要大陆的大部分地区达到了0.5μgm ？3 以上，从而改善了一致性气溶胶质谱仪（AMS）SOA测量。由于表面积增加和成核速率降低，新方案通常使下边界层中大于10 nm的凝结核浓度降低3–30％，但在水过饱和比为0.2％时，它实质上增加了云凝结核的浓度。范围从大洋和高纬度大陆的约5-20％，到南美，澳大利亚和印度尼西亚的某些地区的50％以上。我们的研究凸显了全球气溶胶模型对于明确解释SOG的氧化老化及其对颗粒生长的贡献的重要性。

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