Abstract
Abstract. Marine-sourced organic aerosols (MOAs) have been shown to play an important role in tropospheric chemistry by impacting surface mass, cloud condensation nuclei, and ice nuclei concentrations over remote marine and coastal regions. In this work, an online marine primary organic aerosol emission parameterization, designed to be used for both global and regional models, was implemented into the GEOS-Chem (Global Earth Observing System Chemistry) model. The implemented emission scheme improved the large underprediction of organic aerosol concentrations in clean marine regions (normalized mean bias decreases from −79% when using the default settings to −12% when marine organic aerosols are added). Model predictions were also in good agreement (correlation coefficient of 0.62 and normalized mean bias of −36%) with hourly surface concentrations of MOAs observed during the summertime at an inland site near Paris, France. Our study shows that MOAs have weaker coastal-to-inland concentration gradients than sea-salt aerosols, leading to several inland European cities having >10% of their surface submicron organic aerosol mass concentration with a marine source. The addition of MOA tracers to GEOS-Chem enabled us to identify the regions with large contributions of freshly emitted or aged aerosol having distinct physicochemical properties, potentially indicating optimal locations for future field studies.
Highlights
With the decrease in anthropogenic emissions of particulate matter in many industrialized countries, an increased emphasis has been placed on understanding the inventory of natural aerosol sources (Zare et al, 2014)
The Marine-sourced organic aerosols (MOAs) factor observed in Paris in the summertime by Crippa et al (2013a, b) was not detected in the wintertime (Crippa et al, 2013b, c) because the contribution to total OA was below the detection limit of ∼ 20 ng m−3 (DeCarlo et al, 2006)
The summertime MOA concentrations and marine primary organic aerosols (POAs) emissions predicted by GEOS-Chem were higher in the Northern Hemisphere than in the Southern Hemisphere despite having lower sea spray aerosol (SSA) emissions; this was related to the higher OMSSA in the Northern Hemisphere which is positively related to [chl a] and negatively related to U10 using a logistic curve for both relationships
Summary
With the decrease in anthropogenic emissions of particulate matter in many industrialized countries, an increased emphasis has been placed on understanding the inventory of natural aerosol sources (Zare et al, 2014). Marine-sourced organic aerosols (MOAs), which have been observed at concentrations > 1.0 μg m−3 (Ovadnevaite et al, 2011) and whose estimated global emissions are comparable to that of fossil fuel burning (Spracklen et al, 2008), are one type of natural aerosol with air quality and climate significance (Gantt and Meskhidze, 2013). Uncertainty in the chemical composition of sea spray aerosol (SSA) has been shown to play an important role in determining their climate impact (Tsigaridis et al, 2013). It is important for chemical transport and climate models to take MOA emissions and physicochemical processes into consideration
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