Primary marine aerosol physical flux and chemical composition during a nutrient enrichment experiment in mesocosms in the Mediterranean Sea

Abstract. While primary marine aerosol (PMA) is an important part of global aerosol total emissions, its chemical composition and physical flux as a function of the biogeochemical properties of the seawater still remain highly uncharacterized due to the multiplicity of physical, chemical and biological parameters that are involved in the emission process. Here, two nutrient-enriched mesocosms and one control mesocosm, both filled with Mediterranean seawater, were studied over a 3-week period. PMA generated from the mesocosm waters were characterized in term of chemical composition, size distribution and size-segregated cloud condensation nuclei (CCN), as a function of the seawater chlorophyll a (Chl a) concentration, pigment composition, virus and bacteria abundances. The aerosol number size distribution flux was primarily affected by the seawater temperature and did not vary significantly from one mesocosm to the other. The aerosol number size distribution flux was primarily affected by the seawater temperature and did not vary significantly from one mesocosm to the other. Particle number and CCN aerosol fluxes increase by a factor of 2 when the temperature increases from 22 to 32 °C, for all particle submicron sizes. This effect, rarely observed in previous studies, could be specific to oligotrophic waters and/or to this temperature range. In all mesocosms (enriched and control mesocosms), we detected an enrichment of calcium (+500 %) and a deficit in chloride (−36 %) in the submicron PMA mass compared to the literature inorganic composition of the seawater. There are indications that the chloride deficit and calcium enrichment are linked to biological processes, as they are found to be stronger in the enriched mesocosms. This implies a non-linear transfer function between the seawater composition and PMA composition, with complex processes taking place at the interface during the bubble bursting. We found that the artificial phytoplankton bloom did not affect the CCN activation diameter (D_{p, 50, average} = 59.85±3.52 nm and D_p,50,average = 93.42±5.14 nm for supersaturations of 0.30 and 0.15 % respectively) or the organic fraction of the submicron PMA (average organic to total mass  =  0.31±0.07) compared to the control mesocosm. Contrary to previous observations in natural bloom mesocosm experiments, the correlation between the particle organic fraction and the seawater Chl a was poor, indicating that Chl a is likely not a straightforward proxy for predicting, on a daily scale, PMA organic fraction in models for all types of sea and ocean waters. Instead, the organic fraction of the Aitken mode particles were more significantly linked to heterotrophic flagellates, viruses and dissolved organic carbon (DOC). We stress that different conclusions may be obtained in natural (non-enriched) or non-oligotrophic systems.