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[1] Initial efforts toward developing a combined organic-inorganic sea spray source function parameterization for large-scale models made use of chlorophyll-a (Chl-a) and wind speed as input parameters to combine oceanic biology and atmospheric dynamics. These studies reported a modest correlation coefficient (0.55) between chlorophyll-a and organic matter (OM) enrichment in sea spray, suggesting that chlorophyll-a is only partially suitable for predicting organic enrichment. A reconstructed chlorophyll-a field of the North Atlantic Ocean from GlobColour reveals an improved correlation of 0.72 between the fractional mass contribution of organics in sea spray and chlorophyll-a concentration. A similar analysis, using colored dissolved and detrital organic material absorption and particulate organic carbon concentration, revealed slightly lower correlation coefficients (0.65 and 0.68). These results indicate that to date, chlorophyll-a is the best biological surrogate for predicting sea spray organic enrichment. In fact, considering the minimal difference between the correlation coefficients obtained with the three ocean color products, there is no reason to substitute chlorophyll-a, which is the most accurate parameter obtained from ocean color data, with other biological surrogates being generally affected by larger and less known errors. The observed time lag between chlorophyll-a concentration and organic matter enrichment in aerosol suggests that biological processes in oceanic surface waters and their timescales should be considered when modeling the production of primary marine organic aerosol.Citation: Rinaldi, M., et al. (2013), Is chlorophyll-a the best surrogate for organic matter enrichment in submicron primary marine aerosol?,

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Bursting bubbles at the ocean-surface produce airborne salt-water spray-droplets, in turn, forming climate-cooling marine haze and cloud layers. The reflectance and ultimate cooling effect of these layers is determined by the spray’s water-uptake properties that are modified through entrainment of ocean-surface organic matter (OM) into the airborne droplets. We present new results illustrating a clear dependence of OM mass-fraction enrichment in sea spray (OMss) on both phytoplankton-biomass, determined from Chlorophyll-a (Chl-a) and Net Primary Productivity (NPP). The correlation coefficient for OMss as a function of Chl-a increased form 0.67 on a daily timescale to 0.85 on a monthly timescale. An even stronger correlation was found as a function of NPP, increasing to 0.93 on a monthly timescale. We suggest the observed dependence is through the demise of the bloom, driven by nanoscale biological processes (such as viral infections), releasing large quantities of transferable OM comprising cell debris, exudates and other colloidal materials. This OM, through aggregation processes, leads to enrichment in sea-spray, thus demonstrating an important coupling between biologically-driven plankton bloom termination, marine productivity and sea-spray modification with potentially significant climate impacts.