Sea spray aerosol (SSA) generated by bubble bursting at the ocean surface is an important component of aerosol‐cloud interactions over remote oceans, providing the atmosphere with ice‐nucleating particles (INPs) or particles required for heterogeneous ice nucleation. Studies have shown that organic INPs are emitted during phytoplankton blooms, but changes in INP number concentrations (nINPs) due to ocean biological activity have not been directly demonstrated in natural SSA. In this study, a clean sector sampler was used to differentiate ice nucleation and composition of pristine SSA from terrestrial aerosol at the Mace Head Research Station in August 2015. Average nINPs active at −15 °C (nINPs,−15 °C) were 0.0011 L−1, and large variability (up to a factor of 200) was observed for INPs active warmer than −22 °C. Highest nINPs in the clean sector occurred during a period of elevated marine organic aerosol from offshore biological activity (M1, nINPs,−15 °C = 0.0077 L−1). A peak in nINPs was also observed in terrestrial organic aerosol (T1, nINPs,−15 °C = 0.0076 L−1). The impacts of heating and hydrogen peroxide digestion on nINPs indicate that INPs at Mace Head Research Station were largely organic and that INPs observed during M1 and T1 were biological (i.e., protein containing). Complexities of predicting increases in nINPs due to offshore biological activity are explored. A parameterization for pristine SSA INPs over the North Atlantic Ocean was developed, illustrating that SSA is associated with a factor of 1,000 fewer ice‐nucleating sites per surface area of aerosol compared to mineral dust.

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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.