Isotopic Insights into Organic Composition Differences between Supermicron and Submicron Sea Spray Aerosol

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Abstract

To elucidate the seawater biological and physicochemical factors driving differences in organic composition between supermicron and submicron sea spray aerosol (SSA_super and SSA_sub), carbon isotopic composition (δ13C) measurements were performed on size-segregated, nascent SSA collected during a phytoplankton bloom mesocosm experiment. The δ13C measurements indicate that SSA_super contains a mixture of particulate and dissolved organic material in the bulk seawater. After phytoplankton growth, a greater amount of freshly produced carbon was observed in SSA_super with the proportional contribution being modulated by bacterial activity, emphasizing the importance of the microbial loop in controlling the organic composition of SSA_super. Conversely, SSA_sub exhibited no apparent relationship with biological activity but tracked closely with surface tension measurements probing the topmost ∼0.2-1.5 μm of the sea surface microlayer. This probing depth is similar to a bubble's film thickness at the ocean surface, suggesting that SSA_sub organic composition may be influenced by the presence of surfactants at the air-sea interface that are transferred into SSA_sub by bubble bursting. Our findings illustrate the substantial impact of seawater dynamics on the pronounced organic compositional differences between SSA_super and SSA_sub and demonstrate that these two SSA populations should be considered separately when assessing their contribution to marine aerosols and climate.

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