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Publication abstract: To elucidate the seawater biological and physicochemical factors driving differences in organic composition between supermicron and submicron sea spray aerosol (SSAsuper and SSAsub), carbon isotopic composition (δ13C) measurements were performed on size segregated, nascent SSA collected during a phytoplankton bloom mesocosm experiment. The δ13C measurements indicate that SSAsuper organic composition resembles 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 SSAsuper with the proportional contribution being modulated by bacterial activity, emphasizing the importance of the microbial loop in controlling the organic composition of SSAsuper. Conversely, SSAsub exhibited no apparent relationship with biological activity, but correlated 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 SSAsub organic composition strongly depends on surfactants present at the air sea interface that are transferred into SSAsub by bubble bursting. Our findings illustrate the substantial impact of seawater dynamics on the pronounced organic compositional differences between SSAsuper and SSAsub, and demonstrate that these two SSA populations should be considered separately when assessing their contribution to marine aerosols and climate. Research Data Curation Program, UC San Diego, La Jolla, 92093-0175 (https://lib.ucsd.edu/rdcp) Crocker, Daniel R.; Kaluarachchi P. Chathuri; Cao, Ruochen; Dinasquet, Julie; Franklin, Emily B.; Morris, Clare K.; Nguyen, Tran; Torres, Ralph R.; Martz, Todd R.; Malfatti, Francesca; Goldstein, Allen H.; Tivanski, Alexei V.; Prather, Kimberly A.; Thiemens, Mark H. (2021). Data from: Isotopic Insights into Organic Composition Differences between Supermicron and Submicron Sea Spray Aerosol. In Center for Aerosol Impacts on Chemistry of the Environment (CAICE). UC San Diego Library Digital Collections. https://doi.org/10.6075/J0416X7M