Physical and biogeochemical processes in seawater controlling primary marine aerosol (PMA) production and composition are poorly understood and associated with large uncertainties in estimated fluxes into the atmosphere. PMA production was investigated in the biologically productive NE Pacific Ocean and in biologically productive and oligotrophic regions of the NW Atlantic Ocean. Physicochemical properties of model PMA, produced by aeration of fresh seawater under controlled conditions, were quantified. Diel variability in model PMA mass and number fluxes was observed in biologically productive waters, increasing following sunrise and decreasing to predawn levels overnight. Such variability was not seen in oligotrophic waters. During daytime, surfactant scavenging by aeration in the aerosol generator without replenishing the seawater in the reservoir reduced the model PMA production in productive waters to nighttime levels but had no influence on production from oligotrophic waters. Results suggest bubble plume interactions with sunlight-mediated biogenic surfactants in productive seawater significantly enhanced model PMA production. Key Points Surface ocean biogeochemistry mediates physics of marine aerosol production Diel cycles in biologically productive surface seawater mediate production Observations show chemical processes affecting mass and number production fluxes © 2014. American Geophysical Union. All Rights Reserved.