A dynamic link between ice nucleating particles released in nascent sea spray aerosol and oceanic biological activity during two mesocosm experiments

Emission rates and properties of ice nucleating particles (INPs) are required for proper representation of aerosol-cloud interactions in atmospheric models. Few investigations have quantified marine INP emissions, a potentially important INP source for remote oceanic regions. Previous studies have suggested INPs in sea spray aerosol (SSA) are linked to oceanic biological activity. This proposed link was explored in this study by measuring INP emissions from nascent SSA during phytoplankton blooms during two mesocosm experiments. In a Marine Aerosol Reference Tank (MART) experiment, a phytoplankton bloom was produced with chlorophyll-a (Chl a) concentrations reaching 39 μg L^-1, while Chl a concentrations more representative of natural ocean conditions were obtained during the Investigation into Marine Particle Chemistry and Transfer Science (IMPACTS; peak Chl a of 5 μg L^-1) campaign, conducted in the University of California, San Diego, wave flume. Dynamic trends in INP emissions occurred for INPs active at temperatures > -30°C. Increases in INPs active between -25° and -15°C lagged the peak in Chl a in both studies, suggesting a consistent population of INPs associated with the collapse of phytoplankton blooms. Trends in INP emissions were also compared to aerosol composition, abundances of microbes, and enzyme activity. In general, increases in INP concentrations corresponded to increases in organic species in SSA and the emissions of heterotrophic bacteria, suggesting that both microbes and biomolecules contribute to marine INP populations. INP trends were not directly correlated with a single biological marker in either study. Direct measurements of INP chemistry are needed to accurately identify particles types contributing to marine INP populations.