New insights into modeling an organic mass fraction of sea spray aerosol

As the study of climate change progresses, a need to separate the effects of natural and anthropogenic processes becomes essential in order to correctly forecast the future climate. Due to their massive source regions underlying an atmosphere with low aerosol concentration, marine aerosols derived from sea spray and ocean emitted biogenic volatile organic compounds (BVOCs) are extremely important for the Earth’s radiative budget, regional air quality and biogeochemical cycling of elements. Measurements of freshly-emitted sea spray have revealed that bubble bursting processes, largely responsible for the production of sea salt aerosol, also control sea-to-air transfer of marine organic matter. It has been established that the organic mass fraction of sea spray can be a function of sea-water composition (e.g., concentrations of Chlorophyll-a, [Chl-a], dissolved organic carbon, [DOC], particulate organic carbon, [POC], types of organic carbon, and the amount of surfactants). Current paramaterizations of marine primary organic aerosol emissions use remotely sensed [Chl-a] data as a proxy for oceanic biological activity. However, it has also been shown that the path length, size, and lifetime of bubbles in seawater as well as spatial coverage of seawater surface by streaks or slicks (visible film of a roughly 50 μm thick layer, highly enriched in organics) can have dramatic effect on organic mass fraction of sea spray (OCss). Dynamics of bubble entrainment and the level of microlayer enrichment by organics relative to the underlying bulk water can be controlled by surface wind speed. For bubble entrainment, high winds can increase rising bubble path length and therefore the amount of organics scavenged by the bubble. However, when the surface wind speeds exceed 8 m s-1 breaking of ocean waves can entirely destroy surface organic films and diminish the amount of organics leaving the sea. Despite the probable impact of wind speed, existing parameterizations do not consider the wind speed dependence of OCss. In this study we use remotely sensed data for ocean slick coverage and surface wind speed in conjunction with an upwind averaged concentrations of [Chl-a], [DOC] and [POC] to derive marine primary organic aerosol emission function. Derived empirical relationships between the aerosol and ocean/meteorological data are then compared to observed OCss at Mace Head and Point Reyes National Seashore. MATLAB curve fitting tool revealed that multi-variable regression analysis (with both wind speed and [Chl-a]) yields a significant improvement between model predicted and observed submicron fraction of OCss. The coefficient of determination increased from R2=0.1 for previous parameterizations to R2=0.6. Based on the results of this study we propose that in addition to sea-water composition, future parameterizations of marine primary organic aerosol emissions should include sea spray organic mass fraction dependence on surface wind speed.