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Abstract: Organic matter (OM) constitutes an important contribution to the composition of sub-micron sea-spray aerosol produced from biologically active waters. However, OM emission estimates vary by more than an order of magnitude. To estimate the uncertainties in the OM production estimates a sensitivity analysis has been performed in which various parameters have been varied. These include different sea-spray source functions, satellite-retrieved chlorophyll distributions, and a relationship correlating in situ organic mass measurements with satellite-retrieved chlorophyll data. The starting point was a baseline model from which the annual global emission of the water insoluble organic matter (WIOM) fraction in sea spray has been estimated to be 20.4 Tg. In this baseline the global WIOM emission is dominated by the contribution (80%) of the chlorophyll-poor regions (<0.3 mg m−3). Significant deviations from this estimate are introduced by the choice of the sea-spray source function and the assumed background organic mass fraction, each of which leads to an uncertainty of at least a factor of 2. In particular the chlorophyll-poor regions which dominate the WIOM contribution are strongly affected by the choice of the organic mass fraction parameterisation. The way the chlorophyll data are handled, such as different gap filling approaches, causes deviations in the OM emission that are in the order of 10% and is therefore of less importance. The present research indicates that special attention should be given to the low chlorophyll areas in e.g. the tropics, since there the parameterisations are most uncertain and at the same time these regions dominate total WIOM emissions. [Copyright &y& Elsevier]

Abstract: The chemical composition of marine aerosols as a function of their size is an important parameter for the evaluation of their impact on the global climate system. In this work we model fine particle organic matter emitted by sea spray processes and its influence on the aerosol chemical properties at the global scale using the off-line global Chemistry-Transport Model TM5. TM5 is coupled to a microphysical aerosol dynamics model providing size resolved information on particle masses and numbers. The mass of the emitted sea spray particles is partitioned between water insoluble organic matter (WIOM) and sea salt components in the accumulation mode using a function that relates the emitted organic fraction to the surface ocean chlorophyll-a concentrations. The global emission in the sub-micron size range of organic matter by sea spray process is 8.2 Tg yr−1, compared to 24 Tg fine yr−1 sea-salt emissions. When the marine sources are included, the concentrations of modelled primary particulate organic matter (POM) increase mainly over the oceans. The model predictions of WIOM and sea salt are evaluated against measurements carried out at Mace Head (Northern Hemisphere) and Amsterdam Island (Southern Hemisphere), showing that in clean marine conditions WIOM marine emissions contribute significantly to POM values. [Copyright &y& Elsevier]