1Department of Civil and Environmental Engineering, Carnegie Mellon University, Pittsburgh, PA, USA
2School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA, USA
3School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, GA, USA
4Department of Engineering and Public Policy, Carnegie Mellon University, Pittsburgh, PA, USA
Received: 08 Feb 2011 – Published in Atmos. Chem. Phys. Discuss.: 16 Feb 2011
Abstract. This work estimates the primary marine organic aerosol global emission source and its impact on cloud condensation nuclei (CCN) concentrations by implementing an organic sea spray source function into a series of global aerosol simulations. The source function assumes that a fraction of the sea spray emissions, depending on the local chlorophyll concentration, is organic matter in place of sea salt. Effect on CCN concentrations (at 0.2% supersaturation) is modeled using the Two-Moment Aerosol Sectional (TOMAS) microphysics algorithm coupled to the GISS II-prime general circulation model. The presence of organics affects CCN activity in competing ways: by reducing the amount of solute available in the particle and decreasing surface tension of CCN. To model surfactant effects, surface tension depression data from seawater samples taken near the Georgia coast were applied as a function of carbon concentrations. A global marine organic aerosol emission rate of 17.7 Tg C yr−1 is estimated from the simulations. Marine organics exert a localized influence on CCN(0.2%) concentrations, decreasing regional concentrations by no more than 5% and by less than 0.5% over most of the globe, assuming direct replacement of sea salt aerosol with organic aerosol. The decrease in CCN concentrations results from the fact that the decrease in particle solute concentration outweighs the organic surfactant effects. The low sensitivity of CCN(0.2%) to the marine organic emissions is likely due to the small compositional changes: the mass fraction of OA in accumulation mode aerosol increases by only ~15% in a biologically active region of the Southern Ocean. To test the sensitivity to uncertainty in the sea spray emissions process, we relax the assumption that sea spray aerosol number and mass remain fixed and instead can add to sea spray emissions rather than replace existing sea salt. In these simulations, we find that marine organic aerosol can increase CCN by up to 50% in the Southern Ocean and 3.7% globally during the austral summer. This vast difference in CCN impact highlights the need for further observational exploration of the sea spray aerosol emission process as well as evaluation and development of model parameterizations.
Revised: 07 Oct 2011 – Accepted: 16 Dec 2011 – Published: 02 Jan 2012
Westervelt, D. M., Moore, R. H., Nenes, A., and Adams, P. J.: Effect of primary organic sea spray emissions on cloud condensation nuclei concentrations, Atmos. Chem. Phys., 12, 89-101, doi:10.5194/acp-12-89-2012, 2012.