Modeling the chemistry of the marine boundary layer: Sulphate formation and the role of sea-salt aerosol particles

Abstract

A one-dimensional model is presented that interactively simulates the dynamics and the gas-aqueous phase chemistry of the cloud-topped marine boundary layer. The model is described and tested using observations from the Atlantic Stratocumulus Transition Experiment/Marine Aerosol and Gas Exchange (ASTEX/MAGE) measurement campaign. The comparison generally indicates satisfactory agreement for dynamical properties and chemical species, except for SO2. We present several explanations for this discrepancy. However, a conclusive account is dependent on quantitative information about free tropospheric SO2 and H2O2 that is not available. Furthermore, a series of sensitivity runs is presented to explain the large quantities of non-sea-salt sulphate associated with sea-salt particles, as observed during ASTEX/MAGE. The main conclusions are that most sulphate associated with sea-salt particles is formed in cloud droplets that subsequently evaporate and that only a small amount is formed in deliquesced aerosol particles. The model results are sensitive to changes in the assumed sea-salt emission rate and the overall aerosol size distribution. The latter indicates that a shift in the sea-salt aerosol distribution toward the smaller particle sizes might explain the observed-amount of sulphate associated with sea-salt particles. Copyright 2000 by the American Geophysical Union.