A general circulation model study of the global carbonaceous aerosol distribution

[1] Atmospheric distributions of carbonaceous aerosols are simulated using the Geophysical Fluid Dynamics Laboratory SKYHI general circulation model (GCM) (latitude-longitude resolution of ∼3° × 3.6°). A number of systematic analyses are conducted to investigate the seasonal and interannual variability of the concentrations at specific locations and to investigate the sensitivity of the distributions to various physical parameters. Comparisons are made with several observational data sets. At four specific sites (Mace Head, Mauna Loa, Sable Island, and Bondville) the monthly mean measurements of surface concentrations of black carbon made over several years reveal that the model simulation registers successes as well as failures. Comparisons are also made with averages of measurements made over varying time periods, segregated by geography and rural/remote locations. Generally, the mean measured remote surface concentrations exceed those simulated. Notwithstanding the large variability in measurements and model simulations, the simulations of both black and organic carbon tend to be within about a factor of 2 at a majority of the sites. There are major challenges in conducting comparisons with measurements due to inadequate sampling at some sites, the generally short length of the observational record, and different methods used for estimating the black and organic carbon amounts. The interannual variability in the model and in the few such measurements available points to the need for doing multiyear modeling and to the necessity of comparing with long-term measurements. There are very few altitude profile measurements; notwithstanding the large uncertainties, the present comparisons suggest an overestimation by the model in the free troposphere. The global column burdens of black and organic carbon in the present standard model integration are lower than in previous studies and thus could be regarded as approximately bracketing a lower end of the simulated anthropogenic burden due to these classes of aerosols, based on the current understanding of the carbonaceous aerosol cycle. Of the physical factors examined, the intensity and frequency of precipitation events are critical in governing the column burdens. Biases in the frequency of precipitation are likely the single biggest cause of discrepancies between simulation and observations. This parameter is available from very few sites and thus lacks a comprehensive global data set, unlike, say, monthly mean precipitation. Several multiyear GCM integrations have been performed to evaluate the sensitivity of the global mean black carbon distribution to the principal aerosol parameters, with due regard to variability and statistical significance. The most sensitive parameters, in order of importance, turn out to be the wet deposition, transformation from hydrophobic to hydrophilic state, and the partitioning of the emitted aerosol between the hydrophobic and hydrophilic varieties. From the sensitivity tests, it is estimated that the variations of the global mean column burden and lifetime of black carbon are within about a factor of 2 about their respective standard values. The studies also show that the column burdens over remote regions appear to be most sensitive to changes in each parameter, reiterating the importance of measurements in those locations for a proper evaluation of model simulation of these aerosols.