Global modeling of aerosol dynamics: Model description, evaluation, and interactions between sulfate and nonsulfate aerosols

The IMPACT global chemistry and transport model has been updated to include an aerosol dynamics module. Here it is used to simulate the dynamics of sulfate aerosol and its interaction with nonsulfate aerosol components: carbonaceous aerosol (organic matter (OM) and black carbon (BC)), dust, and sea salt. The sulfate aerosol dynamics is based on the method of modes and moments. In the current implementation, two modes are used for sulfate aerosol (nuclei and accumulation mode), and two moments are predicted within each mode (sulfate aerosol number and mass concentration). The aging of carbonaceous aerosol and dust particles from hydrophobic to hydrophilic depends on the surface coating of sulfate which occurs as a result of the condensation of sulfuric acid gas H 2 SO 4 (g) on their surface, and coagulation with pure sulfate aerosol. The model predicts high sulfate aerosol number concentrations in the nuclei mode (over 10 4 cm −3 ) in the tropical upper troposphere, while accumulation mode sulfate number concentrations are generally within 50–500 cm −3 in most parts of the free troposphere. The model predicted mass concentrations of sulfate, OM, BC, dust, and sea salt, H 2 SO 4 (g) concentration, aerosol number, and size distributions are compared with measurement data. Our model predicts ∼80% of global sulfate existing as a pure sulfate aerosol (9.7% in nuclei and 69.8% in accumulation mode), with 14.3% on carbonaceous aerosol, 3.3% on dust, and 2.7% on sea salt. In the boundary layer, over 40% of sulfate is associated with nonsulfate aerosols in many regions of the world whereas less than 10% of sulfate is associated with nonsulfate aerosols in the upper troposphere. The model predicted mass fraction of sulfate in the sulfate‐carbonaceous aerosol mixture suggests that carbonaceous aerosol in most of the troposphere is internally mixed with sulfate and thus generally hygroscopic except near the source regions where the mass fraction is less than 5%. On the global mean, 54% and 93% of carbonaceous aerosol are coated with sulfate in the boundary layer and in the upper troposphere, respectively. Our result suggests that carbonaceous aerosols have a shorter lifetime (3∼4 days) than predicted (4∼8 days) using models that treat these aerosols as partly hydrophobic with an arbitrary e ‐folding time from hydrophobic to hydrophilic.