Direct radiative forcing and climate effects of anthropogenic aerosols with different mixing states over China

Abstract

An online coupled regional climate and chemistry model was used to investigate the direct effects of anthropogenic aerosols (sulfate, nitrate, black carbon BC and organic carbon OC) with different mixing states over China. Three mixing assumptions were considered, including external (EM), internal (IM, BC-core surrounded by well mixed scattering-shells) and partially internal (PIM, 32.2% of sulfate and nitrate, 35.5% of BC and 48.5% of OC were internally mixed) mixtures. Results indicated that high levels of anthropogenic aerosols were found in Southwest and Central to East China. Regional mean surface loadings of sulfate, nitrate, BC, primary OC over China were 9.56, 3.64, 2.30, and 2.99 μg m−3, respectively. PIM-aerosol optical depth and single scattering albedo, which were consistent with AERONET and satellite observations, were 0.51 ± 0.37 and 0.95 ± 0.02 in Central to East China, implying that proportions of internally mixed aerosols in PIM were reasonable to some degrees. Both aerosol direct radiative forcing (DRF) and corresponding climate responses were sensitive to aerosol mixing states and BC/OC hygroscopicities. The more BC was internally mixed or hydrophilic, the more solar radiation was absorbed, thus leading to more decreases in cloud amount (CA) and subsequently less surface cooling. Combining with the uncertainties of BC/OC hygroscopicities, regional mean PIM-aerosol DRF at the top of atmosphere ranged from −0.78 to −0.61 W m−2 in all-sky and from −5.24 to −4.95 W m−2 in clear-sky. Additionally, responses of cloud amount and water path, total column absorbed solar radiation (TCASR), surface air temperature and precipitation (TP) to PIM-aerosol DRFs over China were about −0.45∼ −0.37%, −0.44 ∼ −0.32 g m−2, +0.69 ∼ +0.72 W m−2, −0.13 ∼ −0.11 K and −4.56 ∼ −4.29%, respectively. These responses were also sensitive to the lateral boundary condition perturbations especially for CA, TCASR and TP, while DRFs themselves were not.