Sensitivity of sulphate aerosol size distributions and CCN concentrations over North America to SOx emissions and H2O2 concentrations

To assess the influence of aerosols on climate, the Northern Aerosol Regional Climate Model (NARCM) is currently being developed. NARCM includes size-segregated aerosols as prognostic and interactive constituents. In this paper, the model is being applied to sulphate aerosol over North America during time periods in July and December 1994. The results give evidence for considerable regional and seasonal variations in sulphate aerosol size distributions over North America. Comparisons of the results with different observations yield a reasonably good agreement in terms of meteorological and physicochemical parameters. Some of the differences in sulphate concentrations and wet deposition rates can be attributed to differences in cloud amounts and precipitation between model results and observations. Indirect tests of the simulated aerosol mass mean diameters are also encouraging. Additional simulations for hypothetical decreases in anthropogenic sulphur emissions and increases in hydrogen peroxide (H2O2) background concentrations are performed for the same time periods to study the responses of concentration, size distribution, and wet deposition of sulphate aerosol to these changes. Also, responses of cloud condensation nuclei (CCN) number concentrations are investigated. The simulation results show that sulphate aerosol concentrations respond almost linearly in both time periods to decreases in sulphur emissions but that CCN number concentrations respond nonlinearly due to decreases in sulphate mass mean diameters. Especially for the December period, increases in hydrogen peroxide background concentrations lead to increases in CCN number concentrations at critical diameters larger than about 0.07 mu m. These results lead to the hypothesis that increased in-cloud oxidation in convective clouds due to future increases in oxidant concentrations may produce larger CCN which eventually can be easily activated in subsequently forming stratiform clouds.