Evaluation of global EMEP MSC-W (rv4.34) WRF (v3.9.1.1) model surface concentrations and wet deposition of reactive N and S with measurements

Atmospheric pollution has many profound effects on human health, ecosystems, and the climate. Of concern are high concentrations and deposition of reactive nitrogen (N-r) species, especially of reduced N (gaseous NH3, particulate NH4+). Atmospheric chemistry and transport models (ACTMs) are crucial to understanding sources and impacts of N-r chemistry and its potential mitigation. Here we undertake the first evaluation of the global version of the EMEP MSC-W ACTM driven by WRF meteorology (1 degrees x1 degrees resolution), with a focus on surface concentrations and wet deposition of N and S species relevant to investigation of atmospheric N-r and secondary inorganic aerosol (SIA). The modelmeasurement comparison is conducted both spatially and temporally, covering 10 monitoring networks worldwide. Model simulations for 2010 compared use of both HTAP and ECLIPSEE (ECLIPSE annual total with EDGAR monthly profile) emissions inventories; those for 2015 used ECLIPSEE only. Simulations of primary pollutants are somewhat sensitive to the choice of inventory in places where regional differences in primary emissions between the two inventories are apparent (e.g. China) but are much less sensitive for secondary components. For example, the difference in modelled global annual mean surface NH3 concentration using the two 2010 inventories is 18 % (HTAP: 0.26 mu g m(-3); ECLIPSEE: 0.31 mu g m(-3)) but is only 3.5 % for NH4+ (HTAP: 0.316 mu g m(-3); ECLIPSEE: 0.305 mu g m(-3)). Comparisons of 2010 and 2015 surface concentrations between the model and measurements demonstrate that the model captures the overall spatial and seasonal variations well for the major inorganic pollutants NH3, NO2, SO2, HNO3, NH4+, NO3-, and SO42- and their wet deposition in East Asia, Southeast Asia, Europe, and North America. The model shows better correlations with annual average measurements for networks in Southeast Asia (mean R for seven species: (R-7) over bar =0.73), Europe ((R-7) over bar =0.67), and North America ((R-7) over bar =0.63) than in East Asia ((R-5) over bar =0.35) (data for 2015), which suggests potential issues with the measurements in the latter network. Temporally, both model and measurements agree on higher NH3 concentrations in spring and summer and lower concentrations in winter. The model slightly underestimates annual total precipitation measurements (by 13 %45 %) but agrees well with the spatial variations in precipitation in all four world regions (0.650.94 R range). High correlations between measured and modelled NH4+ precipitation concentrations are also observed in all regions except East Asia. For annual total wet deposition of reduced N, the greatest consistency is in North America (0.750.82 R range), followed by Southeast Asia (R=0.68) and Europe (R=0.61). Modelmeasurement bias varies between species in different networks; for example, bias for NH4+ and NO3- is largest in Europe and North America and smallest in East Asia and Southeast Asia. The greater uniformity in spatial correlations than in biases suggests that the major driver of modelmeasurement discrepancies (aside from differing spatial representativeness and uncertainties and biases in measurements) are shortcomings in absolute emissions rather than in modelling the atmospheric processes. The comprehensive evaluations presented in this study support the application of this model framework for global analysis of current and potential future budgets and deposition of N-r and SIA.