Impact of urbanization on fine particulate matter concentrations over central Europe

Rural-to-urban transformation (RUT) is the process of turning a rural or natural land surface into an urban one, which brings about important modifications in the surface, causing well-known effects like the urban heat island (UHI), reduced wind speeds, and increased boundary layer heights. Moreover, with concentrated human activities, RUT introduces new emission sources which greatly perturb local and regional air pollution. Particulate matter (PM) is one of the key pollutants responsible for the deterioration of urban air quality and is still a major issue in European cities, with frequent exceedances of limit values. Here we introduce a regional chemistry-climate model (regional climate model RegCM coupled offline to chemistry transport model CAMx) study which quantifies how the process of RUT modified the PM concentrations over central Europe including the underlying controlling mechanisms that contribute to the final PM pollution. Apart from the two most studied ones, (i) urban emissions and (ii) urban canopy meteorological forcing (UCMF; i.e. the impact of modified meteorological conditions on air quality), we also analyse two less studied contributors to RUT's impact on air quality: (iii) the impact of modified dry-deposition velocities (DVs) due to urbanized land use and (iv) the impact of modified biogenic emissions due to urbanization-induced vegetation modifications and changes in meteorological conditions which affect these emissions. To calculate the magnitude of each of these RUT contributors, we perform a cascade of simulations, whereby each contributor is added one by one to the reference state, while focus is given on PM2.5 (particulate matter with diameter less then 2.5 mu m). Its primary and secondary components, namely primary elemental carbon (PEC), sulfates (PSO4), nitrates (PNO3), ammonium (PNH4), and secondary organic aerosol (SOA), are analysed too. The validation using surface measurements showed a systematic negative bias for the total PM2.5, which is probably caused by underestimated organic aerosol and partly by the negative bias in sulfates and elemental carbon. For ammonium and nitrates, the underestimation is limited to the warm season, while for winter, the model tends to overestimate their concentrations. However, in each case, the annual cycle is reasonably captured. We evaluated the RUT impact on PM2.5 over a sample of 19 central European cities and found that the total impact of urbanization is about 2-3 and 1-1.5 mu gm(-3) in winter and summer, respectively. This is mainly driven by the impact of emissions alone causing a slightly higher impact (1.5-3.5 and 1.2-2 mu gm(-3) in winter and summer), while the effect of UCMF was a decrease at about 0.2-0.5 mu gm(-3) (in both seasons), which was mainly controlled by enhanced vertical eddy diffusion, while increases were modelled over rural areas. The transformation of rural land use into an urban one caused an increase in dry-deposition velocities by around 30 %-50 %, which alone resulted in a decrease in PM2.5 by 0.1-0.25 mu gm(-3) in both seasons. Finally, the impact of biogenic emission modifications due to modified land use and meteorological conditions caused a decrease in summer PM2.5 of about 0.1 mu gm(-3), while the winter effects were negligible. The total impact of urbanization on aerosol components is modelled to be (values indicate winter and summer averages) 0.4 and 0.3 mu gm(-3) for PEC, 0.05 and 0.02 mu gm 3 for PSO4, 0.1 and 0.08 mu gm(-3) for PNO3, 0.04 and 0.03 mu gm(-3) for PNH4, and 0 and 0.05 mu gm(-3) for SOA. The main contributor of each of these components was the impact of emissions, which was usually larger than the total impact due to the fact that UCMF was counteracted with a decrease. For each aerosol component, the impact of modified DV was a clear decrease in concentration, and finally, the modifications of biogenic emissions impacted SOA predominantly, causing a summer decrease, while a very small secondary effect of secondary inorganic aerosol was modelled too (they increased). In summary, we showed that when analysing the impact of urbanization on PM pollution, apart from the impact of emissions and the urban canopy meteorological forcing, one also has to consider the effect of modified land use and its impact on dry deposition. These were shown to be important in both seasons. For the effect of modified biogenic emissions, our calculations showed that they act on PM2.5 predominantly through SOA modifications, which only turned out to be important during summer.