1Max Planck Institute for Chemistry, P.O. Box 3020, 55020 Mainz, Germany
2Johannes Gutenberg-University, Institute for Atmospheric Physics, 55099 Mainz, Germany
*now at: Johannes Gutenberg-University, Institute for Atmospheric Physics, 55099 Mainz, Germany
**now at: Institute for Advanced Sustainability Studies, 14467 Potsdam, Germany
Abstract. Major population centers (MPCs), or megacities, represent the largest of growing urban agglomerations with major societal and environmental implications. In terms of air quality, they are seen as localized but strong emission sources of aerosols and trace gases which in turn affect air pollution levels in the city or in downwind regions. In the state-of-the-art atmospheric chemistry general circulation model EMAC, generic aerosol and gas-phase tracers with equal emission source strengths at 46 MPC locations are used to study the balance between local pollution build-up and pollution export, either vertically into the upper troposphere or horizontally in the lower troposphere. The insoluble gas-phase tracers with fixed lifetimes are transported with the atmospheric circulation, while the aerosol tracers also undergo gravitational sedimentation as well as dry and wet deposition processes. The strength of low-level tracer export depends on the location of the emission source and prevailing meteorology, in particular on atmospheric stability and the height of the boundary layer and the mixing out of this layer. In contrast, vertical transport of tracer mass depends on the tracer's solubility: the more soluble a tracer is, the less mass reaches altitudes above five kilometers. Hence, the mass of insoluble gas-phase tracer above five kilometers can be up to ten times higher than the hydrophilic aerosol mass from the same source. In the case of aerosol tracers, pollution build-up around the source is determined by meteorological factors which have only indirect effects on tracer lifetime, like surface wind, boundary layer height, and turbulent mixing, as well as those which affect the lifetime of the tracers such as precipitation. The longer a tracer stays in the atmosphere, the lower is the relative importance of the location of the source to the atmospheric mass, and thus the lower is the relative local pollution build-up. We further use aerosol deposition fields to estimate regions with high deposition, that is more than 1% or more than 5% of the corresponding tracer emission deposited in this region. In doing so, we find that the high deposition areas are larger for aerosols with diameters of 10.0 μm, and these differ less between the MPCs than for aerosols with diameters smaller than 2.5 μm due to faster deposition. Furthermore, cities in regions with high precipitation rates or unfavorable geographic locations, e.g., in a basin, suffer most of this high deposition. Most of the high deposition occurs over land, although about 50% of the MPCs are located along coastlines. By folding the aerosol deposition fields with geographical distributions of cropland, pasture, and forest, the impact on different land ecosystems is assessed. In general, forest is exposed most to deposition from MPCs while pastureland is least affected. Moreover, the impact on humans, measured with a threshold exceedance of pollutant surface mixing ratios, is more dependent on population densities than on the size of the area with a certain mixing ratio.