Long-range transport of pollution to Europe: origins, chemical and transport pathways, and impact on tropospheric composition

Ozone (O3) and aerosols are harmful to human health. Long-range transport sources contribute to the background levels upon which local pollution builds. The goal of this thesis is to describe and quantify the respective contribution of local and long-range transported sources to the O3 and aerosol budget in the framework of European air quality management. This issue is examined using a global model of chemistry and transport, the GEOS-Chem model, constrained by several experimental datasets (e.g. trace gases and aerosol distributions, aerosol optical depth, particulate matter concentrations) taken from field experiments, ground-based sites and satellite. The capabilities of the model to reproduce O3 and aerosol patterns is first examined. The model reproduces well in general the distribution of O3 and related species over the North Atlantic/Europe area. The simulation of particulate matter smaller than 2.5 μm (PM2.5) and aerosol optical depth (AOD) over Europe is also satisfying in general, but this may reflect some compensating errors between individual components (e.g. underestimate of organic matter, and overestimate of sulphate and dust). Intercomparison between the GEOS-Chem and another global model (MOZECH) also reveals possible problems in the water vapour distribution associated with the processes which drive the vertical lifting of pollutant over continental boundary layers. Despite these (relative) deficiencies, the model provides anyway insights about the contribution of long-range transport on the O3 and aerosol loads over Europe. The impact of continental outflow on the O3 chemical tendencies over oceanic regions is quantified. Net O3 photochemical production in polluted air masses travelling over oceanic areas under the influence of continental outflow is enhanced all-year round compared to the background marine environment by 2 to 6 ppbv/day in the boundary layer and by 1 to 3 ppbv/day in the upper troposphere. The origin of O3 long-range sources and their impact on the European O3 budget, as well as the role of changing emissions on this budget over the pasts decades is further investigated. Import of North American O3 into Europe is mainly controlled by meteorological patterns and by photochemical production over the North Atlantic and thus reaches a maximum in summer. In addition, Asia contributes to long-range transported O3 pollution by the Indian summer monsoon easterly winds during summer. During the monsoon period, convection is strong and associated NOx lightning emissions also contribute to high O3 levels, especially in the Mediterranean basin. North American and Asian anthropogenic pollution contribute substantially to the annual O3 burden (integrated over the whole tropospheric column) over Europe, accounting for 11% and 8%, respectively while the European contribution only accounts for 9%. The increase in Asian emissions from 1980 to 1997 have compensated the local reduction of O3 precursors, especially in the free troposphere. Finally, the aerosol load over Europe and the contribution of long and medium-range sources including anthropogenic and biomass burning pollution from North America and mineral dust from North Africa is examined. The model was used to interpret MODIS (Moderate Resolution Imaging Spectroradiometer) AOD and observations provided by the International Consortium for Atmospheric Research on Transport and Transformation (ICARTT) campaign over the North Atlantic and European area. Trans-Atlantic transport of aerosol is controlled by meteorological patterns and scavenging processes and reaches a maximum in spring. North American uxes of aerosols reach Europe at flower altitudes than that of O3 because a larger fraction of aerosols are scavenged in the venting from the boundary layer by frontal passages and deep convection. During high vegetation fire events in the boreal forest of Alaska and Canada, biomass burning pollution could also reach Europe at high altitudes, because a fraction of fire emissions are emitted directly in the free troposphere. Finally, the Saharan region also contributes significantly to the aerosol load over Europe. European sources contribute by 58% and 48% to the surface PM2.5 and column AOD over Europe. The second main sources are the mineral dust which represent in average 20% of the surface PM2.5 and AOD. In summer, North American anthropogenic and biomass burning emissions represent between 2 to 5% of the surface PM2.5 and AOD. The PM2.5 daily standard levels of the World Health organization (WHO) (10 μg/m3) and of the U.S. Environmental Protection Agency (EPA) (65 μg/m3) are often exceeded during dust outbreaks, especially in southern Europe. Long-range transport of anthropogenic and natural pollution is thus an important issue which should be considered in the definition of air quality standards and regulation treaties.

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