Pollution transport efficiency toward the Arctic: Sensitivity to aerosol scavenging and source regions

Isabelle Bey, Quentin Bourgeois
2011
Journal paper

Abstract

The processes driving current changes in Arctic atmospheric composition and climate are still uncertain. In particular the relative contributions of major source regions from the midlatitudes remain a matter of debate in the literature. The objectives of this study are to better quantify the relative contributions of different processes governing the transport of pollution from the midlatitudes to the Arctic and the relative contributions of different geopolitical source regions. We use a suite of observational data sets (including the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaigns and the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) satellite instrument) to constrain a global aerosol simulation from the ECHAM5-HAMMOZ model. Preliminary comparison of model results with vertical profiles of sulfate and black carbon (BC) collected during the ARCTAS campaigns and with aerosol extinction time series retrieved from CALIOP indicates that the model underestimates export of aerosols from the planetary boundary layer to the free troposphere in the midlatitudes and long-range transport of aerosols from the midlatitudes toward the Arctic. In contrast, observed CO profiles are relatively well simulated, which points to a possible problem with wet scavenging. Decreasing the prescribed aerosol scavenging coefficients within the range of experimental data available in the literature significantly improves the agreement with observations. Sulfate and BC burdens in the Arctic increase by a factor 5-6. Annual global lifetimes of sulfate and BC increase from 3.1 to 4.6 days and from 4.4 to 5.9 days, respectively. Using the improved simulation, we find that 59% of sulfate in the Arctic troposphere comes from the oxidation of SO2 emitted in Siberia (19%), Europe (18%), Asia (13%), and North America (9%). Anthropogenic and biomass burning BC emitted in Siberia, Asia, Europe, and North America contributes 29, 27, 25, and 17%, respectively, to the Arctic BC burden. Emissions of aerosols (or precursors) from Siberia and Europe are more susceptible to be transported and subsequently deposited on the Arctic (about 7-12%) compared to those from North America and Asia (1-4%). Overall, the study shows that aerosol scavenging removal processes play a crucial role on the aerosol transport from the midlatitudes toward the Arctic and should be carefully characterized in aerosol models.

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Isabelle Bey, Quentin Bourgeois
2011
Journal paper

Abstract

Official source

https://infoscience.epfl.ch/record/168669?ln=en

About this result

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A multi-model assessment of pollution transport to the Arctic

Isabelle Bey

We examine the response of Arctic gas and aerosol concentrations to perturbations in pollutant emissions from Europe. East and South Asia, and North America using results from a coordinated model intercomparison. These sensitivities to regional emissions (mixing ratio change per unit emission) vary widely across models and species. Intermodel differences are systematic, however, so that the relative importance of different regions is robust. North America contributes the most to Arctic ozone pollution. For aerosols and CO, European emissions dominate at the Arctic surface but East Asian emissions become progressively more important with altitude, and arc dominant in the upper troposphere. Sensitivities show strong seasonality: surface sensitivities typically maximize during boreal winter for European and during spring for East Asian and North American emissions. Mid-tropospheric sensitivities, however, nearly always maximize during spring or summer for all regions. Deposition of black carbon (BC) onto Greenland is most sensitive to North American emissions. North America and Europe each contribute similar to 40% of total BC deposition to Greenland, with similar to 20% from East Asia. Elsewhere in the Arctic, both sensitivity and total BC deposition are dominated by European emissions. Model diversity for aerosols is especially large, resulting primarily from differences in aerosol physical and chemical processing, (including removal). Comparison of modeled aerosol concentrations with observations indicates problems in the models, and perhaps, interpretation of the measurements. For gas phase pollutants such as CO and O-3, which are relatively well-simulated, the processes contributing most to uncertainties depend on the source region and altitude examined. Uncertainties in the Arctic surface CO response to emissions perturbations are dominated by emissions for East Asian sources, while uncertainties in transport, emissions. and oxidation are comparable for European and North American sources. At higher levels. model-to-model variations in transport and oxidation are most important. Differences in photochemistry appear to play the largest role in the intermodel variations in Arctic ozone sensitivity, though transport also contributes substantially in the mid-troposphere.

2008

Aerosol Transport and Distribution

Quentin Bourgeois

The fourth report of the Intergovernmental Panel of Climate Change (IPCC) unambiguously indicates that the climate is changing. Climate change is induced by changes in atmospheric abundances of greenhouse gases and aerosols, solar radiation and land surface properties, which all alter the radiative balance of the Earth. Among them, greenhouse gases and aerosols are likely the compounds affecting the climate the most. While greenhouse gases warm the Earth, aerosols influence its radiative balance by scattering and absorbing solar radiation (the direct effect), and by modifying cloud amount and properties (the indirect effect). The radiative forcing of aerosols on the climate is however the less understood among the various forcings currently considered in the IPCC assessment. This is likely related to the lack of comprehensive and accurate observations of aerosols (and in particular of their vertical distribution) which thus makes global aerosol models difficult to constrain. Recent model intercomparisons have indicated that different assumptions regarding aerosol emissions, formation and growing properties, and removal processes generate large diversities within models. These large diversities are found in particular in the Arctic and the upper troposphere region where extreme surrounding conditions take place, limiting instrument sensitivity and accuracy. The objectives of this thesis are to better quantify the processes driving the aerosol distribution in regions where the uncertainties are the largest, including the Arctic region and the upper troposphere, and to assess the quality of CALIOP observations. For this purpose, we used the fully coupled global climate-aerosol-chemistry ECHAM5-HAMMOZ model conjointly with a suite of remote sensing observations including the CALIOP satellite instrument, which provides the vertical distribution of aerosols. The model predicts the size distribution and composition of aerosols as well as the number concentration of cloud droplets and ice crystals. We first investigated the processes that drive the transport of soluble and insoluble compounds toward the Arctic in the ECHAM5-HAMMOZ model. Recognizing that scavenging processes may be an issue in global models, we "re-visited" their properties in ECHAM5-HAMMOZ. We find that the model better reproduces the aerosol vertical distribution in the northern mid- and high-latitudes, especially in the free troposphere, by decreasing aerosol scavenging coefficients in the model. Using smaller aerosol scavenging coefficients results in an increase of aerosol burden and lifetime, especially in the Arctic. In addition, the Arctic haze phenomenon is better represented in the simulation using decreased aerosol scavenging coefficients. The relative contributions of different processes governing the transport of aerosols from the midlatitudes toward the Arctic together with the relative contributions of different geopolitical source regions were then quantified. We find that Europe and Siberia contribute the most to the Arctic pollution even though Asian anthropogenic emissions are much larger. The model suggests that BC emitted in Siberia and Europe is ten times more efficiently deposited onto the Arctic than BC emitted in Asia. We next investigated an aerosol layer that forms in the vicinity of the tropical tropopause layer (TTL) over the southern Asian and Indian Ocean region. Aerosols in this layer are observed with the CALIOP instrument even though ice clouds partly mask their signal. The aerosol layer follows the Inter Tropical Convergence Zone (ITCZ), which indicates that these aerosols are likely transported during convective processes. The ECHAM5.5-HAM2 model reproduces such an aerosol layer in the TTL over the same region but clearly overestimates CALIOP data. Model results suggest that aerosols in this layer are mostly sulfate particles transported during convective processes and originating from natural sources. The shortwave forcing of this aerosol layer is estimated. Finally, we assessed the accuracy of aerosol extinction retrievals from the CALIOP satellite instrument by comparing them with remote sensing observations such as AERONET, MODIS and MISR over the last four years. Overall, standard CALIOP products underestimate by 50% observed aerosol extinctions. However, this comparison is substantially improved by screening CALIOP data. The comparison of the CALIOP screened product with the ECHAM5.5-HAM2 model shows large disparities in model results. The model reproduces quite well the observed interannual variability and vertical distribution of aerosols in Europe and North Africa while it underestimates them in America and Asia. This is likely due to an underestimate of dust and anthropogenic emissions in North America and Asia.

EPFL2012

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.

EPFL2006