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Many open questions exist about the importance of different sources of carbonaceous aerosol, which is a substantial contributor to the global aerosol budget and, therefore, to climate change and human mortality. In this work, 14C was determined in elemental carbon (EC) and different organic carbon (OC) fractions from ambient urban aerosols with aerodynamic diameter <10 μm collected in Zurich (Switzerland). This enabled a more detailed source attribution of the carbonaceous aerosol mass than is possible with other currently available methods. The three major sources, fossil fuel, wood combustion (both anthropogenic emissions), and biogenic emissions, were quantified, making specific regulatory air quality management measures possible. EC originates nearly exclusively from fossil fuel usage during summer, whereas biomass‐burning emissions become substantial during winter with ∼25%, even though this source contributes only marginally to the local energy consumption. For OC, biogenic sources are dominant in summer with ∼60%, where secondary organic aerosol prevails. Wood combustion accounts for up to ∼41% of OC in winter. Fossil fuels represent ∼30% of OC throughout the year.

International audienceOn the basis of a 2-year comprehensive data set obtained within the CARBOSOL project, seasonal source apportionment of PM2.5 aerosol is attempted for five rural/remote sites in Europe. The approach developed combines radiocarbon measurements with bulk measurements of organic carbon (OC), elemental carbon (EC), and two organic tracers (levoglucosan and cellulose). Source types are lumped into primary emissions from fossil fuel combustion and biomass burning, bioaerosol, and secondary organic aerosol from precursors emitted by fossil and nonfossil sources. Bulk concentration ratios reported for these source types in the literature are used to estimate the source contributions which are constrained by measured radiocarbon concentrations. It has been found that while fossil-related sources predominate EC throughout the year at all sites, the sources of OC are primarily biogenic and markedly different between summer and winter. In winter biomass burning primary emission is the main source, with sizable additional contribution from fossil fuel combustion. In contrast, in summer secondary organic aerosol (SOA) from nonfossil sources becomes predominant (63–76% of TC), with some contribution of SOA from fossil fuel combustion. The results agree well with recent findings of other authors who established the predominance of biogenic SOA for rural sites in summer in Europe. An uncertainty analysis has been conducted, which shows that the main conclusions from this study are robust

[1] Atmospheric levoglucosan has been determined as a proxy for ''biomass smoke'' in samples from six background stations on a west-east transect extending from the Atlantic (Azores) to the mid-European background site KPZ (K-Puszta, Hungary). Concentration levels of levoglucosan (biannual averages) in the west-east transect range from 0.005 mg/m 3 at the oceanic background site AZO (Azores) to 0.52 mg/m 3 at AVE (Aveiro, Portugal). The atmospheric concentration of ''biomass smoke'' (biannual averages) was derived from the levoglucosan data with wood-type-specific conversion factors. Annual averages of wood smoke levels ranged from 0.05 mg/m 3 at AZO to 4.3 mg/m 3 at AVE. Winter (DJF) averages at the low-level sites AVE and KPZ were 10.8 and 6.7 mg/m 3 , respectively. Relative contributions of biomass smoke to organic matter (OM) range from around 9-11% at the elevated sites SIL, PDD and SBO, as well as for AZO, to 36% at the low-level site AVE and 28% at KPZ. Surprisingly high relative concentrations of biomass smoke in OM (68 and 47%) were observed for wintry conditions at the continental low-level CARBOSOL sites AVE and KPZ. Thus biomass smoke is a very important constituent of the organic material in the mid and west European background with summer contributions to organic matter of around 1-6% and winter levels of around 20% at the elevated mountain sites and 47-68% at rural flat terrain sites, not including secondary organic aerosol from biomass combustion sources.

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[1] In the framework of the European CARBOSOL project (Present and Retrospective State of Organic versus Inorganic Aerosol over Europe: Implications for Climate), atmospheric aerosol was continuously sampled for 2 years at six sites along a west-east transect extending from Azores, in the mid-Atlantic Ocean, to K-Puszta (Hungary), in central Europe. Aerosols were analyzed for 210 Pb, inorganic ions, elemental (EC) and organic (OC) carbon, water soluble organic carbon (WSOC), macromolecular type (humic-like) organic substances (HULIS), C 2 -C 5 diacids, cellulose, and levoglucosan. Pooled aerosol filters were also used for the identification of different families of organic compounds by gas chromatography/mass spectrometry, GC/MS, as well as 14 C determinations. The data resulted in a climatological overview of the aerosol composition over Europe in the various seasons, from west to east, and from the boundary layer to the free troposphere. The paper first summarizes the characteristics of the sites and collected samples and then focuses on the aerosol mass partitioning (mass closure, inorganic versus organic, EC versus OC, water soluble versus insoluble OC), giving an insight on the sources of carbonaceous aerosol present in rural and natural background areas in Europe. It also introduces the main role of other companion papers dealing with CARBOSOL aerosol data that are also presented in this issue.Citation: Pio, C. A., et al. (2007), Climatology of aerosol composition (organic versus inorganic) at nonurban sites on a west-east transect across Europe,

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[1] An atmospheric study of C 2 -C 5 dicarboxylic acids was conducted over two years at seven sites located from the Azores to eastern continental European sites. The lowest concentrations of total C 2 -C 5 diacids are observed at the Azores (Portugal) and at 4360 m elevation in the Alps ($50 ng m À3 ), and the highest (400 ng m À3) are observed at the rural K-puszta site (Hungary). Quasi-absent at surface sites, the seasonal cycle of total diacids is characterized by a pronounced summer maximum at elevated sites, the highest summer level (510 ng m À3) being observed at the forested mountain site of Schauinsland (Germany). Whatever site and season, oxalic acid is always the most abundant diacid with a relative abundance higher than 60%. The climatology of C 2 -C 5 diacids in Europe is discussed versus environmental conditions at sites (marine/ continental, rural/forested, boundary layer/free troposphere, and winter/summer). Observations are used to discuss the possible sources of C 2 -C 5 diacids, with special emphasis on their primary versus secondary and natural versus anthropogenic origin. At surface sites in winter, fast secondary productions in wood burning plumes in addition to secondary production from volatile organic carbon (VOC) species emitted by vehicles seem to be important contributors. In summer the impact of anthropogenic sources is weakened and biogenic emissions from vegetation (unsaturated fatty acids, isoprene, oxygenated VOCs, and eventually monoterpenes) likely represent major precursors of diacids. At the Azores, diacids are not only related to long-range transport from continents but also to marine biogenic emissions from phytoplankton, particularly in summer.Citation: Legrand, M., S. Preunkert, T. Oliveira, C. A. Pio, S. Hammer, A. Gelencsér, A. Kasper-Giebl, and P. Laj (2007), Origin of C 2 -C 5 dicarboxylic acids in the European atmosphere inferred from year-round aerosol study conducted at a west-east transect,