Abstract. Organic aerosols (OA) represent one of the major constituents of submicron particulate matter (PM1) and comprise a huge variety of compounds emitted by different sources. Three intensive measurement field campaigns to investigate the aerosol chemical composition all over Europe were carried out within the framework of the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) and the intensive campaigns of European Monitoring and Evaluation Programme (EMEP) during 2008 (May–June and September–October) and 2009 (February–March). In this paper we focus on the identification of the main organic aerosol sources and we define a standardized methodology to perform source apportionment using positive matrix factorization (PMF) with the multilinear engine (ME-2) on Aerodyne aerosol mass spectrometer (AMS) data. Our source apportionment procedure is tested and applied on 25 data sets accounting for two urban, several rural and remote and two high altitude sites; therefore it is likely suitable for the treatment of AMS-related ambient data sets. For most of the sites, four organic components are retrieved, improving significantly previous source apportionment results where only a separation in primary and secondary OA sources was possible. Generally, our solutions include two primary OA sources, i.e. hydrocarbon-like OA (HOA) and biomass burning OA (BBOA) and two secondary OA components, i.e. semi-volatile oxygenated OA (SV-OOA) and low-volatility oxygenated OA (LV-OOA). For specific sites cooking-related (COA) and marine-related sources (MSA) are also separated. Finally, our work provides a large overview of organic aerosol sources in Europe and an interesting set of highly time resolved data for modeling purposes.

[1] This paper investigates the physical and chemical characteristics of biomass burning aerosol over West Africa using data from the UK Facility for Airborne Atmospheric Measurements aircraft. Measurements of biomass burning aerosol were made during the Dust and Biomass-burning Experiment (DABEX) and Dust Outflow and Deposition to the Ocean (DODO) field experiments in January and February 2006. Layers of aged biomass burning aerosols were observed throughout the region, and fresh biomass burning aerosols were encountered during the penetration of smoke plumes at low altitudes. Vertical profiles of aerosol properties across the region are shown. Measurements from an Aerodyne Quadrupole Aerosol Mass Spectrometer (Q-AMS) show changes in chemical composition between fresh and aged biomass burning aerosols, over a region spanning thousands of kilometers. These data represent the first time that continental-scale variability in biomass burning aerosol composition has been observed. However, an almost linear relationship between organic aerosol mass concentration and carbon monoxide concentration was observed across the region. A net carbon loss occurs over the aerosol lifetime in the region owing to a combination of chemical processing and repartitioning of organic mass to the gas phase. Evolution of the number size distribution was observed, with coagulation concluded to be the dominant process involved, a finding supported by coagulation box modeling. Regional-scale emission ratios for organic (0.041) and black carbon (0.0072) with respect to CO have been estimated over West Africa, one of the largest sources of biomass burning globally. Biomass burning emissions from the West African Sahel are poorly represented in the literature, and these results represent important continental-scale emissions. They are in good agreement with literature values from other regions.

[1] The African Monsoon Multidisciplinary Analysis (AMMA) is a major international campaign investigating far-reaching aspects of the African monsoon, climate and the hydrological cycle. A special observing period was established for the dry season (SOP0) with a focus on aerosol and radiation measurements. SOP0 took place during January and February 2006 and involved several ground-based measurement sites across west Africa. These were augmented by aircraft measurements made by the Facility for Airborne Atmospheric Measurements (FAAM) aircraft during the Dust and Biomass-burning Experiment (DABEX), measurements from an ultralight aircraft, and dedicated modeling efforts. We provide an overview of these measurement and modeling studies together with an analysis of the meteorological conditions that determined the aerosol transport and link the results together to provide a balanced synthesis. The biomass burning aerosol was significantly more absorbing than that measured in other areas and, unlike industrial areas, the ratio of excess carbon monoxide to organic carbon was invariant, which may be owing to interaction between the organic carbon and mineral dust aerosol. The mineral dust aerosol in situ filter measurements close to Niamey reveals very little absorption, while other measurements and remote sensing inversions suggest significantly more absorption. The influence of both mineral dust and biomass burning aerosol on the radiation budget is significant throughout the period, implying that meteorological models should include their radiative effects for accurate weather forecasts and climate simulations. Generally, the operational meteorological models that simulate the production and transport of mineral dust show skill at lead times of 5 days or more. Climate models that need to accurately simulate the vertical profiles of both anthropogenic and natural aerosols to accurately represent the direct and indirect effects of aerosols appear to do a reasonable job, although the magnitude of the aerosol scattering is strongly dependent upon the emission data set.

The global organic aerosol (OA) budget is highly uncertain and past studies suggest that models substantially underestimate observed concentrations. Few of these studies have examined the vertical distribution of OA. Furthermore, many model-measurement comparisons have been performed with different models for single field campaigns. We synthesize organic aerosol measurements from 17 aircraft campaigns from 2001–2009 and use these observations to consistently evaluate a GEOS-Chem model simulation. Remote, polluted and fire-influenced conditions are all represented in this extensive dataset. Mean observed OA concentrations range from 0.2–8.2 μg sm⁻³ and make up 15 to 70% of non-refractory aerosol. The standard GEOS-Chem simulation reproduces the observed vertical profile, although observations are underestimated in 13 of the 17 field campaigns (the median observed to simulated ratio ranges from 0.4 to 4.2), with the largest model bias in anthropogenic regions. However, the model is best able to capture the observed variability in these anthropogenically-influenced regions (<i>R</i>²=0.18&minus;0.57), but has little skill in remote or fire-influenced regions. The model bias increases as a function of relative humidity for 11 of the campaigns, possibly indicative of missing aqueous phase SOA production. However, model simulations of aqueous phase SOA suggest a pronounced signature in the mid-troposphere (2–6 km) which is not supported in the observations examined here. Spracklen et al. (2011) suggest adding ~100 Tg yr⁻¹ source of anthropogenically-controlled SOA to close the measurement-model gap, which we add as anthropogenic SOA. This eliminates the model underestimate near source, but leads to overestimates aloft in a few regions and in remote regions, suggesting either additional sinks of OA or higher volatility aerosol at colder temperatures. Sensitivity simulations indicate that fragmentation of organics upon either heterogeneous or gas-phase oxidation could be an important (missing) sink of OA in models, reducing the global SOA burden by 15% and 47% respectively. The best agreement with observations is obtained when the simulated anthropogenically-controlled SOA is increased to ~100 Tg yr⁻¹ accompanied by either a gas-phase fragmentation process or a reduction in the temperature dependence of the organic aerosol partitioning (by decreasing the enthalpy of vaporization from 42 kJ mol⁻¹ to 25 kJ mol^&minus;1). These results illustrate that models may require both additional sources and additional sinks to capture the observed concentrations of organic aerosol