[1] A case of long-range transport of a biomass burning plume from Alaska to Europe is analyzed using a Lagrangian approach. This plume was sampled several times in the free troposphere over North America, the North Atlantic and Europe by three different aircraft during the IGAC Lagrangian 2K4 experiment which was part of the ICARTT/ ITOP measurement intensive in summer 2004. Measurements in the plume showed enhanced values of CO, VOCs and NO y , mainly in form of PAN. Observed O 3 levels increased by 17 ppbv over 5 days. A photochemical trajectory model, CiTTyCAT, was used to examine processes responsible for the chemical evolution of the plume. The model was initialized with upwind data and compared with downwind measurements. The influence of high aerosol loading on photolysis rates in the plume was investigated using in situ aerosol measurements in the plume and lidar retrievals of optical depth as input into a photolysis code (Fast-J), run in the model. Significant impacts on photochemistry are found with a decrease of 18% in O 3 production and 24% in O 3 destruction over 5 days when including aerosols. The plume is found to be chemically active with large O 3 increases attributed primarily to PAN decomposition during descent of the plume toward Europe. The predicted O 3 changes are very dependent on temperature changes during transport and also on water vapor levels in the lower troposphere which can lead to O 3 destruction. Simulation of mixing/dilution was necessary to reproduce observed pollutant levels in the plume. Mixing was simulated using background concentrations from measurements in air masses in close proximity to the plume, and mixing timescales (averaging 6.25 days) were derived from CO changes. Observed and simulated O 3 /CO correlations in the plume were also compared in order to evaluate the photochemistry in the model. Observed slopes change from negative to positive over 5 days. This change, which can be attributed largely to photochemistry, is well reproduced by multiple model runs even if slope values are slightly underestimated suggesting a small underestimation in modeled photochemical O 3 production. The possible impact of this biomass burning plume on O 3 levels in the European boundary layer was also examined by running the model for a further 5 days and comparing with data collected at surface sites, such as Jungfraujoch, which showed small O 3 increases and elevated CO levels. The model predicts significant changes in O 3 over the entire 10 day period due to photochemistry but the signal is largely lost because of the effects of dilution. However, measurements in several other BB plumes over Europe show that O 3 impact of Alaskan fires can be potentially significant over Europe.

Abstract. Trace gas and aerosol data collected in the tropical tropopause layer (TTL) between 12-18.5 km by the M55 Geophysica aircraft as part of the SCOUT-AMMA campaign over West Africa during the summer monsoon in August 2006 have been analysed in terms of their air mass origins. Analysis of domain filling back trajectories arriving over West Africa, and in the specific region of the flights, showed that the M55 flights were generally representative of air masses arriving over West Africa during the first 2 weeks of August, 2006. Air originating from the midlatitude lower stratosphere was under-sampled (in the midupper TTL) whilst air masses uplifted from central Africa (into the lower TTL) were over-sampled in the latter part of the campaign. Signatures of recent (previous 10 days) origins were superimposed on the large-scale westward flow over West Africa. In the lower TTL, air masses were impacted by recent local deep convection over Africa at the level of main convective outflow (350 K, 200 hPa) and on certain days up to 370 K (100 hPa). Estimates of the fraction of air masses influenced by local convection vary from 10 to 50% depending on the method applied and from day to day during the Correspondence to: K. S. Law (kathy.law@latmos.ipsl.fr) campaign. The analysis shows that flights on 7, 8 and 11 August were more influenced by local convection than on 4 and 13 August allowing separation of trace gas and aerosol measurements into "convective" and "non-convective" flights. Strong signatures, particularly in species with short lifetimes (relative to CO 2 ) like CO, NO and fine-mode aerosols were seen during flights most influenced by convection up to 350-365 K. Observed profiles were also constantly perturbed by uplift (as high as 39%) of air masses from the mid to lower troposphere over Asia, India, and oceanic regions resulting in import of clean oceanic (e.g. O 3 -poor) or polluted air masses from Asia (high O 3 , CO, CO 2 ) into West Africa. Thus, recent uplift of CO 2 over Asia may contribute to the observed positive CO 2 gradients in the TTL over West Africa. This suggests a more significant fraction of younger air masses in the TTL and needs to taken into consideration in derivations of mean age of air. Transport of air masses from the mid-latitude lower stratosphere had an impact from the mid-TTL upwards (20-40% above 370 K) during the campaign period importing air masses with high O 3 and NO y . Ozone profiles show a less pronounced lower TTL minimum than observed previously by regular ozonesondes at other tropical locations. Concentrations are less than 100 ppbv in the lower TTL and vertical gradients less steep than in the upper TTL. The air mass origin analysis and simulations of in-situ net Published by Copernicus Publications on behalf of the European Geosciences Union.

Abstract. Pollutant plumes with enhanced concentrations of trace gases and aerosols were observed over the southern coast of West Africa during August 2006 as part of the AMMA wet season field campaign. Plumes were observed both in the mid and upper troposphere. In this study we examined the origin of these pollutant plumes, and their potential to photochemically produce ozone (O 3 ) downwind over the Atlantic Ocean. Their possible contribution to the Atlantic O 3 maximum is also discussed. Runs using the BOLAM mesoscale model including biomass burning carbon monoxide (CO) tracers were used to confirm an origin from central African biomass burning fires. The plumes measured in the mid troposphere (MT) had significantly higher pollutant concentrations over West Africa compared to the upper tropospheric (UT) plume. The mesoscale modelCorrespondence to: E. Real (elsa.real@aero.jussieu.fr) reproduces these differences and the two different pathways for the plumes at different altitudes: transport to the northeast of the fire region, moist convective uplift and transport to West Africa for the upper tropospheric plume versus north-west transport over the Gulf of Guinea for the mid-tropospheric plume. Lower concentrations in the upper troposphere are mainly due to enhanced mixing during upward transport. Model simulations suggest that MT and UT plumes are 16 and 14 days old respectively when measured over West Africa. The ratio of tracer concentrations at 600 hPa and 250 hPa was estimated for 14-15 August in the region of the observed plumes and compares well with the same ratio derived from observed carbon dioxide (CO 2 ) enhancements in both plumes. It is estimated that, for the period 1-15 August, the ratio of Biomass Burning (BB) tracer concentration transported in the UT to the ones transported in the MT is 0.6 over West Africa and the equatorial South Atlantic.Published by Copernicus Publications on behalf of the European Geosciences Union. E. Real et al.: Cross-hemispheric transport of african biomass burningRuns using a photochemical trajectory model, CiTTy-CAT, initialized with the observations, were used to estimate in-situ net photochemical O 3 production rates in these plumes during transport downwind of West Africa. The mid-troposphere plume spreads over altitude between 1.5 and 6 km over the Atlantic Ocean. Even though the plume was old, it was still very photochemically active (mean net O 3 production rates over 10 days of 2.6 ppbv/day and up to 7 ppbv/day during the first days) above 3 km especially during the first few days of transport westward. It is also shown that the impact of high aerosol loads in the MT plume on photolysis rates serves to delay the peak in modelled O 3 concentrations. These results suggest that a significant fraction of enhanced O 3 in mid-troposphere over the Atlantic comes from BB sources during the summer monsoon period. According to simulated occurrence of such transport, BB may be the main source for O 3 enhancement in the equatorial south Atlantic MT, at least in August 2...