E. Real

Université de Versailles Saint-Quentin, Versailles, Île-de-France, France

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Publications (24)51.09 Total impact

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    Real E, Sartelet K
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    ABSTRACT: This paper evaluates the impact of photolysis rate calculation on simulated European air composition and air quality. In particular, the impact of the cloud parametrisation and the impact of aerosols on photolysis rates are analysed. Photolysis rates are simulated using the Fast-JX photolysis scheme and gas and aerosol concentrations over Europe are simulated with the regional chemistry-transport model Polair3D of the Polyphemus platform. The photolysis scheme is first used to update the clear-sky tabulation of photolysis rates used in the previous Polair3D version. Important differences in photolysis rates are simulated, mainly due to updated cross-sections and quantum yields in the Fast-JX scheme. In the previous Polair3D version, clouds were taken into account by multiplying the clear-sky photolysis rates by a correction factor. In the new version, clouds are taken into account more accurately by simulating them directly in the photolysis scheme. Differences in photolysis rates inside clouds can be large but outside clouds, and especially at the ground, differences are small. To take into account the impact of aerosols on photolysis rates, Polair3D and Fast-JX are coupled. Photolysis rates are updated every hour. Large impact on photolysis rates is observed at the ground, decreasing with altitude. The aerosol specie that impact the most photolysis rates is dust especially in south Europe. Strong impact is also observed over anthropogenic emission regions (Paris, The Po and the Ruhr Valley) where mainly nitrate and sulphate reduce the incoming radiation. Differences in photolysis rates lead to changes in gas concentrations, with the largest impact simulated on OH and NO concentrations. At the ground, monthly mean concentrations of both species are reduced over Europe by around 10 to 14% and their tropospheric burden by around 10%. The decrease in OH leads to an increase of the life-time of several species such as VOC. NO2 concentrations are not strongly impacted and O3 concentrations are mostly reduced at the ground (−3%). O3 peaks are systematically decreased because of the NO2 photolysis rate coefficient decrease. Not only gas are impacted but also secondary aerosols, due to changes in gas precursors concentrations. However changes in aerosol species concentrations often compensate each other resulting in a low impact on PM10 and PM2.5 concentrations (lower than 2%). The changes in gas concentrations at the ground induced by the modification of photolysis rates (by aerosols and clouds) are compared to changes induced by 29 different model parametrisations in Roustan et al. (2010). Among the 31 model parametrisations, "including aerosols on photolysis rates calculation" has the strongest impact on OH concentrations and on O3 bias in July. In terms of air quality, ground concentrations (NO2, O3, PM10) are compared with measurements. Changes arising from cloud parametrisation are small. Simulation performances are often slightly better when including aerosol in photolysis rates calculation. The systematic O3 peak reduction leads to large differences in the exceedances of the European O3 standard as calculated by the model, in better agreement with measurements. The number of exceedances of the information and the alert threshold is divided by 2 when the aerosol impact on photochemistry is simulated. This shows the importance of taking into account aerosols impact on photolysis rates in air quality studies.
    Atmospheric Chemistry and Physics 01/2011; · 4.88 Impact Factor
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    ABSTRACT: During African Monsoon Multidisciplinary Analyses (AMMA) airborne measurements of ozone, CO and nitrogen oxides (NOx) were collected by French and German Falcon aircraft near three cities in West Africa (Cotonou, Niamey and Ouagadougou). They have been analysed to identify the good conditions to observe ozone plumes related to city emissions during the monsoon season. Results show that an O3 increase of 40–50 ppbv above the summer average concentration took place during two specific events: one near Cotonou on the coast of the Gulf of Guinea, and the other near Niamey in the Sahel region. In both cases a high level of NOx (3–5 ppbv) is related to the ozone production. Air mass transport simulations with FLEXPART and a tracer simulation with the BOLAM mesoscale model shows that Southern Hemisphere biomass burning emissions are always at higher altitude (>3 km) compared to the city emissions. In Niamey and Ouagadougou, the daily variability of ozone and CO correlates with the FLEXPART analysis showing the role of air mass stagnation near the city for 1–2 days and advection of emissions from the vegetated areas. Absence of ozone enhancements for high CO values can be explained by the occurrence of deep convection near the city. In the Sahel region, convection must be accounted for to understand the small number of observed ozone plumes but also to explain the high level of NOx in the 3–5 ppbv range, due to increasing soil emissions after rainfall. To verify that daily ozone production can reach 20 ppbv day−1 for the NOx and CO conditions encountered near West African cities, a simulation of the CiTTyCAT Lagrangian model was conducted using the observed average chemical composition reported by other aircraft during AMMA. Such ozone production is possible for NOx levels up to 5 ppb showing that West African cities are potentially significant sources of tropospheric ozone.
    Atmospheric Chemistry and Physics. 01/2011; 11(2010-11-10):6349-6366.
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    ABSTRACT: No abstract available.
    ATMOSPHERIC CHEMISTRY AND PHYSICS 10/2010; 10:10939-10940. · 5.51 Impact Factor
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    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 370K (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 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 CO2) 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. O3-poor) or polluted air masses from Asia (high O3, CO, CO2) into West Africa. Thus, recent uplift of CO2 over Asia may contribute to the observed positive CO2 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 O3 and NOy. 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 photochemical O3 production, initialised with observations, suggest that the lower TTL is significantly impacted by uplift of O3 precursors (over Africa and Asia) leading to positive production rates (up to 2 ppbv per day) in the lower and mid TTL even at moderate NOx levels. Photochemical O3 production increases with higher NOx and H2O in air masses with O3 less than 150 ppbv.
    ATMOSPHERIC CHEMISTRY AND PHYSICS 01/2010; 10(2010):10753-10770. · 5.51 Impact Factor
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    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 (O3) downwind over the Atlantic Ocean. Their possible contribution to the Atlantic O3 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 model 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 (CO2) 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. Runs using a photochemical trajectory model, CiTTy- CAT, initialized with the observations, were used to estimate in-situ net photochemical O3 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 O3 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 O3 concentrations. These results suggest that a significant fraction of enhanced O3 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 O3 enhancement in the equatorial south Atlantic MT, at least in August 2006. The upper tropospheric plume was also still photochemically active, although mean net O3 production rates were slower (1.3 ppbv/day). The results suggest that, whilst the transport of BB pollutants to the UT is variable (as shown by the mesoscale model simulations), pollution from biom ss burning can make an important contribution to additional photochemical production of O3 in addition to other important sources such as nitrogen oxides (NOx) from lightning.
    Atmospheric Chemistry and Physics. 01/2010; 10(2010):3027-3046.
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    Atmospheric Chemistry and Physics, v.10, 10753-10770 (2010). 01/2010;
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    ABSTRACT: During the African Monsoon Multidisciplinary Analyses (AMMA) airborne measurements of ozone, CO and nitrogen oxides by the French and German falcon aircraft took place near three cities in West Africa (Cotonou, Niamey and Ouagadougou). Significant ozone production (O3 increase of 40–50 ppbv) took place during two specific events: one near Cotonou on the coast of the Guinea Gulf, and the other near Niamey in the Sahel region. In both cases a high level of NOx (>3 ppbv) is related to the ozone production. The ozone production is mainly driven by the Lagos-Cotonou anthropogenic emissions in Cotonou. In Niamey the combined effect of advection of VOC emissions from the forest and stagnation over the city area and the poorly vegetated soils recently wetted by convected systems is needed to achieve a similar level of ozone precursors. In Ouagadougou no ozone plume is found because of the absence of a pause in the convective activity and of the larger vegetated area around the city which prevented ozone plume formation during the wet season. To discuss the ozone increase near Cotonou two different approaches have been implemented: a FLEXPART simulation to quantify the probability of transport from the SH compared to air mass stagnation over the emission area and a simulation of the BOLAM mesoscale model with two different tracers for the anthropogenic emission (RETRO inventory for 2000) and the biomass burning. The BOLAM model shows a good agreement with the meteorological observations of the aircraft and allows to identify the key influence of the anthropogenic emissions in the first 3 km while the biomass burning plume remains above this altitude. The day to day variability of the ozone and CO in Niamey and Ouagadougou is discussed using FLEXPART simulations of the air mass stagnation in the 12° N–14° N latitude band and northward advection of air masses from the vegetated areas influenced by the biogenic volatile organic compound (VOC) emissions. Both conditions need to be fulfilled to be able to detect ozone increase within the city plume. The first condition is necessary to obtain a significant increase of the NOx concentrations by combining the city emission and the soil emission. It also shows that, contrary to the Niamey conditions, the Ouagadougou air mass transport and its timing respective to the convective activity did not correspond to favourable conditions for O3 formation during the time period of the aircraft data. Finally to check the magnitude of the ozone production related to the observed CO and NOx observations, a 2-days stationary run of the CittyCAT Lagrangian model was conducted at Cotonou location. The initialisation of the chemical concentrations not measured is done by scaling to the NOx and CO concentrations observed in the polluted plume. The scaling factor is derived from the low altitude observations provided by the DF20 and the BAe-146 aircraft during the AMMA campaign. Under such conditions, the simulation show that 50 ppbv of ozone can be produced in a 2-days period.
    Atmospheric Chemistry and Physics 01/2010; · 4.88 Impact Factor
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    ABSTRACT: This paper presents results from a new method, ZooM-CiTTy, that aims to accurately reproduce filamentation observed in profiles of chemically active species in the free troposphere. Lagrangian tracer reconstructions of aircraft measurements across pollutant plumes including a stochastic representation of mixing are coupled with photochemical trajectory simulations, initialized with global model fields. The results provide a high-resolution simulation of trace gases along the flight track together with a detailed picture about the multiple air mass origins influencing chemical composition in the region where plume measurements were taken. This paper builds on results from Pisso et al. (2009) for the dynamic part of the model (the stochastic tracer reconstructions) and focuses on reconstruction of reactive species like O3. The model is evaluated for a case of long-range transport of a forest fire plume from Alaska to Europe. Simulated trace species are compared with measurements made in the plume by the DLR Falcon aircraft flying over Europe, and the role of photochemistry in governing the chemical composition across the plume is evaluated. It is shown that the model reproduces well O3 and NOy concentrations and O3 production per CO in the plumes as well as gradients at plume edges. In particular, because ZooM-CiTTy represents the contribution of several air masses to a measurement at a particular location, the model can reproduce so-called mixing lines between air masses. Results show that photochemistry and mixing contributions vary in different parts of the plume and that resulting trace gas correlations are a combination of these different mixtures. One limitation of the method is the fact that mixing between air masses is only performed at the end of the trajectories. Errors on simulated O3 reconstruction from this formulation are evaluated. These errors seems to be negligible in this case (in the free troposphere, far from emission region) because strong gradients are maintained by large-scale winds. Results from ZooM-CiTTy are also used to evaluate errors due to nonlinearities in O3 photochemistry in coarse-grid models. It is shown that in cases where strong gradients are maintained, errors in net O3 production can be as high as 50% at plumes edges. This new method is interesting to simulate relatively small layering structures observed in the free troposphere, but a more realistic treatment of mixing “en route” is needed if the model has to be used more extensively.
    Journal of Geophysical Research 01/2010; 115(2010-06-18-D12302):1-14. · 3.17 Impact Factor
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    ABSTRACT: In the paper “Air mass origins influencing TTL chemical composition over West Africa during 2006 summer monsoon” by K. S. Law et al. (Atmos. Chem. Phys., 10, 10753–10770, doi:10.5194/acp-10-10753-2010, 2010) a problem occurred in the final production process regarding Fig. 10b.
    Atmospheric Chemistry and Physics. 01/2010; 10(2010):10939-10940.
  • Geochmica et Cosmochimica Acta 06/2009;
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    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 mid-latitude lower stratosphere was under-sampled (in the mid-upper 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 westerly 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 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 short-lived species 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., O3-poor) or polluted air masses from Asia (high O3, CO, CO2) into West Africa. Thus, recent uplift of CO2 over Asia may contribute to the observed positive CO2 gradients in the TTL over West Africa. This suggests a more significant fraction of younger air masses in the TTL making it difficult to derive mean age of air from average gradients. 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 O3 and NOy. 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 photochemical O3 production, initialised with observations, suggest that the lower TTL is significantly impacted by uplift of O3 precursors (over Africa and Asia) leading to positive production rates (up to 2 ppbv per day) in the lower and mid TTL even at moderate NOx levels. Photochemical O3 production increases with higher NOx and H2O in air masses with O3 less than 150 ppbv.
    Atmospheric Chemistry and Physics. 01/2009;
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    ABSTRACT: Pollutant plumes with enhanced levels 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 both the origin of these pollutant plumes and their potential to produce O3 downwind over the Atlantic Ocean. Runs using the BOLAM mesoscale model including biomass burning CO tracers were used to confirm an origin from central African fires. The plumes in the mid troposphere had significantly higher pollutant concentrations due to the fact that transport occurred from a region nearer or even over the fire region. In contrast, plumes transported into the upper troposphere over West Africa had been transported to the north-east of the fire region before being uplifted. Modelled tracer results showed that pollutants resided for between 9 and 12 days over Central Africa before being transported for 4 days, in the case of the mid-troposphere plume and 2 days in the case of the upper tropospheric plume to the measurement location over the southern part of West Africa. Around 35% of the biomass burning tracer was transported into the upper troposphere compared to that remaining in the mid troposphere. Runs using a photochemical trajectory model, CiTTyCAT, were used to estimate the net photochemical O3 production potential of these plumes. The mid tropospheric plume was still very photochemically active (up to 7 ppbv/day) especially during the first few days of transport westward over the Atlantic Ocean. The upper tropospheric plume was also still photochemically active, although at a slower rate (1–2 ppbv/day). Trajectories show this plume being recirculated around an upper tropospheric anticyclone back towards the African continent (around 20° S). The potential of theses plumes to produce O3 supports the hypothesis that biomass burning pollutants are contributing to the observed O3 maxima over the southern Atlantic at this time of year.
    Atmospheric Chemistry and Physics 01/2009; · 4.88 Impact Factor
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    ABSTRACT: The dispersion and mixing of pollutant plumes during long-range transport across the North Atlantic is studied using ensembles of diffusive backward trajectories in order to estimate turbulent diffusivity coefficients in the free troposphere under stratified flow conditions. Values of the order of 0.3–1 m2 s−1 and 1 × 104 m2 s−1 for the vertical and horizontal diffusivity coefficients Dv and Dh , respectively, are derived. Uncertainties related to the method are discussed, and results are compared with previous estimates of atmospheric mixing rates. These diffusivity estimates also yield an estimate of the vertical/horizontal aspect ratio of tracer structures in the troposphere. Results from this case study are used to estimate grid resolutions needed to accurately simulate the intercontinental transport of pollutants as being of the order of 500 m in the vertical and at least 40 km in the horizontal. This work forms the basis of high-resolution chemical simulations using ensembles of diffusive backward trajectories.
    Journal of Geophysical Research 01/2009; 114(2009-D19301):1-11. · 3.17 Impact Factor
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    ABSTRACT: The photochemical evolution of an anthropogenic plume from the New-York/Boston region during its transport at low altitudes over the North Atlantic to the European west coast has been studied using a Lagrangian framework. This plume, originally strongly polluted, was sampled by research aircraft just off the North American east coast on 3 successive days, and 3 days downwind off the west coast of Ireland where another aircraft re-sampled a weakly polluted plume. Changes in trace gas concentrations during transport were reproduced using a photochemical trajectory model including deposition and mixing effects. Chemical and wet deposition processing dominated the evolution of all pollutants in the plume. The mean net O3 production was evaluated to be -5 ppbv/day leading to low values of O3 by the time the plume reached Europe. Wet deposition of nitric acid was responsible for an 80% reduction in this O3 production. If the plume had not encountered precipitation, it would have reached the Europe with O3 levels up to 80-90 ppbv, and CO levels between 120 and 140 ppbv. Photochemical destruction also played a more important role than mixing in the evolution of plume CO due to high levels of both O3 and water vapour showing that CO cannot always be used as a tracer for polluted air masses, especially for plumes transported at low altitudes. The results also show that, in this case, an important increase in the O3/CO slope can be attributed to chemical destruction of CO and not to photochemical O3 production as is often assumed.
    Atmospheric Chemistry and Physics 01/2008; 8(2008):7737-7754. · 4.88 Impact Factor
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    ABSTRACT: During the AMMA2006 campaign, aircraft measurements often revealed the presence of polluted air masses with the chemical characteristics of biomass burning plumes in the free troposphere and in the upper troposphere over the Gulf of Guinea. The analyses carried out within the AMMA project suggest that the main emission region is central Africa during the south hemisphere dry season. This study shows the importance of convective uplift by large mesoscale convective systems for the transport of southern biomass burning emissions into the upper troposphere over West Africa. Such a mechanism allows rapid transport of pollutants up to 14 km where they are transported westward by the tropical easterly jet. The latitudinal distribution of the biomass burning plume and its content in CO, CO2 and O3 is determined with observations onboard three aircrafts (D-F20, BAE-146, M55-Geophysica) for a case study during the Monsoon season in 2006 and increased concentrations are found south of 8°N below 600 hPa and around of 5°N at 200 hPa. An analysis of the origin of the air masses sampled during the AMMA campaign and the transport pathways was carried out using the Lagrangian particle dispersion model FLEXPART and the mesoscale meteorological model BOLAM. The mesoscale model was nudged with cloud top brightness temperatures derived from Meteosat measurements in order to accurately reproduce the position and the life cycle of convective systems over central and western Africa.
    European Geosciences Union, General Assembly 2008; 01/2008
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    ABSTRACT: The photochemical evolution of an anthropogenic plume from the New-York/Boston region during its transport at low altitudes over the North Atlantic to the European west coast has been studied using a Lagrangian framework. This plume, originally strongly polluted, was sampled by research aircraft just off the North American east coast on 3 successive days, and then 3 days downwind off the west coast of Ireland where another aircraft re-sampled a weakly polluted plume. Changes in trace gas concentrations during transport are reproduced using a photochemical trajectory model including deposition and mixing effects. Chemical and wet deposition processing dominated the evolution of all pollutants in the plume. The mean net photochemical O3 production is estimated to be −5 ppbv/day leading to low O3 by the time the plume reached Europe. Model runs with no wet deposition of HNO3 predicted much lower average net destruction of −1 ppbv/day O3, arising from increased levels of NOx via photolysis of HNO3. This indicates that wet deposition of HNO3 is indirectly responsible for 80% of the net destruction of ozone during plume transport. If the plume had not encountered precipitation, it would have reached Europe with O3 concentrations of up to 80 to 90 ppbv and CO between 120 and 140 ppbv. Photochemical destruction also played a more important role than mixing in the evolution of plume CO due to high levels of O3 and water vapour showing that CO cannot always be used as a tracer for polluted air masses, especially in plumes transported at low altitudes. The results also show that, in this case, an increase in O3/CO slopes can be attributed to photochemical destruction of CO and not to photochemical O3 production as is often assumed.
    ATMOSPHERIC CHEMISTRY AND PHYSICS 01/2008; · 5.51 Impact Factor
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    ABSTRACT: 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 NOy, mainly in form of PAN. Observed O3 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 O3 production and 24% in O3 destruction over 5 days when including aerosols. The plume is found to be chemically active with large O3 increases attributed primarily to PAN decomposition during descent of the plume toward Europe. The predicted O3 changes are very dependent on temperature changes during transport and also on water vapor levels in the lower troposphere which can lead to O3 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 O3/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 O3 production. The possible impact of this biomass burning plume on O3 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 O3 increases and elevated CO levels. The model predicts significant changes in O3 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 O3 impact of Alaskan fires can be potentially significant over Europe.
    Journal of Geophysical Research 05/2007; 112(2007-D10S41):1-19. · 3.17 Impact Factor
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    ABSTRACT: During the ICARTT-ITOP Experiment in summer 2004 plumes from large wildfires in North America were transported to Central Europe at 3–8 km altitude above sea level (a.s.l.). These plumes were studied with the DLR (Deutsches Zentrum fuer Luft- und Raumfahrt) research aircraft Falcon which was equipped with an extensive set of in situ aerosol and trace gas instruments. Analyses by the Lagrangian dispersion model FLEXPART provided source regions, transport times and horizontal extent of the fire plumes. Results from the general circulation model ECHAM/MADE and data from previous aerosol studies over Central Europe provided reference vertical profiles of black carbon (BC) mass concentrations for year 2000 conditions with forest fire activities below the long-term average. Smoke plume observations yielded a BC mass fraction of total aerosol mass with respect to PM2.5 of 3–10%. The ratio of BC mass to excess CO was 3–7.5 mg BC (g CO)<sup>-1</sup>. Even after up to 10 days of atmospheric transport, both characteristic properties were of the same order as for fresh emissions. This suggests an efficient lifting of BC from forest fires to higher altitudes with only minor scavenging removal of particulate matter. Maximum aerosol absorption coefficient values were 7–8×10<sup>-6</sup>m<sup>-1</sup> which is about two orders of magnitude above the average European free tropospheric background value. Forest fire aerosol size distributions were characterised by a strong internally mixed accumulation mode centred at modal diameters of 0.25–0.30 μm with an average distribution width of 1.30. Nucleation and small Aitken mode particles were almost completely depleted. Even after more than one week of atmospheric transport, no steady state of the size distribution was observed.
    ATMOSPHERIC CHEMISTRY AND PHYSICS 01/2007; 7(2007):5105-5127. · 5.51 Impact Factor
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    ABSTRACT: In summer 2004 the long-range transport of particles emitted from large forest fires in Canada and Alaska contributed significantly to the aerosol loading of the free troposphere over Europe . Airborne in situ measurements on the intercontinental transport of aerosols from biogenic and anthropogenic origin were performed at the European west coast as a part of the ICARTT-ITOP study (Intercontinental Transport of Ozone and Precursors). During the study the German Falcon 20 E-5 research aircraft was operating from an airport north of Paris. The aircraft was equipped with extensive in-situ aerosol and trace gas instrumentation. Measurement flights were performed over the European west coast probing the entire tropospheric column from the boundary layer to the upper free troposphere. Trajectory analyses were conducted for all the measurement flights and permitted the identification of the plume origin for several forest fires cases. Simultaneously to the airborne in-situ measurements, black carbon data from the high-alpine research station Jungfraujoch (JFJ; 3580 m asl) in Switzerland showed elevated BC levels during this period. Trajectory analyses confirmed that the JFJ station was probing the same forest fire plume as the Falcon during the measurement flights at the European West coast.
    International Aerosol Conference; 09/2006
  • EGU General Assembly 2006; 01/2006

Publication Stats

202 Citations
51.09 Total Impact Points

Institutions

  • 2011
    • Université de Versailles Saint-Quentin
      Versailles, Île-de-France, France
  • 2005–2010
    • Pierre and Marie Curie University - Paris 6
      Lutetia Parisorum, Île-de-France, France
  • 2009
    • LATMOS
      Guyancourt, Île-de-France, France
  • 2007
    • French National Centre for Scientific Research
      Lutetia Parisorum, Île-de-France, France