scholarly journals Emission sources contributing to tropospheric ozone over Equatorial Africa during the summer monsoon

2011 ◽  
Vol 11 (24) ◽  
pp. 13395-13419 ◽  
Author(s):  
I. Bouarar ◽  
K. S. Law ◽  
M. Pham ◽  
C. Liousse ◽  
H. Schlager ◽  
...  

Abstract. A global chemistry-climate model LMDz_INCA is used to investigate the contribution of African and Asian emissions to tropospheric ozone over Central and West Africa during the summer monsoon. The model results show that ozone in this region is most sensitive to lightning NOx and to Central African biomass burning emissions. However, other emission categories also contribute significantly to regional ozone. The maximum ozone changes due to lightning NOx occur in the upper troposphere between 400 hPa and 200 hPa over West Africa and downwind over the Atlantic Ocean. Biomass burning emissions mainly influence ozone in the lower and middle troposphere over Central Africa, and downwind due to westward transport. Biogenic emissions of volatile organic compounds, which can be uplifted from the lower troposphere to higher altitudes by the deep convection that occurs over West Africa during the monsoon season, lead to maximum ozone changes in the lower stratosphere region. Soil NOx emissions over the Sahel region make a significant contribution to ozone in the lower troposphere. In addition, convective uplift of these emissions and subsequent ozone production are also an important source of ozone in the upper troposphere over West Africa. Concerning African anthropogenic emissions, they only make a small contribution to ozone compared to the other emission categories. The model results indicate that most ozone changes due to African emissions occur downwind, especially over the Atlantic Ocean, far from the emission regions. The import of Asian emissions also makes a considerable contribution to ozone concentrations above 150 hPa and has to be taken into account in studies of the ozone budget over Africa. Using IPCC AR5 (Intergovernmental Panel on Climate Change; Fifth Assessment Report) estimates of anthropogenic emissions for 2030 over Africa and Asia, model calculations show larger changes in ozone over Africa due to growth in Asian emissions compared to African emissions over the next 20 yr.

2011 ◽  
Vol 11 (5) ◽  
pp. 13769-13827
Author(s):  
I. Bouarar ◽  
K. S. Law ◽  
M. Pham ◽  
C. Liousse ◽  
H. Schlager ◽  
...  

Abstract. A global chemistry-climate model LMDz_INCA is used to investigate the contribution of African and Asian emissions to tropospheric ozone over central and West Africa during the summer monsoon. The model results show that ozone in this region is most sensitive to lightning NOx and to central African biomass burning emissions. However, other emission categories also contribute significantly to regional ozone. The maximum ozone changes due to lightning NOx occur in the upper troposphere between 400 hPa and 200 hPa over West Africa and downwind over the Atlantic Ocean. Biomass burning emissions mainly influence ozone in the lower and middle troposphere over central Africa, and downwind due to westward transport. Biogenic emissions of volatile organic compounds, which can be uplifted from the lower troposphere into higher altitudes by the deep convection that occurs over West Africa during the monsoon season, dominate the ozone changes in the upper troposphere and lower stratosphere region. Convective uplift of soil NOx emissions over the Sahel region also makes a significant contribution to ozone in the upper troposphere. Concerning African anthropogenic emissions, they make a lower contribution to ozone compared to the other emission categories. The model results indicate that most ozone changes due to African emissions occur downwind, especially over the Atlantic Ocean, far from the emission regions. The influence of Asian emissions should also be taken into account in studies of the ozone budget over Africa since they make a considerable contribution to ozone concentrations above 150 hPa. Using IPCC AR5 (Intergovernmental Panel on Climate Change; Fifth Assessment Report) estimates of anthropogenic emissions for 2030 over Africa and Asia, the model calculations suggest largest changes in ozone due to the growth of emissions over Asia than over Africa over the next 20 years.


2006 ◽  
Vol 6 (6) ◽  
pp. 11465-11520 ◽  
Author(s):  
B. Sauvage ◽  
R. V. Martin ◽  
A. van Donkelaar ◽  
X. Liu ◽  
K. Chance ◽  
...  

Abstract. We use a global chemical transport model (GEOS-Chem) to evaluate the consistency of satellite measurements of lightning flashes and ozone precursors with in situ measurements of tropical tropospheric ozone. The measurements are tropospheric O3, NO2, and HCHO columns from the GOME satellite instrument, lightning flashes from the OTD and LIS instruments, profiles of O3, CO, and relative humidity from the MOZAIC aircraft program, and profiles of O3 from the SHADOZ ozonesonde network. We interpret these multiple data sources with our model to better understand what controls tropical tropospheric ozone. Tropical tropospheric ozone is mainly affected by lightning and convection in the upper troposphere and by surface emissions in the lower troposphere. Scaling the spatial distribution of lightning in the model to the observed flash counts improves the simulation of O3 in the upper troposphere by 5–20 ppbv versus in situ observations and by 1–4 Dobson Units versus GOME retrievals of tropospheric O3 columns. A lightning source strength of 5±2 Tg N/yr best represents in situ observations from aircraft and ozonesonde. Tropospheric NO2 and HCHO columns from GOME are applied to provide top-down constraints on emission inventories of NOx (biomass burning and soils) and VOCs (biomass burning). The top-down biomass burning inventory is larger by a factor of 2 for HCHO and alkenes, and by 2.6 for NOx over northern equatorial Africa. These emissions increase lower tropospheric O3 by 5–20 ppbv, improving the simulation versus aircraft observations, and by 4 Dobson Units versus GOME observations of tropospheric O3 columns. Emission factors in the a posteriori inventory are more consistent with a recent compilation from in situ measurements. The ozone simulation using two different dynamical schemes (GEOS-3 and GEOS-4) is evaluated versus observations; GEOS-4 better represents O3 observations by 5–15 ppbv due to enhanced convective detrainment in the upper troposphere. Heterogeneous uptake of HNO3 on aerosols reduces simulated O3 by 5–7 ppbv, reducing a model bias versus in situ observations over and downwind of deserts. Exclusion of HO2 uptake on aerosols improves O3 by 5 ppbv in biomass burning regions.


2010 ◽  
Vol 10 (6) ◽  
pp. 3027-3046 ◽  
Author(s):  
E. Real ◽  
E. Orlandi ◽  
K. S. Law ◽  
F. Fierli ◽  
D. Josset ◽  
...  

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 north-east 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, CiTTyCAT, 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 biomass 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.


2009 ◽  
Vol 9 (4) ◽  
pp. 17385-17427 ◽  
Author(s):  
E. Real ◽  
E. Orlandi ◽  
K. S. Law ◽  
F. Fierli ◽  
D. Josset ◽  
...  

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.


2010 ◽  
Vol 10 (16) ◽  
pp. 7575-7601 ◽  
Author(s):  
C. E. Reeves ◽  
P. Formenti ◽  
C. Afif ◽  
G. Ancellet ◽  
J.-L. Attié ◽  
...  

Abstract. During June, July and August 2006 five aircraft took part in a campaign over West Africa to observe the aerosol content and chemical composition of the troposphere and lower stratosphere as part of the African Monsoon Multidisciplinary Analysis (AMMA) project. These are the first such measurements in this region during the monsoon period. In addition to providing an overview of the tropospheric composition, this paper provides a description of the measurement strategy (flights performed, instrumental payloads, wing-tip to wing-tip comparisons) and points to some of the important findings discussed in more detail in other papers in this special issue. The ozone data exhibits an "S" shaped vertical profile which appears to result from significant losses in the lower troposphere due to rapid deposition to forested areas and photochemical destruction in the moist monsoon air, and convective uplift of ozone-poor air to the upper troposphere. This profile is disturbed, particularly in the south of the region, by the intrusions in the lower and middle troposphere of air from the southern hemisphere impacted by biomass burning. Comparisons with longer term data sets suggest the impact of these intrusions on West Africa in 2006 was greater than in other recent wet seasons. There is evidence for net photochemical production of ozone in these biomass burning plumes as well as in urban plumes, in particular that from Lagos, convective outflow in the upper troposphere and in boundary layer air affected by nitrogen oxide emissions from recently wetted soils. This latter effect, along with enhanced deposition to the forested areas, contributes to a latitudinal gradient of ozone in the lower troposphere. Biogenic volatile organic compounds are also important in defining the composition both for the boundary layer and upper tropospheric convective outflow. Mineral dust was found to be the most abundant and ubiquitous aerosol type in the atmosphere over Western Africa. Data collected within AMMA indicate that injection of dust to altitudes favourable for long-range transport (i.e. in the upper Sahelian planetary boundary layer) can occur behind the leading edge of mesoscale convective system (MCS) cold-pools. Research within AMMA also provides the first estimates of secondary organic aerosols across the West African Sahel and have shown that organic mass loadings vary between 0 and 2 μg m−3 with a median concentration of 1.07 μg m−3. The vertical distribution of nucleation mode particle concentrations reveals that significant and fairly strong particle formation events did occur for a considerable fraction of measurement time above 8 km (and only there). Very low concentrations were observed in general in the fresh outflow of active MCSs, likely as the result of efficient wet removal of aerosol particles due to heavy precipitation inside the convective cells of the MCSs. This wet removal initially affects all particle size ranges as clearly shown by all measurements in the vicinity of MCSs.


2010 ◽  
Vol 10 (3) ◽  
pp. 7115-7183 ◽  
Author(s):  
C. E. Reeves ◽  
P. Formenti ◽  
C. Afif ◽  
G. Ancellet ◽  
J.-L. Attie ◽  
...  

Abstract. During June, July and August 2006 five aircraft took part in a campaign over West Africa to observe the aerosol content and chemical composition of the troposphere and lower stratosphere as part of the African Monsoon Multidisciplinary Analysis (AMMA) project. These are the first such measurements in this region during the monsoon period. In addition to providing an overview of the tropospheric composition, this paper provides a description of the measurement strategy (flights performed, instrumental payloads, wing-tip to wing-tip comparisons) and points to some of the important findings discussed in more detailed in other papers in this special issue. The ozone data exhibits an "S" shaped vertical profile which appears to result from significant losses in the lower troposphere due to rapid deposition to forested areas and photochemical destruction in the moist monsoon air, and convective uplift of O3-poor air to the upper troposphere. This profile is disturbed, particularly in the south of the region, by the intrusions in the lower and middle troposphere of air from the Southern Hemisphere impacted by biomass burning. Comparisons with longer term data sets suggest the impact of these intrusions on West Africa in 2006 was greater than in other recent wet seasons. There is evidence for net photochemical production of ozone in these biomass burning plumes as well as in urban plumes, in particular that from Lagos, convective outflow in the upper troposphere and in boundary layer air affected by nitrogen oxide emissions from recently wetted soils. This latter effect, along with enhanced deposition to the forested areas, contributes to a latitudinal gradient of ozone in the lower troposphere. Biogenic volatile organic compounds are also important in defining the composition both for the boundary layer and upper tropospheric convective outflow. Mineral dust was found to be the most abundant and ubiquitous aerosol type in the atmosphere over Western Africa. Data collected within AMMA indicate that injection of dust to altitudes favourable for long-range transport (i.e. in the upper Sahelian planetary boundary layer) can occur behind the leading edge of mesoscale convective system (MCS) cold-pools. Research within AMMA also provides the first estimates of secondary organic aerosols (SOA) across the West African Sahel and have shown that organic mass loadings vary between 0 and 2 μg m−3 with a median concentration of 1.07 μg m−3. The vertical distribution of nucleation mode particle concentrations reveals that significant and fairly strong particle formation events did occur for a considerable fraction of measurement time above 8 km (and only there). Very low aerosol concentrations were observed in general in the fresh outflow of active MCSs, likely as the result of efficient wet removal of aerosol particles due to heavy precipitation inside the convective cells of the MCSs. This wet removal initially affects all particle size ranges as clearly shown by all measurements in the vicinity of MCSs.


2016 ◽  
Author(s):  
Gerard Ancellet ◽  
Nikos Daskalakis ◽  
Jean Christophe Raut ◽  
Boris Quennehen ◽  
François Ravetta ◽  
...  

Abstract. The goal of the paper are to: (1) present tropospheric ozone (O3) climatologies in summer 2008 based on a large amount of measurements, during the International Polar Year when the Polar Study using Aircraft, Remote Sensing, Surface Measurements, and Models of Climate Chemistry, Aerosols, and Transport (POLARCAT) campaigns were conducted (2) investigate the processes that determine O3 concentrations in two different regions (Canada and Greenland) that were thoroughly studied using measurements from 3 aircraft and 7 ozonesonde stations. This paper provides an integrated analysis of these observations and the discussion of the latitudinal and vertical variability of tropospheric ozone north of 55° N during this period is performed using a regional model (WFR-Chem). Ozone, CO and potential vorticity (PV) distributions are extracted from the simulation at the measurement locations. The model is able to reproduce the O3 latitudinal and vertical variability but a negative O3 bias of 6–15 ppbv is found in the free troposphere over 4 km, especially over Canada. Ozone average concentrations are of the order of 65 ppbv at altitudes above 4 km both over Canada and Greenland, while they are less than 50 ppbv in the lower troposphere. The relative influence of stratosphere-troposphere exchange (STE) and of ozone production related to the local biomass burning (BB) emissions is discussed using differences between average values of O3, CO and PV for Southern and Northern Canada or Greenland and two vertical ranges in the troposphere: 0–4 km and 4–8 km. For Canada, the model CO distribution and the weak correlation (< 30 %) of O3 and PV suggests that stratosphere-troposphere exchange (STE) is not the major contribution to average tropospheric ozone at latitudes less than 70° N, due to the fact that local biomass burning (BB) emissions were significant during the 2008 summer period. Conversely over Greenland, significant STE is found according to the better O3 versus PV correlation (> 40 %) and the higher 75th PV percentile. A weak negative latitudinal summer ozone gradient −6 to −8 ppbv is found over Canada in the mid troposphere between 4 and 8 km. This is attributed to an efficient O3 photochemical production due to the BB emissions at latitudes less than 65° N, while STE contribution is more homogeneous in the latitude range 55° N to 70° N. A positive ozone latitudinal gradient of 12 ppbv is observed in the same altitude range over Greenland not because of an increasing latitudinal influence of STE, but because of different long range transport from multiple mid-latitude sources (North America, Europe and even Asia for latitudes higher than 77° N).


Author(s):  
Alima Dajuma ◽  
Siélé Silué ◽  
Kehinde O. Ogunjobi ◽  
Heike Vogel ◽  
Evelyne Touré N’Datchoh ◽  
...  

2004 ◽  
Vol 4 (3) ◽  
pp. 3285-3332 ◽  
Author(s):  
B. Sauvage ◽  
V. Thouret ◽  
J.-P. Cammas ◽  
F. Gheusi ◽  
G. Athier ◽  
...  

Abstract. We analyze MOZAIC ozone observations recorded over Equatorial Africa, from April 1997 to March 2003 to give the first ozone climatology of this region. The monthly mean vertical profiles have been systematically analyzed with monthly mean ECMWF data using a Lagrangian-model (LAGRANTO). We assess the roles played by the dynamical features of Equatorial Africa and the intense biomass burning sources within the region in defining the ozone distribution. The lower troposphere exhibits layers of enhanced ozone during the biomass burning season in each hemisphere (boreal winter in the northern tropics and boreal summer in the southern tropics). The monthly mean vertical profiles of ozone are clearly influenced by the local dynamical situation. Over the Gulf of Guinea during boreal winter, the ozone profile is characterized by systematically high ozone below 650 hPa. This is due to the high stability caused by the Harmattan winds in the lower troposphere and the blocking Saharan anticyclone in the middle troposphere that prevents any efficient vertical mixing. In contrast, Central African enhancements are not only found in the lower troposphere but throughout the troposphere. The boreal summer ozone maximum in the lower troposphere of Central Africa continues up to November in the middle troposphere due to the influx of air masses laden with biomass burning products from Brazil and Southern Africa. Despite its southern latitude, Central Africa during the boreal winter is also under the influence of the northern tropical fires. This phenomenon is known as the "ozone paradox". However, the tropospheric ozone columns calculated from the MOZAIC data give evidence that the Tropical Tropospheric Ozone Column (TTOC) maximum over Africa swings from West Africa in DJF to Central Africa in JJA. This contrasts with studies based on TOMS satellite data. A rough assessment of the regional ozone budget shows that the northern tropics fires in boreal winter might contribute up to 20% of the global photochemical ozone production. This study gives the first detailed picture of the ozone distribution over Equatorial Africa that should be used to validate both global models over this region and future satellite products.


Author(s):  
Alima Dajuma ◽  
Siélé Silué ◽  
Kehinde O. Ogunjobi ◽  
Heike Vogel ◽  
Evelyne Touré N’Datchoh ◽  
...  

Sign in / Sign up

Export Citation Format

Share Document