Large contribution of biomass burning emissions to ozone throughout the global remote troposphere

Ozone is the third most important anthropogenic greenhouse gas after carbon dioxide and methane but has a larger uncertainty in its radiative forcing, in part because of uncertainty in the source characteristics of ozone precursors, nitrogen oxides, and volatile organic carbon that directly affect ozone formation chemistry. Tropospheric ozone also negatively affects human and ecosystem health. Biomass burning (BB) and urban emissions are significant but uncertain sources of ozone precursors. Here, we report global-scale, in situ airborne measurements of ozone and precursor source tracers from the NASA Atmospheric Tomography mission. Measurements from the remote troposphere showed that tropospheric ozone is regularly enhanced above background in polluted air masses in all regions of the globe. Ozone enhancements in air with high BB and urban emission tracers (2.1 to 23.8 ppbv [parts per billion by volume]) were generally similar to those in BB-influenced air (2.2 to 21.0 ppbv) but larger than those in urban-influenced air (−7.7 to 6.9 ppbv). Ozone attributed to BB was 2 to 10 times higher than that from urban sources in the Southern Hemisphere and the tropical Atlantic and roughly equal to that from urban sources in the Northern Hemisphere and the tropical Pacific. Three independent global chemical transport models systematically underpredict the observed influence of BB on tropospheric ozone. Potential reasons include uncertainties in modeled BB injection heights and emission inventories, export efficiency of BB emissions to the free troposphere, and chemical mechanisms of ozone production in smoke. Accurately accounting for intermittent but large and widespread BB emissions is required to understand the global tropospheric ozone burden.

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Global-scale distribution of ozone in the remote troposphere from the ATom and HIPPO airborne field missions

Atmospheric Chemistry and Physics ◽

10.5194/acp-20-10611-2020 ◽

2020 ◽

Vol 20 (17) ◽

pp. 10611-10635 ◽

Cited By ~ 2

Author(s):

Ilann Bourgeois ◽

Jeff Peischl ◽

Chelsea R. Thompson ◽

Kenneth C. Aikin ◽

Teresa Campos ◽

...

Keyword(s):

Tropospheric Ozone ◽

Large Scale ◽

Marine Boundary Layer ◽

Global Climate ◽

Global Scale ◽

Ozone Production ◽

Commercial Aircraft ◽

The Pacific ◽

Vertical Distributions ◽

Remote Troposphere

Abstract. Ozone is a key constituent of the troposphere, where it drives photochemical processes, impacts air quality, and acts as a climate forcer. Large-scale in situ observations of ozone commensurate with the grid resolution of current Earth system models are necessary to validate model outputs and satellite retrievals. In this paper, we examine measurements from the Atmospheric Tomography (ATom; four deployments in 2016–2018) and the HIAPER Pole-to-Pole Observations (HIPPO; five deployments in 2009–2011) experiments, two global-scale airborne campaigns covering the Pacific and Atlantic basins. ATom and HIPPO represent the first global-scale, vertically resolved measurements of O3 distributions throughout the troposphere, with HIPPO sampling the atmosphere over the Pacific and ATom sampling both the Pacific and Atlantic. Given the relatively limited temporal resolution of these two campaigns, we first compare ATom and HIPPO ozone data to longer-term observational records to establish the representativeness of our dataset. We show that these two airborne campaigns captured on average 53 %, 54 %, and 38 % of the ozone variability in the marine boundary layer, free troposphere, and upper troposphere–lower stratosphere (UTLS), respectively, at nine well-established ozonesonde sites. Additionally, ATom captured the most frequent ozone concentrations measured by regular commercial aircraft flights in the northern Atlantic UTLS. We then use the repeated vertical profiles from these two campaigns to confirm and extend the existing knowledge of tropospheric ozone spatial and vertical distributions throughout the remote troposphere. We highlight a clear hemispheric gradient, with greater ozone in the Northern Hemisphere, consistent with greater precursor emissions and consistent with previous modeling and satellite studies. We also show that the ozone distribution below 8 km was similar in the extra-tropics of the Atlantic and Pacific basins, likely due to zonal circulation patterns. However, twice as much ozone was found in the tropical Atlantic as in the tropical Pacific, due to well-documented dynamical patterns transporting continental air masses over the Atlantic. Finally, we show that the seasonal variability of tropospheric ozone over the Pacific and the Atlantic basins is driven year-round by transported continental plumes and photochemistry, and the vertical distribution is driven by photochemistry and mixing with stratospheric air. This new dataset provides additional constraints for global climate and chemistry models to improve our understanding of both ozone production and loss processes in remote regions, as well as the influence of anthropogenic emissions on baseline ozone.

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Global-scale distribution of ozone in the remote troposphere from ATom and HIPPO airborne field missions

10.5194/acp-2020-315 ◽

2020 ◽

Author(s):

Ilann Bourgeois ◽

Jeffrey Peischl ◽

Chelsea R. Thompson ◽

Kenneth C. Aikin ◽

Teresa Campos ◽

...

Keyword(s):

Tropospheric Ozone ◽

Large Scale ◽

Marine Boundary Layer ◽

Global Scale ◽

Ozone Production ◽

Commercial Aircraft ◽

Air Masses ◽

The Pacific ◽

Vertical Distributions ◽

Remote Troposphere

Abstract. Ozone is a key constituent of the troposphere where it drives photochemical processes, impacts air quality, and acts as a climate forcer. Large-scale in situ observations of ozone commensurate with the grid resolution of current Earth system models are necessary to validate model outputs and satellite retrievals. In this paper, we examine measurements from the Atmospheric Tomography (ATom, 4 deployments in 2016–2018) and the HIAPER Pole-to-Pole Observations (HIPPO; 5 deployments in 2009–2011) experiments, two global-scale airborne campaigns covering the Pacific (HIPPO and ATom) and Atlantic (ATom) basins. ATom and HIPPO represent the first global-scale, vertically resolved measurements of O3 distributions throughout the troposphere, with HIPPO sampling the Pacific basin and ATom sampling both the Pacific and Atlantic basins. Given the relatively limited temporal resolution of these two campaigns, we first compare ATom and HIPPO ozone data to longer-term observational records to establish the representativeness of our dataset. We show that these two airborne campaigns captured on average 53, 54, and 38 % of the ozone variability in the marine boundary layer, free troposphere, and upper troposphere/lower stratosphere (UTLS), respectively, at nine well-established ozonesonde sites. Additionally, ATom captured the most frequent ozone concentrations measured by regular commercial aircraft flights in the northern Atlantic UTLS. We then use the repeated vertical profiles carried out during these two campaigns to provide a global-scale picture of tropospheric ozone spatial and vertical distributions throughout the remote troposphere. We highlight a clear hemispheric gradient, with greater ozone in the northern hemisphere consistent with greater precursor emissions. We also show that the ozone distribution below 8 km was similar in the extra-tropics of the Atlantic and Pacific basins due to zonal circulation patterns. However, twice as much ozone was found in the tropical Atlantic than in the tropical Pacific, due to well-documented dynamical patterns transporting continental air masses over the Atlantic. We finally show that the seasonal variability of tropospheric ozone over the Pacific and the Atlantic basins is driven by transported continental plumes and photochemistry, and the vertical distribution is driven by photochemistry and mixing with stratospheric air. This new dataset is essential for improving our understanding of both ozone production and loss processes in remote regions, as well as the influence of anthropogenic emissions on baseline ozone.

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Large contribution to secondary organic aerosol from isoprene cloud chemistry

Science Advances ◽

10.1126/sciadv.abe2952 ◽

2021 ◽

Vol 7 (13) ◽

pp. eabe2952

Author(s):

Houssni Lamkaddam ◽

Josef Dommen ◽

Ananth Ranjithkumar ◽

Hamish Gordon ◽

Günther Wehrle ◽

...

Keyword(s):

Radiative Forcing ◽

Flow Reactor ◽

Secondary Organic Aerosol ◽

Cloud Droplet ◽

Organic Aerosol ◽

Global Scale ◽

Oxidation Products ◽

Oh Radicals ◽

Large Contribution ◽

Cloud Processing

Aerosols still present the largest uncertainty in estimating anthropogenic radiative forcing. Cloud processing is potentially important for secondary organic aerosol (SOA) formation, a major aerosol component: however, laboratory experiments fail to mimic this process under atmospherically relevant conditions. We developed a wetted-wall flow reactor to simulate aqueous-phase processing of isoprene oxidation products (iOP) in cloud droplets. We find that 50 to 70% (in moles) of iOP partition into the aqueous cloud phase, where they rapidly react with OH radicals, producing SOA with a molar yield of 0.45 after cloud droplet evaporation. Integrating our experimental results into a global model, we show that clouds effectively boost the amount of SOA. We conclude that, on a global scale, cloud processing of iOP produces 6.9 Tg of SOA per year or approximately 20% of the total biogenic SOA burden and is the main source of SOA in the mid-troposphere (4 to 6 km).

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Analysis of the latitudinal variability of tropospheric ozone in the Arctic using the large number of aircraft and ozonesonde observations in early summer 2008

10.5194/acp-2016-422 ◽

2016 ◽

Author(s):

Gerard Ancellet ◽

Nikos Daskalakis ◽

Jean Christophe Raut ◽

Boris Quennehen ◽

François Ravetta ◽

...

Keyword(s):

Biomass Burning ◽

Tropospheric Ozone ◽

Lower Troposphere ◽

Early Summer ◽

Ozone Production ◽

The Arctic ◽

Integrated Analysis ◽

International Polar Year ◽

Latitude Range ◽

Vertical Variability

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).

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Forecasting carbon monoxide on a global scale for the ATom-1 aircraft mission: insights from airborne and satellite observations and modeling

Atmospheric Chemistry and Physics ◽

10.5194/acp-18-10955-2018 ◽

2018 ◽

Vol 18 (15) ◽

pp. 10955-10971 ◽

Cited By ~ 1

Author(s):

Sarah A. Strode ◽

Junhua Liu ◽

Leslie Lait ◽

Róisín Commane ◽

Bruce Daube ◽

...

Keyword(s):

Biomass Burning ◽

Optical Thickness ◽

Chemical Reactivity ◽

Model Performance ◽

Global Scale ◽

Satellite Observations ◽

Aerosol Optical Thickness ◽

Boreal Summer ◽

Large Contribution ◽

Moderate Resolution Imaging Spectroradiometer

Abstract. The first phase of the Atmospheric Tomography Mission (ATom-1) took place in July–August 2016 and included flights above the remote Pacific and Atlantic oceans. Sampling of atmospheric constituents during these flights is designed to provide new insights into the chemical reactivity and processes of the remote atmosphere and how these processes are affected by anthropogenic emissions. Model simulations provide a valuable tool for interpreting these measurements and understanding the origin of the observed trace gases and aerosols, so it is important to quantify model performance. Goddard Earth Observing System Model version 5 (GEOS-5) forecasts and analyses show considerable skill in predicting and simulating the CO distribution and the timing of CO enhancements observed during the ATom-1 aircraft mission. We use GEOS-5's tagged tracers for CO to assess the contribution of different emission sources to the regions sampled by ATom-1 to elucidate the dominant anthropogenic influences on different parts of the remote atmosphere. We find a dominant contribution from non-biomass-burning sources along the ATom transects except over the tropical Atlantic, where African biomass burning makes a large contribution to the CO concentration. One of the goals of ATom is to provide a chemical climatology over the oceans, so it is important to consider whether August 2016 was representative of typical boreal summer conditions. Using satellite observations of 700 hPa and column CO from the Measurement of Pollution in the Troposphere (MOPITT) instrument, 215 hPa CO from the Microwave Limb Sounder (MLS), and aerosol optical thickness from the Moderate Resolution Imaging Spectroradiometer (MODIS), we find that CO concentrations and aerosol optical thickness in August 2016 were within the observed range of the satellite observations but below the decadal median for many of the regions sampled. This suggests that the ATom-1 measurements may represent relatively clean but not exceptional conditions for lower-tropospheric CO.

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Characterising the seasonal and geographical variability in tropospheric ozone, stratospheric influence and recent changes

Atmospheric Chemistry and Physics ◽

10.5194/acp-19-3589-2019 ◽

2019 ◽

Vol 19 (6) ◽

pp. 3589-3620 ◽

Cited By ~ 9

Author(s):

Ryan S. Williams ◽

Michaela I. Hegglin ◽

Brian J. Kerridge ◽

Patrick Jöckel ◽

Barry G. Latter ◽

...

Keyword(s):

Atmospheric Chemistry ◽

Tropospheric Ozone ◽

Radiative Forcing ◽

Lower Stratosphere ◽

Climate Model ◽

Stratospheric Ozone ◽

Data Availability ◽

Ozone Production ◽

Upper Troposphere ◽

The World

Abstract. The stratospheric contribution to tropospheric ozone (O3) has been a subject of much debate in recent decades but is known to have an important influence. Recent improvements in diagnostic and modelling tools provide new evidence that the stratosphere has a much larger influence than previously thought. This study aims to characterise the seasonal and geographical distribution of tropospheric ozone, its variability, and its changes and provide quantification of the stratospheric influence on these measures. To this end, we evaluate hindcast specified-dynamics chemistry–climate model (CCM) simulations from the European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) model and the Canadian Middle Atmosphere Model (CMAM), as contributed to the International Global Atmospheric Chemistry – Stratosphere-troposphere Processes And their Role in Climate (IGAC-SPARC) (IGAC–SPARC) Chemistry Climate Model Initiative (CCMI) activity, together with satellite observations from the Ozone Monitoring Instrument (OMI) and ozone-sonde profile measurements from the World Ozone and Ultraviolet Radiation Data Centre (WOUDC) over a period of concurrent data availability (2005–2010). An overall positive, seasonally dependent bias in 1000–450 hPa (∼0–5.5 km) sub-column ozone is found for EMAC, ranging from 2 to 8 Dobson units (DU), whereas CMAM is found to be in closer agreement with the observations, although with substantial seasonal and regional variation in the sign and magnitude of the bias (∼±4 DU). Although the application of OMI averaging kernels (AKs) improves agreement with model estimates from both EMAC and CMAM as expected, comparisons with ozone-sondes indicate a positive ozone bias in the lower stratosphere in CMAM, together with a negative bias in the troposphere resulting from a likely underestimation of photochemical ozone production. This has ramifications for diagnosing the level of model–measurement agreement. Model variability is found to be more similar in magnitude to that implied from ozone-sondes in comparison with OMI, which has significantly larger variability. Noting the overall consistency of the CCMs, the influence of the model chemistry schemes and internal dynamics is discussed in relation to the inter-model differences found. In particular, it is inferred that CMAM simulates a faster and shallower Brewer–Dobson circulation (BDC) compared to both EMAC and observational estimates, which has implications for the distribution and magnitude of the downward flux of stratospheric ozone over the most recent climatological period (1980–2010). Nonetheless, it is shown that the stratospheric influence on tropospheric ozone is significant and is estimated to exceed 50 % in the wintertime extratropics, even in the lower troposphere. Finally, long-term changes in the CCM ozone tracers are calculated for different seasons. An overall statistically significant increase in tropospheric ozone is found across much of the world but particularly in the Northern Hemisphere and in the middle to upper troposphere, where the increase is on the order of 4–6 ppbv (5 %–10 %) between 1980–1989 and 2001–2010. Our model study implies that attribution from stratosphere–troposphere exchange (STE) to such ozone changes ranges from 25 % to 30 % at the surface to as much as 50 %–80 % in the upper troposphere–lower stratosphere (UTLS) across some regions of the world, including western Eurasia, eastern North America, the South Pacific and the southern Indian Ocean. These findings highlight the importance of a well-resolved stratosphere in simulations of tropospheric ozone and its implications for the radiative forcing, air quality and oxidation capacity of the troposphere.

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General overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) – integrating aerosol research from nano to global scales

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-11-17941-2011 ◽

2011 ◽

Vol 11 (6) ◽

pp. 17941-18160 ◽

Cited By ~ 4

Author(s):

M. Kulmala ◽

A. Asmi ◽

H. K. Lappalainen ◽

U. Baltensperger ◽

J.-L. Brenguier ◽

...

Keyword(s):

Air Quality ◽

Radiative Forcing ◽

Climate Models ◽

Global Climate ◽

Global Scale ◽

Global Climate Models ◽

Modeling Tools ◽

Emissions Inventory ◽

Airborne Measurements ◽

Aerosol Cloud

Abstract. In this paper we describe and summarize the main achievements of the European Aerosol Cloud Climate and Air Quality Interactions project (EUCAARI). EUCAARI started on 1 January 2007 and ended on 31 December 2010 leaving a rich legacy including: (a) a comprehensive database with a year of observations of the physical, chemical and optical properties of aerosol particles over Europe, (b) the first comprehensive aerosol measurements in four developing countries, (c) a database of airborne measurements of aerosols and clouds over Europe during May 2008, (d) comprehensive modeling tools to study aerosol processes fron nano to global scale and their effects on climate and air quality. In addition a new Pan-European aerosol emissions inventory was developed and evaluated, a new cluster spectrometer was built and tested in the field and several new aerosol parameterizations and computations modules for chemical transport and global climate models were developed and evaluated. This work enabled EUCAARI to improve our understanding of aerosol radiative forcing and air quality-climate interactions. The EUCAARI results can be utilized in European and global environmental policy to assess the aerosol impacts and the corresponding abatement strategies.

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Biomass burning influence on high latitude tropospheric ozone and reactive nitrogen in summer 2008: a multi-model analysis based on POLMIP simulations

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-14-24573-2014 ◽

2014 ◽

Vol 14 (17) ◽

pp. 24573-24621 ◽

Cited By ~ 9

Author(s):

S. R. Arnold ◽

L. K. Emmons ◽

S. A. Monks ◽

K. S. Law ◽

D. A. Ridley ◽

...

Keyword(s):

Biomass Burning ◽

High Latitude ◽

Tropospheric Ozone ◽

Transport Model ◽

Chemical Transport ◽

Ozone Production ◽

The Arctic ◽

Vertical Position ◽

Chemical Transport Model ◽

Fire Emissions

Abstract. We have evaluated tropospheric ozone enhancement in air dominated by biomass burning emissions at high laititudes (> 50˚ N) in July 2008, using 10 global chemical transport model simulations from the POLMIP multi-model comparison exercise. In model air masses dominated by fire emissions, Δ O3/ΔCO values ranged between 0.039 and 0.196 ppbv ppbv−1 (mean: 0.113 ppbv ppbv−1) in freshly fire-influenced air, and between 0.140 and 0.261 ppbv ppbv−1 (mean: 0.193 ppbv) in more aged fire-influenced air. These values are in broad agreement with the range of observational estimates from the literature. Model ΔPAN/ΔCO enhancement ratios show distinct groupings according to the meteorological data used to drive the models. ECMWF-forced models produce larger ΔPAN/ΔCO values (4.44–6.28 pptv ppbv−1) than GEOS5-forced models (2.02–3.02 pptv ppbv−1), which we show is likely linked to differences efficiency of vertical transport during poleward export from mid-latitude source regions. Simulations of a large plume of biomass burning and anthropogenic emissions exported from Asia towards the Arctic using a Lagrangian chemical transport model show that 4 day net ozone change in the plume is sensitive to differences in plume chemical composition and plume vertical position among the POLMIP models. In particular, Arctic ozone evolution in the plume is highly sensitive to initial concentrations of PAN, as well as oxygenated VOCs (acetone, acetaldehyde), due to their role in producing the peroxyacetyl radical PAN precursor. Vertical displacement is also important due to its effects on the stability of PAN, and subsequent effect on NOx abundance. In plumes where net ozone production is limited, we find that the lifetime of ozone in the plume is sensitive to hydrogen peroxide loading, due to the production of HO2 from peroxide photolysis, and the key role of HO2 + O3 in controlling ozone loss. Overall, our results suggest that emissions from biomass burning lead to large-scale photochemical enhancement in high latitude tropospheric ozone during summer.

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Shortwave radiative forcing and efficiency of key aerosol types using AERONET data

Atmospheric Chemistry and Physics ◽

10.5194/acp-12-5129-2012 ◽

2012 ◽

Vol 12 (11) ◽

pp. 5129-5145 ◽

Cited By ~ 92

Author(s):

O. E. García ◽

J. P. Díaz ◽

F. J. Expósito ◽

A. M. Díaz ◽

O. Dubovik ◽

...

Keyword(s):

Biomass Burning ◽

Atmospheric Aerosols ◽

Radiative Forcing ◽

Mineral Dust ◽

High Surface ◽

Global Scale ◽

Free Troposphere ◽

Anthropogenic Aerosols ◽

Radiative Balance ◽

Absorbing Aerosols

Abstract. The shortwave radiative forcing (ΔF) and the radiative forcing efficiency (ΔFeff) of natural and anthropogenic aerosols have been analyzed using estimates of radiation both at the Top (TOA) and at the Bottom Of Atmosphere (BOA) modeled based on AERONET aerosol retrievals. Six main types of atmospheric aerosols have been compared (desert mineral dust, biomass burning, urban-industrial, continental background, oceanic and free troposphere) in similar observational conditions (i.e., for solar zenith angles between 55° and 65°) in order to compare the nearly same solar geometry. The instantaneous ΔF averages obtained vary from −122 ± 37 Wm−2 (aerosol optical depth, AOD, at 0.55 μm, 0.85 ± 0.45) at the BOA for the mixture of desert mineral dust and biomass burning aerosols in West Africa and −42 ± 22 Wm−2 (AOD = 0.9 ± 0.5) at the TOA for the pure mineral dust also in this region up to −6 ± 3 Wm−2 and −4 ± 2 Wm−2 (AOD = 0.03 ± 0.02) at the BOA and the TOA, respectively, for free troposphere conditions. This last result may be taken as reference on a global scale. Furthermore, we observe that the more absorbing aerosols are overall more efficient at the BOA in contrast to at the TOA, where they backscatter less solar energy into the space. The analysis of the radiative balance at the TOA shows that, together with the amount of aerosols and their absorptive capacity, it is essential to consider the surface albedo of the region on which they are. Thus, we document that in regions with high surface reflectivity (deserts and snow conditions) atmospheric aerosols lead to a warming of the Earth-atmosphere system.

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Tropospheric ozone production related to West African city emissions during the 2006 wet season AMMA campaign

Atmospheric Chemistry and Physics ◽

10.5194/acp-11-6349-2011 ◽

2011 ◽

Vol 11 (13) ◽

pp. 6349-6366 ◽

Cited By ~ 5

Author(s):

G. Ancellet ◽

E. Orlandi ◽

E. Real ◽

K. S. Law ◽

H. Schlager ◽

...

Keyword(s):

Tropospheric Ozone ◽

West African ◽

Ozone Production ◽

Lagrangian Model ◽

Air Mass ◽

Airborne Measurements ◽

African Cities ◽

High Level ◽

Sahel Region ◽

The City

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.

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