ALBERT

Description: This paper reports the first record of extreme ozone measurement in Africa. As part of the AMMA program, the ozone vertical profile recorded on 20 December over Cotonou presents exceptionally high ozone concentrations with up to 295 ppbv at 1 km altitude. Retroplumes from the Flexpart model show that the air masses sampled at 1 km over Cotonou on this day come from the burning area situated north-east of Cotonou and pass over Lagos, Nigeria, which is highly impacted by urban pollution. We used the Master Mechanism box model to simulate the chemical composition of the plume during its transit. We find that neither the biomass burning emissions of ozone precursors nor additional urban emissions from Lagos are high enough to simulate more than 120–150 ppbv of ozone. The only way to reach almost 300 ppb of ozone within a few hours is to feed the air mass with large amounts of reactive VOCs as those recorded in the vicinity of petrochemical area. Sensitivity tests show that 250–600 ppbv of VOCs combined with 35–80 ppb of NOx allow the ozone concentrations to be higher than 250 ppb. Nigeria is the first African country with gas extraction and petrochemical industries, and petrochemical explosions frequently happen in the vicinity of Lagos. The hypothesis of a petrochemical explosion in this area is the most likely scenario which explains the 295 ppbv ozone maximum measured over Cotonou, downwind of Lagos.

Description: An ozone climatology based on ozone soundings for the last 15 years has been constructed for model evaluation and comparisons to other observations. Vertical ozone profiles for 41 stations around the globe have been compiled and averaged for the years 1980–1994 and 1995–2009. The climatology provides information about the median and the width of the ozone probability distribution function, as well as interannual variability of ozone between 1995 and 2009, in pressure and tropopause-referenced altitudes. In addition to single stations, regional aggregates are presented, combining stations with similar ozone characteristics. The Hellinger distance is introduced as a new diagnostic to compare the variability of ozone distributions within each region and used for model evaluation purposes. This measure compares not only the mean, but also the shape of distributions. The representativeness of regional aggregates is discussed using independent observations from surface stations and MOZAIC aircraft data. Ozone from all of these data sets show an excellent agreement within the range of the interannual variability, especially if a sufficient number of measurements are available, as is the case for West Europe. Within the climatology, a significant longitudinal variability of ozone in the troposphere and lower stratosphere in the northern mid- and high latitudes is found. The climatology is used to evaluate results from two model intercomparison activities, HTAP for the troposphere and CCMVal2 for the tropopause region and the stratosphere. HTAP ozone is in good agreement with observations in the troposphere within their range of uncertainty, but ozone peaks too early in the Northern Hemisphere spring. The strong gradients of ozone around the tropopause are less well captured by many models. Lower stratospheric ozone is overestimated for all regions by the multi-model mean of CCMVal2 models. Individual models also show major shortcomings in reproducing the shape of ozone probability distribution functions in various regions and different altitudes, which might have significant implications for the radiative budgets in those models.

Description: Biomass burning (BB) in southern Africa is the largest emission source of CO and O3 precursors within Africa during the West African Monsoon (WAM) between June and August. The long range transport and chemical processing of such emissions thus has the potential to exert a dominant influence on the composition of the tropical troposphere over Equatorial Africa (EA) and the Tropical Atlantic Ocean (TAO). We have performed simulations using a three-dimensional global chemistry-transport model (CTM) to quantify the effect that continental transport of such BB plumes has on the EA region. BB emissions from southern Africa were found to exert a significant influence over the TAO and EA between 10° S–20° N. The maximum concentrations in CO and O3 occur between 0–5° S near the position of the African Easterly Jet – South as placed by the European Centre for Medium range Weather Forecasts (ECMWF) meteorological analysis data. By comparing co-located model output with in-situ measurements we show that the CTM fails to capture the tropospheric profile of CO in southern Africa near the main source region of the BB emissions, as well as the "extreme" concentrations of both CO and O3 seen between 600–700 hPa over EA around 6° N. For more northerly locations the model exhibits high background concentrations in both CO and O3 related to BB emissions from southern Africa. By altering both the temporal resolution and the vertical distribution of BB emissions in the model we show that changes in temporal resolution have the largest influence on the transport of trace gases near the source regions, EA, and in the outflow towards the west of Central Africa. Using a set of trajectory calculations we show that the performance of the CTM is heavily constrained by the ECMWF meteorological fields used to drive the CTM, which transport biomass burning plumes from southern Africa into the lower troposphere of the TAO rather than up towards the middle troposphere at 650 hPa. Similar trajectory simulations repeated using an updated meteorological dataset, which assimilates additional measurement data taken around EA, show markedly different origins for pollution events and highlight the current limitations in modelling this tropical region.

Description: In this paper, we analyze tropospheric O3 together with HNO3 during the POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols, and Transport) program, combining observations and model results. Aircraft observations from the NASA ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) and NOAA ARCPAC (Aerosol, Radiation and Cloud Processes affecting Arctic Climate) campaigns during spring and summer of 2008 are used together with the Model for Ozone and Related Chemical Tracers, version 4 (MOZART-4) to assist in the interpretation of the observations in terms of the source attribution and transport of O3 and HNO3 into the Arctic (north of 60° N). The MOZART-4 simulations reproduce the aircraft observations generally well (within 15%), but some discrepancies in the model are identified and discussed. The observed correlation of O3 with HNO3 is exploited to evaluate the MOZART-4 model performance for different air mass types (fresh plumes, free troposphere and stratospheric-contaminated air masses). Based on model simulations of O3 and HNO3 tagged by source type and region, we find that the anthropogenic pollution from the Northern Hemisphere is the dominant source of O3 and HNO3 in the Arctic at pressures greater than 400 hPa, and that the stratospheric influence is the principal contribution at pressures less 400 hPa. During the summer, intense Russian fire emissions contribute some amount to the tropospheric columns of both gases over the American sector of the Arctic. North American fire emissions (California and Canada) also show an important impact on tropospheric ozone in the Arctic boundary layer. Additional analysis of tropospheric O3 measurements from ground-based FTIR and from the IASI satellite sounder made at the Eureka (Canada) and Thule (Greenland) polar sites during POLARCAT has been performed using the tagged contributions. It demonstrates the capability of these instruments for observing pollution at northern high latitudes. Differences between contributions from the sources to the tropospheric columns as measured by FTIR and IASI are discussed in terms of vertical sensitivity associated with these instruments. The first analysis of O3 tropospheric columns observed by the IASI satellite instrument over the Arctic is also provided. Despite its limited vertical sensitivity in the lowermost atmospheric layers, we demonstrate that IASI is capable of detecting low-altitude pollution transported into the Arctic with some limitations.

Description: For the first time, carbon monoxide (CO) and formaldehyde (HCHO) satellite retrievals are used together with methane (CH4) and methyl choloroform (CH3CCl3 or MCF) surface measurements in an advanced inversion system. The CO and HCHO are respectively from the MOPITT and OMI instruments. The multi-species and multi-satellite dataset inversion is done for the 2005–2010 period. The robustness of our results is evaluated by comparing our posterior-modeled concentrations with several sets of independent measurements of atmospheric mixing ratios. The inversion leads to significant changes from the prior to the posterior, in terms of magnitude and seasonality of the CO and CH4 surface fluxes and of the HCHO production by non-methane volatile organic compounds (NMVOC). The latter is significantly decreased, indicating an overestimation of the biogenic NMVOC emissions, such as isoprene, in the GEIA inventory. CO and CH4 surface emissions are increased by the inversion, from 1037 to 1394 TgCO and from 489 to 529 TgCH4 on average for the 2005–2010 period. CH4 emissions present significant interannual variability and a joint CO-CH4 fluxes analysis reveals that tropical biomass burning probably played a role in the recent increase of atmospheric methane.

Description: A modelling experiment has been conceived to assess the impact of transport model errors on methane emissions estimated in an atmospheric inversion system. Synthetic methane observations, obtained from 10 different model outputs from the international TransCom-CH4 model inter-comparison exercise, are combined with a prior scenario of methane emissions and sinks, and integrated into the three-component PYVAR-LMDZ-SACS (PYthon VARiational-Laboratoire de Météorologie Dynamique model with Zooming capability-Simplified Atmospheric Chemistry System) inversion system to produce 10 different methane emission estimates at the global scale for the year 2005. The same methane sinks, emissions and initial conditions have been applied to produce the 10 synthetic observation datasets. The same inversion set-up (statistical errors, prior emissions, inverse procedure) is then applied to derive flux estimates by inverse modelling. Consequently, only differences in the modelling of atmospheric transport may cause differences in the estimated fluxes. In our framework, we show that transport model errors lead to a discrepancy of 27 Tg yr−1 at the global scale, representing 5% of total methane emissions. At continental and annual scales, transport model errors are proportionally larger than at the global scale, with errors ranging from 36 Tg yr−1 in North America to 7 Tg yr−1 in Boreal Eurasia (from 23 to 48%, respectively). At the model grid-scale, the spread of inverse estimates can reach 150% of the prior flux. Therefore, transport model errors contribute significantly to overall uncertainties in emission estimates by inverse modelling, especially when small spatial scales are examined. Sensitivity tests have been carried out to estimate the impact of the measurement network and the advantage of higher horizontal resolution in transport models. The large differences found between methane flux estimates inferred in these different configurations highly question the consistency of transport model errors in current inverse systems. Future inversions should include more accurately prescribed observation covariances matrices in order to limit the impact of transport model errors on estimated methane fluxes.

Description: The Lagrangian particle dispersion model FLEXPART coupled with daily active fire products provided by the MODIS instrument was used to forecast the intrusions of the southern hemispheric fire plumes in the Northern Hemisphere during the AMMA (African Monsoon Multidisciplinary Analysis) fourth airborne campaign from 25 July to 31 August 2006 (Special Operation Period SOP2_a2). The imprint of the biomass burning plumes over the Gulf of Guinea showed a well marked intraseasonal variability which is controlled by the position and strength of the southern hemispheric African Easterly Jet (AEJ-S). Three different periods were identified which correspond to active and break phases of the AEJ-S: 25 July–2 August (active phase), 3 August–8 August (break phase) and 9 August–31 August (active phase). During the AEJ-S active phases, the advection of the biomass burning plumes out over the Atlantic ocean was efficient in the mid-troposphere. During the AEJ-S break phases, pollutants emitted by fires were trapped over the continent where they accumulated. The continental circulation increased the possibility for the biomass burning plumes to reach the convective regions located further north. As a consequence, biomass burning plumes were found in the upper troposphere over the Gulf of Guinea during the AEJ-S break phase. Observational evidences from the ozonesounding network at Cotonou and the carbon monoxide measured by MOPITT confirmed the alternation of the AEJ-S phases with low ozone and CO in the mid-troposphere over the Gulf of Guinea during the break phase.

Description: As part of the African Monsoon Multidisciplinary Analysis (AMMA) program, a total of 98 ozone vertical profiles over Cotonou, Benin, have been measured during a 26 month period (December 2004–January 2007). These regular measurements broadly document the seasonal and interannual variability of ozone in both the troposphere and the lower stratosphere over West Africa for the first time. This data set is complementary to the MOZAIC observations made from Lagos between 0 and 12 km during the period 1998–2004. Both data sets highlight the unique way in which West Africa is impacted by two biomass burning seasons: in December–February (dry season) due to burning in the Sahelian band and in June-August (wet season) due to burning in southern Africa. High interannual variabilities between Cotonou and Lagos data sets and within each data set are observed and are found to be a major characteristic of this region. In particular, the dry and wet seasons are discussed in order to set the data of the Special Observing Periods (SOPs) into a climatological context. Compared to other dry and wet seasons, the 2006 dry and wet season campaigns took place in rather high ozone environments. During the sampled wet seasons, southern intrusions of biomass burning were particularly frequent with concentrations up to 120 ppbv of ozone in the lower troposphere. An insight into the ozone distribution in the upper troposphere and the lower stratosphere (up to 26 km) is given. The first tropospheric columns of ozone based on in-situ data over West Africa are assessed. They compare well with satellite products on seasonal and interannual time-scales, provided that the layer below 850 hPa where the remote instrument is less sensitive to ozone, is removed.

Description: Measurements of ozone vertical profiles are valuable for the evaluation of atmospheric chemistry models and contribute to the understanding of the processes controlling the distribution of tropospheric ozone. The longest record of ozone vertical profiles is provided by ozone sondes, which have a typical frequency of 4 to 12 profiles a month. Here we quantify the uncertainty introduced by low frequency sampling in the determination of means and trends. To do this, the high frequency MOZAIC (Measurements of OZone, water vapor, carbon monoxide and nitrogen oxides by in-service AIrbus airCraft) profiles over airports, such as Frankfurt, have been subsampled at two typical ozone sonde frequencies of 4 and 12 profiles per month. We found the lowest sampling uncertainty on seasonal means at 700 hPa over Frankfurt, with around 5% for a frequency of 12 profiles per month and 10% for a 4 profile-a-month frequency. However the uncertainty can reach up to 15 and 29% at the lowest altitude levels. As a consequence, the sampling uncertainty at the lowest frequency could be higher than the typical 10% accuracy of the ozone sondes and should be carefully considered for observation comparison and model evaluation. We found that the 95% confidence limit on the seasonal mean derived from the subsample created is similar to the sampling uncertainty and suggest to use it as an estimate of the sampling uncertainty. Similar results are found at six other Northern Hemisphere sites. We show that the sampling substantially impacts on the inter-annual variability and the trend derived over the period 1998–2008 both in magnitude and in sign throughout the troposphere. Also, a tropical case is discussed using the MOZAIC profiles taken over Windhoek, Namibia between 2005 and 2008. For this site, we found that the sampling uncertainty in the free troposphere is around 8 and 12% at 12 and 4 profiles a month respectively.