ALBERT

Description: 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.

Description: An eight-year long reanalysis of atmospheric composition data covering the period 2003–2010 was constructed as part of the FP7-funded Monitoring Atmospheric Composition and Climate project by assimilating satellite data into a global model and data assimilation system. This reanalysis provides fields of chemically reactive gases, namely carbon monoxide, ozone, nitrogen oxides, and formaldehyde, as well as aerosols and greenhouse gases globally at a horizontal resolution of about 80 km for both the troposphere and the stratosphere. This paper describes the assimilation system for the reactive gases and presents validation results for the reactive gas analysis fields to document the data set and to give a first indication of its quality. Tropospheric CO values from the MACC reanalysis are on average 10–20% lower than routine observations from commercial aircrafts over airports through most of the troposphere, and have larger negative biases in the boundary layer at urban sites affected by air pollution, possibly due to an underestimation of CO or precursor emissions. Stratospheric ozone fields from the MACC reanalysis agree with ozonesondes and ACE-FTS data to within ±10% in most seasons and regions. In the troposphere the reanalysis shows biases of −5% to +10% with respect to ozonesondes and aircraft data in the extratropics, but has larger negative biases in the tropics. Area-averaged total column ozone agrees with ozone fields from a multi-sensor reanalysis data set to within a few percent. NO2 fields from the reanalysis show the right seasonality over polluted urban areas of the NH and over tropical biomass burning areas, but underestimate wintertime NO2 maxima over anthropogenic pollution regions and overestimate NO2 in northern and southern Africa during the tropical biomass burning seasons. Tropospheric HCHO is well simulated in the MACC reanalysis even though no satellite data are assimilated. It shows good agreement with independent SCIAMACHY retrievals over regions dominated by biogenic emissions with some anthropogenic input, such as the eastern US and China, and also over African regions influenced by biogenic sources and biomass burning.

Description: Carbon monoxide (CO) is a key atmospheric compound that can be remotely sensed by satellite on the global scale. Fifteen years of continuous observations are now available from the MOPITT/Terra mission (2000 to present). Another fifteen and more years of observations will be provided by the IASI/MetOp instrument series (2007–2023〉). In order to study long term variability and trends, a homogeneous record is required, which is not straightforward as the retrieved products are instrument and processing dependent. The present study aims at evaluating the consistency between the CO products derived from the MOPITT and IASI missions, both for total columns and vertical profiles, during a six year overlap period (2008–2013). The analysis is performed by first comparing the available 2013 versions of the retrieval algorithms, and second using a dedicated reprocessing of MOPITT CO profiles and columns based on the IASI a priori constraints. MOPITT v5T total columns are generally slightly higher over land (bias ranging from 0 to 13%) than IASI v20100815 data. When IASI and MOPITT data are retrieved with the same a priori constraints, correlation coefficients are slightly improved. Large discrepancies (total column bias over 15%) observed in the Northern Hemisphere during the winter months are reduced by a factor of 2 to 2.5. The detailed analysis of retrieved vertical profiles compared with collocated aircraft data from the MOZAIC-IAGOS network, illustrates the advantages and disadvantages of a constant vs. a variable a priori. On one hand, MOPITT agrees better with the aircraft profiles for observations with persisting high levels of CO throughout the year due to pollution or seasonal fire activity (because the climatology-based a priori is supposed to be closer to the real atmospheric state). On the other hand, IASI performs better when unexpected events leading to high levels of CO occur, due to the less constrained variance-covariance matrix.

Description: Despite the developments in the global modelling of chemistry and of the parameterization of the physical processes, carbon monoxide (CO) concentrations remain underestimated during Northern Hemisphere (NH) winter by most state-of-the-art chemistry transport models. The consequential model bias can in principle originate from either an underestimation of CO sources or an overestimation of its sinks. We address both the role of surface sources and sinks with a series of MOZART (Model for Ozone And Related Tracers) model sensitivity studies for the year 2008 and compare our results to observational data from ground-based stations, satellite observations, and vertical profiles from measurements on passenger aircraft. In our base case simulation using MACCity (Monitoring Atmospheric Composition and Climate project) anthropogenic emissions, the near-surface CO mixing ratios are underestimated in the Northern Hemisphere by more than 20 ppb from December to April, with the largest bias of up to 75 ppb over Europe in January. An increase in global biomass burning or biogenic emissions of CO or volatile organic compounds (VOCs) is not able to reduce the annual course of the model bias and yields concentrations over the Southern Hemisphere which are too high. Raising global annual anthropogenic emissions with a simple scaling factor results in overestimations of surface mixing ratios in most regions all year round. Instead, our results indicate that anthropogenic CO and, possibly, VOC emissions in the MACCity inventory are too low for the industrialized countries only during winter and spring. Reasonable agreement with observations can only be achieved if the CO emissions are adjusted seasonally with regionally varying scaling factors. A part of the model bias could also be eliminated by exchanging the original resistance-type dry deposition scheme with a parameterization for CO uptake by oxidation from soil bacteria and microbes, which reduces the boreal winter dry deposition fluxes. The best match to surface observations, satellite retrievals, and aircraft observations was achieved when the modified dry deposition scheme was combined with increased wintertime road traffic emissions over Europe and North America (factors up to 4.5 and 2, respectively). One reason for the apparent underestimation of emissions may be an exaggerated downward trend in the Representative Concentration Pathway (RCP) 8.5 scenario in these regions between 2000 and 2010, as this scenario was used to extrapolate the MACCity emissions from their base year 2000. This factor is potentially amplified by a lack of knowledge about the seasonality of emissions. A methane lifetime of 9.7 yr for our basic model and 9.8 yr for the optimized simulation agrees well with current estimates of global OH, but we cannot fully exclude a potential effect from errors in the geographical and seasonal distribution of OH concentrations on the modelled CO.

Description: The Model of Emissions of Gases and Aerosols from Nature (MEGANv2.1) together with the Modern-Era Retrospective Analysis for Research and Applications (MERRA) meteorological fields were used to create a global emission data set of biogenic volatile organic compounds (BVOC) available on a monthly basis for the time period of 1980–2010. This data set, developed under the Monitoring Atmospheric Composition and Climate project (MACC), is called MEGAN–MACC. The model estimated mean annual total BVOC emission of 760 Tg (C) yr−1 consisting of isoprene (70%), monoterpenes (11%), methanol (6%), acetone (3%), sesquiterpenes (2.5%) and other BVOC species each contributing less than 2%. Several sensitivity model runs were performed to study the impact of different model input and model settings on isoprene estimates and resulted in differences of up to ±17% of the reference isoprene total. A greater impact was observed for a sensitivity run applying parameterization of soil moisture deficit that led to a 50% reduction of isoprene emissions on a global scale, most significantly in specific regions of Africa, South America and Australia. MEGAN–MACC estimates are comparable to results of previous studies. More detailed comparison with other isoprene inventories indicated significant spatial and temporal differences between the data sets especially for Australia, Southeast Asia and South America. MEGAN–MACC estimates of isoprene, α-pinene and group of monoterpenes showed a reasonable agreement with surface flux measurements at sites located in tropical forests in the Amazon and Malaysia. The model was able to capture the seasonal variation of isoprene emissions in the Amazon forest.

Description: Within the African Monsoon Multidisciplinary Analysis (AMMA), we investigate the impact of nitrogen oxides produced by lightning (LiNOx) and convective transport during the West African Monsoon (WAM) upon the composition of the upper troposphere (UT) in the tropics. For this purpose, we have performed simulations with 4 state-of-the-art chemistry transport models involved within AMMA, namely MOCAGE, TM4, LMDz-INCA and p-TOMCAT. The model intercomparison is complemented with an evaluation of the simulations based on both spaceborne and airborne observations. The baseline simulations show important differences between the UT CO and O3 distributions simulated by each of the 4 models when compared to measurements of the African latitudinal transect from the MOZAIC program and to distributions measured by the Aura/MLS spaceborne sensor. We show that such model discrepancies can be explained by differences in the convective transport parameterizations and, more particularly, the altitude reached by convective updrafts (ranging between ~200–125 hPa). Concerning UT O3, the majority of models exhibit low concentrations compared to both MOZAIC and MLS observations south of the equator, with good agreement in the Northern Hemisphere. Sensitivity studies are performed to quantify the effect of deep convective transport and the influence of LiNOx production on the UT composition. These clearly indicate that the CO maxima and the elevated O3 concentrations south of the equator are due to convective uplift of air masses impacted by Southern African biomass burning, in agreement with previous studies. Moreover, during the WAM, LiNOx from Africa are responsible for the highest UT O3 enhancements (10–20 ppbv) over the tropical Atlantic between 10° S–20° N. Differences between models are primarily due to the performance of the parameterizations used to simulate lightning activity which are evaluated using spaceborne observations of flash frequency. Combined with comparisons of in-situ NO measurements we show that the models producing the highest amounts of LiNOx over Africa during the WAM (INCA and p-TOMCAT) capture observed NO profiles with the best accuracy, although they both overestimate lightning activity over the Sahel.

Description: An eight-year long reanalysis of atmospheric composition data covering the period 2003–2010 was constructed as part of the FP7 funded Monitoring Atmospheric Composition and Climate project by assimilating satellite data into a global model and data assimilation system. This reanalysis provides fields of chemically reactive gases, namely carbon monoxide, ozone, nitrogen oxides, and formaldehyde, as well as aerosols and greenhouse gases globally at a resolution of about 80 km for both the troposphere and the stratosphere. This paper describes the assimilation system for the reactive gases and presents validation results for the reactive gases analysis fields to document the dataset and to give a first indication of its quality. Tropospheric CO values from the MACC reanalysis are on average 10–20% lower than routine observations from commercial aircrafts over airports through most of the troposphere, and have larger negative biases in the boundary layer at urban sites affected by air pollution, possibly due to an underestimation of CO or precursor emissions. Stratospheric ozone fields from the MACC reanalysis agree with ozone sondes and ACE-FTS data to within ±10% in most situations. In the troposphere the reanalysis shows biases of −5% to +10% with respect to ozone sondes and aircraft data in the extratropics, but has larger negative biases in the tropics. Area averaged total column ozone agrees with ozone fields from a multi sensor reanalysis data set to within a few percent. NO2 fields from the reanalysis show the right seasonality over polluted urban areas of the NH and over tropical biomass burning areas, but underestimate wintertime NO2 maxima over anthropogenic pollution regions and overestimate NO2 in Northern and Southern Africa during the tropical biomass burning seasons. Tropospheric HCHO is well simulated in the MACC reanalysis even though no satellite data are assimilated. It shows good agreement with independent SCIAMACHY retrievals over regions dominated by biogenic emissions with some anthropogenic input, such as the Eastern US and China, and also over African regions influenced by biogenic sources and biomass burning.

Description: Arctic sea ice has decreased dramatically in the past few decades and the Arctic is increasingly open to transit shipping and natural resource extraction. However, large knowledge gaps exist regarding composition and impacts of emissions associated with these activities. Arctic hydrocarbon extraction is currently under development owing to the large oil and gas reserves in the region. Transit shipping through the Arctic as an alternative to the traditional shipping routes is currently underway. These activities are expected to increase emissions of air pollutants and climate forcers (e.g., aerosols, ozone) in the Arctic troposphere significantly in the future. The authors present the first measurements of these activities off the coast of Norway taken in summer 2012 as part of the European Arctic Climate Change, Economy, and Society (ACCESS) project. The objectives include quantifying the impact that anthropogenic activities will have on regional air pollution and understanding the connections to Arctic climate. Trace gas and aerosol concentrations in pollution plumes were measured, including emissions from different ship types and several offshore extraction facilities. Emissions originating from industrial activities (smelting) on the Kola Peninsula were also sampled. In addition, pollution plumes originating from Siberian biomass burning were probed in order to put the emerging local pollution within a broader context. In the near future these measurements will be combined with model simulations to quantify the influence of local anthropogenic activities on Arctic composition. Here the authors present the scientific objectives of the ACCESS aircraft experiment and the the meteorological conditions during the campaign, and they highlight first scientific results from the experiment.