Temporal and vertical variations of aerosol physical and chemical properties over West Africa: AMMA aircraft campaign in summer 2006

While the Sahelian belt in West Africa stretches in the border between the global hot-spots of mineral dust and biomass burning aerosols, the presence of West African Monsoon is expected to create significant vertical and temporal variations in the regional aerosol properties through transport and mixing of particles from various sources (mineral dust, biomass burning, sulfates, sea salt). In order to improve our understanding of the evolution of the aerosol-cloud system over such region across the onset of the summer monsoon, the French ATR-42 research aircraft was deployed in Niamey, Niger (13°30' N, 02°05' E) in summer 2006, during the three special observation periods (SOPs) of the African Monsoon Multidisciplinary Analysis (AMMA) project. These three SOPs covered both dry and wet periods before and after the onset of the Western African Monsoon. <br><br> State of the art physico-chemical aerosol measurements on the ATR-42 showed a notable seasonal transition in averaged number size distributions where (i) the Aitken mode is dominating over the accumulation mode during the dry season preceding the monsoon arrival and (ii) the accumulation mode increasingly gained importance after the onset of the West African monsoon and even dominated the Aitken mode after the monsoon had fully developed. The parameters for the mean log-normal distributions observed in respective layers characterized by the different wind regimes (monsoon layer, SAL, free troposphere) are presented, together with the major particle compositions found in the accumulation mode particles. Thereby, results of this study should facilitate radiative transfer calculations, validation of satellite remote sensors, and detailed transport modeling by partners within and outside the AMMA community. <br><br> Extended analysis of the chemical composition of single aerosol particles by a transmission electron microscope (TEM) coupled to an energy dispersive X-ray spectrometer (EDX) revealed dominance of mineral dust (aluminosilicate) even in the submicron particle size range during the dry period, gradually replaced by prevailing biomass burning and sulfate particles, after the onset of the monsoon period. The spatial and temporal evolution from SOP1 to SOP2a1 and SOP2a2 of the particle physical and chemical properties and associated aerosol hygroscopic properties are remarkably consistent

Airborne measurements of aerosol optical properties related to early spring transport of mid-latitude sources into the Arctic

Airborne lidar and in-situ measurements of the aerosol properties were conducted between Svalbard Island and Scandinavia in April 2008. Evidence of aerosol transport from Europe and Asia is given. The analysis of the aerosol optical properties based on a multiwavelength lidar (355, 532, 1064 nm) including volume depolarization at 355 nm aims at distinguishing the role of the different aerosol sources (Siberian wild fires, Eastern Asia and European anthropogenic emissions). Combining, first aircraft measurements, second FLEXPART simulations with a calculation of the PBL air fraction originating from the three different mid-latitude source regions, and third level-2 CALIPSO data products (i.e. backscatter coefficient 532 nm,volume depolarization and color ratio between 1064 and 532 nm in aerosol layers) along the transport pathways, appears a valuable approach to identify the role of the different aerosol sources even after a transport time larger than 4 days. Optical depth of the aerosol layers are always rather small (<4%) while transported over the Arctic and ratio of the total attenuated backscatter (i.e. including molecular contribution) provide more stable result than conventional aerosol backscatter ratio. Above Asia, CALIPSO data indicate more depolarization (up to 15%) and largest color ratio (>0.5) for the northeastern Asia emissions (i.e. an expected mixture of Asian pollution and dust), while low depolarization together with smaller and quasi constant color ratio (≈0.3) are observed for the Siberian biomass burning emissions. A similar difference is visible between two layers observed by the aircraft above Scandinavia. The analysis of the time evolution of the aerosol optical properties revealed by CALIPSO between Asia and Scandinavia shows a gradual decrease of the aerosol backscatter, depolarization ratio and color ratio which suggests the removal of the largest particles in the accumulation mode. A similar study conducted for a European plume has shown aerosol optical properties intermediate between the two Asian sources with color ratio never exceeding 0.4 and moderate depolarization ratio being always less than 8%, i.e. less aerosol from the accumulation mode

Multi-model evaluation of short-lived pollutant distributions over East Asia during summer 2008

The ability of seven state of the art chemistry-aerosol models to reproduce distributions of tropospheric ozone and its precursors, as well as aerosols over eastern Asia in summer 2008 is evaluated. The study focuses on the performance of models used to assess impacts of pollutants on climate and air quality as part of the EU ECLIPSE project. Models, run using the same ECLIPSE emissions, are compared over different spatial scales to in-situ surface, vertical profile and satellite data. Several rather clear biases are found between model results and observations including overestimation of ozone at rural locations downwind of the main emission regions in China as well as downwind over the Pacific. Several models produce too much ozone over polluted regions which is then transported downwind. Analysis points to different factors related to the ability of models to simulate VOC limited regimes over polluted regions and NOx limited regimes downwind. This may also be linked to biases compared to satellite NO2 indicating overestimation of NO2 over and to the north of the northern China Plain emission region. On the other hand, model NO2 is too low to the south and east of this region and over Korean/Japan. Overestimation of ozone is linked to systematic underestimation of CO particularly at rural sites and downwind of the main Chinese emission regions. This is likely to be due to enhanced destruction of CO by OH. Overestimation of Asian ozone and its transport downwind implies that radiative forcing from this source may be overestimated. Model-observation discrepancies over Beijing do not appear to be due to emission controls linked to the Olympic Games in summer 2008. With regard to aerosols, most models reproduce the satellite-derived AOD patterns over eastern China. Our study nevertheless reveals an overestimation of ECLIPSE model-mean surface BC and sulphate aerosols in urban China in summer 2008. The effect of the short-term emission mitigation in Beijing is too weak to explain the differences between the models. Our results rather point to an overestimation of SO2 emissions, in particular, close to the surface in Chinese urban areas. However, we also identify a clear underestimation of aerosol concentrations over northern India, suggesting that the rapid recent growth of emissions in India, as well as their spatial extension, is underestimated in emission inventories. Model deficiencies in the representation of pollution accumulation due to the Indian monsoon may also be playing a role. Comparison with vertical aerosol lidar measurements highlights a general underestimation of scattering aerosols in the boundary layer associated with overestimation in the free troposphere pointing to modeled aerosol lifetimes that are too long. This is likely linked to a too strong vertical transport and/or insufficient deposition efficiency during transport or export from the boundary layer, rather than chemical processing (in the case of sulphate aerosols). Underestimation of sulphate in the boundary layer implies potentially large errors in simulated aerosol-cloud interactions, via impacts on boundary-layer clouds. This evaluation has important implications for accurate assessment of air pollutants on regional air quality and global climate based on global model calculations. Ideally, models should be run at higher resolution over source regions to better simulate urban-rural pollutant gradients/chemical regimes, and also to better resolve pollutant processing and loss by wet deposition as well as vertical transport. Discrepancies in vertical distributions requires further quantification and improvement since this is a key factor in the determination of radiative forcing from short-lived pollutants

Evaluating the climate and air quality impacts of short-lived pollutants

This paper presents a summary of the work done within the European Union's Seventh Framework Programme project ECLIPSE (Evaluating the Climate and Air Quality Impacts of Short-Lived Pollutants). ECLIPSE had a unique systematic concept for designing a realistic and effective mitigation scenario for short-lived climate pollutants (SLCPs; methane, aerosols and ozone, and their precursor species) and quantifying its climate and air quality impacts, and this paper presents the results in the context of this overarching strategy. The first step in ECLIPSE was to create a new emission inventory based on current legislation (CLE) for the recent past and until 2050. Substantial progress compared to previous work was made by including previously unaccounted types of sources such as flaring of gas associated with oil production, and wick lamps. These emission data were used for present-day reference simulations with four advanced Earth system models (ESMs) and six chemistry transport models (CTMs). The model simulations were compared with a variety of ground-based and satellite observational data sets from Asia, Europe and the Arctic. It was found that the models still underestimate the measured seasonality of aerosols in the Arctic but to a lesser extent than in previous studies. Problems likely related to the emissions were identified for northern Russia and India, in particular. To estimate the climate impacts of SLCPs, ECLIPSE followed two paths of research: the first path calculated radiative forcing (RF) values for a large matrix of SLCP species emissions, for different seasons and regions independently. Based on these RF calculations, the Global Temperature change Potential metric for a time horizon of 20 years (GTP20) was calculated for each SLCP emission type. This climate metric was then used in an integrated assessment model to identify all emission mitigation measures with a beneficial air quality and short-term (20-year) climate impact. These measures together defined a SLCP mitigation (MIT) scenario. Compared to CLE, the MIT scenario would reduce global methane (CH4) and black carbon (BC) emissions by about 50 and 80 %, respectively. For CH4, measures on shale gas production, waste management and coal mines were most important. For non-CH4 SLCPs, elimination of high-emitting vehicles and wick lamps, as well as reducing emissions from gas flaring, coal and biomass stoves, agricultural waste, solvents and diesel engines were most important. These measures lead to large reductions in calculated surface concentrations of ozone and particulate matter. We estimate that in the EU, the loss of statistical life expectancy due to air pollution was 7.5 months in 2010, which will be reduced to 5.2 months by 2030 in the CLE scenario. The MIT scenario would reduce this value by another 0.9 to 4.3 months. Substantially larger reductions due to the mitigation are found for China (1.8 months) and India (11–12 months). The climate metrics cannot fully quantify the climate response. Therefore, a second research path was taken. Transient climate ensemble simulations with the four ESMs were run for the CLE and MIT scenarios, to determine the climate impacts of the mitigation. In these simulations, the CLE scenario resulted in a surface temperature increase of 0.70 ± 0.14 K between the years 2006 and 2050. For the decade 2041–2050, the warming was reduced by 0.22 ± 0.07 K in the MIT scenario, and this result was in almost exact agreement with the response calculated based on the emission metrics (reduced warming of 0.22 ± 0.09 K). The metrics calculations suggest that non-CH4 SLCPs contribute ~ 22 % to this response and CH4 78 %. This could not be fully confirmed by the transient simulations, which attributed about 90 % of the temperature response to CH4 reductions. Attribution of the observed temperature response to non-CH4 SLCP emission reductions and BC specifically is hampered in the transient simulations by small forcing and co-emitted species of the emission basket chosen. Nevertheless, an important conclusion is that our mitigation basket as a whole would lead to clear benefits for both air quality and climate. The climate response from BC reductions in our study is smaller than reported previously, possibly because our study is one of the first to use fully coupled climate models, where unforced variability and sea ice responses cause relatively strong temperature fluctuations that may counteract (and, thus, mask) the impacts of small emission reductions. The temperature responses to the mitigation were generally stronger over the continents than over the oceans, and with a warming reduction of 0.44 K (0.39–0.49) K the largest over the Arctic. Our calculations suggest particularly beneficial climate responses in southern Europe, where surface warming was reduced by about 0.3 K and precipitation rates were increased by about 15 (6–21) mm yr−1 (more than 4 % of total precipitation) from spring to autumn. Thus, the mitigation could help to alleviate expected future drought and water shortages in the Mediterranean area. We also report other important results of the ECLIPSE project

Current model capabilities for simulating black carbon and sulfate concentrations in the Arctic atmosphere: a multi-model evaluation using a comprehensive measurement data set

The concentrations of sulfate, black carbon (BC) and other aerosols in the Arctic are characterized by high values in late winter and spring (so-called Arctic Haze) and low values in summer. Models have long been struggling to capture this seasonality and especially the high concentrations associated with Arctic Haze. In this study, we evaluate sulfate and BC concentrations from eleven different models driven with the same emission inventory against a comprehensive pan-Arctic measurement data set over a time period of 2 years (2008–2009). The set of models consisted of one Lagrangian particle dispersion model, four chemistry transport models (CTMs), one atmospheric chemistry-weather forecast model and five chemistry climate models (CCMs), of which two were nudged to meteorological analyses and three were running freely. The measurement data set consisted of surface measurements of equivalent BC (eBC) from five stations (Alert, Barrow, Pallas, Tiksi and Zeppelin), elemental carbon (EC) from Station Nord and Alert and aircraft measurements of refractory BC (rBC) from six different campaigns. We find that the models generally captured the measured eBC or rBC and sulfate concentrations quite well, compared to previous comparisons. However, the aerosol seasonality at the surface is still too weak in most models. Concentrations of eBC and sulfate averaged over three surface sites are underestimated in winter/spring in all but one model (model means for January–March underestimated by 59 and 37 % for BC and sulfate, respectively), whereas concentrations in summer are overestimated in the model mean (by 88 and 44 % for July–September), but with overestimates as well as underestimates present in individual models. The most pronounced eBC underestimates, not included in the above multi-site average, are found for the station Tiksi in Siberia where the measured annual mean eBC concentration is 3 times higher than the average annual mean for all other stations. This suggests an underestimate of BC sources in Russia in the emission inventory used. Based on the campaign data, biomass burning was identified as another cause of the modeling problems. For sulfate, very large differences were found in the model ensemble, with an apparent anti-correlation between modeled surface concentrations and total atmospheric columns. There is a strong correlation between observed sulfate and eBC concentrations with consistent sulfate/eBC slopes found for all Arctic stations, indicating that the sources contributing to sulfate and BC are similar throughout the Arctic and that the aerosols are internally mixed and undergo similar removal. However, only three models reproduced this finding, whereas sulfate and BC are weakly correlated in the other models. Overall, no class of models (e.g., CTMs, CCMs) performed better than the others and differences are independent of model resolution

Source identification and airborne chemical characterisation of aerosol pollution from long-range transport over Greenland during POLARCAT summer campaign 2008

We deployed an aerosol mass spectrometer during the POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols, and Transport) summer campaign in Greenland in June/July 2008 on the research aircraft ATR-42. Online size resolved chemical composition data of submicron aerosol were collected up to 7.6 km altitude in the region 60 to 71� N and 40 to 60�W. Biomass burning (BB) and fossil fuel combustion (FF) plumes originating from North America, Asia, Siberia and Europe were sampled. Transport pathways of detected plumes included advection below 700 hPa, air mass uplifting in warm conveyor belts, and high altitude transport in the upper troposphere. By means of the Lagrangian particle dispersion model FLEXPART, trace gas analysis of O3 and CO, particle size distributions and aerosol chemical composition 48 pollution events were identified and classified into five chemically distinct categories. Aerosol from North American BB consisted of 22% particulate sulphate, while with increasing anthropogenic and Asian influence aerosol in Asian FF dominated plumes was composed of up to 37% sulphate category mean value. Overall, it was found that the organic matter fraction was larger (85 %) in pollution plumes than for background conditions (71 %). Despite different source regions and emission types the particle oxygen to carbon ratio of all plume classes was around 1 indicating low-volatility highly oxygenated aerosol. The volume size distribution of out-of-plume aerosol showed markedly smaller modes than all other distributions with two Aitken mode diameters of 24 and 43 nm and a geometric standard deviation �g of 1.12 and 1.22, respectively, while another very broad mode was found at 490 nm (�g =2.35). Nearly pure BB particles from North America exhibited an Aitken mode at 66 nm (�g =1.46) and an accumulation mode diameter of 392 nm (�g =1.76). An aerosol lifetime, including all processes from emission to detection, in the range between 7 and 11 days was derived for North American emissions

New insights into the atmospheric mercury cycling in central Antarctica and implications on a continental scale

Under the framework of the GMOS project (Global Mercury Observation System) atmospheric mercury monitoring has been implemented at Concordia Station on the high-altitude Antarctic plateau (75°06′ S, 123°20′ E, 3220 m above sea level). We report here the first year-round measurements of gaseous elemental mercury (Hg(0)) in the atmosphere and in snowpack interstitial air on the East Antarctic ice sheet. This unique data set shows evidence of an intense oxidation of atmospheric Hg(0) in summer (24-hour daylight) due to the high oxidative capacity of the Antarctic plateau atmosphere in this period of the year. Summertime Hg(0) concentrations exhibited a pronounced daily cycle in ambient air with maximal concentrations around midday. Photochemical reactions and chemical exchange at the air–snow interface were prominent, highlighting the role of the snowpack on the atmospheric mercury cycle. Our observations reveal a 20 to 30 % decrease of atmospheric Hg(0) concentrations from May to mid-August (winter, 24 h darkness). This phenomenon has not been reported elsewhere and possibly results from the dry deposition of Hg(0) onto the snowpack. We also reveal the occurrence of multi-day to weeklong atmospheric Hg(0) depletion events in summer, not associated with depletions of ozone, and likely due to a stagnation of air masses above the plateau triggering an accumulation of oxidants within the shallow boundary layer. Our observations suggest that the inland atmospheric reservoir is depleted in Hg(0) in summer. Due to katabatic winds flowing out from the Antarctic plateau down the steep vertical drops along the coast and according to observations at coastal Antarctic stations, the striking reactivity observed on the plateau most likely influences the cycle of atmospheric mercury on a continental scale

Physical and chemical properties of pollution aerosol particles transported from North America to Greenland as measured during the POLARCAT summer campaign

Within the framework of the POLARCAT-France campaign, aerosol physical, chemical and optical properties over Greenland were measured onboard the French ATR-42 research aircraft. The origins of CO excess peaks detected in the aircraft measurements then have been identified through FLEXPART simulations. The study presented here focuses particularly on the characterization of air masses transported from the North American continent to Greenland. Air masses that picked up emissions from Canadian boreal forest fires as well as from the cities on the American east coast were identified and selected for a detailed study. Measurements of CO concentrations, aerosol chemical composition, aerosol number size distributions, aerosol volume volatile fractions and aerosol light absorption (mainly from black carbon) are used in order to study the relationship between CO enhancement (ΔCO), aerosol particle concentrations and number size distributions. Aerosol number size distributions (normalised with their respective ΔCO) are in good agreement with previous studies. Nonetheless, wet scavenging may have occurred along the pathway between the emission sources and Greenland leading to a less pronounced accumulation mode in the POLARCAT data. Chemical analyses from mass spectrometry show that submicrometer aerosol particles are mainly composed of sulphate and organics. The observed bimodal (Aitken and accumulation) aerosol number size distributions show a significant enhancement in Aitken mode particles. Furthermore, results from the thermodenuder analysis demonstrate the external mixture of boreal fire (BF) air masses from North America (NA). This is particularly observed in the accumulation mode, containing a volume fraction of up to 25–30% of refractory material at the applied temperature of 280 °C. NA anthropogenic air masses with only 6% refractory material in the accumulation mode can be clearly distinguished from BF air masses. Overall, during the campaign rather small amounts of black carbon from the North American continent were transported towards Greenland during the summer POLARCAT observation period, which also is a valuable finding with respect to potential climate impacts of black carbon in the Arctic

East Asian Monsoon and Tropospheric Ozone from IASI/MetOp

International audienceAs an important greenhouse gas and air pollutant in the troposphere, monitoring of tropospheric ozone (O3) is essential to understand its impact on air quality, chemical composition and climate. In this presentation, two independent studies using O3 measurements from the Infrared atmospheric Sounding Interferometer (IASI) are presented. First, sensitivity studies are performed to investigate the origin of the systematic IASI O3 positive bias with respect to independent observations, which is reported in the literature. Second, the East Asian monsoon variability is assessed using six years of IASI tropospheric O3 columns. The study shows the ability of the instrument to detect the effect of the monsoon on the tropospheric ozone column and to reproduce the strength of the monsoon from one year to the other. Focusing on the period of May-August 2011, the WRF-Chem model is used at the surface and in the troposphere in conjunction with IASI to assess the meteorological and dynamical effects during the monsoon period on the tropospheric ozone column