Comparison of long term tropospheric ozone trends measured by lidar and ECC ozonesondes from 1991 to 2010 in Southern France

International audienceECC (Electrochemical Concentration Cell) ozonesondes and UV DIAL (DIfferential Absorption Lidar) measurements have been carried out simultaneously at OHP (Observatoire de Haute Provence, 44°N, 6.7°E, 690 m) since 1991. A unique long-term trend assessment by two different instruments operated routinely at the same location is possible. Air mass trajectories have been calculated for all the ozone observations available at OHP. The bias between the seasonal mean calculated with lidar and ECC ozone vertical profiles for 4 time- periods of 5 years is 0.6 ppbv in the free troposphere (4-8 km). Larger differences (> 10 ppbv) are explained by the need for clear sky conditions during lidar observations. The measurements of both instruments have been combined to decrease the impact of short-term atmospheric variability on the trend estimate

The megapoli paris campaign for urban aerosol characterisation - a comprehensive data set for air quality model evaluation

International audienceWithin the FP7 MEGAPOLI project, two intensive field campaigns have been conducted in the Greater Paris region during July 2009 and January/February 2010. The major aim was to quantify sources of primary and secondary aerosol, and the interaction with gaseous precursors, in and around a large agglomeration in temperate latitudes. From this campaign, a comprehensive data set will be built which will be available for urban and regional scale air quality model evaluation. The paper will present campaign objectives and set-up, first results, and specific benchmarks, which should be most useful for model evaluation

Comparison of lidar-derived PM10 with regional modeling and ground-based observations in the frame of MEGAPOLI experiment

International audienceAn innovative approach using mobile lidar measurements was implemented to test the performances of chemistry-transport models in simulating mass concentrations (PM10) predicted by chemistry-transport models. A ground-based mobile lidar (GBML) was deployed around Paris onboard a van during the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) summer experiment in July 2009. The measurements performed with this Rayleigh-Mie lidar are converted into PM10 profiles using optical-to-mass relationships previously established from in situ measurements performed around Paris for urban and peri-urban aerosols. The method is described here and applied to the 10 measurements days (MD). MD of 1, 15, 16 and 26 July 2009, corresponding to different levels of pollution and atmospheric conditions, are analyzed here in more details. Lidar-derived PM10 are compared with results of simulations from POLYPHEMUS and CHIMERE chemistry-transport models (CTM) and with ground-based observations from the AIRPARIF network. GBML-derived and AIRPARIF in situ measurements have been found to be in good agreement with a mean Root Mean Square Error RMSE (and a Mean Absolute Percentage Error MAPE) of 7.2 μg m−3 (26.0%) and 8.8 μg m−3 (25.2%) with relationships assuming peri-urban and urban-type particles, respectively. The comparisons between CTMs and lidar at ~200 m height have shown that CTMs tend to underestimate wet PM10 concentrations as revealed by the mean wet PM10 observed during the 10 MD of 22.4, 20.0 and 17.5 μg m−3 for lidar with peri-urban relationship, and POLYPHEMUS and CHIMERE models, respectively. This leads to a RMSE (and a MAPE) of 6.4 μg m−3 (29.6%) and 6.4 μg m−3 (27.6%) when considering POLYPHEMUS and CHIMERE CTMs, respectively. Wet integrated PM10 computed (between the ground and 1 km above the ground level) from lidar, POLYPHEMUS and CHIMERE results have been compared and have shown similar results with a RMSE (and MAPE) of 6.3 mg m−2 (30.1%) and 5.2 mg m−2 (22.3%) with POLYPHEMUS and CHIMERE when comparing with lidar-derived PM10 with periurban relationship. The values are of the same order of magnitude than other comparisons realized in previous studies. The discrepancies observed between models and measured PM10 can be explained by difficulties to accurately model the background conditions, the positions and strengths of the plume, the vertical turbulent diffusion (as well as the limited vertical model resolutions) and chemical processes as the formation of secondary aerosols. The major advantage of using vertically resolved lidar observations in addition to surface concentrations is to overcome the problem of limited spatial representativity of surface measurements. Even for the case of a well-mixed boundary layer, vertical mixing is not complete, especially in the surface layer and near source regions. Also a bad estimation of the mixing layer height would introduce errors in simulated surface concentrations, which can be detected using lidar measurements. In addition, horizontal spatial representativity is larger for altitude integrated measurements than for surface measurements, because horizontal inhomogeneities occurring near surface sources are dampened

Record-breaking ozone loss in the Arctic winter 2010/2011: comparison with 1996/1997

We present a detailed discussion of the chemical and dynamical processes in the Arctic winters 1996/1997 and 2010/2011 with high resolution chemical transport model (CTM) simulations and space-based observations. In the Arctic winter 2010/2011, the lower stratospheric minimum temperatures were below 195 K for a record period of time, from December to mid-April, and a strong and stable vortex was present during that period. Simulations with the Mimosa-Chim CTM show that the chemical ozone loss started in early January and progressed slowly to 1 ppmv (parts per million by volume) by late February. The loss intensified by early March and reached a record maximum of ~2.4 ppmv in the late March–early April period over a broad altitude range of 450–550 K. This coincides with elevated ozone loss rates of 2–4 ppbv sh^(−1) (parts per billion by volume/sunlit hour) and a contribution of about 30–55% and 30–35% from the ClO-ClO and ClO-BrO cycles, respectively, in late February and March. In addition, a contribution of 30–50% from the HO_x cycle is also estimated in April. We also estimate a loss of about 0.7–1.2 ppmv contributed (75%) by the NO_x cycle at 550–700 K. The ozone loss estimated in the partial column range of 350–550 K exhibits a record value of ~148 DU (Dobson Unit). This is the largest ozone loss ever estimated in the Arctic and is consistent with the remarkable chlorine activation and strong denitrification (40–50%) during the winter, as the modeled ClO shows ~1.8 ppbv in early January and ~1 ppbv in March at 450–550 K. These model results are in excellent agreement with those found from the Aura Microwave Limb Sounder observations. Our analyses also show that the ozone loss in 2010/2011 is close to that found in some Antarctic winters, for the first time in the observed history. Though the winter 1996/1997 was also very cold in March–April, the temperatures were higher in December–February, and, therefore, chlorine activation was moderate and ozone loss was average with about 1.2 ppmv at 475–550 K or 42 DU at 350–550 K, as diagnosed from the model simulations and measurements

Multiple symptoms of total ozone recovery inside the Antarctic vortex during austral spring

The long-term evolution of total ozone column inside the Antarctic polar vortex is investigated over the 1980-2016 period. Trend analyses are performed using a multilinear regression (MLR) model based on various proxies (heat flux, QBO, solar flux, AAO and aerosols). Annual total ozone column corresponding to the mean monthly values inside the vortex in September and during the period of maximum ozone depletion from September 15th to October 15th are used. Total ozone columns from combined TOMS-N7, SBUV-N9, TOMS-EP and OMI-TOMS satellite datasets and the Multi-Sensor Reanalysis (MRS-2) dataset are considered in the study. Ozone trends are computed by a piecewise trend model (PWT) before and after the turnaround in 2001. In order to evaluate total ozone within the vortex, two classification methods are used, based on the potential vorticity gradient as a function of equivalent latitude. The first standard one, considers this gradient at a single isentropic level (475K or 550K), while the second one uses a range of isentropic levels between 400K and 600K. The regression model includes a new proxy that represents the stability of the vortex during the studied month period. The determination coefficient (R2) between observations and modeled values increases by ~0.05 when this proxy is included in the MLR model. The higher R2 (0.93-0.95) and the minimum residuals are found for the second classification method in the case of both datasets and months periods. Trends in September are statistically significant at 2 sigma level with values ranging between 1.85 and 2.67 DU yr-1 depending on the methods and data sets. This result confirms the recent studies of Antarctic ozone healing during that month. Trends after 2001 are 2 to 3 times lower than before the turnaround year as expected from the response to the slowly ODS decrease in Polar regions.Estimated trends in the 15Sept-15Oct period are smaller than in September. They vary from 1.15 to 1.78 DU yr-1 and are hardly significant at 2 level. Ozone recovery is also confirmed by a steady decrease of the relative area of total ozone values lower than 150 DU within the vortex in the 15Sept-15Oct period since 2010. Comparison of the evolution of the ozone hole area in September and October show a decrease in September, confirming the later formation of the ozone hole during that month.Fil: Pazmino, Andrea. Universidad Paris Saclay; FranciaFil: Godin Beekmann, Sophie. Universidad Paris Saclay; FranciaFil: Hauchecorne, Alain. Universidad Paris Saclay; FranciaFil: Claud, Chantal. Ecole Polytechnique; FranciaFil: Khaykin, Sergey. Universidad Paris Saclay; FranciaFil: Goutail, Florence. Universidad Paris Saclay; FranciaFil: Wolfram, Elian Augusto. Consejo Nacional de Investigaciones Científicas y Técnicas. Instituto de Investigaciones Científicas y Técnicas para la Defensa. Centro de Investigación en Láseres y Aplicaciones; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Unidad de Investigación y Desarrollo Estratégico para la Defensa. Ministerio de Defensa. Unidad de Investigación y Desarrollo Estratégico para la Defensa; Argentina. Ministerio de Defensa; ArgentinaFil: Salvador, Jacobo Omar. Consejo Nacional de Investigaciones Científicas y Técnicas. Instituto de Investigaciones Científicas y Técnicas para la Defensa. Centro de Investigación en Láseres y Aplicaciones; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Unidad de Investigación y Desarrollo Estratégico para la Defensa. Ministerio de Defensa. Unidad de Investigación y Desarrollo Estratégico para la Defensa; Argentina. Ministerio de Defensa; Argentina. Universidad Tecnológica Nacional. Facultad Regional Buenos Aires; Argentina. Universidad Nacional de la Patagonia Austral; ArgentinaFil: Quel, Eduardo Jaime. Consejo Nacional de Investigaciones Científicas y Técnicas. Instituto de Investigaciones Científicas y Técnicas para la Defensa. Centro de Investigación en Láseres y Aplicaciones; Argentina. Ministerio de Defensa; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas. Unidad de Investigación y Desarrollo Estratégico para la Defensa. Ministerio de Defensa. Unidad de Investigación y Desarrollo Estratégico para la Defensa; Argentin

SCIAMACHY formaldehyde observations: constraint for isoprene emission estimates over Europe?

Formaldehyde (HCHO) is an important intermediate compound in the degradation of volatile organic compounds (VOCs) in the troposphere. Sources of HCHO are largely dominated by its secondary production from VOC oxidation, methane and isoprene being the main precursors in unpolluted areas. As a result of the moderate lifetime of HCHO, its spatial distribution is determined by reactive hydrocarbon emissions. We focus here on Europe and investigate the influence of the different emissions on HCHO tropospheric columns with the CHIMERE chemical transport model in order to interpret the comparisons between SCIAMACHY and simulated HCHO columns. Europe was never specifically studied before for these purposes using satellite observations. The bias between measurements and model is less than 20% on average. The differences are discussed according to the errors on the model and the observations and remaining discrepancies are attributed to a misrepresentation of biogenic emissions. This study requires the characterisation of: (1) the model errors and performances concerning formaldehyde. The errors on the HCHO columns, mainly related to chemistry and mixed emission types, are evaluated to 2×10<sup>15</sup> molecule/cm<sup>2</sup> and the model performances evaluated using surface measurements are satisfactory (~13%); (2) the observation errors that define the needs in spatial and temporal averaging for meaningful comparisons. Using SCIAMACHY observations as constraint for biogenic isoprene emissions in an inverse modelling scheme reduces their uncertainties by about a factor of two in region of intense emissions. The retrieved correction factors for the isoprene emissions range from a factor of 0.15 (North Africa) to a factor of 2 (Poland, the United Kingdom) depending on the regions

Comparison between simulated and observed chemical composition of fine aerosols in Paris (France) during springtime: contribution of regional versus continental emissions

Hourly concentrations of inorganic salts (ions) and carbonaceous material in fine aerosols (aerodynamic diameter, A.D. <2.5 μm) have been determined experimentally from fast measurements performed for a 3-week period in spring 2007 in Paris (France). The sum of these two chemical components (ions and carbonaceous aerosols) has shown to account for most of the fine aerosol mass (PM<sub>2.5</sub>). This time-resolved dataset allowed investigating the factors controlling the levels of PM<sub>2.5</sub> in Paris and showed that polluted periods with PM<sub>2.5</sub> > 15 μg m<sup>−3</sup> were characterized by air masses of continental (North-Western Europe) origin and chemical composition made by 75% of ions. By contrast, periods with clean marine air masses have shown the lowest PM<sub>2.5</sub> concentrations (typically of about 10 μg m<sup>−3</sup>); carbonaceous aerosols contributing for most of this mass (typically 75%). <br><br> In order to better discriminate between local and continental contributions to the observed chemical composition and concentrations of PM<sub>2.5</sub> over Paris, a comparative study was performed between this time-resolved dataset and the outputs of a chemistry transport model (CHIMERE), showing a relatively good capability of the model to reproduce the time-limited intense maxima observed in the field for PM<sub>2.5</sub> and ion species. Different model scenarios were then investigated switching off local and European (North-Western and Central) emissions. Results of these scenarios have clearly shown that most of the ions observed over Paris during polluted periods, were either transported or formed in-situ from gas precursors transported from Northern Europe. On the opposite, long-range transport from Europe appeared to weakly contribute to the levels of carbonaceous aerosols observed over Paris. <br><br> The model failed to properly account for the concentration levels and variability of secondary organic aerosols (SOA) determined experimentally by the EC-tracer method. The abundance of SOA (relatively to organic aerosol, OA) was as much as 75%, showing a weak dependence on air masses origin. Elevated SOA/OA ratios were also observed for air masses having residence time above ground of less than 10 h, suggesting intense emissions and/or photochemical processes leading to rapid formation of secondary organic aerosols

Coherence of long-term stratospheric ozone vertical distribution time series used for the study of ozone recovery at a northern mid-latitude station

The coherence of stratospheric ozone time series retrieved from various observational records is investigated at Haute-Provence Observatory (OHP–43.93° N, 5.71° E). The analysis is accomplished through the intercomparison of collocated ozone measurements of Light Detection and Ranging (lidar) with Solar Backscatter UltraViolet(/2) (SBUV(/2)), Stratospheric Aerosol and Gas Experiment II (SAGE~II), Halogen Occultation Experiment (HALOE), Microwave Limb Sounder (MLS) on Upper Atmosphere Research Satellite (UARS) and Aura and Global Ozone Monitoring by Occultation of Stars (GOMOS) satellite observations as well as with in situ ozonesondes and ground-based Umkehr measurements performed at OHP. A detailed statistical study of the relative differences of ozone observations over the whole stratosphere is performed to detect any specific drift in the data. On average, all instruments show their best agreement with lidar at 20–40 km, where deviations are within ±5 %. Discrepancies are somewhat higher below 20 and above 40 km. The agreement with SAGE II data is remarkable since average differences are within ±1 % at 17–41 km. In contrast, Umkehr data underestimate systematically the lidar measurements in the whole stratosphere with a near zero bias at 16–8 hPa (~30 km). Drifts are estimated using simple linear regression for the data sets analysed in this study, from the monthly averaged difference time series. The derived values are less than ±0.5 % yr<sup>−1</sup> in the 20–40 km altitude range and most drifts are not significant at the 2<i>σ</i> level. We also discuss the possibilities of extending the SAGE II and HALOE data with the GOMOS and Aura MLS data in consideration with relative offsets and drifts since the combination of such data sets are likely to be used for the study of stratospheric ozone recovery in the future

Application of mobile aerosol and trace gas measurements for the investigation of megacity air pollution emissions: the Paris metropolitan area

For the investigation of megacity emission development and the impact outside the source region, mobile aerosol and trace gas measurements were carried out in the Paris metropolitan area between 1 July and 31 July 2009 (summer conditions) and 15 January and 15 February 2010 (winter conditions) in the framework of the European Union FP7 MEGAPOLI project. Two mobile laboratories, MoLa and MOSQUITA, were deployed, and here an overview of these measurements and an investigation of the applicability of such measurements for the analysis of megacity emissions are presented. Both laboratories measured physical and chemical properties of fine and ultrafine aerosol particles as well as gas phase constituents of relevance for urban pollution scenarios. The applied measurement strategies include cross-section measurements for the investigation of plume structure and quasi-Lagrangian measurements axially along the flow of the city's pollution plume to study plume aging processes. Results of intercomparison measurements between the two mobile laboratories represent the adopted data quality assurance procedures. Most of the compared measurement devices show sufficient agreement for combined data analysis. For the removal of data contaminated by local pollution emissions a video tape analysis method was applied. Analysis tools like positive matrix factorization and peak integration by key analysis applied to high-resolution time-of-flight aerosol mass spectrometer data are used for in-depth data analysis of the organic particulate matter. Several examples, including a combination of MoLa and MOSQUITA measurements on a cross section through the Paris emission plume, are provided to demonstrate how such mobile measurements can be used to investigate the emissions of a megacity. A critical discussion of advantages and limitations of mobile measurements for the investigation of megacity emissions completes this work