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Aerosol forecasts by the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecasting System aerosol module (IFS-AER) for the years 2016–2019 (cycles 41r1–46r1) are compared to vertical profiles of particle backscatter from the Deutscher Wetterdienst (DWD) ceilometer network. The system has been developed in the Copernicus Atmosphere Monitoring Service (CAMS) and its precursors. The focus of this article is to evaluate the realism of the vertical aerosol distribution from 0.4 to 8 km above ground, coded in the shape, bias and temporal variation of the profiles. The common physical quantity, the attenuated backscatter β∗(z), is directly measured and calculated from the model mass mixing ratios of the different particle types using the model's inherent aerosol microphysical properties. Pearson correlation coefficients of daily average simulated and observed vertical profiles between r=0.6–0.8 in summer and 0.7–0.95 in winter indicate that most of the vertical structure is captured. It is governed by larger β∗(z) in the mixing layer and comparably well captured with the successive model versions. The aerosol load tends to be biased high near the surface, underestimated in the mixing layer and realistic at small background values in the undisturbed free troposphere. A seasonal cycle of the bias below 1 km height indicates that aerosol sources and/or lifetimes are overestimated in summer and pollution episodes are not fully resolved in winter. Long-range transport of Saharan dust or fire smoke is captured and timely, only the dispersion to smaller scales is not resolved in detail. Over Germany, β∗(z) values from Saharan dust and sea salt are considerably overestimated. Differences between model and ceilometer profiles are investigated using observed in situ mass concentrations of organic matter (OM), black carbon, SO4, NO3, NH4 and proxies for mineral dust and sea salt near the surface. Accordingly, SO4 and OM sources as well as gas-to-particle partitioning of the NO3–NH4 system are too strong. The top of the mixing layer on average appears too smooth and several hundred meters too low in the model. Finally, a discussion is included of the considerable uncertainties in the observations as well as the conversion from modeled to observed physical quantities and from necessary adaptions of varying resolutions and definitions.

Here, we present the final, commercially available, version of a mobility particle size spectrometer that is able to access the 1 nm particle size range for ambient atmospheric measurements.The overall system performance was tested in a multitude of laboratory experiments, determining various size dependent parameters like DMA’s transfer function, DMA penetration efficiency, PSM and CPC counting efficiency. With the knowledge of these parameters, we are able to define a well-known overall system performance, a critical prerequisite for measurements that start at 1 nm sized particles.The instrument originates from a collaboration of Grimm Aerosol Technik, Germany and Airmodus Ltd, Finland, combining a Grimm SMPS+C system with the Airmodus Particle Size Magnifier (PSM). Accordingly, it is named: PSMPS.The main system components comprise a modified version of the short Grimm Differential Mobility Analyzer (Grimm S-DMA), the diethylene glycol-based PSM (Airmodus A10) and the new butanol-based CPC (Grimm 5417). The modified S-DMA is specially optimized for the transmission of small ions. Typically, it is operated with an aerosol sample flow rate of 2.5 L/min and a sheath flow rate of 10 L/min, allowing particle size distribution measurements from 1.1-55.7 nm. The PSM is used to lower the detection efficiency of the Grimm CPC below 2 nm in electrical mobility equivalent diameter. The new Grimm 5417 CPC is an upgraded version of the well-known 5416 CPC, that features two switchable aerosol sample flow rates of 0.3 and 0.6 L/min and also supplies the S-DMA with sheath airflow rates of either 3.0 or 10.0 L/min.In this presentation, we will introduce the features and performance of the PSMPS system, will highlight some laboratory characterization tests and report the results from an ambient aerosol measurement campaign at the Hohenpeissenberg Observatory of the German meteorological service (DWD), monitoring new particle formation events starting at a particles size of 1nm.

In order to assess the global evolution of aerosol parameters affecting climate change, a long-term trend analyses of aerosol optical properties were performed on time series from 52 stations situated across five continents. The time series of measured scattering, backscattering and absorption coefficients as well as the derived single scattering albedo, backscattering fraction, scattering and absorption Ångström exponents covered at least 10 years and up to 40 years for some stations. The non-parametric seasonal Mann–Kendall (MK) statistical test associated with several prewhitening methods and with the Sen's slope were used as main trend analysis methods. Comparisons with General Least Mean Square associated with Autoregressive Bootstrap (GLS/ARB) and with standard Least Mean Square analysis (LMS) enabled confirmation of the detected MK statistically significant trends and the assessment of advantages and limitations of each method. Currently, scattering and backscattering coefficients trends are mostly decreasing in Europe and North America and are not statistically significant in Asia, while polar stations exhibit a mix of increasing and decreasing trends. A few increasing trends are also found at some stations in North America and Australia. Absorption coefficients time series also exhibit primarily decreasing trends. For single scattering albedo, 52 % of the sites exhibit statistically significant positive trends, mostly in Asia, Eastern/Northern Europe and Arctic, 18 % of sites exhibit statistically significant negative trends, mostly in central Europe and central North America, while the remaining 30 % of sites have trends, which are not statistically significant. In addition to evaluating trends for the overall time series, the evolution of the trends in sequential 10 year segments was also analyzed. For scattering and backscattering, statistically significant increasing 10 year trends are primarily found for earlier periods (10 year trends ending in 2010–2015) for polar stations and Mauna Loa. For most of the stations, the present-day statistically significant decreasing 10 year trends of the single scattering albedo were preceded by not statistically significant and statistically significant increasing 10 year trends. The effect of air pollution abatement policies in continental North America is very obvious in the 10 year trends of the scattering coefficient – there is a shift to statistically significant negative trends in 2010–2011 for all stations in the eastern and central US. This long-term trend analysis of aerosol radiative properties with a broad spatial coverage enables a better global view of potential aerosol effects on climate changes.

High altitude stations are often emphasized as free tropospheric measuring sites but they remain influenced by atmospheric boundary layer (ABL) air masses due to convective transport processes. The local and meso-scale topographical features around the station are involved in the convective boundary layer development and in the formation of thermally induced winds leading to ABL air lifting. The station altitude alone is not a sufficient parameter to characterize the ABL influence. In this study, a topography analysis is performed allowing calculation of a newly defined index called ABL-TopoIndex. The ABL-TopoIndex is constructed in order to correlate with the ABL influence at the high altitude stations and long-term aerosol time series are used to assess its validity. Topography data from the global digital elevation model GTopo30 were used to calculate five parameters for 43 high and 3 middle altitude stations situated on five continents. The geometric mean of these five parameters determines a topography based index called ABL-TopoIndex, which can be used to rank the high altitude stations as a function of the ABL influence. To construct the ABL-TopoIndex, we rely on the criteria that the ABL influence will be low if the station is one of the highest points in the mountainous massif, if there is a large altitude difference between the station and the valleys or high plains, if the slopes around the station are steep, and finally if the inverse drainage basin potentially reflecting the source area for thermally lifted pollutants to reach the site is small. All stations on volcanic islands exhibit a low ABL-TopoIndex, whereas stations in the Himalayas and the Tibetan Plateau have high ABL-TopoIndex values. Spearman's rank correlation between aerosol optical properties and number concentration from 28 stations and the ABL-TopoIndex, the altitude and the latitude are used to validate this topographical approach. Statistically significant (SS) correlations are found between the 5th and 50th percentiles of all aerosol parameters and the ABL-TopoIndex, whereas no SS correlation is found with the station altitude. The diurnal cycles of aerosol parameters seem to be best explained by the station latitude although a SS correlation is found between the amplitude of the diurnal cycles of the absorption coefficient and the ABL-TopoIndex. © 2018 Author(s)., The authors gratefully acknowledge the following persons and organizations. – Wolfgang Schwanghart, the programmer of the TopoToolBox for putting his codes as a freeware and for all the kind and always rapid support he offers. – CHC: the Chacaltaya consortium and Laboratory for Atmospheric Physics at UMSA for taking care of the station and collecting the data. Swedish participation was supported by the Swedish Foundation for International Cooperation in Research and Higher Education (STINT) and the Swedish research council FORMAS. – CMN: the European Commission funded ACTRIS, ACTRIS2 EU project and NEXTDATA National project funded by MIUR. – IZO: Global Atmospheric Watch program funded by AEMET and by the project AEROATLAN (CGL2015-66299-P), funded by the Ministry of Economy and Competitiveness of Spain and the European Regional Development Fund (ERDF). – JFJ: International Foundation High Altitude Research Stations Jungfraujoch and Gornergrat (HFSJG) and the Federal Office of Meteorology and Climatology, MeteoSwiss, within the Swiss program of the Global Atmosphere Watch (GAW) of the World Meteorological Organization, funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement no. 654109 (ACTRIS2), and the Swiss State Secretariat for Education, Research and Innovation (SERI) under contract no. 15.0159-1. The opinions expressed and arguments employed herein do not necessarily reflect the official views of the Swiss Government. – LLN: the Taiwan Environmental Protection Administration. – MSA and MSY: MINECO (Spanish Ministry of Economy and Competitiveness), the MAGRAMA (Spanish Ministry of Agriculture, Food and Environment), the Generalitat de Catalunya (AGAUR 2014 SGR33 and the DGQA) and FEDER funds under the PRISMA project (CGL2012-39623-C02/00). This work has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 654109. Marco Pandolfi is funded by a Ramón y Cajal Fellowship (RYC-2013-14036) awarded by the Spanish Ministry of Economy and Competitiveness.

Aerosol particles are essential constituents of the Earth’s atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence time resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in-situ near-surface segment of the atmospheric observations system. This paper will provide the widest effort so far to document variability of climate-relevant in-situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High quality data from more than 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single scattering albedo and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information including data provision procedures, quality control and analysis, data policy and usage of the ground-based aerosol measurements network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully-characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.

This work describes results obtained from the 2016 Aerosol Chemical Speciation Monitor (ACSM) intercomparison exercise performed at the Aerosol Chemical Monitor Calibration Center (ACMCC, France). Fifteen quadrupole ACSMs (Q_ACSM) from the European Research Infrastructure for the observation of Aerosols, Clouds and Trace gases (ACTRIS) network were calibrated using a new procedure that acquires calibration data under the same operating conditions as those used during sampling and hence gets information representative of instrument performance. The new calibration procedure notably resulted in a decrease in the spread of the measured sulfate mass concentrations, improving the reproducibility of inorganic species measurements between ACSMs as well as the consistency with co-located independent instruments. Tested calibration procedures also allowed for the investigation of artifacts in individual instruments, such as the overestimation of m/z 44 from organic aerosol. This effect was quantified by the m/z (mass-to-charge) 44 to nitrate ratio measured during ammonium nitrate calibrations, with values ranging from 0.03 to 0.26, showing that it can be significant for some instruments. The fragmentation table correction previously proposed to account for this artifact was applied to the measurements acquired during this study. For some instruments (those with high artifacts), this fragmentation table adjustment led to an “overcorrection” of the f44 (m/z 44/Org) signal. This correction based on measurements made with pure NH4NO3, assumes that the magnitude of the artifact is independent of chemical composition. Using data acquired at different NH4NO3 mixing ratios (from solutions of NH4NO3 and (NH4)2SO4) we observe that the magnitude of the artifact varies as a function of composition. Here we applied an updated correction, dependent on the ambient NO3 mass fraction, which resulted in an improved agreement in organic signal among instruments. This work illustrates the benefits of integrating new calibration procedures and artifact corrections, but also highlights the benefits of these intercomparison exercises to continue to improve our knowledge of how these instruments operate, and assist us in interpreting atmospheric chemistry. © 2019, © 2019 Author(s). Published with license by Taylor & Francis Group, LLC., Funding text #1 aLaboratoire de Météorologie Physique (LaMP), Aubiere, France; bInstitut National de l’Environnement Industriel et des Risques (INERIS), Verneuil-en-Halatte, France; cLaboratoire des Sciences du Climat et de l’Environnement (LSCE), CNRS-CEA-UVSQ, Gif-sur-Yvette, France; dAerodyne Research, Inc, Billerica, Massachusetts, USA; eEnvironment Energy and Water Research Center, The Cyprus Institute, Nicosia, Cyprus; fEstonian Environmental Research Center (EERC), Tallinn, Estonia; gFinnish meteorological institute (FMI), Helsinki, Finland; hIERSD, National Observatory of Athens, Athens, Greece; iDepartment of the Environment, Centre for Energy, Environment and Technology Research (CIEMAT), Madrid, Spain; jDeutscher Wetterdienst, Meteorologisches Observatorium Hohenpeißenberg, Hohenpeißenberg, Germany; kInstitute for Atmospheric and Earth System Research (INAR)/Physics, Faculty of Science, University of Helsinki, Helsinki, Finland; lLeibniz Institute for Tropospheric Research, Leipzig, Germany; mEnvironmental Research Group, MRC-HPA Centre for Environment and Health, King’s College London, London, United Kingdom; nInstitute of Environmental Assessment and Water Research (IDAEA-CSIC), Barcelona, Spain; oLaboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen PSI, Switzerland; pNational Institute of R&D for Optoelectronics (INOE), Ilfov, Romania; qProambiente S.c.r.l CNR Research Area, Bologna, Italy Funding text #2 This project has received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement No 654109. The US Department of Energy Small Business Innovative Research program (award number DE-SC0017041) provided support for development of ACSM calibration procedures. CNRS, CEA, and INERIS are acknowledged for financial support of the ACMCC. The intercomparison campaign and the following data treatment have been conducted in collaboration with the French reference laboratory for air quality monitoring (LCSQA), funded by the French Ministry of Environment. COST action CA16109 Chemical On-Line cOmpoSition and Source Apportionment of fine aerosoLs COLOSSAL grant is gratefully acknowledged for the support of data workshops. M.C. Minguillón acknowledges the Ramón y Cajal fellowship awarded by the Spanish Ministry of Economy, Industry and Competitiveness. The CIEMAT participation has been partially funded by MINECO/AEI/FEDER, UE (CGL2017-85344-R and CGL2017-90884-REDT) and TIGAS-CM (Y2018/EMT- 5177) Project. PSI is grateful for financial support by the Federal Office for the Environment in Switzerland.

This work reports the first statistical analysis of multi-annual data on tropospheric aerosols from the German Ultrafine Aerosol Network (GUAN). Compared to other networks worldwide, GUAN with 17 measurement locations has the most sites equipped with particle number size distribution (PNSD) and equivalent black carbon (eBC) instruments and the most site categories in Germany ranging from city street/roadside to High Alpine. As we know, the variations of eBC and particle number concentration (PNC) are influenced by several factors such as source, transformation, transport and deposition. The dominant controlling factor for different pollutant parameters might be varied, leading to the different spatio-temporal variations among the measured parameters. Currently, a study of spatio-temporal variations of PNSD and eBC considering the influences of both site categories and spatial scale is still missing. Based on the multi-site dataset of GUAN, the goal of this study is to investigate how pollutant parameters may interfere with spatial characteristics and site categories.

A series of major eruptions of the Eyjafjallajökull volcano in Iceland started on 14 April 2010 and continued until the end of May 2010. The volcanic emissions moved over nearly the whole of Europe and were observed first on 16 April 2010 in Southern Germany with different remote sensing systems from the ground and space. Enhanced PM10 and SO2 concentrations were detected on 17 April at mountain stations (Zugspitze/Schneefernerhaus and Schauinsland) as well as in Innsbruck by in situ measurement devices. On 19 April intensive vertical mixing and advection along with clear-sky conditions facilitated the entrainment of volcanic material down to the ground. The subsequent formation of a stably stratified lower atmosphere with limited mixing near the ground during the evening of 19 April led to an additional enhancement of near-surface particle concentrations. Consequently, on 19 April and 20 April exceedances of the daily threshold value for particulate matter (PM10) were reported at nearly all monitoring stations of the North Alpine foothills as well as at mountain and valley stations in the northern Alps. The chemical analyses of ambient PM10 at monitoring stations of the North Alpine foothills yielded elevated Titanium concentrations on 19/20 April which prove the presence of volcanic plume material. Following this result the PM10 threshold exceedances are also associated with the volcanic plume. The entrainment of the volcanic plume material mainly affected the concentrations of coarse particles (>1 μm) – interpreted as volcanic ash – and ultrafine particles (

An inventory of Sahara dust (SD) events at the Hohenpeiβenberg Global Atmosphere Watch station (Germany) is presented for the period 1997–2013. Based on daily in-situ measurements, high Ca 2+ -ion concentrations and large particle volume concentrations at diameters d p ≈ 0.5–7 μm are inferred as indicators for days influenced by SD. The resulting SD catalogue agrees with SD time series from Schneefernerhaus, Augsburg and Jungfraujoch stations. On average, SD occurs in 5–15 SD events (SDE) per year covering about 10–60 days/yr in the mixing layer. SDE exhibit a clear seasonality with spring and early autumn maxima, and typically last for 1–3 days. SDE are equally frequent but more significant at Alpine levels due to lower background. Wet deposition of Ca 2+ at the surface is little correlated (R 2 = 0.14) with particle Ca 2+ on a daily basis and yields an average annual Ca 2+ immission of 0.22 ± 0.04 g/m 2 yr, about 40% of which is due to SD. The majority of outstanding weekly Fe and Al depositions are associated with SDE. SD contributes about 0.5 ± 0.1 μg/m 3 to the total particle mass with a decreasing trend from 6% to 4% (−0.1%/yr) in the 1997–2013 period. Except from one, all threshold exceedances according to European legislation (daily PM 10 > 50 μg/m 3 ) at Hohenpeiβenberg are due to SD. Implications are discussed with respect to SD-related circulation patterns, SD-induced temperature anomalies in weather forecast models and the capability of aerosol models to capture SDE.

In this paper, we present a comparison of European Centre for Medium-Range Weather Forecast Integrated Forecast System (ECMWF-IFS) model simulation of aerosol backscatter profiles with measurements of the ceilometer network operated by the German weather service (DWD) over 1 year from September 2015 to August 2016. As the model output provides mass mixing ratios of different types of aerosol whereas the ceilometers don't, it is necessary to determine a common physical quantity for the comparison. We have chosen the attenuated backscatter β* for this purpose. The β*-profiles are calculated from the mass mixing ratios of the model output assuming the inherent aerosol microphysical properties. Comparison of the attenuated backscatter, averaged between an altitude from 0.2 km (typical overlap range of ceilometers) and 1 km, showed slightly larger values from the model. To investigate possible reasons for the differences, we have examined the role of the hygroscopic growth of particles and the particle shape. Our results show that using a more recent particle growth model would result in a ~ 22 % reduction of particle backscatter for sea salt aerosols, corresponding to a 10 %-reduction of the total backscatter signal on average. Accounting for non-spherical dust particles in the model would reduce attenuated backscatter of dust particles by ~ 30 %. As the concentration of dust aerosol is in general very low in Germany, a significant effect on the total backscatter signal is restricted to dust episodes. In summary, consideration of both effects tend to improve the agreement between model and observations, but without leading to a perfect consistency. In addition a case study was conducted to investigate the agreement of the spatiotemporal distribution of particles. It was found that for a dust episode in April 2016 the arrival time of the dust layer and its vertical extent very well agree between model and ceilometer measurements for several stations. However, due to the large set of parameters characterizing the aerosol distribution and the complexity of the ceilometer retrieval an automated and quantitative comparison scheme for β*-profiles is still missing. Consequently, the representativeness of the case study remains open.

Photogrammetric methods and analysis results for contrails observed with wide-angle cameras are described. Four cameras of two different types (view angle < 90° or whole-sky imager) at the ground at various positions are used to track contrails and to derive their altitude, width, and horizontal speed. Camera models for both types are described to derive the observation angles for given image coordinates and their inverse. The models are calibrated with sightings of the Sun, the Moon and a few bright stars. The methods are applied and tested in a case study. Four persistent contrails crossing each other together with a short-lived one are observed with the cameras. Vertical and horizontal positions of the contrails are determined from the camera images to an accuracy of better than 200 m and horizontal speed to 0.2 m s−1. With this information, the aircraft causing the contrails are identified by comparison to traffic waypoint data. The observations are compared with synthetic camera pictures of contrails simulated with the contrail prediction model CoCiP, a Lagrangian model using air traffic movement data and numerical weather prediction (NWP) data as input. The results provide tests for the NWP and contrail models. The cameras show spreading and thickening contrails suggesting ice-supersaturation in the ambient air. The ice-supersaturated layer is found thicker and more humid in this case than predicted by the NWP model used. The simulated and observed contrail positions agree up to differences caused by uncertain wind data. The contrail widths, which depend on wake vortex spreading, ambient shear and turbulence, were partly wider than simulated.

High altitude stations are often emphasized as free tropospheric measuring sites but they remain influenced by atmospheric boundary layer (ABL) air masses due to convective transport processes. The local and meso-scale topographical features around the station are involved in the convective boundary layer development and in the formation of thermally induced winds leading to ABL air lifting. The station altitude is not a sufficient parameter to characterize the ABL influence. Topography data from the global digital elevation model GTopo30 were used to calculate 5 parameters for 46 high altitude stations situated in five continents. The geometric mean of these 5 parameters determines a topography based index called ABL-TopoIndex which can be used to rank the high altitude stations as a function of the ABL influence. To construct the ABL-TopoIndex, we rely on the criteria that the ABL influence will be low if the station is one of the highest points in the mountainous massif, if there is a large altitude difference between the station and the valleys or plateaus, if the slopes around the station are steep, and finally if the drainage basin for air convection is small. All stations on volcanic islands exhibit a low ABL-TopoIndex whereas stations in the Himalaya and the Tibetan Plateau have high ABL-TopoIndex values. Spearman's rank correlation between aerosol optical properties and number concentration from 28 stations and the ABL-TopoIndex, the altitude and the latitude are used to validate this topographical approach. Statistically significant (s.s.) correlations are found between the 5 and 50 percentiles of all aerosol parameters and the ABL-TopoIndex whereas no s.s. correlation is found with the station altitude. The diurnal cycles of aerosol parameters seem to be best explained by the station latitude although a s.s. correlation is found between the amplitude of the diurnal cycles of the absorption coefficient and the ABL-TopoIndex. Finally, the main flow paths for air convection were calculated for various ABL heights.

Currently many ground-based atmospheric stations include in-situ measurements of aerosol physical and optical properties, resulting in more than 20 long-term (> 10 yr) aerosol measurement sites in the Northern Hemisphere and Antarctica. Most of these sites are located at remote locations and monitor the aerosol particle number concentration, wavelength-dependent light scattering, backscattering, and absorption coefficients. The existence of these multi-year datasets enables the analysis of long-term trends of these aerosol parameters, and of the derived light scattering Ångström exponent and backscatter fraction. Since the aerosol variables are not normally distributed, three different methods (the seasonal Mann-Kendall test associated with the Sen's slope, the generalized least squares fit associated with an autoregressive bootstrap algorithm for confidence intervals, and the least-mean square fit applied to logarithms of the data) were applied to detect the long-term trends and their magnitudes. To allow a comparison among measurement sites, trends on the most recent 10 and 15 yr periods were calculated. No significant trends were found for the three continental European sites. Statistically significant trends were found for the two European marine sites but the signs of the trends varied with aerosol property and location. Statistically significant decreasing trends for both scattering and absorption coefficients (mean slope of −2.0% yr−1) were found for most North American stations, although positive trends were found for a few desert and high-altitude sites. The difference in the timing of emission reduction policy for the Europe and US continents is a likely explanation for the decreasing trends in aerosol optical parameters found for most American sites compared to the lack of trends observed in Europe. No significant trends in scattering coefficient were found for the Arctic or Antarctic stations, whereas the Arctic station had a negative trend in absorption coefficient. The high altitude Pacific island station of Mauna Loa presents positive trends for both scattering and absorption coefficients.

The potential of a new generation of ceilometer instruments for aerosol monitoring has been studied in the Ceilometer Lidar Comparison (CLIC) study. The used ceilometer was developed by Jenoptik, Germany, and is designed to find both thin cirrus clouds at tropopause level and aerosol layers at close ranges during day and night-time. The comparison study was performed to determine up to which altitude the ceilometers are capable to deliver particle backscatter coefficient profiles. For this, the derived ceilometer profiles are compared to simultaneously measured lidar profiles at the same wavelength. The lidar used for the comparison was the multi-wavelengths Raman lidar PollyXT. To demonstrate the capabilities and limits of ceilometers for the derivation of particle backscatter coefficient profiles from their measurements two examples of the comparison results are shown. Two cases, a daytime case with high background noise and a less noisy night-time case, are chosen. In both cases the ceilometer profiles compare well with the lidar profiles in atmospheric structures like aerosol layers or the boundary layer top height. However, the determination of the correct magnitude of the particle backscatter coefficient needs a calibration of the ceilometer data with an independent measurement of the aerosol optical depth by a sun photometer. To characterizes the ceilometers signal performance with increasing altitude a comprehensive signal-to-noise ratio study was performed. During daytime the signal-to-noise ratio is higher than 1 up to 4–5 km depending on the aerosol content. In our night-time case the SNR is higher than 1 even up to 8.5 km, so that also aerosol layers in the upper troposphere had been detected by the ceilometer.

Volcanic emissions from the Eyjafjallajökull volcano eruption on the Southern fringe of Iceland in April 2010 were detected at the Global Atmosphere Watch (GAW) station Zugspitze/Hohenpeissenberg (Germany) by means of in-situ measurements, ozone sondes and ceilometers. Information from the German Meteorological Service (DWD) ceilometer network (Flentje et al., 2010) aided identifying the air mass origin. We discuss ground level in-situ measurements of sulphur dioxide (SO2), sulphuric acid (H2SO4) and particulate matter as well as ozone sonde profiles and column measurements of SO2 by a Brewer spectrometer. At Hohenpeissenberg, a number of reactive gases, e.g. carbon monoxide and nitrogen oxides, and particle properties, e.g. size distribution and ionic composition, were additionally measured during this period. Our results describe the arrival of the volcanic plume at Zugspitze and Hohenpeissenberg during 16 and 17 April 2010 and its residence in the planetary boundary layer (PBL) for several days thereafter. The ash plume was first seen in the ceilometer backscatter profiles at Hohenpeissenberg in about 6–7 km altitude. After entrainment into the PBL at noon of 17 April, largely enhanced values of sulphur dioxide, sulphuric acid and super-micron-particle number concentration were recorded at Zugspitze/Hohenpeissenberg till 21 April.

Three global Chemistry Transport Models – MOZART, MOCAGE, and TM5 – as well as MOZART coupled to the IFS meteorological model including assimilation of ozone (O3) and carbon monoxide (CO) satellite column retrievals, have been compared to surface measurements and MOZAIC vertical profiles in the troposphere over Western/Central Europe for summer 2003. The models reproduce the meteorological features and enhancement of pollution during the period 2–14 August, but not fully the ozone and CO mixing ratios measured during that episode. Modified normalised mean biases are around −25% (except ~5% for MOCAGE) in the case of ozone and from −80% to −30% for CO in the boundary layer above Frankfurt. The coupling and assimilation of CO columns from MOPITT overcomes some of the deficiencies in the treatment of transport, chemistry and emissions in MOZART, reducing the negative biases to around 20%. The high reactivity and small dry deposition velocities in MOCAGE seem to be responsible for the overestimation of O3 in this model. Results from sensitivity simulations indicate that an increase of the horizontal resolution to around 1°×1° and potential uncertainties in European anthropogenic emissions or in long-range transport of pollution cannot completely account for the underestimation of CO and O3 found for most models. A process-oriented TM5 sensitivity simulation where soil wetness was reduced results in a decrease in dry deposition fluxes and a subsequent ozone increase larger than the ozone changes due to the previous sensitivity runs. However this latest simulation still underestimates ozone during the heat wave and overestimates it outside that period. Most probably, a combination of the mentioned factors together with underrepresented biogenic emissions in the models, uncertainties in the modelling of vertical/horizontal transport processes in the proximity of the boundary layer as well as limitations of the chemistry schemes are responsible for the underestimation of ozone (overestimation in the case of MOCAGE) and CO found in the models during this extreme pollution event.

The German Ultrafine Aerosol Network (GUAN) is a cooperative atmospheric observation network, which aims at improving the scientific understanding of aerosol-related effects in the troposphere. The network addresses research questions dedicated to both climate- and health-related effects. GUAN's core activity has been the continuous collection of tropospheric particle number size distributions and black carbon mass concentrations at 17 observation sites in Germany. These sites cover various environmental settings including urban traffic, urban background, rural background, and Alpine mountains. In association with partner projects, GUAN has implemented a high degree of harmonisation of instrumentation, operating procedures, and data evaluation procedures. The quality of the measurement data is assured by laboratory intercomparisons as well as on-site comparisons with reference instruments. This paper describes the measurement sites, instrumentation, quality assurance, and data evaluation procedures in the network as well as the EBAS repository, where the data sets can be obtained (doi:10.5072/guan).

Three extended airborne Differential Absorption Lidar (DIAL) sections of tropospheric water vapour across the tropical and sub-tropical Atlantic in March 2004 are compared to short-term forecasts of the European Centre for Medium Range Weather Forecasts (ECMWF). The humidity fields between 28° S and 36° N exhibit large inter air-mass gradients and reflect typical transport patterns of low- and mid-latitudes like convection (e.g. Hadley circulation), subsidence and baroclinic development with stratospheric intrusion. These processes re-distribute water vapour vertically such that locations with extraordinary dry/moist air-masses are observed in the lower/upper troposphere, respectively. The mixing ratios range over 3 orders of magnitude. Back-trajectories are used to trace and characterize the observed air-masses. Overall, the observed water vapour distributions are largely reproduced by the short-term forecasts at 0.25° resolution (T799/L91), the correlation ranges from 0.69 to 0.92. Locally, large differences occur due to comparably small spatial shifts in presence of strong gradients. Systematic deviations are found associated with specific atmospheric domains. The planetary boundary layer in the forecast is too moist and to shallow. Convective transport of humidity to the middle and upper troposphere tends to be overestimated. Potential impacts arising from data assimilation and model physics are considered. The matching of air-mass boundaries (transport) is discussed with repect to scales and the representativity of the 2-D sections for the 3-D humidity field. The normalized bias of the model with respect to the observations is 6%, 11% and 0% (moist model biases) for the three along-flight sections, whereby however the lowest levels are excluded.

We present the results of an analysis performed for tropical cyclone Davina, a storm that lasted for 20 days and crossed the southern Indian Ocean during late winter 1999. From February to March of the same year an experimental campaign, called APE-THESEO, took place in the western Indian Ocean. It aimed to study the microphysical processes occurring in tropical cirrus and the transport of tracers across the tropical tropopause. To accomplish this task, two aircraft were deployed: the DLR Falcon and the M-55 Geophysica. Both of them were equipped with a large number of in situ and remote sensing instruments. On 9 March 1999 the two airplanes took measurements right above and inside the eye of Davina.

The European MACC (Monitoring Atmospheric Composition and Climate) project is preparing the operational Copernicus Atmosphere Monitoring Service (CAMS), one of the services of the European Copernicus Programme on Earth observation and environmental services. MACC uses data assimilation to combine in situ and remote sensing observations with global and regional models of atmospheric reactive gases, aerosols, and greenhouse gases, and is based on the Integrated Forecasting System of the European Centre for Medium-Range Weather Forecasts (ECMWF). The global component of the MACC service has a dedicated validation activity to document the quality of the atmospheric composition products. In this paper we discuss the approach to validation that has been developed over the past 3 years. Topics discussed are the validation requirements, the operational aspects, the measurement data sets used, the structure of the validation reports, the models and assimilation systems validated, the procedure to introduce new upgrades, and the scoring methods. One specific target of the MACC system concerns forecasting special events with high-pollution concentrations. Such events receive extra attention in the validation process. Finally, a summary is provided of the results from the validation of the latest set of daily global analysis and forecast products from the MACC system reported in November 2014.

The Monitoring Atmospheric Composition and Climate (MACC) project represents the European Union's Copernicus Atmosphere Monitoring Service (CAMS) (http://www.copernicus.eu/), which became fully operational during 2015. The global near-real-time MACC model production run for aerosol and reactive gases provides daily analyses and 5-day forecasts of atmospheric composition fields. It is the only assimilation system worldwide that is operational to produce global analyses and forecasts of reactive gases and aerosol fields. We have investigated the ability of the MACC analysis system to simulate tropospheric concentrations of reactive gases covering the period between 2009 and 2012. A validation was performed based on carbon monoxide (CO), nitrogen dioxide (NO2) and ozone (O3) surface observations from the Global Atmosphere Watch (GAW) network, the O3 surface observations from the European Monitoring and Evaluation Programme (EMEP) and, furthermore, NO2 tropospheric columns, as well as CO total columns, derived from satellite sensors. The MACC system proved capable of reproducing reactive gas concentrations with consistent quality; however, with a seasonally dependent bias compared to surface and satellite observations – for northern hemispheric surface O3 mixing ratios, positive biases appear during the warm seasons and negative biases during the cold parts of the year, with monthly modified normalised mean biases (MNMBs) ranging between −30 and 30 % at the surface. Model biases are likely to result from difficulties in the simulation of vertical mixing at night and deficiencies in the model's dry deposition parameterisation. Observed tropospheric columns of NO2 and CO could be reproduced correctly during the warm seasons, but are mostly underestimated by the model during the cold seasons, when anthropogenic emissions are at their highest level, especially over the US, Europe and Asia. Monthly MNMBs of the satellite data evaluation range from values between −110 and 40 % for NO2 and at most −20 % for CO, over the investigated regions. The underestimation is likely to result from a combination of errors concerning the dry deposition parameterisation and certain limitations in the current emission inventories, together with an insufficiently established seasonality in the emissions.

Beddows, D. C. S. ... et. al.-- 22 pages, 11 figures, 1 table, supplementary material related to this article is available online at http://www.atmos-chem-phys.net/14/4327/2014/acp-14-4327-2014-supplement.pdf, Clusteranalysis of particle number size distributions frombackground sites across Europeis presented. This generated a total of nine clusters of particle size distributions which could be further combined into two main groups, namely: a south-to-north category (four clusters) and a west-to-east category (five clusters). The first group was identified as most frequently being detected inside and around northern Germany and neighbouring countries, showing clear evidence of local afternoon nucleation and growth events that could be linked to movement of air masses from south to north arriving ultimately at the Arctic contributing to Arctic haze.The second group of particle size spectra proved to have narrower size distributions and collectively showed a dependence of modal diameter upon the longitude of the site (west to east) at which they were most frequently detected.These clusters indicated regional nucleation (at the coastal sites) growing to larger modes further inland. The apparent growth rate of the modal diameter was around 0.6-0.9 nm h-1. Four specific air mass back-trajectories were successively taken as case studies to examine in real time the evolution of aerosol size distributions across Europe. While aerosol growth processes can be observed as aerosol traverses Europe, the processes are often obscured by the addition of aerosol by emissions en route. This study revealed that some of the 24 stations exhibit more complex behaviour than others, especially when impacted by local sources or a variety of different air masses. Overall, the aerosol size distribution clustering analysis greatly simplifies the complex data set and allows a description of aerosol aging processes, which reflects the longer-term average development of particle number size distributions as air masses advect across Europe. © 2014 Author(s), The National Centre for Atmospheric Science is funded by the UK Natural Environment Research Council. This work was also supported by the European Union EUCAARI (Contract Ref. 036833) and EUSAAR (Contract Ref. 026140) research projects

An analysis of mountain polar stratospheric cloud observations by solar absorption FTIR from Kiruna/Sweden was performed and compared with co-located airborne lidar measurements. The infrared cloud spectral signature and optical depth indicated water ice particles compatible with the high backscatter and depolarization ratio of the lidar signal. Retrieval of mean particle properties from the FTIR spectrum depend on the assumed width of the particle size distribution and range from 2.0 to 1.1 µm radius and from 1.9 to 5.1 cm−3 number density. The volume density is well determined with 63.8–60.2 µm³/cm³ equivalent to about 2.5 ppmv of condensed water at 20 hPa. Simulations of lidar backscatter ratio based on these results are consistent with the lidar observations.

We have analysed the trends of total aerosol particle number concentrations (N) measured at long-term measurement stations involved either in the Global Atmosphere Watch (GAW) and/or EU infrastructure project ACTRIS. The sites are located in Europe, North America, Antarctica, and on Pacific Ocean islands. The majority of the sites showed clear decreasing trends both in the full-length time series, and in the intra-site comparison period of 2001–2010, especially during the winter months. Several potential driving processes for the observed trends were studied, and even though there are some similarities between N trends and air temperature changes, the most likely cause of many northern hemisphere trends was found to be decreases in the anthropogenic emissions of primary particles, SO2 or some co-emitted species. We could not find a consistent agreement between the trends of N and particle optical properties in the few stations with long time series of all of these properties. The trends of N and the proxies for cloud condensation nuclei (CCN) were generally consistent in the few European stations where the measurements were available. This work provides a useful comparison analysis for modelling studies of trends in aerosol number concentrations.

It is important to understand the relative contribution of primary and secondary particles to regional and global aerosol so that models can attribute aerosol radiative forcing to different sources. In large-scale models, there is considerable uncertainty associated with treatments of particle formation (nucleation) in the boundary layer (BL) and in the size distribution of emitted primary particles, leading to uncertainties in predicted cloud condensation nuclei (CCN) concentrations. Here we quantify how primary particle emissions and secondary particle formation influence size-resolved particle number concentrations in the BL using a global aerosol microphysics model and aircraft and ground site observations made during the May 2008 campaign of the European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI). We tested four different parameterisations for BL nucleation and two assumptions for the emission size distribution of anthropogenic and wildfire carbonaceous particles. When we emit carbonaceous particles at small sizes (as recommended by the Aerosol Intercomparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with diameter >50 nm (N50) and >100 nm (N100) were well captured by the model (R2≥0.8) and the normalised mean bias (NMB) was also small (−18% for N50 and −1% for N100). Emission of carbonaceous particles at larger sizes, which we consider to be more realistic for low spatial resolution global models, results in equally good correlation but larger bias (R2≥0.8, NMB = −52% and −29%), which could be partly but not entirely compensated by BL nucleation. Within the uncertainty of the observations and accounting for the uncertainty in the size of emitted primary particles, BL nucleation makes a statistically significant contribution to CCN-sized particles at less than a quarter of the ground sites. Our results show that a major source of uncertainty in CCN-sized particles in polluted European air is the emitted size of primary carbonaceous particles. New information is required not just from direct observations, but also to determine the "effective emission size" and composition of primary particles appropriate for different resolution models., JRC.H.2-Air and Climate

Two years of harmonized aerosol number size distribution data from 24 European field monitoring sites have been analysed. The results give a comprehensive overview of the European near surface aerosol particle number concentrations and number size distributions between 30 and 500 nm of dry particle diameter. Spatial and temporal distribution of aerosols in the particle sizes most important for climate applications are presented. We also analyse the annual, weekly and diurnal cycles of the aerosol number concentrations, provide log-normal fitting parameters for median number size distributions, and give guidance notes for data users. Emphasis is placed on the usability of results within the aerosol modelling community. We also show that the aerosol number concentrations of Aitken and accumulation mode particles (with 100 nm dry diameter as a cut-off between modes) are related, although there is significant variation in the ratios of the modal number concentrations. Different aerosol and station types are distinguished from this data and this methodology has potential for further categorization of stations aerosol number size distribution types. The European submicron aerosol was divided into characteristic types: Central European aerosol, characterized by single mode median size distributions, unimodal number concentration histograms and low variability in CCN-sized aerosol number concentrations; Nordic aerosol with low number concentrations, although showing pronounced seasonal variation of especially Aitken mode particles; Mountain sites (altitude over 1000 m a.s.l.) with a strong seasonal cycle in aerosol number concentrations, high variability, and very low median number concentrations. Southern and Western European regions had fewer stations, which decreases the regional coverage of these results. Aerosol number concentrations over the Britain and Ireland had very high variance and there are indications of mixed air masses from several source regions; the Mediterranean aerosol exhibit high seasonality, and a strong accumulation mode in the summer. The greatest concentrations were observed at the Ispra station in Northern Italy with high accumulation mode number concentrations in the winter. The aerosol number concentrations at the Arctic station Zeppelin in Ny-AA lesund in Svalbard have also a strong seasonal cycle, with greater concentrations of accumulation mode particles in winter, and dominating summer Aitken mode indicating more recently formed particles. Observed particles did not show any statistically significant regional work-week or weekday related variation in number concentrations studied. Analysis products are made for open-access to the research community, available in a freely accessible internet site. The results give to the modelling community a reliable, easy-to-use and freely available comparison dataset of aerosol size distributions.

A near real-time system for assimilation and forecasts of aerosols, greenhouse and trace gases, extending the ECMWF Integrated Forecasting System (IFS), has been developed in the framework of the Global and regional Earth-system Monitoring using Satellite and in-situ data (GEMS) project. The GEMS aerosol modeling system is novel as it is the first aerosol model fully coupled to a numerical weather prediction model with data assimilation. A reanalysis of the period 2003-2009 has been carried out with the same system. During its development phase, the aerosol system was first run for the time period January 2003 to December 2004 and included sea salt, desert dust, organic matter, black carbon, and sulfate aerosols. In the analysis, Moderate Resolution Imaging Spectroradiometer (MODIS) total aerosol optical depth (AOD) at 550 nm over ocean and land (except over bright surfaces) was assimilated. This work evaluates the performance of the aerosol system by means of case studies. The case studies include (1) the summer heat wave in Europe in August 2003, characterized by forest fire aerosol and conditions of high temperatures and stagnation, favoring photochemistry and secondary aerosol formation, (2) a large Saharan dust event in March 2004, and (3) periods of high and low sea salt aerosol production. During the heat wave period in 2003, the linear correlation coefficients between modeled and observed AOD (550 nm) and between modeled and observed PM2.5 mass concentrations are 0.82 and 0.71, respectively, for all investigated sites together. The AOD is slightly and the PM2.5 mass concentration is clearly overestimated by the aerosol model during this period. The simulated sulfate mass concentration is significantly correlated with observations but is distinctly overestimated. The horizontal and vertical locations of the main features of the aerosol distribution during the Saharan dust outbreak are generally well captured, as well as the timing of the AOD peaks. The aerosol model simulates winter sea salt AOD reasonably well, however, showing a general overestimation. Summer sea salt events show a better agreement. Overall, the assimilation of MODIS AOD data improves the subsequent aerosol predictions when compared with observations, in particular concerning the correlation and AOD peak values. The assimilation is less effective in correcting a positive (PM2.5, sulfate mass concentration, Angstrm exponent) or negative (desert dust plume AOD) model bias. Copyright 2011 by the American Geophysical Union.

The spatial structure and the progression speed of the first ash layer from the Icelandic Eyjafjallajökull volcano which reached Germany on 16/17 April is investigated from remote sensing data and numerical simulations. The ceilometer network of the German Meteorological Service was able to follow the progression of the ash layer over the whole of Germany. This first ash layer turned out to be a rather shallow layer of only several hundreds of metres thickness which was oriented slantwise in the middle troposphere and which was brought downward by large-scale sinking motion over Southern Germany and the Alps. Special Raman lidar measurements, trajectory analyses and in-situ observations from mountain observatories helped to confirm the volcanic origin of the detected aerosol layer. Ultralight aircraft measurements permitted the detection of the arrival of a second major flush of volcanic material in Southern Germany. Numerical simulations with the Eulerian meso-scale model MCCM were able to reproduce the temporal and spatial structure of the ash layer. Comparisons of the model results with the ceilometer network data on 17 April and with the ultralight aircraft data on 19 April were satisfying. This is the first example of a model validation study from this ceilometer network data.

A near real-time assimilation and forecast system of aerosols has been developed by integration in the ECMWF IFS code within the GEMS project. The GEMS aerosol modeling system is novel as it is the first aerosol model fully coupled to a NWP model with data assimilation. Aerosol optical depth (AOD) data of the MODIS instrument on Terra and Aqua satellites was assimilated. The performance of the aerosol model was evaluated by the means of case studies. The assimilation of MODIS AOD improved the subsequent aerosol predictions when compared with observations, in particular concerning correlations and AOD peak values. The assimilation is less effective in correcting a positive or a negative bias.

The German Meteorological Service (DWD) operates about 52 lidar ceilometers within its synoptic observations network, covering Germany. These affordable low-power lidar systems provide spatially and temporally high resolved aerosol backscatter profiles which can operationally provide quasi 3-D distributions of particle backscatter intensity. Intentionally designed for cloud height detection, recent significant improvements allow following the development of the boundary layer and to detect denser particle plumes in the free tropospere like volcanic ash, Saharan dust or fire smoke. Thus the network builds a powerful aerosol plume alerting and tracking system. If auxiliary aerosol information is available, the particle backscatter coefficient, the extinction coefficient and even particle mass concentrations may be estimated, with however large uncertainties. Therefore, large synergistic benefit is achieved if the ceilometers are linked to existing lidar networks like EARLINET or integrated into WMO's envisioined Global Aerosol Lidar Observation Network GALION. To this end, we demonstrate the potential and limitations of ceilometer networks by means of three representative aerosol episodes over Europe, namely Sahara dust, Mediterranean fire smoke and, more detailed, the Icelandic Eyjafjoll volcano eruption from mid April 2010 onwards. The DWD (Jenoptik CHM15k) lidar ceilometer network tracked the Eyjafjoll ash layers over Germany and roughly estimated peak extinction coefficients and mass concentrations on 17 April of 4–6(± 2) 10-4 m−1 and 500–750(± 300) μg/m−3, respectively, based on co-located aerosol optical depth, nephelometer (scattering coefficient) and particle mass concentration measurements. Though large, the uncertainties are small enough to let the network suit for example as aviation advisory tool, indicating whether the legal flight ban threshold of presently 2 mg/m3 is imminent to be exceeded.

This paper synthesizes data on aerosol (particulate matter, PM) physical and chemical characteristics, which were obtained over the past decade in aerosol research and monitoring activities at more than 60 natural background, rural, near-city, urban, and kerbside sites across Europe. The data include simultaneously measured PM10 and/or PM2.5 mass on the one hand, and aerosol particle number concentrations or PM chemistry on the other hand. The aerosol data presented in our previous works (Van Dingenen et al., 2004; Putaud et al., 2004) were updated and merged to those collected in the framework of the EU supported European Cooperation in the field of Scientific and Technical action COST633 (Particulate matter: Properties related to health effects). A number of conclusions from our previous studies were confirmed. There is no single ratio between PM2.5 and PM10 mass concentrations valid for all sites, although fairly constant ratios ranging from 0.5 to 0.9 are observed at most individual sites. There is no general correlation between PM mass and particle number concentrations, although particle number concentrations increase with PM2.5 levels at most sites. The main constituents of both PM10 and PM2.5 are generally organic matter, sulfate and nitrate. Mineral dust can also be a major constituent of PM10 at kerbside sites and in Southern Europe. There is a clear decreasing gradient in SO4 2- and NO3 - contribution to PM10 when moving from rural to urban to kerbside sites. In contrast, the total carbon/PM10 ratio increases from rural to kerbside sites. Some new conclusions were also drawn from this work: the ratio between ultrafine particle and total particle number concentration decreases with PM2.5 concentration at all sites but one, and significant gradients in PM chemistry are observed when moving from Northwestern, to Southern to Central Europe. Compiling an even larger number of data sets would have further increased the significance of our conclusions, but collecting all the aerosol data sets obtained also through research projects remains a tedious task. © 2009 Elsevier Ltd. All rights reserved., This paper is a contribution to the COST Action 633 “Particulate matter: Properties related to health effects”.

The aerosol light absorption coefficient is an essential parameter involved in atmospheric radiation budget calculations. The Aethalometer (AE) has the great advantage of measuring the aerosol light absorption coefficient at several wavelengths, but the derived absorption coefficients are systematically too high when compared to reference methods. Up to now, four different correction algorithms of the AE absorption coefficients have been proposed by several authors. A new correction scheme based on these previously published methods has been developed, which accounts for the optical properties of the aerosol particles embedded in the filter. All the corrections have been tested on six datasets representing different aerosol types and loadings and include multi-wavelength AE and white-light AE. All the corrections have also been evaluated through comparison with a Multi-Angle Absorption Photometer (MAAP) for four datasets lasting between 6 months and five years. The modification of the wavelength dependence by the different corrections is analyzed in detail. The performances and the limits of all AE corrections are determined and recommendations are given.

[1] This study presents the new aerosol assimilation system, developed at the European Centre for Medium-Range Weather Forecasts, for the Global and regional Earth-system Monitoring using Satellite and in-situ data (GEMS) project. The aerosol modeling and analysis system is fully integrated in the operational four-dimensional assimilation apparatus. Its purpose is to produce aerosol forecasts and reanalyses of aerosol fields using optical depth data from satellite sensors. This paper is the second of a series which describes the GEMS aerosol effort. It focuses on the theoretical architecture and practical implementation of the aerosol assimilation system. It also provides a discussion of the background errors and observations errors for the aerosol fields, and presents a subset of results from the 2-year reanalysis which has been run for 2003 and 2004 using data from the Moderate Resolution Imaging Spectroradiometer on the Aqua and Terra satellites. Independent data sets are used to show that despite some compromises that have been made for feasibility reasons in regards to the choice of control variable and error characteristics, the analysis is very skillful in drawing to the observations and in improving the forecasts of aerosol optical depth.

The implementation and application of a newly developed coupled system combining ECMWF's integrated forecast system (IFS) with global chemical transport models (CTMs) is presented. The main objective of the coupled system is to enable the IFS to simulate key chemical species without the necessity to invert the complex source and sink processes such as chemical reactions, emission and deposition. Thus satellite observations of atmospheric composition can be assimilated into the IFS using its 4D-VAR algorithm. In the coupled system, the IFS simulates only the transport of chemical species. The coupled CTM provides to the IFS the concentration tendencies due to emission injection, deposition and chemical conversion. The CTMs maintain their own transport schemes and are fed with meteorological data at hourly resolution from the IFS. The CTM used in the coupled system can be either MOZART-3, TM5 or MOCAGE. The coupling is achieved via the special-purpose OASIS4 software. The scientific integrity of the coupled system is proven by analysing the difference between stand-alone CTM simulations and the tracer fields in the coupled IFS. The IFS concentration fields match the CTM fields for about 48 h with the biggest differences occurring in the planetary boundary layer (PBL). The coupled system is a good test bed for process-oriented comparison of the coupled CTM. As an example, the vertical structure of chemical conversion and emission injection is studied for a ten day period over Central Europe for the three CTMs.

Lidar standards are needed to ensure quality and lidar product control at the interface between lidar manufacturers and lidar users. Meanwhile three lidar standards have been published by German and international standardization organizations. This paper describes the cooperation between the lidar technique inventors, lidar instrument constructors, and lidar product users to establish useful standards. Presently a backscatter lidar standard is elaborated in Germany. Key points of this standard are presented here. Two German standards were already accepted as international standards by the International Organization for Standardization (ISO). Hence, German and international organizations for the establishment of lidar standards are introduced to encourage a cooperative work on lidar standards by lidar scientists.

The results of a multimodel forecasting effort to predict mountain wave–induced polar stratospheric clouds (PSCs) for airborne science during the third Stratospheric Aerosol and Gas Experiment (SAGE III) Ozone Loss and Validation Experiment (SOLVE)/Third European Stratospheric Experiment on Ozone (THESEO 2000) Arctic ozone campaign are assessed. The focus is on forecasts for five flights of NASA's instrumented DC-8 research aircraft in which PSCs observed by onboard aerosol lidars were identified as wave related. Aircraft PSC measurements over northern Scandinavia on 25–27 January 2000 were accurately forecast by the mountain wave models several days in advance, permitting coordinated quasi-Lagrangian flights that measured their composition and structure in unprecedented detail. On 23 January 2000 mountain wave ice PSCs were forecast over eastern Greenland. Thick layers of wave-induced ice PSC were measured by DC-8 aerosol lidars in regions along the flight track where the forecasts predicted enhanced stratospheric mountain wave amplitudes. The data from these flights, which were planned using this forecast guidance, have substantially improved the overall understanding of PSC microphysics within mountain waves. Observations of PSCs south of the DC-8 flight track on 30 November 1999 are consistent with forecasts of mountain wave–induced ice clouds over southern Scandinavia, and are validated locally using radiosonde data. On the remaining two flights wavelike PSCs were reported in regions where no mountain wave PSCs were forecast. For 10 December 1999, it is shown that locally generated mountain waves could not have propagated into the stratosphere where the PSCs were observed, confirming conclusions of other recent studies. For the PSC observed on 14 January 2000 over northern Greenland, recent work indicates that nonorographic gravity waves radiated from the jet stream produced this PSC, confirming the original forecast of no mountain wave influence. This forecast is validated further by comparing with a nearby ER-2 flight segment to the south of the DC-8, which intercepted and measured local stratospheric mountain waves with properties similar to those predicted. In total, the original forecast guidance proves to be consistent with PSC data acquired from all five of these DC-8 flights. The work discussed herein highlights areas where improvements can be made in future wave PSC forecasting campaigns, such as use of anelastic rather than Boussinesq linearized gridpoint models and a need to forecast stratospheric gravity waves from sources other than mountains.

[1] Airborne differential absorption lidar (DIAL) measurements of tropospheric water vapor and aerosol/clouds are presented from transfers across the North Atlantic on 13–15 May and 16–18 June 2002. The intense dynamical activity over the Atlantic is reflected in complex structures like deep tropopause folds, extended dry layers, and tilted aerosol filaments. Intrusions with H2O mixing ratios below 0.03 g kg−1 regularly develop along the storm track over intense cyclones and correspond to analyzed (European Centre for Medium-Range Weather Forecasts (ECMWF)) or simulated (MM5) potential vorticity anomalies. Sloping folds are typically 1 km thick in vertical profiles but on horizontal sections resemble long filaments with widths of a few hundred kilometers. Filaments of solid, roughly micron-sized particles occur inside and along the axes of the tropopause folds. The particles most likely originate in forest fires, from where they are injected to the lower stratosphere by deep convection and later on reenter the troposphere in developing baroclinic disturbances. Their laminar appearance indicates that these intrusions have not yet been mixed but are eroded on timescales significantly larger than a few days by stretching-thinning, stirring, and only finally, turbulent diffusion. MM5 mesoscale model simulations and, with less accuracy, also ECMWF analyses are capable of reproducing the dynamical structures associated with the observed dry intrusions. However, deep inside the intrusions where scales are small, even the MM5-simulated water vapor mixing ratios are more than twice those observed. The large dynamical range of water vapor mixing ratios (3 orders of magnitude) and large gradients (>2 g kg−1 km−1 at the intrusions' boundaries) constitute a challenge for future space-borne water vapor DIAL systems.

International audience; For the first time three different remote sensing instruments ? a sub-millimeter radiometer, a differential optical absorption spectrometer in the UV-visible spectral range, and a lidar ? were deployed aboard DLR's meteorological research aircraft Falcon 20 to validate a large number of SCIAMACHY level 2 and off-line data products such as O3, NO2, N2O, BrO, OClO, H2O, aerosols, and clouds. Within two validation campaigns of the SCIA-VALUE mission (SCIAMACHY VALidation and Utilization Experiment) extended latitudinal cross-sections stretching from polar regions to the tropics as well as longitudinal cross sections at polar latitudes at about 70° N and the equator were generated. This contribution gives an overview over the campaigns performed and reports on the observation strategy for achieving the validation goals. We also emphasize the synergetic use of the novel set of aircraft instrumentation and the usefulness of this innovative suite of remote sensing instruments for satellite validation.

For the first time three different remote sensing instruments – a sub-millimeter radiometer, a differential optical absorption spectrometer in the UV-visible spectral range, and a lidar – were deployed aboard DLR's meteorological research aircraft Falcon 20 to validate a large number of SCIAMACHY level 2 and off-line data products such as O3, NO2, N2O, BrO, OClO, H2O, aerosols, and clouds. Within two main validation campaigns of the SCIA-VALUE mission (SCIAMACHY VALidation and Utilization Experiment) extended latitudinal cross-sections stretching from polar regions to the tropics as well as longitudinal cross sections at polar latitudes at about 70° N and the equator have been generated. This contribution gives an overview over the campaigns performed and reports on the observation strategy for achieving the validation goals. We also emphasize the synergetic use of the novel set of aircraft instrumentation and the usefulness of this innovative suite of remote sensing instruments for satellite validation.