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The first three Arctic winters of the ACE mission represented two extremes of winter variability: Stratospheric sudden warmings (SSWs) in 2004 and 2006 were among the strongest, most prolonged on record; 2005 was a record cold winter. Canadian Arctic Atmospheric Chemistry Experiment (ACE) Validation Campaigns were conducted at Eureka (80° N, 86° W) during each of these winters. New satellite measurements from ACE-Fourier Transform Spectrometer (ACE-FTS), Sounding of the Atmosphere using Broadband Emission Radiometry (SABER), and Aura Microwave Limb Sounder (MLS), along with meteorological analyses and Eureka lidar temperatures, are used to detail the meteorology in these winters, to demonstrate its influence on transport, and to provide a context for interpretation of ACE-FTS and validation campaign observations. During the 2004 and 2006 SSWs, the vortex broke down throughout the stratosphere, reformed quickly in the upper stratosphere, and remained weak in the middle and lower stratosphere. The stratopause reformed at very high altitude, near 75 km. ACE measurements covered both vortex and extra-vortex conditions in each winter, except in late-February through mid-March 2004 and 2006, when the strong, pole-centered vortex that reformed after the SSWs resulted in ACE sampling only inside the vortex in the middle through upper stratosphere. The 2004 and 2006 Eureka campaigns were during the recovery from the SSWs, with the redeveloping vortex over Eureka. 2005 was the coldest winter on record in the lower stratosphere, but with an early final warming in mid-March. The vortex was over Eureka at the start of the 2005 campaign, but moved away as it broke up. Disparate temperature profile structure and vortex evolution resulted in much lower (higher) temperatures in the upper (lower) stratosphere in 2004 and 2006 than in 2005. Satellite temperatures agree well with lidar data up to 50–60 km, and ACE-FTS, MLS and SABER show good agreement in high-latitude temperatures throughout the winters. Consistent with a strong, cold upper stratospheric vortex and enhanced radiative cooling after the SSWs, MLS and ACE-FTS trace gas measurements show strongly enhanced descent in the upper stratospheric vortex in late January through March 2006 compared to that in 2005.
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Global water vapour total column amounts have been retrieved from spectral data provided by the Global Ozone Monitoring Experiment (GOME) flying on ERS-2, which was launched in April 1995, and the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) onboard ENVISAT launched in March 2002. For this purpose the Air Mass Corrected Differential Optical Absorption Spectroscopy (AMC-DOAS) approach has been used. The combination of the data from both instruments provides us with a long-term global data set spanning more than 11 years with the potential of extension up to 2020 by GOME-2 data on MetOp. <br><br> Using linear and non-linear methods from time series analysis and standard statistics the trends of H<sub>2</sub>O columns and their errors have been calculated. In this study, factors affecting the trend such as the length of the time series, the magnitude of the variability of the noise, and the autocorrelation of the noise are investigated. Special emphasis has been placed on the calculation of the statistical significance of the observed trends, which reveal significant local changes from −5% per year to +5% per year. These significant trends are distributed over the whole globe. Increasing trends have been calculated for Greenland, East Europe, Siberia and Oceania, whereas decreasing trends have been observed for the northwest USA, Central America, Amazonia, Central Africa and the Arabian Peninsular.
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The spatial-temporal distributions and sources of sand and dust storm (SDS) in East Asia from 2001 to 2006 were investigated on the basis of visibility and PM<sub>10</sub> data from the routine SDS and weather monitoring networks run by CMA (China Meteorological Administration). A power functional relationships between PM<sub>10</sub> and visibility was found among various regions generally with a good correlation (r<sup>2</sup>=0.90), especially in Asian SDS source regions. In addition, three SDS occurrence centers, i.e. western China, Mongolia and northern China, were identified with the Mongolia source contributing more dust to the downwind areas including Korea and Japan than other two sources. Generally, high PM<sub>10</sub> concentrations were observed in most areas of northern China. The highest value was obtained in the center of western China with a spring daily mean value of 876 μgm<sup>−3</sup>, and the value in other source regions exceeds 200 μgm<sup>−3</sup>. These data sets together with the satellite observations in China form the main observation database for the evaluation and data assimilation of CUACE/Dust system – an operational SDS forecasting system for East Asia.
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The increased resolution of numerical weather prediction models allows nowadays addressing more realistically urban meteorology and air pollution processes. This has triggered new interest in modelling and describing experimentally the specific features and processes of urban areas. Recent developments and results performed within the EU-funded project FUMAPEX on integrated systems for forecasting urban meteorology and air pollution are reported here. Sensitivity studies with respect to optimum resolution, parametrisation of urban roughness and surface exchange fluxes and the role of urban soil layers are carried out with advanced meso- or sub-meso meteorological models. They show that sensible improvements can be achieved by higher model resolution that is accompanied with better description of urban surface features. Recommendations, especially with respect to advanced urban air quality forecasting and information systems, are given together with an assessment of the needed further research and data.
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The Leipzig Aerosol Cloud Interaction Simulator (LACIS) was used to investigate the hygroscopic growth and activation of sea-salt particles which were generated from three different sea-water samples. The measurements showed that the sea-salt particles exhibit a slightly reduced hygroscopic growth compared to pure NaCl particles. Köhler theory was utilized to model the hygroscopic growth of these particles. Some parameters used in this model are unknown for sea-salt. These parameters are combined in an "ionic density" ρ<sub>ion</sub>. For each sea-salt sample an average ρ<sub>ion</sub> was determined by fitting the Köhler equation to the data from the hygroscopic growth measurements. LACIS was also used to measure the activation of the sea-salt particles at three different supersaturations: 0.11%, 0.17% and 0.32%. A CCN-closure was tested by calculating the critical diameters D<sub>crit</sub> for the sea-salt particles at these supersaturations, using the Köhler model and the corresponding ρ<sub>ion</sub> as derived from the hygroscopic growth data. These calculated critical diameters were compared to the measured ones. Measured and calculated values of D<sub>crit</sub> agree within the level of uncertainty. Based on this successful closure, a new parameterization to describe sea-salt-particle hygroscopic growth (at RH>95%) and activation has been developed.
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Most estimates of sea spray aerosol source functions have used indirect means to infer the rate of production as a function of wind speed. Only recently has the technology become available to make high frequency measurements of aerosol spectra suitable for direct eddy correlation determination of the sea spray particle flux. This was accomplished in this study by combining a newly developed fast aerosol particle counter with an ultrasonic anemometer which allowed for eddy covariance measurements of size-segregated particle fluxes. The aerosol instrument is the Compact Lightweight Aerosol Spectrometer Probe (CLASP) – capable of measuring 8-channel size spectra for mean radii between 0.15 and 3.5 µm at 10 Hz. The first successful measurements were made during the Waves, Air Sea Fluxes, Aerosol and Bubbles (WASFAB) field campaign in October 2005 in Duck (NC, USA). The method and initial results are presented and comparisons are made with recent sea spray source functions from the literature.
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The Match method for the quantification of polar chemical ozone loss is investigated mainly with respect to the impact of the transport of air masses across the vortex edge. For the winter 2002/03, we show that significant transport across the vortex edge occurred and was simulated by the Chemical Lagrangian Model of the Stratosphere. In-situ observations of inert tracers and ozone from HAGAR on the Geophysica aircraft and balloon-borne sondes, and remote observations from MIPAS on the ENVISAT satellite were reproduced well by CLaMS. The model even reproduced a small vortex remnant that remained a distinct feature until June 2003 and was also observed in-situ by a balloon-borne whole air sampler. We use this CLaMS simulation to quantify the impact of transport across the vortex edge on ozone loss estimates from the Match method. We show that a time integration of the determined vortex average ozone loss rates, as performed in Match, results in a larger ozone loss than the polar vortex average ozone loss in CLaMS. The determination of the Match ozone loss rates is also influenced by the transport of air across the vortex edge. We use the model to investigate how the sampling of the ozone sondes on which Match is based represents the vortex average ozone loss rate. Both the time integration of ozone loss and the determination of ozone loss rates for Match are evaluated using the winter 2002/2003 CLaMS simulation. These impacts can explain the majority of the differences between CLaMS and Match column ozone loss. While the investigated effects somewhat reduce the apparent discrepancy in January ozone loss rates reported earlier, a distinct discrepancy between simulations and Match remains. However, its contribution to the accumulated ozone loss over the winter is not large.
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Imperfect representation of vertical mixing near the surface in atmospheric transport models leads to uncertainties in modelled tracer mixing ratios. When using the atmosphere as an integrator to derive surface-atmosphere exchange from mixing ratio observations made in the atmospheric boundary layer, this uncertainty has to be quantified and taken into account. A comparison between radiosonde-derived mixing heights and mixing heights derived from ECMWF meteorological data during May–June 2005 in Europe revealed random discrepancies of about 40% for the daytime with insignificant bias errors, and much larger values approaching 100% for nocturnal mixing layers with bias errors also exceeding 50%. The Stochastic Time Inverted Lagrangian Transport (STILT) model was used to propagate this uncertainty into CO<sub>2</sub> mixing ratio uncertainties, accounting for spatial and temporal error covariance. Average values of 3 ppm were found for the 2 month period, indicating that this represents a large fraction of the overall uncertainty. A pseudo data experiment shows that the error propagation with STILT avoids biases in flux retrievals when applied in inversions. The results indicate that flux inversions employing transport models based on current generation meteorological products have misrepresented an important part of the model error structure likely leading to biases in the estimated mean and uncertainties. We strongly recommend including the solution presented in this work: better, higher resolution atmospheric models, a proper description of correlated random errors, and a modification of the overall sampling strategy.
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Detailed investigations of the chemical and microphysical properties of rural continental aerosols were performed during the HAZE2002 experiment, which was conducted in May 2002 at the Meteorological Observatory Hohenpeissenberg (DWD) in Southern Germany. <br><br> Online measurements included: Size-resolved chemical composition of submicron particles; total particle number concentrations and size distributions over the diameter range of 3 nm to 9 μm; gas-phase concentration of monoterpenes, CO, O<sub>3</sub>, OH, and H<sub>2</sub>SO<sub>4</sub>. Filter sampling and offline analytical techniques were used to determine: Fine particle mass (PM2.5), organic, elemental and total carbon in PM2.5 (OC2.5, EC2.5, TC2.5), and selected organic compounds (dicarboxylic acids, polycyclic aromatic hydrocarbons, proteins). <br><br> Overall, the non-refractory components of submicron particles detected by aerosol mass spectrometry (PM1, 6.6±5.4 μg m<sup>−3</sup>, arithmetic mean and standard deviation) accounted for ~62% of PM2.5 determined by filter gravimetry (10.6±4.7 μg m<sup>−3</sup>). The relative proportions of non-refractory submicron particle components were: (23±39)% ammonium nitrate, (27±23)% ammonium sulfate, and (50±40)% organics (OM1). OM1 was closely correlated with PM1 (<i>r</i><sup>2</sup>=0.9) indicating a near-constant ratio of non-refractory organics and inorganics. <br><br> The average ratio of OM1 to OC2.5 was 2.1±1.4, indicating a high proportion of heteroelements in the organic fraction of the sampled rural aerosol. This is consistent with the high ratio of oxygenated organic aerosol (OOA) over hydrocarbon-like organic aerosol (HOA) inferred from the AMS results (4:1), and also with the high abundance of proteins (~3%) indicating a high proportion of primary biological material (~30%) in PM2.5. This finding was confirmed by low abundance of PAHs (<1 ng m<sup>−3</sup>) and EC (<1 μg m<sup>−3</sup>) in PM2.5 and detection of several secondary organic aerosol compounds (dicarboxylic acids) and their precursors (monoterpenes). <br><br> New particle formation was observed almost every day with particle number concentrations exceeding 10<sup>4</sup> cm<sup>−3</sup> (nighttime background level 1000–2000 cm<sup>−3</sup>). Closer inspection of two major events indicated that the observed nucleation agrees with ternary H<sub>2</sub>SO<sub>4</sub>/H<sub>2</sub>O/NH<sub>3</sub> nucleation and that condensation of both organic and inorganic species contributed to particle growth.
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A new method is proposed to estimate the spatial and temporal variability of the solar radiative flux reaching the surface over land (DSSF), as well as the Aerosol Radiative Forcing (ARF), in cloud-free atmosphere. The objective of regional applications of the method is attainable by using the visible broadband of METEOSAT-7 satellite instrument which scans Europe and Africa on a half-hourly basis. The method relies on a selection of best correspondence between METEOSAT-7 radiance and radiative transfer computations. <br><br> The validation of DSSF is performed comparing retrievals with ground-based measurements acquired in two contrasted environments: an urban site near Paris and a continental background site located South East of France. The study is concentrated on aerosol episodes occurring around the 2003 summer heat wave, providing 42 cases of comparison for variable solar zenith angle (from 59° to 69°), variable aerosol type (biomass burning emissions and urban pollution), and variable aerosol optical thickness (a factor 6 in magnitude). The method reproduces measurements of DSSF within an accuracy assessment of 20 W m<sup>−2</sup> (5% in relative) in 70% of the situations, and within 40 W m<sup>−2</sup> in 90% of the situations, for the two case studies considered here. <br><br> Considering aerosol is the main contributor in changing the measured radiance at the top of the atmosphere, DSSF temporal variability is assumed to be caused only by aerosols, and consequently ARF at ground level and over land is also retrieved: ARF is computed as the difference between DSSF and a parameterised aerosol-free reference level. Retrievals are linearly correlated with the ground-based measurements of the aerosol optical thickness (AOT): sensitivity is included between 120 and 160 W m<sup>−2</sup> per unity of AOT at 440 nm. AOT being an instantaneous measure indicative of the aerosol columnar amount, we prove the feasibility to infer instantaneous aerosol radiative impact at the ground level over land with METEOSAT-7 visible channel.
