[1] This paper provides a review of stratosphere-troposphere exchange (STE), with a focus on processes in the extratropics. It also addresses the relevance of STE for tropospheric chemistry, particularly its influence on the oxidative capacity of the troposphere. After summarizing the current state of knowledge, the objectives of the project Influence of Stratosphere-Troposphere Exchange in a Changing Climate on Atmospheric Transport and Oxidation Capacity (STACCATO), recently funded by the European Union, are outlined. Several papers in this Journal of Geophysical ResearchAtmospheres special section present the results of this project, of which this paper gives an overview. STACCATO developed a new concept of STE in the extratropics, explored the capacities of different types of methods and models to diagnose STE, and identified their various strengths and shortcomings. Extensive measurements were made in central Europe, including the first monitoring over an extended period of time of beryllium-10 ( 10 Be), to provide a suitable database for case studies of stratospheric intrusions and for model validation. Photochemical models were used to examine the impact of STE on tropospheric ozone and the oxidizing capacity of the troposphere. Studies of the present interannual variability of STE and projections into the future were made using reanalysis data and climate models.

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

New estimates of the various contributions to the radiative forcing (RF) from aviation are presented, mainly based on results from the TRADEOFF project that update those of the Intergovernmental Panel on Climate Change (IPCC, 1999). The new estimate of the total RF from aviation for 2000 is approximately the same as that of the IPCC's estimate for 1992. This is mainly a consequence of the strongly reduced RF from contrails, which compensates the increase due to increased traffic from 1992 to 2000. The RF from other aviation-induced cirrus clouds might be as large as the present estimate of the total RF (without cirrus). However, our present knowledge on these aircraft-induced cirrus clouds is too poor to provide a reliable estimate of the associated RF. ZusammenfassungNeue Abschätzungen der einzelnen Beiträge zum Strahlungsantrieb des Luftverkehrs werden vorgestellt, die im Wesentlichen auf Ergebnissen des TRADEOFF-Projektes beruhen und die die IPCC-Abschätzungen (1999) aktualisieren. Der neue Wert für den gesamten Strahlungsantrieb des Luftverkehrs im Jahr 2000 ist in etwa gleich groß wie die IPCCAbschätzung für das Jahr 1992. Das ist im Wesentlichen eine Folge des stark reduzierten Strahlungsantriebes durch Kondensstreifen, wodurch der Anstieg aufgrund der Zunahme des Verkehrs von 1992 bis 2000 kompensiert wird. Der Antrieb durch andere luftverkehrsinduzierte Wolken könnte ebenso groß sein wie die neue Abschätzung für den gesamten Strahlungsantrieb (ohne Zirren). Jedoch ist unser heutiges Wissen über diese luftverkehrsinduzierten Wolken nicht gut genug, um belastbare Aussagen über den damit verbundenen Strahlungsantrieb zu machen. IntroductionMore than 5 years have passed since the publication of the 1999 IPCC Special Report "Aviation and the Global Atmosphere" (Penner et al., 1999 Shine et al., 1990) is considered as a metric of climate change (Fuglestvedt et al., 2003): for many perturbations of species radiatively active in the atmosphere, in particular for well-mixed greenhouse gases, the radiative forcing RF is proportional to the expected equilibrium climate change in terms of global mean surface temperature change ∆T s ,where λ is the climate sensitivity parameter (unit K/(Wm -2 )). The use of equation (1) implicitly assumes that λ is independent of the forcing mechanism. However, it is well documented that λ varies by more than a factor of two among models, reflecting, e.g., different parameterisations implemented (e.g., Cess et al., 1990;Prather et al., 1999). The proportionality in equation (1) forms one of the bases for the Kyoto Protocol and for emissions trading of the gases in the Kyoto "basket", as RF is one of the terms entering the Global Warming Potential (GWP).Recent studies (e.g., Stuber et. al., 2001; Joshi et al., 2003¸Cook andHighwood, 2003) have shown that λ is not constant for a range of perturbations to radiatively active species, in particular if the additional radiatively active species are inhomogeneously distributed, as is the case for aviation-induced ozone changes. Alre...

Recent findings, based on both ground-based and satellite measurements, have established that there has been an apparent downward trend in the total column amount of ozone over mid-latitude areas of the Northern Hemisphere in all seasons. Measurements of the altitude profile of the change in the ozone concentration have established that decreases are taking place in the lower stratosphere in the region of highest ozone concentration. Analysis of updated ozone records, through March of 1991, including 29 stations in the former Soviet Union, and analysis of independently calibrated satellite data records from the Total Ozone Mapping Spectrometer and Stratospheric Aerosol and Gas Experiment instruments confirm many of the findings originally derived from the Dobson record concerning northern midlatitude changes in ozone. The data from many instruments now provide a fairly consistent picture of the change that has occurred in stratospheric ozone levels.

[1] A new data set of high-quality homogenized daily maximum and minimum summer air temperature series from 246 stations in the eastern Mediterranean region (including

[1] Regular aerosol extinction and backscatter measurements using a UV Raman lidar have been performed from January 2001 to December 2004 at Thessaloniki, Greece (40.5°N, 22.9°E), in the framework of the European Aerosol Research Lidar Network (EARLINET). Profiles of the aerosol extinction coefficient, backscatter coefficient, and extinction-to-backscatter ratio (so-called ''lidar ratio'') were acquired under nighttime conditions and have been used for statistical investigations. The statistical analysis was made both for the planetary boundary layer and for the free troposphere. It was found that the 4-year mean boundary layer particle optical depth at 355 nm was 0.44 ± 0.18, and the total aerosol optical depth was 0.63 ± 0.27. Free tropospheric particles account on the average for 30% of the total aerosol optical depth, ranging from 5% (clean free troposphere conditions) to 55% (mainly Saharan dust events). For the cases examined, the integral of the lidar-derived extinction coefficient was in good agreement with colocated aerosol optical depth measurements at 355 nm obtained with a Brewer spectroradiometer. The mean value of the lidar ratio at 355 nm derived, for the period of measurements at Thessaloniki, was 40 sr with a standard deviation of 21 sr. Mean height profiles of the particle lidar ratio, extinction, and backscatter coefficients are shown along with their seasonal dependence, showing a significant seasonal variability in the free troposphere. An analysis of the data using back trajectories showed also a dependence of the aerosol optical depth and the lidar ratio on the origin of the air mass, with higher values mostly corresponding to air masses originating from the northeast Balkans and eastern Europe.Citation: Amiridis, V

Spectral solar UV radiation measurements performed at Thessaloniki, Greece (40øN), are presented, and the influence of various atmospheric constituents such as total ozone, cloud cover, and columnar SO2 on these measurements is examined. By comparing UV radiation measurements at days with different total ozone amounts the magnification factor was calculated. Its values range from I to 20, depending on the wavelength and the total ozone. A relationship between the UV radiation and the cloud cover was established, being representative only for measurements at 50 ø solar zenith angle. In addition, the influence of columnar SO2 variations on UV irradiances was also studied. Finally, an attempt was made to compare the relative influence of these parameters on UV radiation, which proved that total ozone is the major factor controlling the solar UVB radiation received at the ground. ß _.* •.' .4, ß ,. ß ß ß ß ß ß ß ee ß eß ß ß ß ß ß ß ß ß . ß (b) ß ß ß ß ß

Abstract. We present a comparison of tropospheric NO 2 from OMI measurements to the median of an ensemble of Regional Air Quality (RAQ) models, and an intercomparison of the contributing RAQ models and two global models for the period July 2008-June 2009 over Europe. The model forecasts were produced routinely on a daily basis in the context of the European GEMS ("Global and regional Earth-system (atmosphere) Monitoring using Satellite and in-situ data") project. The tropospheric vertical column of the RAQ ensemble median shows a spatial distribution which agrees well with the OMI NO 2 observations, with a correlation r=0.8. This is higher than the correlations from any one of the individual RAQ models, which supports the use of a model ensemble approach for regional air pollution forecasting. The global models show high correlations compared Correspondence to: V. Huijnen (huijnen@knmi.nl) to OMI, but with significantly less spatial detail, due to their coarser resolution. Deviations in the tropospheric NO 2 columns of individual RAQ models from the mean were in the range of 20-34% in winter and 40-62% in summer, suggesting that the RAQ ensemble prediction is relatively more uncertain in the summer months.The ensemble median shows a stronger seasonal cycle of NO 2 columns than OMI, and the ensemble is on average 50% below the OMI observations in summer, whereas in winter the bias is small. On the other hand the ensemble median shows a somewhat weaker seasonal cycle than NO 2 surface observations from the Dutch Air Quality Network, and on average a negative bias of 14%.Full profile information was available for two RAQ models and for the global models. For these models the retrieval averaging kernel was applied. Minor differences are found for area-averaged model columns with and without applying the kernel, which shows that the impact of replacing the a priori profiles by the RAQ model profiles is on average small.Published by Copernicus Publications on behalf of the European Geosciences Union. V. Huijnen et al.:Comparison of NO 2 in regional and global models to OMI However, the contrast between major hotspots and rural areas is stronger for the direct modeled vertical columns than the columns where the averaging kernels are applied, related to a larger relative contribution of the free troposphere and the coarse horizontal resolution in the a priori profiles compared to the RAQ models.In line with validation results reported in the literature, summertime concentrations in the lowermost boundary layer in the a priori profiles from the DOMINO product are significantly larger than the RAQ model concentrations and surface observations over the Netherlands. This affects the profile shape, and contributes to a high bias in OMI tropospheric columns over polluted regions. The global models indicate that the upper troposphere may contribute significantly to the total column and it is important to account for this in comparisons with RAQ models. A combination of upper troposphere model biases, the a priori profile effec...