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Operational retrievals of tropospheric trace gases from space-borne spectrometers are based on one-dimensional radiative transfer models. To minimize cloud effects, trace gas retrievals generally implement a simple cloud model based on radiometric cloud fraction estimates and photon path length corrections. The latter relies on measurements of the oxygen collision pair (O2–O2) absorption at 477 nm or on the oxygen A-band around 760 nm to determine an effective cloud height. In reality however, the impact of clouds is much more complex, involving unresolved sub-pixel clouds, scattering of clouds in neighbouring pixels, and cloud shadow effects, such that unresolved three-dimensional effects due to clouds may introduce significant biases in trace gas retrievals. Although clouds have significant effects on trace gas retrievals, the current cloud correction schemes are based on a simple cloud model, and the retrieved cloud parameters must be interpreted as effective values. Consequently, it is difficult to assess the accuracy of the cloud correction only based on analysis of the accuracy of the cloud retrievals, and this study focuses solely on the impact of the 3D cloud structures on the trace gas retrievals. In order to quantify this impact, we study NO2 as a trace gas example and apply standard retrieval methods including approximate cloud corrections to synthetic data generated by the state-of-the-art three-dimensional Monte Carlo radiative transfer model MYSTIC. A sensitivity study is performed for simulations including a box cloud, and the dependency on various parameters is investigated. The most significant bias is found for cloud shadow effects under polluted conditions. Biases depend strongly on cloud shadow fraction, NO2 profile, cloud optical thickness, solar zenith angle, and surface albedo. Several approaches to correct NO2 retrievals under cloud shadow conditions are explored. We find that air mass factors calculated using fitted surface albedo or corrected using the O2–O2 slant column density can partly mitigate cloud shadow effects. However, these approaches are limited to cloud-free pixels affected by surrounding clouds. A parameterization approach is presented based on relationships derived from the sensitivity study. This allows measurements to be identified for which the standard NO2 retrieval produces a significant bias and therefore provides a way to improve the current data flagging approach.

Three-dimensional (3D) cloud structures may impact atmospheric trace gas products from ultraviolet–visible (UV–Vis) sounders. We used synthetic and observational data to identify and quantify possible cloud-related bias in NO2 tropospheric vertical column density (TVCD). The synthetic data were based on high-resolution large eddy simulations which were input to a 3D radiative transfer model. The simulated visible spectra for low-earth-orbiting and geostationary geometries were analysed with standard retrieval methods and cloud correction schemes that are employed in operational NO2 satellite products. For the observational data, the NO2 products from the TROPOspheric Monitoring Instrument (TROPOMI) were used, while the Visible Infrared Imaging Radiometer Suite (VIIRS) provided high-spatial-resolution cloud and radiance data. NO2 profile shape, cloud shadow fraction, cloud top height, cloud optical depth, and solar zenith and viewing angles were identified as the metrics being the most important in identifying 3D cloud impacts on NO2 TVCD retrievals. For a solar zenith angle less than about 40∘ the synthetic data show that the NO2 TVCD bias is typically below 10 %, while for larger solar zenith angles the NO2 TVCD is low-biased by tens of percent. The horizontal variability of NO2 and differences in TROPOMI and VIIRS overpass times make it challenging to identify a similar bias in the observational data. However, for optically thick clouds above 3000 m, a low bias appears to be present in the observational data.

Retrievals of trace gas concentrations from satellite observations are mostly performed for clear regions or regions with low cloud coverage. However, even fully clear pixels can be affected by clouds in the vicinity, either by shadowing or by scattering of radiation from clouds in the clear region. Quantifying the error of retrieved trace gas concentrations due to cloud scattering is a difficult task. One possibility is to generate synthetic data by three-dimensional (3D) radiative transfer simulations using realistic 3D atmospheric input data, including 3D cloud structures. Retrieval algorithms may be applied on the synthetic data, and comparison to the known input trace gas concentrations yields the retrieval error due to cloud scattering. In this paper we present a comprehensive synthetic dataset which has been generated using the Monte Carlo radiative transfer model MYSTIC (Monte Carlo code for the phYSically correct Tracing of photons In Cloudy atmospheres). The dataset includes simulated spectra in two spectral ranges (400–500 nm and the O2A-band from 755–775 nm). Moreover it includes layer air mass factors (layer-AMFs) calculated at 460 nm. All simulations are performed for a fixed background atmosphere for various sun positions, viewing directions and surface albedos. Two cloud setups are considered: the first includes simple box clouds with various geometrical and optical thicknesses. This can be used to systematically investigate the sensitivity of the retrieval error on solar zenith angle, surface albedo and cloud parameters. Corresponding 1D simulations are also provided. The second includes realistic three-dimensional clouds from an ICON large eddy simulation (LES) for a region covering Germany and parts of surrounding countries. The scene includes cloud types typical of central Europe such as shallow cumulus, convective cloud cells, cirrus and stratocumulus. This large dataset can be used to quantify the trace gas concentration retrieval error statistically. Along with the dataset, the impact of horizontal photon transport on reflectance spectra and layer-AMFs is analysed for the box-cloud scenarios. Moreover, the impact of 3D cloud scattering on the NO2 vertical column density (VCD) retrieval is presented for a specific LES case. We find that the retrieval error is largest in cloud shadow regions, where the NO2 VCD is underestimated by more than 20 %. The dataset is available for the scientific community to assess the behaviour of trace gas retrieval algorithms and cloud correction schemes in cloud conditions with 3D structure.

In early October 2020, northern Europe experienced an episode with poor air quality due to high concentrations of particulate matter (PM). At several sites in Norway, recorded weekly values exceeded historical maximum PM10 concentrations from the past 4 to 10 years. Daily mean PM10 values at Norwegian sites were up to 97 µg m−3 and had a median value of 59 µg m−3. We analysed this severe pollution episode caused by long-range atmospheric transport based on surface and remote sensing observations and transport model simulations to understand its causes. Samples from three sites in mainland Norway and the Arctic remote station Zeppelin (Svalbard) showed strong contributions from mineral dust to PM10 (23 %–36 % as a minimum and 31 %–45 % as a maximum) and biomass burning (8 %–16 % to 19 %–21 %). Atmospheric transport simulations indicate that Central Asia was the main source region for mineral dust observed in this episode. The biomass burning fraction can be attributed to forest fires in Ukraine and southern Russia, but we cannot exclude other sources contributing, like fires elsewhere, because the model underestimates observed concentrations. The combined use of remote sensing, surface measurements, and transport modelling proved effective in describing the episode and distinguishing its causes.

The Airborne ROmanian Measurements of Aerosols and Trace gases (AROMAT) campaigns took place in Romania in September 2014 and August 2015. They focused on two sites: the Bucharest urban area and large power plants in the Jiu Valley. The main objectives of the campaigns were to test recently developed airborne observation systems dedicated to air quality studies and to verify their applicability for the validation of space-borne atmospheric missions such as the TROPOspheric Monitoring Instrument (TROPOMI)/Sentinel-5 Precursor (S5P). We present the AROMAT campaigns from the perspective of findings related to the validation of tropospheric NO2, SO2, and H2CO. We also quantify the emissions of NOx and SO2 at both measurement sites. We show that tropospheric NO2 vertical column density (VCD) measurements using airborne mapping instruments are well suited for satellite validation in principle. The signal-to-noise ratio of the airborne NO2 measurements is an order of magnitude higher than its space-borne counterpart when the airborne measurements are averaged at the TROPOMI pixel scale. However, we show that the temporal variation of the NO2 VCDs during a flight might be a significant source of comparison error. Considering the random error of the TROPOMI tropospheric NO2 VCD (σ), the dynamic range of the NO2 VCDs field extends from detection limit up to 37 σ (2.6×1016 molec. cm−2) and 29 σ (2×1016 molec. cm−2) for Bucharest and the Jiu Valley, respectively. For both areas, we simulate validation exercises applied to the TROPOMI tropospheric NO2 product. These simulations indicate that a comparison error budget closely matching the TROPOMI optimal target accuracy of 25 % can be obtained by adding NO2 and aerosol profile information to the airborne mapping observations, which constrains the investigated accuracy to within 28 %. In addition to NO2, our study also addresses the measurements of SO2 emissions from power plants in the Jiu Valley and an urban hotspot of H2CO in the centre of Bucharest. For these two species, we conclude that the best validation strategy would consist of deploying ground-based measurement systems at well-identified locations.

Atmospheric turbulence and in particular its effect on tracer dispersion may be measured by cameras sensitive to the absorption of ultraviolet (UV) sunlight by sulfur dioxide (SO2), a gas that can be considered a passive tracer over short transport distances. We present a method to simulate UV camera measurements of SO2 with a 3D Monte Carlo radiative transfer model which takes input from a large eddy simulation (LES) of a SO2 plume released from a point source. From the simulated images the apparent absorbance and various plume density statistics (centre-line position, meandering, absolute and relative dispersion, and skewness) were calculated. These were compared with corresponding quantities obtained directly from the LES. Mean differences of centre-line position, absolute and relative dispersions, and skewness between the simulated images and the LES were generally found to be smaller than or about the voxel resolution of the LES. Furthermore, sensitivity studies were made to quantify how changes in solar azimuth and zenith angles, aerosol loading (background and in plume), and surface albedo impact the UV camera image plume statistics. Changing the values of these parameters within realistic limits has negligible effects on the centre-line position, meandering, absolute and relative dispersions, and skewness of the SO2 plume. Thus, we demonstrate that UV camera images of SO2 plumes may be used to derive plume statistics of relevance for the study of atmospheric turbulent dispersion.

Recent years have seen the increasing inclusion of per-retrieval prognostic (predictive) uncertainty estimates within satellite aerosol optical depth (AOD) data sets, providing users with quantitative tools to assist in the optimal use of these data. Prognostic estimates contrast with diagnostic (i.e. relative to some external truth) ones, which are typically obtained using sensitivity and/or validation analyses. Up to now, however, the quality of these uncertainty estimates has not been routinely assessed. This study presents a review of existing prognostic and diagnostic approaches for quantifying uncertainty in satellite AOD retrievals, and it presents a general framework to evaluate them based on the expected statistical properties of ensembles of estimated uncertainties and actual retrieval errors. It is hoped that this framework will be adopted as a complement to existing AOD validation exercises; it is not restricted to AOD and can in principle be applied to other quantities for which a reference validation data set is available. This framework is then applied to assess the uncertainties provided by several satellite data sets (seven over land, five over water), which draw on methods from the empirical to sensitivity analyses to formal error propagation, at 12 Aerosol Robotic Network (AERONET) sites. The AERONET sites are divided into those for which it is expected that the techniques will perform well and those for which some complexity about the site may provide a more severe test. Overall, all techniques show some skill in that larger estimated uncertainties are generally associated with larger observed errors, although they are sometimes poorly calibrated (i.e. too small or too large in magnitude). No technique uniformly performs best. For powerful formal uncertainty propagation approaches such as optimal estimation, the results illustrate some of the difficulties in appropriate population of the covariance matrices required by the technique. When the data sets are confronted by a situation strongly counter to the retrieval forward model (e.g. potentially mixed land–water surfaces or aerosol optical properties outside the family of assumptions), some algorithms fail to provide a retrieval, while others do but with a quantitatively unreliable uncertainty estimate. The discussion suggests paths forward for the refinement of these techniques.

Highly unusual open fires burned in western Greenland between 31 July and 21 August 2017, after a period of warm, dry and sunny weather. The fires burned on peatlands that became vulnerable to fires by permafrost thawing. We used several satellite data sets to estimate that the total area burned was about 2345 ha. Based on assumptions of typical burn depths and emission factors for peat fires, we estimate that the fires consumed a fuel amount of about 117 kt C and emitted about 23.5 t of black carbon (BC) and 731 t of organic carbon (OC), including 141 t of brown carbon (BrC). We used a Lagrangian particle dispersion model to simulate the atmospheric transport and deposition of these species. We find that the smoke plumes were often pushed towards the Greenland ice sheet by westerly winds, and thus a large fraction of the emissions (30 %) was deposited on snow- or ice-covered surfaces. The calculated deposition was small compared to the deposition from global sources, but not entirely negligible. Analysis of aerosol optical depth data from three sites in western Greenland in August 2017 showed strong influence of forest fire plumes from Canada, but little impact of the Greenland fires. Nevertheless, CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) lidar data showed that our model captured the presence and structure of the plume from the Greenland fires. The albedo changes and instantaneous surface radiative forcing in Greenland due to the fire emissions were estimated with the SNICAR model and the uvspec model from the libRadtran radiative transfer software package. We estimate that the maximum albedo change due to the BC and BrC deposition was about 0.007, too small to be measured. The average instantaneous surface radiative forcing over Greenland at noon on 31 August was 0.03–0.04 W m−2, with locally occurring maxima of 0.63–0.77 W m−2 (depending on the studied scenario). The average value is up to an order of magnitude smaller than the radiative forcing from other sources. Overall, the fires burning in Greenland in the summer of 2017 had little impact on the Greenland ice sheet, causing a small extra radiative forcing. This was due to the – in a global context – still rather small size of the fires. However, the very large fraction of the emissions deposited on the Greenland ice sheet from these fires could contribute to accelerated melting of the Greenland ice sheet if these fires become several orders of magnitude larger under future climate.

In atmospheric tracer experiments, a substance is released into the turbulent atmospheric flow to study the dispersion parameters of the atmosphere. That can be done by observing the substance's concentration distribution downwind of the source. Past experiments have suffered from the fact that observations were only made at a few discrete locations and/or at low time resolution. The Comtessa project (Camera Observation and Modelling of 4-D Tracer Dispersion in the Atmosphere) is the first attempt at using ultraviolet (UV) camera observations to sample the three-dimensional (3-D) concentration distribution in the atmospheric boundary layer at high spatial and temporal resolution. For this, during a three-week campaign in Norway in July 2017, sulfur dioxide (SO2), a nearly passive tracer, was artificially released in continuous plumes and nearly instantaneous puffs from a 9 m high tower. Column-integrated SO2 concentrations were observed with six UV SO2 cameras with sampling rates of several hertz and a spatial resolution of a few centimetres. The atmospheric flow was characterised by eddy covariance measurements of heat and momentum fluxes at the release mast and two additional towers. By measuring simultaneously with six UV cameras positioned in a half circle around the release point, we could collect a data set of spatially and temporally resolved tracer column densities from six different directions, allowing a tomographic reconstruction of the 3-D concentration field. However, due to unfavourable cloudy conditions on all measurement days and their restrictive effect on the SO2 camera technique, the presented data set is limited to case studies. In this paper, we present a feasibility study demonstrating that the turbulent dispersion parameters can be retrieved from images of artificially released puffs, although the presented data set does not allow for an in-depth analysis of the obtained parameters. The 3-D trajectories of the centre of mass of the puffs were reconstructed enabling both a direct determination of the centre of mass meandering and a scaling of the image pixel dimension to the position of the puff. The latter made it possible to retrieve the temporal evolution of the puff spread projected to the image plane. The puff spread is a direct measure of the relative dispersion process. Combining meandering and relative dispersion, the absolute dispersion could be retrieved. The turbulent dispersion in the vertical is then used to estimate the effective source size, source timescale and the Lagrangian integral time. In principle, the Richardson–Obukhov constant of relative dispersion in the inertial subrange could be also obtained, but the observation time was not sufficiently long in comparison to the source timescale to allow an observation of this dispersion range. While the feasibility of the methodology to measure turbulent dispersion could be demonstrated, a larger data set with a larger number of cloud-free puff releases and longer observation times of each puff will be recorded in future studies to give a solid estimate for the turbulent dispersion under a variety of stability conditions.

Aerosol-layer height is essential for understanding the impact of aerosols on the climate system. As part of the European Space Agency Aerosol_cci project, aerosol-layer height as derived from passive thermal and solar satellite sensors measurements have been compared with aerosol-layer heights estimated from CALIOP measurements. The Aerosol_cci project targeted dust-type aerosol for this study. This ensures relatively unambiguous aerosol identification by the CALIOP processing chain. Dust-layer height was estimated from thermal IASI measurements using four different algorithms (from BIRA-IASB, DLR, LMD, LISA) and from solar GOME-2 (KNMI) and SCIAMACHY (IUP) measurements. Due to differences in overpass time of the various satellites, a trajectory model was used to move the CALIOP-derived dust heights in space and time to the IASI, GOME-2 and SCIAMACHY dust height pixels. It is not possible to construct a unique dust-layer height from the CALIOP data. Thus two CALIOP-derived layer heights were used: the cumulative extinction height defined as the height where the CALIOP extinction column is half of the total extinction column, and the geometric mean height, which is defined as the geometrical mean of the top and bottom heights of the dust layer. In statistical average over all IASI data there is a general tendency to a positive bias of 0.5–0.8 km against CALIOP extinction-weighted height for three of the four algorithms assessed, while the fourth algorithm has almost no bias. When comparing geometric mean height there is a shift of −0.5 km for all algorithms (getting close to zero for the three algorithms and turning negative for the fourth). The standard deviation of all algorithms is quite similar and ranges between 1.0 and 1.3 km. When looking at different conditions (day, night, land, ocean), there is more detail in variabilities (e.g. all algorithms overestimate more at night than during the day). For the solar sensors it is found that on average SCIAMACHY data are lower by −1.097 km (−0.961 km) compared to the CALIOP geometric mean (cumulative extinction) height, and GOME-2 data are lower by −1.393 km (−0.818 km).

Accurate gas velocity measurements in emission plumes are highly desirable for various atmospheric remote sensing applications. The imaging technique of UV SO2 cameras is commonly used to monitor SO2 emissions from volcanoes and anthropogenic sources (e.g. power plants, ships). The camera systems capture the emission plumes at high spatial and temporal resolution. This allows the gas velocities in the plume to be retrieved directly from the images. The latter can be measured at a pixel level using optical flow (OF) algorithms. This is particularly advantageous under turbulent plume conditions. However, OF algorithms intrinsically rely on contrast in the images and often fail to detect motion in low-contrast image areas. We present a new method to identify ill-constrained OF motion vectors and replace them using the local average velocity vector. The latter is derived based on histograms of the retrieved OF motion fields. The new method is applied to two example data sets recorded at Mt Etna (Italy) and Guallatiri (Chile). We show that in many cases, the uncorrected OF yields significantly underestimated SO2 emission rates. We further show that our proposed correction can account for this and that it significantly improves the reliability of optical-flow-based gas velocity retrievals. In the case of Mt Etna, the SO2 emissions of the north-eastern crater are investigated. The corrected SO2 emission rates range between 4.8 and 10.7 kg s−1 (average of 7.1 ± 1.3 kg s−1) and are in good agreement with previously reported values. For the Guallatiri data, the emissions of the central crater and a fumarolic field are investigated. The retrieved SO2 emission rates are between 0.5 and 2.9 kg s−1 (average of 1.3 ± 0.5 kg s−1) and provide the first report of SO2 emissions from this remotely located and inaccessible volcano.

The ozone profile records of a large number of limb and occultation satellite instruments are widely used to address several key questions in ozone research. Further progress in some domains depends on a more detailed understanding of these data sets, especially of their long-term stability and their mutual consistency. To this end, we made a systematic assessment of 14 limb and occultation sounders that, together, provide more than three decades of global ozone profile measurements. In particular, we considered the latest operational Level-2 records by SAGE II, SAGE III, HALOE, UARS MLS, Aura MLS, POAM II, POAM III, OSIRIS, SMR, GOMOS, MIPAS, SCIAMACHY, ACE-FTS and MAESTRO. Central to our work is a consistent and robust analysis of the comparisons against the ground-based ozonesonde and stratospheric ozone lidar networks. It allowed us to investigate, from the troposphere up to the stratopause, the following main aspects of satellite data quality: long-term stability, overall bias and short-term variability, together with their dependence on geophysical parameters and profile representation. In addition, it permitted us to quantify the overall consistency between the ozone profilers. Generally, we found that between 20 and 40 km the satellite ozone measurement biases are smaller than ±5 %, the short-term variabilities are less than 5–12 % and the drifts are at most ±5 % decade−1 (or even ±3 % decade−1 for a few records). The agreement with ground-based data degrades somewhat towards the stratopause and especially towards the tropopause where natural variability and low ozone abundances impede a more precise analysis. In part of the stratosphere a few records deviate from the preceding general conclusions; we identified biases of 10 % and more (POAM II and SCIAMACHY), markedly higher single-profile variability (SMR and SCIAMACHY) and significant long-term drifts (SCIAMACHY, OSIRIS, HALOE and possibly GOMOS and SMR as well). Furthermore, we reflected on the repercussions of our findings for the construction, analysis and interpretation of merged data records. Most notably, the discrepancies between several recent ozone profile trend assessments can be mostly explained by instrumental drift. This clearly demonstrates the need for systematic comprehensive multi-instrument comparison analyses.

Traditional validation of atmospheric profiles is based on the intercomparison of two or more data sets in predefined ranges or classes of a given observational characteristic such as latitude or solar zenith angle. In this study we trained a self-organising map (SOM) with a full time series of relative difference profiles of SCIAMACHY limb v5.02 and lidar ozone profiles from seven observation sites. Each individual observation characteristic was then mapped to the obtained SOM to investigate to which degree variation in this characteristic is explanatory for the variation seen in the SOM map. For the studied data sets, altitude-dependent relations for the global data set were found between the difference profiles and studied variables. From the lowest altitude studied (18 km) ascending, the most influencing factors were found to be longitude, followed by solar zenith angle and latitude, sensor age and again solar zenith angle together with the day of the year at the highest altitudes studied here (up to 45 km). After accounting for both latitude and longitude, residual partial correlations with a reduced magnitude are seen for various factors. However, (partial) correlations cannot point out which (combination) of the factors drives the observed differences between the ground-based and satellite ozone profiles as most of the factors are inter-related. Clustering into three classes showed that there are also some local dependencies, with for instance one cluster having a much stronger correlation with the sensor age (days since launch) between 36 and 42 km. The proposed SOM-based approach provides a powerful tool for the exploration of differences between data sets without being limited to a priori defined data subsets.

In this study we have analyzed whether tourist cruise ships have an influence on measured sulfur dioxide (SO2), ozone (O3), Aitken mode particle and equivalent black carbon (EBC) concentrations at Ny Ålesund and Zeppelin Mountain on Svalbard in the Norwegian Arctic during summer. We separated the measurement data set into periods when ships were present and periods when ships were not present in the Kongsfjord area, according to a long-term record of the number of passengers visiting Ny Ålesund. We show that when ships with more than 50 passengers cruise in the Kongsfjord, measured daytime mean concentrations of 60 nm particles and EBC in summer show enhancements of 72 and 45%, respectively, relative to values when ships are not present. Even larger enhancements of 81 and 72% were found for stagnant conditions. In contrast, O3 concentrations were 5% lower on average and 7% lower under stagnant conditions, due to titration of O3 with the emitted nitric oxide (NO). The differences between the two data subsets are largest for the highest measured percentiles, while relatively small differences were found for the median concentrations, indicating that ship plumes are sampled relatively infrequently even when ships are present although they carry high pollutant concentrations. We estimate that the ships increased the total summer mean concentrations of SO2, 60 nm particles and EBC by 15, 18 and 11%, respectively. Our findings have two important implications. Firstly, even at such a remote Arctic observatory as Zeppelin, the measurements can be influenced by tourist ship emissions. Careful data screening is recommended before summertime Zeppelin data is used for data analysis or for comparison with global chemistry transport models. However, Zeppelin remains as one of the most valuable Arctic observatories, as most other Arctic observatories face even larger local pollution problems. Secondly, given landing statistics of tourist ships on Svalbard, it is suspected that large parts of the Svalbard archipelago are affected by cruise ship emissions. Thus, our results may be taken as a warning signal of future pan-Arctic conditions if Arctic shipping becomes more frequent and emission regulations are not strict enough.

An unprecedented ozone loss occurred in the Arctic in spring 2011. The details of the event are revisited from the twice-daily total ozone and NO2 column measurements of the eight SAOZ/NDACC (Système d'Analyse par Observation Zénithale/Network for Detection of Atmospheric Composition Changes) stations in the Arctic. It is shown that the total ozone depletion in the polar vortex reached 38% (approx. 170 DU) by the end of March, which is larger than the 30% of the previous record in 1996. Aside from the long extension of the cold stratospheric NAT PSC period, the amplitude of the event is shown to be resulting from a record daily total ozone loss rate of 0.7% d−1 after mid-February, never seen before in the Arctic but similar to that observed in the Antarctic over the last 20 yr. This high loss rate is attributed to the absence of NOx in the vortex until the final warming, in contrast to all previous winters where, as shown by the early increase of NO2 diurnal increase, partial renoxification occurs by import of NOx or HNO3 from the outside after minor warming episodes, leading to partial chlorine deactivation. The cause of the absence of renoxification and thus of high loss rate, is attributed to a vortex strength similar to that of the Antarctic but never seen before in the Arctic. The total ozone reduction on 20 March was identical to that of the 2002 Antarctic winter, which ended around 20 September, and a 15-day extension of the cold period would have been enough to reach the mean yearly amplitude of the Antarctic ozone hole. However there is no sign of trend since 1994, either in PSC (polar stratospheric cloud) volume (volume of air cold enough to allow formation of PSCs), early winter denitrification, late vortex renoxification, and vortex strength or in total ozone loss. The unprecedented large Arctic ozone loss in 2011 appears to result from an extreme meteorological event and there is no indication of possible strengthening related to climate change.

The eruption of the Icelandic volcano Eyjafjallajökull in April–May 2010 represents a "natural experiment" to study the impact of volcanic emissions on a continental scale. For the first time, quantitative data about the presence, altitude, and layering of the volcanic cloud, in conjunction with optical information, are available for most parts of Europe derived from the observations by the European Aerosol Research Lidar NETwork (EARLINET). Based on multi-wavelength Raman lidar systems, EARLINET is the only instrument worldwide that is able to provide dense time series of high-quality optical data to be used for aerosol typing and for the retrieval of particle microphysical properties as a function of altitude. In this work we show the four-dimensional (4-D) distribution of the Eyjafjallajökull volcanic cloud in the troposphere over Europe as observed by EARLINET during the entire volcanic event (15 April–26 May 2010). All optical properties directly measured (backscatter, extinction, and particle linear depolarization ratio) are stored in the EARLINET database available at http://www.earlinet.org. A specific relational database providing the volcanic mask over Europe, realized ad hoc for this specific event, has been developed and is available on request at http://www.earlinet.org. During the first days after the eruption, volcanic particles were detected over Central Europe within a wide range of altitudes, from the upper troposphere down to the local planetary boundary layer (PBL). After 19 April 2010, volcanic particles were detected over southern and south-eastern Europe. During the first half of May (5–15 May), material emitted by the Eyjafjallajökull volcano was detected over Spain and Portugal and then over the Mediterranean and the Balkans. The last observations of the event were recorded until 25 May in Central Europe and in the Eastern Mediterranean area. The 4-D distribution of volcanic aerosol layering and optical properties on European scale reported here provides an unprecedented data set for evaluating satellite data and aerosol dispersion models for this kind of volcanic events.

The April–May, 2010 volcanic eruptions of Eyjafjallajökull, Iceland caused significant economic and social disruption in Europe whilst state of the art measurements and ash dispersion forecasts were heavily criticized by the aviation industry. Here we demonstrate for the first time that large improvements can be made in quantitative predictions of the fate of volcanic ash emissions, by using an inversion scheme that couples a priori source information and the output of a Lagrangian dispersion model with satellite data to estimate the volcanic ash source strength as a function of altitude and time. From the inversion, we obtain a total fine ash emission of the eruption of 8.3 ± 4.2 Tg for particles in the size range of 2.8–28 μm diameter. We evaluate the results of our model results with a posteriori ash emissions using independent ground-based, airborne and space-borne measurements both in case studies and statistically. Subsequently, we estimate the area over Europe affected by volcanic ash above certain concentration thresholds relevant for the aviation industry. We find that during three episodes in April and May, volcanic ash concentrations at some altitude in the atmosphere exceeded the limits for the "Normal" flying zone in up to 14 % (6–16 %), 2 % (1–3 %) and 7 % (4–11 %), respectively, of the European area. For a limit of 2 mg m−3 only two episodes with fractions of 1.5 % (0.2–2.8 %) and 0.9 % (0.1–1.6 %) occurred, while the current "No-Fly" zone criterion of 4 mg m−3 was rarely exceeded. Our results have important ramifications for determining air space closures and for real-time quantitative estimations of ash concentrations. Furthermore, the general nature of our method yields better constraints on the distribution and fate of volcanic ash in the Earth system.

During the POLARCAT summer campaign in 2008, two episodes (2–5 July and 7–10 July 2008) occurred where low-pressure systems traveled from Siberia across the Arctic Ocean towards the North Pole. The two cyclones had extensive smoke plumes from Siberian forest fires and anthropogenic sources in East Asia embedded in their associated air masses, creating an excellent opportunity to use satellite and aircraft observations to validate the performance of atmospheric transport models in the Arctic, which is a challenging model domain due to numerical and other complications. Here we compare transport simulations of carbon monoxide (CO) from the Lagrangian transport model FLEXPART and the Eulerian chemical transport model TOMCAT with retrievals of total column CO from the IASI passive infrared sensor onboard the MetOp-A satellite. The main aspect of the comparison is how realistic horizontal and vertical structures are represented in the model simulations. Analysis of CALIPSO lidar curtains and in situ aircraft measurements provide further independent reference points to assess how reliable the model simulations are and what the main limitations are. The horizontal structure of mid-latitude pollution plumes agrees well between the IASI total column CO and the model simulations. However, finer-scale structures are too quickly diffused in the Eulerian model. Applying the IASI averaging kernels to the model data is essential for a meaningful comparison. Using aircraft data as a reference suggests that the satellite data are biased high, while TOMCAT is biased low. FLEXPART fits the aircraft data rather well, but due to added background concentrations the simulation is not independent from observations. The multi-data, multi-model approach allows separating the influences of meteorological fields, model realisation, and grid type on the plume structure. In addition to the very good agreement between simulated and observed total column CO fields, the results also highlight the difficulty to identify a data set that most realistically represents the actual pollution state of the Arctic atmosphere.

The validation of ozone profiles retrieved by satellite instruments through comparison with data from ground-based instruments is important to monitor the evolution of the satellite instrument, to assist algorithm development and to allow multi-mission trend analyses. In this study we compare ozone profiles derived from GOMOS night-time observations with measurements from lidar, microwave radiometer and balloon sonde. Collocated pairs are analysed for dependence on several geophysical and instrument observational parameters. Validation results are presented for the operational ESA level 2 data (GOMOS version 5.00) obtained during nearly seven years of observations and a comparison using a smaller dataset from the previous processor (version 4.02) is also included. The profiles obtained from dark limb measurements (solar zenith angle >107°) when the provided processing flag is properly considered match the ground-based measurements within ±2 percent over the altitude range 20 to 40 km. Outside this range, the pairs start to deviate more and there is a latitudinal dependence: in the polar region where there is a higher amount of straylight contamination, differences start to occur lower in the mesosphere than in the tropics, whereas for the lower part of the stratosphere the opposite happens: the profiles in the tropics reach less far down as the signal reduces faster because of the higher altitude at which the maximum ozone concentration is found compared to the mid and polar latitudes. Also the bias is shifting from mostly negative in the polar region to more positive in the tropics Profiles measured under "twilight" conditions are often matching the ground-based measurements very well, but care has to be taken in all cases when dealing with "straylight" contaminated profiles. For the selection criteria applied here (data within 800 km, 3 degrees in equivalent latitude, 20 h (5 h above 50 km) and a relative ozone error in the GOMOS data of 20% or less), no dependence was found on stellar magnitude, star temperature, nor the azimuth angle of the line of sight. No evidence of a temporal trend was seen either in the bias or frequency of outliers, but a comparison applying less strict data selection criteria might show differently.

An analytical inversion method has been developed to estimate the vertical profile of SO2 emissions from volcanic eruptions. The method uses satellite-observed total SO2 columns and an atmospheric transport model (FLEXPART) to exploit the fact that winds change with altitude – thus, the position and shape of the volcanic plume bear information on its emission altitude. The method finds the vertical emission distribution which minimizes the total difference between simulated and observed SO2 columns while also considering a priori information. We have tested the method with the eruption of Jebel at Tair, Yemen, on 30 September 2007 for which a comprehensive observational data set from various satellite instruments (AIRS, OMI, SEVIRI, CALIPSO) is available. Using satellite data from the first 24 h after the eruption for the inversion, we found an emission maximum near 16 km above sea level (a.s.l.), and secondary maxima near 5, 9, 12 and 14 km a.s.l. 60% of the emission occurred above the tropopause. The emission profile obtained in the inversion was then used to simulate the transport of the plume over the following week. The modeled plume agrees very well with SO2 total columns observed by OMI, and its altitude agrees with CALIPSO aerosol observations to within 1–2 km. The inversion result is robust against various changes in both the a priori and the observations. Even when using only SEVIRI data from the first 15 h after the eruption, the emission profile was reasonably well estimated. The method is computationally very fast. It is therefore suitable for implementation within an operational environment, such as the Volcanic Ash Advisory Centers, to predict the threat posed by volcanic ash for air traffic. It could also be helpful for assessing the sulfur input into the stratosphere, be it in the context of volcanic processes or also for proposed geo-engineering techniques to counteract global warming.

Erythemaly weighted UV and total UV-A irradiance measured at the ALOMAR (Arctic Lidar Observatory for Middle Atmosphere Research; 69° N, 16° E) in June 2007 by two Kipp & Zonen UV broadband meters type, UV-S-EA-T, are examined. One unit is mounted on rotating vertical plane and the other is permanently fixed horizontally. The UV broadband meters measure simultaneously to compare UV irradiances on vertical and horizontal planes. The entire range of such relative exposure variations during clear-sky and overcast conditions over ALOMAR in the period March–June 2007 is examined using STAR and Radonic1 model (developed at the Meteorological Institute, University of Munich) for various action spectra: erythema, UV-A, and vitamin D3. The model and observations support that the daily means of relative exposures are quite stable, i.e., vary within the range 0.4–0.6 with the mean around 0.5 when the averaged intra-day, day-to-day, and seasonal changes of the relative erythemal exposures are considered. It seems that multiplication of the daily mean dose from a broadband meter placed horizontally by the factor of 0.5 gives reasonable estimation of the daily mean exposure on a vertically oriented receiver randomly oriented towards the Sun. The model studies during clear-sky conditions show that the extreme value and daily variability of relative exposure are the highest for UV-A, next for erythemal UV, then for vitamin D3 weighed UV irradiance. The minima of relative exposure (~0.20–0.30) are almost the same for all weighting functions. The comparison of model simulations and measurements suggests that specific cloud configuration could lead to significant enhancement of UV exposure of rotating receiver.

In spring 2006 a special meteorological situation occurred in the European Arctic region giving record high levels of air pollution. The synoptic situation resulted in extensive transport of pollution predominantly from agricultural fires in Eastern Europe into the Arctic region and record high air-pollution levels were measured at the Zeppelin observatory at Ny-Ålesund (78°54' N, 11°53' E) in the period from 25 April to 12 May. In the present study we investigate the optical properties of the aerosols from this extreme event and we estimate the radiative forcing of this episode. We examine the aerosol optical properties from the source region and into the European Arctic and explore the evolution of the episode and the changes in the optical properties. A number of sites in Eastern Europe, Northern Scandinavia and Svalbard are included in the study. The observations show that the maximum AOD was from 2–3 May at all sites and varies from 0.52 to 0.87, and the corresponding Ångstrøm exponent was relatively large. Lidar measurements from Minsk, ALOMAR (Arctic Lidar Observatory for Middle Atmosphere Research at Andenes) and Ny-Ålesund show that the aerosol layer was below 3 km at all sites the height is decreasing from the source region and into the Arctic. For the AERONET sites included (Minsk, Toravere, Hornsund) we have further studied the evolution of the aerosol size. The single scattering albedo at Svalbard is provided for two sites; Ny-Ålesund and Hornsund. Importantly the calculated single scattering albedo based on the aerosol chemical composition and size distribution from Ny-Ålesund and the AERONET measurements at Hornsund are consistent. We have found strong agreement between the satellite daily MODIS AOD and the ground-based AOD observations. This agreement is crucial for accurate radiative forcing calculations. We calculate a strong negative radiative forcing for the most polluted days employing the analysed ground based data, MODIS AOD and a multi-stream model for radiative transfer of solar radiation. During this specific pollution event the forcing reached values as low as −35 W m−2 in the region. For comparison, the direct forcing of a corresponding aerosol layer with a typical AOD of 0.05 for the season is around −5 W m−2.

This paper characterizes vertical ozone profiles retrieved with the IMK-IAA (Institute for Meteorology and Climate Research, Karlsruhe – Instituto de Astrofisica de Andalucia) science-oriented processor from high spectral resolution data (until March 2004) measured by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) aboard the environmental satellite Envisat. Bias determination and precision validation is performed on the basis of correlative measurements by ground-based lidars, Fourier transform infrared spectrometers, and microwave radiometers as well as balloon-borne ozonesondes, the balloon-borne version of MIPAS, and two satellite instruments (Halogen Occultation Experiment and Polar Ozone and Aerosol Measurement III). Percentage mean differences between MIPAS and the comparison instruments for stratospheric ozone are generally within ±10%. The precision in this altitude region is estimated at values between 5 and 10% which gives an accuracy of 15 to 20%. Below 18 km, the spread of the percentage mean differences is larger and the precision degrades to values of more than 20% depending on altitude and latitude. The main reason for the degraded precision at low altitudes is attributed to undetected thin clouds which affect MIPAS retrievals, and to the influence of uncertainties in the water vapor concentration.

In spring 2006, the European Arctic was abnormally warm, setting new historical temperature records. During this warm period, smoke from agricultural fires in Eastern Europe intruded into the European Arctic and caused the most severe air pollution episodes ever recorded there. This paper confirms that biomass burning (BB) was indeed the source of the observed air pollution, studies the transport of the smoke into the Arctic, and presents an overview of the observations taken during the episode. Fire detections from the MODIS instruments aboard the Aqua and Terra satellites were used to estimate the BB emissions. The FLEXPART particle dispersion model was used to show that the smoke was transported to Spitsbergen and Iceland, which was confirmed by MODIS retrievals of the aerosol optical depth (AOD) and AIRS retrievals of carbon monoxide (CO) total columns. Concentrations of halocarbons, carbon dioxide and CO, as well as levoglucosan and potassium, measured at Zeppelin mountain near Ny Ålesund, were used to further corroborate the BB source of the smoke at Spitsbergen. The ozone (O3) and CO concentrations were the highest ever observed at the Zeppelin station, and gaseous elemental mercury was also elevated. A new O3 record was also set at a station on Iceland. The smoke was strongly absorbing – black carbon concentrations were the highest ever recorded at Zeppelin – and strongly perturbed the radiation transmission in the atmosphere: aerosol optical depths were the highest ever measured at Ny Ålesund. We furthermore discuss the aerosol chemical composition, obtained from filter samples, as well as the aerosol size distribution during the smoke event. Photographs show that the snow at a glacier on Spitsbergen became discolored during the episode and, thus, the snow albedo was reduced. Samples of this polluted snow contained strongly elevated levels of potassium, sulphate, nitrate and ammonium ions, thus relating the discoloration to the deposition of the smoke aerosols. This paper shows that, to date, BB has been underestimated as a source of aerosol and air pollution for the Arctic, relative to emissions from fossil fuel combustion. Given its significant impact on air quality over large spatial scales and on radiative processes, the practice of agricultural waste burning should be banned in the future.

We discuss the quality of the two available SCIAMACHY limb ozone profile products. They were retrieved with the University of Bremen IFE's algorithm version 1.61 (hereafter IFE), and the official ESA offline algorithm (hereafter OL) versions 2.4 and 2.5. The ozone profiles were compared to a suite of correlative measurements from ground-based lidar and microwave, sondes, SAGE II and SAGE III (Stratospheric Aerosol and Gas Experiment). To correct for the expected Envisat pointing errors, which have not been corrected implicitly in either of the algorithms, we applied a constant altitude shift of -1.5 km to the SCIAMACHY ozone profiles. The IFE ozone profile data between 16 and 40 km are biased low by 3-6%. The average difference profiles have a typical standard deviation of 10% between 20 and 35 km. We show that more than 20% of the SCIAMACHY official ESA offline (OL) ozone profiles version 2.4 and 2.5 have unrealistic ozone values, most of these are north of 15° S. The remaining OL profiles compare well to correlative instruments above 24 km. Between 20 and 24 km, they underestimate ozone by 15±5%.

An empirical technique for retrieving profiles of the square of the Brunt-Väisälä frequency, ωB2, from MST radar return signal power is presented. The validity of the technique, which is applied over the altitude range 1.0-15.7km, is limited to those altitudes at which the humidity contributions to the mean vertical gradient of generalised potential refractive index, M, can be ignored. Although this is commonly assumed to be the case above the first few kilometres of the atmosphere, it is shown that humidity contributions can be significant right up to the tropopause level. In specific circumstances, however, the technique is valid over large sections of the troposphere. Comparisons of radar- and (balloon-borne) radiosonde-derived ωB2 profiles are typically quantitatively and qualitatively well matched. However, the horizontal separation between the radar and the radiosondes (which were launched at the radar site) increases with increasing altitude. Under conditions of mountain wave activity, which can be highly localised, large discrepancies can occur at lower-stratospheric altitudes. This demonstrates the fact that radiosonde observations cannot necessarily be assumed to be representative of the atmosphere above the launch site.

We present a case study of a noctilucent cloud (NLC) display appearing on 10-11 August 2000 over Northern Sweden. Clear wave structures were visible in the clouds and time-lapse photography was used to derive the parameters characterising the gravity waves which could account for the observed NLC modulation. Using two nearby atmospheric radars, the Esrange MST Radar data and Andoya MF radar, we have identified gravity waves propagating upward from the upper stratosphere to NLC altitudes. The wave parameters derived from the radar measurements support the suggestion that gravity waves are responsible for the observed complex wave dynamics in the NLC.

The formation of polar stratospheric clouds (PSCs) is closely related to wave activity on different scales since waves propagating into the stratosphere perturb the temperature profile. We present here a case study of the development of visible PSCs (mother-of-pearl clouds), appearing at the polar vortex edge on 9 January 1997, under-taken by means of ground-based cameras. It is shown that the presence of stratospheric clouds may be detected semi-automatically and that short-term dynamics such as altitude variations can be tracked in three dimensions. The PSC field showed distinct features separated by approximately 20 km, which implies wave-induced temperature variations on that scale. The wave-induced characteristics were further emphasised by the fact that the PSCs moved within a sloping spatial surface. The appearance of visible mother-of-pearl clouds seems to be related to leewave-induced cooling of air masses, where the synoptic temperature has been close to (but not necessarily below) the threshold temperatures for PSC condensation.Key words. Atmospheric composition and structure (aerosols and particles) – Meteorology and atmospheric dynamics (middle atmosphere dynamics; instruments and techniques)

A European campaign of ground-based radar, lidar and optical measurements was carried out during the winter of 1996/1997 (28 December-2 February) to study lee waves in the northern part of Scandinavia. The participants operated ozone lidars, backscatter lidars and MST radars at ALOMAR/Andoya and Esrange/Kiruna, and an ALIS imaging system in Kiruna. The Andoya site was generally windward of the Scandinavian mountains, the Kiruna site on the leeward side. The goal of the experiment was to examine the influence of lee waves on the formation of Polar Stratospheric Clouds (PSCs). This paper studies the radar data from MST-radar ESRAD located at Esrange [68.°N, 21.°E], i.e. in the lee of the mountains. We present three cases where strong lee waves were observed: in one case they propagated upwards to the lower stratosphere and in the other two cases they were trapped or absorbed in the troposphere. We examine the local waves and the direction and strength of the local wind using the radar, the synoptic meteorological situation using weather maps (European Meteorological Bulletin) and the synoptic stratospheric temperatures using ECMWF data. We observed that waves propagate up to the stratosphere during frontal passages. When anticyclonic ridges are present, the propagation to the stratosphere is very weak. This is due to trapping of the waves at or below the tropopause. We also show that the radar data alone can be used to characterise the different weather conditions for the three cases studied (through the variation of the height of the tropopause). The synoptic stratospheric temperatures in the three cases were similar, and were above the expected threshold for PSC formation. Lidar and visual observation of PSCs and nacreous clouds, respectively, showed that these were present only in the case when the lee waves propagated up to the lower stratosphere.Key words. Atmospheric composition and structure (aerosols and particles) · Electromagnetic (wave propa- gation) · Meteorology and atmospheric dynamics (mesoscale meteorology)

Safety and reliability of constructions operated are predicted using the known mechanical properties of materials and geometry of cross-sections, and also the known internal forces. The extensometry technique (electro-resistant tensometers, wire gauges, sensor systems) is a common method applied under laboratory conditions to determine the deformation state of a material. The construction sector rarely uses ultrasonic extensometry with the acoustoelastic (AE) method which is based on the relation between the direction of ultrasonic waves and the direction of normal stresses. It is generally used to identify stress states of machine or vehicles parts, mainly made of steel, characterized by high homogeneity and a lack of inherent internal defects. The AE effect was detected in autoclaved aerated concrete (AAC), which is usually used in masonry units. The acoustoelastic effect was used in the tests described to identify the complex stress state in masonry walls (masonry units) made of AAC. At first, the relationships were determined for mean hydrostatic stresses P and mean compressive stresses σ 3 with relation to velocities of the longitudinal ultrasonic wave c p . These stresses were used to determine stresses σ 3 . The discrete approach was used which consists in analyzing single masonry units. Changes in velocity of longitudinal waves were identified at a test stand to control the stress states of an element tested by the digital image correlation (DIC) technique. The analyses involved density and the impact of moisture content of AAC. Then, the method was verified on nine walls subjected to axial compression and the model was validated with the FEM micromodel. It was demonstrated that mean compressive stresses σ 3 and hydrostatic stresses, which were determined for the masonry using the method considered, could be determined even up to ca. 75% of failure stresses at the acceptable error level of 15%. Stresses σ 1 parallel to bed joints were calculated using the known mean hydrostatic stresses and mean compressive stresses σ 3 .

We present comparisons between estimates of the aerosol optical thickness and the Ångström exponent in Northern Norway and Svalbard based on data from AERONET (Aerosol Robotic Network) stations at Andenes (69.28°N, 16.01°E, 379 m altitude) and Hornsund (77.00°N, 15.56°E, 10 m altitude) for the period 2008-2013. The five/six-year annual mean values for the aerosol optical thickness at 500 nm τ(500) at Andenes and Hornsund both were 0.09. At Hornsund, there was less variation of the monthly mean value of τ(500) than at Andenes. The annual mean values of the Ångström exponent α at Andenes and Hornsund were 1.29 and 1.34, respectively. At Andenes and Hornsund α was found to be larger than 1.1 in 68% and 84% of the observations, respectively, indicating that fine-mode particles were dominating at both sites. Both sites had a similar aerosol size distribution during summer although one site is in an arctic area while the other site is in a subarctic area.