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Temperature fluctuations induced by mountain waves can play a crucial role in the formation of polar stratospheric clouds (PSCs). In particular, the cold phase of the waves can lower local temperatures sufficiently to trigger PSC formation, even when large-scale background temperatures are too high. To provide new quantitative constraints on the relevance of this effect, this study analyzes a decade (2002–2012) of ice PSC detections obtained from Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) measurements and ERA5 data in the polar winter lower stratosphere. In the MIPAS observations, we find that approximately 52 % of the Arctic ice PSCs and 26 % of the Antarctic ice PSCs are detected at temperatures above the local Tice. Ice PSCs above Tice are concentrated around mountainous regions and their downwind directions. A backward-trajectory analysis is performed to investigate the temperature history of each ice PSC observation. The cumulative fraction of ice PSCs above Tice increases as the trajectory gets closer to the observation point. The most significant change in the fraction of ice PSCs above Tice occurs within the 6 h preceding the observations. At the observation point, the mean fractions of ice PSCs above Tice, taking into account temperature fluctuations along the backward trajectory, are 33 % in the Arctic and 9 % in the Antarctic. The results provide a quantitative assessment of the occurrence of ice PSCs above Tice in connection with orographic waves. Additionally, the observational statistics presented can be utilized for comparison with chemistry climate simulations.

Satellite-based observations of free-tropospheric water vapour isotopologue ratios (HDO / H2O, expressed in form of the δ value δD) with good global and temporal coverage have become available recently. We investigate the potential of these observations for constraining the uncertainties of the atmospheric analyses fields of specific humidity (q), temperature (T), and δD and of variables that capture important properties of the atmospheric water cycle, namely the vertical velocity (ω), the latent heating rate (Q2), and the precipitation rate (Prcp). Our focus is on the impact of the δD observations relative to the impact achieved by the observation of q and T, which are much more easily observed by satellites and are routinely in use for atmospheric analyses. For our investigations we use an Observing System Simulation Experiment; i.e. we simulate the satellite observations of q, T, and δD with known uncertainties and coverage (e.g. observations are not available for cloudy conditions, i.e. at locations where the atmosphere is vertically unstable). Then we use the simulated observations within a Kalman-filter-based assimilation framework in order to evaluate their potential for improving the quality of atmospheric analyses. The study is made for low latitudes (30° S to 30° N) and for 40 d between mid-July and the end of August 2016. We find that q observations generally have the largest impacts on the analyses' quality and that T observations have stronger impacts overall than δD observations. We show that there is no significant impact of δD observations for stable atmospheric conditions; however, for very unstable conditions, the impact of δD observations is significant and even slightly stronger than the respective impact of T observations. Very unstable conditions are rare but are related to extreme events (e.g. storms, flooding); i.e. the δD observations significantly impact the analyses' quality of the events that have the largest societal consequences. The fact that no satellite observations are available at the location and time of the unstable conditions indicates a remote impact of δD observations that are available elsewhere. Concerning real-world applications, we conclude that the situation of δD satellite observations is very promising but that further improving the model's linkage between convective processes and the larger-scale δD fields might be needed for optimizing the assimilation impact of real-world δD observations.

China stands out as a major contributor to anthropogenic methane (CH4) emissions, with coal mine methane (CMM) playing a crucial role. To control and reduce CH4 emissions, China has made a dedicated commitment and formulated an ambitious mitigation plan. To verify the progress made, the consistent acquisition of independent CH4 emission data is required. This paper aims to implement a wind-assigned anomaly method for the precise determination of regional-scale CMM emissions within the coal-rich Shanxi province. We use the TROPOspheric Monitoring Instrument (TROPOMI) CH4 observations from May 2018 to May 2023, coupled with ERA5 wind and a bottom-up inventory dataset based on the IPCC (Intergovernmental Panel on Climate Change) Tier 2 approach covering the Changzhi, Jincheng, and Yangquan regions of the Shanxi province. The derived emission strengths are 8.4 × 1026 molec. s−1 (0.706 Tg yr−1, ±25 %), 1.4 × 1027 molec. s−1 (1.176 Tg yr−1, ±20 %), and 4.9 × 1026 molec. s−1 (0.412 Tg yr−1, ±21 %), respectively. Our results exhibit biases of −18 %, 8 %, and 14 %, respectively, when compared to the IPCC Tier 2 bottom-up inventory. Larger discrepancies are found when comparing the estimates to the Copernicus Atmosphere Monitoring Service global anthropogenic emissions (CAMS-GLOB-ANT) and Emissions Database for Global Atmospheric Research (EDGARv7.0) inventories (64 %–176 %), suggesting that the two inventories may be overestimating CH4 emissions from the studied coal mining regions. Our estimates provide a comprehensive characterization of the regions within the Shanxi province, contribute to the validation of emission inventories, and provide additional insights into CMM emission mitigation.

Satellite data records of stratospheric water vapour have been compared to balloon-borne frost point hygrometer (FP) profiles that are coincident in space and time. The satellite data records of 15 different instruments cover water vapour data available from January 2000 through December 2016. The hygrometer data are from 27 stations all over the world in the same period. For the comparison, real or constructed averaging kernels have been applied to the hygrometer profiles to adjust them to the measurement characteristics of the satellite instruments. For bias evaluation, we have compared satellite profiles averaged over the available temporal coverage to the means of coincident FP profiles for individual stations. For drift determinations, we analysed time series of relative differences between spatiotemporally coincident satellite and hygrometer profiles at individual stations. In a synopsis we have also calculated the mean biases and drifts (and their respective uncertainties) for each satellite record over all applicable hygrometer stations in three altitude ranges (10–30 hPa, 30–100 hPa, and 100 hPa to tropopause). Most of the satellite data have biases % and average drifts % yr−1 in at least one of the respective altitude ranges. Virtually all biases are significant in the sense that their uncertainty range in terms of twice the standard error of the mean does not include zero. Statistically significant drifts (95 % confidence) are detected for 35 % of the ≈ 1200 time series of relative differences between satellites and hygrometers.

Nitrogen dioxide (NO2) air pollution provides valuable information for quantifying NOx (NOx = NO + NO2) emissions and exposures. This study presents a comprehensive method to estimate average tropospheric NO2 emission strengths derived from 4-year (May 2018–June 2022) TROPOspheric Monitoring Instrument (TROPOMI) observations by combining a wind-assigned anomaly approach and a machine learning (ML) method, the so-called gradient descent algorithm. This combined approach is firstly applied to the Saudi Arabian capital city of Riyadh, as a test site, and yields a total emission rate of 1.09×1026 molec. s−1. The ML-trained anomalies fit very well with the wind-assigned anomalies, with an R2 value of 1.0 and a slope of 0.99. Hotspots of NO2 emissions are apparent at several sites: over a cement plant and power plants as well as over areas along highways. Using the same approach, an emission rate of 1.99×1025 molec. s−1 is estimated in the Madrid metropolitan area, Spain. Both the estimate and spatial pattern are comparable with the Copernicus Atmosphere Monitoring Service (CAMS) inventory. Weekly variations in NO2 emission are highly related to anthropogenic activities, such as the transport sector. The NO2 emissions were reduced by 16 % at weekends in Riyadh, and high reductions were found near the city center and in areas along the highway. An average weekend reduction estimate of 28 % was found in Madrid. The regions with dominant sources are located in the east of Madrid, where residential areas and the Madrid-Barajas airport are located. Additionally, due to the COVID-19 lockdowns, the NO2 emissions decreased by 21 % in March–June 2020 in Riyadh compared with the same period in 2019. A much higher reduction (62 %) is estimated for Madrid, where a very strict lockdown policy was implemented. The high emission strengths during lockdown only persist in the residential areas, and they cover smaller areas on weekdays compared with weekends. The spatial patterns of NO2 emission strengths during lockdown are similar to those observed at weekends in both cities. Although our analysis is limited to two cities as test examples, the method has proven to provide reliable and consistent results. It is expected to be suitable for other trace gases and other target regions. However, it might become challenging in some areas with complicated emission sources and topography, and specific NO2 decay times in different regions and seasons should be taken into account. These impacting factors should be considered in the future model to further reduce the uncertainty budget.

Intensive coal mining activities in the Upper Silesian Coal Basin (USCB) in southern Poland are resulting in large amounts of methane (CH4) emissions. Annual CH4 emissions reached 448 kt according to the European Pollutant Release and Transfer Register (E-PRTR, 2017). As a CH4 emission hotspot in Europe, it is of importance to investigate its emission sources and make accurate emission estimates. In this study, we use satellite-based total column-averaged dry-air mole fraction of CH4 (XCH4) from the TROPOspheric Monitoring Instrument (TROPOMI) and tropospheric XCH4 (TXCH4) from the Infrared Atmospheric Sounding Interferometer (IASI). In addition, the high-resolution model forecasts, XCH4 and TXCH4, from the Copernicus Atmosphere Monitoring Service (CAMS) are used to estimate the CH4 emission rate averaged over 3 years (November 2017–December 2020) in the USCB region (49.3–50.8∘ N and 18–20∘ E). The wind-assigned anomaly method is first validated using the CAMS forecast data (XCH4 and TXCH4), showing a good agreement with the CAMS GLOBal ANThropogenic emission (CAMS-GLOB-ANT) inventory. It indicates that the wind-assigned method works well. This wind-assigned method is further applied to the TROPOMI XCH4 and TROPOMI + IASI TXCH4 by using the Carbon dioxide and Methane (CoMet) inventory derived for the year 2018. The calculated averaged total CH4 emissions over the USCB region is about 496 kt yr−1 (5.9×1026 molec. s−1) for TROPOMI XCH4 and 437 kt yr−1 (5.2×1026 molec. s−1) for TROPOMI + IASI TXCH4. These values are very close to the ones given in the E-PRTR inventory (448 kt yr−1) and the ones in the CoMet inventory (555 kt yr−1), and are thus in agreement with these inventories. The similar estimates of XCH4 and TXCH4 also imply that for a strong source, the dynamically induced variations of the CH4 mixing ratio in the upper troposphere and lower stratosphere region are of secondary importance. Uncertainties from different error sources (background removal and noise in the data, vertical wind shear, wind field segmentation, and angle of the emission cone) are approximately 14.8 % for TROPOMI XCH4 and 11.4 % for TROPOMI + IASI TXCH4. These results suggest that our wind-assigned method is quite robust and might also serve as a simple method to estimate CH4 or CO2 emissions for other regions.

The thermal infrared nadir spectra of IASI (Infrared Atmospheric Sounding Interferometer) are successfully used for retrievals of different atmospheric trace gas profiles. However, these retrievals offer generally reduced information about the lowermost tropospheric layer due to the lack of thermal contrast close to the surface. Spectra of scattered solar radiation observed in the near-infrared and/or shortwave infrared, for instance by TROPOMI (TROPOspheric Monitoring Instrument), offer higher sensitivity near the ground and are used for the retrieval of total-column-averaged mixing ratios of a variety of atmospheric trace gases. Here we present a method for the synergetic use of IASI profile and TROPOMI total-column level 2 retrieval products. Our method uses the output of the individual retrievals and consists of linear algebra a posteriori calculations (i.e. calculation after the individual retrievals). We show that this approach has strong theoretical similarities to applying the spectra of the different sensors together in a single retrieval procedure but with the substantial advantage of being applicable to data generated with different individual retrieval processors, of being very time efficient, and of directly benefiting from the high quality and most recent improvements of the individual retrieval processors. We demonstrate the method exemplarily for atmospheric methane (CH4). We perform a theoretical evaluation and show that the a posteriori combination method yields a total-column-averaged CH4 product (XCH4) that conserves the good sensitivity of the corresponding TROPOMI product while merging it with the high-quality upper troposphere–lower stratosphere (UTLS) CH4 partial-column information of the corresponding IASI product. As a consequence, the combined product offers additional sensitivity for the tropospheric CH4 partial column, which is not provided by the individual TROPOMI nor the individual IASI product. The theoretically predicted synergetic effect is verified by comparisons to CH4 reference data obtained from collocated XCH4 measurements at 14 globally distributed TCCON (Total Carbon Column Observing Network) stations, CH4 profile measurements made by 36 individual AirCore soundings, and tropospheric CH4 data derived from continuous ground-based in situ observations made at two nearby Global Atmospheric Watch (GAW) mountain stations. The comparisons clearly demonstrate that the combined product can reliably detect the actual variations of atmospheric XCH4, CH4 in the UTLS, and CH4 in the troposphere. A similar good reliability for the latter is not achievable by the individual TROPOMI and IASI products.

Nineteen limb-viewing data sets (occultation, passive thermal, and UV scattering) and two nadir upper tropospheric humidity (UTH) data sets are intercompared and also compared to frost-point hygrometer balloon sondes. The upper troposphere considered here covers the pressure range from 300–100 hPa. UTH is a challenging measurement, because concentrations vary between 2–1000 ppmv (parts per million by volume), with sharp changes in vertical gradients near the tropopause. Cloudiness in this region also makes the measurement challenging. The atmospheric temperature is also highly variable ranging from 180–250 K. The assessment of satellite-measured UTH is based on coincident comparisons with balloon frost-point hygrometer sondes, multi-month mapped comparisons, zonal mean time series comparisons, and coincident satellite-to-satellite comparisons. While the satellite fields show similar features in maps and time series, quantitatively they can differ by a factor of 2 in concentration, with strong dependencies on the amount of UTH. Additionally, time-lag response-corrected Vaisala RS92 radiosondes are compared to satellites and the frost-point hygrometer measurements. In summary, most satellite data sets reviewed here show on average ∼30 % agreement amongst themselves and frost-point data but with an additional ∼30 % variability about the mean bias. The Vaisala RS92 sonde, even with a time-lag correction, shows poor behavior for pressures less than 200 hPa.

This work employs ground- and space-based observations, together with model data, to study columnar abundances of atmospheric trace gases (XH2O, XCO2, XCH4 and XCO) in two high-latitude Russian cities, St. Petersburg and Yekaterinburg. Two portable COllaborative Column Carbon Observing Network (COCCON) spectrometers were used for continuous measurements at these locations during 2019 and 2020. Additionally, a subset of data of special interest (a strong gradient in XCH4 and XCO was detected) collected in the framework of a mobile city campaign performed in 2019 using both instruments is investigated. All studied satellite products (TROPOMI, OCO-2, GOSAT, MUSICA IASI) show generally good agreement with COCCON observations. Satellite and ground-based observations at high latitudes are much sparser than at low or mid latitudes, which makes direct coincident comparisons between remote-sensing observations more difficult. Therefore, a method of scaling continuous Copernicus Atmosphere Monitoring Service (CAMS) model data to the ground-based observations is developed and used for creating virtual COCCON observations. These adjusted CAMS data are then used for satellite validation, showing good agreement in both Peterhof and Yekaterinburg. The gradients between the two study sites (ΔXgas) are similar between CAMS and CAMS-COCCON datasets, indicating that the model gradients are in agreement with the gradients observed by COCCON. This is further supported by a few simultaneous COCCON and satellite ΔXgas measurements, which also agree with the model gradient. With respect to the city campaign observations recorded in St Petersburg, the downwind COCCON station measured obvious enhancements for both XCH4 (10.6 ppb) and XCO (9.5 ppb), which is nicely reflected by TROPOMI observations, which detect city-scale gradients of the order 9.4 ppb for XCH4 and 12.5 ppb for XCO.

Water vapour and ozone are important for the thermal and radiative balance of the upper troposphere (UT) and lowermost stratosphere (LMS). Both species are modulated by transport processes. Chemical and microphysical processes affect them differently. Thus, representing the different processes and their interactions is a challenging task for dynamical cores, chemical modules and microphysical parameterisations of state-of-the-art atmospheric model components. To test and improve the models, high-resolution measurements of the UT–LMS are required. Here, we use measurements taken in a flight of the GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) instrument on HALO (High Altitude and LOng Range Research Aircraft). The German research aircraft HALO performed a research flight on 26 February 2016 that covered deeply subsided air masses of the aged 2015/16 Arctic vortex, high-latitude LMS air masses, a highly textured region affected by troposphere-to-stratosphere exchange and high-altitude cirrus clouds. Therefore, it provides a challenging multifaceted case study for comparing GLORIA observations with state-of-the-art atmospheric model simulations in a complex UT–LMS region at a late stage of the Arctic winter 2015/16. Using GLORIA observations in this manifold scenario, we test the ability of the numerical weather prediction (NWP) model ICON (ICOsahedral Nonhydrostatic) with the extension ART (Aerosols and Reactive Trace gases) and the chemistry–climate model (CCM) EMAC (ECHAM5/MESSy Atmospheric Chemistry – fifth-generation European Centre Hamburg general circulation model/Modular Earth Submodel System) to model the UT–LMS composition of water vapour (H2O), ozone (O3), nitric acid (HNO3) and clouds. Within the scales resolved by the respective model, we find good overall agreement of both models with GLORIA. The applied high-resolution ICON-ART set-up involving an R2B7 nest (local grid refinement with a horizontal resolution of about 20 km), covering the HALO flight region, reproduces mesoscale dynamical structures well. Narrow moist filaments in the LMS observed by GLORIA at tropopause gradients in the context of a Rossby wave breaking event and in the vicinity of an occluded Icelandic low are clearly reproduced by the model. Using ICON-ART, we show that a larger filament in the west was transported horizontally into the Arctic LMS in connection with a jet stream split associated with poleward breaking of a cyclonically sheared Rossby wave. Further weaker filaments are associated with an older tropopause fold in the east. Given the lower resolution (T106) of the nudged simulation of the EMAC model, we find that this model also reproduces these features well. Overall, trace gas mixing ratios simulated by both models are in a realistic range, and major cloud systems observed by GLORIA are mostly reproduced. However, we find both models to be affected by a well-known systematic moist bias in the LMS. Further biases are diagnosed in the ICON-ART O3, EMAC H2O and EMAC HNO3 distributions. Finally, we use sensitivity simulations to investigate (i) short-term cirrus cloud impacts on the H2O distribution (ICON-ART), (ii) the overall impact of polar winter chemistry and microphysical processing on O3 and HNO3 (ICON-ART and EMAC), (iii) the impact of the model resolution on simulated parameters (EMAC), and (iv) consequences of scavenging processes by cloud particles (EMAC). We find that changing the horizontal model resolution results in notable systematic changes for all species in the LMS, while scavenging processes play a role only in the case of HNO3. We discuss the model biases and deficits found in this case study that potentially affect forecasts and projections (adversely) and provide suggestions for further model improvements.

IASI (Infrared Atmospheric Sounding Interferometer) is the core instrument of the currently three Metop (Meteorological operational) satellites of EUMETSAT (European Organization for the Exploitation of Meteorological Satellites). The MUSICA IASI processing has been developed in the framework of the European Research Council project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water). The processor performs an optimal estimation of the vertical distributions of water vapour (H2O), the ratio between two water vapour isotopologues (the HDO/H2O ratio), nitrous oxide (N2O), methane (CH4), and nitric acid (HNO3) and works with IASI radiances measured under cloud-free conditions in the spectral window between 1190 and 1400 cm−1. The retrieval of the trace gas profiles is performed on a logarithmic scale, which allows the constraint and the analytic treatment of ln [HDO]−ln [H2O] as a proxy for the HDO/H2O ratio. Currently, the MUSICA IASI processing has been applied to all IASI measurements available between October 2014 and June 2021 and about two billion individual retrievals have been performed. Here we describe the MUSICA IASI full retrieval product data set. The data set is made available in the form of netCDF data files that are compliant with version 1.7 of the CF (Climate and Forecast) metadata convention. For each individual retrieval these files contain information on the a priori usage and constraint, the retrieved atmospheric trace gas and temperature profiles, profiles of the leading error components, and information on vertical representativeness in the form of the averaging kernels as well as averaging kernel metrics, which are more handy than the full kernels. We discuss data filtering options and give examples of the high horizontal and continuous temporal coverage of the MUSICA IASI data products. For each orbit an individual standard output data file is provided with comprehensive information for each individual retrieval, resulting in a rather large data volume (about 40 TB for the almost 7 years of data with global daily coverage). This, at a first glance, apparent drawback of large data files and data volume is counterbalanced by multiple possibilities of data reuse, which are briefly discussed. Examples of standard data output files and a README .pdf file informing users about access to the total data set are provided via https://doi.org/10.35097/408 (Schneider et al., 2021b). In addition, an extended output data file is made available via https://doi.org/10.35097/412 (Schneider et al., 2021a). It contains the same variables as the standard output files together with Jacobians (and spectral responses) for many different uncertainty sources and gain matrices (due to this additional variables it is called the extended output). We use these additional data for assessing the typical impact of different uncertainty sources – like surface emissivity or spectroscopic parameters – and different cloud types on the retrieval results. The extended output file is limited to 74 example observations (over a polar, mid-latitudinal, and tropical site); its data volume is only 73 MB, and it is thus recommended to users for having a quick look at the data.

The objective of this study is to derive methane (CH4) emissions from three landfills, which are found to be the most significant CH4 sources in the metropolitan area of Madrid in Spain. We derive CH4 emissions from the CH4 enhancements observed by spaceborne and ground-based instruments. We apply satellite-based measurements from the TROPOspheric Monitoring Instrument (TROPOMI) and the Infrared Atmospheric Sounding Interferometer (IASI) together with measurements from the ground-based COllaborative Carbon Column Observing Network (COCCON) instruments. In 2018, a 2-week field campaign for measuring the atmospheric concentrations of greenhouse gases was performed in Madrid in the framework of Monitoring of the Greenhouse Gases Concentrations in Madrid (MEGEI-MAD) project. Five COCCON instruments were deployed at different locations around the Madrid city center, enabling the observation of total column-averaged CH4 mixing ratios (XCH4). Considering the prevalent wind regimes, we calculate the wind-assigned XCH4 anomalies for two opposite wind directions. Pronounced bipolar plumes are found when applying the method to NO2, which implies that our method of wind-assigned anomaly is suitable to estimate enhancements of trace gases at the urban level from satellite-based measurements. For quantifying the CH4 emissions, the wind-assigned plume method is applied to the TROPOMI XCH4 and to the lower tropospheric CH4 / dry-air column ratio (TXCH4) of the combined TROPOMI+IASI product. As CH4 emission strength we estimate 7.4 × 1025 ± 6.4 × 1024 molec. s−1 from the TROPOMI XCH4 data and 7.1 × 1025 ± 1.0 × 1025 molec. s−1 from the TROPOMI+IASI merged TXCH4 data. We use COCCON observations to estimate the local source strength as an independent method. COCCON observations indicate a weaker CH4 emission strength of 3.7 × 1025 molec. s−1 from a local source (the Valdemingómez waste plant) based on observations from a single day. This strength is lower than the one derived from the satellite observations, and it is a plausible result. This is because the analysis of the satellite data refers to a larger area, covering further emission sources in the study region, whereas the signal observed by COCCON is generated by a nearby local source. All emission rates estimated from the different observations are significantly larger than the emission rates provided via the official Spanish Register of Emissions and Pollutant Sources.

We present a global and multi-annual space-borne dataset of tropospheric {H2O, δD} pairs that is based on radiance measurements from the nadir thermal infrared sensor IASI (Infrared Atmospheric Sounding Interferometer) on board the Metop satellites of EUMETSAT (European Organisation for the Exploitation of Meteorological Satellites). This dataset is an a posteriori processed extension of the MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water) IASI full product dataset as presented in Schneider et al. (2021b). From the independently retrieved H2O and δD proxy states, their a priori settings and constraints, and their error covariances provided by the IASI full product dataset, we generate an optimal estimation product for pairs of H2O and δD. Here, this standard MUSICA method for deriving {H2O, δD} pairs is extended using an a posteriori reduction of the constraints for improving the retrieval sensitivity at dry conditions. By applying this improved water isotopologue post-processing for all cloud-free MUSICA IASI retrievals, this yields a {H2O, δD} pair dataset for the whole period from October 2014 to December 2020 with global coverage twice per day (local morning and evening overpass times). In total, the dataset covers more than 1500 million individually processed observations. The retrievals are most sensitive to variations in {H2O, δD} pairs within the free troposphere, with up to 30 % of all retrievals containing vertical profile information in the {H2O, δD} pair product. After applying appropriate quality filters, the largest number of reliable pair data arises for tropical and subtropical summer regions, but higher latitudes also show a considerable amount of reliable data. Exemplary time series over the tropical Atlantic and West Africa are chosen to illustrate the potential of the MUSICA IASI {H2O, δD} pair data for atmospheric moisture pathway studies. Furthermore, in order to facilitate the application of this rather comprehensive MUSICA IASI {H2O, δD} pair dataset (referred to as Level-2), we additionally provide the data in a re-gridded and simplified format (Level-3) with focus on the quality-filtered {H2O, δD} pairs in the free troposphere. A technical documentation for guiding the use of both datasets is attached as the Supplement. Finally, the Level-2 dataset is referenced with the DOI https://doi.org/10.35097/415 (Diekmann et al., 2021a) and the Level-3 dataset with DOI https://doi.org/10.35097/495 (Diekmann et al., 2021b).

Measurements of the pollution trace gases ethane (C2H6), ethyne (C2H2), formic acid (HCOOH), and peroxyacetyl nitrate (PAN) were performed in the North Atlantic upper troposphere and lowermost stratosphere (UTLS) region with the airborne limb imager GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) with high spatial resolution down to cloud top. Observations were made during flights with the German research aircraft HALO (High Altitude and LOng Range Research Aircraft) in the frame of the WISE (Wave-driven ISentropic Exchange) campaign, which was carried out in autumn 2017 from Shannon (Ireland) and Oberpfaffenhofen (Germany). Enhanced volume mixing ratios (VMRs) of up to 2.2 ppbv C2H6, 0.2 ppbv C2H2, 0.9 ppbv HCOOH, and 0.4 ppbv PAN were detected during the flight on 13 September 2017 in the upper troposphere and around the tropopause above the British Isles. Elevated quantities of PAN were measured even in the lowermost stratosphere (locally up to 14 km), likely reflecting the fact that this molecule has the longest lifetime of the four species discussed herein. Backward trajectory calculations as well as global three-dimensional Chemical Lagrangian Model of the Stratosphere (CLaMS) simulations with artificial tracers of air mass origin have shown that the main sources of the observed pollutant species are forest fires in North America and anthropogenic pollution in South Asia and Southeast Asia uplifted and moved within the Asian monsoon anticyclone (AMA) circulation system. After release from the AMA, these species or their precursor substances are transported by strong tropospheric winds over large distances, depending on their particular atmospheric lifetime of up to months. Observations are compared to simulations with the atmospheric models EMAC (ECHAM5/MESSy Atmospheric Chemistry) and CAMS (Copernicus Atmosphere Monitoring Service). These models are qualitatively able to reproduce the measured VMR enhancements but underestimate the absolute amount of the increase. Increasing the emissions in EMAC by a factor of 2 reduces the disagreement between simulated and measured results and illustrates the importance of the quality of emission databases used in chemical models.

In this paper, we compare column-averaged dry-air mole fractions of water vapor (XH2O) retrievals from the COllaborative Carbon Column Observing Network (COCCON) with retrievals from two co-located high-resolution Fourier transform infrared (FTIR) spectrometers as references at two boreal sites, Kiruna, Sweden, and Sodankylä, Finland, from 6 March 2017 to 20 September 2019. In the framework of the Network for the Detection of Atmospheric Composition Change (NDACC), an FTIR spectrometer is operated at Kiruna. The H2O product derived from these observations has been generated with the MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water (MUSICA) processor. In Sodankylä, a Total Carbon Column Observing Network (TCCON) spectrometer is operated, and the official XH2O data as provided by TCCON are used for this study. The datasets are in good overall agreement, with COCCON data showing a wet bias of (49.20±58.61) ppm ((3.33±3.37) %, R2=0.9992) compared with MUSICA NDACC and (56.32±45.63) ppm ((3.44±1.77) %, R2=0.9997) compared with TCCON. Furthermore, the a priori H2O volume mixing ratio (VMR) profiles (MAP) used as a priori information in the TCCON retrievals (also adopted for COCCON retrievals) are evaluated with respect to radiosonde (Vaisala RS41) profiles at Sodankylä. The MAP and radiosonde profiles show similar shapes and a good linear correlation of integrated XH2O, indicating that MAP is a reasonable approximation of the true atmospheric state and an appropriate choice for the scaling retrieval methods as applied by COCCON and TCCON. COCCON shows a reduced dry bias (−14.96 %) in comparison with TCCON (−19.08 %) with respect to radiosonde XH2O. Finally, we investigate the quality of satellite data at high latitudes. For this purpose, the COCCON XH2O is compared with retrievals from the Infrared Atmospheric Sounding Interferometer (IASI) generated with the MUSICA processor (MUSICA IASI) and with retrievals from the TROPOspheric Monitoring Instrument (TROPOMI). Both paired datasets generally show good agreement and similar correlations at the two sites. COCCON measures 4.64 % less XH2O at Kiruna and 3.36 % less at Sodankylä with respect to MUSICA IASI, whereas COCCON measures 9.71 % more XH2O at Kiruna and 7.75 % more at Sodankylä compared with TROPOMI. Our study supports the assumption that COCCON also delivers a well-characterized XH2O data product. This emphasizes that this approach might complement the TCCON network with respect to satellite validation efforts. This is the first published study where COCCON XH2O has been compared with MUSICA NDACC and TCCON retrievals and has been used for MUSICA IASI and TROPOMI validation.

El futuro del sistema Tierra-atmósfera dependerá, en gran medida, de nuestra capacidad para entender todos los procesos que están conduciendo al calentamiento global, y sus consecuencias climáticas, y, en este contexto, los gases de efecto invernadero (GEIs) juegan un papel clave como uno de los principales motores del cambio climático. Con esta idea nace el proyecto de investigación INMENSE (IASI for Surveying Methane and Nitrous Oxide in the Troposphere), el cual tiene como objetivo mejorar nuestra compresión de los balances atmosféricos de dos de los más importantes GEIs, el metano (CH4) y el óxido nitroso (N2O). Para ello, el proyecto INMENSE ha generado nuevas observaciones de concentraciones de CH4 y N2O en la troposfera media/alta a escala global a partir de las medidas satelitales del sensor IASI (Infrared Atmospheric Sounding Interferometer), que vuela a bordo de los satélites meteorológicos EUMETSAT/Metop. En este trabajo los productos INMENSE IASI de CH4 y N2O son presentados, caracterizados y extensamente validados usando una base de datos de referencia multiplataforma (perfiles verticales de avión, medidas in-situ y remotas desde superficie). Esta completa validación sugiere que los productos IASI de CH4 y N2O tienen una precisión entre el 1-3% y un error sistemático del 2%, así como que son consistentes temporal y espacialmente. Por último, las observaciones IASI de CH4 y N2O sobre la Península Ibérica han sido comparadas a las simulaciones del modelo de transporte químico MOCAGE, analizando el grado de acuerdo entre ambas bases de datos.

The annual variation of δD in the tropical lower stratosphere is a critical indicator for the relative importance of different processes contributing to the transport of water vapour through the cold tropical tropopause region into the stratosphere. Distinct observational discrepancies of the δD annual variation were visible in the works of Steinwagner et al. (2010) and Randel et al. (2012). Steinwagner et al. (2010) analysed MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) observations retrieved with the IMK/IAA (Institut für Meteorologie und Klimaforschung in Karlsruhe, Germany, in collaboration with the Instituto de Astrofísica de Andalucía in Granada, Spain) processor, while Randel et al. (2012) focused on ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer) observations. Here we reassess the discrepancies based on newer MIPAS (IMK/IAA) and ACE-FTS data sets, also showing for completeness results from SMR (Sub-Millimetre Radiometer) observations and a ECHAM/MESSy (European Centre for Medium-Range Weather Forecasts Hamburg and Modular Earth Submodel System) Atmospheric Chemistry (EMAC) simulation (Eichinger et al., 2015b). Similar to the old analyses, the MIPAS data set yields a pronounced annual variation (maximum about 75 ‰), while that derived from the ACE-FTS data set is rather weak (maximum about 25 ‰). While all data sets exhibit the phase progression typical for the tape recorder, the annual maximum in the ACE-FTS data set precedes that in the MIPAS data set by 2 to 3 months. We critically consider several possible reasons for the observed discrepancies, focusing primarily on the MIPAS data set. We show that the δD annual variation in the MIPAS data up to an altitude of 40 hPa is substantially impacted by a “start altitude effect”, i.e. dependency between the lowermost altitude where MIPAS retrievals are possible and retrieved data at higher altitudes. In itself this effect does not explain the differences with the ACE-FTS data. In addition, there is a mismatch in the vertical resolution of the MIPAS HDO and H2O data (being consistently better for HDO), which actually results in an artificial tape-recorder-like signal in δD. Considering these MIPAS characteristics largely removes any discrepancies between the MIPAS and ACE-FTS data sets and shows that the MIPAS data are consistent with a δD tape recorder signal with an amplitude of about 25 ‰ in the lowermost stratosphere.

The Arctic winter 2015/16 was characterized by cold stratospheric temperatures. Here we present a comprehensive view of the temporal evolution of chlorine in the lowermost stratosphere over the course of the studied winter. We utilize two-dimensional vertical cross sections of ozone (O3) and chlorine nitrate (ClONO2), measured by the airborne limb imager GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) during the POLSTRACC/GW-LCYCLE II/GWEX/SALSA campaigns, to investigate the tropopause region in detail. Observations from three long-distance flights in January, February, and March 2016 are discussed. ClONO2 volume mixing ratios up to 1100 pptv were measured at 380 K potential temperature in mesoscale structures. Similar mesoscale structures are also visible in O3 measurements. Both trace gas measurements are applied to evaluate simulation results from the chemistry transport model CLaMS (Chemical Lagrangian Model of the Stratosphere) and the chemistry–climate model EMAC (ECHAM5/MESSy Atmospheric Chemistry). These comparisons show agreement within the expected performance of these models. Satellite measurements from Aura/MLS (Microwave Limb Sounder) and SCISAT/ACE-FTS (Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) provide an overview over the whole winter and information about the stratospheric situation above the flight altitude. Time series of these satellite measurements reveal unusually low hydrochloric acid (HCl) and ClONO2 at 380 K from the beginning of January to the end of February 2016, while chlorine monoxide (ClO) is strongly enhanced. In March 2016, unusually rapid chlorine deactivation into HCl is observed instead of deactivation into ClONO2, the more typical pathway for deactivation in the Arctic. Chlorine deactivation observed in the satellite time series is well reproduced by CLaMS. Sensitivity simulations with CLaMS demonstrate the influence of low abundances of O3 and reactive nitrogen (NOy) due to ozone depletion and sedimentation of NOy-containing particles, respectively. On the basis of the different altitude and time ranges of these effects, we conclude that the substantial chlorine deactivation into HCl at 380 K arose as a result of very low ozone abundances together with low temperatures. Additionally, CLaMS estimates ozone depletion of at least 0.4 ppmv at 380 K and 1.75 ppmv at 490 K, which is comparable to other extremely cold Arctic winters. We have used CLaMS trajectories to analyze the history of enhanced ClONO2 measured by GLORIA. In February, most of the enhanced ClONO2 is traced back to chlorine deactivation that had occurred within the past few days prior to the GLORIA measurement. In March, after the final warming, air masses in which chlorine has previously been deactivated into ClONO2 have been transported in the remnants of the polar vortex towards the location of measurement for at least 11 d.

Within the framework of the second SPARC (Stratosphere-troposphere Processes And their Role in Climate) water vapour assessment (WAVAS-II), profile-to-profile comparisons of stratospheric and lower mesospheric water vapour were performed by considering 33 data sets derived from satellite observations of 15 different instruments. These comparisons aimed to provide a picture of the typical biases and drifts in the observational database and to identify data-set-specific problems. The observational database typically exhibits the largest biases below 70 hPa, both in absolute and relative terms. The smallest biases are often found between 50 and 5 hPa. Typically, they range from 0.25 to 0.5 ppmv (5 % to 10 %) in this altitude region, based on the 50 % percentile over the different comparison results. Higher up, the biases increase with altitude overall but this general behaviour is accompanied by considerable variations. Characteristic values vary between 0.3 and 1 ppmv (4 % to 20 %). Obvious data-set-specific bias issues are found for a number of data sets. In our work we performed a drift analysis for data sets overlapping for a period of at least 36 months. This assessment shows a wide range of drifts among the different data sets that are statistically significant at the 2σ uncertainty level. In general, the smallest drifts are found in the altitude range between about 30 and 10 hPa. Histograms considering results from all altitudes indicate the largest occurrence for drifts between 0.05 and 0.3 ppmv decade−1. Comparisons of our drift estimates to those derived from comparisons of zonal mean time series only exhibit statistically significant differences in slightly more than 3 % of the comparisons. Hence, drift estimates from profile-to-profile and zonal mean time series comparisons are largely interchangeable. As for the biases, a number of data sets exhibit prominent drift issues. In our analyses we found that the large number of MIPAS data sets included in the assessment affects our general results as well as the bias summaries we provide for the individual data sets. This is because these data sets exhibit a relative similarity with respect to the remaining data sets, despite the fact that they are based on different measurement modes and different processors implementing different retrieval choices. Because of that, we have by default considered an aggregation of the comparison results obtained from MIPAS data sets. Results without this aggregation are provided on multiple occasions to characterise the effects due to the numerous MIPAS data sets. Among other effects, they cause a reduction of the typical biases in the observational database.

Within the framework of the second SPARC (Stratosphere-troposphere Processes And their Role in Climate) water vapour assessment (WAVAS-II), we evaluated five data sets of δD(H2O) obtained from observations by Odin/SMR (Sub-Millimetre Radiometer), Envisat/MIPAS (Environmental Satellite/Michelson Interferometer for Passive Atmospheric Sounding), and SCISAT/ACE-FTS (Science Satellite/Atmospheric Chemistry Experiment – Fourier Transform Spectrometer) using profile-to-profile and climatological comparisons. These comparisons aimed to provide a comprehensive overview of typical uncertainties in the observational database that could be considered in the future in observational and modelling studies. Our primary focus is on stratospheric altitudes, but results for the upper troposphere and lower mesosphere are also shown. There are clear quantitative differences in the measurements of the isotopic ratio, mainly with regard to comparisons between the SMR data set and both the MIPAS and ACE-FTS data sets. In the lower stratosphere, the SMR data set shows a higher depletion in δD than the MIPAS and ACE-FTS data sets. The differences maximise close to 50 hPa and exceed 200 ‰. With increasing altitude, the biases decrease. Above 4 hPa, the SMR data set shows a lower δD depletion than the MIPAS data sets, occasionally exceeding 100 ‰. Overall, the δD biases of the SMR data set are driven by HDO biases in the lower stratosphere and by H2O biases in the upper stratosphere and lower mesosphere. In between, in the middle stratosphere, the biases in δD are the result of deviations in both HDO and H2O. These biases are attributed to issues with the calibration, in particular in terms of the sideband filtering, and uncertainties in spectroscopic parameters. The MIPAS and ACE-FTS data sets agree rather well between about 100 and 10 hPa. The MIPAS data sets show less depletion below approximately 15 hPa (up to about 30 ‰), due to differences in both HDO and H2O. Higher up this behaviour is reversed, and towards the upper stratosphere the biases increase. This is driven by increasing biases in H2O, and on occasion the differences in δD exceed 80 ‰. Below 100 hPa, the differences between the MIPAS and ACE-FTS data sets are even larger. In the climatological comparisons, the MIPAS data sets continue to show less depletion in δD than the ACE-FTS data sets below 15 hPa during all seasons, with some variations in magnitude. The differences between the MIPAS and ACE-FTS data have multiple causes, such as differences in the temporal and spatial sampling (except for the profile-to-profile comparisons), cloud influence, vertical resolution, and the microwindows and spectroscopic database chosen. Differences between data sets from the same instrument are typically small in the stratosphere. Overall, if the data sets are considered together, the differences in δD among them in key areas of scientific interest (e.g. tropical and polar lower stratosphere, lower mesosphere, and upper troposphere) are too large to draw robust conclusions on atmospheric processes affecting the water vapour budget and distribution, e.g. the relative importance of different mechanisms transporting water vapour into the stratosphere.

Time series of stratospheric and lower mesospheric water vapour using 33 data sets from 15 different satellite instruments were compared in the framework of the second SPARC (Stratosphere-troposphere Processes And their Role in Climate) water vapour assessment (WAVAS-II). This comparison aimed to provide a comprehensive overview of the typical uncertainties in the observational database that can be considered in the future in observational and modelling studies, e.g addressing stratospheric water vapour trends. The time series comparisons are presented for the three latitude bands, the Antarctic (80°–70° S), the tropics (15° S–15° N) and the Northern Hemisphere mid-latitudes (50°–60° N) at four different altitudes (0.1, 3, 10 and 80 hPa) covering the stratosphere and lower mesosphere. The combined temporal coverage of observations from the 15 satellite instruments allowed the consideration of the time period 1986–2014. In addition to the qualitative comparison of the time series, the agreement of the data sets is assessed quantitatively in the form of the spread (i.e. the difference between the maximum and minimum volume mixing ratios among the data sets), the (Pearson) correlation coefficient and the drift (i.e. linear changes of the difference between time series over time). Generally, good agreement between the time series was found in the middle stratosphere while larger differences were found in the lower mesosphere and near the tropopause. Concerning the latitude bands, the largest differences were found in the Antarctic while the best agreement was found for the tropics. From our assessment we find that most data sets can be considered in future observational and modelling studies, e.g. addressing stratospheric and lower mesospheric water vapour variability and trends, if data set specific characteristics (e.g. drift) and restrictions (e.g. temporal and spatial coverage) are taken into account.

We present model simulations with the atmospheric chemistry–climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC) nudged toward European Centre for Medium-Range Weather Forecasts (ECMWF) ERA-Interim reanalyses for the Arctic winters 2009/2010 and 2010/2011. This study is the first to perform an extensive assessment of the performance of the EMAC model for Arctic winters as previous studies have only made limited evaluations of EMAC simulations which also were mainly focused on the Antarctic winter stratosphere. We have chosen the two extreme Arctic winters 2009/2010 and 2010/2011 to evaluate the formation of polar stratospheric clouds (PSCs) and the representation of the chemistry and dynamics of the polar winter stratosphere in EMAC. The EMAC simulations are compared to observations by the Michelson Interferometer for Passive Atmospheric Soundings (Envisat/MIPAS) and the observations from the Aura Microwave Limb Sounder (Aura/MLS). The Arctic winter 2010/2011 was one of the coldest stratospheric winters on record, leading to the strongest depletion of ozone measured in the Arctic. The Arctic winter 2009/2010 was, from the climatological perspective, one of the warmest stratospheric winters on record. However, it was distinguished by an exceptionally cold stratosphere (colder than the climatological mean) from mid-December 2009 to mid-January 2010, leading to prolonged PSC formation and existence. Significant denitrification, the removal of HNO3 from the stratosphere by sedimentation of HNO3-containing polar stratospheric cloud particles, occurred in that winter. In our comparison, we focus on PSC formation and denitrification. The comparisons between EMAC simulations and satellite observations show that model and measurements compare well for these two Arctic winters (differences for HNO3 generally within ±20 %) and thus that EMAC nudged toward ECMWF ERA-Interim reanalyses is capable of giving a realistic representation of the evolution of PSCs and associated sequestration of gas-phase HNO3 in the polar winter stratosphere. However, simulated PSC volume densities are smaller than the ones derived from Envisat/MIPAS observations by a factor of 3–7. Further, PSCs in EMAC are not simulated as high up (in altitude) as they are observed. This underestimation of PSC volume density and vertical extension of the PSCs results in an underestimation of the vertical redistribution of HNO3 due to denitrification/re-nitrification. The differences found here between model simulations and observations stipulate further improvements in the EMAC set-up for simulating PSCs.

The 2015/2016 Arctic winter was one of the coldest stratospheric winters in recent years. A stable vortex formed by early December and the early winter was exceptionally cold. Cold pool temperatures dropped below the nitric acid trihydrate (NAT) existence temperature of about 195 K, thus allowing polar stratospheric clouds (PSCs) to form. The low temperatures in the polar stratosphere persisted until early March, allowing chlorine activation and catalytic ozone destruction. Satellite observations indicate that sedimentation of PSC particles led to denitrification as well as dehydration of stratospheric layers. Model simulations of the 2015/2016 Arctic winter nudged toward European Centre for Medium-Range Weather Forecasts (ECMWF) analysis data were performed with the atmospheric chemistry–climate model ECHAM5/MESSy Atmospheric Chemistry (EMAC) for the Polar Stratosphere in a Changing Climate (POLSTRACC) campaign. POLSTRACC is a High Altitude and Long Range Research Aircraft (HALO) mission aimed at the investigation of the structure, composition and evolution of the Arctic upper troposphere and lower stratosphere (UTLS). The chemical and physical processes involved in Arctic stratospheric ozone depletion, transport and mixing processes in the UTLS at high latitudes, PSCs and cirrus clouds are investigated. In this study, an overview of the chemistry and dynamics of the 2015/2016 Arctic winter as simulated with EMAC is given. Further, chemical–dynamical processes such as denitrification, dehydration and ozone loss during the 2015/2016 Arctic winter are investigated. Comparisons to satellite observations by the Aura Microwave Limb Sounder (Aura/MLS) as well as to airborne measurements with the Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) performed aboard HALO during the POLSTRACC campaign show that the EMAC simulations nudged toward ECMWF analysis generally agree well with observations. We derive a maximum polar stratospheric O3 loss of ∼ 2 ppmv or 117 DU in terms of column ozone in mid-March. The stratosphere was denitrified by about 4–8 ppbv HNO3 and dehydrated by about 0.6–1 ppmv H2O from the middle to the end of February. While ozone loss was quite strong, but not as strong as in 2010/2011, denitrification and dehydration were so far the strongest observed in the Arctic stratosphere in at least the past 10 years.

In the framework of the second SPARC (Stratosphere-troposphere Processes And their Role in Climate) water vapour assessment (WAVAS-II), the amplitudes and phases of the annual, semi-annual and quasi-biennial variation in stratospheric and lower mesospheric water were compared using 30 data sets from 13 different satellite instruments. These comparisons aimed to provide a comprehensive overview of the typical uncertainties in the observational database which can be considered in subsequent observational and modelling studies. For the amplitudes, a good agreement of their latitude and altitude distribution was found. Quantitatively there were differences in particular at high latitudes, close to the tropopause and in the lower mesosphere. In these regions, the standard deviation over all data sets typically exceeded 0.2 ppmv for the annual variation and 0.1 ppmv for the semi-annual and quasi-biennial variation. For the phase, larger differences between the data sets were found in the lower mesosphere. Generally the smallest phase uncertainties can be observed in regions where the amplitude of the variability is large. The standard deviations of the phases for all data sets were typically smaller than a month for the annual and semi-annual variation and smaller than 5 months for the quasi-biennial variation. The amplitude and phase differences among the data sets are caused by a combination of factors. In general, differences in the temporal variation of systematic errors and in the observational sampling play a dominant role. In addition, differences in the vertical resolution of the data, the considered time periods and influences of clouds, aerosols as well as non-local thermodynamic equilibrium (NLTE) effects cause differences between the individual data sets.

More than a decade ago it was suggested that a cooling of stratospheric temperatures by 1 K or an increase of 1 ppmv of stratospheric water vapour could promote denitrification, the permanent removal of nitrogen species from the stratosphere by solid polar stratospheric cloud (PSC) particles. In fact, during the two Arctic winters 2009/10 and 2010/11 the strongest denitrification in the recent decade was observed. Sensitivity studies along air parcel trajectories are performed to test how a future stratospheric water vapour (H2O) increase of 1 ppmv or a temperature decrease of 1 K would affect PSC formation. We perform our study based on measurements made during the Arctic winter 2010/11. Air parcel trajectories were calculated 6 days backward in time based on PSCs detected by CALIPSO (Cloud Aerosol Lidar and Infrared Pathfinder satellite observations). The sensitivity study was performed on single trajectories as well as on a trajectory ensemble. The sensitivity study shows a clear prolongation of the potential for PSC formation and PSC existence when the temperature in the stratosphere is decreased by 1 K and water vapour is increased by 1 ppmv. Based on 15 years of satellite measurements (2000–2014) from UARS/HALOE, Envisat/MIPAS, Odin/SMR, Aura/MLS, Envisat/SCIAMACHY and SCISAT/ACE-FTS it is further investigated if there is a decrease in temperature and/or increase of water vapour (H2O) observed in the polar regions similar to that observed at midlatitudes and in the tropics. Performing linear regression analyses we derive from the Envisat/MIPAS (2002–2012) and Aura/MLS (2004–2014) observations predominantly positive changes in the potential temperature range 350 to 1000 K. The linear changes in water vapour derived from Envisat/MIPAS observations are largely insignificant, while those from Aura/MLS are mostly significant. For the temperature neither of the two instruments indicate any significant changes. Given the strong inter-annual variation observed in water vapour and particular temperature the severe denitrification observed in 2010/11 cannot be directly related to any changes in water vapour and temperature since the millennium. However, the observations indicate a clear correlation between cold winters and enhanced water vapour mixing ratios. This indicates a connection between dynamical and radiative processes that govern water vapour and temperature in the Arctic lower stratosphere.

Record breaking loss of ozone (O3) in the Arctic stratosphere has been reported in winter–spring 2010/2011. We examine in detail the composition and transformations occurring in the Arctic polar vortex using total column and vertical profile data products for O3, bromine oxide (BrO), nitrogen dioxide (NO2), chlorine dioxide (OClO), and polar stratospheric clouds (PSC) retrieved from measurements made by SCIAMACHY (Scanning Imaging Absorption SpectroMeter for Atmospheric CHartography) on-board Envisat (Environmental Satellite), as well as total column ozone amount, retrieved from the measurements of GOME-2 (Global Ozone Monitoring Experiment) on MetOp-A (Meteorological Experimental Satellite). Similarly we use the retrieved data from DOAS (Differential Optical Absorption Spectroscopy) measurements made in Ny-Ålesund (78.55° N, 11.55° E). A chemical transport model (CTM) has been used to relate and compare Arctic winter–spring conditions in 2011 with those in the previous year. In late winter–spring 2010/2011 the chemical ozone loss in the polar vortex derived from SCIAMACHY observations confirms findings reported elsewhere. More than 70% of O3 was depleted by halogen catalytic cycles between the 425 and 525 K isentropic surfaces, i.e. in the altitude range ~16–20 km. In contrast, during the same period in the previous winter 2009/2010, a typical warm Arctic winter, only slightly more than 20% depletion occurred below 20 km, while 40% of O3 was removed above the 575 K isentrope (~23 km). This loss above 575 K is explained by the catalytic destruction by NOx descending from the mesosphere. In both Arctic winters 2009/2010 and 2010/2011, calculated O3 losses from the CTM are in good agreement to our observations and other model studies. The mid-winter 2011 conditions, prior to the catalytic cycles being fully effective, are also investigated. Surprisingly, a significant loss of O3 around 60%, previously not discussed in detail, is observed in mid-January 2011 below 500 K (~19 km) and sustained for approximately 1 week. The low O3 region had an exceptionally large spatial extent. The situation was caused by two independently evolving tropopause elevations over the Asian continent. Induced adiabatic cooling of the stratosphere favoured the formation of PSC, increased the amount of active chlorine for a short time, and potentially contributed to higher polar ozone loss later in spring.

The international research project RECONCILE has addressed central questions regarding polar ozone depletion, with the objective to quantify some of the most relevant yet still uncertain physical and chemical processes and thereby improve prognostic modelling capabilities to realistically predict the response of the ozone layer to climate change. This overview paper outlines the scope and the general approach of RECONCILE, and it provides a summary of observations and modelling in 2010 and 2011 that have generated an in many respects unprecedented dataset to study processes in the Arctic winter stratosphere. Principally, it summarises important outcomes of RECONCILE including (i) better constraints and enhanced consistency on the set of parameters governing catalytic ozone destruction cycles, (ii) a better understanding of the role of cold binary aerosols in heterogeneous chlorine activation, (iii) an improved scheme of polar stratospheric cloud (PSC) processes that includes heterogeneous nucleation of nitric acid trihydrate (NAT) and ice on non-volatile background aerosol leading to better model parameterisations with respect to denitrification, and (iv) long transient simulations with a chemistry-climate model (CCM) updated based on the results of RECONCILE that better reproduce past ozone trends in Antarctica and are deemed to produce more reliable predictions of future ozone trends. The process studies and the global simulations conducted in RECONCILE show that in the Arctic, ozone depletion uncertainties in the chemical and microphysical processes are now clearly smaller than the sensitivity to dynamic variability.

Although the links between stratospheric dynamics, climate and weather have been demonstrated, direct observations of stratospheric winds are lacking, in particular at altitudes above 30 km. We report observations of winds between 8 and 0.01 hPa (~35–80 km) from October 2009 to April 2010 by the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) on the International Space Station. The altitude range covers the region between 35–60 km where previous space-borne wind instruments show a lack of sensitivity. Both zonal and meridional wind components were obtained, though not simultaneously, in the latitude range from 30° S to 55° N and with a single profile precision of 7–9 m s–1 between 8 and 0.6 hPa and better than 20 m s–1 at altitudes above. The vertical resolution is 5–7 km except in the upper part of the retrieval range (10 km at 0.01 hPa). In the region between 1–0.05 hPa, an absolute value of the mean difference < 2 m s–1 is found between SMILES profiles retrieved from different spectroscopic lines and instrumental settings. Good agreement (absolute value of the mean difference of ~2 m s–1) is also found with the European Centre for Medium-Range Weather Forecasts (ECMWF) analysis in most of the stratosphere except for the zonal winds over the equator (difference > 5 m s−1). In the mesosphere, SMILES and ECMWF zonal winds exhibit large differences (> 20 m s–1), especially in the tropics. We illustrate our results by showing daily and monthly zonal wind variations, namely the semi-annual oscillation in the tropics and reversals of the flow direction between 50–55° N during sudden stratospheric warmings. The daily comparison with ECMWF winds reveals that in the beginning of February, a significantly stronger zonal westward flow is measured in the tropics at 2 hPa compared to the flow computed in the analysis (difference of ~20 m s–1). The results show that the comparison between SMILES and ECMWF winds is not only relevant for the quality assessment of the new SMILES winds, but it also provides insights on the quality of the ECMWF winds themselves. Although the instrument was not specifically designed for measuring winds, the results demonstrate that space-borne sub-mm wave radiometers have the potential to provide good quality data for improving the stratospheric winds in atmospheric models.

A modified form of tracer–tracer correlations of N2O and O3 has been used as a tool for the evaluation of atmospheric photochemical models. Applying this method, monthly averages of N2O and O3 are derived for both hemispheres by partitioning the data into altitude (or potential temperature) bins and then averaging over a fixed interval of N2O. In a previous study, the method has been successfully applied to the evaluation of two chemical transport models (CTMs) and one chemistry–climate model (CCM) using a 1 yr climatology derived from the Odin Sub-Millimetre Radiometer (Odin/SMR). However, the applicability of a 1 yr climatology of monthly averages of N2O and O3 has been questioned due to the inability of some CCMs to simulate a specific year for the evaluation of CCMs. In this study, satellite measurements from Odin/SMR, the Aura Microwave Limb Sounder (Aura/MLS), the Michelson Interferometer for Passive Atmospheric Sounding on ENVISAT (ENVISAT/MIPAS), and the Cryogenic Infrared Spectrometers and Telescopes for the Atmosphere (CRISTA-1 and CRISTA-2) as well as model simulations from the Whole Atmosphere Community Climate Model (WACCM) are considered. By using seven to eight years of satellite measurements derived between 2003 and 2010 from Odin/SMR, Aura/MLS, ENVISAT/MIPAS and six years of model simulations from WACCM, the interannual variability of lower stratospheric monthly averages of N2O and O3 is assessed. It is shown that the interannual variability of the monthly averages of N2O and O3 is low, and thus can be easily distinguished from model deficiencies. Furthermore, it is investigated why large differences are found between Odin/SMR observations and model simulations from the Karlsruhe Simulation Model of the Middle Atmosphere (KASIMA) and the atmospheric general circulation model ECHAM5/Messy1 for the Northern and Southern Hemisphere tropics (0° to 30° N and 0° to −30° S, respectively). The differences between model simulations and observations are most likely caused by an underestimation of the quasi-biennial oscillation and tropical upwelling by the models as well as due to biases and/or instrument noise from the satellite instruments. A realistic consideration of the QBO in the model reduces the differences between model simulation and observations significantly. Finally, an intercomparison between Odin/SMR, Aura/MLS, ENVISAT/MIPAS and WACCM was performed. The comparison shows that these data sets are generally in good agreement, although some known biases of the data sets are clearly visible in the monthly averages. Nevertheless, the differences caused by the uncertainties of the satellite data sets are sufficiently small and can be clearly distinguished from model deficiencies. Thus, the method applied in this study is not only a valuable tool for model evaluation, but also for satellite data intercomparisons.

The Department of Meteorology at Stockholm University operates the Esrange Rayleigh/Raman lidar at Esrange (68° N, 21° E) near the Swedish city of Kiruna. This paper describes the design and first measurements of the new pure rotational-Raman channel of the Esrange lidar. The Esrange lidar uses a pulsed Nd:YAG solid-state laser operating at 532 nm as light source with a repetition rate of 20 Hz and a pulse energy of 350 mJ. The minimum vertical resolution is 150 m and the integration time for one profile is 5000 shots. The newly implemented channel allows for measurements of atmospheric temperature at altitudes below 35 km and is currently optimized for temperature measurements between 180 and 200 K. This corresponds to conditions in the lower Arctic stratosphere during winter. In addition to the temperature measurements, the aerosol extinction coefficient and the aerosol backscatter coefficient at 532 nm can be measured independently. Our filter-based design minimizes the systematic error in the obtained temperature profile to less than 0.51 K. By combining rotational-Raman measurements (5–35 km height) and the integration technique (30–80 km height), the Esrange lidar is now capable of measuring atmospheric temperature profiles from the upper troposphere up to the mesosphere. With the improved setup, the system can be used to validate current lidar-based polar stratospheric cloud classification schemes. The new capability of the instrument measuring temperature and aerosol extinction furthermore enables studies of the thermal structure and variability of the upper troposphere/lower stratosphere. Although several lidars are operated at polar latitudes, there are few instruments that are capable of measuring temperature profiles in the troposphere, stratosphere, and mesosphere, as well as aerosols extinction in the troposphere and lower stratosphere with daylight capability.

Remote sensing measurements from the Cryogenic Infrared Spectrometers and Telescope for the Atmosphere – New Frontiers (CRISTA-NF) during a flight on 29 July 2006 are presented. This flight is part of the AMMA-SCOUT-O3 measurement campaign, where CRISTA-NF was deployed on the high-flying research aircraft M55-Geophysica. The flight path was located over Italy and the Mediterranean Sea and crossed over the subtropical jet twice. Measurements of temperature, and the volume mixing ratios of water vapor (H2O), ozone (O3), nitric acid (HNO3) and peroxyacetyl nitrate (PAN) are available with a vertical resolution of up to 500 m between about 6 to 21 km altitude. CRISTA-NF observes these trace gases simultaneously and provides a quasi-2-D view of the transition region between the troposphere and the stratosphere. The observation of these different trace gases allows to determine tropospheric and stratospheric air masses. As expected, higher abundances are found where the main source of the trace gases is located: in the stratosphere for O3 and in the troposphere for H2O and PAN. Tracer-tracer correlations between O3 and PAN are used to identify the mixed tropospheric and lowermost stratospheric air at the subtropical jet and around the thermal tropopause north of the jet. An intrusion of stratospheric air into the troposphere associated with the subtropical jet is found in the CRISTA-NF observations. The observations indicate that the intrusion is connected to a tropopause fold which is not resolved in the ECMWF analysis data. The intrusion was reproduced in a simulation with the Chemical Lagrangian Model of the Stratosphere (CLaMS). The CLaMS simulation shows, that the lowermost stratospheric air masses in the intrusion where transported along the the subtropical jet. The tropospheric air masses around the intrusion originate from the vicinity of the Asian monsoon anticyclone. This work discusses the nature of the observed processes at the subtropical jet based on the CRISTA-NF observations and the CLaMS simulation.

The type of Polar stratospheric clouds (PSCs) as well as their temporal and spatial extent are important for the occurrence of heterogeneous reactions in the polar stratosphere. The formation of PSCs depends strongly on temperature. However, the mechanisms of the formation of solid PSCs are still poorly understood. Recent satellite studies of Antarctic PSCs have shown that their formation can be associated with deep-tropospheric clouds which have the ability to cool the lower stratosphere radiatively and/or adiabatically. In the present study, lidar measurements aboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite were used to investigate whether the formation of Arctic PSCs can be associated with deep-tropospheric clouds as well. Deep-tropospheric cloud systems have a vertical extent of more than 6.5 km with a cloud top height above 7 km altitude. PSCs observed by CALIPSO during the Arctic winter 2007/2008 were classified according to their type (STS, NAT, or ice) and to the kind of underlying tropospheric clouds. Our analysis reveals that 172 out of 211 observed PSCs occurred in connection with tropospheric clouds. 72% of these 172 observed PSCs occurred above deep-tropospheric clouds. We also find that the type of PSC seems to be connected to the characteristics of the underlying tropospheric cloud system. During the Arctic winter 2007/2008 PSCs consisting of ice were mainly observed in connection with deep-tropospheric cloud systems while no ice PSC was detected above cirrus. Furthermore, we find no correlation between the occurrence of PSCs and the top temperature of tropospheric clouds. Thus, our findings suggest that Arctic PSC formation is connected to adiabatice cooling, i.e. dynamic effects rather than radiative cooling.

The sedimentation of HNO3 containing Polar Stratospheric Cloud (PSC) particles leads to a permanent removal of HNO3 and thus to a denitrification of the stratosphere, an effect which plays an important role in stratospheric ozone depletion. The polar vortex in the Arctic winter 2009/2010 was very cold and stable between end of December and end of January. Strong denitrification between 475 to 525 K was observed in the Arctic in mid of January by the Odin Sub Millimetre Radiometer (Odin/SMR). This was the strongest denitrification that had been observed in the entire Odin/SMR measuring period (2001–2010). Lidar measurements of PSCs were performed in the area of Kiruna, Northern Sweden with the IRF (Institutet för Rymdfysik) lidar and with the Esrange lidar in January 2010. The measurements show that PSCs were present over the area of Kiruna during the entire period of observations. The formation of PSCs during the Arctic winter 2009/2010 is investigated using a microphysical box model. Box model simulations are performed along air parcel trajectories calculated six days backward according to the PSC measurements with the ground-based lidar in the Kiruna area. From the temperature history of the backward trajectories and the box model simulations we find two PSC regions, one over Kiruna according to the measurements made in Kiruna and one north of Scandinavia which is much colder, reaching also temperatures below Tice. Using the box model simulations along backward trajectories together with the observations of Odin/SMR, Aura/MLS (Microwave Limb Sounder), CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) and the ground-based lidar we investigate how and by which type of PSC particles the denitrification that was observed during the Arctic winter 2009/2010 was caused. From our analysis we find that due to an unusually strong synoptic cooling event in mid January, ice particle formation on NAT may be a possible formation mechanism during that particular winter that may have caused the denitrification observed in mid January. In contrast, the denitrification that was observed in the beginning of January could have been caused by the sedimentation of NAT particles that formed on mountain wave ice clouds.

During the ASTAR (Arctic Study of Tropospheric Aerosol and Radiation) campaign nucleation mode particles (4 to 13 nm) were quite frequently observed at altitudes below 4000 m. However, in the upper free troposphere, nucleation mode particles were only observed once, namely during the flight on 24 May 2004 (7000 m). To investigate if vertical motion were the reason for this difference that on one particular day nucleation mode particles were observed but not on the other days we employ a microphysical box model. The box model simulations were performed along air parcel trajectories calculated 6-d backwards based on European Center for Medium-Range Weather Forecasts (ECMWF) meteorological analyses using state parameters such as pressure and temperature in combination with additional parameters such as vertical stability. Box model simulations were performed for the 24 May where nucleation mode particles were observed (nucleation event) as well as for the days with measurements before and after (22 and 26 May) which are representative for no nucleation (non-nucleation event). A nucleation burst was simulated along all trajectories, however, in the majority of the simulations the nucleation rate was either too low or too high so that no nucleation mode particles were left at the time when the measurements were performed. Further, the simulation results could be divided into three cases. Thereby, we found that for case 1 the temperature was the only driving mechanism for the formation of new particles while for case 2 and 3 vertical motion have influenced the formation of new particles. The reason why nucleation mode particles were observed on 24 May, but not on the other days, can be explained by the conditions under which particle formation occurred. On 24 May the particle formation was caused by a slow updraft, while on the other two days the particle formation was caused by a fast updraft.

1-year data sets of monthly averaged nitrous oxide (N2O) and ozone (O3) derived from satellite measurements were used as a tool for the evaluation of atmospheric photochemical models. Two 1-year data sets, one solar occultation data set derived from the Improved Limb Atmospheric Spectrometer (ILAS and ILAS-II) and one limb sounding data set derived from the Odin Sub-Millimetre Radiometer (Odin/SMR) were employed. Here, these data sets are used for the evaluation of two Chemical Transport Models (CTMs), the Karlsruhe Simulation Model of the Middle Atmosphere (KASIMA) and the Chemical Lagrangian Model of the Stratosphere (CLaMS) as well as for one Chemistry-Climate Model (CCM), the atmospheric chemistry general circulation model ECHAM5/MESSy1 (E5M1) in the lower stratosphere with focus on the Northern Hemisphere. Since the Odin/SMR measurements cover the entire hemisphere, the evaluation is performed for the entire hemisphere as well as for the low latitudes, midlatitudes and high latitudes using the Odin/SMR 1-year data set as reference. To assess the impact of using different data sets for such an evaluation study we repeat the evaluation for the polar lower stratosphere using the ILAS/ILAS-II data set. Only small differences were found using ILAS/ILAS-II instead of Odin/SMR as a reference, thus, showing that the results are not influenced by the particular satellite data set used for the evaluation. The evaluation of CLaMS, KASIMA and E5M1 shows that all models are in agreement with Odin/SMR and ILAS/ILAS-II. Differences are generally in the range of ±20%. Larger differences (up to −40%) are found in all models at 500±25 K for N2O mixing ratios greater than 200 ppbv, thus in air masses of tropical character. Generally, the largest differences were found for the tropics and the lowest for the polar regions. However, an underestimation of polar winter ozone loss was found both in KASIMA and E5M1 both in the Northern and Southern Hemisphere.

During the CRISTA-1 mission three pronounced fingerlike structures reaching from the lower latitudes to the mid-latitudes, so-called streamers, were observed in the measurements of several trace gases in early November 1994. A simulation of these streamers in previous studies employing the KASIMA (Karlsruhe Simulation Model of the Middle Atmosphere) and ROSE (Research on Ozone in the Stratosphere and its Evolution) model, both being Eulerian models, show that their formation is due to adiabatic transport processes. Here, the impact of mixing on the development of these streamers is investigated. These streamers were simulated with the CLaMS model (Chemical Lagrangian Model of the Stratosphere), a Lagrangian model, using N2O as long-lived tracer. Using several different initialisations the results were compared to the KASIMA simulations and CRISTA (Cryogenic Infrared Spectrometer and Telescope for the Atmosphere) observations. Further, since the KASIMA model was employed to derive a 9-year climatology, the quality of the reproduction of streamers from such a study was tested by the comparison of the KASIMA results with CLaMS and CRISTA. The streamers are reproduced well for the Northern Hemisphere in the simulations of CLaMS and KASIMA for the 6 November 1994. However, in the CLaMS simulation a stronger filamentation is found while larger discrepancies between KASIMA and CRISTA were found especially for the Southern Hemisphere. Further, compared to the CRISTA observations the mixing ratios of N2O are in general underestimated in the KASIMA simulations. An improvement of the simulations with KASIMA was obtained for a simulation time according to the length of the CLaMS simulation. To quantify the differences between the simulations with CLaMS and KASIMA, and the CRISTA observations, the probability density function technique (PDF) is used to interpret the tracer distributions. While in the PDF of the KASIMA simulation the small scale structures observed by CRISTA are smoothed out due to the numerical diffusion in the model, the PDFs derived from CRISTA observations can be reproduced by CLaMS by optimising the mixing parameterisation. Further, this procedure gives information on small-scale variabilities not resolved by the CRISTA observations.