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A new upper stratospheric (35–60 km) temperature data product has been produced using Optical Spectrograph and InfraRed Imager System (OSIRIS) limb-scattered spectra that now spans over 22 years. Temperature is calculated by first estimating the Rayleigh scattering signal and then integrating hydrostatic balance combined with the ideal gas law. Uncertainties are estimated to be 1–5 K, with a vertical resolution of 3–4 km. Correlative comparisons with the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) and the Microwave Limb Sounder on Aura (MLS) are consistent with these uncertainty estimates and generally have no regions of statistically significant drift. The data product has been publicly released as part of the nominal OSIRIS v7.3 processing.

Air quality measurements from geostationary orbit by the instrument TEMPO (Tropospheric Emissions: Monitoring of Pollution) will offer an unprecedented view of atmospheric composition over North America. Measurements over Canadian latitudes, however, offer unique challenges: TEMPO's lines of sight are shallower, the sun is lower, and snow cover is more common. All of these factors increase the impact of the sphericity and the horizontal inhomogeneity of the atmosphere on the accuracy of the air quality measurements. Air mass factors encapsulate the complex paths of the measured sunlight, but traditionally they ignore horizontal variability. For the high spatial resolution of modern instruments such as TEMPO, the error due to neglecting horizontal variability is magnified and needs to be characterized. Here we present developments to SASKTRAN, the radiative transfer framework developed at the University of Saskatchewan, to calculate air mass factors in a spherical atmosphere, with and without consideration of horizontal inhomogeneity. Recent upgrades to SASKTRAN include first-order spherical corrections for the discrete ordinates method and the capacity to compute air mass factors with the Monte Carlo method. Together with finite-difference air mass factors via the successive orders method, this creates a robust framework for computing air mass factors. One-dimensional air mass factors from all three methods are compared in detail and are found to be in good agreement. Two-dimensional air mass factors are computed with the deterministic successive orders method, demonstrating an alternative for a calculation which would typically be done only with a nondeterministic Monte Carlo method. The two-dimensional air mass factors are used to analyze a simulated TEMPO-like measurement over Canadian latitudes. The effect of a sharp horizontal feature in surface albedo and NO2 was quantified while varying the distance of the feature from the intended measurement location. Such a feature in the surface albedo or NO2 could induce errors on the order of 5 % to 10 % at a distance of 50 km, and their combination could induce errors on the order of 10 % as far as 100 km away.

Trends in stratospheric trace gases like HCl, N2O, O3, and NOy show a hemispheric asymmetry over the last 2 decades, with trends having opposing signs in the Northern Hemisphere and Southern Hemisphere. Here we use N2O, a long-lived tracer with a tropospheric source, as a proxy for stratospheric circulation in the multiple linear regression model used to calculate stratospheric trace gas trends. This is done in an effort to isolate trends due to circulation changes from trends due to the chemical effects of ozone-depleting substances. Measurements from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) and the Optical Spectrograph and InfraRed Imager System (OSIRIS) are considered, along with model results from the Whole Atmosphere Community Climate Model (WACCM). Trends in HCl, O3, and NOy for 2004–2018 are examined. Using the N2O regression proxy, we show that observed HCl increases in the Northern Hemisphere are due to changes in the stratospheric circulation. We also show that negative O3 trends above 30 hPa in the Northern Hemisphere can be explained by a change in the circulation but that negative ozone trends at lower levels cannot. Trends in stratospheric NOy are found to be largely consistent with trends in N2O.

The Limb Imaging Fourier Transform Spectrometer Experiment (LIFE) instrument is a balloon-borne prototype of a satellite instrument designed to take vertical images of atmospheric limb emission spectra in the 700–1400 cm−1 wavenumber range from the upper-troposphere–lower-stratosphere (UTLS) altitude region of the atmosphere. The prototype builds on the success of past and existing instruments while reducing the complexity of the imaging design. This paper details the results of a demonstration flight on a stabilized stratospheric balloon gondola from Timmins, Canada, in August 2019. Retrievals of vertical trace gas profiles for the important greenhouse gases H2O, O3, CH4, and N2O, as well as HNO3, are performed using an optimal estimation approach and the SASKTRAN radiative transfer model. The retrieved profiles are compared to approximately coincident observations made by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) solar occultation and Microwave Limb Sounder (MLS) instruments. An evaluation of the LIFE measurements is performed, and areas of improvement are identified. This work increases the overall technical readiness of the approach for future balloon, aircraft, and space applications.

In this paper, we present the updated SAGE-CCI-OMPS+ climate data record of monthly zonal mean ozone profiles. This dataset covers the stratosphere and combines measurements by nine limb and occultation satellite instruments – SAGE II (Stratospheric Aerosol and Gases Experiment II), OSIRIS (Optical Spectrograph and InfraRed Imaging System), MIPAS (Michelson Interferometer for Passive Atmospheric Sounding), SCIAMACHY (SCanning Imaging Spectrometer for Atmospheric CHartographY), GOMOS (Global Ozone Monitoring by Occultation of Stars), ACE-FTS (Atmospheric Chemistry Experiment Fourier Transform Spectrometer), OMPS-LP (Ozone Monitor Profiling Suite Limb Profiler), POAM (Polar Ozone and Aerosol Measurement) III, and SAGE III/ISS (Stratospheric Aerosol and Gases Experiment III on the International Space Station). Compared to the original version of the SAGE-CCI-OMPS dataset (Sofieva et al., 2017b), the update includes new versions of MIPAS, ACE-FTS, and OSIRIS datasets and introduces data from additional sensors (POAM III and SAGE III/ISS) and retrieval processors (OMPS-LP). In this paper, we show detailed intercomparisons of ozone profiles from different instruments and data versions, with a focus on the detection of possible drifts in the datasets. The SAGE-CCI-OMPS+ dataset has a better coverage of polar regions and of the upper troposphere and the lower stratosphere (UTLS) than the previous dataset. We also studied the influence of including new datasets on ozone trends, which are estimated using multiple linear regression. The changes in the merged dataset do not change the overall morphology of post-1997 ozone trends; statistically significant trends are observed in the upper stratosphere. The largest changes in ozone trends are observed in polar regions, especially in the Southern Hemisphere. The updated SAGE-CCI-OMPS+ dataset contains profiles of deseasonalized anomalies and ozone concentrations from 1984 to 2021, in 10∘ latitude bins from 90∘ S to 90∘ N and in the altitude range from 10 to 50 km. The dataset is open access and available at https://climate.esa.int/en/projects/ozone/data/ (last access: 9 March 2023) and at ftp://cci_web@ftp-ae.oma.be/esacci (ESA Climate Office; last access: 9 March 2023).

This study presents upper troposphere–lower stratosphere (UTLS) water vapour and ozone climatologies generated from 14 years (June 2004 to May 2018) of measurements made by three Canadian limb-viewing satellite instruments: the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), the Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (MAESTRO), and the Optical Spectrograph and InfraRed Imaging System (OSIRIS; ozone only). This selection of instruments was chosen to explore the capability of these Canadian instruments in representing the UTLS and to enable analysis of the impact of different measurement sampling patterns. The water vapour and ozone climatologies have been constructed using tropopause-relative potential temperature and equivalent-latitude coordinates in an effort to best represent the distribution of these two gases in the UTLS, which is characterized by a high degree of dynamic and geophysical variability. Zonal-mean multiyear-mean climatologies are provided with 5∘ equivalent latitude and 10 K potential temperature spacing and have been constructed on a monthly, seasonal (3-month), and yearly basis. These climatologies are examined in-depth for two 3-month periods, December–January–February and June–July–August, and are compared to reference climatologies constructed from the Canadian Middle Atmosphere Model 39-year specified dynamics (CMAM39-SD) run, subsampled to the times and locations of the satellite measurements, in order to evaluate the consistency of water vapour and ozone between the datasets. Specifically, this method of using a subsampled model addresses the impact of each instrument's measuring pattern and allows for the quantification of the influence of different measurement patterns on multiyear climatologies. This in turn permits a more consistent evaluation of the distributions of these two gas species, as assessed through the differences between the model and measurement climatologies. For water vapour, the average absolute relative difference between CMAM39-SD and ACE-FTS differed between the two versions of ACE-FTS by less than 8 %, while the MAESTRO climatologies were found to differ by 15 %–41 % from ACE-FTS, depending on the version of ACE-FTS and the season. When considering the ozone climatologies, those constructed from the two ACE-FTS versions agreed to within 2 % overall, and the OSIRIS ozone climatologies agreed with these to within 10 %. The MAESTRO ozone climatologies differ from those from ACE-FTS and OSIRIS by 30 %–35 % and 25 %, respectively, albeit with regions of better agreement within the UTLS. These findings indicate that this set of Canadian limb sounders yields generally similar water vapour and ozone distributions in the UTLS, with some exceptions for MAESTRO depending on the season and gas species.

The v7.2 NO2 retrieval for the Optical Spectrograph and InfraRed Imager System (OSIRIS) was designed to improve sensitivity in the upper troposphere–lower stratosphere (UTLS) and to reduce an observed low bias in the previous version, v6.0. The details of this retrieval are described and then the data are compared to coincident NO2 profiles from the Atmospheric Chemistry Experiment–Fourier Transform Spectrometer (ACE-FTS) and the Stratospheric Aerosol and Gas Experiment III on the International Space Station (SAGE III/ISS). The PRATMO photochemical box model was used to account for differences in the measurement times of the instruments: all datasets were scaled to the same local solar time of 12:00 LST. Coincident ACE-FTS and OSIRIS NO2 measurements agree within 20 % throughout much of the stratosphere. Coincident SAGE III/ISS and OSIRIS NO2 measurements also agree within 20 %, with OSIRIS biased low at all altitudes and latitudes. The ACE-FTS, OSIRIS, and SAGE III-ISS NO2 monthly zonal mean data show very similar variability in time at most altitude and latitudes.

After decades of depletion in the 20th century, near-global ozone now shows clear signs of recovery in the upper stratosphere. The ozone column, however, has remained largely constant since the turn of the century, mainly due to the evolution of lower stratospheric ozone. In the tropical lower stratosphere, ozone is expected to decrease as a consequence of enhanced upwelling driven by increasing greenhouse gas concentrations, and this is consistent with observations. There is recent evidence, however, that mid-latitude ozone continues to decrease as well, contrary to model predictions. These changes are likely related to dynamical variability, but the impact of changing circulation patterns on stratospheric ozone is not well understood. Here we use merged measurements from the Stratospheric Aerosol and Gas Experiment II (SAGE II), the Optical Spectrograph and InfraRed Imaging System (OSIRIS), and SAGE III on the International Space Station (SAGE III/ISS) to quantify ozone trends in the 2000–2021 period. We implement a sampling correction for the OSIRIS and SAGE III/ISS datasets and assess trend significance, taking into account the temporal differences with respect to Aura Microwave Limb Sounder data. We show that ozone has increased by 2 %–6 % in the upper and 1 %–3 % in the middle stratosphere since 2000, while lower stratospheric ozone has decreased by similar amounts. These decreases are significant in the tropics (>95 % confidence) but not necessarily at mid-latitudes (>80 % confidence). In the upper and middle stratosphere, changes since 2010 have pointed to hemispheric asymmetries in ozone recovery. Significant positive trends are present in the Southern Hemisphere, while ozone at northern mid-latitudes has remained largely unchanged in the last decade. These differences might be related to asymmetries and long-term variability in the Brewer–Dobson circulation. Circulation changes impact ozone in the lower stratosphere even more. In tropopause-relative coordinates, most of the negative trends in the tropics lose significance, highlighting the impacts of a warming troposphere and increasing tropopause altitudes.

Smoke from wildfires is a significant source of air pollution, which can adversely impact air quality and ecosystems downwind. With the recently increasing intensity and severity of wildfires, the threat to air quality is expected to increase. Satellite-derived biomass burning emissions can fill in gaps in the absence of aircraft or ground-based measurement campaigns and can help improve the online calculation of biomass burning emissions as well as the biomass burning emissions inventories that feed air quality models. This study focuses on satellite-derived NOx emissions using the high-spatial-resolution TROPOspheric Monitoring Instrument (TROPOMI) NO2 dataset. Advancements and improvements to the satellite-based determination of forest fire NOx emissions are discussed, including information on plume height and effects of aerosol scattering and absorption on the satellite-retrieved vertical column densities. Two common top-down emission estimation methods, (1) an exponentially modified Gaussian (EMG) and (2) a flux method, are applied to synthetic data to determine the accuracy and the sensitivity to different parameters, including wind fields, satellite sampling, noise, lifetime, and plume spread. These tests show that emissions can be accurately estimated from single TROPOMI overpasses. The effect of smoke aerosols on TROPOMI NO2 columns (via air mass factors, AMFs) is estimated, and these satellite columns and emission estimates are compared to aircraft observations from four different aircraft campaigns measuring biomass burning plumes in 2018 and 2019 in North America. Our results indicate that applying an explicit aerosol correction to the TROPOMI NO2 columns improves the agreement with the aircraft observations (by about 10 %–25 %). The aircraft- and satellite-derived emissions are in good agreement within the uncertainties. Both top-down emissions methods work well; however, the EMG method seems to output more consistent results and has better agreement with the aircraft-derived emissions. Assuming a Gaussian plume shape for various biomass burning plumes, we estimate an average NOx e-folding time of 2 ±1 h from TROPOMI observations. Based on chemistry transport model simulations and aircraft observations, the net emissions of NOx are 1.3 to 1.5 times greater than the satellite-derived NO2 emissions. A correction factor of 1.3 to 1.5 should thus be used to infer net NOx emissions from the satellite retrievals of NO2.

In this paper, we present the MErged GRIdded Dataset of Ozone Profiles (MEGRIDOP) in the stratosphere with a resolved longitudinal structure, which is derived from data from six limb and occultation satellite instruments: GOMOS, SCIAMACHY and MIPAS on Envisat, OSIRIS on Odin, OMPS on Suomi-NPP, and MLS on Aura. The merged dataset was generated as a contribution to the European Space Agency Climate Change Initiative Ozone project (Ozone_cci). The period of this merged time series of ozone profiles is from late 2001 until the end of 2018. The monthly mean gridded ozone profile dataset is provided in the altitude range from 10 to 50 km in bins of 10∘ latitude × 20∘ longitude. The merging is performed using deseasonalized anomalies. The created MEGRIDOP dataset can be used for analyses that probe our understanding of stratospheric chemistry and dynamics. To illustrate some possible applications, we created a climatology of ozone profiles with resolved longitudinal structure. We found zonal asymmetry in the climatological ozone profiles at middle and high latitudes associated with the polar vortex. At northern high latitudes, the amplitude of the seasonal cycle also has a longitudinal dependence. The MEGRIDOP dataset has also been used to evaluate regional vertically resolved ozone trends in the stratosphere, including the polar regions. It is found that stratospheric ozone trends exhibit longitudinal structures at Northern Hemisphere middle and high latitudes, with enhanced trends over Scandinavia and the Atlantic region. This agrees well with previous analyses and might be due to changes in dynamical processes related to the Brewer–Dobson circulation.

The Stratosphere-troposphere Processes and their Role in Climate (SPARC) Data Initiative (SPARC, 2017) performed the first comprehensive assessment of currently available stratospheric composition measurements obtained from an international suite of space-based limb sounders. The initiative's main objectives were (1) to assess the state of data availability, (2) to compile time series of vertically resolved, zonal monthly mean trace gas and aerosol fields, and (3) to perform a detailed intercomparison of these time series, summarizing useful information and highlighting differences among datasets. The datasets extend over the region from the upper troposphere to the lower mesosphere (300–0.1 hPa) and are provided on a common latitude–pressure grid. They cover 26 different atmospheric constituents including the stratospheric trace gases of primary interest, ozone (O3) and water vapor (H2O), major long-lived trace gases (SF6, N2O, HF, CCl3F, CCl2F2, NOy), trace gases with intermediate lifetimes (HCl, CH4, CO, HNO3), and shorter-lived trace gases important to stratospheric chemistry including nitrogen-containing species (NO, NO2, NOx, N2O5, HNO4), halogens (BrO, ClO, ClONO2, HOCl), and other minor species (OH, HO2, CH2O, CH3CN), and aerosol. This overview of the SPARC Data Initiative introduces the updated versions of the SPARC Data Initiative time series for the extended time period 1979–2018 and provides information on the satellite instruments included in the assessment: LIMS, SAGE I/II/III, HALOE, UARS-MLS, POAM II/III, OSIRIS, SMR, MIPAS, GOMOS, SCIAMACHY, ACE-FTS, ACE-MAESTRO, Aura-MLS, HIRDLS, SMILES, and OMPS-LP. It describes the Data Initiative's top-down climatological validation approach to compare stratospheric composition measurements based on zonal monthly mean fields, which provides upper bounds to relative inter-instrument biases and an assessment of how well the instruments are able to capture geophysical features of the stratosphere. An update to previously published evaluations of O3 and H2O monthly mean time series is provided. In addition, example trace gas evaluations of methane (CH4), carbon monoxide (CO), a set of nitrogen species (NO, NO2, and HNO3), the reactive nitrogen family (NOy), and hydroperoxyl (HO2) are presented. The results highlight the quality, strengths and weaknesses, and representativeness of the different datasets. As a summary, the current state of our knowledge of stratospheric composition and variability is provided based on the overall consistency between the datasets. As such, the SPARC Data Initiative datasets and evaluations can serve as an atlas or reference of stratospheric composition and variability during the “golden age” of atmospheric limb sounding. The updated SPARC Data Initiative zonal monthly mean time series for each instrument are publicly available and accessible via the Zenodo data archive (Hegglin et al., 2020).

A comprehensive inter-comparison of seven radiative transfer models in the limb scattering geometry has been performed. Every model is capable of accounting for polarization within a spherical atmosphere. Three models (GSLS, SASKTRAN-HR, and SCIATRAN) are deterministic, and four models (MYSTIC, SASKTRAN-MC, Siro, and SMART-G) are statistical using the Monte Carlo technique. A wide variety of test cases encompassing different atmospheric conditions, solar geometries, wavelengths, tangent altitudes, and Lambertian surface reflectances have been defined and executed for every model. For the majority of conditions it was found that the models agree to better than 0.2 % in the single-scatter test cases and better than 1 % in the scalar and vectorial test cases with multiple scattering included, with some larger differences noted at high values of surface reflectance. For the first time in limb geometry, the effect of atmospheric refraction was compared among four models that support it (GSLS, SASKTRAN-HR, SCIATRAN, and SMART-G). Differences among most models with multiple scattering and refraction enabled were less than 1 %, with larger differences observed for some models. Overall the agreement among the models with and without refraction is better than has been previously reported in both scalar and vectorial modes.

The Stratospheric Aerosol and Gas Experiment (SAGE) III has been operating on the International Space Station (ISS) since mid-2017. Nitrogen dioxide (NO2) number density profiles are routinely retrieved from SAGE III/ISS solar occultation measurements in the middle atmosphere. Although NO2 density varies throughout the day due to photochemistry, the standard SAGE NO2 retrieval algorithm neglects these variations along the instrument's line of sight by assuming that the number density has a constant gradient within a given vertical layer of the atmosphere. This assumption will result in a retrieval bias for a species like NO2 that changes rapidly across the terminator. In this work we account for diurnal variations in retrievals of NO2 from the SAGE III/ISS measurements, and we determine the impact of this algorithm improvement on the resulting NO2 number densities. The first step in applying the diurnal correction is to use publicly available SAGE III/ISS products to convert the retrieved number density profiles to optical depth profiles. The retrieval is then re-performed with a new matrix that applies photochemical scale factors for each point along the line of sight according to the changing solar zenith angle. In general NO2 that is retrieved by accounting for these diurnal variations is more than 10 % lower than the standard algorithm below 30 km. This effect is greatest in winter at high latitudes and generally greater for sunrise occultations than sunset. Comparisons with coincident profiles from the Optical Spectrograph and InfraRed Imager System (OSIRIS) show that NO2 from SAGE III/ISS is generally biased high; however the agreement improves by up to 20 % in the mid-stratosphere when diurnal variations are accounted for in the retrieval. We conclude that diurnal variations along the SAGE III/ISS line of sight are an important term to consider for NO2 analyses at altitudes below 30 km.

In this work, we analyze the seasonal dependence of ozone trends in the stratosphere using four long-term merged data sets, SAGE-CCI-OMPS, SAGE-OSIRIS-OMPS, GOZCARDS, and SWOOSH, which provide more than 30 years of monthly zonal mean ozone profiles in the stratosphere. We focus here on trends between 2000 and 2018. All data sets show similar results, although some discrepancies are observed. In the upper stratosphere, the trends are positive throughout all seasons and the majority of latitudes. The largest upper-stratospheric ozone trends are observed during local winter (up to 6 % per decade) and equinox (up to 3 % per decade) at mid-latitudes. In the equatorial region, we find a very strong seasonal dependence of ozone trends at all altitudes: the trends vary from positive to negative, with the sign of transition depending on altitude and season. The trends are negative in the upper-stratospheric winter (−1 % per decade to −2 % per decade) and in the lower-stratospheric spring (−2 % per decade to −4 % per decade), but positive (2 % per decade to 3 % per decade) at 30–35 km in spring, while the opposite pattern is observed in summer. The tropical trends below 25 km are negative and maximize during summer (up to −2 % per decade) and spring (up to −3 % per decade). In the lower mid-latitude stratosphere, our analysis points to a hemispheric asymmetry: during local summers and equinoxes, positive trends are observed in the south (+1 % per decade to +2 % per decade), while negative trends are observed in the north (−1 % per decade to −2 % per decade). We compare the seasonal dependence of ozone trends with available analyses of the seasonal dependence of stratospheric temperature trends. We find that ozone and temperature trends show positive correlation in the dynamically controlled lower stratosphere and negative correlation above 30 km, where photochemistry dominates. Seasonal trend analysis gives information beyond that contained in annual mean trends, which can be helpful in order to better understand the role of dynamical variability in short-term trends and future ozone recovery predictions.

Isentropic mixing across and above the subtropical jet is a significant mechanism for stratosphere–troposphere exchange. In this work, we show new observational evidence on the role of this process in moistening the lowermost stratosphere. The new measurement, obtained from the Spatial Heterodyne Observations of Water (SHOW) instrument during a demonstration flight on the NASA's ER-2 high-altitude research aircraft, captured an event of poleward water vapour transport, including a fine-scale (vertically <∼1 km) moist filament above the local tropopause in a high-spatial-resolution two-dimensional cross section of the water vapour distribution. Analysis of these measurements combined with ERA5 reanalysis data reveals that this poleward mixing of air with enhanced water vapour occurred in the region of a double tropopause following a large Rossby wave-breaking event. These new observations highlight the importance of high-resolution measurements in resolving processes that are important to the lowermost-stratosphere water vapour budget.

Stratospheric aerosols are of a great importance to the scientific community, predominantly because of their role in climate, but also because accurate knowledge of aerosol characteristics is relevant for trace gas retrievals from remote-sensing instruments. There are several data sets published which provide aerosol extinction coefficients in the stratosphere. However, for the instruments measuring in the limb-viewing geometry, the use of this parameter is associated with uncertainties resulting from the need to assume an aerosol particle size distribution (PSD) within the retrieval process. These uncertainties can be mitigated if PSD information is retrieved. While occultation instruments provide more accurate information on the aerosol extinction coefficient, in this study, it was shown that limb instruments are more sensitive to the smaller particles in the visible–near-infrared spectral range. However, the sensitivity of occultation instruments improves if the UV part of the wavelength spectrum is considered. A data set containing PSD information was recently retrieved from SCIAMACHY limb measurements and provides two parameters of the unimodal lognormal PSD for the SCIAMACHY operational period (2002–2012). In this study, the data set is expanded by aerosol extinction coefficients and Ångström exponents calculated from the retrieved PSD parameters. Parameter errors for the recalculated Ångström exponents and aerosol extinction coefficients are assessed using synthetic retrievals. For the extinction coefficient the resulting parameter error is within ±25 %, and for the Ångström exponent, it is better than 10 %. The SCIAMACHY aerosol extinction coefficients recalculated from PSD parameters are compared to those from SAGE II. The differences between the instruments vary from 0 % to 25 % depending on the wavelength. Ångström exponent comparison with SAGE II shows differences between 10 % at 31 km and 40 % at 18 km. Comparisons with SAGE II, however, suffer from the low number of collocated profiles. Furthermore, the Ångström exponents obtained from the limb-viewing instrument OSIRIS are used for the comparison. This comparison shows an average difference within 7 %. The time series of these differences do not show signatures of any remarkable events (e.g., volcanic eruptions or biomass burning events). In addition, the temporal behaviour of the Ångström exponent in the tropics is analyzed using the SCIAMACHY data set. It is shown that there is no trivial relation between the Ångström exponent value at a single wavelength pair and the PSD because the same value of Ångström exponent can be obtained from an infinite number of combinations of the PSD parameters.

The Spatial Heterodyne Observations of Water instrument (SHOW) is a limb-sounding satellite prototype that utilizes the Spatial Heterodyne Spectroscopy (SHS) technique, operating in a limb-viewing configuration, to observe limb-scattered sunlight in a vibrational band of water vapour within a spectral window from 1363 to 1366 nm. The goal is to retrieve high vertical and horizontal resolution measurements of water vapour in the upper troposphere and lower stratosphere. The prototype instrument has been configured for observations from NASA's ER-2 high-altitude airborne remote science airplane. Flying at a maximum altitude of ∼21.34 km with a maximum speed of ∼760 km h−1, the ER-2 provides a stable platform to simulate observations from a low-earth orbit satellite. Demonstration flights were performed from the ER-2 during an observation campaign from 15 to 22 July 2017. In this paper, we present the laboratory characterization work and the level 0 to level 1 processing of flight data that were obtained during an engineering flight performed on 18 July 2017. Water vapour profile retrievals are presented and compared to in situ radiosonde measurements made of the same approximate column of air. These measurements are used to validate the SHOW measurement concept and examine the sensitivity of the technique.

The Limb Profiler (LP) is a part of the Ozone Mapping and Profiler Suite launched on board of the Suomi NPP satellite in October 2011. The LP measures solar radiation scattered from the atmospheric limb in ultraviolet and visible spectral ranges between the surface and 80 km. These measurements of scattered solar radiances allow for the retrieval of ozone profiles from cloud tops up to 55 km. The LP started operational observations in April 2012. In this study we evaluate more than 5.5 years of ozone profile measurements from the OMPS LP processed with the new NASA GSFC version 2.5 retrieval algorithm. We provide a brief description of the key changes that had been implemented in this new algorithm, including a pointing correction, new cloud height detection, explicit aerosol correction and a reduction of the number of wavelengths used in the retrievals. The OMPS LP ozone retrievals have been compared with independent satellite profile measurements obtained from the Aura Microwave Limb Sounder (MLS), Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) and Odin Optical Spectrograph and InfraRed Imaging System (OSIRIS). We document observed biases and seasonal differences and evaluate the stability of the version 2.5 ozone record over 5.5 years. Our analysis indicates that the mean differences between LP and correlative measurements are well within required ±10 % between 18 and 42 km. In the upper stratosphere and lower mesosphere (> 43 km) LP tends to have a negative bias. We find larger biases in the lower stratosphere and upper troposphere, but LP ozone retrievals have significantly improved in version 2.5 compared to version 2 due to the implemented aerosol correction. In the northern high latitudes we observe larger biases between 20 and 32 km due to the remaining thermal sensitivity issue. Our analysis shows that LP ozone retrievals agree well with the correlative satellite observations in characterizing vertical, spatial and temporal ozone distribution associated with natural processes, like the seasonal cycle and quasi-biennial oscillations. We found a small positive drift ∼ 0.5 % yr−1 in the LP ozone record against MLS and OSIRIS that is more pronounced at altitudes above 35 km. This pattern in the relative drift is consistent with a possible 100 m drift in the LP sensor pointing detected by one of our altitude-resolving methods.

Ozone forms in the Earth's atmosphere from the photodissociation of molecular oxygen, primarily in the tropical stratosphere. It is then transported to the extratropics by the Brewer–Dobson circulation (BDC), forming a protective ozone layer around the globe. Human emissions of halogen-containing ozone-depleting substances (hODSs) led to a decline in stratospheric ozone until they were banned by the Montreal Protocol, and since 1998 ozone in the upper stratosphere is rising again, likely the recovery from halogen-induced losses. Total column measurements of ozone between the Earth's surface and the top of the atmosphere indicate that the ozone layer has stopped declining across the globe, but no clear increase has been observed at latitudes between 60° S and 60° N outside the polar regions (60–90°). Here we report evidence from multiple satellite measurements that ozone in the lower stratosphere between 60° S and 60° N has indeed continued to decline since 1998. We find that, even though upper stratospheric ozone is recovering, the continuing downward trend in the lower stratosphere prevails, resulting in a downward trend in stratospheric column ozone between 60° S and 60° N. We find that total column ozone between 60° S and 60° N appears not to have decreased only because of increases in tropospheric column ozone that compensate for the stratospheric decreases. The reasons for the continued reduction of lower stratospheric ozone are not clear; models do not reproduce these trends, and thus the causes now urgently need to be established.

In this paper, we present a merged dataset of ozone profiles from several satellite instruments: SAGE II on ERBS, GOMOS, SCIAMACHY and MIPAS on Envisat, OSIRIS on Odin, ACE-FTS on SCISAT, and OMPS on Suomi-NPP. The merged dataset is created in the framework of the European Space Agency Climate Change Initiative (Ozone_cci) with the aim of analyzing stratospheric ozone trends. For the merged dataset, we used the latest versions of the original ozone datasets. The datasets from the individual instruments have been extensively validated and intercompared; only those datasets which are in good agreement, and do not exhibit significant drifts with respect to collocated ground-based observations and with respect to each other, are used for merging. The long-term SAGE–CCI–OMPS dataset is created by computation and merging of deseasonalized anomalies from individual instruments. The merged SAGE–CCI–OMPS dataset consists of deseasonalized anomalies of ozone in 10° latitude bands from 90° S to 90° N and from 10 to 50 km in steps of 1 km covering the period from October 1984 to July 2016. This newly created dataset is used for evaluating ozone trends in the stratosphere through multiple linear regression. Negative ozone trends in the upper stratosphere are observed before 1997 and positive trends are found after 1997. The upper stratospheric trends are statistically significant at midlatitudes and indicate ozone recovery, as expected from the decrease of stratospheric halogens that started in the middle of the 1990s and stratospheric cooling.

Ozone profile trends over the period 2000 to 2016 from several merged satellite ozone data sets and from ground-based data measured by four techniques at stations of the Network for the Detection of Atmospheric Composition Change indicate significant ozone increases in the upper stratosphere, between 35 and 48 km altitude (5 and 1 hPa). Near 2 hPa (42 km), ozone has been increasing by about 1.5 % per decade in the tropics (20° S to 20° N), and by 2 to 2.5 % per decade in the 35 to 60° latitude bands of both hemispheres. At levels below 35 km (5 hPa), 2000 to 2016 ozone trends are smaller and not statistically significant. The observed trend profiles are consistent with expectations from chemistry climate model simulations. This study confirms positive trends of upper stratospheric ozone already reported, e.g., in the WMO/UNEP Ozone Assessment 2014 or by Harris et al. (2015). Compared to those studies, three to four additional years of observations, updated and improved data sets with reduced drift, and the fact that nearly all individual data sets indicate ozone increase in the upper stratosphere, all give enhanced confidence. Uncertainties have been reduced, for example for the trend near 2 hPa in the 35 to 60° latitude bands from about ±5 % (2σ) in Harris et al. (2015) to less than ±2 % (2σ). Nevertheless, a thorough analysis of possible drifts and differences between various data sources is still required, as is a detailed attribution of the observed increases to declining ozone-depleting substances and to stratospheric cooling. Ongoing quality observations from multiple independent platforms are key for verifying that recovery of the ozone layer continues as expected.

CMAM30 is a 30-year data set extending from 1979 to 2010 that is generated using a version of the Canadian Middle Atmosphere Model (CMAM) in which the winds and temperatures are relaxed to the Interim Reanalysis product from the European Centre for Medium-Range Weather Forecasts (ERA-Interim). The data set has dynamical fields that are very close to the reanalysis below 1 hPa and chemical tracers that are self-consistent with respect to the model winds and temperature. The chemical tracers are expected to be close to actual observations. The data set is here compared to two satellite records – the Atmospheric Chemistry Experiment Fourier transform spectrometer and the Odin Optical Spectrograph and Infrared Imaging System – for the purpose of validating the temperature, ozone, water vapour and methane fields. Data from the Aura microwave limb sounder are also used for validation of the chemical processing in the polar vortex. It is found that the CMAM30 temperature is warmer by up to 5 K in the stratosphere, with a low bias in the mesosphere of ~ 5–15 K. Ozone is reasonable (±15 %), except near the tropopause globally and in the Southern Hemisphere winter polar vortex. Water vapour is consistently low by 10–20 %, with corresponding high methane of 10–20 %, except in the Southern Hemisphere polar vortex. Discrepancies in this region are shown to stem from the treatment of polar stratospheric cloud formation in the model.

As part of European Space Agency's (ESA) climate change initiative, high vertical resolution ozone profiles from three instruments all aboard ESA's Envisat (GOMOS, MIPAS, SCIAMACHY) and ESA's third party missions (OSIRIS, SMR, ACE-FTS) are to be combined in order to create an essential climate variable data record for the last decade. A prerequisite before combining data is the examination of differences and drifts between the data sets. In this paper, we present a detailed analysis of ozone profile differences based on pairwise collocated measurements, including the evolution of the differences with time. Such a diagnosis is helpful to identify strengths and weaknesses of each data set that may vary in time and introduce uncertainties in long-term trend estimates. The analysis reveals that the relative drift between the sensors is not statistically significant for most pairs of instruments. The relative drift values can be used to estimate the added uncertainty in physical trends. The added drift uncertainty is estimated at about 3 % decade−1 (1σ). Larger differences and variability in the differences are found in the lowermost stratosphere (below 20 km) and in the mesosphere.

Trends in the vertical distribution of ozone are reported and compared for a number of new and recently revised data sets. The amount of ozone-depleting compounds in the stratosphere (as measured by equivalent effective stratospheric chlorine – EESC) was maximised in the second half of the 1990s. We examine the periods before and after the peak to see if any change in trend is discernible in the ozone record that might be attributable to a change in the EESC trend, though no attribution is attempted. Prior to 1998, trends in the upper stratosphere (~ 45 km, 4 hPa) are found to be −5 to −10 % per decade at mid-latitudes and closer to −5 % per decade in the tropics. No trends are found in the mid-stratosphere (28 km, 30 hPa). Negative trends are seen in the lower stratosphere at mid-latitudes in both hemispheres and in the deep tropics. However, it is hard to be categorical about the trends in the lower stratosphere for three reasons: (i) there are fewer measurements, (ii) the data quality is poorer, and (iii) the measurements in the 1990s are perturbed by aerosols from the Mt Pinatubo eruption in 1991. These findings are similar to those reported previously even though the measurements for the main satellite and ground-based records have been revised. There is no sign of a continued negative trend in the upper stratosphere since 1998: instead there is a hint of an average positive trend of ~ 2 % per decade in mid-latitudes and ~ 3 % per decade in the tropics. The significance of these upward trends is investigated using different assumptions of the independence of the trend estimates found from different data sets. The averaged upward trends are significant if the trends derived from various data sets are assumed to be independent (as in Pawson et al., 2014) but are generally not significant if the trends are not independent. This occurs because many of the underlying measurement records are used in more than one merged data set. At this point it is not possible to say which assumption is best. Including an estimate of the drift of the overall ozone observing system decreases the significance of the trends. The significance will become clearer as (i) more years are added to the observational record, (ii) further improvements are made to the historic ozone record (e.g. through algorithm development), and (iii) the data merging techniques are refined, particularly through a more rigorous treatment of uncertainties.

In the framework of the SI2N (SPARC (Stratosphere-troposphere Processes And their Role in Climate)/IO3C (International Ozone Commission)/IGACO-O3 (Integrated Global Atmospheric Chemistry Observations – Ozone)/NDACC (Network for the Detection of Atmospheric Composition Change)) initiative, several long-term vertically resolved merged ozone data sets produced from satellite measurements have been analysed and compared. This paper presents an overview of the methods, assumptions, and challenges involved in constructing such merged data sets, as well as the first thorough intercomparison of seven new long-term satellite data sets. The analysis focuses on the representation of the annual cycle, interannual variability, and long-term trends for the period 1984–2011, which is common to all data sets. Overall, the best agreement amongst data sets is seen in the mid-latitude lower and middle stratosphere, with larger differences in the equatorial lower stratosphere and the upper stratosphere globally. In most cases, differences in the choice of underlying instrument records that were merged produced larger differences between data sets than the use of different merging techniques. Long-term ozone trends were calculated for the period 1984–2011 using a piecewise linear regression with a change in trend prescribed at the end of 1997. For the 1984–1997 period, trends tend to be most similar between data sets (with largest negative trends ranging from −4 to −8% decade−1 in the mid-latitude upper stratosphere), in large part due to the fact that most data sets are predominantly (or only) based on the SAGE-II record. Trends in the middle and lower stratosphere are much smaller, and, particularly for the lower stratosphere, large uncertainties remain. For the later period (1998–2011), trends vary to a greater extent, ranging from approximately −1 to +5% decade−1 in the upper stratosphere. Again, middle and lower stratospheric trends are smaller and for most data sets not significantly different from zero. Overall, however, there is a clear shift from mostly negative to mostly positive trends between the two periods over much of the profile.

We present the results of an extensive validation program of the most recent version of ozone vertical profiles retrieved with the IMK/IAA (Institute for Meteorology and Climate Research/Instituto de Astrofísica de Andalucía) MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) research level 2 processor from version 5 spectral level 1 data. The time period covered corresponds to the reduced spectral resolution period of the MIPAS instrument, i.e., January 2005–April 2012. The comparison with satellite instruments includes all post-2005 satellite limb and occultation sensors that have measured the vertical profiles of tropospheric and stratospheric ozone: ACE-FTS, GOMOS, HALOE, HIRDLS, MLS, OSIRIS, POAM, SAGE II, SCIAMACHY, SMILES, and SMR. In addition, balloon-borne MkIV solar occultation measurements and ground-based Umkehr measurements have been included, as well as two nadir sensors: IASI and SBUV. For each reference data set, bias determination and precision assessment are performed. Better agreement with reference instruments than for the previous data version, V5R_O3_220 (Laeng et al., 2014), is found: the known high bias around the ozone vmr (volume mixing ratio) peak is significantly reduced and the vertical resolution at 35 km has been improved. The agreement with limb and solar occultation reference instruments that have a known small bias vs. ozonesondes is within 7% in the lower and middle stratosphere and 5% in the upper troposphere. Around the ozone vmr peak, the agreement with most of the satellite reference instruments is within 5%; this bias is as low as 3% for ACE-FTS, MLS, OSIRIS, POAM and SBUV.

Peak stratospheric chlorofluorocarbon (CFC) and other ozone depleting substance (ODS) concentrations were reached in the mid- to late 1990s. Detection and attribution of the expected recovery of the stratospheric ozone layer in an atmosphere with reduced ODSs as well as efforts to understand the evolution of stratospheric ozone in the presence of increasing greenhouse gases are key current research topics. These require a critical examination of the ozone changes with an accurate knowledge of the spatial (geographical and vertical) and temporal ozone response. For such an examination, it is vital that the quality of the measurements used be as high as possible and measurement uncertainties well quantified. In preparation for the 2014 United Nations Environment Programme (UNEP)/World Meteorological Organization (WMO) Scientific Assessment of Ozone Depletion, the SPARC/IO3C/IGACO-O3/NDACC (SI2N) Initiative was designed to study and document changes in the global ozone profile distribution. This requires assessing long-term ozone profile data sets in regards to measurement stability and uncertainty characteristics. The ultimate goal is to establish suitability for estimating long-term ozone trends to contribute to ozone recovery studies. Some of the data sets have been improved as part of this initiative with updated versions now available. This summary presents an overview of stratospheric ozone profile measurement data sets (ground and satellite based) available for ozone recovery studies. Here we document measurement techniques, spatial and temporal coverage, vertical resolution, native units and measurement uncertainties. In addition, the latest data versions are briefly described (including data version updates as well as detailing multiple retrievals when available for a given satellite instrument). Archive location information for each data set is also given.

Vertical profiles of the rate of linear change (trend) in the altitude range 15–50 km are determined from decadal O3 time series obtained from SCIAMACHY1/ENVISAT2 measurements in limb-viewing geometry. The trends are calculated by using a multivariate linear regression. Seasonal variations, the quasi-biennial oscillation, signatures of the solar cycle and the El Niño–Southern Oscillation are accounted for in the regression. The time range of trend calculation is August 2002–April 2012. A focus for analysis are the zonal bands of 20° N–20° S (tropics), 60–50° N, and 50–60° S (midlatitudes). In the tropics, positive trends of up to 5% per decade between 20 and 30 km and negative trends of up to 10% per decade between 30 and 38 km are identified. Positive O3 trends of around 5% per decade are found in the upper stratosphere in the tropics and at midlatitudes. Comparisons between SCIAMACHY and EOS MLS3 show reasonable agreement both in the tropics and at midlatitudes for most altitudes. In the tropics, measurements from OSIRIS4/Odin and SHADOZ5 are also analysed. These yield rates of linear change of O3 similar to those from SCIAMACHY. However, the trends from SCIAMACHY near 34 km in the tropics are larger than MLS and OSIRIS by a factor of around two. 1 SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY 2 European environmental research satellite 3 Earth Observing System (EOS) Microwave Limb Sounder (MLS) 4 Optical Spectrograph and InfraRed Imager System 5 Southern Hemisphere ADditional OZonesondes

In this paper, we present a HARMonized dataset of OZone profiles (HARMOZ) based on limb and occultation measurements from Envisat (GOMOS, MIPAS and SCIAMACHY), Odin (OSIRIS, SMR) and SCISAT (ACE-FTS) satellite instruments. These measurements provide high-vertical-resolution ozone profiles covering the altitude range from the upper troposphere up to the mesosphere in years 2001–2012. HARMOZ has been created in the framework of the European Space Agency Climate Change Initiative project. The harmonized dataset consists of original retrieved ozone profiles from each instrument, which are screened for invalid data by the instrument teams. While the original ozone profiles are presented in different units and on different vertical grids, the harmonized dataset is given on a common pressure grid in netCDF (network common data form)-4 format. The pressure grid corresponds to vertical sampling of ~ 1 km below 20 km and 2–3 km above 20 km. The vertical range of the ozone profiles is specific for each instrument, thus all information contained in the original data is preserved. Provided altitude and temperature profiles allow the representation of ozone profiles in number density or mixing ratio on a pressure or altitude vertical grid. Geolocation, uncertainty estimates and vertical resolution are provided for each profile. For each instrument, optional parameters, which are related to the data quality, are also included. For convenience of users, tables of biases between each pair of instruments for each month, as well as bias uncertainties, are provided. These tables characterize the data consistency and can be used in various bias and drift analyses, which are needed, for instance, for combining several datasets to obtain a long-term climate dataset. This user-friendly dataset can be interesting and useful for various analyses and applications, such as data merging, data validation, assimilation and scientific research. The dataset is available at http://www.esa-ozone-cci.org/?q=node/161 or at doi:10.5270/esa-ozone_cci-limb_occultation_profiles-2001_2012-v_1-201308.

We observed ozone (O3) in the vertical region between 250 and 0.0005 hPa (~ 12–96 km) using the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) on the Japanese Experiment Module (JEM) of the International Space Station (ISS) between 12 October 2009 and 21 April 2010. The new 4 K superconducting heterodyne receiver technology of SMILES allowed us to obtain a one order of magnitude better signal-to-noise ratio for the O3 line observation compared to past spaceborne microwave instruments. The non-sun-synchronous orbit of the ISS allowed us to observe O3 at various local times. We assessed the quality of the vertical profiles of O3 in the 100–0.001 hPa (~ 16–90 km) region for the SMILES NICT Level 2 product version 2.1.5. The evaluation is based on four components: error analysis; internal comparisons of observations targeting three different instrumental setups for the same O3 625.371 GHz transition; internal comparisons of two different retrieval algorithms; and external comparisons for various local times with ozonesonde, satellite and balloon observations (ENVISAT/MIPAS, SCISAT/ACE-FTS, Odin/OSIRIS, Odin/SMR, Aura/MLS, TELIS). SMILES O3 data have an estimated absolute accuracy of better than 0.3 ppmv (3%) with a vertical resolution of 3–4 km over the 60 to 8 hPa range. The random error for a single measurement is better than the estimated systematic error, being less than 1, 2, and 7%, in the 40–1, 80–0.1, and 100–0.004 hPa pressure regions, respectively. SMILES O3 abundance was 10–20% lower than all other satellite measurements at 8–0.1 hPa due to an error arising from uncertainties of the tangent point information and the gain calibration for the intensity of the spectrum. SMILES O3 from observation frequency Band-B had better accuracy than that from Band-A. A two month period is required to accumulate measurements covering 24 h in local time of O3 profile. However such a dataset can also contain variation due to dynamical, seasonal, and latitudinal effects.

In spring 2011, the Arctic polar vortex was stronger than in any other year on record. As the polar vortex started to break up in April, ozone and NO2 columns were measured with UV-visible spectrometers above the Polar Environment Atmospheric Research Laboratory (PEARL) in Eureka, Canada (80.05° N, 86.42° W) using the differential optical absorption spectroscopy (DOAS) technique. These ground-based column measurements were complemented by Ozone Monitoring Instrument (OMI) and Optical Spectrograph and Infra-Red Imager System (OSIRIS) satellite measurements, Global Modeling Initiative (GMI) simulations, and meteorological quantities. On 8 April 2011, NO2 columns above PEARL from the DOAS, OMI, and GMI datasets were approximately twice as large as in previous years. On this day, temperatures and ozone volume mixing ratios above Eureka were high, suggesting enhanced chemical production of NO2 from NO. Additionally, GMI NOx (NO + NO2) and N2O fields suggest that downward transport along the vortex edge and horizontal transport from lower latitudes also contributed to the enhanced NO2. The anticyclone that transported lower-latitude NOx above PEARL became frozen-in and persisted in dynamical and GMI N2O fields until the end of the measurement period on 31 May 2011. Ozone isolated within this frozen-in anticyclone (FrIAC) in the middle stratosphere was lost due to reactions with the enhanced NOx. Below the FrIAC (from the tropopause to 700 K), NOx driven ozone loss above Eureka was larger than in previous years, according to GMI monthly average ozone loss rates. Using the passive tracer technique, with passive ozone profiles from the Lagrangian Chemistry and Transport Model, ATLAS, ozone losses since 1 December 2010 were calculated at 600 K. In the air mass that was above Eureka on 20 May 2011, ozone losses reached 4.2 parts per million by volume (ppmv) (58%) and 4.4 ppmv (61%), when calculated using GMI and OSIRIS ozone profiles, respectively. This gas-phase ozone loss led to a more rapid decrease in ozone column amounts above Eureka in April/May 2011 compared with previous years. Ground-based, OMI, and GMI ozone total columns all decreased by more than 100 DU from 15 April to 20 May. Two lows in the ozone columns were also investigated and were attributed to a vortex remnant passing above Eureka at ~500 K on 12/13 May and an ozone mini-hole on 22/23 May.

The Optical Spectrograph and Infra-Red Imager System (OSIRIS) and the Atmospheric Chemistry Experiment (ACE) have been taking measurements from space since 2001 and 2003, respectively. This paper presents intercomparisons between ozone and NO2 measured by the ACE and OSIRIS satellite instruments and by ground-based instruments at the Polar Environment Atmospheric Research Laboratory (PEARL), which is located at Eureka, Canada (80° N, 86° W) and is operated by the Canadian Network for the Detection of Atmospheric Change (CANDAC). The ground-based instruments included in this study are four zenith-sky differential optical absorption spectroscopy (DOAS) instruments, one Bruker Fourier transform infrared spectrometer (FTIR) and four Brewer spectrophotometers. Ozone total columns measured by the DOAS instruments were retrieved using new Network for the Detection of Atmospheric Composition Change (NDACC) guidelines and agree to within 3.2%. The DOAS ozone columns agree with the Brewer spectrophotometers with mean relative differences that are smaller than 1.5%. This suggests that for these instruments the new NDACC data guidelines were successful in producing a homogenous and accurate ozone dataset at 80° N. Satellite 14–52 km ozone and 17–40 km NO2 partial columns within 500 km of PEARL were calculated for ACE-FTS Version 2.2 (v2.2) plus updates, ACE-FTS v3.0, ACE-MAESTRO (Measurements of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation) v1.2 and OSIRIS SaskMART v5.0x ozone and Optimal Estimation v3.0 NO2 data products. The new ACE-FTS v3.0 and the validated ACE-FTS v2.2 partial columns are nearly identical, with mean relative differences of 0.0 ± 0.2% and −0.2 ± 0.1% for v2.2 minus v3.0 ozone and NO2, respectively. Ozone columns were constructed from 14–52 km satellite and 0–14 km ozonesonde partial columns and compared with the ground-based total column measurements. The satellite-plus-sonde measurements agree with the ground-based ozone total columns with mean relative differences of 0.1–7.3%. For NO2, partial columns from 17 km upward were scaled to noon using a photochemical model. Mean relative differences between OSIRIS, ACE-FTS and ground-based NO2 measurements do not exceed 20%. ACE-MAESTRO measures more NO2 than the other instruments, with mean relative differences of 25–52%. Seasonal variation in the differences between NO2 partial columns is observed, suggesting that there are systematic errors in the measurements and/or the photochemical model corrections. For ozone spring-time measurements, additional coincidence criteria based on stratospheric temperature and the location of the polar vortex were found to improve agreement between some of the instruments. For ACE-FTS v2.2 minus Bruker FTIR, the 2007–2009 spring-time mean relative difference improved from −5.0 ± 0.4% to −3.1 ± 0.8% with the dynamical selection criteria. This was the largest improvement, likely because both instruments measure direct sunlight and therefore have well-characterized lines-of-sight compared with scattered sunlight measurements. For NO2, the addition of a ±1° latitude coincidence criterion improved spring-time intercomparison results, likely due to the sharp latitudinal gradient of NO2 during polar sunrise. The differences between satellite and ground-based measurements do not show any obvious trends over the missions, indicating that both the ACE and OSIRIS instruments continue to perform well.

The long term evolution of stratospheric ozone and water vapour has been investigated by extending satellite time series to April 2008. For ozone, we examine monthly average ozone values from various satellite data sets for nine latitude and altitude bins covering 60° S to 60° N and 20–45 km and covering the time period of 1979–2008. Data are from the Stratospheric Aerosol and Gas Experiment (SAGE I+II), the HALogen Occultation Experiment (HALOE), the Solar BackscatterUltraViolet-2 (SBUV/2) instrument, the Sub-Millimetre Radiometer (SMR), the Optical Spectrograph InfraRed Imager System (OSIRIS), and the SCanning Imaging Absorption spectroMeter for Atmospheric CHartograpY (SCIAMACHY). Monthly ozone anomalies are calculated by utilising a linear regression model, which also models the solar, quasi-biennial oscillation (QBO), and seasonal cycle contributions. Individual instrument ozone anomalies are combined producing an all instrument average. Assuming a turning point of 1997 and that the all instrument average is represented by good instrumental long term stability, the largest statistically significant ozone declines (at two sigma) from 1979–1997 are seen at the mid-latitudes between 35 and 45 km, namely −7.2%±0.9%/decade in the Northern Hemisphere and −7.1%±0.9%/in the Southern Hemisphere. Furthermore, for the period 1997 to 2008 we find that the same locations show the largest ozone recovery (+1.4% and +0.8%/decade respectively) compared to other global regions, although the estimated trend model errors indicate that the trend estimates are not significantly different from a zero trend at the 2 sigma level. An all instrument average is also constructed from water vapour anomalies during 1991–2008, using the SAGE II, HALOE, SMR, and the Microwave Limb Sounder (Aura/MLS) measurements. We report that the decrease in water vapour values after 2001 slows down around 2004–2005 in the lower tropical stratosphere (20–25 km) and has even shown signs of increasing until present. We show that a similar correlation is also seen with the temperature measured at 100 hPa during this same period.

The Canadian ACE (Atmospheric Chemistry Experiment) mission is dedicated to the retrieval of a large number of atmospheric trace gas species using the solar occultation technique in the infrared and UV/visible spectral domain. However, two additional solar disk imagers (at 525 nm and 1020 nm) were added for a number of reasons, including the retrieval of aerosol and cloud products. In this paper, we present first comparison results for these imager aerosol/cloud optical extinction coefficient profiles, with the ones derived from measurements performed by 3 solar occultation instruments (SAGE II, SAGE III, POAM III), one stellar occultation instrument (GOMOS) and one limb sounder (OSIRIS). The results indicate that the ACE imager profiles are of good quality in the upper troposphere/lower stratosphere, although the aerosol extinction for the visible channel at 525 nm contains a significant negative bias at higher altitudes, while the relative differences indicate that ACE profiles are almost always too high at 1020 nm. Both problems are probably related to ACE imager instrumental issues.

On 6 December 2002, during winter darkness, an extraordinary event occurred in the sky, as viewed from Longyearbyen (78° N, 15° E), Svalbard, Norway. At 07:30 UT the southeast sky was surprisingly lit up in a deep red colour. The light increased in intensity and spread out across the sky, and at 10:00 UT the illumination was observed to reach the zenith. The event died out at about 12:30 UT. Spectral measurements from the Auroral Station in Adventdalen confirm that the light was scattered sunlight. Even though the Sun was between 11.8 and 14.6deg below the horizon during the event, the measured intensities of scattered light on the southern horizon from the scanning photometers coincided with the rise and setting of the Sun. Calculations of actual heights, including refraction and atmospheric screening, indicate that the event most likely was scattered solar light from a target below the horizon. This is also confirmed by the OSIRIS instrument on board the Odin satellite. The deduced height profile indicates that the scattering target is located 18–23km up in the stratosphere at a latitude close to 73–75° N, southeast of Longyearbyen. The temperatures in this region were found to be low enough for Polar Stratospheric Clouds (PSC) to be formed. The target was also identified as PSC by the LIDAR systems at the Koldewey Station in Ny-Ålesund (79° N, 12° E). The event was most likely caused by solar illuminated type II Polar Stratospheric Clouds that scattered light towards Svalbard. Two types of scenarios are presented to explain how light is scattered. Keywords. Atmospheric composition and structure (Transmissions and scattering of radiation; Middle atmospherecomposition and chemistry; Instruments and techniques) – History of geophysics (Atmospheric Sciences; The red-sky phenomena)