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Abstract Two-dimensional (2D) van der Waals (vdW) magnets have sparked widespread attention due to their potential in spintronic applications as well as in fundamental physics. Ferromagnetic vdW compound Fe3GeTe2 (FGT) and its Ga variants have garnered significant interest due to their itinerant magnetism, correlated states, and high magnetic transition temperature. Experimental studies have demonstrated the tunability of FGT’s Curie temperature, T C , through adjustments in quintuple layer numbers (QL) and carrier concentrations, n. However, the underlying mechanism remains elusive. In this study, we employ molecular beam epitaxy (MBE) to synthesize 2D FGT films down to 1 QL with precise layer control, facilitating an exploration of the band structure and the evolution of itinerant carrier density. Angle-resolved photoemission spectroscopy (ARPES) reveals significant band structure changes at the ultra-thin limit, while first-principles calculations elucidate the band evolution from 1 QL to bulk, largely governed by interlayer coupling. Additionally, we find that n is intrinsically linked to the number of QL and temperature, with a critical value triggering the magnetic phase transition. Our findings underscore the pivotal role of band structure and itinerant electrons in governing magnetic phase transitions in such 2D vdW magnetic materials.

Understanding optical and radiative properties of aerosols and clouds is critical to reducing uncertainties in climate models. For over 10 years, the Observatory of Atmospheric Physics in Reunion (OPAR; 21.079° S, 55.383° E) has been operating three active lidar instruments, named lidar 1200 (Li1200), stratospheric ozone lidar (LiO3S), and tropospheric ozone lidar (LiO3T), providing time series of vertical profiles from 3 to 45 km of the aerosol extinction and backscatter coefficients at 355 and 532 nm as well as the linear depolarization ratio at 532 nm. This work provides a full technical description of the three systems, the details about the methods chosen for the signal preprocessing and processing, and an uncertainty analysis. About 1737 nighttime averaged profiles were manually screened to provide cloud-free and artifact-free profiles. Data processing consisted of Klett inversion to retrieve aerosol optical products from preprocessed files. The measurement frequency was lower during the wet season and the holiday periods. There is a good correlation between the Li1200 and LiO3S instruments in terms of stratospheric aerosol optical depth (AOD) at 355 nm (0.001–0.107; R=0.92±0.01) and with LiO3T in terms of Ångström exponent 355/532 (0.079–1.288; R=0.90±0.13). The lowest values of the averaged uncertainty in the aerosol backscatter coefficient for the three time series are 64.4 ± 31.6 % for LiO3S, 50.3 ± 29.0 % for Li1200, and 69.1 ± 42.7 % for LiO3T. These relative uncertainties are high for the three instruments because of the very low values of extinction and backscatter coefficients for background aerosols above Maïdo observatory. Uncertainty increases due to the signal-to-noise ratio (SNR) decrease above 25 km for LIO3S and Li1200 and above 20 km for LiO3T. The lidar ratio (LR) is responsible for an uncertainty increase below 18 km (10 km) for LiO3S and Li1200 (LiO3T). LiO3S is the most stable instrument at 355 nm due to fewer technical modifications and fewer misalignments. Li1200 is a valuable addition meant to fill in the gaps in the LiO3S time series at 355 nm or for specific case studies about the middle and low troposphere. Data described in this work are available at https://doi.org/10.26171/rwcm-q370 (Gantois et al., 2024).

The Sentinel-5 Precursor (S5P) satellite operated by the European Space Agency has carried the TROPOspheric Monitoring Instrument (TROPOMI) on a Sun-synchronous low-Earth orbit since 13 October 2017. The S5P mission has acquired more than 5 years of TROPOMI nadir ozone profile data retrieved from the level 0 to 1B processor version 2.0 and the level 1B to 2 optimal-estimation-based processor version 2.4.0. The latter is described in detail in this work, followed by the geophysical validation of the resulting ozone profiles for the period May 2018 to April 2023. Comparison of TROPOMI ozone profile data to co-located ozonesonde and lidar measurements used as references concludes to a median agreement better than 5 % to 10 % in the troposphere. The bias goes up to −15 % in the upper stratosphere (35–45 km) where it can exhibit vertical oscillations. The comparisons show a dispersion of about 30 % in the troposphere and 10 % to 20 % in the upper troposphere to lower stratosphere and in the middle stratosphere, which is close to mission requirements. Chi-square tests of the observed differences confirm on average the validity of the ex ante (prognostic) satellite and ground-based data uncertainty estimates in the middle stratosphere above about 20 km. Around the tropopause and below, the mean chi-square value increases up to about four, meaning that the ex ante TROPOMI uncertainty is underestimated. The information content of the ozone profile retrieval is characterised by about five to six vertical subcolumns of independent information and a vertical sensitivity (i.e. the fraction of the information that originates from the measurement) nearly equal to unity at altitudes from about 20 to 50 km, decreasing rapidly at altitudes above and below. The barycentre of the retrieved information is usually close to the nominal retrieval altitude in the 20–50 km altitude range, with positive and negative offsets of up to 10 km below and above this range, respectively. The effective vertical resolution of the profile retrieval usually ranges within 10–15 km, with a minimum close to 7 km in the middle stratosphere. Increased sensitivities and higher effective vertical resolutions are observed at higher solar zenith angles (above about 60°), as can be expected, and correlate with higher retrieved ozone concentrations. The vertical sensitivity of the TROPOMI tropospheric ozone retrieval is found to depend on the solar zenith angle, which translates into a seasonal and meridian dependence of the bias with respect to reference measurements. A similar although smaller effect can be seen for the viewing zenith angle. Additionally, the bias is negatively correlated with the surface albedo for the lowest three ozone subcolumns (0–18 km), despite the albedo's apparently slightly positive correlation with the retrieval degrees of freedom in the signal. For the 5 years of TROPOMI ozone profile data that are available now, an overall positive drift is detected for the same three subcolumns, while a negative drift is observed above (24–32 km), resulting in a negligible vertically integrated drift.

Stratospheric ozone is an important constituent of the atmosphere. Significant changes in its concentrations have great consequences for the environment in general and for ecosystems in particular. Here, we analyse ground-based, ozonesonde and satellite ozone measurements to examine the ozone depletion and the spatiotemporal trends in ozone in the tropics during the past 5 decades (1980–2020). The amount of column ozone in the tropics is relatively small (250–270 DU) compared to high and mid-latitudes (Northern Hemisphere (NH) 275–425 DU; Southern Hemisphere (SH) 275–350 DU). In addition, the tropical total ozone trend is very small (±0–0.2 DU yr−1), as estimated for the period 1998–2022. No observational evidence is found regarding the indications or signatures of severe stratospheric ozone depletion in the tropics in contrast to a recent claim. Finally, current understanding and observational evidence do not provide any support for the possibility of an ozone hole occurring outside Antarctica today with respect to the present-day stratospheric halogen levels.

Ozone depletion over the polar regions is monitored each year by satellite- and ground-based instruments. In this study, the vortex-averaged ozone loss over the last 3 decades is evaluated for both polar regions using the passive ozone tracer of the chemical transport model TOMCAT/SLIMCAT and total ozone observations from Système d'Analyse par Observation Zénithale (SAOZ) ground-based instruments and Multi-Sensor Reanalysis (MSR2). The passive-tracer method allows us to determine the evolution of the daily rate of column ozone destruction and the magnitude of the cumulative column loss at the end of the winter. Three metrics are used in trend analyses that aim to assess the ozone recovery rate over both polar regions: (1) the maximum ozone loss at the end of the winter, (2) the onset day of ozone loss at a specific threshold, and (3) the ozone loss residuals computed from the differences between annual ozone loss and ozone loss values regressed with respect to sunlit volume of polar stratospheric clouds (VPSCs). This latter metric is based on linear and parabolic regressions for ozone loss in the Northern Hemisphere and Southern Hemisphere, respectively. In the Antarctic, metrics 1 and 3 yield trends of −2.3 % and −2.2 % per decade for the 2000–2021 period, significant at 1 and 2 standard deviations (σ), respectively. For metric 2, various thresholds were considered at the total ozone loss values of 20 %, 25 %, 30 %, 35 %, and 40 %, all of them showing a time delay as a function of year in terms of when the threshold is reached. The trends are significant at the 2σ level and vary from 3.5 to 4.2 d per decade between the various thresholds. In the Arctic, metric 1 exhibits large interannual variability, and no significant trend is detected; this result is highly influenced by the record ozone losses in 2011 and 2020. Metric 2 is not applied in the Northern Hemisphere due to the difficulty in finding a threshold value in enough of the winters. Metric 3 provides a negative trend in Arctic ozone loss residuals with respect to the sunlit VPSC fit of −2.00 ± 0.97 (1σ) % per decade, with limited significance at the 2σ level. With such a metric, a potential quantitative detection of ozone recovery in the Arctic springtime lower stratosphere can be made.

Nabro volcano (13.37°N, 41.70°E) in Eritrea erupted on 13 June 2011 generating a layer of sulfate aerosols that persisted in the stratosphere for months. For the first time we report on ground-based lidar observations of the same event from every continent in the Northern Hemisphere, taking advantage of the synergy between global lidar networks such as EARLINET, MPLNET and NDACC with independent lidar groups and satellite CALIPSO to track the evolution of the stratospheric aerosol layer in various parts of the globe. The globally averaged aerosol optical depth (AOD) due to the stratospheric volcanic aerosol layers was of the order of 0.018 ± 0.009 at 532 nm, ranging from 0.003 to 0.04. Compared to the total column AOD from the available collocated AERONET stations, the stratospheric contribution varied from 2% to 23% at 532 nm.

This study presents an updated evaluation of stratospheric ozone profile trends in the 60∘ S–60∘ N latitude range over the 2000–2020 period using an updated version of the Long-term Ozone Trends and Uncertainties in the Stratosphere (LOTUS) regression model that was used to evaluate such trends up to 2016 for the last WMO Ozone Assessment (2018). In addition to the derivation of detailed trends as a function of latitude and vertical coordinates, the regressions are performed with the datasets averaged over broad latitude bands, i.e. 60–35∘ S, 20∘ S–20∘ N and 35–60∘ N. The same methodology as in the last assessment is applied to combine trends in these broad latitude bands in order to compare the results with the previous studies. Longitudinally resolved merged satellite records are also considered in order to provide a better comparison with trends retrieved from ground-based records, e.g. lidar, ozonesondes, Umkehr, microwave and Fourier transform infrared (FTIR) spectrometers at selected stations where long-term time series are available. The study includes a comparison with trends derived from the REF-C2 simulations of the Chemistry Climate Model Initiative (CCMI-1). This work confirms past results showing an ozone increase in the upper stratosphere, which is now significant in the three broad latitude bands. The increase is largest in the Northern and Southern Hemisphere midlatitudes, with ∼2.2 ± 0.7 % per decade at ∼2.1 hPa and ∼2.1 ± 0.6 % per decade at ∼3.2 hPa respectively compared to ∼1.6 ± 0.6 % per decade at ∼2.6 hPa in the tropics. New trend signals have emerged from the records, such as a significant decrease in ozone in the tropics around 35 hPa and a non-significant increase in ozone in the southern midlatitudes at about 20 hPa. Non-significant negative ozone trends are derived in the lowermost stratosphere, with the most pronounced trends in the tropics. While a very good agreement is obtained between trends from merged satellite records and the CCMI-1 REF-C2 simulation in the upper stratosphere, observed negative trends in the lower stratosphere are not reproduced by models at southern and, in particular, at northern midlatitudes, where models report an ozone increase. However, the lower-stratospheric trend uncertainties are quite large, for both measured and modelled trends. Finally, 2000–2020 stratospheric ozone trends derived from the ground-based and longitudinally resolved satellite records are in reasonable agreement over the European Alpine and tropical regions, while at the Lauder station in the Southern Hemisphere midlatitudes they show some differences.

The Observatoire de Haute Provence (OHP) weekly electrochemical concentration cell (ECC) ozonesonde data have been homogenized for the period 1991–2021 according to the recommendations of the Ozonesonde Data Quality Assessment (O3S-DQA) panel. The assessment of the ECC homogenization benefit has been carried out using comparisons with other ozone-measuring ground-based instruments at the same station (lidar, surface measurements) and with colocated satellite observations of the O3 vertical profile by Microwave Limb Sounder (MLS). The major differences between uncorrected and homogenized ECC data are related to a change of ozonesonde type in 1997, removal of the pressure dependency of the ECC background current and correction of internal pump temperature. The original 3–4 ppbv positive bias between ECC and lidar in the troposphere is corrected with the homogenization. The ECC 30-year trends of the seasonally adjusted ozone concentrations are also significantly improved in both the troposphere and the stratosphere after the ECC homogenization, as shown by the ECC/lidar or ECC/surface ozone trend comparisons. A −0.19 % yr−1 negative trend of the normalization factor (NT) calculated using independent measurements of the total ozone column (TOC) at OHP disappears after homogenization of the ECC data. There is, however, a remaining −3.7 % negative bias in the TOC which is likely related to an underestimate of the ECC concentrations in the stratosphere above 50 hPa. Differences between TOC measured by homogenized ECC and satellite observations show a smaller bias of −1 %. Comparisons between homogenized ECC and OHP stratospheric lidar and MLS observations below 26 km are slightly negative (−2 %) or positive (+2 %), respectively. The comparisons with both lidar and satellite observations suggest that homogenization increases the negative bias of the ECC to values lower than −6 % above 28 km. The reason for this bias is still unclear, but a possible explanation might be related to freezing or evaporation of the sonde solution in the stratosphere.

The intensity and position of the Southern Hemisphere stratospheric polar vortex edge is evaluated as a function of equivalent latitude over the period 1979–2020 on three isentropic levels (475, 550, and 675 K) from ECMWF ERA-Interim reanalysis. The study also includes an analysis of the onset and breakup dates of the polar vortex, which are determined from wind thresholds (e.g., 15.2, 20, and 25 m s−1) along the vortex edge. The vortex edge is stronger in late winter, during September–October–November, with the period of strongest intensity occurring later at the lowermost level. During the same period, we observe a lower variability of the edge position. A long-term increase in the vortex edge intensity and break-up date is observed during 1979–1999, linked to the increase in the ozone hole. A long-term decrease in the vortex onset date related to the 25 m s−1 wind threshold is also observed at 475 K during this period. The solar cycle and to a lower extent the quasi-biennial oscillation (QBO) and El Niño–Southern Oscillation (ENSO) modulate the interannual evolution of the strength of the vortex edge and the vortex breakup dates. A stronger vortex edge and longer vortex duration are observed in solar minimum (minSC) years, with the QBO and ENSO further modulating the solar cycle influence, especially at 475 and 550 K: during west QBO (wQBO) phases, the difference between vortex edge intensity for minSC and maxSC years is smaller than during east QBO (eQBO) phases. The polar vortex edge is stronger and lasts longer for maxSC/wQBO years than for maxSC/eQBO years. ENSO has a weaker impact but the vortex edge is somewhat stronger during cold ENSO phases for both minSC and maxSC years.

The long-term record of Umkehr measurements from four NOAA Dobson spectrophotometers was reprocessed after updates to the instrument calibration procedures. In addition, a new data quality-control tool was developed for the Dobson automation software (WinDobson). This paper presents a comparison of Dobson Umkehr ozone profiles from NOAA ozone network stations – Boulder, the Haute-Provence Observatory (OHP), the Mauna Loa Observatory (MLO), Lauder – against several satellite records, including Aura Microwave Limb Sounder (MLS; ver. 4.2), and combined solar backscatter ultraviolet (SBUV) and Ozone Mapping and Profiler Suite (OMPS) records (NASA aggregated and NOAA cohesive datasets). A subset of satellite data is selected to match Dobson Umkehr observations at each station spatially (distance less than 200 km) and temporally (within 24 h). Umkehr Averaging kernels (AKs) are applied to vertically smooth all overpass satellite profiles prior to comparisons. The station Umkehr record consists of several instrumental records, which have different optical characterizations, and thus instrument-specific stray light contributes to the data processing errors and creates step changes in the record. This work evaluates the overall quality of Umkehr long-term measurements at NOAA ground-based stations and assesses the impact of the instrumental changes on the stability of the Umkehr ozone profile record. This paper describes a method designed to correct biases and discontinuities in the retrieved Umkehr profile that originate from the Dobson calibration process, repair, or optical realignment of the instrument. The Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA-2) Global Modeling Initiative (M2GMI) and NASA Global Modeling Initiative chemistry transport model (GMI CTM) ozone profile model output matched to station location and date of observation is used to evaluate instrumental step changes in the Umkehr record. Homogenization of the Umkehr record and discussion of the apparent stray light error in retrieved ozone profiles are the focus of this paper. Homogenization of ground-based records is of great importance for studies of long-term ozone trends and climate change.

The evolution of NO2, considered as a proxy for air pollution, was analyzed to evaluate the impact of the first lockdown (17 March–10 May 2020) over the Île-de-France region (Paris and surroundings). Tropospheric NO2 columns measured by two UV-Visible Système d'Analyse par Observation Zénithale (SAOZ) spectrometers were analyzed to compare the evolution of NO2 between urban and suburban sites during the lockdown. The urban site is the observation platform QualAir (48∘50′ N / 2∘21′ E) at the Sorbonne University Pierre and Marie Curie Campus in the center of Paris. The suburban site is located at Guyancourt (48∘46′N / 2∘03′E), Versailles Saint-Quentin-en-Yvelines University, 24 km southwest of Paris. Tropospheric NO2 columns above Paris and Guyancourt have shown similar values during the whole lockdown period from March to May 2020. A decade of data sets were filtered to consider air masses at both sites with similar meteorological conditions. The median NO2 columns and the surface measurements of Airparif (Air Quality Observatory in Île de France) during the lockdown period in 2020 were compared to the extrapolated values estimated from a linear trend analysis for the 2011–2019 period at each station. Negative NO2 trends of −1.5 Pmolec. cm−2 yr−1 (∼ −6.3 % yr−1) are observed from the columns, and trends of −2.2 µg m−3 yr−1 (∼ −3.6 % yr−1) are observed from the surface concentration. The negative anomaly in tropospheric columns in 2020 attributed to the lockdown (and related emission reductions) was found to be 56 % at Paris and 46 % at Guyancourt, respectively. A similar anomaly was found in the data of surface concentrations, amounting to 53 % and 28 % at the urban and suburban sites, accordingly.

A two-part intercomparison campaign was conducted at Observatoire de Haute-Provence (OHP) for the validation of lidar ozone and temperature profiles using the mobile NASA Stratospheric Ozone Lidar (NASA STROZ), satellite overpasses from the Microwave Limb Sounder (MLS), the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER), meteorological radiosondes launched from Nîmes, and locally launched ozonesondes. All the data were submitted and compared “blind”, before the group could see results from the other instruments. There was good agreement between all ozone measurements between 20 and 40 km, with differences of generally less than 5 % throughout this region. Below 20 km, SABER and MLS measured significantly more ozone than the lidars or ozonesondes. Temperatures for all lidars were in good agreement between 30 and 60 km, with differences on the order of ±1 to 3 K. Below 30 km, the OHP lidar operating at 532 nm has a significant cool bias due to contamination by aerosols. Systematic, altitude-varying bias up to ±5 K compared to the lidars was found for MLS at many altitudes. SABER temperature profiles are generally closer to the lidar profiles, with up 3 K negative bias near 50 km. Total uncertainty estimates for ozone and temperature appear to be realistic for nearly all systems. However, it does seem that the very low estimated uncertainties of lidars between 30 and 50 km, between 0.1 and 1 K, are not achieved during Lidar Validation Network for the Detection of Atmospheric Composition Change (NDACC) Experiment (LAVANDE). These estimates might have to be increased to 1 to 2 K.

Aerosol backscatter coefficients were calculated using multiwavelength aerosol extinction products from the SAGE II and III/ISS instruments (SAGE: Stratospheric Aerosol and Gas Experiment). The conversion methodology is presented, followed by an evaluation of the conversion algorithm's robustness. The SAGE-based backscatter products were compared to backscatter coefficients derived from ground-based lidar at three sites (Table Mountain Facility, Mauna Loa, and Observatoire de Haute-Provence). Further, the SAGE-derived lidar ratios were compared to values from previous balloon and theoretical studies. This evaluation includes the major eruption of Mt. Pinatubo in 1991, followed by the atmospherically quiescent period beginning in the late 1990s. Recommendations are made regarding the use of this method for evaluation of aerosol extinction profiles collected using the occultation method.

A direct-detection Rayleigh–Mie Doppler lidar for measuring horizontal wind speed in the middle atmosphere (10 to 50 km altitude) has been deployed at Observatoire de Haute-Provence (OHP) in southern France starting from 1993. After a recent upgrade, the instrument gained the capacity of wind profiling between 5 and 75 km altitude with vertical resolution up to 115 m and temporal resolution up to 5 min. The lidar comprises a monomode Nd:Yag laser emitting at 532 nm, three telescope assemblies and a double-edge Fabry–Pérot interferometer for detection of the Doppler shift in the backscattered light. In this article, we describe the instrument design, recap retrieval methodology and provide an updated error estimate for horizontal wind. The evaluation of the wind lidar performance is done using a series of 12 time-coordinated radiosoundings conducted at OHP. A point-by-point intercomparison shows a remarkably small average bias of 0.1 m s−1 between the lidar and the radiosonde wind profiles with a standard deviation of 2.3 m s−1. We report examples of a weekly and an hourly observation series, reflecting various dynamical events in the middle atmosphere, such as a sudden stratospheric warming event in January 2019 and an occurrence of a stationary gravity wave, generated by the flow over the Alps. A qualitative comparison between the wind profiles from the lidar and the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecast System is also discussed. Finally, we present an example of early validation of the European Space Agency (ESA) Aeolus space-borne wind lidar using its ground-based predecessor.

We have derived values of the ultraviolet index (UVI) at solar noon using the Tropospheric Ultraviolet Model (TUV) driven by ozone, temperature and aerosol fields from climate simulations of the first phase of the Chemistry-Climate Model Initiative (CCMI-1). Since clouds remain one of the largest uncertainties in climate projections, we simulated only the clear-sky UVI. We compared the modelled UVI climatologies against present-day climatological values of UVI derived from both satellite data (the OMI-Aura OMUVBd product) and ground-based measurements (from the NDACC network). Depending on the region, relative differences between the UVI obtained from CCMI/TUV calculations and the ground-based measurements ranged between −5.9 % and 10.6 %. We then calculated the UVI evolution throughout the 21st century for the four Representative Concentration Pathways (RCPs 2.6, 4.5, 6.0 and 8.5). Compared to 1960s values, we found an average increase in the UVI in 2100 (of 2 %–4 %) in the tropical belt (30∘ N–30∘ S). For the mid-latitudes, we observed a 1.8 % to 3.4 % increase in the Southern Hemisphere for RCPs 2.6, 4.5 and 6.0 and found a 2.3 % decrease in RCP 8.5. Higher increases in UVI are projected in the Northern Hemisphere except for RCP 8.5. At high latitudes, ozone recovery is well identified and induces a complete return of mean UVI levels to 1960 values for RCP 8.5 in the Southern Hemisphere. In the Northern Hemisphere, UVI levels in 2100 are higher by 0.5 % to 5.5 % for RCPs 2.6, 4.5 and 6.0 and they are lower by 7.9 % for RCP 8.5. We analysed the impacts of greenhouse gases (GHGs) and ozone-depleting substances (ODSs) on UVI from 1960 by comparing CCMI sensitivity simulations (1960–2100) with fixed GHGs or ODSs at their respective 1960 levels. As expected with ODS fixed at their 1960 levels, there is no large decrease in ozone levels and consequently no sudden increase in UVI levels. With fixed GHG, we observed a delayed return of ozone to 1960 values, with a corresponding pattern of change observed on UVI, and looking at the UVI difference between 2090s values and 1960s values, we found an 8 % increase in the tropical belt during the summer of each hemisphere. Finally we show that, while in the Southern Hemisphere the UVI is mainly driven by total ozone column, in the Northern Hemisphere both total ozone column and aerosol optical depth drive UVI levels, with aerosol optical depth having twice as much influence on the UVI as total ozone column does.

Subpolar regions in the Southern Hemisphere are influenced by the Antarctic polar vortex during austral spring, which induces high and short-term ozone variability at different altitudes, mainly into the stratosphere. This variation may affect considerably the total ozone column changing the harmful UV radiation that reaches the surface. With the aim of studying ozone with a high time resolution at different altitudes in subpolar regions, a millimetre-wave radiometer (MWR) was installed at the Observatorio Atmosférico de la Patagonia Austral (OAPA), Río Gallegos, Argentina (51.6∘ S, 69.3∘ W), in 2011. This instrument provides ozone profiles with a time resolution of ∼1 h, which enables studies of short-term ozone mixing ratio variability from 25 to ∼70 km in altitude. This work presents the MWR ozone observations between October 2014 and 2015, focusing on an atypical event of the polar vortex and Antarctic ozone hole influence over Río Gallegos detected from the MWR measurements at 27 and 37 km during November of 2014. During the event, the MWR observations at both altitudes show a decrease in ozone followed by a local peak of ozone amount of the order of hours. This local recovery is observed thanks to the high time resolution of the MWR mentioned. The advected potential vorticity (APV) calculated from the MIMOSA high-resolution advection model (Modélisation Isentrope du transport Méso-échelle de l'Ozone Stratosphérique par Advection) was also analysed at two isentropic levels (levels of constant potential temperature) of 675 and 950 K (∼27 and ∼37 km of altitude, respectively) to understand and explain the dynamics at both altitudes and correlate the ozone rapid recovery with the passage of a tongue with low PV values over Río Gallegos. In addition, the MWR dataset was compared for the first time with measurements obtained from the Microwave Limb Sounder (MLS) at individual altitude levels (27, 37 and 65 km) and with the differential absorption lidar (DIAL) installed in the OAPA to analyse the correspondence between the MWR and independent instruments. The MWR–MLS comparison presents a reasonable correlation with mean bias errors of +5 %, −11 % and −7 % at 27, 37 and 65 km, respectively. The MWR–DIAL comparison at 27 km also presents good agreement, with a mean bias error of −1 %.

This paper provides a detailed description of a first-principle optimal estimation method (OEM) applied to ozone retrieval analysis using differential absorption lidar (DIAL) measurements. The air density, detector dead times, background coefficients, and lidar constants are simultaneously retrieved along with ozone density profiles. Using an averaging kernel, the OEM provides the vertical resolution of the retrieval as a function of altitude. A maximum acceptable height at which the a priori has a small contribution to the retrieval is calculated for each profile as well. Moreover, a complete uncertainty budget including both systematic and statistical uncertainties is given for each individual retrieved profile. Long-term stratospheric DIAL ozone measurements have been carried out at the Observatoire de Haute-Provence (OHP) since 1985. The OEM is applied to three nights of measurements at OHP during an intensive ozone campaign in July 2017 for which coincident lidar–ozonesonde measurements are available. The retrieved ozone density profiles are in good agreement with both traditional analysis and the ozonesonde measurements. For the three nights of measurements, below 15 km the difference between the OEM and the sonde profiles is less than 25 %, and at altitudes between 15 and 25 km the difference is less than 10 %; the OEM can successfully catch many variations in ozone, which are detected in the sonde profiles due to its ability to adjust its vertical resolution as the signal varies. Above 25 km the difference between the OEM and the sonde profiles does not exceed 20 %.

Observing stratospheric ozone is essential to assess whether the Montreal Protocol has succeeded in saving the ozone layer by banning ozone depleting substances. Recent studies have reported positive trends, indicating that ozone is recovering in the upper stratosphere at mid-latitudes, but the trend magnitudes differ, and uncertainties are still high. Trends and their uncertainties are influenced by factors such as instrumental drifts, sampling patterns, discontinuities, biases, or short-term anomalies that may all mask a potential ozone recovery. The present study investigates how anomalies, temporal measurement sampling rates, and trend period lengths influence resulting trends. We present an approach for handling suspicious anomalies in trend estimations. For this, we analysed multiple ground-based stratospheric ozone records in central Europe to identify anomalous periods in data from the GROund-based Millimetre-wave Ozone Spectrometer (GROMOS) located in Bern, Switzerland. The detected anomalies were then used to estimate ozone trends from the GROMOS time series by considering the anomalous observations in the regression. We compare our improved GROMOS trend estimate with results derived from the other ground-based ozone records (lidars, ozonesondes, and microwave radiometers), that are all part of the Network for the Detection of Atmospheric Composition Change (NDACC). The data indicate positive trends of 1 % decade−1 to 3 % decade−1 at an altitude of about 39 km (3 hPa), providing a confirmation of ozone recovery in the upper stratosphere in agreement with satellite observations. At lower altitudes, the ground station data show inconsistent trend results, which emphasize the importance of ongoing research on ozone trends in the lower stratosphere. Our presented method of a combined analysis of ground station data provides a useful approach to recognize and to reduce uncertainties in stratospheric ozone trends by considering anomalies in the trend estimation. We conclude that stratospheric trend estimations still need improvement and that our approach provides a tool that can also be useful for other data sets.

We have compared 2433 nights of Rayleigh lidar temperatures measured at L'Observatoire de Haute Provence (OHP) with co-located temperature measurements from the Microwave Limb Sounder (MLS) and the Sounding of the Atmosphere by Broadband Emission Radiometry instrument (SABER). The comparisons were conducted using data from January 2002 to March 2018 in the geographic region around the observatory (43.93∘ N, 5.71∘ E). We have found systematic differences between the temperatures measured from the ground-based lidar and those measured from the satellites, which suggest non-linear distortions in the satellite altitude retrievals. We see a winter stratopause cold bias in the satellite measurements with respect to the lidar (−6 K for SABER and −17 K for MLS), a summer mesospheric warm bias (6 K near 60 km), and a vertically structured bias for MLS (−4 to 4 K). We have corrected the stratopause height of the satellite measurements using the lidar temperatures and have seen an improvement in the comparison. The winter relative cold bias between the lidar and SABER has been reduced to 1 K in both the stratosphere and mesosphere and the summer mesospheric warm bias is reduced to 2 K. Stratopause altitude corrections have reduced the relative cold bias between the lidar and MLS by 4 K in the early autumn and late spring but were unable to address the apparent vertical oscillations in the MLS temperature profiles.

The objective of this paper and its companion (Wing et al., 2018) is to show that ground-based lidar temperatures are a stable, accurate, and precise data set for use in validating satellite temperatures at high vertical resolution. Long-term lidar observations of the middle atmosphere have been conducted at the Observatoire de Haute-Provence (OHP), located in southern France (43.93° N, 5.71° E), since 1978. Making use of 20 years of high-quality co-located lidar measurements, we have shown that lidar temperatures calculated using the Rayleigh technique at 532 nm are statistically identical to lidar temperatures calculated from the non-absorbing 355 nm channel of a differential absorption lidar (DIAL) system. This result is of interest to members of the Network for the Detection of Atmospheric Composition Change (NDACC) ozone lidar community seeking to produce validated temperature products. Additionally, we have addressed previously published concerns of lidar–satellite relative warm bias in comparisons of upper-mesospheric and lower-thermospheric (UMLT) temperature profiles. We detail a data treatment algorithm which minimizes known errors due to data selection procedures, a priori choices, and initialization parameters inherent in the lidar retrieval. Our algorithm results in a median cooling of the lidar-calculated absolute temperature profile by 20 K at 90 km altitude with respect to the standard OHP NDACC lidar temperature algorithm. The confidence engendered by the long-term cross-validation of two independent lidars and the improved lidar temperature data set is exploited in Wing et al. (2018) for use in multi-year satellite validations.

Atmospheric ozone plays a key role in air quality and the radiation budget of the Earth, both directly and through its chemical influence on other trace gases. Assessments of the atmospheric ozone distribution and associated climate change therefore demand accurate vertically resolved ozone observations with both stratospheric and tropospheric sensitivity, on both global and regional scales, and both in the long term and at shorter timescales. Such observations have been acquired by two series of European nadir-viewing ozone profilers, namely the scattered-light UV–visible spectrometers of the GOME family, launched regularly since 1995 (GOME, SCIAMACHY, OMI, GOME-2A/B, TROPOMI, and the upcoming Sentinel-5 series), and the thermal infrared emission sounders of the IASI type, launched regularly since 2006 (IASI on Metop platforms and the upcoming IASI-NG on Metop-SG). In particular, several Level-2 retrieved, Level-3 monthly gridded, and Level-4 assimilated nadir ozone profile data products have been improved and harmonized in the context of the ozone project of the European Space Agency's Climate Change Initiative (ESA Ozone_cci). To verify their fitness for purpose, these ozone datasets must undergo a comprehensive quality assessment (QA), including (a) detailed identification of their geographical, vertical, and temporal domains of validity; (b) quantification of their potential bias, noise, and drift and their dependences on major influence quantities; and (c) assessment of the mutual consistency of data from different sounders. For this purpose we have applied to the Ozone_cci Climate Research Data Package (CRDP) released in 2017 the versatile QA and validation system Multi-TASTE, which has been developed in the context of several heritage projects (ESA's Multi-TASTE, EUMETSAT's O3M-SAF, and the European Commission's FP6 GEOmon and FP7 QA4ECV). This work, as the second in a series of four Ozone_cci validation papers, reports for the first time on data content studies, information content studies and ground-based validation for both the GOME- and IASI-type climate data records combined. The ground-based reference measurements have been provided by the Network for the Detection of Atmospheric Composition Change (NDACC), NASA's Southern Hemisphere Additional Ozonesonde programme (SHADOZ), and other ozonesonde and lidar stations contributing to the World Meteorological Organisation's Global Atmosphere Watch (WMO GAW). The nadir ozone profile CRDP quality assessment reveals that all nadir ozone profile products under study fulfil the GCOS user requirements in terms of observation frequency and horizontal and vertical resolution. Yet all L2 observations also show sensitivity outliers in the UTLS and are strongly correlated vertically due to substantial averaging kernel fluctuations that extend far beyond the kernel's 15 km FWHM. The CRDP typically does not comply with the GCOS user requirements in terms of total uncertainty and decadal drift, except for the UV–visible L4 dataset. The drift values of the L2 GOME and OMI, the L3 IASI, and the L4 assimilated products are found to be overall insignificant, however, and applying appropriate altitude-dependent bias and drift corrections make the data fit for climate and atmospheric composition monitoring and modelling purposes. Dependence of the Ozone_cci data quality on major influence quantities – resulting in data screening suggestions to users – and perspectives for the Copernicus Sentinel missions are additionally discussed.

The long-term evolution of total ozone column inside the Antarctic polar vortex is investigated over the 1980–2017 period. Trend analyses are performed using a multilinear regression (MLR) model based on various proxies for the evaluation of ozone interannual variability (heat flux, quasi-biennial oscillation, solar flux, Antarctic oscillation and aerosols). Annual total ozone column measurements corresponding to the mean monthly values inside the vortex in September and during the period of maximum ozone depletion from 15 September to 15 October are used. Total ozone columns from the Multi-Sensor Reanalysis version 2 (MSR-2) dataset and from a combined record based on TOMS and OMI satellite datasets with gaps filled by MSR-2 (1993–1995) are considered in the study. Ozone trends are computed by a piece-wise trend (PWT) proxy that includes two linear functions before and after the turnaround year in 2001 and a parabolic function to account for the saturation of the polar ozone destruction. In order to evaluate average total ozone within the vortex, two classification methods are used, based on the potential vorticity gradient as a function of equivalent latitude. The first standard one considers this gradient at a single isentropic level (475 or 550 K), while the second one uses a range of isentropic levels between 400 and 600 K. The regression model includes a new proxy (GRAD) linked to the gradient of potential vorticity as a function of equivalent latitude and representing the stability of the vortex during the studied month. The determination coefficient (R2) between observations and modelled values increases by ∼ 0.05 when this proxy is included in the MLR model. Highest R2 (0.92–0.95) and minimum residuals are obtained for the second classification method for both datasets and months. Trends in September over the 2001–2017 period are statistically significant at 2σ level with values ranging between 1.84 ± 1.03 and 2.83 ± 1.48 DU yr−1 depending on the methods and considered proxies. This result confirms the recent studies of Antarctic ozone healing during that month. Trends from 2001 are 2 to 3 times smaller than before the turnaround year, as expected from the response to the slowly ozone-depleting substances decrease in polar regions. For the first time, significant trends are found for the period of maximum ozone depletion. Estimated trends from 2001 for the 15 September–15 October period over 2001–2017 vary from 1.21 ± 0.83 to 1.96 DU ± 0.99 yr−1 and are significant at 2σ level. MLR analysis is also applied to the ozone mass deficit (OMD) metric for both periods, considering a threshold at 220 DU and total ozone columns south of 60° S. Significant trend values are observed for all cases and periods. A decrease of OMD of 0.86 ± 0.36 and 0.65 ± 0.33 Mt yr−1 since 2001 is observed in September and 15 September–15 October, respectively. Ozone recovery is also confirmed by a steady decrease of the relative area of total ozone values lower than 175 DU within the vortex in the 15 September–15 October period since 2010 and a delay in the occurrence of ozone levels below 125 DU since 2005.

This paper is focusing on the representativeness of single lidar stations for zonally averaged ozone profile variations over the middle and upper stratosphere. From the lower to the upper stratosphere, ozone profiles from single or grouped lidar stations correlate well with zonal means calculated from the Solar Backscatter Ultraviolet Radiometer (SBUV) satellite overpasses. The best representativeness with significant correlation coefficients is found within ±15° of latitude circles north or south of any lidar station. This paper also includes a multivariate linear regression (MLR) analysis on the relative importance of proxy time series for explaining variations in the vertical ozone profiles. Studied proxies represent variability due to influences outside of the earth system (solar cycle) and within the earth system, i.e. dynamic processes (the Quasi Biennial Oscillation, QBO; the Arctic Oscillation, AO; the Antarctic Oscillation, AAO; the El Niño Southern Oscillation, ENSO), those due to volcanic aerosol (aerosol optical depth, AOD), tropopause height changes (including global warming) and those influences due to anthropogenic contributions to atmospheric chemistry (equivalent effective stratospheric chlorine, EESC). Ozone trends are estimated, with and without removal of proxies, from the total available 1980 to 2015 SBUV record. Except for the chemistry related proxy (EESC) and its orthogonal function, the removal of the other proxies does not alter the significance of the estimated long-term trends. At heights above 15 hPa an inflection point between 1997 and 1999 marks the end of significant negative ozone trends, followed by a recent period between 1998 and 2015 with positive ozone trends. At heights between 15 and 40 hPa the pre-1998 negative ozone trends tend to become less significant as we move towards 2015, below which the lower stratosphere ozone decline continues in agreement with findings of recent literature.

Surface ultraviolet radiation (SUR) is not an increasing concern after the implementation of the Montreal Protocol and the recovery of the ozone layer Morgenstern et al.(2008). However, large uncertainties remain in the prediction of future changes of SUR Bais et al.(2015). Several studies pointed out that UV-B impacts the biosphere Erickson et al.(2015), especially the aquatic system, which plays a central part in the biogeochemical cycle Hader et al.(2007). It can affect phytoplankton productivity Smith and Cullen(1995). This influence can result in either positive or negative feedback on climate (Zepp et al., 2007). Global circulation model simulations predict an acceleration of the Brewer-Dobson circulation over the next century (Butchart, 2014), which would lead to a decrease in ozone levels in the tropics and an enhancement at higher latitudes (Hegglin and Shepherd, 2009). Reunion Island is located in the tropics (21° S, 55° E), in a part of the world where the amount of ozone in the ozone column is naturally low. In addition, this island is mountainous and the marine atmosphere is often clean with low aerosol concentrations. Thus, measurements show much higher SUR than at other sites at the same latitude or at midlatitudes. Ground-based measurements of SUR have been taken on Reunion Island by a Bentham DTMc300 spectroradiometer since 2009. This instrument is affiliated with the Network for the Detection of Atmospheric Composition Change (NDACC). In order to quantify the future evolution of SUR in the tropics, it is necessary to validate a model against present observations. This study is designed to be a preliminary parametric and sensitivity study of SUR modelling in the tropics. We developed a local parameterisation using the Tropospheric Ultraviolet and Visible Model (TUV; Madronich, 1993) and compared the output of TUV to multiple years of Bentham spectral measurements. This comparison started in early 2009 and continued until 2016. Only clear-sky SUR was modelled, so we needed to sort out the clear-sky measurements. We used two methods to detect cloudy conditions: the first was based on an observer's hourly report on the sky cover, while the second was based on applying Long and Ackerman(2000)'s algorithm to broadband pyranometer data to obtain the cloud fraction and then discriminating clear-sky windows on SUR measurements. Long et al. (2006)'s algorithm, with the co-located pyranometer data, gave better results for clear-sky filtering than the observer's report. Multiple model inputs were tested to evaluate the model sensitivity to different parameters such as total ozone column, aerosol optical properties, extraterrestrial spectrum or ozone cross section. For total column ozone, we used ground-based measurements from the SAOZ (Système d'Analyse par Observation Zénithale) spectrometer and satellite measurements from the OMI and SBUV instruments, while ozone profiles were derived from radio-soundings and the MLS ozone product. Aerosol optical properties came from a local aerosol climatology established using a Cimel photometer. Since the mean difference between various inputs of total ozone column was small, the corresponding response on UVI modelling was also quite small, at about 1 %. The radiative amplification factor of total ozone column on UVI was also compared for observations and the model. Finally, we were able to estimate UVI on Reunion Island with, at best, a mean relative difference of about 0.5 %, compared to clear-sky observations.

After 43 years of inactivity, the Calbuco volcano, which is located in the southern part of Chile, erupted on 22 April 2015. The space–time evolutions (distribution and transport) of its aerosol plume are investigated by combining satellite (CALIOP, IASI, OMPS), in situ aerosol counting (LOAC OPC) and lidar observations, and the MIMOSA advection model. The Calbuco aerosol plume reached the Indian Ocean 1 week after the eruption. Over the Reunion Island site (21° S, 55.5° E), the aerosol signal was unambiguously enhanced in comparison with background conditions, with a volcanic aerosol layer extending from 18 to 21 km during the May–July period. All the data reveal an increase by a factor of ∼ 2 in the SAOD (stratospheric aerosol optical depth) with respect to values observed before the eruption. The aerosol mass e-folding time is approximately 90 days, which is rather close to the value ( ∼ 80 days) reported for the Sarychev eruption. Microphysical measurements obtained before, during, and after the eruption reflecting the impact of the Calbuco eruption on the lower stratospheric aerosol content have been analyzed over the Reunion Island site. During the passage of the plume, the volcanic aerosol was characterized by an effective radius of 0.16 ± 0.02 µm with a unimodal size distribution for particles above 0.2 µm in diameter. Particle concentrations for sizes larger than 1 µm are too low to be properly detected by the LOAC OPC. The aerosol number concentration was ∼ 20 times higher that observed before and 1 year after the eruption. According to OMPS and lidar observations, a tendency toward conditions before the eruption was observed by April 2016. The volcanic aerosol plume is advected eastward in the Southern Hemisphere and its latitudinal extent is clearly bounded by the subtropical barrier and the polar vortex. The transient behavior of the aerosol layers observed above Reunion Island between May and July 2015 reflects an inhomogeneous spatio-temporal distribution of the plume, which is controlled by the localization of these dynamical barriers.

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.

We validate the Ozone Monitoring Instrument (OMI) Ozone Profile (PROFOZ) product from October 2004 through December 2014 retrieved by the Smithsonian Astrophysical Observatory (SAO) algorithm against ozonesonde observations. We also evaluate the effects of OMI row anomaly (RA) on the retrieval by dividing the dataset into before and after the occurrence of serious OMI RA, i.e., pre-RA (2004–2008) and post-RA (2009–2014). The retrieval shows good agreement with ozonesondes in the tropics and midlatitudes and for pressure ∼ 50 hPa after applying OMI averaging kernels to ozonesonde data. The MBs of the stratospheric ozone column (SOC, the ozone column from the tropopause pressure to the ozonesonde burst pressure) are within 2 % with SDs of ∼ 50 hPa. The SOC MBs increase up to 3 % with SDs as great as 6 % and the TOC SDs increase up to 30 %. The comparison generally degrades at larger solar zenith angles (SZA) due to weaker signals and additional sources of error, leading to worse performance at high latitudes and during the midlatitude winter. Agreement also degrades with increasing cloudiness for pressure > ∼ 100 hPa and varies with cross-track position, especially with large MBs and SDs at extreme off-nadir positions. In the tropics and midlatitudes, the post-RA comparison is considerably worse with larger SDs reaching 2 % in the stratosphere and 8 % in the troposphere and up to 6 % in TOC. There are systematic differences that vary with latitude compared to the pre-RA comparison. The retrieval comparison demonstrates good long-term stability during the pre-RA period but exhibits a statistically significant trend of 0.14–0.7 % year−1 for pressure −1 in SOC, and −0. 33 DU year−1 in TOC during the post-RA period. The spatiotemporal variation of retrieval performance suggests the need to improve OMI's radiometric calibration especially during the post-RA period to maintain the long-term stability and reduce the latitude/season/SZA and cross-track dependency of retrieval quality.

The article presents new high-quality continuous stratospheric aerosol observations spanning 1994–2015 at the French Observatoire de Haute-Provence (OHP, 44° N, 6° E) obtained by two independent, regularly maintained lidar systems operating within the Network for Detection of Atmospheric Composition Change (NDACC). Lidar series are compared with global-coverage observations by Stratospheric Aerosol and Gas Experiment (SAGE II), Global Ozone Monitoring by Occultation of Stars (GOMOS), Optical Spectrograph and InfraRed Imaging System (OSIRIS), Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP), and Ozone Mapping Profiling Suite (OMPS) satellite instruments, altogether covering the time span of OHP lidar measurements. Local OHP and zonal-mean satellite series of stratospheric aerosol optical depth are in excellent agreement, allowing for accurate characterization of stratospheric aerosol evolution and variability at northern midlatitudes during the last 2 decades. The combination of local and global observations is used for a careful separation between volcanically perturbed and quiescent periods. While the volcanic signatures dominate the stratospheric aerosol record, the background aerosol abundance is found to be modulated remotely by the poleward transport of convectively cleansed air from the deep tropics and aerosol-laden air from the Asian monsoon region. The annual cycle of background aerosol at midlatitudes, featuring a minimum during late spring and a maximum during late summer, correlates with that of water vapor from the Aura Microwave Limb Sounder (MLS). Observations covering two volcanically quiescent periods over the last 2 decades provide an indication of a growth in the nonvolcanic component of stratospheric aerosol. A statistically significant factor of 2 increase in nonvolcanic aerosol since 1998, seasonally restricted to late summer and fall, is associated with the influence of the Asian monsoon and growing pollution therein.

A standardized approach for the definition and reporting of vertical resolution of the ozone and temperature lidar profiles contributing to the Network for the Detection for Atmospheric Composition Change (NDACC) database is proposed. Two standardized definitions homogeneously and unequivocally describing the impact of vertical filtering are recommended. The first proposed definition is based on the width of the response to a finite-impulse-type perturbation. The response is computed by convolving the filter coefficients with an impulse function, namely, a Kronecker delta function for smoothing filters, and a Heaviside step function for derivative filters. Once the response has been computed, the proposed standardized definition of vertical resolution is given by Δz = δz × HFWHM, where δz is the lidar's sampling resolution and HFWHM is the full width at half maximum (FWHM) of the response, measured in sampling intervals. The second proposed definition relates to digital filtering theory. After applying a Laplace transform to a set of filter coefficients, the filter's gain characterizing the effect of the filter on the signal in the frequency domain is computed, from which the cut-off frequency fC, defined as the frequency at which the gain equals 0.5, is computed. Vertical resolution is then defined by Δz = δz∕(2fC). Unlike common practice in the field of spectral analysis, a factor 2fC instead of fC is used here to yield vertical resolution values nearly equal to the values obtained with the impulse response definition using the same filter coefficients. When using either of the proposed definitions, unsmoothed signals yield the best possible vertical resolution Δz = δz (one sampling bin). Numerical tools were developed to support the implementation of these definitions across all NDACC lidar groups. The tools consist of ready-to-use “plug-in” routines written in several programming languages that can be inserted into any lidar data processing software and called each time a filtering operation occurs in the data processing chain. When data processing implies multiple smoothing operations, the filtering information is analytically propagated through the multiple calls to the routines in order for the standardized values of vertical resolution to remain theoretically and numerically exact at the very end of data processing.

A standardized approach for the definition, propagation, and reporting of uncertainty in the ozone differential absorption lidar data products contributing to the Network for the Detection for Atmospheric Composition Change (NDACC) database is proposed. One essential aspect of the proposed approach is the propagation in parallel of all independent uncertainty components through the data processing chain before they are combined together to form the ozone combined standard uncertainty. The independent uncertainty components contributing to the overall budget include random noise associated with signal detection, uncertainty due to saturation correction, background noise extraction, the absorption cross sections of O3, NO2, SO2, and O2, the molecular extinction cross sections, and the number densities of the air, NO2, and SO2. The expression of the individual uncertainty components and their step-by-step propagation through the ozone differential absorption lidar (DIAL) processing chain are thoroughly estimated. All sources of uncertainty except detection noise imply correlated terms in the vertical dimension, which requires knowledge of the covariance matrix when the lidar signal is vertically filtered. In addition, the covariance terms must be taken into account if the same detection hardware is shared by the lidar receiver channels at the absorbed and non-absorbed wavelengths. The ozone uncertainty budget is presented as much as possible in a generic form (i.e., as a function of instrument performance and wavelength) so that all NDACC ozone DIAL investigators across the network can estimate, for their own instrument and in a straightforward manner, the expected impact of each reviewed uncertainty component. In addition, two actual examples of full uncertainty budget are provided, using nighttime measurements from the tropospheric ozone DIAL located at the Jet Propulsion Laboratory (JPL) Table Mountain Facility, California, and nighttime measurements from the JPL stratospheric ozone DIAL located at Mauna Loa Observatory, Hawai'i.

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

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.

A detailed analysis of the polar ozone loss processes during 10 recent Antarctic winters is presented with high-resolution MIMOSA–CHIM (Modèle Isentrope du transport Méso-échelle de l'Ozone Stratosphérique par Advection avec CHIMie) model simulations and high-frequency polar vortex observations from the Aura microwave limb sounder (MLS) instrument. The high-frequency measurements and simulations help to characterize the winters and assist the interpretation of interannual variability better than either data or simulations alone. Our model results for the Antarctic winters of 2004–2013 show that chemical ozone loss starts in the edge region of the vortex at equivalent latitudes (EqLs) of 65–67° S in mid-June–July. The loss progresses with time at higher EqLs and intensifies during August–September over the range 400–600 K. The loss peaks in late September–early October, when all EqLs (65–83° S) show a similar loss and the maximum loss (> 2 ppmv – parts per million by volume) is found over a broad vertical range of 475–550 K. In the lower stratosphere, most winters show similar ozone loss and production rates. In general, at 500 K, the loss rates are about 2–3 ppbv sh−1 (parts per billion by volume per sunlit hour) in July and 4–5 ppbv sh−1 in August–mid-September, while they drop rapidly to 0 by mid-October. In the middle stratosphere, the loss rates are about 3–5 ppbv sh−1 in July–August and October at 675 K. On average, the MIMOSA–CHIM simulations show that the very cold winters of 2005 and 2006 exhibit a maximum loss of ~ 3.5 ppmv around 550 K or about 149–173 DU over 350–850 K, and the warmer winters of 2004, 2010, and 2012 show a loss of ~ 2.6 ppmv around 475–500 K or 131–154 DU over 350–850 K. The winters of 2007, 2008, and 2011 were moderately cold, and thus both ozone loss and peak loss altitudes are between these two ranges (3 ppmv around 500 K or 150 ± 10 DU). The modeled ozone loss values are in reasonably good agreement with those estimated from Aura MLS measurements, but the model underestimates the observed ClO, largely due to the slower vertical descent in the model during spring.

A methodology for the round-robin evaluation and the geophysical validation of ozone profile data retrieved from nadir UV backscatter satellite measurements is detailed and discussed, consisting of data set content studies, information content studies, co-location studies, and comparisons with reference measurements. Within the European Space Agency's Climate Change Initiative on ozone (Ozone_cci project), the proposed round-robin procedure is applied to two nadir ozone profile data sets retrieved at the Royal Netherlands Meteorological Institute (KNMI) and the Rutherford Appleton Laboratory (RAL, United Kingdom), using their respective OPERA v1.26 and RAL v2.1 optimal estimation algorithms, from MetOp-A GOME-2 (i.e. the second generation Global Ozone Monitoring Experiment on the first Meteorological Operational Satellite) measurements taken in 2008. The ground-based comparisons use ozonesonde and lidar profiles as reference data, acquired by the Network for the Detection of Atmospheric Composition Change (NDACC), Southern Hemisphere Additional Ozonesonde programme (SHADOZ), and other stations of the World Meteorological Organisation's Global Atmosphere Watch (WMO GAW). This direct illustration highlights practical issues that inevitably emerge from discrepancies in e.g. profile representation and vertical smoothing, for which different recipes are investigated and discussed. Several approaches for information content quantification, vertical resolution estimation, and reference profile resampling are compared and applied as well. The paper concludes with compliance estimates of the two GOME-2 ozone profile data sets with user requirements from the Global Climate Observing System (GCOS) and from climate modellers.

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

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.

Drifts, trends and periodic variations were calculated from monthly zonally averaged ozone profiles. The ozone profiles were derived from level-1b data of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) by means of the scientific level-2 processor run by the Karlsruhe Institute of Technology (KIT), Institute for Meteorology and Climate Research (IMK). All trend and drift analyses were performed using a multilinear parametric trend model which includes a linear term, several harmonics with period lengths from 3 to 24 months and the quasi-biennial oscillation (QBO). Drifts at 2-sigma significance level were mainly negative for ozone relative to Aura MLS and Odin OSIRIS and negative or near zero for most of the comparisons to lidar measurements. Lidar stations used here include those at Hohenpeissenberg (47.8° N, 11.0° E), Lauder (45.0° S, 169.7° E), Mauna Loa (19.5° N, 155.6° W), Observatoire Haute Provence (43.9° N, 5.7° E) and Table Mountain (34.4° N, 117.7° W). Drifts against the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) were found to be mostly insignificant. The assessed MIPAS ozone trends cover the time period of July 2002 to April 2012 and range from −0.56 ppmv decade−1 to +0.48 ppmv decade−1 (−0.52 ppmv decade−1 to +0.47 ppmv decade−1 when displayed on pressure coordinates) depending on altitude/pressure and latitude. From the empirical drift analyses we conclude that the real ozone trends might be slightly more positive/less negative than those calculated from the MIPAS data, by conceding the possibility of MIPAS having a very small (approximately within −0.3 ppmv decade−1) negative drift for ozone. This leads to drift-corrected trends of −0.41 ppmv decade−1 to +0.55 ppmv decade−1 (−0.38 ppmv decade−1 to +0.53 ppmv decade−1 when displayed on pressure coordinates) for the time period covered by MIPAS Envisat measurements, with very few negative and large areas of positive trends at mid-latitudes for both hemispheres around and above 30 km (~10 hPa). Negative trends are found in the tropics around 25 and 35 km (~25 and 5 hPa), while an area of positive trends is located right above the tropical tropopause. These findings are in good agreement with the recent literature. Differences of the trends compared with the recent literature could be explained by a possible shift of the subtropical mixing barriers. Results for the altitude–latitude distribution of amplitudes of the quasi-biennial, annual and the semi-annual oscillation are overall in very good agreement with recent findings.

Since the nineties, atmospheric measurement systems have been deployed at Reunion Island, mainly for monitoring the atmospheric composition in the framework of NDSC/NDACC (Network for the Detection of Stratospheric Change/Network for the Detection of Atmospheric Composition Change). The location of Reunion Island presents a great interest because there are very few multi-instrumented stations in the tropics and particularly in the southern hemisphere. In 2012, a new observatory was commissioned in Maïdo at 2200 m above sea level: it hosts various instruments for atmospheric measurements, including lidar systems, spectro-radiometers and in situ gas and aerosol measurements. This new high-altitude Maïdo station provides an opportunity: 1. to improve the performance of the optical instruments above the marine boundary layer, and to open new perspectives on upper troposphere and lower stratosphere studies; 2. to develop in situ measurements of the atmospheric composition for climate change surveys, in a reference site in the tropical/subtropical region of the southern hemisphere; 3. to offer trans-national access to host experiments or measurement campaigns for focused process studies.

The trends and variability of ozone are assessed over a northern mid-latitude station, Haute-Provence Observatory (OHP: 43.93° N, 5.71° E), using total column ozone observations from the Dobson and Système d'Analyse par Observation Zénithale spectrometers, and stratospheric ozone profile measurements from light detection and ranging (lidar), ozonesondes, Stratospheric Aerosol and Gas Experiment (SAGE) II, Halogen Occultation Experiment (HALOE) and Aura Microwave Limb Sounder (MLS). A multivariate regression model with quasi-biennial oscillation (QBO), solar flux, aerosol optical thickness, heat flux, North Atlantic Oscillation (NAO) and a piecewise linear trend (PWLT) or equivalent effective stratospheric chlorine (EESC) functions is applied to the ozone anomalies. The maximum variability of ozone in winter/spring is explained by QBO and heat flux in the ranges 15–45 km and 15–24 km, respectively. The NAO shows maximum influence in the lower stratosphere during winter, while the solar flux influence is largest in the lower and middle stratosphere in summer. The total column ozone trends estimated from the PWLT and EESC functions are of −1.47 ± 0.27 and −1.40 ± 0.25 DU yr−1, respectively, over the period 1984–1996 and about 0.55 ± 0.30 and 0.42 ± 0.08 DU yr−1, respectively, over the period 1997–2010. The ozone profiles yield similar and significant EESC-based and PWLT trends for 1984–1996, and are about −0.5 and −0.8% yr−1 in the lower and upper stratosphere, respectively. For 1997–2010, the EESC-based and PWLT estimates are of the order of 0.3 and 0.1% yr−1, respectively, in the 18–28 km range, and at 40–45 km, EESC provides significant ozone trends larger than the insignificant PWLT results. Furthermore, very similar vertical trends for the respective time periods are also deduced from another long-term satellite-based data set (GOZCARDS–Global OZone Chemistry And Related trace gas Data records for the Stratosphere) sampled at northern mid-latitudes. Therefore, this analysis unveils ozone recovery signals from total column ozone and profile measurements at OHP, and hence in the northern mid-latitudes.

Aerosols from the Sarychev volcano eruption (Kuril Islands, northeast of Japan) were observed in the Arctic lower stratosphere a few days after the strongest SO2 injection which occurred on 15 and 16 June 2009. From the observations provided by the Infrared Atmospheric Sounding Interferometer (IASI) an estimated 0.9 Tg of sulphur dioxide was injected into the upper troposphere and lower stratosphere (UTLS). The resultant stratospheric sulphate aerosols were detected from satellites by the Optical Spectrograph and Infrared Imaging System (OSIRIS) limb sounder and by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) and from the surface by the Network for the Detection of Atmospheric Composition Changes (NDACC) lidar deployed at OHP (Observatoire de Haute-Provence, France). By the first week of July the aerosol plume had spread out over the entire Arctic region. The Sarychev-induced stratospheric aerosol over the Kiruna region (north of Sweden) was measured by the Stratospheric and Tropospheric Aerosol Counter (STAC) during eight balloon flights planned in August and September 2009. During this balloon campaign the Micro Radiomètre Ballon (MicroRADIBAL) and the Spectroscopie d'Absorption Lunaire pour l'Observation des Minoritaires Ozone et NOx (SALOMON) remote-sensing instruments also observed these aerosols. Aerosol concentrations returned to near-background levels by spring 2010. The effective radius, the surface area density (SAD), the aerosol extinction, and the total sulphur mass from STAC in situ measurements are enhanced with mean values in the range 0.15–0.21 μm, 5.5–14.7 μm2 cm−3, 5.5–29.5 × 10−4 km−1, and 4.9–12.6 × 10−10 kg[S] kg−1[air], respectively, between 14 km and 18 km. The observed and modelled e-folding time of sulphate aerosols from the Sarychev eruption is around 70–80 days, a value much shorter than the 12–14 months calculated for aerosols from the 1991 eruption of Mt Pinatubo. The OSIRIS stratospheric aerosol optical depth (AOD) at 750 nm is enhanced by a factor of 6, with a value of 0.02 in late July compared to 0.0035 before the eruption. The HadGEM2 and MIMOSA model outputs indicate that aerosol layers in polar region up to 14–15 km are largely modulated by stratosphere–troposphere exchange processes. The spatial extent of the Sarychev plume is well represented in the HadGEM2 model with lower altitudes of the plume being controlled by upper tropospheric troughs which displace the plume downward and upper altitudes around 18–20 km, in agreement with lidar observations. Good consistency is found between the HadGEM2 sulphur mass density and the value inferred from the STAC observations, with a maximum located about 1 km above the tropopause ranging from 1 to 2 × 10−9 kg[S] kg−1[air], which is one order of magnitude higher than the background level.

Record-low ozone column densities (with a minimum of 212 DU) persisted over three weeks at the Río Gallegos NDACC (Network for the Detection of Atmospheric Composition Change) station (51.5° S, 69.3° W) in November 2009. Total ozone remained two standard deviations below the climatological mean for five consecutive days during this period. The statistical analysis of 30 years of satellite data from the Multi Sensor Reanalysis (MSR) database for Río Gallegos revealed that such a long-lasting low-ozone episode is a rare occurrence. The event is examined using height-resolved ozone lidar measurements at Río Gallegos, and observations from satellite and ground-based instruments. The computed relative difference between the measured total ozone and the climatological monthly mean shows reductions varying between 10 and 30% with an average decrease of 25%. The mean absolute difference of total ozone column with respect to climatological monthly mean ozone column is around 75 DU. Extreme values of the UV index (UVI) were measured at the ground for this period, with the daily maximum UVI of around 13 on 15 and 28 November. The high-resolution MIMOSA-CHIM (Modélisation Isentrope du transport Méso-échelle de l'Ozone Stratosphérique par Advection) model was used to interpret the ozone depletion event. An ozone decrease of about 2 ppmv was observed in mid-November at the 550 K isentropic level (~22 km). The position of Río Gallegos relative to the polar vortex was classified using equivalent latitude maps. During the second week of November, the vortex was over the station at all isentropic levels, but after 20 November and until the end of the month, only the 10 lower levels in the stratosphere were affected by vortex overpasses with ozone poor air masses. A rapid recovery of the ozone column density was observed later, due to an ozone rich filament moving over Río Gallegos between 18 and 24 km in the first two weeks of December 2009.

We present a detailed discussion of the chemical and dynamical processes in the Arctic winters 1996/1997 and 2010/2011 with high resolution chemical transport model (CTM) simulations and space-based observations. In the Arctic winter 2010/2011, the lower stratospheric minimum temperatures were below 195 K for a record period of time, from December to mid-April, and a strong and stable vortex was present during that period. Simulations with the Mimosa-Chim CTM show that the chemical ozone loss started in early January and progressed slowly to 1 ppmv (parts per million by volume) by late February. The loss intensified by early March and reached a record maximum of ~2.4 ppmv in the late March–early April period over a broad altitude range of 450–550 K. This coincides with elevated ozone loss rates of 2–4 ppbv sh−1 (parts per billion by volume/sunlit hour) and a contribution of about 30–55% and 30–35% from the ClO-ClO and ClO-BrO cycles, respectively, in late February and March. In addition, a contribution of 30–50% from the HOx cycle is also estimated in April. We also estimate a loss of about 0.7–1.2 ppmv contributed (75%) by the NOx cycle at 550–700 K. The ozone loss estimated in the partial column range of 350–550 K exhibits a record value of ~148 DU (Dobson Unit). This is the largest ozone loss ever estimated in the Arctic and is consistent with the remarkable chlorine activation and strong denitrification (40–50%) during the winter, as the modeled ClO shows ~1.8 ppbv in early January and ~1 ppbv in March at 450–550 K. These model results are in excellent agreement with those found from the Aura Microwave Limb Sounder observations. Our analyses also show that the ozone loss in 2010/2011 is close to that found in some Antarctic winters, for the first time in the observed history. Though the winter 1996/1997 was also very cold in March–April, the temperatures were higher in December–February, and, therefore, chlorine activation was moderate and ozone loss was average with about 1.2 ppmv at 475–550 K or 42 DU at 350–550 K, as diagnosed from the model simulations and measurements.

The long-term evolution of stratospheric ozone at different stations in the low and mid-latitudes is investigated. The analysis is performed by comparing the collocated profiles of ozone lidars, at the northern mid-latitudes (Meteorological Observatory Hohenpeißenberg, Haute-Provence Observatory, Tsukuba and Table Mountain Facility), tropics (Mauna Loa Observatory) and southern mid-latitudes (Lauder), with ozonesondes and space-borne sensors (SBUV(/2), SAGE II, HALOE, UARS MLS and Aura MLS), extracted around the stations. Relative differences are calculated to find biases and temporal drifts in the measurements. All measurement techniques show their best agreement with respect to the lidar at 20–40 km, where the differences and drifts are generally within ±5% and ±0.5% yr−1, respectively, at most stations. In addition, the stability of the long-term ozone observations (lidar, SBUV(/2), SAGE II and HALOE) is evaluated by the cross-comparison of each data set. In general, all lidars and SBUV(/2) exhibit near-zero drifts and the comparison between SAGE II and HALOE shows larger, but insignificant drifts. The RMS of the drifts of lidar and SBUV(/2) is 0.22 and 0.27% yr−1, respectively at 20–40 km. The average drifts of the long-term data sets, derived from various comparisons, are less than ±0.3% yr−1 in the 20–40 km altitude at all stations. A combined time series of the relative differences between SAGE II, HALOE and Aura MLS with respect to lidar data at six sites is constructed, to obtain long-term data sets lasting up to 27 years. The relative drifts derived from these combined data are very small, within ±0.2% yr−1.

In order to test the validity of ultraviolet index (UVI) satellite products and UVI model simulations for general public information, intercomparison involving three satellite instruments (SCIAMACHY, OMI and GOME-2), the Chemistry and Transport Model, Modélisation de la Chimie Atmosphérique Grande Echelle (MOCAGE), and ground-based instruments was performed in 2008 and 2009. The intercomparison highlighted a systematic high bias of ~1 UVI in the OMI clear-sky products compared to the SCIAMACHY and TUV model clear-sky products. The OMI and GOME-2 all-sky products are close to the ground-based observations with a low 6 % positive bias, comparable to the results found during the satellite validation campaigns. This result shows that OMI and GOME-2 all-sky products are well appropriate to evaluate the UV-risk on health. The study has pointed out the difficulty to take into account either in the retrieval algorithms or in the models, the large spatial and temporal cloud modification effect on UV radiation. This factor is crucial to provide good quality UV information. OMI and GOME-2 show a realistic UV variability as a function of the cloud cover. Nevertheless these satellite products do not sufficiently take into account the radiation reflected by clouds. MOCAGE numerical forecasts show good results during periods with low cloud covers, but are actually not adequate for overcast conditions; this is why Météo-France currently uses human-expertised cloudiness (rather than direct outputs from Numerical Prediction Models) together with MOCAGE clear-sky UV indices for its operational forecasts. From now on, the UV monitoring could be done using free satellite products (OMI, GOME-2) and operational forecast for general public by using modelling, as long as cloud forecasts and the parametrisation of the impact of cloudiness on UV radiation are adequate.

The coherence of stratospheric ozone time series retrieved from various observational records is investigated at Haute-Provence Observatory (OHP–43.93° N, 5.71° E). The analysis is accomplished through the intercomparison of collocated ozone measurements of Light Detection and Ranging (lidar) with Solar Backscatter UltraViolet(/2) (SBUV(/2)), Stratospheric Aerosol and Gas Experiment II (SAGE~II), Halogen Occultation Experiment (HALOE), Microwave Limb Sounder (MLS) on Upper Atmosphere Research Satellite (UARS) and Aura and Global Ozone Monitoring by Occultation of Stars (GOMOS) satellite observations as well as with in situ ozonesondes and ground-based Umkehr measurements performed at OHP. A detailed statistical study of the relative differences of ozone observations over the whole stratosphere is performed to detect any specific drift in the data. On average, all instruments show their best agreement with lidar at 20–40 km, where deviations are within ±5 %. Discrepancies are somewhat higher below 20 and above 40 km. The agreement with SAGE II data is remarkable since average differences are within ±1 % at 17–41 km. In contrast, Umkehr data underestimate systematically the lidar measurements in the whole stratosphere with a near zero bias at 16–8 hPa (~30 km). Drifts are estimated using simple linear regression for the data sets analysed in this study, from the monthly averaged difference time series. The derived values are less than ±0.5 % yr−1 in the 20–40 km altitude range and most drifts are not significant at the 2σ level. We also discuss the possibilities of extending the SAGE II and HALOE data with the GOMOS and Aura MLS data in consideration with relative offsets and drifts since the combination of such data sets are likely to be used for the study of stratospheric ozone recovery in the future.

The GOMOS ozone profiles have been analysed to evaluate the GOMOS ability to capture the long-term ozone evolution at mid-latitudes during the expected recovery phase of the ozone layer. Version 5 of the operational GOMOS ozone data has been compared with data from two of the longest ground-based instruments based on different techniques and already involved with many other previous space instrument validations. Comparisons between ground-based and GOMOS data confirm the occurrence of spurious retrievals mainly occurring since 2006. Using a selected set of data it is shown that some bad retrievals are induced by the increasing dark charge of the detectors combined with an inadequate method for its correction. This effect does not only induce a continuous bias, but is rather exhibiting a bimodal distribution including the correct profiles and the bad retrievals. For long-term analyses it is recommended filtering the data according to background light conditions and star temperature (spectrum shape). The new method of the dark charge estimate proposed to be implemented in the version 6 of the ESA algorithm seems to significantly reduce the occurrence of such effects and should allow to monitor stratospheric ozone using GOMOS data with greater confidence.

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

The polar stratospheric ozone loss during the Arctic winters 2004/2005–2009/2010 is investigated by using high resolution simulations from the chemical transport model Mimosa-Chim and observations from Aura Microwave Limb Sounder (MLS), by applying the passive tracer technique. The winter 2004/2005 shows the coldest temperatures, highest area of polar stratospheric clouds and strongest chlorine activation in 2004/2005–2009/2010. The ozone loss diagnosed from both simulations and measurements inside the polar vortex at 475 K ranges from 0.7 ppmv in the warm winter 2005/2006 to 1.5–1.7 ppmv in the cold winter 2004/2005. Halogenated (chlorine and bromine) catalytic cycles contribute to 75–90% of the ozone loss at this level. At 675 K the lowest loss of 0.3–0.5 ppmv is computed in 2008/2009, and the highest loss of 1.3 ppmv is estimated in 2006/2007 by the model and in 2004/2005 by MLS. Most of the ozone loss (60–75%) at this level results from nitrogen catalytic cycles rather than halogen cycles. At both 475 and 675 K levels the simulated ozone and ozone loss evolution inside the vortex is in reasonably good agreement with the MLS observations. The ozone partial column loss in 350–850 K deduced from the model calculations at the MLS sampling locations inside the polar vortex ranges between 43 DU in 2005/2006 and 109 DU in 2004/2005, while those derived from the MLS observations range between 26 DU and 115 DU for the same winters. The partial column ozone depletion derived in that vertical range is larger than that estimated in 350–550 K by 19±7 DU on average, mainly due to NOx chemistry. The column ozone loss estimates from both Mimosa-Chim and MLS in 350–850 K are generally in good agreement with those derived from ground-based ultraviolet-visible spectrometer total ozone observations for the respective winters, except in 2010.

The passive tracer method is used to estimate ozone loss from ground-based measurements in the Antarctic. A sensitivity study shows that the ozone depletion can be estimated within an accuracy of ~4%. The method is then applied to the ground-based observations from Arrival Heights, Belgrano, Concordia, Dumont d'Urville, Faraday, Halley, Marambio, Neumayer, Rothera, South Pole, Syowa, and Zhongshan for the diagnosis of ozone loss in the Antarctic. On average, the ten-day boxcar average of the vortex mean ozone column loss deduced from the ground-based stations was about 55±5% in 2005–2009. The ozone loss computed from the ground-based measurements is in very good agreement with those derived from satellite measurements (OMI and SCIAMACHY) and model simulations (REPROBUS and SLIMCAT), where the differences are within ±3–5%. The historical ground-based total ozone observations in October show that the depletion started in the late 1970s, reached a maximum in the early 1990s and stabilised afterwards due to saturation. There is no indication of ozone recovery yet. At southern mid-latitudes, a reduction of 20–50% is observed for a few days in October–November at the newly installed Rio Gallegos station. Similar depletion of ozone is also observed episodically during the vortex overpasses at Kerguelen in October–November and at Macquarie Island in July–August of the recent winters. This illustrates the significance of measurements at the edges of Antarctica.