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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 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 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.

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 %.

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.

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.

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.

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.

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.

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.

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.

This paper presents extensive {bias determination} analyses of ozone observations from the Atmospheric Chemistry Experiment (ACE) satellite instruments: the ACE Fourier Transform Spectrometer (ACE-FTS) and the Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation (ACE-MAESTRO) instrument. Here we compare the latest ozone data products from ACE-FTS and ACE-MAESTRO with coincident observations from nearly 20 satellite-borne, airborne, balloon-borne and ground-based instruments, by analysing volume mixing ratio profiles and partial column densities. The ACE-FTS version 2.2 Ozone Update product reports more ozone than most correlative measurements from the upper troposphere to the lower mesosphere. At altitude levels from 16 to 44 km, the average values of the mean relative differences are nearly all within +1 to +8%. At higher altitudes (45–60 km), the ACE-FTS ozone amounts are significantly larger than those of the comparison instruments, with mean relative differences of up to +40% (about +20% on average). For the ACE-MAESTRO version 1.2 ozone data product, mean relative differences are within ±10% (average values within ±6%) between 18 and 40 km for both the sunrise and sunset measurements. At higher altitudes (~35–55 km), systematic biases of opposite sign are found between the ACE-MAESTRO sunrise and sunset observations. While ozone amounts derived from the ACE-MAESTRO sunrise occultation data are often smaller than the coincident observations (with mean relative differences down to −10%), the sunset occultation profiles for ACE-MAESTRO show results that are qualitatively similar to ACE-FTS, indicating a large positive bias (mean relative differences within +10 to +30%) in the 45–55 km altitude range. In contrast, there is no significant systematic difference in bias found for the ACE-FTS sunrise and sunset measurements.

The variability of total ozone and UV radiation from Total Ozone Mapping Spectrometer (TOMS) measurements is analyzed as a function of polar vortex occurrences over the southern subpolar regions during the 1997–2005 period. The analysis of vortex occurrences showed high interannual variability in the 40° S–60° S latitude band with a longitudinal asymmetry showing the largest frequencies over the 90° W–90° E region. The impact of vortex occurrences on UV radiation and ozone in clear sky conditions was determined from the comparison between the measurements inside the vortex and a climatology obtained from data outside the vortex over the studied period. Clear sky conditions were determined from TOMS reflectivity data. For measurements outside the vortex, clear sky conditions were selected for reflectivity values lower than 7.5%, while for measurements inside the vortex, a relaxed threshold was determined from statistically similar UV values as a function of reflectivity. UV changes and ozone differences from the climatology were analyzed in the 40° S–50° S and 50° S–60° S latitude bands during the spring period (September to November). The largest UV increases and ozone decreases, reaching ~200% and ~65%, respectively, were found in the 50° S–60° S latitude band in September and October. The heterogeneous ozone loss during vortex occurrences was estimated using a chemical transport model. The largest impact of vortex occurrences was found in October with mean UV increase, total ozone decrease and accumulated ozone loss in the 350–650 K range of, respectively, 47%, 30% and 57%. The region close to South America is the most affected by the Antarctic ozone depletion due to the combined effect of large number of vortex occurrences, lower cloud cover and large ozone decrease. This region would be the most vulnerable in case of cloud cover decrease, due to more frequent occurrence of ozone poor air masses during austral spring.

The EU CANDIDOZ project investigated the chemical and dynamical influences on decadal ozone trends focusing on the Northern Hemisphere. High quality long-term ozone data sets, satellite-based as well as ground-based, and the long-term meteorological reanalyses from ECMWF and NCEP are used together with advanced multiple regression models and atmospheric models to assess the relative roles of chemistry and transport in stratospheric ozone changes. This overall synthesis of the individual analyses in CANDIDOZ shows clearly one common feature in the NH mid latitudes and in the Arctic: an almost monotonic negative trend from the late 1970s to the mid 1990s followed by an increase. In most trend studies, the Equivalent Effective Stratospheric Chlorine (EESC) which peaked in 1997 as a consequence of the Montreal Protocol was observed to describe ozone loss better than a simple linear trend. Furthermore, all individual analyses point to changes in dynamical drivers, such as the residual circulation (responsible for the meridional transport of ozone into middle and high latitudes) playing a key role in the observed turnaround. The changes in ozone transport are associated with variations in polar chemical ozone loss via heterogeneous ozone chemistry on PSCs (polar stratospheric clouds). Synoptic scale processes as represented by the new equivalent latitude proxy, by conventional tropopause altitude or by 250 hPa geopotential height have also been successfully linked to the recent ozone increases in the lowermost stratosphere. These show significant regional variation with a large impact over Europe and seem to be linked to changes in tropospheric climate patterns such as the North Atlantic Oscillation. Some influence in recent ozone increases was also attributed to the rise in solar cycle number 23. Changes from the late 1970s to the mid 1990s were found in a number of characteristics of the Arctic vortex. However, only one trend was found when more recent years are also considered, namely the tendency for cold winters to become colder.

The study presents the climatological characteristics of stratospheric ozone observed over Reunion Island using in-situ (ozonesonde and SAOZ) and satellite (UARS-HALOE, SAGE-II and TOMS) measurements. It uses co-localised ozonesondes (from September 1992 to February 2005) and SAOZ measurements (from January 1993 to December 2004), SAGE-II data from October 1984 to February 1999 (~15 years), HALOE data from January 1991 to February 2005 (~15 years), and NIMBUS/TOMS data from January 1978 to December 2004 (27 years). The satellite measurements correspond to overpasses located nearby Reunion Island (21° S; 55° E). The height profiles of ozone concentration obtained from ozonesonde (0.5–29.5 km) show less bias in comparison with the HALOE and SAGE-II measurements. Though, the satellite (HALOE and SAGE-II) measurements underestimate the tropospheric ozone, they are in good agreement for the heights above 15 km. The bias between the measurements and the normalized ozone profile constructed from the ozonesonde and SAGE-II satellite measurement shows that the SAGE-II measurements are more accurate than the HALOE measurements in the lower stratosphere. The monthly variation of ozone concentration derived from ozonesonde and HALOE shows a nearly annual cycle with a maximum concentration during winter/spring and minimum concentration during summer/autumn months. The time evolution of total column ozone obtained from TOMS, SAOZ and the one computed from ozonesonde and SAGE-II, exhibits similar behaviour with analogous trends as above. The TOMS variation displays a higher value of total column ozone of about 3–5 DU (10%) in comparison with the SAOZ and the integrated ozone from ozonesonde and SAGE-II.

This paper is devoted to an intercomparison of ozone vertical profiles retrieved from the measurements of scattered solar radiation performed by the SCIAMACHY instrument in the limb viewing geometry. Three different inversion algorithms including the prototype of the operational Level 1 to 2 processor to be operated by the European Space Agency are considered. Unlike usual validation studies, this comparison removes the uncertainties arising when comparing measurements made by different instruments probing slightly different air masses and focuses on the uncertainties specific to the modeling-retrieval problem only. The intercomparison was performed for 5 selected orbits of SCIAMACHY showing a good overall agreement of the results in the middle stratosphere, whereas considerable discrepancies were identified in the lower stratosphere and upper troposphere altitude region. Additionally, comparisons with ground-based lidar measurements are shown for selected profiles demonstrating an overall correctness of the retrievals.

The Michelson Interferometer for Passive Atmospheric Sounding (MIPAS), on-board the European ENVIronmental SATellite (ENVISAT) launched on 1 March 2002, is a middle infrared Fourier Transform spectrometer measuring the atmospheric emission spectrum in limb sounding geometry. The instrument is capable to retrieve the vertical distribution of temperature and trace gases, aiming at the study of climate and atmospheric chemistry and dynamics, and at applications to data assimilation and weather forecasting. MIPAS operated in its standard observation mode for approximately two years, from July 2002 to March 2004, with scans performed at nominal spectral resolution of 0.025 cm−1 and covering the altitude range from the mesosphere to the upper troposphere with relatively high vertical resolution (about 3 km in the stratosphere). Only reduced spectral resolution measurements have been performed subsequently. MIPAS data were re-processed by ESA using updated versions of the Instrument Processing Facility (IPF v4.61 and v4.62) and provided a complete set of level-2 operational products (geo-located vertical profiles of temperature and volume mixing ratio of H2O, O3, HNO3, CH4, N2O and NO2) with quasi continuous and global coverage in the period of MIPAS full spectral resolution mission. In this paper, we report a detailed description of the validation of MIPAS-ENVISAT operational ozone data, that was based on the comparison between MIPAS v4.61 (and, to a lesser extent, v4.62) O3 VMR profiles and a comprehensive set of correlative data, including observations from ozone sondes, ground-based lidar, FTIR and microwave radiometers, remote-sensing and in situ instruments on-board stratospheric aircraft and balloons, concurrent satellite sensors and ozone fields assimilated by the European Center for Medium-range Weather Forecasting. A coordinated effort was carried out, using common criteria for the selection of individual validation data sets, and similar methods for the comparisons. This enabled merging the individual results from a variety of independent reference measurements of proven quality (i.e. well characterized error budget) into an overall evaluation of MIPAS O3 data quality, having both statistical strength and the widest spatial and temporal coverage. Collocated measurements from ozone sondes and ground-based lidar and microwave radiometers of the Network for the Detection Atmospheric Composition Change (NDACC) were selected to carry out comparisons with time series of MIPAS O3 partial columns and to identify groups of stations and time periods with a uniform pattern of ozone differences, that were subsequently used for a vertically resolved statistical analysis. The results of the comparison are classified according to synoptic and regional systems and to altitude intervals, showing a generally good agreement within the comparison error bars in the upper and middle stratosphere. Significant differences emerge in the lower stratosphere and are only partly explained by the larger contributions of horizontal and vertical smoothing differences and of collocation errors to the total uncertainty. Further results obtained from a purely statistical analysis of the same data set from NDACC ground-based lidar stations, as well as from additional ozone soundings at middle latitudes and from NDACC ground-based FTIR measurements, confirm the validity of MIPAS O3 profiles down to the lower stratosphere, with evidence of larger discrepancies at the lowest altitudes. The validation against O3 VMR profiles using collocated observations performed by other satellite sensors (SAGE II, POAM III, ODIN-SMR, ACE-FTS, HALOE, GOME) and ECMWF assimilated ozone fields leads to consistent results, that are to a great extent compatible with those obtained from the comparison with ground-based measurements. Excellent agreement in the full vertical range of the comparison is shown with respect to collocated ozone data from stratospheric aircraft and balloon instruments, that was mostly obtained in very good spatial and temporal coincidence with MIPAS scans. This might suggest that the larger differences observed in the upper troposphere and lowermost stratosphere with respect to collocated ground-based and satellite O3 data are only partly due to a degradation of MIPAS data quality. They should be rather largely ascribed to the natural variability of these altitude regions and to other components of the comparison errors. By combining the results of this large number of validation data sets we derived a general assessment of MIPAS v4.61 and v4.62 ozone data quality. A clear indication of the validity of MIPAS O3 vertical profiles is obtained for most of the stratosphere, where the mean relative difference with the individual correlative data sets is always lower than ±10%. Furthermore, these differences always fall within the combined systematic error (from 1 hPa to 50 hPa) and the standard deviation is fully consistent with the random error of the comparison (from 1 hPa to ~30–40 hPa). A degradation in the quality of the agreement is generally observed in the lower stratosphere and upper troposphere, with biases up to 25% at 100 hPa and standard deviation of the global mean differences up to three times larger than the combined random error in the range 50–100 hPa. The larger differences observed at the bottom end of MIPAS retrieved profiles can be associated, as already noticed, to the effects of stronger atmospheric gradients in the UTLS that are perceived differently by the various measurement techniques. However, further components that may degrade the results of the comparison at lower altitudes can be identified as potentially including cloud contamination, which is likely not to have been fully filtered using the current settings of the MIPAS cloud detection algorithm, and in the linear approximation of the forward model that was used for the a priori estimate of systematic error components. The latter, when affecting systematic contributions with a random variability over the spatial and temporal scales of global averages, might result in an underestimation of the random error of the comparison and add up to other error sources, such as the possible underestimates of the p and T error propagation based on the assumption of a 1 K and 2% uncertainties, respectively, on MIPAS temperature and pressure retrievals. At pressure lower than 1 hPa, only a small fraction of the selected validation data set provides correlative ozone data of adequate quality and it is difficult to derive quantitative conclusions about the performance of MIPAS O3 retrieval for the topmost layers.

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

A description of the long-term data series of stratospheric ozone at the Observatoire de Haute-Provence is presented. At this station, data sets with temporal length of a decade or more are provided in the framework of the Network for Detection of Stratospheric Change by ground-based experiments: Dobson spectrophotometer (in both column and Umkehr mode), lidar and ozonesondes. The data time series obtained from these various instruments operated simultaneously at a single site and complemented by SAGE II space-borne measurements are first described with respect to instrumental uncertainties, sampling rate and time evolution. These data series are then compared to each other in terms of sampling rate and average vertical profiles. The difference between the mean ozone profiles of the data sets can partly be explained by the different sampling rate of the instruments. Using the overlap and the complementarity of the various data sets, a preliminary estimate of the long-term evolution of ozone over the last decade over Southern France is conducted. Trend values for both total column and vertical profiles are derived using the multi-regression statistical model AMOUNTS O3. In the 25–40 km altitude range, a similar ozone decrease from –4% to –10% is observed from lidar, Umkehr and SAGE II data series in good agreement with previous estimates. In the lower stratosphere (15–25 km), large negative trends in the ozone vertical profile are observed. In addition, the negative trend of –5.4% in total ozone inferred from the Dobson measurements over the period 1983–1995 is in good agreement with the integrated trend profile.Key words: Atmospheric composition and structure (evolution of the atmosphere; middle atmosphere – composition and chemistry; instruments and techniques)