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.

We have studied data from two satellite occultation instruments in order to generate a high vertical resolution homogeneous ozone time series of 26 yr. The Stratospheric Aerosol and Gas Experiment (SAGE) II solar occultation instrument and the Global Ozone Monitoring by Occultation of Stars (GOMOS) instrument measured ozone profiles in the stratosphere and mesosphere from 1984–2005 and 2002–2012, respectively. Global coverage, good vertical resolution, and the self-calibrating measurement method make data from these instruments valuable for the detection of changes in vertical distribution of ozone over time. As both instruments share a common measurement period from 2002–2005, it is possible to inter-calibrate the data sets. We investigate how well these measurements agree with each other and combine all the data to produce a new stratospheric ozone profile data set. Above 55 km, SAGE II measurements show much less ozone than the GOMOS nighttime measurements as a consequence of the well-known diurnal variation of ozone in the mesosphere. Between 35–55 km, SAGE II sunrise and sunset measurements differ from GOMOS' measurements to different extents. Sunrise measurements show 2% less ozone than GOMOS, whereas sunset measurements show 4% more ozone than GOMOS. Differences can be explained qualitatively by the diurnal variation of ozone in the stratosphere recently observed by SMILES and modeled by chemical transport models. Between 25–35 km, SAGE II sunrise and sunset measurements and GOMOS measurements agree within 1%. The observed ozone bias between collocated measurements of SAGE II sunrise/sunset and GOMOS night measurements is used to align the two data sets. The combined data set covers the time period 1984–2011, latitudes 60° S–60° N, and the altitude range of 20–60 km. Profile data are given on a 1 km vertical grid, and with a resolution of 1 month in time and 10° in latitude. The combined ozone data set is analyzed by fitting a time series model to the data. We assume a linear trend with an inflection point (so-called "hockey stick" form). The best estimate for the point of inflection was found to be the year 1997 for ozone between altitudes 35 and 45 km. At all latitudes and altitudes from 35 to 50 km we find a clear change in ozone trend before and after the inflection time. From 38 to 45 km, a negative trend of 4% per decade (statistically significant at 95% level) at the equator has changed to a small positive trend of 0–2% per decade. At mid-latitudes, the negative trend of 4–8% per decade has changed to to a small positive trend of 0–2% per decade. At mid-latitudes near 20 km, the ozone loss has still increased whereas in the tropics a recovery is ongoing.

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

We present a global distribution of surface methane (CH₄) emission estimates for 2000–2012 derived using the CarbonTracker Europe-CH₄ (CTE-CH₄) data assimilation system. In CTE-CH₄, anthropogenic and biospheric CH₄ emissions are simultaneously estimated based on constraints of global atmospheric in situ CH₄ observations. The system was configured to either estimate only anthropogenic or biospheric sources per region, or to estimate both categories simultaneously. The latter increased the number of optimizable parameters from 62 to 78. In addition, the differences between two numerical schemes available to perform turbulent vertical mixing in the atmospheric transport model TM5 were examined. Together, the system configurations encompass important axes of uncertainty in inversions and allow us to examine the robustness of the flux estimates. The posterior emission estimates are further evaluated by comparing simulated atmospheric CH₄ to surface in situ observations, vertical profiles of CH₄ made by aircraft, remotely sensed dry-air total column-averaged mole fraction (XCH₄) from the Total Carbon Column Observing Network (TCCON), and XCH₄ from the Greenhouse gases Observing Satellite (GOSAT). The evaluation with non-assimilated observations shows that posterior XCH₄ is better matched with the retrievals when the vertical mixing scheme with faster interhemispheric exchange is used. Estimated posterior mean total global emissions during 2000–2012 are 516 ± 51 Tg CH₄ yr⁻¹, with an increase of 18 Tg CH₄ yr⁻¹ from 2000–2006 to 2007–2012. The increase is mainly driven by an increase in emissions from South American temperate, Asian temperate and Asian tropical TransCom regions. In addition, the increase is hardly sensitive to different model configurations ( < 2 Tg CH₄ yr⁻¹ difference), and much smaller than suggested by EDGAR v4.2 FT2010 inventory (33 Tg CH₄ yr⁻¹), which was used for prior anthropogenic emission estimates. The result is in good agreement with other published estimates from inverse modelling studies (16–20 Tg CH₄ yr⁻¹). However, this study could not conclusively separate a small trend in biospheric emissions (−5 to +6.9 Tg CH₄ yr⁻¹) from the much larger trend in anthropogenic emissions (15–27 Tg CH₄ yr⁻¹). Finally, we find that the global and North American CH₄ balance could be closed over this time period without the previously suggested need to strongly increase anthropogenic CH₄ emissions in the United States. With further developments, especially on the treatment of the atmospheric CH₄ sink, we expect the data assimilation system presented here will be able to contribute to the ongoing interpretation of changes in this important greenhouse gas budget.