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Ozone data derived from the TROPOMI sensor onboard the Sentinel-5 Precursor satellite are showing an atypical ozone hole feature in the polar region of the Northern hemisphere (Arctic) in spring 2020. A persistent ozone hole pattern with minimum total ozone column values around or below 220 Dobson units (DU) was seen for the first time over the Arctic for about 5 weeks in March and early April 2020. Usually an ozone hole with such low total ozone column values has only been observed in the polar Southern hemisphere (Antarctic) in spring over the last 4 decades, but not over the Arctic. The ozone hole pattern was caused by a particularly stable polar vortex in the stratosphere, enabling a persistent cold stratosphere at higher latitudes, a prerequisite for ozone depletion through heterogeneous chemistry. Based on the ERA5 reanalysis from ECMWF, the Northern winter 2019/2020 (from December to March) showed minimum polar cap temperatures consistently below 195 K around 20 km altitude, which enabled enhanced formation of polar stratospheric clouds. The special situation in spring 2020 is compared and discussed in context with two other ozone hole-like features in spring 1997 and 2011 that were showing comparable dynamical conditions in the stratosphere in combination with low total ozone column values. However, during these years total ozone columns below 220 DU over larger areas and over several consecutive days have not been observed. The similarities and differences of the atmospheric conditions of these three events and possible explanations are presented and discussed. It becomes apparent that the monthly mean of the minimum total ozone column value for March 2020 (i.e. 221 DU) was clearly below the respective values found in March 1997 (i.e. 267 DU) and 2011 (i.e. 252 DU), which emphasizes the noteworthiness of the evolution of the polar stratospheric ozone layer in Northern hemisphere spring 2020. These results provide a first description and classification of the development of the Arctic ozone hole in boreal spring 2020 and highlight its peculiarity.

In a previous study the quasi-instantaneous chemical impacts (rapid adjustments) of strongly enhanced methane (CH4) mixing ratios have been analyzed. However, to quantify the influence of the respective slow climate feedbacks on the chemical composition it is necessary to include the radiation driven temperature feedback. Therefore, we perform sensitivity simulations with doubled and fivefold present-day (year 2010) CH4 mixing ratios with the chemistry-climate model EMAC and include in a novel set-up a mixed layer ocean model to account for tropospheric warming. We find that the slow climate feedbacks counteract the reduction of the hydroxyl radical in the troposphere, which is caused by the strongly enhanced CH4 mixing ratios. Thereby also the resulting prolongation of the tropospheric CH4 lifetime is weakened compared to the quasi-instantaneous response considered previously. Changes in the stratospheric circulation evolve clearly with the warming of the troposphere. The Brewer-Dobson circulation strengthens, affecting the response of trace gases, such as ozone, water vapour and CH4 in the stratosphere, and also causing stratospheric temperature changes. In the middle and upper stratosphere, the increase of stratospheric water vapour is reduced with respect to the quasi-instantaneous response. Weaker increases of the hydroxyl radical cause the chemical depletion of CH4 to be less strongly enhanced and thus the in situ source of stratospheric water vapour as well. However, in the lower stratosphere water vapour increases more strongly when tropospheric warming is accounted for enlarging its overall radiative impact. The response of the stratospheric adjusted temperatures driven by slow climate feedbacks is dominated by these increases of stratospheric water vapour, as well as strongly decreased ozone mixing ratios above the tropical tropopause, which result from enhanced tropical upwelling. While rapid radiative adjustments from ozone and stratospheric water vapour make an essential contribution to the effective CH4 radiative forcing, the radiative impact of the respective slow feedbacks is rather moderate. In line with this, the climate sensitivity from CH4 changes in this chemistry-climate model setup is not significantly different from the climate sensitivity in carbon dioxide-driven simulations, provided that the CH4 effective radiative forcing includes the rapid adjustments from ozone and stratospheric water vapour changes.

One of the key questions in the air quality and climate sciences is how tropospheric ozone concentrations will change in the future. This will depend on two factors: changes in stratosphere-to-troposphere transport (STT) and changes in tropospheric chemistry. Here we aim to identify robust changes in STT using simulations from the Chemistry Climate Model Initiative (CCMI) under a common climate change scenario (RCP6.0). We use two idealized stratospheric tracers to isolate changes in transport: stratospheric ozone (O3S), which is exactly like ozone but has no chemical sources in the troposphere, and st80, a passive tracer with fixed volume mixing ratio in the stratosphere. We find a robust increase in the tropospheric columns of these two tracers across the models. In particular, stratospheric ozone in the troposphere is projected to increase 10 %–16 % by the end of the 21st century in the RCP6.0 scenario. Future STT is enhanced in the subtropics due to the strengthening of the shallow branch of the Brewer–Dobson circulation (BDC) in the lower stratosphere and of the upper part of the Hadley cell in the upper troposphere. The acceleration of the deep branch of the BDC in the Northern Hemisphere (NH) and changes in eddy transport contribute to increased STT at high latitudes. These STT trends are caused by greenhouse gas (GHG) increases, while phasing out of ozone-depleting substances (ODS) does not lead to robust transport changes. Nevertheless, the decline of ODS increases the reservoir of ozone in the lower stratosphere, which results in enhanced STT of O3S at middle and high latitudes. A higher emission scenario (RCP8.5) produces stronger STT trends, with increases in tropospheric column O3S more than 3 times larger than those in the RCP6.0 scenario by the end of the 21st century.

Methane (CH4) is the second most important greenhouse gas, which atmospheric concentration is influenced by human activities and currently on a sharp rise. We present a study with numerical simulations using a Chemistry-Climate-Model (CCM), which are performed to assess possible consequences of strongly enhanced CH4 concentrations in the Earth's atmosphere for the climate.Our analysis includes experiments with 2xCH4 and 5xCH4 present day (2010) lower boundary mixing ratios using the CCM EMAC. The simulations are conducted with prescribed oceanic conditions, mimicking present day tropospheric temperatures as its changes are largely suppressed. By doing so we are able to investigate the quasi-instantaneous chemical impact on the atmosphere. We find that the massive increase in CH4 strongly influences the tropospheric chemistry by reducing the OH abundance and thereby extending the tropospheric CH4 lifetime as well as the residence time of other chemical pollutants. The region above the tropopause is impacted by a substantial rise in stratospheric water vapor (SWV). The stratospheric ozone (O3) column increases overall, but SWV induced stratospheric cooling also leads to enhanced ozone depletion in the Antarctic lower stratosphere. Regional patterns of ozone change are affected by modification of stratospheric dynamics, i.e. increased tropical up-welling and stronger meridional transport towards the polar regions. We calculate the net radiative impact (RI) of the 2xCH4 experiment to be 0.69 W m-2 and for the 5xCH4 experiment to be 1.79 W m-2. A substantial part of the RI is contributed by chemically induced O3 and SWV changes, in line with previous radiative forcing estimates and is for the first time splitted and spatially asigned to its chemical contributors.This numerical study using a CCM with prescibed oceanic conditions shows the rapid responses to significantly enhanced CH4 mixing ratios, which is the first step towards investigating the impact of possible strong future CH4 emissions on atmospheric chemistry and its feedback on climate.

Methane (CH4) is the second most important anthropogenic greenhouse gas and its atmospheric abundance is rising rapidly at the moment (e.g. Nisbet et al., 2019). We assess the effects of doubled and fivefold present-day (2010) CH4 lower boundary mixing ratios on the basis of sensitivity simulations with thechemistry-climate model EMAC. As a follow-up on Winterstein et al. (2019) we investigate slow adjustments by applying a mixed layer ocean (MLO) modelinstead of prescribed oceanic conditions. In the simulations with prescribed oceanic conditions, tropospheric temperature changes are largely suppressed,while with MLO tropospheric temperatures adjust to the forcing. In the present study we compare the changes in the MLO sensitivity simulations to thesensitivity simulations with prescribed oceanic conditions (Winterstein et al., 2019). Comparing the responses of these two sets of sensitivity simulations separates rapid adjustments and the effects of slow climate feedbacks associated with tropospheric warming.The chemical interactions in the stratosphere in the MLO set-up (slow adjustments) compare in general well with the results of Winterstein et al. (2019) (rapid adjustments). The increase of stratospheric water vapor is albeit 5 % (15 %) points weaker in the MLO doubling (fivefolding) experiment compared to the doubling (fivefolding) experiment with prescribed oceanic conditions in line with a weaker increase of stratospheric OH. Stronger O3 decrease and CH4increase in the lowermost tropical stratosphere in the MLO sensitivity simulations compared to the sensitivity simulations with prescribed oceanic conditions indicate a more distinct strengthening of tropical up-welling due to tropospheric warming in the MLO set-up. The MLO simulations also show evidence of a strengthening of the Brewer-Dobson Circulation. When separating the quasi-instantaneous chemically induced O3 response from the O3 response pattern in the MLO set-up, the O3 response to slow climate feedbacks remains. This pattern is consistent with the O3 response to slow climate feedbacks induced by increases of CO2.This first of its kind study shows the climatic impact of strongly enhanced CH4 mixing ratios and how the slow climate response of tropospheric warming potentially damp instantaneous chemical feedbacks.

In this paper, we compare model calculations of ozone profiles and their variability for the period 1998 to 2016 with satellite and lidar profiles at five ground-based stations. Under the investigation is the temporal impact of the stratospheric halogen reduction (chemical processes) and increase in greenhouse gases (i.e., global warming) on stratospheric ozone changes. Attention is given to the effect of greenhouse gases on ultraviolet-B radiation at ground level. Our chemistry transport and chemistry climate models (Oslo CTM3 and EMAC CCM) indicate that (a) the effect of halogen reduction is maximized in ozone recovery at 1&ndash, 7 hPa and observed at all lidar stations, and (b) significant impact of greenhouse gases on stratospheric ozone recovery is predicted after the year 2050. Our study indicates that solar ultraviolet-B irradiance that produces DNA damage would increase after the year 2050 by +1.3% per decade. Such change in the model is driven by a significant decrease in cloud cover due to the evolution of greenhouse gases in the future and an insignificant trend in total ozone. If our estimates prove to be true, then it is likely that the process of climate change will overwhelm the effect of ozone recovery on UV-B irradiance in midlatitudes.

This investigation is motivated by the results presented by Montzka et al. (2018). They discussed a strong deviation of the assumed emissions of chlorofluorocarbon-11 (CFC-11, CFCl3) in the past 15 years, which indicates a violation of the Montreal Protocol for the protection of the ozone layer. A Chemistry-Climate Model (CCM) study is performed, investigating the consequences of a constant CFC-11 surface mixing ratio for stratospheric ozone: In comparison to a reference simulation (REF-C2), where a decrease of the CFC-11 surface mixing ratio of about 50 % is assumed from the early 2000s to the middle of the century, a sensitivity simulation (SEN-C2-fCFC11) is carried out where after the year 2002 the CFC-11 surface mixing ratio is kept constant until 2050. Differences between these two simulations are shown. These illustrate possible effects on stratospheric ozone. The total column ozone (TCO) in the 2040s (i.e. the years 2041–2050) is in particular affected in both polar regions in winter and spring. At the end of the 2040s maximum discrepancies of TCO are identified with reduced ozone values of up to around 30 Dobson Units (in the order of 10 %) in the SEN simulation. An analysis of the respective partial column ozone (PCO) for the stratosphere indicates that strongest ozone changes are calculated for the polar lower stratosphere, where they are mainly driven by the enhanced stratospheric chlorine content and associated heterogeneous chemical processes. Furthermore, it turns out that the calculated ozone changes, especially in the upper stratosphere, are smaller than expected. In this altitude region the additional ozone depletion due to the catalysis by reactive chlorine is compensated partly by other processes related to enhanced ozone production or reduced ozone loss, for instance from nitrous oxide (NOx).

Methane (CH4) is the second most important greenhouse gas, which atmospheric concentration is influenced by human activities. In this study, numerical simulations with a chemistry-climate model (CCM) are performed aiming to assess possible consequences of significantly enhanced CH4 concentrations in the Earth's atmosphere for the climate. We analyze experiments with 2xCH4 and 5xCH4 present day (2010) mixing ratio and its quasi-instantaneous chemical impact on the atmosphere. The massive increase in CH4 strongly influences the tropospheric chemistry by reducing the hydroxyl radical (OH) abundance and thereby extending the CH4 lifetime as well as the residence time of other chemical pollutants. The region above the tropopause is impacted by a substantial rise in stratospheric water vapor (SWV). The stratospheric ozone (O3) column increases overall, but SWV induced stratospheric cooling also leads to a enhanced ozone depletion in the Antarctic lower stratosphere. Regional patterns of ozone change are affected by modification of stratospheric dynamics, i.e. increased tropical up-welling and stronger meridional transport towards the polar regions. We calculate the net radiative impact (RI) of the 2xCH4 experiment to be 0.69 W/m2 and for the 5xCH4 experiment to be 1.79 W/m2. A substantial part of the RI is contributed by chemically induced O3 and SWV changes, in line with previous radiative forcing estimates. To our knowledge this is the first numerical study using a CCM with respect to two/fivefold CH4 concentrations and it is therefore an overdue analysis as it emphasizes the impact of possible strong future CH4 emissions on atmospheric chemistry and its feedback on climate.

Simulated stratospheric temperatures over the period 1979–2016 in models from the Chemistry-Climate Model Initiative are compared with recently updated and extended satellite data sets. The multimodel mean global temperature trends over 1979–2005 are -0.88 ± 0.23, -0.70 ± 0.16, and -0.50 ± 0.12 K/decade for the Stratospheric Sounding Unit (SSU) channels 3 (~40–50 km), 2 (~35–45 km), and 1 (~25–35 km), respectively (with 95% confidence intervals). These are within the uncertainty bounds of the observed temperature trends from two reprocessed SSU data sets. In the lower stratosphere, the multimodel mean trend in global temperature for the Microwave Sounding Unit channel 4 (~13–22 km) is -0.25 ± 0.12 K/decade over 1979–2005, consistent with observed estimates from three versions of this satellite record. The models and an extended satellite data set comprised of SSU with the Advanced Microwave Sounding Unit-A show weaker global stratospheric cooling over 1998–2016 compared to the period of intensive ozone depletion (1979–1997). This is due to the reduction in ozone-induced cooling from the slowdown of ozone trends and the onset of ozone recovery since the late 1990s. In summary, the results show much better consistency between simulated and satellite-observed stratospheric temperature trends than was reported by Thompson et al. (2012, https://doi.org/10.1038/nature11579) for the previous versions of the SSU record and chemistry-climate models. The improved agreement mainly comes from updates to the satellite records; the range of stratospheric temperature trends over 1979–2005 simulated in Chemistry-Climate Model Initiative models is comparable to the previous generation of chemistry-climate models.

Chemistry-climate models (CCMs) project an earlier return of northern mid-latitude total column ozone to 1980 values compared to the southern mid-latitudes. The chemical and dynamical drivers of this hemispheric difference are investigated in this study. The hemispheric asymmetry in return dates is a robust result across different CCMs and is qualitatively independent of the method used to estimate return dates. However, the differences in dates of return to 1980 levels between the southern and northern mid-latitudes can vary between 0 and 30 yr across the range of CCM projections analyzed. Positive linear trends in ozone lead to an earlier return of ozone than expected from the return of Cly to 1980 levels. This forward shift is stronger in the Northern than in the Southern Hemisphere because (i) trends have a larger effect on return dates if the sensitivity of ozone to Cly is lower and (ii) the trends in the Northern Hemisphere are stronger than in the Southern Hemisphere. An attribution analysis performed with two CCMs shows that chemically-induced changes in ozone are the major driver of the earlier return of ozone to 1980 levels in northern mid-latitudes; therefore transport changes are of minor importance. This conclusion is supported by the fact that the spread in the simulated hemispheric difference in return dates across an ensemble of twelve models is only weakly related to the spread in the simulated hemispheric asymmetry of trends in the strength of the Brewer–Dobson circulation. The causes for chemically-induced asymmetric ozone trends relevant for the total column ozone return date differences are found to be (i) stronger increases in ozone production due to enhanced NOx concentrations in the Northern Hemisphere lowermost stratosphere and troposphere, (ii) stronger decreases in the destruction rates of ozone by the NOx cycle in the Northern Hemisphere lower stratosphere linked to effects of dynamics and temperature on NOx concentrations, and (iii) an increasing efficiency of heterogeneous ozone destruction by Cly in the Southern Hemisphere mid-latitudes as a~result of decreasing lower stratospheric temperatures.

This paper reviews the current state and development of different numerical model classes that are used to simulate the global atmospheric system, particularly Earth’s climate and climate-chemistry connections. The focus is on Chemistry-Climate Models. In general, these serve to examine dynamical and chemical processes in the Earth atmosphere, their feedback, and interaction with climate. Such models have been established as helpful tools in addition to analyses of observational data. Definitions of the global model classes are given and their capabilities as well as weaknesses are discussed. Examples of scientific studies indicate how numerical exercises contribute to an improved understanding of atmospheric behavior. There, the focus is on synergistic investigations combining observations and model results. The possible future developments and challenges are presented, not only from the scientific point of view but also regarding the computer technology and respective consequences for numerical modeling of atmospheric processes. In the future, a stronger cross-linkage of subject-specific scientists is necessary, to tackle the looming challenges. It should link the specialist discipline and applied computer science.

Future projections of tropical total column ozone (TCO) are challenging, as its evolution is affected not only by the expected decline of ozone depleting substances but also by the uncertain increase of greenhouse gas (GHG) emissions. To assess the range of tropical TCO projections, we analyze simulations with a chemistry-climate model forced by three different GHG scenarios (Representative Concentration Pathway (RCP) 4.5, RCP6.0, and RCP8.5). We find that tropical TCO will be lower by the end of the 21st century compared to the 1960s in all scenarios with the largest decrease in the medium RCP6.0 scenario. Uncertainties of the projected TCO changes arise from the magnitude of stratospheric column decrease and tropospheric ozone increase which both strongly vary between the scenarios. In the three scenario simulations the stratospheric column decrease is not compensated by the increase in tropospheric ozone. The concomitant increase in harmful ultraviolet irradiance reaches up to 15% in specific regions in the RCP6.0 scenario.

Monthly averaged surface erythemal solar irradiance (UV-Ery) for local noon from 1960 to 2100 has been derived using radiative transfer calculations and projections of ozone, temperature and cloud change from 14 chemistry climate models (CCM), as part of the CCMVal-2 activity of SPARC. Our calculations show the influence of ozone depletion and recovery on erythemal irradiance. In addition, we investigate UV-Ery changes caused by climate change due to increasing greenhouse gas concentrations. The latter include effects of both stratospheric ozone and cloud changes. The derived estimates provide a global picture of the likely changes in erythemal irradiance during the 21st century. Uncertainties arise from the assumed scenarios, different parameterizations – particularly of cloud effects on UV-Ery – and the spread in the CCM projections. The calculations suggest that relative to 1980, annually mean UV-Ery in the 2090s will be on average ~12 % lower at high latitudes in both hemispheres, ~3 % lower at mid latitudes, and marginally higher (~1 %) in the tropics. The largest reduction (~16 %) is projected for Antarctica in October. Cloud effects are responsible for 2–3 % of the reduction in UV-Ery at high latitudes, but they slightly moderate it at mid-latitudes (~1 %). The year of return of erythemal irradiance to values of certain milestones (1965 and 1980) depends largely on the return of column ozone to the corresponding levels and is associated with large uncertainties mainly due to the spread of the model projections. The inclusion of cloud effects in the calculations has only a small effect of the return years. At mid and high latitudes, changes in clouds and stratospheric ozone transport by global circulation changes due to greenhouse gases will sustain the erythemal irradiance at levels below those in 1965, despite the removal of ozone depleting substances. At northern high latitudes (60°–90°), the projected decreases in cloud transmittance towards the end of the 21st century will reduce the yearly average surface erythemal irradiance by ~5 % with respect to the 1960s.

Chemistry-climate models (CCMs) are commonly used to simulate the past and future development of Earth's ozone layer. The fully coupled chemistry schemes calculate the chemical production and destruction of ozone interactively and ozone is transported by the simulated atmospheric flow. Due to the complexity of the processes acting on ozone it is not straightforward to disentangle the influence of individual processes on the temporal development of ozone concentrations. A method is introduced here that quantifies the influence of chemistry and transport on ozone concentration changes and that is easily implemented in CCMs and chemistry-transport models (CTMs). In this method, ozone tendencies (i.e. the time rate of change of ozone) are partitioned into a contribution from ozone production and destruction (chemistry) and a contribution from transport of ozone (dynamics). The influence of transport on ozone in a specific region is further divided into export of ozone out of that region and import of ozone from elsewhere into that region. For this purpose, a diagnostic is used that disaggregates the ozone mixing ratio field into 9 separate fields according to in which of 9 predefined regions of the atmosphere the ozone originated. With this diagnostic the ozone mass fluxes between these regions are obtained. Furthermore, this method is used here to attribute long-term changes in ozone to chemistry and transport. The relative change in ozone from one period to another that is due to changes in production or destruction rates, or due to changes in import or export of ozone, are quantified. As such, the diagnostics introduced here can be used to attribute changes in ozone on monthly, interannual and long-term time-scales to the responsible mechanisms. Results from a CCM simulation are shown here as examples, with the main focus of the paper being on introducing the method., Geoscientific Model Development, 4 (2), ISSN:1991-9603, ISSN:1991-959X

Although the Montreal Protocol now controls the production and emission of ozone depleting substances, the timing of ozone recovery is unclear. There are many other factors affecting the ozone layer, in particular climate change is expected to modify the speed of re-creation of the ozone layer. Therefore, long-term observations are needed to monitor the further evolution of the stratospheric ozone layer. Measurements from satellite instruments provide global coverage and are supplementary to selective ground-based observations. The combination of data derived from different space-borne instruments is needed to produce homogeneous and consistent long-term data records. They are required for robust investigations including trend analysis. For the first time global total ozone columns from three European satellite sensors GOME (ERS-2), SCIAMACHY (ENVISAT), and GOME-2 (METOP-A) are combined and added up to a continuous time series starting in June 1995. On the one hand it is important to monitor the consequences of the Montreal Protocol and its amendments; on the other hand multi-year observations provide the basis for the evaluation of numerical models describing atmospheric processes, which are also used for prognostic studies to assess the future development. This paper gives some examples of how to use satellite data products to evaluate model results with respective data derived from observations, and to disclose the abilities and deficiencies of atmospheric models. In particular, multi-year mean values derived from the Chemistry-Climate Model E39C-A are used to check climatological values and the respective standard deviations.

Simulations with the fully coupled climate-chemistry model E39/C suggest that the 1990 aircraft NO x emissions contributed substantially to the Northern Hemisphere NO x (30-40%) and ozone (3-4%) tropospheric burdens. Ozone production rates are increased by air traffic NO x emissions in the mid- and upper troposphere, whereas ozone loss rates are increased in the lower troposphere but decreased at cruise altitudes. The latter reduction results from increased tropospheric NO and NO 2 concentrations and a change in the OH:HO 2 ratio at cruise altitudes. Sensitivity studies showed that feedback processes between chemical species and dynamics are not altered significantly by air traffic. However, the results are sensitive to the lightning NO x emission patterns, the vertical resolution of the model at tropopause altitudes, model domain, and maximum flight level.

Aircraft emissions of NO x amount to a small proportion of total emissions of NO x from man-made and natural sources. However, NO x from subsonic aircraft are directly emitted in the upper troposphere and lower stratosphere and have a relatively strong effect on the production of ozone (O 3 ), a greenhouse gas, in that region. Furthermore air traffic is expected to increase significantly in the next decades. Possibilities for reducing the environmental impacts of air traffic by operational, technological and economic measures are currently under discussion. One potential option is to reduce flight altitudes. As a first step we investigate the effect of lowering cruise altitudes by 1 km on the chemical composition of the atmosphere for a subsonic fleet in 2015. Other parameters are deliberately kept constant, e.g., fuel consumption and NO x emissions. The simulations with the coupled climate-chemistry model E39/C clearly show that this fleet leads to a significantly smaller ozone increase compared to a fleet with a standard cruise altitude. In the northern hemisphere aircraft cause an ozone increase of 12.5 Tg for a 2015 simulation. The reduction in the ozone increase of 1.5 Tg is greater than the estimated additional ozone increase of 0.3 Tg due to decreased aerodynamic efficiency and therefore higher fuel consumption and NO x emissions. This value (1.2 Tg) is in the order of 10% relative to the simulated aircraft induced ozone increase of 12.5 Tg.

Tropospheric NO2 plays a variety of significant roles in atmospheric chemistry. In the troposphere it is one of the most significant precursors of photochemical ozone (O3) production and nitric acid (HNO3). In this study tropospheric NO2 columns were calculated by the fully coupled chemistry-climate model ECHAM4.L39(DLR)/CHEM. These have been compared with tropospheric NO2 columns, retrieved using the tropospheric excess method from measurements by the Global Ozone Monitoring Experiment (GOME) of up-welling earthshine radiance and the extraterrestrial irradiance. GOME is part of the core payload of the second European Research Satellite (ERS-2). For this study the first five years of GOME measurements have been used. The period of five years of observational data is sufficiently long to facilitate for the first time a comparison based on climatological averages with global coverage, focussing on the geographical distribution of the tropospheric NO2. A new approach of analysing regional differences (i.e. on continental scales) by calculating individual averages for different environments provides more detailed information about specific NOx sources and of their seasonal variations. The results obtained enable the validity of the model NO2 source distribution and the assumptions used to separate tropospheric and stratospheric parts of the NO2 column amount from the satellite measurements to be investigated.

This paper presents the operational retrieval of tropical tropospheric ozone columns (TOC) from the Second Global Ozone Monitoring Experiment (GOME-2) instruments using the convective-cloud-differential (CCD) method. The retrieval is based on total ozone and cloud property data provided by the GOME Data Processor (GDP) 4.7, and uses above-cloud and clear-sky ozone column measurements to derive a monthly mean TOC between 20° N and 20° S. Validation of the GOME-2 TOC with several tropical ozonesonde sites shows good agreement, with a high correlation between the GOME-2 and sonde measurements, and small biases within ~ 3 DU. The TOC data have been used in combination with tropospheric NO2 measurements from GOME-2 to analyse the effect of the 2009–2010 El Niño–Southern Oscillation (ENSO) on the tropospheric ozone distribution in the tropics. El-Niño induced dry conditions in September–October 2009 resulted in relatively high tropospheric ozone columns over the southern Indian Ocean and northern Australia, while La Niña conditions in September–October 2010 resulted in a strong increase in tropospheric NO2 in South America, and enhanced ozone in the eastern Pacific and South America. Comparisons of the GOME-2 tropospheric ozone data with simulations of the ECHAM/MESSy Atmospheric Chemistry (EMAC) model for 2009 El Nino conditions, illustrate the usefulness of the GOME-2 TOC measurements in evaluating chemistry climate models. Evaluation of CCMs with appropriate satellite observations helps to identify strengths and weaknesses of the model systems, providing a better understanding of driving mechanisms and adequate relations and feedbacks in the Earth atmosphere, and finally leading to improved models.

In this study, we provide a new perspective on the current state of the ozone layer using a comprehensive long-term total ozone data record which has been recently released within the framework of the European Space Agency's Climate Change Initiative. Based on a multivariate regression analysis, we disentangle various aspects of ozone change and variability on global and regional scales, thus enabling the monitoring of the effectiveness of the Montreal Protocol. Given dominant natural variability the expected midlatitude onset of ozone recovery is still not significant and would need additional 5 years of observations to be unequivocally detectable. A regional increase in the tropics is a likely manifestation of a long-term change in El Nino–Southern Oscillation intensity over the last two decades induced by strong El Nino in 1997/1998 and strong La Nina in 2010/2011.

The 1770s stand out as an epoch making period in the research of the atmospheric composition. During this decade, several of the most important constituents were identified and named. In 1774, J. Priestley and C.W. Scheele independently discovered oxygen. In the same year, Scheele identified chlorine and in 1777 nitrogen. Priestley discovered nitrous oxide (N2O) in 1773, hydrogen chloride (HCl) and ammonia (NH3) in 1774, sulphur dioxide (SO2) in 1775 and carbon monoxide (CO) in 1779.

Ozone (O3) is formed in the atmosphere when oxygen atoms (O) react with oxygen molecules (O2). In the upper atmosphere solar UV radiation of wavelengths shorter than 242 nm can photolyze O2 molecules and thereby produce O atoms. Since oxygen strongly absorbs solar UV, O2 photolysis is restricted to the upper atmosphere. Figure 3.1, displaying absorption features of oxygen and ozone as a function of wavelength, shows that UV of wavelengths shorter than 242 nm is completely absorbed in the middle atmosphere and definitely does not reach the troposphere. Thus the resulting ozone layer is confined to the middle atmosphere, i.e. the stratosphere and mesosphere.

The troposphere is the lowest atmospheric layer whose upper boundary, the tropopause, extends from about 18 km altitude in the tropics to 8 km in the polar region. Thus, it comprises about 90 % of the total mass of the Earth’s atmosphere. It contains the air we breathe and the water we drink. Biogenic source gases produced in soils and in the ocean are released into the troposphere, where they are carried along and mixed by winds and turbulences related to the weather systems. It is the troposphere, too, which we use as a waste dump for all kinds of waste gases of human civilisation, from industry, power plants, heating, transportation and other sources.

In 1974 the world was alarmed by Molina and Rowland’s famous paper (Ref. [21], of Chap. 3) predicting a severe depletion of the ozone layer caused by the continuous liberation of chlorofluorocarbons (CFCs) 11 and 12, CCl3F and CCl2F2, respectively. At that time about 700,000 t of these substances were released every year, as spray can propellant, refrigerants, solvents and foam blowing agents, with about 10 % annual emission increase. These CFCs were extremely useful: inert like noble gases, non-inflammable, non-toxic, without smell or taste. But just because of their inertness they are not decomposed in the troposphere, they accumulate and gradually get mixed to the higher layers of the atmosphere, where, by UV attack and reactions with excited oxygen atoms, Cl atoms are liberated which catalytically destroy ozone (see Sect. 3.1.3).

The development of the future atmospheric chemical composition is investigated with respect to NO y and O 3 by means of the off-line coupled dynamic-chemical general circulation model ECHAM3/CHEM. Two time slice experiments have been performed for the years 1992 and 2015, which include changes in sea surface temperatures, greenhouse gas concentrations, emissions of CFCs, NO x and other species, i.e., the 2015 simulation accounts for changes in chemically relevant emissions and for a climate change and its impact on air chemistry. The 2015 simulation clearly shows a global increase in ozone except for large areas of the lower stratosphere, where no significant changes or even decreases in the ozone concentration are found. For a better understanding of the importance of (A) emissions like NO x and CFCs, (B) future changes of air temperature and water vapour concentration, and (C) other dynamical parameters, like precipitation and changes in the circulation, diabatic circulation, stratosphere-troposphere-exchange, the simulation of the future atmosphere has been performed stepwise. This method requires a climate-chemistry model without interactive coupling of chemical species. Model results show that the direct effect of emissions (A) plays a major role for the composition of the future atmosphere, but they also clearly show that climate change (B and C) has a significant impact and strongly reduces the NO y and ozone concentration in the lower stratosphere. DOI: 10.1034/j.1600-0889.2001.d01-10.x

The future development of stratospheric ozone layer depends on the concentration of chlorine and bromine containing species. The stratosphere is also expected to be affected by future enhanced concentrations of greenhouse gases. These result in a cooling of the winter polar stratosphere and to more stable polar vortices which leads to enhanced chemical depletion and reduced transport of ozone into high latitudes. One of the driving forces behind the interest in stratospheric ozone is the impact of ozone on solar UV-B radiation. In this study UV scenarios have been constructed based on ozone predictions from the chemistry-climate model runs carried out by GISS, UKMO and DLR. Since cloudiness, albedo and terrain height are also important factors, climatological values of these quantities are taken into account in the UV calculations. Relative to 1979–92 conditions, for the 2010–2020 time period the GISS model results indicate a springtime enhancement of erythemal UV doses of up to 90% in the 60–90 °N region and an enhancement of 100% in the 60–90 °S region. The corresponding maximum increases in the annual Northern Hemispheric UV doses are estimated to be 14% in 2010–20, and 2% in 2040–50. In the Southern Hemisphere 40% enhancement is expected during 2010–20 and 27% during 2040–50.

The effect of future subsonic aircraft emissions on the chemical composition of the atmosphere is investigated by means of the coupled dynamic-chemical circulation model ECHAM3/CHEM. Present (1992) and future (2015 and 2050) atmospheric compositions are simulated with three sets of time slice experiments. Expected changes of the sea surface temperatures (SST), surface emissions of CFCs, greenhouse gases (GHG), and NOx (=NO+NO2) are prescribed. Model results show future increases in NOx and O3 due to aircraft NOx emissions, which scale almost linearily with the magnitude of the emission. The calculated climate change reduces the NOx concentration as well as its increase due to aircraft emissions by more than 10% at flight altitude in 2015. However, the aircraft induced ozone perturbation decreases only slightly when climate change is regarded.

The importance of dynamics for stratospheric ozone distribution in the northern hemisphere is investigated by using multiannual simulations of the coupled dynamic-chemical general circulation model ECHAM3/CHEM. This model includes a parameterization for heterogeneous reactions on the surfaces of polar stratospheric clouds (PSCs) and on sulfate aerosols. A warm and a cold stratospheric winter are examined to estimate the range of chemical ozone loss in the model due to heterogeneous reactions on PSCs. Ozone depletion in the model mainly occurs inside the polar vortex. An additional ozone reduction due to heterogeneous reactions on PSCs is found outside the polar vortex. Secondary vortex formation and vortex contraction after an elongation lead to a transport of air masses with chemically reduced ozone values out of the vortex. Except for such events the edge of the modeled polar vortex acts as a barrier to transport. During the formation of secondary vortices no additional heterogeneous reactions occur therein. Other dynamic events, such as the elongation of the polar vortex and its displacement to lower latitudes, lead to an intense ozone depletion. A minor stratospheric warming in the model causes a total deactivation of chlorine compounds and prevents further ozone depletion. In midlatitudes, the amplitude of short-term variations of total ozone is amplified by PSC heterogeneous chemical ozone reduction.

ECHAM3/CHEM is used to estimate the future development of the ozone layer. The general circulation model ECHAM3 and the chemistry module CHEM are coupled in a CTM-like mode, i.e. no feedback of simulated chemical species on radiation is considered. Currently CHEM does not include bromine chemistry. Two time-slice experiments representing 1991 and 2015 conditions are carried out. Chemical species are transported by winds calculated with different CO 2 mixing ratios as a proxy for other greenhouse-gases. For 2015, the adopted increase of CO 2 and the corresponding modification of the sea-surface temperature lead to a warming of the troposphere and a cooling of the stratosphere. The assessment for 2015 indicates that the ozone layer will not homogeneously recover, despite the employed decrease of chlorine in the model. Whereas in low and mid-latitudes an ascent of stratospheric O 3 is obvious, no significant increase of O 3 is found in the polar regions during spring time.

The global three-dimensional dynamic-chemical model ECHAM3/CHEM is employed to estimate the impact of present and future sub- and supersonic aircraft NOx emissions on ozone. Multinual simulations are performed to investigate changes of large-scale climatological features. An increase of tropospheric ozone of 3–4% is found in the Northern Hemisphere for a present day scenario, independently from season. No indications for significant ozone changes are indicated in the lower stratosphere. NOx emissions expected for the year 2015 by sub- and supersonic (500 civil aircraft, Mach 2.4, EINOx=15) air traffic yield much larger ozone changes in the model. An ozone increase of approximately 15% is predicted near the cruise altitude of future subsonic air traffic. This is accompanied by a clear ozone reduction of 3–4% in the lower stratosphere caused by supersonic aircraft. A stronger decrease of ozone is detected in polar winter due to the impact of heterogeneous reactions on polar stratospheric clouds.

[1] The upper troposphere/lower stratosphere (UTLS) region plays an important role in the climate system. Changes in the structure and chemical composition of this region result in particularly large changes in radiative forcings of the atmosphere. Quantifying the processes that control UTLS composition (e.g., stratosphere-troposphere exchange) therefore represents a crucial task. We assess the influence of uncertainties in the atmospheric mixing strength on global UTLS distributions of greenhouse gases (water vapor, ozone, methane, and nitrous oxide) and associated radiative effects. The study is based on multiannual simulations with the Chemical Lagrangian Model of the Stratosphere (CLaMS) driven by ERA-Interim meteorological data and on a state-of-the-art radiance code. Mixing, the irreversible part of transport, is controlled by the local horizontal strain and vertical shear of the atmospheric flow. We find that simulated radiative effects of water vapor and ozone, both characterized by steep gradients in the UTLS, are particularly sensitive to uncertainties of the atmospheric mixing strength. Globally averaged radiative effects are about 0.72 and 0.17 W/m2for water vapor and ozone, respectively. For ozone, the largest impact of mixing uncertainties is observed in the extra-tropical lower stratosphere.

Since the early 1980s significant depletion of the ozone layer in the stratosphere, in other words the ozone hole, has been observed every year over the South Pole area in Antarctic spring. In the meantime destruction of stratospheric ozone has been detected globally. Emissions of man-made halogenated chemicals play a dominant role in ozone loss. Combined analyses of observations and numerical modeling help to understand the complex interplay of the dynamic and chemical processes involved. Evaluated models provide a base for predicting the future recovery of the ozone layer expected for the middle of this century.

The climate system of the Earth atmosphere is affected by a complex interplay of dynamical, physical and chemical processes acting in the troposphere (atmospheric layer reaching from the Earth surface up to about 12 km height) and the Middle Atmosphere, i.e. the stratosphere (from about 12 to 50 km) and the mesosphere (from 50 to 100 km). Moreover, mutual influences between these atmospheric layers must be taken into account to get a complete picture of the Earth climate system. An outstanding example which can be used to describe some of the complex connections of atmospheric processes is the evolution of the ozone layer in the stratosphere and its interrelation with climate change. The stratospheric ozone layer (located around 15 to 35 km) protects life on Earth because it filters out a large part of the ultraviolet (UV) radiation (wavelength range between 100 nm and 380 nm) which is emitted by the sun. The almost complete absorption of the energyintensive solar UV-B radiation (280-320 nm) is especially important. UV-B radiation particularly affects plants, animals and people. Increased UV-B radiation can, for example, adversely impact photosynthesis, cause skin cancer and weaken the immune system. In addition, absorption of solar UV radiation by the stratospheric ozone layer causes the temperature of the stratosphere to increase with height, creating a stable layer that limits strong vertical air movement. This plays a key role for the Earth’s climate system. Approximately 90% of the total ozone amount is found in the stratosphere. Only 10% is in the troposphere; ozone concentrations in the troposphere are much lower than in the stratosphere. Data derived from observations (measurements from satellites and ground-based instruments) and respective results from numerical simulations with atmospheric models are used to describe and explain recent alterations of the dynamics and chemistry of the atmosphere. Since the beginning of the 1980ies in each year the ozone hole develops over Antarctica during spring season (i.e. September to November), showing a decrease in the total amount of ozone of up to 70% (see Figure 4). Especially in the lower stratosphere (about 15-25 km altitude), ozone is almost completely destroyed during this season. Relatively shortly after the discovery of the ozone hole, the extreme thinning of the ozone layer in the south-polar

The discovery of the ozone hole over Antarctica in 1985 was a surprise for science. For a few years the reasons of the ozone hole was speculated about. Soon it was obvious that predominant meteorological conditions led to a specific situation developing in this part of the atmosphere: Very low temperatures initiate chemical processes that at the end cause extreme ozone depletion at altitudes of between about 15 and 30 km. So-called polar stratospheric clouds play a key role. Such clouds develop at temperatures below about 195 K. Heterogeneous chemical reactions on cloud particles initiate the destruction of ozone molecules. The future evolution of the ozone layer will not only depend on the further development of concentrations of ozone-depleting substances, but also significantly on climate change.

The discovery of the ozone hole over Antarctica in 1985 was a surprise for science. For a few years the reasons of the ozone hole was speculated about. Soon it was obvious that predominant meteorological conditions led to a specific situation developing in this part of the atmosphere: Very low temperatures initiate chemical processes that at the end cause extreme ozone depletion at altitudes of between about 15 and 30 km. So-called polar stratospheric clouds play a key role. Such clouds develop at temperatures below about 195 K. Heterogeneous chemical reactions on cloud particles initiate the destruction of ozone molecules. The future evolution of the ozone layer will not only depend on the further development of concentrations of ozone-depleting substances, but also significantly on climate change.

International audience; Coupled chemistry-climate model simulations covering the recent past and continuing throughout the 21st century have been completed with a range of different models. Common forcings are used for the halogen amounts and greenhouse gas concentrations, as expected under the Montreal Protocol (with amendments) and Intergovernmental Panel on Climate Change A1b Scenario. The simulations of the Antarctic ozone hole are compared using commonly used diagnostics: the minimum ozone, the maximum area of ozone below 220 DU, and the ozone mass deficit below 220 DU. Despite the fact that the processes responsible for ozone depletion are reasonably well understood, a wide range of results is obtained. Comparisons with observations indicate that one of the reasons for the model underprediction in ozone hole area is the tendency for models to underpredict, by up to 35%, the area of low temperatures responsible for polar stratospheric cloud formation. Models also typically have species gradients that are too weak at the edge of the polar vortex, suggesting that there is too much mixing of air across the vortex edge. Other models show a high bias in total column ozone which restricts the size of the ozone hole (defined by a 220 DU threshold). The results of those models which agree best with observations are examined in more detail. For several models the ozone hole does not disappear this century but a small ozone hole of up to three million square kilometers continues to occur in most springs even after 2070.

International audience; Simulations of 15 coupled chemistry climate models, for the period 1960–2100, are presented. The models include a detailed stratosphere, as well as including a realistic representation of the tropospheric climate. The simulations assume a consistent set of changing greenhouse gas concentrations, as well as temporally varying chlorofluorocarbon concentrations in accordance with observations for the past and expectations for the future. The ozone results are analyzed using a nonparametric additive statistical model. Comparisons are made with observations for the recent past, and the recovery of ozone, indicated by a return to 1960 and 1980 values, is investigated as a function of latitude. Although chlorine amounts are simulated to return to 1980 values by about 2050, with only weak latitudinal variations, column ozone amounts recover at different rates due to the influence of greenhouse gas changes. In the tropics, simulated peak ozone amounts occur by about 2050 and thereafter total ozone column declines. Consequently, simulated ozone does not recover to values which existed prior to the early 1980s. The results also show a distinct hemispheric asymmetry, with recovery to 1980 values in the Northern Hemisphere extratropics ahead of the chlorine return by about 20 years. In the Southern Hemisphere midlatitudes, ozone is simulated to return to 1980 levels only 10 years ahead of chlorine. In the Antarctic, annually averaged ozone recovers at about the same rate as chlorine in high latitudes and hence does not return to 1960s values until the last decade of the simulations.

The Institute of Atmospheric Physics of the German Aerospace Center (DLR) uses the numerical model system ECHAM/MESSy Atmospheric Chemistry (EMAC). The model has a flexible modular structure and allows for coupled chemistry-climate simulations. Typical fields of application are related to questions regarding Earth’s climate, atmospheric chemical composition, and aerosol characteristics. In its current setup, the performance of EMAC on LRZ/ALTIX allows for multi-decadal simulations with climatologically significant results. The good performance demonstrates the multi-purpose capabilities of LRZ/ALTIX because EMAC involves various different numerical concepts and implementations of parallel decomposition. Our EMAC activities on LRZ/ALTIX are devoted to both model development and production simulations. The former comprise a new upper-boundary representation, a chemistry-transport mode, the inclusion of a mixed-layer ocean, and full-Lagrangian transport and dynamics. The latter tackle, for instance, questions related to the environmental impact of anthropogenic aerosol and gaseous substances.

The response of stratospheric climate and circulation to increasing amounts of greenhouse gases (GHGs) and ozone recovery in the twenty-first century is analyzed in simulations of 11 chemistry–climate models using near-identical forcings and experimental setup. In addition to an overall global cooling of the stratosphere in the simulations (0.59 ± 0.07 K decade−1 at 10 hPa), ozone recovery causes a warming of the Southern Hemisphere polar lower stratosphere in summer with enhanced cooling above. The rate of warming correlates with the rate of ozone recovery projected by the models and, on average, changes from 0.8 to 0.48 K decade−1 at 100 hPa as the rate of recovery declines from the first to the second half of the century. In the winter northern polar lower stratosphere the increased radiative cooling from the growing abundance of GHGs is, in most models, balanced by adiabatic warming from stronger polar downwelling. In the Antarctic lower stratosphere the models simulate an increase in low temperature extremes required for polar stratospheric cloud (PSC) formation, but the positive trend is decreasing over the twenty-first century in all models. In the Arctic, none of the models simulates a statistically significant increase in Arctic PSCs throughout the twenty-first century. The subtropical jets accelerate in response to climate change and the ozone recovery produces a westward acceleration of the lower-stratospheric wind over the Antarctic during summer, though this response is sensitive to the rate of recovery projected by the models. There is a strengthening of the Brewer–Dobson circulation throughout the depth of the stratosphere, which reduces the mean age of air nearly everywhere at a rate of about 0.05 yr decade−1 in those models with this diagnostic. On average, the annual mean tropical upwelling in the lower stratosphere (∼70 hPa) increases by almost 2% decade−1, with 59% of this trend forced by the parameterized orographic gravity wave drag in the models. This is a consequence of the eastward acceleration of the subtropical jets, which increases the upward flux of (parameterized) momentum reaching the lower stratosphere in these latitudes.

Today the topics “ozone layer” and “ozone hole” have been placed on the back burner in public discussions of climate change. Since the mid-1980s it has been known that primarily chlorofluorocarbons (CFCs) and also halocarbons (compounds where carbon atoms are linked to fluorine, chlorine, bromine, or iodine, but also to hydrogen) are mainly responsible for the destruction of the ozone layer in the stratosphere (atmospheric layer at an altitude of 12 to 50 km). Hence the production and usage of these substances were nearly fully prohibited in the Montreal Protocol (1987) and in subsequent agreements. As a consequence of these international treaties the strong increase of CFC concentrations in the troposphere (atmospheric layer up to an altitude of about 12 km) has halted (Figure 1). Since the mid-1990s the amount of CFCs in the troposphere has been decreasing. As a result, a reduction in the stratospheric chlorine concentration has been observed in recent years. Therefore it is expected that the ozone layer will increase in thickness and that the ozone hole over the Antarctic will disappear. Owing to the long lifetimes of CFCs in the atmosphere, it will take until about the middle of this century before the stratospheric chlorine level returns to the values measured in the 1960s. One could conclude that the ozone layer will fully recover by the middle of this century. However, the reconstruction of the ozone layer also depends on other atmospheric processes which complicate a reliable assessment of the future evolution. As a result of increased concentrations of well-mixed greenhouse gases in the atmosphere (e.g. CO2, CH4, and N2O), the troposphere warms (greenhouse effect) and the stratosphere cools (enhanced emission of long-wavelength thermal radiation). A multitude of chemical reactions in the atmosphere depend on the predominating temperature. For example, the ozone content in the middle and upper stratosphere increases with decreasing temperature since the most important ozone-destroying reactions (homogeneous gasphase reactions) slow down. In contrast, lower temperatures in the lower stratosphere over the polar regions cause stronger ozone depletion as a result of heterogeneous chemical reactions on very cold cloud particles. As a consequence of changes in the thermal structure of the atmosphere, dynamic processes in the atmosphere are changing and impacting the distribution of the trace gases that have longer lifetimes. So far, studies with numerical atmospheric models, so-called climate–chemistry models (CCMs), have not provided a consistent picture with regard to the speed of ozone recovery. Results derived from model simulations agree on the point that the regeneration of the ozone layer will develop with regional differences. Model calculations indicate that, overall, processes related to climate change will cause an accelerated recovery of the ozone layer. Most CCMs predict a return to the ozone levels observed in the 1960s clearly before the middle of this century (Figure 2). Figure 1. Hemispheric monthly mean values of tropospheric mixing ratios (in ppt=parts per trillion=10 ) of the most important CFCs (CFC-12=CF2Cl2, CFC-11=CFCl3, and CFC-113=Cl2FC-CClF2). Crosses indicate measured values for the northern hemisphere, triangles for the southern hemisphere. Recent results are shown in the insets. (Taken from Figure 1-1 in Ref. [1].) AGAGE=Advanced Global Atmospheric Gases Experiment, ESRL=Earth System Research Laboratory, UCI=University of California, Irvine.

Beside the analyses of data derived from field and laboratory measurements, results from numerical models are useful to better understand the thermal and dynamical structure as well as the chemical composition of the Earth’s atmosphere. In the recent past Climate-Chemistry Models have been developed to investigate mutual effects of radiative, dynamical and chemical processes, in particular to examine the connections of atmospheric chemistry and climate change in detail. These models also provide a basis for prognostic studies of the future evolution of atmospheric dynamics and chemical composition, for example to assess the timing of the recovery of the stratospheric ozone layer.

A new global three-dimensional (latitude, pressure, time) zonal mean monthly mean ozone database, from 1979 to 2100, has been created. The database extends from 87.5°S to 87.5°N at a 5° latitude resolution and from 878 hPa to 0.0460 hPa in 70 pressure levels ∼1 km apart. The full period is divided into two sub-periods, viz: (1) observations from 1979 to 2006 obtained from several sources of high vertical resolution ozone profile measurements, and (2) extensions from 2007 to 2100 based on chemistry climate model (CCM) projections. At each latitude and pressure level the CCM ozone time series are shifted and scaled to better match the measurements from 1997 to 2006 to ensure a smooth transition from observations to model output. This new database is expected to provide ozone boundary conditions suitable for long-term global climate model simulations.

For the first time a purely Lagrangian transport algorithm is applied in a fully coupled chemistry-climate model (CCM). We use the numerically non-diffusive Lagrangian scheme ATTILA instead of the operational semi-Lagrangian scheme for the transport of water vapour, cloud water and chemical trace species in the CCM E39C. The new model version including the Lagrangian scheme is referred to as E39C-A. The implications of the Lagrangian transport scheme for stratospheric model dynamics and tracer distributions in E39C-A are evaluated by comparison with observations and results of the previous model version E39C. We found in a previous paper that several deficiencies in stratospheric dynamics in E39C originate from a pronounced modelled wet bias and an associated cold bias in the extra-tropical lowermost stratosphere. Contrary to the semi-Lagrangian scheme ATTILA shows a largely reduced meridional transport of water vapour from the tropical upper troposphere into the extratropical lowermost stratosphere. The reduction of the moisture and temperature bias in E39C-A leads to a significant advancement of stratospheric dynamics in terms of the mean state as well as annual and interannual variability. In this study we show that as a consequence of both, the favourable numerical characteristics of the Lagrangian transport scheme and the improved model dynamics, E39C-A generally shows more realistic distributions of chemical trace species: Compared to E39C high stratospheric chlorine (Cly) concentrations extend further downward. Therefore E39C-A realistically covers the altitude of maximum ozone depletion in the stratosphere. The location of the ozonopause, i.e. the transition from low tropospheric to high stratospheric ozone values, is also clearly improved in E39C-A. Not only the spatial distribution but also the temporal evolution of stratospheric Cly in the past is realistically reproduced in E39C-A which is an important step towards a more reliable projection of future changes, especially of stratospheric ozone. Despite a large number of improvements there are still remaining model deficiencies like a general overestimation of total column ozone.

A statistical framework to evaluate the performance of chemistry-climate models with respect to the interaction between meteorology and column ozone during northern hemisphere mid-winter, in particularly January, is used. Different statistical diagnostics from four chemistry-climate models (E39C, ME4C, UMUCAM, ULAQ) are compared with the ERA-40 re-analysis. First, we analyse vertical coherence in geopotential height anomalies as described by linear correlations between two different pressure levels (30 and 200 hPa) of the atmosphere. In addition, linear correlations between column ozone and geopotential height anomalies at 200 hPa are discussed to motivate a simple picture of the meteorological impacts on column ozone on interannual timescales. Secondly, we discuss characteristic spatial structures in geopotential height and column ozone anomalies as given by their first two empirical orthogonal functions. Finally, we describe the covariance patterns between reconstructed anomalies of geopotential height and column ozone. In general we find good agreement between the models with higher horizontal resolution (E39C, ME4C, UMUCAM) and ERA-40. The Pacific-North American (PNA) pattern emerges as a useful qualitative benchmark for the model performance. Models with higher horizontal resolution and high upper boundary (ME4C and UMUCAM) show good agreement with the PNA tripole derived from ERA-40 data, including the column ozone modulation over the Pacfic sector. The model with lowest horizontal resolution does not show a classic PNA pattern (ULAQ), and the model with the lowest upper boundary (E39C) does not capture the PNA related column ozone variations over the Pacific sector. Those discrepancies have to be taken into account when providing confidence intervals for climate change integrations.

Rising tropical sea surface temperatures alter atmospheric dynamics at heights of 16 kilometers or more.

Simulations from eleven coupled chemistry-climate models (CCMs) employing nearly identical forcings have been used to project the evolution of stratospheric ozone throughout the 21st century. The model-to-model agreement in projected temperature trends is good, and all CCMs predict continued, global mean cooling of the stratosphere over the next 5 decades, increasing from around 0.25 K/decade at 50 hPa to around 1 K/ decade at 1 hPa under the Intergovernmental Panel on Climate Change (IPCC) Special Report on Emissions Scenarios (SRES) A1B scenario. In general, the simulated ozone evolution is mainly determined by decreases in halogen concentrations and continued cooling of the global stratosphere due to increases in greenhouse gases (GHGs). Column ozone is projected to increase as stratospheric halogen concentrations return to 1980s levels. Because of ozone increases in the middle and upper stratosphere due to GHGinduced cooling, total ozone averaged over midlatitudes, outside the polar regions, and globally, is projected to increase to 1980 values between 2035 and 2050 and before lower stratospheric halogen amounts decrease to 1980 values. In the polar regions the CCMs simulate small temperature trends in the first and second half of the 21st century in midwinter. Differences in stratospheric inorganic chlorine (Cly) among the CCMs are key to diagnosing the intermodel differences in simulated ozone recovery, in particular in the Antarctic. It is found that there are substantial quantitative differences in the simulated Cly, with the October mean Antarctic Cly peak value varying from less than 2 ppb to over 3.5 ppb in the CCMs, and the date at which the Cly returns to 1980 values varying from before 2030 to after 2050. There is a similar variation in the timing of recovery of Antarctic springtime column ozone back to 1980 values. As most models underestimate peak Cly near 2000, ozone recovery in the Antarctic could occur even later, between 2060 and 2070. In the Arctic the column ozone increase in spring does not follow halogen decreases as closely as in the Antarctic, reaching 1980 values before Arctic halogen amounts decrease to 1980 values and before the Antarctic. None of the CCMs predict future large decreases in the Arctic column ozone. By 2100, total column ozone is projected to be substantially above 1980 values in all regions except in the tropics.

We investigate the extent to which commonly considered quantities, based on total column ozone observations and simulations, are applicable as measures of ozone loss in the polar vortices. Such quantities have been used frequently in ozone assessments by the World Meteorological Organization (WMO) and to assess the performance of chemistry-climate models. The most commonly considered quantity is monthly mean column ozone poleward of a latitude of 63° in spring. For the Arctic, these monthly means were found to be insensitive to the exact choice of the latitude threshold, unlike the Antarctic where greater sensitivity was found. Choosing a threshold based on the location of the transport barrier at the vortex boundary instead of geometric latitude led to a roughly similar year-to-year variability of the monthly means, but in particular years deviations of several tens of Dobson units occurred. Moreover, the minimum of daily total ozone minima poleward of a particular latitude, another popular measure, is debatable, insofar as it relies on one single measurement or model grid point. For Arctic conditions, this minimum value occurred often in air outside polar vortex, both in the observations and in a chemistry-climate model. As a result, we recommend that the minimum of daily minima no longer be used when comparing polar ozone loss in observations and models. As a possible alternative, we suggest considering the minimum of daily average total ozone poleward of a particular equivalent latitude (or in the vortex) in spring. This definition both obviates relying on one single data point and reduces the impact of year-to-year variability in the Arctic vortex breakup on ozone loss measures. However, compact relations of such simple measures with meteorological quantities that describe the potential for polar heterogeneous chlorine activation and thus ozone loss were not found. Therefore, we argue that where possible, more sophisticated measures of chemical polar ozone loss that include additional information to disentangle the impact of transport and chemistry on ozone, should be employed.

One of the most significant events in the evolution of the ozone layer over southern mid-latitudes since the late 1970s was the large decrease observed in 1985. This event remains unexplained and a detailed investigation of the mechanisms responsible for the event has not previously been undertaken. In this study, the 1985 Southern Hemisphere mid-latitude total column ozone anomaly is analyzed in detail based on observed daily total column ozone fields, stratospheric dynamical fields, and calculated diagnostics of stratospheric mixing. The 1985 anomaly appears to result from a combination of (i) an anomaly in the meridional circulation resulting from the westerly phase of the equatorial quasi-biennial oscillation (QBO), (ii) weaker transport of ozone from its tropical mid-stratosphere source across the sub-tropical barrier to mid-latitudes related to the particular phasing of the QBO with respect to the annual cycle, and (iii) a solar cycle induced reduction in ozone. Similar QBO and solar cycle influences prevailed in 1997 and 2006 when again total column ozone was found to be suppressed over southern mid-latitudes. The results based on observations are compared and contrasted with analyses of ozone and dynamical fields from the ECHAM4.L39(DLR)/CHEM coupled chemistry-climate model (hereafter referred to as E39C). Equatorial winds in the E39C model are nudged towards observed winds between 10° S and 10° N and the ability of this model to produce an ozone anomaly in 1985, similar to that observed, confirms the role of the QBO in effecting the anomaly.