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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., Atmospheric Chemistry and Physics, 11 (15), ISSN:1680-7375, ISSN:1680-7367

While chemistry-climate models are able to reproduce many characteristics of the global total column ozone field and its long-term evolution, they have fared less well in simulating the commonly used diagnostic of the area of the Antarctic ozone hole i.e. the area within the 220 Dobson Unit (DU) contour. Two possible reasons for this are: (1) the underlying Global Climate Model (GCM) does not correctly simulate the size of the polar vortex, and (2) the stratospheric chemistry scheme incorporated into the GCM, and/or the model dynamics, results in systematic biases in the total column ozone fields such that the 220 DU contour is no longer appropriate for delineating the edge of the ozone hole. Both causes are examined here with a view to developing ozone hole area diagnostics that better suit measurement-model inter-comparisons. The interplay between the shape of the meridional mixing barrier at the edge of the vortex and the meridional gradients in total column ozone across the vortex edge is investigated in measurements and in 5 chemistry-climate models (CCMs). Analysis of the simulation of the polar vortex in the CCMs shows that the first of the two possible causes does play a role in some models. This in turn affects the ability of the models to simulate the large observed meridional gradients in total column ozone. The second of the two causes also strongly affects the ability of the CCMs to track the observed size of the ozone hole. It is shown that by applying a common algorithm to the CCMs for selecting a delineating threshold unique to each model, a more appropriate diagnostic of ozone hole area can be generated that shows better agreement with that derived from observations., Atmospheric Chemistry and Physics, 9 (17), ISSN:1680-7375, ISSN:1680-7367

The Southern Hemisphere (SH) zonal-mean circulation change in response to Antarctic ozone depletion is re-visited by examining a set of the latest model simulations archived for the Chemistry-Climate Model Initiative (CCMI) project. All models reasonably well reproduce Antarctic ozone depletion in the late 20th century. The related SH-summer circulation changes, such as a poleward intensification of westerly jet and a poleward expansion of the Hadley cell, are also well captured. All experiments exhibit quantitatively the same multi-model mean trend, irrespective of whether the ocean is coupled or prescribed. Results are also quantitatively similar to those derived from the Coupled Model Intercomparison Project phase 5 (CMIP5) high-top model simulations in which the stratospheric ozone is mostly prescribed with monthly- and zonally-averaged values. These results suggest that the ozone-hole-induced SH-summer circulation changes are robust across the models irrespective of the specific chemistry-atmosphere-ocean coupling., Environmental Research Letters, 13 (5), ISSN:1748-9326, ISSN:1748-9318

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.

In recent years a number of chemistry-climate models have been developed with an emphasis on the stratosphere. Such models cover a wide range of time scales of integration and vary considerably in complexity. The results of specific diagnostics are here analysed to examine the differences amongst individual models and observations, to assess the consistency of model predictions, with a particular focus on polar ozone. For example, many models indicate a significant cold bias in high latitudes, the "cold pole problem", particularly in the southern hemisphere during winter and spring. This is related to wave propagation from the troposphere which can be improved by improving model horizontal resolution and with the use of non-orographic gravity wave drag. As a result of the widely differing modelled polar temperatures, different amounts of polar stratospheric clouds are simulated which in turn result in varying ozone values in the models. The results are also compared to determine the possible future behaviour of ozone, with an emphasis on the polar regions and mid-latitudes. All models predict eventual ozone recovery, but give a range of results concerning its timing and extent. Differences in the simulation of gravity waves and planetary waves as well as model resolution are likely major sources of uncertainty for this issue. In the Antarctic, the ozone hole has probably reached almost its deepest although the vertical and horizontal extent of depletion may increase slightly further over the next few years. According to the model results, Antarctic ozone recovery could begin any year within the range 2001 to 2008. The limited number of models which have been integrated sufficiently far indicate that full recovery of ozone to 1980 levels may not occur in the Antarctic until about the year 2050. For the Arctic, most models indicate that small ozone losses may continue for a few more years and that recovery could begin any year within the range 2004 to 2019. The start of ozone recovery in the Arctic is therefore expected to appear later than in the Antarctic. Further, interannual variability will tend to mask the signal for longer than in the Antarctic, delaying still further the date at which ozone recovery may be said to have started. Because of this inherent variability of the system, the decadal evolution of Arctic ozone will not necessarily be a direct response to external forcing., Atmospheric Chemistry and Physics, 3, ISSN:1680-7375, ISSN:1680-7367

Major mid-winter stratospheric sudden warmings (SSWs) are the largest instance of wintertime variability in the Arctic stratosphere. Because SSWs are able to cause significant surface weather anomalies on intra-seasonal timescales, several previous studies have focused on their potential future change, as might be induced by anthropogenic forcings. However, a wide range of results have been reported, from a future increase in the frequency of SSWs to an actual decrease. Several factors might explain these contradictory results, notably the use of different metrics for the identification of SSWs and the impact of large climatological biases in single-model studies. To bring some clarity, we here revisit the question of future SSW changes, using an identical set of metrics applied consistently across 12 different models participating in the Chemistry–Climate Model Initiative. Our analysis reveals that no statistically significant change in the frequency of SSWs will occur over the 21st century, irrespective of the metric used for the identification of the event. Changes in other SSW characteristics – such as their duration, deceleration of the polar night jet, and the tropospheric forcing – are also assessed: again, we find no evidence of future changes over the 21st century.

Projections of stratospheric ozone from a suite of chemistry-climate models (CCMs) have been analyzed. In addition to a reference simulation where anthropogenic halogenated ozone depleting substances (ODSs) and greenhouse gases (GHGs) vary with time, sensitivity simulations with either ODS or GHG concentrations fixed at 1960 levels were performed to disaggregate the drivers of projected ozone changes. These simulations were also used to assess the two distinct milestones of ozone returning to historical values (ozone return dates) and ozone no longer being influenced by ODSs (full ozone recovery). The date of ozone returning to historical values does not indicate complete recovery from ODSs in most cases, because GHG-induced changes accelerate or decelerate ozone changes in many regions. In the upper stratosphere where CO2-induced stratospheric cooling increases ozone, full ozone recovery is projected to not likely have occurred by 2100 even though ozone returns to its 1980 or even 1960 levels well before (~2025 and 2040, respectively). In contrast, in the tropical lower stratosphere ozone decreases continuously from 1960 to 2100 due to projected increases in tropical upwelling, while by around 2040 it is already very likely that full recovery from the effects of ODSs has occurred, although ODS concentrations are still elevated by this date. In the midlatitude lower stratosphere the evolution differs from that in the tropics, and rather than a steady decrease in ozone, first a decrease in ozone is simulated from 1960 to 2000, which is then followed by a steady increase through the 21st century. Ozone in the midlatitude lower stratosphere returns to 1980 levels by ~2045 in the Northern Hemisphere (NH) and by ~2055 in the Southern Hemisphere (SH), and full ozone recovery is likely reached by 2100 in both hemispheres. Overall, in all regions except the tropical lower stratosphere, full ozone recovery from ODSs occurs significantly later than the return of total column ozone to its 1980 level. The latest return of total column ozone is projected to occur over Antarctica (~2045–2060) whereas it is not likely that full ozone recovery is reached by the end of the 21st century in this region. Arctic total column ozone is projected to return to 1980 levels well before polar stratospheric halogen loading does so (~2025–2030 for total column ozone, cf. 2050–2070 for Cly+60×Bry) and it is likely that full recovery of total column ozone from the effects of ODSs has occurred by ~2035. In contrast to the Antarctic, by 2100 Arctic total column ozone is projected to be above 1960 levels, but not in the fixed GHG simulation, indicating that climate change plays a significant role., Atmospheric Chemistry and Physics, 10 (19), ISSN:1680-7375, ISSN:1680-7367

The connection between the El Niño Southern Oscillation (ENSO) and the Northern polar stratosphere has been established from observations and atmospheric modeling. Here a systematic inter-comparison of the sensitivity of the modeled stratosphere to ENSO in Chemistry Climate Models (CCMs) is reported. This work uses results from a number of the CCMs included in the 2006 ozone assessment. In the lower stratosphere, the mean of all model simulations reports a warming of the polar vortex during strong ENSO events in February–March, consistent with but smaller than the estimate from satellite observations and ERA40 reanalysis. The anomalous warming is associated with an anomalous dynamical increase of column ozone north of 70° N that is accompanied by coherent column ozone decrease in the Tropics, in agreement with that deduced from the NIWA column ozone database, implying an increased residual circulation in the mean of all model simulations during ENSO. The spread in the model responses is partly due to the large internal stratospheric variability and it is shown that it crucially depends on the representation of the tropospheric ENSO teleconnection in the models., Atmospheric Chemistry and Physics, 9 (22), ISSN:1680-7375, ISSN:1680-7367

We analyse simulations performed for the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion caused by anthropogenic stratospheric chlorine and bromine. We consider a total of 155 simulations from 20 models, including a range of sensitivity studies which examine the impact of climate change on ozone recovery. For the control simulations (unconstrained by nudging towards analysed meteorology) there is a large spread (±20DU in the global average) in the predictions of the absolute ozone column. Therefore, the model results need to be adjusted for biases against historical data. Also, the interannual variability in the model results need to be smoothed in order to provide a reasonably narrow estimate of the range of ozone return dates. Consistent with previous studies, but here for a Representative Concentration Pathway (RCP) of 6.0, these new CCMI simulations project that global total column ozone will return to 1980 values in 2049 (with a 1σ uncertainty of 2043–2055). At Southern Hemisphere mid-latitudes column ozone is projected to return to 1980 values in 2045 (2039–2050), and at Northern Hemisphere mid-latitudes in 2032 (2020–2044). In the polar regions, the return dates are 2060 (2055–2066) in the Antarctic in October and 2034 (2025–2043) in the Arctic in March. The earlier return dates in the Northern Hemisphere reflect the larger sensitivity to dynamical changes. Our estimates of return dates are later than those presented in the 2014 Ozone Assessment by approximately 5–17 years, depending on the region, with the previous best estimates often falling outside of our uncertainty range. In the tropics only around half the models predict a return of ozone to 1980 values, around 2040, while the other half do not reach the 1980 value. All models show a negative trend in tropical total column ozone towards the end of the 21st century. The CCMI models generally agree in their simulation of the time evolution of stratospheric chlorine and bromine, which are the main drivers of ozone loss and recovery. However, there are a few outliers which show that the multi-model mean results for ozone recovery are not as tightly constrained as possible. Throughout the stratosphere the spread of ozone return dates to 1980 values between models tends to correlate with the spread of the return of inorganic chlorine to 1980 values. In the upper stratosphere, greenhouse gas-induced cooling speeds up the return by about 10–20 years. In the lower stratosphere, and for the column, there is a more direct link in the timing of the return dates of ozone and chlorine, especially for the large Antarctic depletion. Comparisons of total column ozone between the models is affected by different predictions of the evolution of tropospheric ozone within the same scenario, presumably due to differing treatment of tropospheric chemistry. Therefore, for many scenarios, clear conclusions can only be drawn for stratospheric ozone columns rather than the total column. As noted by previous studies, the timing of ozone recovery is affected by the evolution of N2O and CH4. However, quantifying the effect in the simulations analysed here is limited by the few realisations available for these experiments compared to internal model variability. The large increase in N2O given in RCP 6.0 extends the ozone return globally by ∼15 years relative to N2O fixed at 1960 abundances, mainly because it allows tropical column ozone to be depleted. The effect in extratropical latitudes is much smaller. The large increase in CH4 given in the RCP 8.5 scenario compared to RCP 6.0 also lengthens ozone return by ∼15 years, again mainly through its impact in the tropics. Overall, our estimates of ozone return dates are uncertain due to both uncertainties in future scenarios, in particular those of greenhouse gases, and uncertainties in models. The scenario uncertainty is small in the short term but increases with time, and becomes large by the end of the century. There are still some model–model differences related to well-known processes which affect ozone recovery. Efforts need to continue to ensure that models used for assessment purposes accurately represent stratospheric chemistry and the prescribed scenarios of ozone-depleting substances, and only those models are used to calculate return dates. For future assessments of single forcing or combined effects of CO2, CH4, and N2O on the stratospheric column ozone return dates, this work suggests that it is more important to have multi-member (at least three) ensembles for each scenario from every established participating model, rather than a large number of individual models., Atmospheric Chemistry and Physics, 18 (11), ISSN:1680-7375, ISSN:1680-7367

The representation of the Tropical Tropopause Layer (TTL) in 13 different Chemistry Climate Models (CCMs) designed to represent the stratosphere is analyzed. Simulations for 1960–2005 and 1980–2100 are analyzed. Simulations for 1960–2005 are compared to reanalysis model output. CCMs are able to reproduce the basic structure of the TTL. There is a large (10 K) spread in annual mean tropical cold point tropopause temperatures. CCMs are able to reproduce historical trends in tropopause pressure obtained from reanalysis products. Simulated historical trends in cold point tropopause temperatures are not consistent across models or reanalyses. The pressure of both the tropical tropopause and the level of main convective outflow appear to have decreased (increased altitude) in historical runs as well as in reanalyses. Decreasing pressure trends in the tropical tropopause and level of main convective outflow are also seen in the future. Models consistently predict decreasing tropopause and convective outflow pressure, by several hPa/decade. Tropical cold point temperatures are projected to increase by 0.09 K/decade. Tropopause anomalies are highly correlated with tropical surface temperature anomalies and with tropopause level ozone anomalies, less so with stratospheric temperature anomalies. Simulated stratospheric water vapor at 90 hPa increases by up to 0.5–1 ppmv by 2100. The result is consistent with the simulated increase in temperature, highlighting the correlation of tropopause temperatures with stratospheric water vapor., Atmospheric Chemistry and Physics, 9 (5), ISSN:1680-7375, ISSN:1680-7367

Major mid-winter stratospheric sudden warmings (SSWs) are the largest instance of wintertime variability in the Arctic stratosphere. Because SSWs are able to cause significant surface weather anomalies on intra-seasonal timescales, several previous studies have focused on their potential future change, as might be induced by anthropogenic forcings. However, a wide range of results have been reported, from a future increase in the frequency of SSWs to an actual decrease. Several factors might explain these contradictory results, notably the use of different metrics for the identification of SSWs and the impact of large climatological biases in single-model studies. To bring some clarity, we here revisit the question of future SSW changes, using an identical set of metrics applied consistently across 12 different models participating in the Chemistry–Climate Model Initiative. Our analysis reveals that no statistically significant change in the frequency of SSWs will occur over the 21st century, irrespective of the metric used for the identification of the event. Changes in other SSW characteristics – such as their duration, deceleration of the polar night jet, and the tropospheric forcing – are also assessed: again, we find no evidence of future changes over the 21st century., Atmospheric Chemistry and Physics, 18 (15), ISSN:1680-7375, ISSN:1680-7367

This thesis is concerned with the role of internal gravity waves (IGWs) in the stratospheric dynamics and variability demonstrating the effect of spatiotemporal distribution of their activity on the stratospheric dynamics and transport. The first part introduces a theoretical overview of the most recent as well as classical approaches used for description of the wave-mean interaction in the middle atmosphere. Methodology for an IGW analysis from the GPS radio occultation density data is described in the next chapter and the advantages of utilization of density data are listed. The third chapter presents results describing the peculiar dynamics and anomalous IGW activity in the Eastern Asia/Northern Pacific region. An important part is dedicated to a discussion of accuracy limits and usability of different IGW activity proxies. The possible impact of the localized IGW activity is investigated using a mechanistic middle and upper atmosphere model in the last chapter. Sensitivity simulations are used to demonstrate an important role of the spatial distribution of IGW activity for a formation of planetary waves and for the longitudinal variability of the Brewer-Dobson circulation. Implications for the middle atmospheric and climate change research are discussed along with consequences for parameterizations of...

Als Vorläufergase von Ozon nehmen Stickoxide eine zentrale Rolle in der Atmosphärenchemie ein. Die großräumige Verteilung von Stickoxiden in der UTLS ist jedoch noch nicht hinreichend bekannt. In dieser Arbeit wurde die Verteilung von NO und NOy anhand von Stickoxidmessungen, die an Bord eines Linienflugzeugs durchgeführt werden, untersucht. Die NOy sowie die NO Mischungsverhältnisse zeigen klare saisonale und regionale Abhängigkeiten. Der Einfluss des Flugverkehrs auf die Stickoxide wird abgeschätzt. Ferner wurde das Messinstrument um einen NO2 Konverter erweitert. As an ozone precursor, nitrogen oxides play a key role in atmospheric chemistry. However, the large scale distribution of nitrogen oxides in the UTLS is not well known yet. This work focuses on the large scale NO and NOy distribution. Measurements were performed aboard a passenger aircraft. NOy and NO volume mixing ratios show clear seasonal and regional dependencies. The impact of aviation on the measured nitrogen oxide distribution was analyzed. As part of this work the NO/NOy-Instrument was enlarged by a photolytic NO2 converter.

Global distributions of profiles of sulphur hexafluoride (SF6) have been retrieved from limb emission spectra recorded by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat covering the period September 2002 to March 2004. Individual SF6 profiles have a precision of 0.5 pptv below 25 km altitude and a vertical resolution of 4–6 km up to 35 km altitude. These data have been validated versus in situ observations obtained during balloon flights of a cryogenic whole-air sampler. For the tropical troposphere a trend of 0.230±0.008 pptv/yr has been derived from the MIPAS data, which is in excellent agreement with the trend from ground-based flask and in situ measurements from the National Oceanic and Atmospheric Administration Earth System Research Laboratory, Global Monitoring Division. For the data set currently available, based on at least three days of data per month, monthly 5° latitude mean values have a 1σ standard error of 1%. From the global SF6 distributions, global daily and monthly distributions of the apparent mean age of air are inferred by application of the tropical tropospheric trend derived from MIPAS data. The inferred mean ages are provided for the full globe up to 90° N/S, and have a 1σ standard error of 0.25 yr. They range between 0 (near the tropical tropopause) and 7 years (except for situations of mesospheric intrusions) and agree well with earlier observations. The seasonal variation of the mean age of stratospheric air indicates episodes of severe intrusion of mesospheric air during each Northern and Southern polar winter observed, long-lasting remnants of old, subsided polar winter air over the spring and summer poles, and a rather short period of mixing with midlatitude air and/or upward transport during fall in October/November (NH) and April/May (SH), respectively, with small latitudinal gradients, immediately before the new polar vortex starts to form. The mean age distributions further confirm that SF6 is destroyed in the mesosphere to a considerable degree. Model calculations with the Karlsruhe simulation model of the middle atmosphere (KASIMA) chemical transport model agree well with observed global distributions of the mean age only if the SF6 sink reactions in the mesosphere are included in the model.