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This study analyses the variability and trends of ultraviolet-B (UV-B, wavelength 280–320 nm) radiation that can cause DNA damage. The variability and trends caused by climate change due to enhanced greenhouse gas (GHG) concentrations. The analysis is based on DNA-active irradiance, total ozone, total cloud cover, and surface albedo calculations with the European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) chemistry–climate model (CCM) free-running simulations following the RCP 6.0 climate scenario for the period 1960–2100. The model output is evaluated with DNA-active irradiance ground-based measurements, satellite SBUV (v8.7) total-ozone measurements, and satellite MODerate-resolution Imaging Spectroradiometer (MODIS) Terra cloud cover data. The results show that the model reproduces the observed variability and change in total ozone, DNA-active irradiance, and cloud cover for the period 2000–2018 quite well according to the statistical comparisons. Between 50∘ N–50∘ S, the DNA-damaging UV radiation is expected to decrease until 2050 and to increase thereafter, as was shown previously by Eleftheratos et al. (2020). This change is associated with decreases in the model total cloud cover and negative trends in total ozone after about 2050 due to increasing GHGs. The new study confirms the previous work by adding more stations over low latitudes and mid-latitudes (13 instead of 5 stations). In addition, we include estimates from high-latitude stations with long-term measurements of UV irradiance (three stations in the northern high latitudes and four stations in the southern high latitudes greater than 55∘). In contrast to the predictions for 50∘ N–50∘ S, it is shown that DNA-active irradiance will continue to decrease after the year 2050 over high latitudes because of upward ozone trends. At latitudes poleward of 55∘ N, we estimate that DNA-active irradiance will decrease by 8.2 %±3.8 % from 2050 to 2100. Similarly, at latitudes poleward of 55∘ S, DNA-active irradiance will decrease by 4.8 % ± 2.9 % after 2050. The results for the high latitudes refer to the summer period and not to the seasons when ozone depletion occurs, i.e. in late winter and spring. The contributions of ozone, cloud, and albedo trends to the DNA-active irradiance trends are estimated and discussed.

A tropospheric ozone time series from 1995 until end 2022 has been generated within ESA’s Climate Change Initiative+ programme. The GOME-type Tropical Tropospheric Ozone Essential Climate Variable (GTTO-ECV) satellite data record combines data from GOME, SCIAMACHY, OMI and the three GOME-2 missions. The retrieval is based on the Convective Cloud Differential technique, which limits the coverage to the tropical belt (20°S to 20°N). We generated two monthly mean data sets at 1° x 1° resolution: one corresponds to a tropospheric column up to 200 hPa as in the previous CCI data release (Heue et al., 2016), while the other is limited to 270 hPa and includes the operational Sentinel-5P data as an additional sensor. An internal reprocessing of S5P CCD using 200 hPa is planned but might not be ready in time. Besides a consistent reprocessing of the CCD data for individual sensors, we also updated the harmonising scheme. The mean bias as well as the mean annual cycle relative to the reference instrument (OMI) are used to correct for the differences between the sensors.Heue et al (2016) claimed a mean tropospheric ozone trend of +0.7 DU/decade (1995-2015). How did the trend change with the extended data set? The GTTO-ECV data record will be used to investigate the tropical mean trend as well as temporal and local changes in the trends. Also, a comparison with modelled tropospheric ozone data and the respective trends might be given.As a second data product we provide the global S5P-BASCOE tropospheric ozone data. The complete time series of the S5P total ozone columns has been reprocessed recently. The reprocessing includes an update of the Level1 data as well as reprocessed cloud and O3 total columns. We use the reprocessed OFFL ozone data set in combination with BASCOE assimilation constrained stratospheric ozone profiles to calculate the tropospheric ozone columns. Relative to ground-based observations the total OFFL columns show a small positive bias. Before the retrieval of the tropospheric ozone column this bias is subtracted. The updated tropospheric ozone columns might also be compared to modelled tropospheric ozone columns.

Methane (CH4), the second most important greenhouse gas directly emitted by human activity, is removed from the atmosphere via chemical degradation.In this study we assess the radiative feedback from atmospheric CH4 resulting from changes in its chemical sink, which is mainly the oxidation with the hydroxyl radical (OH) and, which is influenced by temperature and the chemical composition of the atmosphere.We present results from numerical simulations with the chemistry-climate model EMAC perturbed by either CO2 or CH4 increase.The essential innovation in the simulation set-up is the use of CH4 emission fluxes instead of prescribed CH4 concentrations at the lower boundary. This means that changes in the chemical sink can feed back on the atmospheric CH4 concentration without constraints.For both forcing agents, CO2 and CH4, we explore so called rapid radiative adjustments in simulations with prescribed sea surface temperatures, as well as slow radiative feedbacks and the climate sensitivity in respective simulations using an interactive oceanic mixed layer.To quantify individual physical and chemical radiative adjustments and feedbacks we use the partial radiative perturbation method in offline simulations with a radiative transfer model consistent with the one used in the online simulations.First results show a negative feedback of atmospheric CH4 in a warming and moistening troposphere. As water vapour is a precursor of OH, increased humidity leads to increasing OH mixing ratios. This leads in turn to a shortening of the CH4 lifetime and a reduction of the CH4 mixing ratios accordingly. This decrease in CH4 also affects the response of tropospheric ozone (O3) leading to a less pronounced increase of O3 in the tropical upper troposphere compared to previous studies of the O3 response following a CO2 perturbation (Dietmüller et al., 2014;Nowack et al., 2015;Marsh et al., 2016).

This study analyses the variability and trends of ultraviolet-B (UV-B, wavelength 280–320 nm) radiation that can cause DNA damage. The variability and trends caused by climate change due to enhanced greenhouse gas (GHG) concentrations. The analysis is based on DNA-active irradiance, total ozone, total cloud cover, and surface albedo calculations with the European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) chemistry–climate model (CCM) free-running simulations following the RCP 6.0 climate scenario for the period 1960–2100. The model output is evaluated with DNA-active irradiance ground-based measurements, satellite SBUV (v8.7) total-ozone measurements, and satellite MODerate-resolution Imaging Spectroradiometer (MODIS) Terra cloud cover data. The results show that the model reproduces the observed variability and change in total ozone, DNA-active irradiance, and cloud cover for the period 2000–2018 quite well according to the statistical comparisons. Between 50∘ N–50∘ S, the DNA-damaging UV radiation is expected to decrease until 2050 and to increase thereafter, as was shown previously by Eleftheratos et al. (2020). This change is associated with decreases in the model total cloud cover and negative trends in total ozone after about 2050 due to increasing GHGs. The new study confirms the previous work by adding more stations over low latitudes and mid-latitudes (13 instead of 5 stations). In addition, we include estimates from high-latitude stations with long-term measurements of UV irradiance (three stations in the northern high latitudes and four stations in the southern high latitudes greater than 55∘). In contrast to the predictions for 50∘ N–50∘ S, it is shown that DNA-active irradiance will continue to decrease after the year 2050 over high latitudes because of upward ozone trends. At latitudes poleward of 55∘ N, we estimate that DNA-active irradiance will decrease by 8.2 %±3.8 % from 2050 to 2100. Similarly, at latitudes poleward of 55∘ S, DNA-active irradiance will decrease by 4.8 % ± 2.9 % after 2050. The results for the high latitudes refer to the summer period and not to the seasons when ozone depletion occurs, i.e. in late winter and spring. The contributions of ozone, cloud, and albedo trends to the DNA-active irradiance trends are estimated and discussed.

Air masses within the Asian monsoon anticyclone (AMA) show anomalous signatures in various trace gases. In this study, we analyze how air masses are transported from the planetary boundary layer (PBL) to the AMA via multiannual trajectory anlyses. While previous studies analyzed the PBL to AMA transport mainly for individual monsoon seasons or particular periods, we focus on the climatological perspective and on the interannual and intraseasonal variability. To this end we employ backward trajectories, which were computed using reanalysis data. Based on these trajectories, we analyze air mass transport from the PBL to the AMA during northern summer (June–August) for 14 summer seasons. Further, we backtrack forward trajectories from a free-running chemistry-climate model (CCM) simulation, which includes parametrized Lagrangian convection. The analysis of this additional model data set helps us to carve out robust or sensitive features of PBL to AMA transport with respect to the employed model. Results from both the trajectory model and the Lagrangian CCM emphasize the robustness of the three-dimensional transport pathways from the PBL to the AMA. Air masses are transported upwards on the eastern side of the AMA and are uplifted within the full AMA domain above. While this is in agreement with previous modelling studies, we refine the picture of the so-called "conduit" (Bergman et al., 2013). The contributions from the Tibetan Plateau (TP; 17 % vs. 15 %) and the West Pacific (around 12 %) are similar in both model results. However, the contributions from the Indian subcontinent and South-East Asia are considerably larger in the Lagrangian CCM data, which might point towards the importance of convective transport for PBL to AMA transport for these regions. The analysis of both model data sets highlights the interannual and intraseasonal variability with respect to PBL source regions of the AMA. Additionally, we analyze the relation of the interannual east-west displacement of the AMA – which we find to be related to the monsoon Hadley index – to the transport behaviour and find that there are differences for "east" and "west years", the main transport characteristics, however, are comparable. Regarding the intraseasonal variability our trajectory model results show that transport from the PBL over the Tibetan Plateau (TP) to the AMA is weak in early June (less than 4 % of the AMA air masses), whereas in August TP air masses contribute considerably (roughly 24 %). The evolution of the contribution from the TP is supported by data from the Lagrangian CCM and is related to the northward shift of the subtropical jet and the AMA during this period. This result may help to reconcile previous results and further highlights the need of taking the subseasonal (and interannual) variability of the AMA and associated transport into account.

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.

One of the key questions in the air quality and climate sciences is how will tropospheric ozone concentrations 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 implemented in the models to examine changes in transport. We find that 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 lead to enhanced STT in the subtropics. The acceleration of the deep branch of the BDC in the NH and changes in eddy transport contribute to increase STT at high latitudes. In the SH, the deep branch does not accelerate due to the dynamical effects of the ozone hole recovery.

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.

The South Asian High (SAH) is an important component of the summer monsoon system in Asia. In this study we investigate the location and drivers of the SAH at 100 hPa during the boreal summers of 1979 to 2014 on interannual, seasonal and synoptic timescales using seven reanalyses and observational data. Our comparison of the different reanalyses focuses especially on the bimodality of the SAH, i.e. the two preferred modes of the SAH centre location: the Iranian Plateau to the west and the Tibetan Plateau to the east. We find that only the National Centers for Environmental Prediction–National Center of Atmospheric Research (NCEP–NCAR) reanalysis shows a clear bimodal structure of the SAH centre distribution with respect to daily and pentad (5 day) mean data. Furthermore, the distribution of the SAH centre location is highly variable from year to year. As in simple model studies, which connect the SAH to heating in the tropics, we find that the mean seasonal cycle of the SAH and its centre are dominated by the expansion of convection in the South Asian region (70–130° E × 15–30° N) on the south-eastern border of the SAH. A composite analysis of precipitation and outgoing long-wave radiation data with respect to the location of the SAH centre reveals that a more westward (eastward) location of the SAH is related to stronger (weaker) convection and rainfall over India and weaker (stronger) precipitation over the western Pacific.

This study investigates the abrupt and severe water vapour decline in the stratosphere beginning in the year 2000 (the "millennium water vapour drop") and other similarly strong stratospheric water vapour reductions by means of various simulations with the state-of-the-art Chemistry-Climate Model (CCM) EMAC (ECHAM/MESSy Atmospheric Chemistry Model). The model simulations differ with respect to the prescribed sea surface temperatures (SSTs) and whether nudging is applied or not. The CCM EMAC is able to most closely reproduce the signature and pattern of the water vapour drop in agreement with those derived from satellite observations if the model is nudged. Model results confirm that this extraordinary water vapour decline is particularly obvious in the tropical lower stratosphere and is related to a large decrease in cold point temperature. The drop signal propagates under dilution to the higher stratosphere and to the poles via the Brewer–Dobson circulation (BDC). We found that the driving forces for this significant decline in water vapour mixing ratios are tropical sea surface temperature (SST) changes due to a coincidence with a preceding strong El Niño–Southern Oscillation event (1997/1998) followed by a strong La Niña event (1999/2000) and supported by the change of the westerly to the easterly phase of the equatorial stratospheric quasi-biennial oscillation (QBO) in 2000. Correct (observed) SSTs are important for triggering the strong decline in water vapour. There are indications that, at least partly, SSTs contribute to the long period of low water vapour values from 2001 to 2006. For this period, the specific dynamical state of the atmosphere (overall atmospheric large-scale wind and temperature distribution) is important as well, as it causes the observed persistent low cold point temperatures. These are induced by a period of increased upwelling, which, however, has no corresponding pronounced signature in SSTs anomalies in the tropics. Our free-running simulations do not capture the drop as observed, because a) the cold point temperature has a low bias and thus the water vapour variability is reduced and b) because they do not simulate the appropriate dynamical state. Large negative water vapour declines are also found in other years and seem to be a feature which can be found after strong combined El Niño/La Niña events if the QBO west phase during La Niña changes to the east phase.

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.

An important driver of climate change is stratospheric water vapour (SWV), which in turn is influenced by the oxidation of atmospheric methane (CH4). In order to parameterize the production of water vapour (H2O) from CH4 oxidation, it is often assumed that the oxidation of one CH4 molecule yields exactly two molecules of H2O. However, this assumption is based on an early study, which also gives evidence, that this is not true at all altitudes. In the current study we re-evaluate this assumption with a comprehensive systematic analysis using a state-of-the art Chemistry-Climate model (CCM), namely the ECHAM/MESSy Atmospheric Chemistry (EMAC) model, and present three approaches to investigate the yield of H2O and hydrogen gas (H2) from CH4 oxidation. We thereby make use of Module Efficiently Calculating the Chemistry of the Atmosphere (MECCA) in a box model and global model configuration. Furthermore, we use the kinetic chemistry tagging technique (MECCA-TAG) to investigate the chemical pathways between CH4, H2O and H2, by being able to distinguish hydrogen atoms stemming from CH4 and other sources. We apply three approaches, which all agree that assuming a yield of 2 overestimates the production of H2O in the lower stratosphere (calculated as 1.5–1.7). Additionally, transport and subsequent photochemical processing of longer-lived intermediates raise the local yield values in the upper stratosphere and lower mesosphere above 2 (maximum > 2.2). In the middle and upper mesosphere, the influence of loss and recycling of H2O increases, making it a crucial factor in the parameterization of the yield of H2O from CH4 oxidation. An additional sensitivity study with the Chemistry As A Boxmodel Application (CAABA) shows a dependence of the yield on the hydroxyl radical (OH) abundance. No significant temperature dependence is found. We focus representatively on the tropical zone between 23° S–23° N, where seasonal variations are negligible. It is found in the global approach that presented results are mostly valid for mid latitudes as well. Our conclusions question the use of a constant yield of H2O from CH4 oxidation in climate modeling and encourage to apply comprehensive parameterizations that follow the vertical profiles of the H2O yield derived here and take the chemical H2O loss into account.

Trend estimates with different signs are reported in the literature for lower stratospheric water vapour considering the time period between the late 1980s and 2010. The NOAA (National Oceanic and Atmospheric Administration) frost point hygrometer (FPH) observations at Boulder (Colorado, 40.0° N, 105.2° W) indicate positive trends (about 0.12 ppmv decade−1–0.45 ppmv decade−1). Contrary, negative trends (approximately −0.15 ppmv decade−1–−0.05 ppmv decade−1) are derived from a merged zonal mean satellite data set for a latitude band around the Boulder latitude. Overall, the trend differences between the two data sets range from about 0.25 ppmv decade−1 to 0.45 ppmv decade−1, depending on altitude. A possible explanation for these discrepancies is a different temporal behaviour at Boulder and the zonal mean, which simply indicates a sampling bias. In this work we investigate trend differences between Boulder and the zonal mean using primarily simulations from ECHAM/MESSy (European Centre for Medium-Range Weather Forecasts Hamburg/Modular Earth Submodel System) Atmospheric Chemistry (EMAC), WACCM (Whole Atmosphere Community Climate Model), CMAM (Canadian Middle Atmosphere Model) and CLaMS (Chemical Lagrangian Model of the Stratosphere). On shorter time scales we address this aspect also based on satellite observations from UARS/HALOE (Upper Atmosphere Research Satellite/Halogen Occultation Experiment), Envisat/MIPAS (Environmental Satellite/Michelson Interferometer for Passive Atmospheric Sounding) and Aura/MLS (Microwave Limb Sounder). Overall, both the simulations and observations exhibit trend differences between Boulder and the zonal mean. The differences are dependent on altitude and the time period considered. The model simulations indicate only small trend differences between Boulder and the zonal mean for the time period between the late 1980s and 2010. These are clearly not sufficient to explain the discrepancies between the trend estimates derived from the FPH observations and the merged zonal mean satellite data set. Unless the simulations underrepresent variability or the trend differences originate from smaller spatial and temporal scales than resolved by the model simulations, trends at Boulder for this time period should be quite representative also for the zonal mean and even other latitude bands. Trend differences for a decade of data are larger and need to be kept in mind when comparing results for Boulder and the zonal mean on this time scale. Beyond that, we find that the trend estimates for the time period between the late 1980s and 2010 also significantly differ among the simulations. They are larger than those derived from the merged satellite data set and smaller than the trend estimates derived from the FPH observations.

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.

In this study the stratospheric variability is analysed from decadal to seasonal timescales. Relevant processes for the decadal timescale are identified by means of power spectral analysis. The inspection of the ERA-Interim reanalysis data set shows considerably high variability at the 12 and 6 months period. But also in the extra tropical region at intra-annual to seasonal timescales clear peaks in the power spectrum arise. In addition to that, the quasi-biennial oscillation (QBO) obviously contributes to the stratospheric variability at decadal timescales. Regarding the power spectrum of EMAC 2.52 model simulations, only a model configuration with a vertical resolution smaller than 1 km in the stratosphere is capable to capture the relevant features of the spectrum. In particular, the model with a coarser distribution of vertical levels cannot reproduce the QBO signal. The analysis of the corresponding wave spectra reveals that, if the vertical resolution is insufficient, primarily the Mixed-Rossby-Gravity waves cannot be adequately reproduced. Estimates made by linear wave theory show that for reanalysis data the Mixed-Rossby-Gravity waves with equivalent depths between 50 m to 250 m are relevant for the QBO. In order to resolve these relevant waves, model simulations need to consider a vertical resolution of at least 1 km.

The stratospheric climate and variability from simulations of sixteen chemistry-climate models is evaluated. On average the polar night jet is well reproduced though its variability is less well reproduced with a large spread between models. Polar temperature biases are less than 5 K except in the Southern Hemisphere (SH) lower stratosphere in spring. The accumulated area of low temperatures responsible for polar stratospheric cloud formation is accurately reproduced for the Antarctic but underestimated for the Arctic. The shape and position of the polar vortex is well simulated, as is the tropical upwelling in the lower stratosphere. There is a wide model spread in the frequency of major sudden stratospheric warnings (SSWs), late biases in the breakup of the SH vortex, and a weak annual cycle in the zonal wind in the tropical upper stratosphere. Quantitatively, "metrics" indicate a wide spread in model performance for most diagnostics with systematic biases in many, and poorer performance in the SH than in the Northern Hemisphere (NH). Correlations were found in the SH between errors in the final warming, polar temperatures, the leading mode of variability, and jet strength, and in the NH between errors in polar temperatures, frequency of major SSWs, and jet strength. Models with a stronger QBO have stronger tropical upwelling and a colder NH vortex. Both the qualitative and quantitative analysis indicate a number of common and long-standing model problems, particularly related to the simulation of the SH and stratospheric variability. Copyright 2011 by the American Geophysical Union.

The South Asian High (SAH) is an important component of the summer monsoon system in Asia. In this study we investigate the location and drivers of the SAH at 100 hPa during the boreal summers of 1979 to 2014 on interannual, seasonal and synoptic time scales using six reanalyses. Special focus lies on the bimodality of the SAH, i.e. the two preferred modes of the SAH centre location: the Iranian Plateau to the west and the Tibetan Plateau to the east. We find that only the National Centers for Environmental Prediction – National Center of Atmospheric Research (NCEP/NCAR) reanalysis shows a clear bimodal structure of the SAH centre distribution with respect to daily and pentad (5-day mean) data. Furthermore, the distribution of the SAH centre location is highly variable from year-to-year. As in simple model studies, which connect the SAH to heating in the tropics, we find that the mean seasonal cycle of the SAH and its centre are dominated by the expansion of convection in the South Asian region (70° E–130° E × 15° N–30° N) on the southeastern border of the SAH. A composite analysis of precipitation and OLR data with respect to the location of the SAH centre reveals that a more westward (eastward) location of the SAH is related to stronger (weaker) convection and rainfall over India and stronger (weaker) precipitation over the West Pacific.

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.

The assessment model for ultraviolet radiation and risk "AMOUR" is applied to output from two chemistry-climate models (CCMs). Results from the UK Chemistry and Aerosols CCM are used to quantify the worldwide skin cancer risk avoided by the Montreal Protocol and its amendments: by the year 2030, two million cases of skin cancer have been prevented yearly, which is 14% fewer skin cancer cases per year. In the "World Avoided," excess skin cancer incidence will continue to grow dramatically after 2030. Results from the CCM E39C-A are used to estimate skin cancer risk that had already been inevitably committed once ozone depletion was recognized: excess incidence will peak mid 21st century and then recover or even super-recover at the end of the century. When compared with a "No Depletion" scenario, with ozone undepleted and cloud characteristics as in the 1960s throughout, excess incidence (extra yearly cases skin cancer per million people) of the "Full Compliance with Montreal Protocol" scenario is in the ranges: New Zealand: 100-150, Congo: -10-0, Patagonia: 20-50, Western Europe: 30-40, China: 90-120, South-West USA: 80-110, Mediterranean: 90-100 and North-East Australia: 170-200. This is up to 4% of total local incidence in the Full Compliance scenario in the peak year.

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

Chemistry-Climate Model (CCM) simulations are commonly used to project the past and future development of the dynamics and chemistry of the stratosphere, and in particular the ozone layer. So far, CCMs are usually not interactively coupled to an ocean model, so that sea surface temperatures (SSTs) and sea ice coverage are prescribed in the simulations. While for future integrations SSTs have to be taken from precalculated climate model projections, for CCM experiments resembling the past either modelled or observed SSTs can be used. This study addresses the question to which extent atmospheric climatologies and long-term trends for the recent past simulated in the CCM E39C-A differ when choosing either observed or modelled SSTs. Furthermore, the processes of how the SST signal is communicated to the atmosphere, and in particular to the stratosphere are examined. Two simulations that differ only with respect to the prescribed SSTs and that span years 1960 to 1999 are used. Significant differences in temperature and ozone climatologies between the model simulations are found. The differences in ozone are attributed to differences in the meridional circulation, which are in turn driven by weaker wave forcing in the simulation with generally lower SSTs. The long-term trends over 40 years in annual mean temperature and ozone differ only in the troposphere, where temperatures are directly influenced by the local SST trends. Differences in temperature and ozone trends are only found on shorter time scales. The trends in tropical upwelling, as a measure of the strength of the Brewer-Dobson circulation (BDC), differ strongly between the simulations. A reverse from negative to positive trends is found in the late 1970s in the simulation using observed SSTs while trends are positive throughout the simulation when using modelled SSTs. The increase in the BDC is a robust feature of the simulations only after about 1980 and is evident mainly in the tropics in the lower stratosphere.