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Solar radiation management through artificially increasing the amount of stratospheric sulfate aerosol is being considered as a possible climate engineering method. To overcome the challenge of transporting the necessary amount of sulfur to the stratosphere, Quaglia and co-workers suggest deliberate emissions of carbonyl sulfide (OCS), a long-lived precursor of atmospheric sulfate. In their paper, published in Atmospheric Chemistry and Physics in 2022, they outline two scenarios with OCS emissions either at the Earth's surface or in the tropical upper troposphere and calculate the expected radiative forcing using a climate model. In our opinion, the study (i) neglects a significantly higher surface uptake that will inevitably be induced by the elevated atmospheric OCS concentrations and (ii) overestimates the net cooling effect of this OCS geoengineering approach due to some questionable parameterizations and assumptions in the radiative forcing calculations. In this commentary, we use state-of-the-art models to show that at the mean atmospheric OCS mixing ratios of the two emissions scenarios, the terrestrial biosphere and the oceans are expected to take up more OCS than is being released to reach these levels. Using chemistry climate models with a long-standing record for estimating the climate forcing of OCS and stratospheric aerosols, we also show that the net radiative forcing of the emission scenarios suggested by Quaglia and co-workers is smaller than suggested and insufficient to offset any significant portion of anthropogenically induced climate change. Our conclusion is that a geoengineering approach using OCS will not work under any circumstances and should not be considered further.

A previous model intercomparison of the Tambora aerosol cloud has highlighted substantial differences among simulated volcanic aerosol properties in the pre-industrial stratosphere and has led to questions about the applicability of global aerosol models for large-magnitude explosive eruptions prior to the observational period. Here, we compare the evolution of the stratospheric aerosol cloud following the well-observed June 1991 Mt. Pinatubo eruption simulated with six interactive stratospheric aerosol microphysics models to a range of observational data sets. Our primary focus is on the uncertainties regarding initial SO2 emission following the Pinatubo eruption, as prescribed in the Historical Eruptions SO2 Emission Assessment experiments (HErSEA), in the framework of the Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP). Six global models with interactive aerosol microphysics took part in this study: ECHAM6-SALSA, EMAC, ECHAM5-HAM, SOCOL-AERv2, ULAQ-CCM, and UM-UKCA. Model simulations are performed by varying the SO2 injection amount (ranging between 5 and 10 Tg S) and the altitude of injection (between 18–25 km). The comparisons show that all models consistently demonstrate faster reduction from the peak in sulfate mass burden in the tropical stratosphere. Most models also show a stronger transport towards the extratropics in the Northern Hemisphere, at the expense of the observed tropical confinement, suggesting a much weaker subtropical barrier in all the models, which results in a shorter e-folding time compared to the observations. Furthermore, simulations in which more than 5 Tg S in the form of SO2 is injected show an initial overestimation of the sulfate burden in the tropics and, in some models, in the Northern Hemisphere and a large surface area density a few months after the eruption compared to the values measured in the tropics and the in situ measurements over Laramie. This draws attention to the importance of including processes such as the ash injection for the removal of the initial SO2 and aerosol lofting through local heating.

This paper presents model simulations of stratospheric aerosols with a focus on explosive volcanic eruptions. Using various (occultation and limb-based) satellite instruments, providing vertical profiles of sulfur dioxide (SO2) and aerosol extinction, we characterized the chemical and radiative influence of volcanic aerosols for the period between 1990 and 2019. We established an improved and extended volcanic SO2 emission inventory that includes more than 500 explosive volcanic eruptions reaching the upper troposphere and the stratosphere. Each perturbation identified was derived from the satellite data and incorporated as a three-dimensional SO2 plume into a chemistry-climate model without the need for additional assumptions about altitude distribution and eruption duration as needed for a “point source” approach. The simultaneous measurements of SO2 and aerosol extinction by up to four satellite instruments enabled a reliable conversion of extinction measurements into injected SO2. In the chemistry-climate model, the SO2 from each individual plume was converted into aerosol particles and their optical properties were determined. Furthermore, the aerosol optical depth (AOD) and the instantaneous radiative forcing on climate were calculated online. Combined with model improvements, the results of the simulations are consistent with the observations of the various satellites. Slight deviations between the observations and model simulations were found for the large volcanic eruption of Pinatubo in 1991 and cases where simultaneous satellite observations were not unique or too sparse. Weak- and medium-strength volcanic eruptions captured in satellite data and the Smithsonian database typically inject about 10 to 50 kt SO2 directly into the upper troposphere/lower stratosphere (UTLS) region or the sulfur species are transported via convection and advection. Our results confirm that these relatively minor eruptions, which occur quite frequently, can nevertheless contribute to the stratospheric aerosol layer and are relevant for the Earth's radiation budget. These minor eruptions cause a total global instantaneous radiative forcing of the order of −0.1 W m−2 at the top of the atmosphere (TOA) compared to a background stratospheric aerosol forcing of about −0.04 W m−2. Medium-strength eruptions injecting about 400 kt SO2 into the stratosphere or accumulation of consecutive smaller eruptions can lead to a total instantaneous forcing of about −0.3 W m−2. We show that it is critical to include the contribution of the extratropical lowermost stratospheric aerosol in the forcing calculations.

Enhanced aerosol abundance in the upper troposphere and lower stratosphere (UTLS) associated with the Asian summer monsoon (ASM) is referred to as the Asian Tropopause Aerosol Layer (ATAL). The chemical composition, microphysical properties, and climate effects of aerosols in the ATAL have been the subject of discussion over the past decade. In this work, we use the ECHAM/MESSy Atmospheric Chemistry (EMAC) general circulation model at a relatively fine grid resolution (about 1.1×1.1∘) to numerically simulate the emissions, chemistry, and transport of aerosols and their precursors in the UTLS within the ASM anticyclone during the years 2010–2012. We find a pronounced maximum of aerosol extinction in the UTLS over the Tibetan Plateau, which to a large extent is caused by mineral dust emitted from the northern Tibetan Plateau and slope areas, lofted to an altitude of at least 10 km, and accumulating within the anticyclonic circulation. We also find that the emissions and convection of ammonia in the central main body of the Tibetan Plateau make a great contribution to the enhancement of gas-phase NH3 in the UTLS over the Tibetan Plateau and ASM anticyclone region. Our simulations show that mineral dust, water-soluble compounds, such as nitrate and sulfate, and associated liquid water dominate aerosol extinction in the UTLS within the ASM anticyclone. Due to shielding of high background sulfate concentrations outside the anticyclone from volcanoes, a relative minimum of aerosol extinction within the anticyclone in the lower stratosphere is simulated, being most pronounced in 2011, when the Nabro eruption occurred. In contrast to mineral dust and nitrate concentrations, sulfate increases with increasing altitude due to the larger volcano effects in the lower stratosphere compared to the upper troposphere. Our study indicates that the UTLS over the Tibetan Plateau can act as a well-defined conduit for natural and anthropogenic gases and aerosols into the stratosphere.

This paper presents decadal simulations of stratospheric and tropospheric aerosol and its radiative effects by the chemistry general circulation model EMAC constrained with satellite observations in the framework of the ESA Aerosol CCI project such as GOMOS (Global Ozone Monitoring by Occultation of Stars) and (A)ATSR ((Advanced) Along Track Scanning Radiometer) on the ENVISAT (European Environmental Satellite), IASI (Infrared Atmospheric Sounding Interferometer) on MetOp (Meteorological Operational Satellite), and, additionally, OSIRIS (Optical Spectrograph and InfraRed Imaging System). In contrast to most other studies, the extinctions and optical depths from the model are compared to the observations at the original wavelengths of the satellite instruments covering the range from the UV (ultraviolet) to terrestrial IR (infrared). This avoids conversion artifacts and provides additional constraints for model aerosol and interpretation of the observations.MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) SO2 limb measurements are used to identify plumes of more than 200 volcanic eruptions. These three-dimensional SO2 plumes are added to the model SO2 at the eruption times. The interannual variability in aerosol extinction in the lower stratosphere, and of stratospheric aerosol radiative forcing at the tropopause, is dominated by the volcanoes. To explain the seasonal cycle of the GOMOS and OSIRIS observations, desert dust simulated by a new approach and transported to the lowermost stratosphere by the Asian summer monsoon and tropical convection turns out to be essential. This also applies to the radiative heating by aerosol in the lowermost stratosphere. The existence of wet dust aerosol in the lowermost stratosphere is indicated by the patterns of the wavelength dependence of extinction in observations and simulations. Additional comparison with (A)ATSR total aerosol optical depth at different wavelengths and IASI dust optical depth demonstrates that the model is able to represent stratospheric as well as tropospheric aerosol consistently.

The Stratospheric Sulfur and its Role in Climate (SSiRC) Interactive Stratospheric Aerosol Model Intercomparison Project (ISA-MIP) explores uncertainties in the processes that connect volcanic emission of sulfur gas species and the radiative forcing associated with the resulting enhancement of the stratospheric aerosol layer. The central aim of ISA-MIP is to constrain and improve interactive stratospheric aerosol models and reduce uncertainties in the stratospheric aerosol forcing by comparing results of standardized model experiments with a range of observations. In this paper we present four co-ordinated inter-model experiments designed to investigate key processes which influence the formation and temporal development of stratospheric aerosol in different time periods of the observational record. The Background (BG) experiment will focus on microphysics and transport processes under volcanically quiescent conditions, when the stratospheric aerosol is controlled by the transport of aerosols and their precursors from the troposphere to the stratosphere. The Transient Aerosol Record (TAR) experiment will explore the role of small- to moderate-magnitude volcanic eruptions, anthropogenic sulfur emissions, and transport processes over the period 1998–2012 and their role in the warming hiatus. Two further experiments will investigate the stratospheric sulfate aerosol evolution after major volcanic eruptions. The Historical Eruptions SO2 Emission Assessment (HErSEA) experiment will focus on the uncertainty in the initial emission of recent large-magnitude volcanic eruptions, while the Pinatubo Emulation in Multiple models (PoEMS) experiment will provide a comprehensive uncertainty analysis of the radiative forcing from the 1991 Mt Pinatubo eruption.

The modelling of aerosol radiative forcing is a major cause of uncertainty in the assessment of global and regional atmospheric energy budgets and climate change. One reason is the strong dependence of the aerosol optical properties on the mixing state of aerosol components, such as absorbing black carbon and, predominantly scattering sulfates. Using a new column version of the aerosol optical properties and radiative-transfer code of the ECHAM/MESSy atmospheric-chemistry–climate model (EMAC), we study the radiative transfer applying various mixing states. The aerosol optics code builds on the AEROPT (AERosol OPTical properties) submodel, which assumes homogeneous internal mixing utilising the volume average refractive index mixing rule. We have extended the submodel to additionally account for external mixing, partial external mixing and multilayered particles. Furthermore, we have implemented the volume average dielectric constant and Maxwell Garnett mixing rule. We performed regional case studies considering columns over China, India and Africa, corroborating much stronger absorption by internal than external mixtures. Well-mixed aerosol is a good approximation for particles with a black-carbon core, whereas particles with black carbon at the surface absorb significantly less. Based on a model simulation for the year 2005, we calculate that the global aerosol direct radiative forcing for homogeneous internal mixing differs from that for external mixing by about 0.5 W m−2.

The photolysis of HONO is important for the atmospheric HOx (OH + HO2) radical budget and ozone formation, especially in polluted air. Nevertheless, owing to the incomplete knowledge of HONO sources, realistic HONO mechanisms have not yet been implemented in global models. We investigated measurement data sets from 15 field measurement campaigns conducted in different countries worldwide. It appears that the HONO/NOx ratio is a good proxy predictor for HONO mixing ratios under different atmospheric conditions. From the robust relationship between HONO and NOx, a representative mean HONO/NOx ratio of 0.02 has been derived. Using a global chemistry-climate model and employing this HONO/NOx ratio, realistic HONO levels are simulated, being about one order of magnitude higher than the reference calculations that only consider the reaction OH + NO → HONO. The resulting enhancement of HONO significantly impacts HOx levels and photo-oxidation products (e.g, O3, PAN), mainly in polluted regions. Furthermore, the relative enhancements in OH and secondary products are higher in winter than in summer, thus enhancing the oxidation capacity in polluted regions, especially in winter when other photolytic OH sources are of minor importance. Our results underscore the need to improve the understanding of HONO chemistry and its representation in atmospheric models.

Globally, carbonyl sulphide (COS) is the most abundant sulphur gas in the atmosphere. Our chemistry-climate model (CCM) of the lower and middle atmosphere with aerosol module realistically simulates the background stratospheric sulphur cycle, as observed by satellites in volcanically quiescent periods. The model results indicate that upward transport of COS from the troposphere largely controls the sulphur budget and the aerosol loading of the background stratosphere. This differs from most previous studies which indicated that short-lived sulphur gases are also important. The model realistically simulates the modulation of the particulate and gaseous sulphur abundance in the stratosphere by the quasi-biennial oscillation (QBO). In the lowermost stratosphere organic carbon aerosol contributes significantly to extinction. Further, using a chemical radiative convective model and recent spectra, we compute that the direct radiative forcing efficiency by 1 kg of COS is 724 times that of 1 kg CO2. Considering an anthropogenic fraction of 30% (derived from ice core data), this translates into an overall direct radiative forcing by COS of 0.003 W m−2. The direct global warming potentials of COS over time horizons of 20 and 100 yr are GWP(20 yr) = 97 and GWP(100 yr) = 27, respectively (by mass). Furthermore, stratospheric aerosol particles produced by the photolysis of COS (chemical feedback) contribute to a negative direct solar radiative forcing, which in the CCM amounts to −0.007 W m−2 at the top of the atmosphere for the anthropogenic fraction, more than two times the direct warming forcing of COS. Considering that the lifetime of COS is twice that of stratospheric aerosols the warming and cooling tendencies approximately cancel.

The submodel PSC of the ECHAM5/MESSy Atmospheric Chemistry model (EMAC) has been developed to simulate the main types of polar stratospheric clouds (PSC). The parameterisation of the supercooled ternary solutions (STS, type 1b PSC) in the submodel is based on Carslaw et al. (1995b), the thermodynamic approach to simulate ice particles (type 2 PSC) on Marti and Mauersberger (1993). For the formation of nitric acid trihydrate (NAT) particles (type 1a PSC) two different parameterisations exist. The first is based on an instantaneous thermodynamic approach from Hanson and Mauersberger (1988), the second is new implemented and considers the growth of the NAT particles with the aid of a surface growth factor based on Carslaw et al. (2002). It is possible to choose one of this NAT parameterisation in the submodel. This publication explains the background of the submodel PSC and the use of the submodel with the goal of simulating realistic PSC in EMAC.

We describe the setup and first results of an inverse modelling system for atmospheric N2O, based on a four-dimensional variational (4DVAR) technique and the atmospheric transport zoom model TM5. We focus in this study on the European domain, utilizing a comprehensive set of quasi-continuous measurements over Europe, complemented by N2O measurements from the Earth System Research Laboratory of the National Oceanic and Atmospheric Administration (NOAA/ESRL) cooperative global air sampling network. Despite ongoing measurement comparisons among networks parallel measurements at a limited number of stations show that significant offsets exist among the different laboratories. Since the spatial gradients of N2O mixing ratios are of the same order of magnitude as these biases, the direct use of these biased datasets would lead to significant errors in the derived emissions. Therefore, in order to also use measurements with unknown offsets, a new bias correction scheme has been implemented within the TM5-4DVAR inverse modelling system, thus allowing the simultaneous assimilation of observations from different networks. The N2O bias corrections determined in the TM5-4DVAR system agree within ~0.1 ppb (dry-air mole fraction) with the bias derived from the measurements at monitoring stations where parallel NOAA discrete air samples are available. The N2O emissions derived for the northwest European and east European countries for 2006 show good agreement with the bottom-up emission inventories reported to the United Nations Framework Convention on Climate Change (UNFCCC). Moreover, the inverse model can significantly narrow the uncertainty range reported in N2O emission inventories for these countries, while the lack of measurements does not allow to reduce the uncertainties of emission estimates in southern Europe. Several sensitivity experiments were performed to test the robustness of the results. It is shown that also inversions without detailed a priori spatio-temporal emission distributions are capable to reproduce major regional emission patterns within the footprint of the existing atmospheric network, demonstrating the strong constraints of the atmospheric observations on the derived emissions.

Moist convection in global modelling contributes significantly to the transport of energy, momentum, water and trace gases and aerosols within the troposphere. Since convective clouds are on a scale too small to be resolved in a global model their effects have to be parameterised. However, the whole process of moist convection and especially its parameterisations are associated with uncertainties. In contrast to previous studies on the impact of convection on trace gases, which had commonly neglected the convective transport for some or all compounds, we investigate this issue by examining simulations with five different convection schemes. This permits an uncertainty analysis due to the process formulation, without the inconsistencies inherent in entirely neglecting deep convection or convective tracer transport for one or more tracers. Both the simulated mass fluxes and tracer distributions are analysed. Investigating the distributions of compounds with different characteristics, e.g., lifetime, chemical reactivity, solubility and source distributions, some differences can be attributed directly to the transport of these compounds, whereas others are more related to indirect effects, such as the transport of precursors, chemical reactivity in certain regions, and sink processes. The model simulation data are compared with the average regional profiles of several measurement campaigns, and in detail with two campaigns in fall and winter 2005 in Suriname and Australia, respectively. The shorter-lived a compound is, the larger the differences and consequently the uncertainty due to the convection parameterisation are, as long as it is not completely controlled by local production that is independent of convection and its impacts (e.g. water vapour changes). Whereas for long-lived compounds like CO or O3 the mean differences between the simulations are less than 25%), differences for short-lived compounds reach up to ±100% with different convection schemes. A rating of an overall "best" performing scheme is difficult, since the optimal performance depends on the region and compound.

The atmospheric chemistry general circulation model ECHAM5/MESSy1 has been extended by processes that parameterise particle precipitation. Several types of particle precipitation that directly affect NOy and HOx concentrations in the middle atmosphere are accounted for and discussed in a series of papers. In the companion paper, the ECHAM5/MESSy1 solar proton event parametrisation is discussed, while in the current paper we focus on low energy electrons (LEE) that produce NOx in the upper atmosphere. For the flux of LEE NOx into the top of the model domain a novel technique which can be applied to most atmospheric chemistry general circulation models has been developed and is presented here. The technique is particularly useful for models with an upper boundary between the stratopause and mesopause and therefore cannot directly incorporate upper atmospheric NOx production. The additional NOx source parametrisation is based on a measure of geomagnetic activity, the Ap index, which has been shown to be a good proxy for LEE NOx interannual variations. HALOE measurements of LEE NOx that has been transported into the stratosphere are used to develop a scaling function which yields a flux of NOx that is applied to the model top. We describe the implementation of the parametrisation as the submodel SPACENOX in ECHAM5/MESSy1 and discuss the results from test simulations. The NOx enhancements are shown to be in good agreement with independent measurements. Ap index data is available for almost one century, thus the parametrisation is suitable for simulations of the recent climate.

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.

We have estimated changes in surface solar ultraviolet (UV) radiation under cloud free conditions in the 21st century based on simulations of 11 coupled Chemistry-Climate Models (CCMs). The total ozone columns and vertical profiles of ozone and temperature projected from CCMs were used as input to a radiative transfer model in order to calculate the corresponding erythemal irradiance levels. Time series of monthly erythemal irradiance received at the surface during local noon are presented for the period 1960 to 2100. Starting from the first decade of the 21st century, the surface erythemal irradiance decreases globally as a result of the projected stratospheric ozone recovery at rates that are larger in the first half of the 21st century and smaller towards its end. This decreasing tendency varies with latitude, being more pronounced over areas where stratospheric ozone has been depleted the most after 1980. Between 2000 and 2100 surface erythemal irradiance is projected to decrease over midlatitudes by 5 to 15%, while at the southern high latitudes the decrease is twice as much. In this study we have not included effects from changes in cloudiness, surface reflectivity and tropospheric aerosol loading, which will likely be affected in the future due to climate change. Consequently, over some areas the actual changes in future UV radiation may be different depending on the evolution of these parameters.

The GABRIEL airborne field measurement campaign, conducted over the Guyanas in October 2005, produced measurements of hydroxyl radical (OH) concentration which are significantly higher than can be simulated using current generation models of atmospheric chemistry. Based on the hypothesis that this "missing OH" is due to an as-yet undiscovered mechanism for recycling OH during the oxidation chain of isoprene, we determine that an OH recycling of about 40–50% (compared with 5–10% in current generation isoprene oxidation mechanisms) is necessary in order for our modelled OH to approach the lower error bounds of the OH observed during GABRIEL. Such a large amount of OH in our model leads to unrealistically low mixing ratios of isoprene. In order for our modelled isoprene mixing ratios to match those observed during the campaign, we also require that the effective rate constant for the reaction of isoprene with OH be reduced by about 50% compared with the lower bound of the range recommended by IUPAC. We show that a reasonable explanation for this lower effective rate constant could be the segregation of isoprene and OH in the mixed layer. Our modelling results are consistent with a global, annual isoprene source of about 500 Tg(C) yr−1, allowing experimentally derived and established isoprene flux rates to be reconciled with global models.

Glyoxal, the smallest dicarbonyl, which has recently been observed from space, is expected to provide indications on volatile organic compounds (VOC) oxidation and secondary aerosol formation in the troposphere. Glyoxal (CHOCHO) is known to be mostly of natural origin and is produced during biogenic VOC oxidation. However, a number of anthropogenically emitted hydrocarbons, like acetylene and aromatics, have been positively identified as CHOCHO precursors. The present study investigates the contribution of pollution to the CHOCHO levels by taking into account the secondary chemical formation of CHOCHO from precursors emitted from biogenic, anthropogenic and biomass burning sources. The impact of potential primary land emissions of CHOCHO is also investigated. A global 3-dimensional chemistry transport model of the troposphere (TM4-ECPL) able to simulate the gas phase chemistry coupled with all major aerosol components is used. The secondary anthropogenic contribution from fossil fuel and industrial VOCs emissions oxidation to the CHOCHO columns is found to reach 20–70% in the industrialized areas of the Northern Hemisphere and 3–20% in the tropics. This secondary CHOCHO source is on average three times larger than that from oxidation of VOCs from biomass burning sources. The chemical production of CHOCHO is calculated to equal to about 56 Tg y−1 with 70% being produced from biogenic hydrocarbons oxidation, 17% from acetylene, 11% from aromatic chemistry and 2% from ethene and propene. CHOCHO is destroyed in the troposphere primarily by reaction with OH radicals (23%) and by photolysis (63%), but it is also removed from the atmosphere through wet (8%) and dry deposition (6%). Potential formation of secondary organic aerosol through CHOCHO losses on/in aerosols and clouds is neglected here due to the significant uncertainties associated with the underlying chemistry. The global annual mean CHOCHO burden and lifetime in the model domain are estimated to be 0.02 Tg (equal to the global burden seen by SCIAMACHY over land for the year 2005) and about 3 h, respectively. The model results are compared with satellite observations of CHOCHO columns. When accounting only for the secondary sources of CHOCHO in the model, the model underestimates CHOCHO columns observed by satellites. This is attributed to an overestimate of CHOCHO sinks or a missing global source of about 20 Tg y−1. Using the current primary emissions of CHOCHO from biomass burning together with the anthropogenic combustion sources of about 7 Tg y−1 leads to an overestimate by the model over hot spot areas.

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.

The chemistry climate model ECHAM5/MESSy1 (E5/M1) in a setup extending from the surface to 80 km with a vertical resolution of about 600 m near the tropopause with nudged tropospheric meteorology allows a direct comparison with satellite data of chemical species at the same time and location. Here we present results out of a transient 10~years simulation for the period of the Antarctic vortex split in September 2002, where data of MIPAS on the ENVISAT-satellite are available. For the first time this satellite instrument opens the opportunity, to evaluate all stratospheric nitrogen containing species simultaneously with a good global coverage, including the source gas N2O and ozone which allows an estimate for NOx-production in the stratosphere. We show correlations between simulated and observed species in the altitude region between 10 and 50 hpa for different latitude belts, together with the Probability Density Functions (PDFs) of model results and observations. This is supplemented by global maps on pressure levels showing the comparison between the satellite and the simulated data sampled at the same time and location. We demonstrate that the model in most cases captures the partitioning in the nitrogen family, the diurnal cycles and the spatial distribution within experimental uncertainty. This includes even variations due to tropospheric clouds. There appears to be, however, a problem to reproduce the observed nighttime partitioning between N2O5 and NO2 in the middle stratosphere using the recommended set of reaction coefficients and photolysis data.

The mechanisms responsible for the extreme dryness of the stratosphere have been debated for decades. A key difficulty has been the lack of comprehensive models which are able to reproduce the observations. Here we examine results from the coupled lower-middle atmosphere chemistry general circulation model ECHAM5/MESSy1 together with satellite observations. Our model results match observed temperatures in the tropical lower stratosphere and realistically represent the seasonal and inter-annual variability of water vapor. The model reproduces the very low water vapor mixing ratios (below 2 ppmv) periodically observed at the tropical tropopause near 100 hPa, as well as the characteristic tape recorder signal up to about 10 hPa, providing evidence that the dehydration mechanism is well-captured. Our results confirm that the entry of tropospheric air into the tropical stratosphere is forced by large-scale wave dynamics, whereas radiative cooling regionally decelerates upwelling and can even cause downwelling. Thin cirrus forms in the cold air above cumulonimbus clouds, and the associated sedimentation of ice particles between 100 and 200 hPa reduces water mass fluxes by nearly two orders of magnitude compared to air mass fluxes. Transport into the stratosphere is supported by regional net radiative heating, to a large extent in the outer tropics. During summer very deep monsoon convection over Southeast Asia, centered over Tibet, moistens the stratosphere.

We report results from a multiple linear regression analysis of long-term total ozone observations (1979 to 2000, by TOMS/SBUV), of temperature reanalyses (1958 to 2000, NCEP), and of two chemistry-climate model simulations (1960 to 1999, by ECHAM4.L39(DLR)/CHEM (=E39/C), and MAECHAM4-CHEM). The model runs are transient experiments, where observed sea surface temperatures, increasing source gas concentrations (CO2, CFCs, CH4, N2O, NOx), 11-year solar cycle, volcanic aerosols and the quasi-biennial oscillation (QBO) are all accounted for. MAECHAM4-CHEM covers the atmosphere from the surface up to 0.01 hPa (≈80 km). For a proper representation of middle atmosphere (MA) dynamics, it includes a parametrization for momentum deposition by dissipating gravity wave spectra. E39/C, on the other hand, has its top layer centered at 10 hPa (≈30 km). It is targeted on processes near the tropopause, and has more levels in this region. Despite some problems, both models generally reproduce the observed amplitudes and much of the observed low-latitude patterns of the various modes of interannual variability in total ozone and lower stratospheric temperature. In most aspects MAECHAM4-CHEM performs slightly better than E39/C. MAECHAM4-CHEM overestimates the long-term decline of total ozone, whereas underestimates the decline over Antarctica and at northern mid-latitudes. The true long-term decline in winter and spring above the Arctic may be underestimated by a lack of TOMS/SBUV observations in winter, particularly in the cold 1990s. Main contributions to the observed interannual variations of total ozone and lower stratospheric temperature at 50 hPa come from a linear trend (up to -10 DU/decade at high northern latitudes, up to -40 DU/decade at high southern latitudes, and around -0.7 K/decade over much of the globe), from the intensity of the polar vortices (more than 40 DU, or 8 K peak to peak), the QBO (up to 20 DU, or 2 K peak to peak), and from tropospheric weather (up to 20 DU, or 2 K peak to peak). Smaller variations are related to the 11-year solar cycle (generally less than 15 DU, or 1 K), or to ENSO (up to 10 DU, or 1 K). These observed variations are replicated well in the simulations. Volcanic eruptions have resulted in sporadic changes (up to -30 DU, or +3 K). At low latitudes, patterns are zonally symmetric. At higher latitudes, however, strong, zonally non-symmetric signals are found close to the Aleutian Islands or south of Australia. Such asymmetric features appear in the model runs as well, but often at different longitudes than in the observations. The results point to a key role of the zonally asymmetric Aleutian (or Australian) stratospheric anti-cyclones for interannual variations at high-latitudes, and for coupling between polar vortex strength, QBO, 11-year solar cycle and ENSO.

The new Modular Earth Submodel System (MESSy) describes atmospheric chemistry and meteorological processes in a modular framework, following strict coding standards. It has been coupled to the ECHAM5 general circulation model, which has been slightly modified for this purpose. A 90-layer model setup up to 0.01 hPa was used at spectral T42 resolution to simulate the lower and middle atmosphere. With the high vertical resolution the model simulates the Quasi-Biennial Oscillation. The model meteorology has been tested to check the influence of the changes to ECHAM5 and the radiation interactions with the new representation of atmospheric composition. In the simulations presented here a Newtonian relaxation technique was applied in the tropospheric part of the domain to weakly nudge the model towards the analysed meteorology during the period 1998–2005. This allows an efficient and direct evaluation with satellite and in-situ data. It is shown that the tropospheric wave forcing of the stratosphere in the model suffices to reproduce major stratospheric warming events leading e.g. to the vortex split over Antarctica in 2002. Characteristic features such as dehydration and denitrification caused by the sedimentation of polar stratospheric cloud particles and ozone depletion during winter and spring are simulated well, although ozone loss in the lower polar stratosphere is slightly underestimated. The model realistically simulates stratosphere-troposphere exchange processes as indicated by comparisons with satellite and in situ measurements. The evaluation of tropospheric chemistry presented here focuses on the distributions of ozone, hydroxyl radicals, carbon monoxide and reactive nitrogen compounds. In spite of minor shortcomings, mostly related to the relatively coarse T42 resolution and the neglect of inter-annual changes in biomass burning emissions, the main characteristics of the trace gas distributions are generally reproduced well. The MESSy submodels and the ECHAM5/MESSy1 model output are available through the internet on request.

A transient simulation with the interactively coupled chemistry-climate model (CCM) E39/C has been carried out which covers the 40-year period between 1960 and 1999. Forcing of natural and anthropogenic origin is prescribed where the characteristics are sufficiently well known and the typical timescales are slow compared to synoptic timescale so that the simulated atmospheric chemistry and climate evolve under a 'slowly' varying external forcing. Based on observations, sea surface temperature (SST) and ice cover are prescribed. The increase of greenhouse gas and chlorofluorocarbon concentrations, as well as nitrogen oxide emissions are taken into account. The 11-year solar cycle is considered in the calculation of heating rates and photolysis of chemical species. The three major volcanic eruptions during that time (Agung, 1963; El Chichon, 1982; Pinatubo, 1991) are considered. The quasi-biennial oscillation (QBO) is forced by linear relaxation, also known as nudging, of the equatorial zonal wind in the lower stratosphere towards observed zonal wind profiles. Beyond a reasonable reproduction of mean parameters and long-term variability characteristics there are many apparent features of episodic similarities between simulation and observation: In the years 1986 and 1988 the Antarctic ozone holes are smaller than in the other years of that decade. In mid-latitudes of the Southern Hemisphere ozone anomalies resemble the corresponding observations, especially in 1985, 1989, 1991/1992, and 1996. In the Northern Hemisphere, the episode between the late 1980s and the first half of the 1990s is dynamically quiet, in particular, no stratospheric warming is found between 1988 and 1993. As observed, volcanic eruptions strongly influence dynamics and chemistry, though only for few years. Obviously, planetary wave activity is strongly driven by the prescribed SST and modulated by the QBO. Preliminary evidence of realistic cause and effect relationships strongly suggests that detailed process-oriented studies will be a worthwhile endeavour.

We have compared satellite and balloon observations of methane (CH4) and hydrogen fluoride (HF) during the Arctic winter 1999/2000 with results from the MA-ECHAM4 middle atmospheric general circulation model (GCM). For this purpose, the meteorology in the model was nudged towards ECMWF analyses. This nudging technique is shown to work well for this middle atmospheric model, and offers good opportunities for the simulation of chemistry and transport processes. However, caution must be used inside the polar vortex, particularly late in the winter. The current study focuses on transport of HF and CH4, initialized with satellite measurements from the HALOE instrument aboard the UARS satellite. We have compared the model results with HALOE data and balloon measurements throughout the winter, and analyzed the uncertainties associated with tracer initialization, boundary conditions and the passive tracer assumption. This comparison shows that the model represents some aspects of the Arctic vortex well, including relatively small-scale features. However, while profiles outside the vortex match observations well, the model underestimates HF and overestimates CH4 concentrations inside the vortex, particularly in the middle stratosphere. This problem is also evident in a comparison of vortex descent rates based upon vortex average tracer profiles from MA-ECHAM4, and various observations. This could be due to an underestimate of diabatic subsidence in the model, or due to too much mixing between vortex and non-vortex air.

Actinic fluxes at large solar zenith angles (SZAs) are important for atmospheric chemistry, especially under twilight conditions in polar winter and spring. The results of a sensitivity experiment employing the fully coupled 3D chemistry-climate model ECHAM4.L39(DLR)/CHEM have been analysed to quantify the impact of SZAs larger than 87.5º on dynamical and chemical processes in the lower stratosphere, in particular their influence on the ozone layer. Although the actinic fluxes at SZAs larger than 87.5º are small, ozone concentrations are significantly affected because daytime photolytic ozone destruction is switched on earlier, especially at the end of polar night the conversion of Cl2 and Cl2O2 into ClO in the lower stratosphere. Comparing climatological mean ozone column values of a simulation considering SZAs up to 93º with those of the sensitivity run with SZAs confined to 87.5º total ozone is reduced by about 20% in the polar Southern Hemisphere, i.e., the ozone hole is "deeper'' if twilight conditions are considered in the model because there is about 4 weeks more time for ozone destruction. This causes an additional cooling of the polar lower stratosphere (50 hPa) up to -4 K with obvious consequences for chemical processes. In the Northern Hemisphere the impact of large SZAs cannot be determined on the basis of climatological mean values due to the pronounced dynamic variability of the stratosphere in winter and spring. This study clearly shows the necessity of considering large SZAs for the calculation of photolysis rates in atmospheric 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.

The coupled climate-chemistry model ECHAM4.L39(DLR)/CHEM is presented which enables a simultaneous treatment of meteorology and atmospheric chemistry and their feedbacks. This is the first model which interactively combines a general circulation model with a chemical model, employing most of the important reactions and species necessary to describe the stratospheric and upper tropospheric ozone chemistry, and which is computationally fast enough to allow long-term integrations with currently available computer resources. This is possible as the model time-step used for the chemistry can be chosen as large as the integration time-step for the dynamics. Vertically the atmosphere is discretized by 39 levels from the surface up to the top layer which is centred at 10 hPa, with a relatively high vertical resolution of approximately 700 m near the extra-tropical tropopause. We present the results of a control simulation representing recent conditions (1990) and compare it to available observations. The focus is on investigations of stratospheric dynamics and chemistry relevant to describe the stratospheric ozone layer. ECHAM4.L39(DLR)/CHEM reproduces main features of stratospheric dynamics in the arctic vortex region, including stratospheric warming events. This constitutes a major improvement compared to earlier model versions. However, apparent shortcomings in Antarctic circulation and temperatures persist. The seasonal and interannual variability of the ozone layer is simulated in accordance with observations. Activation and deactivation of chlorine in the polar stratospheric vortices and their inter-hemispheric differences are reproduced. Considering methane oxidation as part of the dynamic-chemistry feedback results in an improved representation of the spatial distribution of stratospheric water vapour concentrations. The current model constitutes a powerful tool to investigate, for instance, the combined direct and indirect effects of anthropogenic trace gas emissions.Key words. Atmospheric composition and structure (middle atmosphere – composition and chemistry) – Meteorology and atmospheric dynamics (general circulation; middle atmosphere dynamics)

Severe chemical ozone loss has been detected in the Arctic in the winter and spring of 1995-96 by a variety of methods. Extreme reductions in column ozone due to halogen catalysed chemistry were derived from measurements of the Halogen Occultation Experiment (HALOE) on board the Upper Atmosphere Research Satellite in the Arctic vortex. Here, we discuss further aspects of the HALOE observations in the Arctic over this period. Potential problems, both in the data themselves and in the methodology of the data analysis are considered and the reason for the differences between the Arctic ozone losses deduced from HALOE data version 17 and 18 is analysed. Moreover, it is shown that HALOE measurements in the Arctic in winter and spring 1995-96 compare well with observations by other ground-based and satellite instruments.Key words. Chemical ozone loss (Arctic vortex 1995 · 96; halogen chemistry)

The comprehensive chemistry module CHEM has been developed for application in general circulation models (GCMs) describing tropospheric and stratospheric chemistry, including photochemical reactions and heterogeneous reactions on sulphate aerosols and polar stratospheric clouds. It has been coupled to the spectral atmospheric GCM ECHAM3. The model configuration used in the current study has been run in an "off-line" mode, i.e. the calculated chemical species do not affect the radiative forcing of the dynamic fields. First results of a 15-year model integration indicate that the model ECHAM3/CHEM runs are numerically efficient and stable, i.e. that no model drift can be detected in dynamic and chemical parameters. The model reproduces the main features regarding ozone, in particular intra- and interannual variability. The ozone columns are somewhat higher than observed (approximately 10%), while the amplitude of the annual cycle is in agreement with observations. A comparison with HALOE data reveals, however, a serious model deficiency regarding lower-stratosphere dynamics at high latitudes. Contrary to what is concluded by observations, the lower stratosphere is characterized by slight upward motions in the polar regions, so that some of the mentioned good agreements must be considered as fortuitous. Nevertheless, ECHAM3/CHEM well describes the chemical processes leading to ozone reduction. It has been shown that the mean fraction of the northern hemisphere, which is covered by polar stratospheric clouds (PSCs) as well as the temporal appearance of PSCs in the model, is in fair agreement with observations. The model results show an activation of chlorine inside the polar vortex which is stronger in the southern than in the northern winter hemisphere, yielding an ozone hole over the Antarctic; this hole, however, is also caused to a substantial degree by the dynamics. Interhemispheric differences concerning reformation of chlorine reservoir species HCl and ClONO2 in spring have also been well reproduced by the model.Key words. Atmospheric composition and structure · Middle atmosphere · Meteorology and atmospheric dynamics · Climatology · General circulation

The representation of the Tropical Tropopause Layer in 13 different Chemistry Climate Models designed to represent the stratosphere is analyzed. Simulations for 1960-present and 1980-2100 are analyzed and compared to reanalysis model output. Results indicate that the models are able to reproduce the basic structure of the TTL. There is a large spread in cold point tropopause temperatures that may be linked to variation in TTL ozone values. The models are generally able to reproduce historical trends in tropopause pressure obtained from reanalysis products. Simulated historical trends in cold point tropopause temperatures and in the meridional extent of the TTL are not consistent across models. The pressure of both the tropical tropopause and the level of main convective outflow appear to be decreasing (increasing altitude) in historical runs. Similar trends are seen in the future. Models consistently predict decreasing tropopause and convective outflow pressure, by several hPa/decade. Tropical cold point temperatures increase by 0.2 K/decade. This indicates that tropospheric warming dominates stratospheric cooling at the tropical tropopause. Stratospheric water vapor at 100 hPa increases by up to 0.5-1 ppmv by 2100. This is less than implied directly by the temperature and methane increases, highlighting the correlation of tropopause temperatures with stratospheric water vapor, but also the complex nature of TTL transport. [ABSTRACT FROM AUTHOR]