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This study developed a next‐generation atmospheric aerosol/chemistry‐climate model, the BCC_AGCM_CUACE2.0. Then, the performance of the model for nitrate was evaluated, and the nitrate direct radiative forcing (DRF) and effective radiative forcing (ERF) due to aerosol‐radiation interactions were simulated for the present day (2010), near‐term future (2030), and middle‐term future (2050) under the Representative Concentration Pathway 4.5, 6.0, and 8.5 scenarios relative to the preindustrial era (1850). The model reproduced the distributions and seasonal changes in nitrate loading well, and simulated surface concentrations matched observations in Europe, North America, and China. Current global mean annual loading of nitrates was predicted to increase by 1.50 mg m−2 relative to 1850, with the largest increases occurring in East Asia (9.44 mg m−2), Europe (4.36 mg m−2), and South Asia (3.09 mg m−2). The current global mean annual ERF of nitrates was −0.28 W m−2 relative to 1850. Due to global reductions in pollutant emissions, the nitrate ERF values were predicted to decrease to −0.17, −0.20, and −0.24 W m−2 in 2030 and −0.07, −0.18, and −0.19 W m−2 in 2050 for Representative Concentration Pathway 4.5, 6.0, and 8.5 relative to 1850, respectively. Although global mean nitrate values showed a declining trend, future nitrate loading remained high in East Asia and South Asia.

With the gradual yet unequivocal phasing out of ozone depleting substances (ODSs), the environmental crisis caused by the discovery of an ozone hole over the Antarctic has lessened in severity and a promising recovery of the ozone layer is predicted in this century. However, strong volcanic activity can also cause ozone depletion that might be severe enough to threaten the existence of life on Earth. In this study, a transport model and a coupled chemistry-climate model were used to simulate the impacts of super volcanoes on ozone depletion. The volcanic eruptions in the experiments were the 1991 Mount Pinatubo eruption and a 100 × Pinatubo size eruption. The results show that the percentage of global mean total column ozone depletion in the 2050 RCP8.5 100 × Pinatubo scenario is approximately 6% compared to two years before the eruption and 6.4% in tropics. An identical simulation, 100 × Pinatubo eruption only with natural source ODSs, produces an ozone depletion of 2.5% compared to two years before the eruption, and with 4.4% loss in the tropics. Based on the model results, the reduced ODSs and stratospheric cooling lighten the ozone depletion after super volcanic eruption.

In the extratropical atmosphere, Rossby waves (RWs) and internal gravity waves (GWs) propagating from the troposphere mediate a coupling with the middle atmosphere by influencing the dynamics herein. In the current generation chemistry-climate models (CCMs), RW effects are well resolved while GW effects have to be parameterized. Here, we analyze orographic GW (OGW) interaction with resolved dynamics in a comprehensive CCM on the time scale of days. For this, we apply a recently developed method of strong OGW drag event composites for the three strongest northern hemisphere OGW hotspots. We show that locally-strong OGW events considerably alter the properties of resolved wave propagation into the middle atmosphere, which subsequently influences zonal winds and RW transience. Our results demonstrate that the influence of OGWs is critically dependent on the hotspot region, which underlines the OGW-resolved dynamics interaction being a two-way process.

Reconstructions of volcanic aerosol forcing and its climatic impacts are undermined by uncertainties in both the models used to build these reconstructions as well as the proxy and observational records used to constrain those models. Reducing these uncertainties has been a priority and in particular, several modelling groups have developed interactive stratospheric aerosol models. Provided with an initial volcanic injection of sulfur dioxide, these models can interactively simulate the life cycle and optical properties of sulfate aerosols, and their effects on climate. In contrast, most climate models that took part in the Coupled Model Intercomparison Project Phase 5 and 6 (CMIP6) directly prescribe perturbations in atmospheric optical properties associated with an eruption. However, before the satellite era, the volcanic forcing dataset used for CMIP6 mostly relies on a relatively simple aerosol model and a volcanic sulfur inventory derived from ice-cores, both of which have substantial associated uncertainties.In this study, we produced a new set of historical simulations using the UK Earth System Model UKESM1, with interactive stratospheric aerosol capability (referred to as interactive runs hereafter) instead of directly prescribing the CMIP6 volcanic forcing dataset as was done for CMIP6 (standard runs, hereafter). We used one of the most recent volcanic sulfur inventories as input for the interactive runs, in which aerosol properties are consistent with the model chemistry, microphysics and atmospheric components. We analyzed how the stratospheric aerosol optical depth, the radiative forcing and the climate response to volcanic eruptions differed between interactive and standard runs, and how these compare to observations and proxy records. In particular, we investigate in detail the differences in the response to the large-magnitude Krakatoa 1883 eruption between the two sets of runs. We also discuss differences for the 1979-2015 period where the forcing data in standard runs is directly constrained from satellite observations. Our results shed new light on uncertainties affecting the reconstruction of past volcanic forcing and highlight some of the benefits and disadvantages of using interactive stratospheric aerosol capabilities instead of a unique prescribed volcanic forcing dataset in CMIP’s historical runs.

Methane (CH4), the second most important greenhouse gas in terms of radiative forcing, is on the rise; but there are extensive opportunities for mitigation with existing technologies. Anthropogenic emissions account for around 60% of the global methane source, and the recent atmospheric methane growth rate puts us on a trajectory comparable to the most extreme future methane scenarios in the sixth Coupled Model Intercomparison Project (CMIP6). We use a new methane emissions-driven configuration of the UK Earth System Model (UKESM1) to explore the role of anthropogenic methane in the earth system. The full methane cycle is represented, including surface deposition, chemistry and interactive wetland emissions. As a baseline scenario we used Shared Socioeconomic Pathway 3-7.0 (SSP3-7.0) – the highest methane emissions scenario in CMIP6. In an idealised experiment, all anthropogenic methane emissions were instantaneously stopped from 2015 onwards in a coupled atmosphere-ocean simulation running from 2015-2050, to make a net-zero anthropogenic methane emissions scenario. Within a decade, significant changes can be seen in atmospheric composition and climate, compared to SSP3-7.0. The atmospheric methane burden declines to below pre-industrial levels within 12 years, and by the late 2030s reaches a constant level around 44% below that of the present day (2015). The tropospheric ozone burden and surface mean ozone concentrations decreased by 12% and 15% respectively by 2050 – key in terms of limiting global warming as well as improving air quality and human health. By 2050 the net-zero anthropogenic methane scenario results in a global mean surface temperature (GMST) 1˚C lower than the baseline, a significant value in the context of climate goals such as the Paris Agreement. Through decomposition of the radiation budget, the change in climate can be directly attributed to the reduction in methane and indirectly to the resulting changes in ozone, clouds and ozone precursors such as CO. In addition, the changes in climate result in impacts on the interactive wetland emissions via changes in temperature and wetland extent, highlighting the coupled nature of methane in the earth system. Cessation of anthropogenic methane emissions has profound impacts on near-term warming and on tropospheric ozone, but ultimately cannot single-handedly achieve the necessary reductions for meeting Paris goals.

We present the first results of modelling of the short-living cosmogenic isotope 7Be production, deposition, and transport using the chemistry-climate model SOCOLv3.0 aimed to study solar-terrestrial interactions and climate changes. We implemented an interactive deposition scheme, based on gas tracers with and without nudging to the known meteorological fields. Production of 7Be was modelled using the 3D time-dependent Cosmic Ray induced Atmospheric Cascade (CRAC) model. The simulations were compared with the real concentrations (activity) and depositions measurements of 7Be in the air and water at Finnish stations. We have successfully reproduced and estimated the variability of the cosmogenic isotope 7Be produced by the galactic cosmic rays (GCR) on time scales longer than about a month, for the period of 2002–2008. The agreement between the modelled and measured data is very good (within 12%) providing a solid validation for the ability of the SOCOL CCM to reliably model production, transport, and deposition of cosmogenic isotopes, which is needed for precise studies of cosmic-ray variability in the past.

10 pags., 4 figs., Many Chemistry-Climate Models (CCMs) include a simplified treatment of brominated very short-lived (VSL) species by assuming CHBr as a surrogate for VSL. However, neglecting a comprehensive treatment of VSL in CCMs may yield an unrealistic representation of the associated impacts. Here, we use the Community Atmospheric Model with Chemistry (CAM-Chem) CCM to quantify the tropospheric and stratospheric changes between various VSL chemical approaches with increasing degrees of complexity (i.e., surrogate, explicit, and full). Our CAM-Chem results highlight the improved accuracy achieved by considering a detailed treatment of VSL photochemistry, including sea-salt aerosol dehalogenation and heterogeneous recycling on ice-crystals. Differences between the full and surrogate schemes maximize in the lowermost stratosphere and midlatitude free troposphere, resulting in a latitudinally dependent reduction of ∼1–7 DU in total ozone column and a ∼5%–15% decrease of the OH/HO ratio. We encourage all CCMs to include a complete chemical treatment of VSL in the troposphere and stratosphere., This study has been funded by the European Union's Horizon 2020 Re-search and Innovation program (Project ‘ERC-2016-COG 726349 CLIMAHAL’), and supported by the Consejo Superior de Investigaciones Científicas of Spain. Computing resources and support are provided by the Computational and Information System Laboratory (CISL,2017). R. P. Fernandez would like to thank financial support from CONICET, ANPCyT (PICT 2015-0714), UNCuyo (SeCTyP M032/3853) and UTN (PID 4920-194/2018). NCAR is sponsored by NSF under grant number 1852977. R. J. Salawitch appreciates support from the NASA (grant ACMP 80NSSC19K0983). The authors thank two anonymous reviewers for their constructive comments

We describe the baseline model configuration and simulation characteristics of the Geophysical Fluid Dynamics Laboratory (GFDL)'s Atmosphere Model version 4.1 (AM4.1), which builds on developments at GFDL over 2013–2018 for coupled carbon‐chemistry‐climate simulation as part of the sixth phase of the Coupled Model Intercomparison Project. In contrast with GFDL's AM4.0 development effort, which focused on physical and aerosol interactions and which is used as the atmospheric component of CM4.0, AM4.1 focuses on comprehensiveness of Earth system interactions. Key features of this model include doubled horizontal resolution of the atmosphere (~200 to ~100 km) with revised dynamics and physics from GFDL's previous‐generation AM3 atmospheric chemistry‐climate model. AM4.1 features improved representation of atmospheric chemical composition, including aerosol and aerosol precursor emissions, key land‐atmosphere interactions, comprehensive land‐atmosphere‐ocean cycling of dust and iron, and interactive ocean‐atmosphere cycling of reactive nitrogen. AM4.1 provides vast improvements in fidelity over AM3, captures most of AM4.0's baseline simulations characteristics, and notably improves on AM4.0 in the representation of aerosols over the Southern Ocean, India, and China—even with its interactive chemistry representation—and in its manifestation of sudden stratospheric warmings in the coldest months. Distributions of reactive nitrogen and sulfur species, carbon monoxide, and ozone are all substantially improved over AM3. Fidelity concerns include degradation of upper atmosphere equatorial winds and of aerosols in some regions.

We report airborne measurements of acetaldehyde (CH(3)CHO) during the first and second deployments of the National Aeronautics and Space Administration (NASA) Atmospheric Tomography Mission (ATom). The budget of CH(3)CHO is examined using the Community Atmospheric Model with chemistry (CAM-chem), with a newly-developed online air-sea exchange module. The upper limit of the global ocean net emission of CH(3)CHO is estimated to be 34 Tg a(−1) (42 Tg a(−1) if considering bubble-mediated transfer), and the ocean impacts on tropospheric CH(3)CHO are mostly confined to the marine boundary layer. Our analysis suggests that there is an unaccounted CH(3)CHO source in the remote troposphere and that organic aerosols can only provide a fraction of this missing source. We propose that peroxyacetic acid (PAA) is an ideal indicator of the rapid CH(3)CHO production in the remote troposphere. The higher-than-expected CH(3)CHO measurements represent a missing sink of hydroxyl radicals (and halogen radical) in current chemistry-climate models.

With low concentrations of tropospheric aerosol, the Southern Ocean offers a "natural laboratory" for studies of aerosol–cloud interactions. Aerosols over the Southern Ocean are produced from biogenic activity in the ocean, which generates sulfate aerosol via dimethylsulfide (DMS) oxidation, and from strong winds and waves that lead to bubble bursting and sea spray emission. Here, we evaluate the representation of Southern Ocean aerosols in the Hadley Centre Global Environmental Model version 3, Global Atmosphere 7.1 (HadGEM3-GA7.1) chemistry–climate model. Compared with aerosol optical depth (AOD) observations from two satellite instruments (the Moderate Resolution Imaging Spectroradiometer, MODIS-Aqua c6.1, and the Multi-angle Imaging Spectroradiometer, MISR), the model simulates too-high AOD during winter and too-low AOD during summer. By switching off DMS emission in the model, we show that sea spray aerosol is the dominant contributor to AOD during winter. In turn, the simulated sea spray aerosol flux depends on near-surface wind speed. By examining MODIS AOD as a function of wind speed from the ERA-Interim reanalysis and comparing it with the model, we show that the sea spray aerosol source function in HadGEM3-GA7.1 overestimates the wind speed dependency. We test a recently developed sea spray aerosol source function derived from measurements made on a Southern Ocean research voyage in 2018. In this source function, the wind speed dependency of the sea spray aerosol flux is less than in the formulation currently implemented in HadGEM3-GA7.1. The new source function leads to good agreement between simulated and observed wintertime AODs over the Southern Ocean; however, it reveals partially compensating errors in DMS-derived AOD. While previous work has tested assumptions regarding the seawater climatology or sea–air flux of DMS, we test the sensitivity of simulated AOD, cloud condensation nuclei and cloud droplet number concentration to three atmospheric sulfate chemistry schemes. The first scheme adds DMS oxidation by halogens and the other two test a recently developed sulfate chemistry scheme for the marine troposphere; one tests gas-phase chemistry only, while the second adds extra aqueous-phase sulfate reactions. We show how simulated sulfur dioxide and sulfuric acid profiles over the Southern Ocean change as a result and how the number concentration and particle size of the soluble Aitken, accumulation and coarse aerosol modes are affected. The new DMS chemistry scheme leads to a 20% increase in the number concentration of cloud condensation nuclei and cloud droplets, which improves agreement with observations. Our results highlight the importance of atmospheric chemistry for simulating aerosols and clouds accurately over the Southern Ocean.

An important source of polar stratospheric clouds (PSCs), which play a crucial role in controlling polar stratospheric ozone depletion, is from the temperature fluctuations induced by mountain waves, enabling stratospheric temperatures to fall below the threshold value for PSC formation in the cold phases of these waves even if the synoptic-scale temperatures are too high. However, this formation mechanism is usually missing in chemistry–climate models because these temperature fluctuations are neither resolved nor parameterised. Here, we investigate the representation of parameterised stratospheric mountain-wave-induced temperature fluctuations over the Antarctic Peninsula from a 30-year run of the global chemistry-climate configuration of the UM-UKCA model against climatologies of Atmospheric Infrared Sounder (AIRS) radiance measurements and high-resolution radiosonde temperature soundings from Rothera. The results demonstrate that the local mountain wave-induced cooling phases computed by the scheme are in relatively good agreement with both sets of observations. For example, the scheme is able to capture the observed probability distribution of the temperature fluctuations, particularly the cold tails of the distribution that are critical for exceeding the temperature threshold for PSC formation. Further analysis shows that the increased stratospheric cooling induced by the scheme results in a large increase in total PSC ‘pseudo-volume’ of the area over the Antarctic Peninsula where the model temperature exceeds the temperature threshold of formation of PSCs.

The organic aerosols (OA) contribute significantly to fine particulate mass in the atmosphere, however, most global climate models do not include elaborate treatment associated with the production of secondary organic aerosols (SOA) involving complex chemical processes to save computational time. As a result, the concentrations of SOA simulated by these climate models are often highly uncertain. Moreover, very limited research has been done on SOA and its precursors, particularly on the contribution of individual sources towards the SOA concentrations across India. In this study, we investigate the sensitivity of the production of SOA from different VOC sources and different atmospheric oxidants by the Community Atmospheric Model version 4 coupled with an extensive interactive atmospheric chemistry module (CAM4-Chem). The main objective of our present research is to understand the contribution of individual sources of VOCs towards the production and distribution of SOA across the Indian region. We carried out a series of systematically designed simulations using the CAM4-Chem model to understand the sensitivity of simulated SOA over the Indian region to changes in only emissions of VOCs from anthropogenic, biogenic, and biomass burning emissions from preindustrial (PI) to present-day (PD) period. In order to avoid the influence of changes in meteorology from PI to PD on the production of SOA, all simulations are performed for the same period from 2004 to 2014 with identical meteorology prescribed to the model based on MERRA2 data, while the VOC emissions from anthropogenic, biogenic, and biomass burning sources are allowed to change from PI to PD in different simulations. Our results show that the simulated distribution of SOA over the Indian region in PD is linked to the significant changes in the emissions of VOCs from anthropogenic, biogenic, and biomass burning emissions sources from PI to PD. We find that the changes in emissions of VOCs from biogenic sources from PI to PD associated with land use and land cover changes contribute significantly along with the changes in emissions from anthropogenic sources towards the total changes in SOA distribution over the Indian region over the same period. The global annual mean burden of SOA from our sensitivity simulations vary in the range of 0.65Tg to 0.80Tg due to variations in emission of different VOCs that are precursors to the production of SOA in the atmosphere. These sensitivity simulations improve our understanding of atmospheric chemistry and specifically about the formation of SOA from different precursor gases originating from diverse anthropogenic, biogenic, and biomass burning emissions sources. More results with greater detail will be presented.

Urban areas are recognised as a significant source of greenhouse gas emissions (GHG), such as carbon dioxide (CO2) and methane (CH4). The total amount of urban GHG emissions, especially for CH4, however, is not well quantified. Here we report on airborne in situ measurements using a Picarro G1301-m analyser aboard the DLR Cessna Grand Caravan to study GHG emissions downwind of the German capital city Berlin. In total, five aircraft-based mass balance experiments were conducted in July 2018 within the Urban Climate Under Change [UC]2 project. The detection and isolation of the Berlin plume was often challenging because of comparatively small GHG signals above variable atmospheric background concentrations. However, on July 20th enhancements of up to 4 ppm CO2 and 21 ppb CH4 were observed over a horizontal extent of roughly 45 to 65 km downwind of Berlin. These enhanced mixing ratios are clearly distinguishable from the background and can partly be assigned to city emissions. The estimated CO2 emission flux of 1.39 ± 0.75 t s-1 is in agreement with current inventories, while the CH4 emission flux of 5.20 ± 1.61 kg s-1 is almost two times larger than the highest reported value in the inventories. We localized the source area with HYSPLIT trajectory calculations and the high resolution numerical model MECO(n) (down to ~1 km), and investigated the contribution from sewage-treatment plants and waste deposition to CH4, which are treated differently by the emission inventories. Our work highlights the importance of a) strong CH4 sources in the surroundings of Berlin and b) a detailed knowledge of GHG inflow mixing ratios to suitably estimate emission rates.

We have found distinct long-period changes in erythemal UV radiation (Qer) characterized by a pronounced decrease at the end of the 1970s and a statistically significant positive trend of more than 5%/10 years since 1979 over the territory of the Moscow region according to the measurements and reconstruction model. The positive Qer trend is shown to be associated mainly with a decrease in the effective cloud amount and total ozone content (TOC). Due to these variations, UV resources have significantly changed in spring for the population with the most vulnerable skin type I, which means a transition from the UV optimum to UV moderate excess conditions. The simulation experiments using the INM-RSHU chemistry climate model (CCM) for several scenarios with and without anthropogenic factors have revealed that the variations in the anthropogenic emissions of halogens have the most significant impact on the variability of TOC and Qer. Among natural factors, noticeable effects are observed due to volcanic aerosol. The calculations of the cloud transmittance of Qer are generally consistent with the measurements; however, they do not reproduce the observed value of the positive trend.

Ozone loss pathways and their rates in the ozone quasi-biennial oscillation (QBO), which is simulated by a chemistry-climate model developed by the Meteorological Research Institute of Japan, are evaluated using an ob- jective pathway analysis program (PAP). The analyzed chemical system contains catalytic cycles caused by NOx , HOx , ClOx , Ox , and BrOx . PAP quantified the rates of all significant catalytic ozone loss cycles, and evaluated the partitioning among these cycles. The QBO amplitude of the sum of all cycles amounts to about 4 and 14 % of the annual mean of the total ozone loss rate at 10 and 20 hPa, respectively. The contribution of catalytic cycles to the QBO of the ozone loss rate is found to be as follows: NOx cycles contribute the largest fraction (50 – 85 %) of the QBO amplitude of the total ozone loss rate; HOx cycles are the second-largest (20 – 30 %) below 30 hPa and the third-largest (about 10 %) above 20 hPa; Ox cycles rank third (5 – 20 %) below 30 hPa and second (about 20 %) above 20 hPa; ClOx cycles rank fourth (5 – 10 %); and BrOx cycles are almost negligible. The relative contribution of the NOx and Ox cycles to the QBO amplitude of ozone loss differs by up to 10 % and 20 %, respectively, from their contribution to the annual mean ozone loss rate. The ozone QBO at 20 hPa is mainly driven by ozone transport, which then alters the ozone loss rate. In contrast, the ozone QBO at 10 hPa is driven chemically by NOx and the temperature dependence of [O]/[O3], which results from the temperature dependence of the reaction O + O2 + M → O3 + M. In addition, the ozone QBO at 10 hPa is influenced by the overhead ozone column, which affects [O]/[O3] (through ozone photolysis) and the ozone production rate (through oxygen photolysis).

Specified dynamics (SD) schemes relax the circulation in climate models toward a reference meteorology to simulate historical variability. These simulations are widely used to isolate the dynamical contributions to variability and trends in trace gas species. However, it is not clear if trends in the stratospheric overturning circulation are properly reproduced by SD schemes. This study assesses numerous SD schemes and modeling choices in the Community Earth System Model (CESM) Whole Atmosphere Chemistry Climate Model (WACCM) to determine a set of best practices for reproducing interannual variability and trends in tropical stratospheric upwelling estimated by reanalyses. Nudging toward the reanalysis meteorology as is typically done in SD simulations expectedly changes the model’s mean upwelling compared to its free-running state, but does not accurately reproduce upwelling trends present in the underlying reanalysis. In contrast, nudging to anomalies from the climatological winds or from the zonal mean winds and temperatures preserves WACCM’s climatology and better reproduces trends in stratospheric upwelling. An SD scheme’s performance in simulating the acceleration of the shallow branch of the mean meridional circulation from 1980–2017 hinges on its ability to simulate the downward shift of subtropical lower stratospheric wave momentum forcing. Key to this is not nudging the zonal-mean temperature field. Gravity wave momentum forcing, which drives a substantial fraction of the upwelling in WACCM, cannot be constrained by nudging and presents an upper-limit on the performance of these schemes.

31 pags., 12 figs., 6 tabs. -- Open Access funded by Creative Commons Atribution Licence 4.0. -- jame20925-sup-0001_Supporting_Information.pdf, Current chemistry climate models do not include polar emissions and chemistry of halogens. This work presents the first implementation of an interactive polar module into the very short-lived (VSL) halogen version of the Community Atmosphere Model with Chemistry (CAM-Chem) model. The polar module includes photochemical release of molecular bromine, chlorine, and interhalogens from the sea-ice surface, and brine diffusion of iodine biologically produced underneath and within porous sea-ice. It also includes heterogeneous recycling of inorganic halogen reservoirs deposited over fresh sea-ice surfaces and snow-covered regions. The polar emission of chlorine, bromine, and iodine reach approximately 32, 250, and 39 Gg/year for Antarctica and 33, 271, and 4 Gg/year for the Arctic, respectively, with a marked seasonal cycle mainly driven by sunlight and sea-ice coverage. Model results are validated against polar boundary layer measurements of ClO, BrO, and IO, and satellite BrO and IO columns. This validation includes satellite observations of IO over inner Antarctica for which an iodine “leapfrog” mechanism is proposed to transport active iodine from coastal source regions to the interior of the continent. The modeled chlorine and bromine polar sources represent up to 45% and 80% of the global biogenic VSL and VSL emissions, respectively, while the Antarctic sea-ice iodine flux is ~10 times larger than that from the Southern Ocean. We present the first estimate of the contribution of polar halogen emissions to the global tropospheric halogen budget. CAM-Chem includes now a complete representation of halogen sources and chemistry from pole-to-pole and from the Earth's surface up to the stratopause., This study has been funded by the European Research Council Executive Agency under the European Union′s Horizon 2020 Research and Innovation program (Project “ERC‐2016‐COG 726349 CLIMAHAL”) and supported by the Consejo Superior de Investigaciones Científicas (CSIC) of Spain. Computing resources, support, and data storage are provided and maintained by the Computational and Information System Laboratory from the National Center of Atmospheric Research (CISL,2017). R. P. F. would like to thank CONICET, ANPCyT (PICT 2015‐0714), UNCuyo (SeCTyP M032/3853), and UTN (PID 4920‐194/2018) for the financial support. Partial funding for this work was provided by the Korea Polar Research Institute (KOPRI) project (PE18200). The contributions of the University of Bremen have been supported by the State of Bremen, the German Research Foundation (DFG), the German Aerospace (DLR), and the European Space Agency (ESA). We gratefully acknowledge the funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) —Projektnummer 268020496—TRR 172, within the Transregional Collaborative Research Center “ArctiC Amplification: Climate Relevant Atmospheric and SurfaCe Processes,and Feedback Mechanisms (AC)3 ” in subproject C03 as well as the support by the University of Bremen Institutional Strategy Measure M8 in the framework of the DFG Excellence Initiative.

We use the Goddard Earth Observing System Chemistry-Climate Model (GEOSCCM), a contributor to both the 2010 and 2014 WMO Ozone Assessment Reports, to show that inclusion of 5 parts per trillion (ppt) of stratospheric bromine (Bry) from very short-lived substances (VSLS) is responsible for about a decade delay in ozone hole recovery. These results partially explain the significantly later recovery of Antarctic ozone noted in the 2014 report, as bromine from VSLS was not included in the 2010 Assessment. We show multiple lines of evidence that simulations that account for VSLS Bry are in better agreement with both total column BrO and the seasonal evolution of Antarctic ozone reported by the Ozone Monitoring Instrument (OMI) on NASA's Aura satellite. In addition, the near zero ozone levels observed in the deep Antarctic lower stratospheric polar vortex are only reproduced in a simulation that includes this Bry source from VSLS.

To achieve better agreement of simulated Arctic winter stratospheric dynamic with observations assimilation procedure nudging was incorporated in CCM SOCOL. Trajectories based on SOCOL output winds demonstrate the reasonable agreement with trajectories based on reanalysis data inside the polar vortex and can be used for analysis and forecast of ozone related processes in winter-spring seasons. Obtained results of several recent major Arctic SSW events analysis show that CCM SOCOL could be used for SSW forecast over the period up to 8 days.

Primary biological aerosol particles (PBAPs) may impact human health and aerosol-climate interactions. The role of PBAPs in the earth system is associated with large uncertainties, related to source estimates and atmospheric transport. We used a chemistry-climate model to simulate PBAPs in the atmosphere including bacteria, fungal spores and pollen. Three fungal spore emission parameterizations have been evaluated against an updated set of spore counts synthesized from observations reported in the literature. The comparison indicates an optimal fit for the emission parameterization proposed by Heald and Spracklen (2009), although the model significantly over-predicts PBAP concentrations in some locations. Additional evaluation was performed by comparing our combined bacteria and fungal spore simulations to a global dataset of fluorescent biological aerosol particle (FBAP) concentrations. The model predicts the sum total of measured PBAP concentrations relatively well, with an over- or under-prediction of less than a factor of 2 compared to FBAP. The ratio of bacteria to fungal spores reflects a greater difference, however, and the simulated bacteria concentrations outnumber the simulated fungal spore concentrations in almost all locations. Further, the modeled fungal spore results under-predict the FBAP concentrations, which are used here as a rough proxy for spores. Uncertainties related to technical aspects of the FBAP and direct-counting spore measurements challenge the ability to further refine quantitative comparison on this scale. We estimate that the global PBAPs mass concentration (apart from desert dust and sea salt aerosols), i.e. of fungal spores and pollen, amounts to 19 % and 52 % of the total aerosol mass, respectively.

Bromine from very short lived substances (VSLS), primarily from natural oceanic sources, contributes substantially to the stratospheric bromine loading. This source of stratospheric bromine has so far been ignored in most chemistry climate model calculations of stratospheric ozone trends. Here we present a transient simulation with the chemistry climate model EMAC for the period 1960–2005 including emissions of the five brominated VSLS CHBr3, CH2Br2, CH2BrCl, CHBrCl2, and CHBr2Cl. The emissions lead to a realistic stratospheric bromine loading of about 20 pptv for present-day conditions. Comparison with a standard model simulation without VSLS shows large differences in modeled ozone in the extratropical lowermost stratosphere and in the troposphere. Differences in ozone maximize in the Antarctic Ozone Hole, resulting in more than 20% less ozone when VSLS are included. Even though the emissions of VSLS are assumed to be constant in time, the model simulation with VSLS included shows a much larger ozone decrease in the lowermost stratosphere during the 1979–1995 period and a faster ozone increase during 1996–2005, in better agreement with observed ozone trends than the standard simulation without VSLS emissions.

Within the framework of the global chemistry climate model ECHAM-HAMMOZ a novel explicit coupling between the sectional aerosol model HAM-SALSA and the chemistry model MOZ was established to form isoprene derived secondary organic aerosol (iSOA). Isoprene oxidation in the chemistry model MOZ is described by a semi-explicit scheme consisting of 147 reactions, embedded in a detailed atmospheric chemical mechanism with a total of 779 reactions. Low volatile compounds (LVOC) produced during isoprene photooxidation are identified and explicitly partitioned by HAM-SALSA. A group contribution method was used to estimate their evaporation enthalpies and corresponding saturation vapor pressures, which are used by HAM-SALSA to calculate the saturation concentration of each LVOC. With this method, every single precursor is tracked in terms of condensation and evaporation in each aerosol size bin. This approach lead to the identification of ISOP(OOH)2 as a main contributor to iSOA formation. Further, reactive uptake of isoprene epoxidiols (IEPOX) and isoprene derived glyoxal were included as iSOA sources. The parameterization of IEPOX reactive uptake includes a dependency on aerosol pH value. This model framework connecting semi-explicit isoprene oxidation with explicit treatment of aerosol tracers leads to a global, annual isoprene SOA yield of 16 % relative to the primary oxidation of isoprene by OH, NO3, and ozone. With 445 Tg (392 TgC) isoprene emitted, an iSOA source of 148 Tg (61 TgC) is simulated. The major part of iSOA in ECHAM-HAMMOZ is produced by IEPOX (24.4 TgC) and ISOP(OOH)2 (28.3 TgC). The main sink process is particle wet deposition which removes 143 Tg (59 TgC). The iSOA burden reaches 1.6 Tg (0.7 TgC) in the year 2012.

We have improved an ozone DIfferential Absorption Lidar (DIAL) system, originally developed in March 2010. The improved DIAL system consists of a Nd:YAG laser and a 2 m Raman cell filled with 8.1 × 105 Pa of CO2 gas which generate four Stokes lines (276, 287, 299, and 312 nm) of stimulated Raman scattering, and two receiving telescopes with diameters of 49 and 10 cm. Using this system, 44 ozone profiles were observed in the 1–6 km altitude range over Saga (33.24° N, 130.29° E) in 2012. High-ozone layers were observed at around 2 km altitude during April and May. Ozone column amounts within the 1–6 km altitude range were almost constant (19.1 DU on average) from January to March, and increased to 26.7 DU from late April to July. From mid-July through August, ozone column amounts decreased greatly to 14.3 DU because of exchanges of continental and maritime air masses. Then in mid-September they increased again to 22.1 DU within 1−6 km, and subsequently decreased slowly to 17.3 DU, becoming almost constant by December. The Meteorological Research Institute's chemistry–climate model version 2 (MRI-CCM2) successfully predicted most of these ozone variations with the following exceptions. MRI-CCM2 could not predict the high-ozone volume mixing ratios measured at around 2 km altitude on 5 May and 11 May, possibly in part because emissions were assumed in the model to be constant (climatological data were used). Ozone volume mixing ratios predicted by MRI-CCM2 were low in the 2–6 km range on 7 July and high in the 1–4 km range on 19 July compared with those measured by DIAL.

Recent observations reveal a seasonally occurring layer of aerosol located from 0° to 100°E, 20° to 45°N and extending vertically from about 13 km to 18 km; this has been termed the Asian tropopause aerosol layer (ATAL), and its existence is closely associated with the Asian summer monsoon circulation. Observational studies argue that the ATAL is a recent phenomenon, as the layer is not observed in the satellite record prior to 1998. This suggests that the ATAL may be of anthropogenic origin associated with a shift in the dominant regional emission of sulfur dioxide (SO2) to China and India in the late 1990s. Here we test the hypothesis that SO2emitted from Asia led to the formation of the ATAL using an aerosol microphysical model coupled to a global chemistry climate model. This is the first modeling study to specifically examine the ATAL and its possible origin. From our results, we conclude that the ATAL is most likely due to anthropogenic emissions, but its source cannot solely be attributed to emissions from Asia. Specifically, the results indicate that Chinese and Indian emissions contribute ∼30% of the sulfate aerosol extinction in the ATAL during volcanically quiescent periods. We also show that even small volcanic eruptions preclude our ability to make any conclusions about the existence of the ATAL before 1998 with observations alone.

Tropospheric ozone is a potent greenhouse gas, biological irritant and significant source of highly reactive hydroxyl radicals. Simulations with a chemistry climate model suggest that shifts in atmospheric circulation can account for the seasonally dependent trends in tropospheric ozone levels observed at Mauna Loa, Hawaii, over the past three decades.

We present the third generation of the coupled chemistry–climate model (CCM) SOCOL (modeling tools for studies of SOlar Climate Ozone Links). The most notable modifications compared to the previous model version are (1) the dynamical core has been updated with the fifth generation of the middle-atmosphere general circulation model MA-ECHAM (European Centre/HAMburg climate model), and (2) the advection of the chemical species is now calculated by a mass-conserving and shape-preserving flux-form transport scheme instead of the previously used hybrid advection scheme. The whole chemistry code has been rewritten according to the ECHAM5 infrastructure and transferred to Fortran95. In contrast to its predecessors, SOCOLvs3 is now fully parallelized. The performance of the new SOCOL version is evaluated on the basis of transient model simulations (1975–2004) with different horizontal (T31 and T42) resolutions, following the approach of the CCMVal-1 model validation activity. The advanced advection scheme significantly reduces the artificial loss and accumulation of tracer mass in regions with strong gradients that was observed in previous model versions. Compared to its predecessors, SOCOLvs3 generally shows more realistic distributions of chemical trace species, especially of total inorganic chlorine, in terms of the mean state, but also of the annual and interannual variability. Advancements with respect to model dynamics are for example a better representation of the stratospheric mean state in spring, especially in the Southern Hemisphere, and a slowdown of the upward propagation in the tropical lower stratosphere. Despite a large number of improvements model deficiencies still remain. Examples include a too-fast vertical ascent and/or horizontal mixing in the tropical stratosphere, the cold temperature bias in the lowermost polar stratosphere, and the overestimation of polar total ozone loss during Antarctic springtime., Geoscientific Model Development, 6 (5), ISSN:1991-9603, ISSN:1991-959X

A biogenic emission scheme based on the Model of Emissions of Gases and Aerosols from Nature (MEGAN) version 2.1 (Guenther et al., 2012) has been integrated into the ECHAM6-HAMMOZ chemistry climate model in order to calculate the emissions from terrestrial vegetation of 32 compounds. The estimated annual global total for the simulation period (2000–2012) is 634 Tg C yr−1. Isoprene is the main contributor to the average emission total accounting for 66 % (417 Tg C yr−1), followed by several monoterpenes (12 %), methanol (7 %), acetone (3.6 %) and ethene (3.6 %). Regionally, most of the high annual emissions are found to be associated to tropical regions and tropical vegetation types. In order to evaluate the implementation of the biogenic model in ECHAM-HAMMOZ, global and regional BVOC emissions of the reference simulation were compared to previous published experiment results with the MEGAN model. Several sensitivity simulations were performed to study the impact of different model input and parameters related to the vegetation cover and the ECHAM6 climate. BVOC emissions obtained with the biogenic model are within the range of previous published estimates. The large range of emission estimates can be attributed to the use of different input data and empirical coefficients within different setups of the MEGAN model. The biogenic model shows a high sensitivity to the changes in plant functional type (PFT) distributions and associated emission factors for most of the compounds. The global emission impact for isoprene is about −9 %, but reaches +75 % for α-pinene when switching to PFT-dependent emission factor distributions. Isoprene emissions show the highest sensitivity to soil moisture impact, with a global decrease of 12.5 % when the soil moisture activity factor is included in the model parameterization. Nudging ECHAM6 climate towards ERA-Interim reanalysis has impact on the biogenic emissions, slightly lowering the global total emissions and their interannual variability.

We present an overview of state-of-the-art chemistry-climate and -transport models that are used within the Chemistry-Climate Model Initiative (CCMI). CCMI aims to conduct a detailed evaluation of participating models using process-oriented diagnostics derived from observations in order to gain confidence in the models' projections of the stratospheric ozone layer, air quality, where applicable global climate change, and the interactions between them. Interpretation of these diagnostics requires detailed knowledge of the radiative, chemical, dynamical, and physical processes incorporated in the models. Also an understanding of the degree to which CCMI recommendations for simulations have been followed is necessary to understand model response to anthropogenic and natural forcing and also to explain inter-model differences. This becomes even more important given the ongoing development and the ever-growing complexity of these models. This paper also provides an overview of the available CCMI simulations with the aim to inform CCMI data users.

The global climate model ECHAM/MESSy Atmospheric Chemistry (EMAC) is used to study climate change and air quality scenarios. The EMAC model is constituted by a nonlocal dynamical part with low scalability, and local physical/chemical processes with high scalability. The EMAC chemistry-climate model does not benefit from the support of accelerators which are nowadays installed in many HPC systems. We study strategies to offload the calculation of the atmospheric chemistry to accelerator technologies (GPU and Intel MIC), as in typical model configurations this is the most computational resource-demanding subtask. The proposed solutions extend the Kinetic Pre Processor (KPP) general purpose open-source software tool used in atmospheric chemistry.

This study presents a new ion-neutral chemical model coupled into the Whole Atmosphere Community Climate Model (WACCM). The ionospheric D region (altitudes ~ 50–90 km) chemistry is based on the Sodankylä Ion and Neutral Chemistry (SIC) model, a 1-dimensional model containing 306 ion-neutral and ionrecombination reactions of neutral species, positive and negative ions, and electrons. The SIC mechanism was reduced using the Simulation Error Minimization Connectivity Method (SEM-CM) to produce a reaction scheme of 181 ion-molecule reactions. This scheme describes the concentration profiles at altitudes between 20 km and 120 km of a set of major neutral species (HNO3, O3, H2O2, NO, NO2, HO2, OH, N2O5) and ions (O2+, O4+, NO+, NO+(H2O), O2+(H2O), H+(H2O), H+(H2O)2, H+(H2O)3, H+(H2O)4, O3−, NO2−, O−, O2, OH−, O2−(H2O), O2−(H2O)2, O4−, CO3−, CO3−(H2O), CO4−, HCO3−, NO2−, NO3−, NO3−(H2O), NO3(H2O)2, NO3−(HNO3), NO3−(HNO3)2, Cl−, ClO−), which agree with the full SIC mechanism within a 5 % tolerance. Four 3D model simulations were then performed, using the impact of the January 2005 Solar Proton Event (SPE) on D region HOx and NOx chemistry as a test case of four different model versions: the standard WACCM (no negative ions and a very limited set of positive ions); WACCM-SIC (standard WACCM with the full SIC chemistry of positive and negative ions); WACCM-D (standard WACCM with a heuristic reduction of the SIC chemistry, recently used to examine HNO3 formation following an SPE); and WACCM-rSIC (standard WACCM with a reduction of SIC chemistry using the SEM-CM Method). Standard WACCM misses the HNO3 enhancement during the SPE, while the full and reduced model versions predict significant NOx, HOx and HNO3 enhancements in the mesosphere during solar proton events. The SEM-CM reduction also identifies the important ion-molecule reactions that affect the partitioning of odd nitrogen (NOx), odd hydrogen (HOx), and O3 in the stratosphere and mesosphere.

This technical note presents an overview of the Chemistry-Climate Model Validation Diagnostic (CCMVal-Diag) tool for model evaluation. The CCMVal-Diag tool is a flexible and extensible open source package that facilitates the complex evaluation of global models. Models can be compared to other models, ensemble members (simulations with the same model), and/or many types of observations. The tool can also compute quantitative performance metrics. The initial construction and application is to coupled Chemistry-Climate Models (CCMs) participating in CCMVal, but the evaluation of climate models that submitted output to the Coupled Model Intercomparison Project (CMIP) is also possible. The package has been used to assist with analysis of simulations for the 2010 WMO/UNEP Scientific Ozone Assessment and the SPARC Report on the Evaluation of CCMs. The CCMVal-Diag tool is described and examples of how it functions are presented, along with links to detailed descriptions, instructions and source code. The CCMVal-Diag tool is supporting model development as well as quantifying model improvements, both for different versions of individual models and for different generations of community-wide collections of models used in international assessments. The code allows further extensions by different users for different applications and types, e.g. to other components of the Earth System. User modifications are encouraged and easy to perform with a minimum of coding.

The eruption of Mount Pinatubo produced the largest loading of stratospheric sulphate aerosol in the twentieth century. This heated the tropical lower stratosphere, affecting stratospheric circulation, and provided enhanced surface area for heterogeneous chemistry. These factors combined to produce record low values of "global" total ozone column. Though well studied, there remains some uncertainty about the attribution of this low ozone, with contributions from both chemical and dynamical effects. We take a complementary approach to previous studies, nudging the potential temperature and horizontal winds in the new UKCA chemistry climate model to reproduce the atmospheric response and assess the impact on global total ozone. We then combine model runs and observations to distinguish between chemical and dynamical effects. To estimate the effects of increased heterogeneous chemistry on ozone we compare runs with volcanically enhanced and background surface aerosol density. The modelled depletion of global ozone peaks at about 7 DU in early 1993, in good agreement with values obtained from observations. We subtract the modelled aerosol induced ozone loss from the observed ozone record and attribute the remaining variability to `dynamical' effects. The remaining variability is dominated by the QBO. We also examine tropical and mid-latitude ozone, diagnosing contributions from El Niño in the tropics and identifying dynamically driven low ozone in northern mid-latitudes, which we interpret as possible evidence of changes in the QBO. We conclude that, on a global scale, the record lows of extra-polar ozone are produced by the increased heterogeneous chemistry, although there is evidence for dynamics produced low ozone in certain regions, including northern mid-latitudes.

The strength of the Brewer–Dobson circulation (BDC) in a changing climate is studied using multidecadal simulations covering the 1960–2100 period with a coupled chemistry–climate model, to examine the seasonality of the change of the BDC. The model simulates an intensification of the BDC in both the past (1960–2004) and future (2005–2100) climate, but the seasonal cycle is different. In the past climate simulation, nearly half of the tropical upward mass flux increase occurs in December–February, whereas in the future climate simulation the enhancement of the BDC is uniformly distributed in each of the four seasons. A downward control analysis implies that this different seasonality is caused mainly by the behavior of the Southern Hemisphere planetary wave forcing, which exhibits a very different long-term trend during solstice seasons in the past and future. The Southern Hemisphere summer planetary wave activity is investigated in detail, and its evolution is found to be closely related to ozone depletion and recovery. In the model results for the past, about 60% of the lower-stratospheric mass flux increase is caused by ozone depletion, but because of model ozone trend biases, the atmospheric effect was likely smaller than this. The remaining fraction of the mass flux increase is attributed primarily to greenhouse gas increase. The downward control analysis also reveals that orographic gravity waves contribute significantly to the increase of downward mass flux in the Northern Hemisphere winter lower stratosphere.

Aviation contributes to anthropogenic climate impact through various emissions. Mobility becomes more and more important to society and hence air transportation is expected to grow further over the next decades. Reducing the climate impact from aviation emissions and building a climate-friendly air transportation system are required for a sustainable development of commercial aviation. A climate optimized routing, which avoids climate sensitive regions by re-routing horizontally and vertically, is an important approach for climate impact reduction. The idea includes a number of different routing strategies (routing options) and shows a great potential for the reduction. To evaluate this, the impact of not only CO2 but also non-CO2 emissions must be considered. CO2 is a long-lived and stable gas, while non-CO2 emissions are short-lived and vary regionally. This study introduces AirTraf (version 1.0) for climate impact evaluations that performs global air traffic simulations on long time scales, including effects of local weather conditions on the emissions. AirTraf was developed as a new submodel of the ECHAM5/MESSy Atmospheric Chemistry (EMAC) model. Air traffic information comprises Eurocontrol's Base of Aircraft Data (BADA Revision 3.9) and International Civil Aviation Organization (ICAO) engine performance data. Fuel use and emissions were calculated by the total energy model based on the BADA methodology and DLR fuel flow method. The flight trajectory optimization was performed by a Genetic Algorithm (GA) with respect to routing options. In the model development phase, two benchmark tests were performed for great circle and flight time routing options. The first test showed that the great circle calculations were accurate to within ±0.05 %, compared to those calculated by other published code. The second test showed that the optimal solution sufficiently converged to the theoretical true-optimal solution. The difference in flight time between the two solutions is less than 0.01 %. The dependence of optimal solutions on initial populations was analyzed. We found that the influence was small (around 0.01 %). The trade-off between the accuracy of GA optimizations and the number of function evaluations is clarified and the appropriate population and generation sizing is discussed. The results showed that a large reduction in number of function evaluations of around 90 % can be achieved with only a small decrease in the accuracy of less than 0.1 %. Finally, one-day AirTraf simulations are demonstrated with the great circle and the flight time routing options for a specific winter day. 103 trans-Atlantic flight plans were used, assuming an Airbus A330-301 aircraft. The results confirmed that AirTraf simulates the air traffic properly for the two options. In addition, the GA successfully found the time-optimal flight trajectories for all airport pairs, reflecting local weather conditions. The consistency check for the one-day AirTraf simulations verified that calculated flight time, fuel consumption, NOx emission index and aircraft weights are comparable to reference data.

A combined three-dimensional global model of the chemistry and dynamics of the lower and middle atmosphere (up to 90 km from the Earth’s surface) is described. With the use of this model within the AMIP2 (1979–1995) program, numerical calculations were performed with consideration for the interactive coupling between the ozone content, radiation heating, and atmospheric circulation. Comparisons were made between calculated and observed data on the ozone content and temperature. Heterogeneous processes on the surface of polar stratospheric clouds were shown to be important for a correct simulation of the spatial and temporal distribution of atmospheric ozone.

We present the Efficient CH4-CO-OH chemistry module (ECCOH) that allows for the simulation of the methane, carbon monoxide and hydroxyl radical (CH4-CO-OH) system, within a chemistry climate model, carbon cycle model, or earth system model. The computational efficiency of the module allows many multi-decadal sensitivity simulations of the CH4-CO-OH system, which primarily determines the global atmospheric oxidizing capacity. This capability is important for capturing the nonlinear feedbacks of the CH4-CO-OH system and understanding the perturbations to methane, CO and OH and the concomitant impacts on climate. We implemented the ECCOH chemistry module into the NASA GEOS-5 Atmospheric Global Circulation Model (AGCM), performed multiple sensitivity simulations of the CH4-CO-OH system over two decades, and evaluated the model output with surface and satellite datasets of methane and CO. The favorable comparison of output from the ECCOH chemistry module (as configured in the GEOS-5 AGCM) with observations demonstrates the fidelity of the module for use in scientific research.

We have created a new interactive model for coupled chemistry–climate studies of the stratosphere. The model combines the detailed stratospheric chemistry modules developed and tested in the SLIMCAT/ TOMCAT off-line chemical transport models (CTM) with a version of the Met Office Unified Model (UM). The resulting chemistry–climate model (CCM), called UMCHEM, has a detailed description of stratospheric gas-phase and heterogeneous chemistry. The chemical fields of O3, N2O, CH4 and H2O are used interactively in the radiative heating calculation. We present results from a series of 10-year ‘time-slice’ experiments for 2000 and 2050 conditions. The UMCHEM model performs well in reproducing basic features of the stratosphere. The distribution of long-lived tracers and ‘age of air’ compare well with observations. For O3, the model tends to underestimate the stratospheric column at high latitudes by ∼ 20 DU. This is due to an underestimate of poleward transport in the mid-low stratosphere. The UMCHEM reproduces well the seasonal cycle in monthly mean column O3 at mid-high latitudes, though the variability is slightly smaller than observations and smaller than in the SLIMCAT CTM. Other comparisons with the CTM, which has an identical chemistry scheme, show differences resulting from the models' meteorologies. For example, while the CTM reproduces the observed NOy versus N2O correlation, the UMCHEM overestimates the slope by about a factor of 2. Including full chemistry in the UM causes important differences in the model's meteorology. As the zonal mean ozone climatology used in the UM is larger than that calculated in UMCHEM, with a maximum difference of 4 ppmv in the upper stratosphere, the UMCHEM temperature is about 4 K lower in the Antarctic lower stratosphere and 1–6 K higher in the upper stratosphere. The age of air is less in the basic UM by about 1–3 months in the lower stratosphere but slightly greater in the upper stratosphere. Coupling of the more realistic stratospheric chemistry water vapour warms the model stratosphere by ∼1–2 K. This water vapour coupling also results in a decrease in ozone with a maximum difference of about 250 ppbv in the tropical and southern high-latitude upper stratosphere, while in the tropical lower stratosphere ozone concentrations are increased by up to 30 ppbv. For 2050 conditions, the model produces a column O3 5% higher than present-day values in the tropics, about 15% higher in the Arctic winter/spring and up to 90% higher in the much smaller Antarctic O3 hole. This large O3 increase more than offsets the effect of cooling in the Antarctic late spring induced by greenhouse gases. Copyright © 2005 Royal Meteorological Society

We report results from two pairs of chemistry-climate model simulations using the same climate model but different chemical perturbations. In each pair of experiments an ozone change was triggered by a simple change in the chemistry. One pair of model experiments looked at the impact of Polar Stratospheric Clouds (PSCs) and the other pair at the impact of short lived halogenated species on composition and circulation. The model response is complex with both positive and negative changes in ozone concentration, depending on location. These changes result from coupling between composition, temperature and circulation. Even though the causes of the modelled ozone changes are different, the high latitude Southern Hemisphere response in the lower stratosphere is similar. In both pairs of experiments the high latitude circulation changes, as evidenced by N2O differences, suggesting a slightly longer-lasting/stronger stratospheric descent in runs with higher ozone destruction. We contrast the idealised model behaviour with interannual variability in ozone and N2O as observed by the MIPAS instrument on ENVISAT, highlighting the similarity of the modelled climate equilibrium changes to the year 2006/2007 in observations. We conclude that the climate system can respond quite sensitively to small chemical perturbations, that circulation adjustments seen in the model can occur in reality, and that coupled chemistry-climate models are needed for an assessment of future ozone and climate changes.

In this study we investigate the long-term variations in the stratospheric age spectra using simulations of the 21st century with the Goddard Earth Observing System Chemistry- Climate Model (GEOSCCM). Our purposes are to characterize the long-term changes in the age spectra and identify processes that cause the decrease of the mean age in a warming climate. Changes in the age spectra in the 21st century simulations are characterized by decreases in the modal age, the mean age, the spectral width, and the tail decay timescale. Our analyses show that the decrease in the mean age is caused by two processes: the acceleration of the residual circulation that increases the young air masses in the stratosphere, and the weakening of the recirculation that leads to the decrease of tail of the age spectra and the decrease of the old air masses. The weakening of the stratospheric recirculation is also strongly correlated with the increase of the residual circulation. One important result of this study is that the decrease of the tail of the age spectra makes an important contribution to the decrease of the main age. Long-term changes in the stratospheric isentropic mixing are investigated. Mixing increases in the subtropical lower stratosphere, but its impact on the age spectra is outweighed by the increase of the residual circulation. The impacts of the long-term changes in the age spectra on long-lived chemical traces are also investigated. 37 2

A modeling system based on the air quality model CAMx driven off-line by the regional climate model RegCM3 is used for assessing the impact of lateral boundary conditions and anthropogenic emissions on tropospheric ozone over Europe for the period 1996–2006. The RegCM3 and CAMx simulations were performed on a 50 km × 50 km grid over Europe with RegCM3 driven by NCEP reanalysis fields. Average monthly concentration values obtained from the global chemistry climate model ECHAM5-MOZ were used as chemical boundary conditions for the CAMx simulations. The present period (1996–2006) was simulated four times. The first run was forced with time and space invariable lateral chemical boundary conditions and EMEP emissions based on the year 1996. The second decadal simulation was based on ECHAM5-MOZ chemical boundary conditions and emissions both fixed for the year 1996. The third decadal simulation was based on ECHAM5-MOZ chemical boundary conditions with interannual variation but fixed emissions from the year 1996. Finally, the fourth decadal simulation was based on ECHAM5-MOZ chemical boundary conditions and emissions, both having interannual variation. Simulated ozone concentrations are compared against measurements from the EMEP network in order to evaluate the modeling system.

[1] The stratospheric age spectrum is the probability distribution function of the transit times since a stratospheric air parcel had last contact with a tropospheric boundary region. Previous age spectrum studies have focused on its annual mean properties. Knowledge of the age spectrum's seasonal variability is very limited. In this study, we investigate the seasonal variations of the stratospheric age spectra using the pulse tracer method in the Goddard Earth Observing System Chemistry Climate Model (GEOSCCM). The relationships between the age spectrum and the boundary impulse response (BIR) are reviewed, and a simplified method to reconstruct seasonally varying age spectra is introduced. The age spectra in GEOSCCM have strong seasonal cycles, especially in the lowermost and lower stratosphere and in the subtropical overworld. These changes reflect the seasonal evolution of the Brewer-Dobson circulation, isentropic mixing, and transport barriers. We also investigate the seasonal and interannual variations of the BIRs. Our results clearly show that computing an ensemble of seasonally dependent BIRs is necessary in order to capture the seasonal and annual mean properties of the stratospheric age spectrum.