Search

We present the coupling of the Jena Scheme for Biosphere–Atmosphere Coupling in Hamburg version 4 (JSBACHv4) to the ECHAM/MESSy Atmospheric Chemistry (EMAC) model. With JSBACH, the soil water bucket model in EMAC is replaced by a diffusive hydrological transport model for soil water that includes water storage and infiltration in five soil layers, preventing soil from drying too rapidly and reducing biases in soil temperature and moisture. A three-layer soil scheme is implemented, and phase changes in water in the soil are considered. The leaf area index (LAI) climatology in EMAC has been substituted with a phenology module calculating the LAI. Multiple land cover types are included to provide a state-dependent surface albedo, which accounts for the absorption of solar radiation by vegetation. Plant net primary productivity, leaf area index and surface roughness are calculated according to the plant functional types. This paper provides a detailed evaluation of the new coupled model based on observations and reanalysis data, including ERA5/ERA5-Land datasets, Global Precipitation Climatology Project (GPCP) data and Moderate Resolution Imaging Spectroradiometer (MODIS) satellite data. Land surface temperature (LST), terrestrial water storage (TWS), surface albedo (α), net top-of-atmosphere radiation flux (RadTOA), precipitation (precip), leaf area index (LAI), fraction of absorbed photosynthetic active radiation (FAPAR) and gross primary productivity (GPP) are evaluated in particular. The strongest correlation (r) between reanalysis data and the newly coupled model is found for LST (r=0.985, with an average global bias of −1.546 K), α (r=0.947, with an average global bias of −0.015) and RadTOA (r=0.907, with an average global bias of 3.56 W m−2). Precipitation exhibits a correlation with the GPCP dataset of 0.523 and an average global bias of 0.042 mm d−1. The LAI optimisation yields a correlation of 0.637 with observations and a global mean deviation of −0.212. FAPAR and GPP exemplify two of the many additional variables made available through JSBACH in EMAC. FAPAR and observations show a correlation of 0.663, with an average global difference of −0.223, while the correlation for GPP and observations is 0.564 and the average global difference is −0.001 kg carbon km−1. Benefiting from the numerous added features within the simulated land system, the representation of soil moisture is improved, which is critical for vegetation modelling. This improvement can be attributed to a general increase in soil moisture and water storage in deeper soil layers and a closer alignment of simulated TWS with observations, mitigating the previously widespread problem of soil drought. We show that the numerous newly added components strongly improve the land surface, e.g. soil moisture, TWS and LAI, while surface parameters, such as LST, surface albedo or RadTOA, which were mostly prescribed according to climatologies, remain similar. The coupling of JSBACH brings EMAC a step closer towards a holistic comprehensive Earth system model and extends its versatility.

Upper-tropospheric deep convective outflows during an event on 10–11 June 2019 over central Europe are analysed in ensembles of the operational Icosahedral Nonhydrostatic (ICON) numerical weather prediction model. Both a parameterised and an explicit representation of deep convective systems is studied. Near-linear response of deep convective outflow strength to net latent heating is found for parameterised convection, while different but physically coherent patterns of outflow variability are found in convection-permitting simulations at 1 km horizontal grid spacing. We investigate if the conceptual model for outflow strength proposed in our previous idealised large-eddy simulation (LES) study is able to explain the variation in outflow strength in a real-case scenario. Convective organisation and aggregation induce a non-linear increase in the magnitude of deep convective outflows with increasing net latent heating in convection-permitting simulations, consistent with the conceptual model. However, in contrast to expectations from the conceptual model, a dependence of the outflow strength on the dimensionality of convective overturning (two-dimensional versus three-dimensional) cannot be fully corroborated from the real-case simulations. Our results strongly suggest that the interactions between gravity waves emitted by heating in individual deep convective elements within larger organised convective systems are of prime importance for the representation of divergent outflow strength from organised convection in numerical models.

Aqueous-phase chemical processes in clouds, fog, and deliquescent aerosols are known to alter atmospheric composition and acidity significantly. Traditionally, global and regional models predict aerosol composition by relying on thermodynamic equilibrium models and neglect non-equilibrium processes. Here, we present the AERosol CHEMistry (GMXe–AERCHEM, v1.0) sub-submodel developed for the Modular Earth Submodel System (MESSy) as an add-on to the thermodynamic equilibrium model (i.e. ISORROPIA-II) used by MESSy's Global Modal-aerosol eXtension (GMXe) submodel. AERCHEM allows the representation of non-equilibrium aqueous-phase chemistry of varying complexity in deliquescent fine aerosols. We perform a global simulation for the year 2010 by using the available detailed kinetic model for the chemistry of inorganic and small oxygenated organics. We evaluate AERCHEM's performance by comparing the simulated concentrations of sulfate, nitrate, ammonium, and chloride to in situ measurements of three monitoring networks. Overall, AERCHEM reproduces observed concentrations reasonably well. We find that, especially in the USA, the consideration of non-equilibrium chemistry in deliquescent aerosols reduces the model bias for sulfate, nitrate, and ammonium when compared to simulated concentrations by ISORROPIA-II. Over most continental regions, fine-aerosol acidity simulated by AERCHEM is similar to the predictions by ISORROPIA-II, but simulated aerosol acidity tends to be slightly lower in most regions. The consideration of non-equilibrium chemistry in deliquescent aerosols leads to a significantly higher aerosol acidity in the marine boundary layer, which is in line with observations and recent literature. AERCHEM allows an investigation of the global-scale impact of aerosol non-equilibrium chemistry on atmospheric composition. This will aid in the exploration of key multiphase processes and improve the model predictions for oxidation capacity and aerosols in the troposphere.

This study explores the differences in performance and results by various versions of the ISORROPIA thermodynamic module implemented within the ECHAM/MESSy Atmospheric Chemistry (EMAC) model. Three different versions of the module were used, ISORROPIA II v1, ISORROPIA II v2.3, and ISORROPIA-lite. First, ISORROPIA II v2.3 replaced ISORROPIA II v1 in EMAC to improve pH predictions close to neutral conditions. The newly developed ISORROPIA-lite has been added to EMAC alongside ISORROPIA II v2.3. ISORROPIA-lite is more computationally efficient and assumes that atmospheric aerosols exist always as supersaturated aqueous (metastable) solutions, while ISORROPIA II includes the option to allow for the formation of solid salts at low RH conditions (stable state). The predictions of EMAC by employing all three aerosol thermodynamic models were compared to each other and evaluated against surface measurements from three regional observational networks in the polluted Northern Hemisphere (Interagency Monitoring of Protected Visual Environments (IMPROVE), European Monitoring and Evaluation Programme (EMEP), and Acid Deposition Monitoring Network of East Asia (EANET)). The differences between ISORROPIA II v2.3 and ISORROPIA-lite were minimal in all comparisons with the normalized mean absolute difference for the concentrations of all major aerosol components being less than 11 % even when different phase state assumptions were used. The most notable differences were lower aerosol concentrations predicted by ISORROPIA-lite in regions with relative humidity in the range of 20 % to 60 % compared to the predictions of ISORROPIA II v2.3 in stable mode. The comparison against observations yielded satisfactory agreement especially over the USA and Europe but higher deviations over East Asia, where the overprediction of EMAC for nitrate was as high as 4 µg m−3 (∼20 %). The mean annual aerosol pH predicted by ISORROPIA-lite was on average less than a unit lower than ISORROPIA II v2.3 in stable mode, mainly for coarse-mode aerosols over the Middle East. The use of ISORROPIA-lite accelerated EMAC by nearly 5 % compared to the use of ISORROPIA II v2.3 even if the aerosol thermodynamic calculations consume a relatively small fraction of the EMAC computational time. ISORROPIA-lite can therefore be a reliable and computationally efficient alternative to the previous thermodynamic module in EMAC.

Satellite instruments provide high-temporal-resolution data on a global scale, but extracting 3D information from current instruments remains a challenge. Most observational data are two-dimensional (2D), offering either cloud top information or vertical profiles. We trained a neural network (Res-UNet) to merge high-resolution satellite images from the Meteosat Second Generation (MSG) Spinning Enhanced Visible and InfraRed Imager (SEVIRI) with 2D CloudSat radar reflectivities to generate 3D cloud structures. The Res-UNet extrapolates the 2D reflectivities across the full disk of MSG SEVIRI, enabling a reconstruction of the cloud intensity, height, and shape in three dimensions. The imbalance between cloudy and clear-sky CloudSat profiles results in an overestimation of cloud-free pixels. Our root mean square error (RMSE) accounts for 2.99 dBZ. This corresponds to 6.6 % error on a reflectivity scale between −25 and 20 dBZ. While the model aligns well with CloudSat data, it simplifies multi-level and mesoscale clouds in particular. Despite these limitations, the results can bridge data gaps and support research in climate science such as the analysis of deep convection over time and space.

Emissions of biogenic volatile organic compounds (BVOCs) from the terrestrial biosphere play a significant role in major atmospheric processes. BVOCs are highly reactive compounds that influence the atmosphere's oxidation capacity and also serve as precursors for the formation of aerosols that influence global radiation budgets. Emissions depend on the response of vegetation to atmospheric conditions (primarily temperature and light), as well as other stresses, e.g. from droughts and herbivory. The El Niño–Southern Oscillation (ENSO) is a naturally occurring cycle arising from anomalies in the sea surface temperature (SST) in the tropical Pacific. ENSO perturbs the natural seasonality of weather systems on both global and regional scales and is considered the most significant driver of climate variability. Several studies have evaluated the sensitivity of BVOC fluxes during ENSO events using historical transient simulations. While this approach employs realistic scenarios, it is difficult to assess the impact of ENSO alone given the multiple types of climate forcing, e.g. from anthropogenic emissions of CO2 and aerosol. In this study, a global atmospheric chemistry–climate model with enabled interactive vegetation was used to conduct two sets of simulations: (1) isolated ENSO event simulations, in which a single ENSO event is used to perturb otherwise baseline conditions, and (2) sustained ENSO simulations, in which the same ENSO conditions are reproduced for an extended period of time. From the isolated ENSO events, we present global and regional BVOC emission changes resulting from the immediate response of vegetation to atmospheric states. More focus is given to the sustained ENSO simulations, which have the benefit of reducing the internal variability for more robust statistics when linking atmospheric and vegetation variables with BVOC flux anomalies. Additionally, these simulations explore long-term changes in the biosphere with potential shifts in vegetation in this possible climate mode, accounting for the prospect of increased intensity and frequency of ENSO with climate change. Our results show that strong El Niño events increase global isoprene emission fluxes by 2.9 % and that one single ENSO event perturbs the Earth system so markedly that BVOC emission fluxes do not return to baseline emissions within several years after the event. We show that persistent ENSO conditions shift the vegetation to a new quasi-equilibrium state, leading to an amplification of BVOC emission changes with up to a 19 % increase in isoprene fluxes over the Amazon. We provide evidence that BVOC-induced changes in plant phenology, such as the leaf area index (LAI), have a significant influence on BVOC emissions in the sustained ENSO climate mode.

Upper-tropospheric outflow is analysed in cloud-resolving large-eddy simulations. Thereby, the role of convective organization, latent heating, and other factors in upper-tropospheric divergent-outflow variability from deep convection is diagnosed using a set of more than 80 large-eddy simulations because the outflows are thought to be an important feedback from (organized) deep convection to large-scale atmospheric flows; perturbations in those outflows may sometimes propagate into larger-scale perturbations. Upper-tropospheric divergence is found to be controlled by net latent heating and convective organization. At low precipitation rates isolated convective cells have a stronger mass divergence than squall lines. The squall line divergence is the weakest (relative to the net latent heating) when the outflow is purely 2D in the case of an infinite-length squall line. At high precipitation rates the mass divergence discrepancy between the various modes of convection reduces. Hence, overall, the magnitude of divergent outflow is explained by the latent heating and the dimensionality of the outflow, which together create a non-linear relation.

Earth system models (ESMs) integrate previously separate models of the ocean, atmosphere and vegetation into one comprehensive modelling system enabling the investigation of interactions between different components of the Earth system. Global isoprene and monoterpene emissions from terrestrial vegetation, which represent the most important source of volatile organic compounds (VOCs) in the Earth system, need to be included in global and regional chemical transport models given their major chemical impacts on the atmosphere. Due to the feedback of vegetation activity involving interactions with weather and climate, a coupled modelling system between vegetation and atmospheric chemistry is recommended to address the fate of biogenic volatile organic compounds (BVOCs). In this work, further development in linking LPJ-GUESS, a global dynamic vegetation model, to the atmospheric-chemistry-enabled atmosphere–ocean general circulation model EMAC is presented. New parameterisations are included to calculate the foliar density and leaf area density (LAD) distribution from LPJ-GUESS information. The new vegetation parameters are combined with existing LPJ-GUESS output (i.e. leaf area index and cover fractions) and used in empirically based BVOC modules in EMAC. Estimates of terrestrial BVOC emissions from EMAC's submodels ONEMIS and MEGAN are evaluated using (1) prescribed climatological vegetation boundary conditions at the land–atmosphere interface and (2) dynamic vegetation states calculated in LPJ-GUESS (replacing the “offline” vegetation inputs). LPJ-GUESS-driven global emission estimates for isoprene and monoterpenes from the submodel ONEMIS were 546 and 102 Tg yr−1, respectively. MEGAN determines 657 and 55 Tg of isoprene and monoterpene emissions annually. The new vegetation-sensitive BVOC fluxes in EMAC are in good agreement with emissions from the semi-process-based module in LPJ-GUESS. The new coupled system is used to evaluate the temperature and vegetation sensitivity of BVOC fluxes in doubling CO2 scenarios. This work provides evidence that the new coupled model yields suitable estimates for global BVOC emissions that are responsive to vegetation dynamics. It is concluded that the proposed model set-up is useful for studying land–biosphere–atmosphere interactions in the Earth system.

A chain of processes is identified that regulates much of the spread in an ensemble of squall lines in large eddy simulations with tight initial conditions. Patterns of gravity wave propagation de-correlate and restructure the initial condition spread until a second phase of convective initiation is taking place, i.e. after 30 min of simulation time. Subsequently, variability in this convective initiation and mass overturn is associated with differences in cold pool propagation within the ensemble (propagation at 2–4 m s−1. An ensemble sensitivity analysis reveals that anomalies in squall-line-relative flow with respect to the ensemble mean are also associated with the secondary convective initiation. Downdraughts are fed with extra air by a convergence zone on the rearward flank of the updraughts. An analysis of difference growth within the ensemble shows that a substantial proportion of variability is explained by cold pool propagation contrasts during this stage (30–80 min), which is partly removed when a feature-relative perspective is taken. The patterns of coherent variability exist on the timescale of an hour and dissipate subsequently (80–100 min).

We employ the ECHAM5/MESSy2 atmospheric chemistry general circulation model (EMAC) that incorporates calculations of gas-phase and heterogeneous chemistry coupled with the ozone cycle and aerosol formation, transport, and microphysics to calculate the 1991 Pinatubo volcanic cloud. We considered simultaneous injections of SO2, volcanic ash, and water vapor. We conducted multiple ensemble simulations with different injection configurations to test the evolution of SO2, SO42-, ash masses, stratospheric aerosol optical depth, surface area density (SAD), and the stratospheric temperature response against available observations. We found that the volcanic cloud evolution is sensitive to the altitude where volcanic debris is initially injected and the initial concentrations of the eruption products that affect radiative heating and lofting of the volcanic cloud. The numerical experiments with the injection of 12 Mt SO2, 75 Mt of volcanic ash, and 150 Mt of water vapor at 20 km show the best agreement with the observation aerosol optical depth and stratospheric temperature response. Volcanic water injected by eruptive jet and/or intruding through the tropopause accelerates SO2 oxidation. But the mass of volcanic water retained in the stratosphere is controlled by the stratospheric temperature at the injection level. For example, if volcanic materials are released in the cold point above the tropical tropopause, most of the injected water freezes and sediments as ice crystals. The water vapor directly injected into the volcanic cloud increases the SO42- mass and stratospheric aerosol optical depth by about 5 %. The coarse ash comprises 98 % of the ash injected mass. It sediments within a few days, but aged submicron ash could stay in the stratosphere for a few months providing SAD for heterogeneous chemistry. The presence of ash accelerates the SO2 oxidation by 10 %–20 % due to heterogeneous chemistry, radiative heating, lofting, and faster dispersion of volcanic debris. Ash aging affects its lifetime and optical properties, almost doubling the ash radiative heating. The 2.5-year simulations show that the stratospheric temperature anomalies forced by radiative heating of volcanic debris in our experiments with the 20 km injection height agree well with observations and reanalysis data. This indicates that the model captures the long-term evolution and climate effect of the Pinatubo volcanic cloud. The volcanic cloud's initial lofting, facilitated by ash particles' radiative heating, controls the oxidation rate of SO2. Ash accelerates the formation of the sulfate layer in the first 2 months after the eruption. We also found that the interactive calculations of OH and heterogeneous chemistry increase the volcanic cloud sensitivity to water vapor and ash injections. All those factors must be accounted for in modeling the impact of large-scale volcanic injections on climate and stratospheric chemistry.

An updated and expanded representation of organics in the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) has been evaluated. First, the comprehensive Mainz Organic Mechanism (MOM) in the submodel MECCA (Module Efficiently Calculating the Chemistry of the Atmosphere) was activated with explicit degradation of organic species up to five carbon atoms and a simplified mechanism for larger molecules. Second, the ORACLE submodel (version 1.0) now considers condensation on aerosols for all organics in the mechanism. Parameterizations for aerosol yields are used only for the lumped species that are not included in the explicit mechanism. The simultaneous usage of MOM and ORACLE allows an efficient estimation of not only the chemical degradation of the simulated volatile organic compounds but also the contribution of organics to the growth and fate of (organic) aerosol, with the complexity of the mechanism largely increased compared to EMAC simulations with more simplified chemistry. The model evaluation presented here reveals that the OH concentration is reproduced well globally, whereas significant biases for observed oxygenated organics are present. We also investigate the general properties of the aerosols and their composition, showing that the more sophisticated and process-oriented secondary aerosol formation does not degrade the good agreement of previous model configurations with observations at the surface, allowing further research in the field of gas–aerosol interactions.

From 27 July to 10 August 2017, the airborne StratoClim mission took place in Kathmandu, Nepal, where eight mission flights were conducted with the M-55 Geophysica up to altitudes of 20 km. New particle formation (NPF) was identified by the abundant presence of nucleation-mode aerosols, with particle diameters dp smaller than 15 nm, which were in-situ-detected by means of condensation nuclei (CN) counter techniques. NPF fields in clear skies as well as in the presence of cloud ice particles (dp > 3 µm) were encountered at upper troposphere–lowermost stratosphere (UTLS) levels and within the Asian monsoon anticyclone (AMA). NPF-generated nucleation-mode particles in elevated concentrations (Nnm) were frequently found together with cloud ice (in number concentrations Nice of up to 3 cm−3) at heights between ∼ 11 and 16 km. From a total measurement time of ∼ 22.5 h above 10 km altitude, in-cloud NPF was in sum detected over ∼ 1.3 h (∼ 50 % of all NPF records throughout StratoClim). Maximum Nnm of up to ∼ 11 000 cm−3 was detected coincidently with intermediate ice particle concentrations Nice of 0.05–0.1 cm−3 at comparatively moderate carbon monoxide (CO) contents of ∼ 90–100 nmol mol−1. Neither under clear-sky nor during in-cloud NPF do the highest Nnm concentrations correlate with the highest CO mixing ratios, suggesting that an elevated pollutant load is not a prerequisite for NPF. Under clear-air conditions, NPF with elevated Nnm (> 8000 cm−3) occurred slightly less often than within clouds. In the presence of cloud ice, NPF with Nnm between 1500–4000 cm−3 was observed about twice as often as under clear-air conditions. NPF was not found when ice water contents exceeded 1000 µmol mol−1 in very cold air (< 195 K) at tropopause levels. This indicates a reduction in NPF once deep convection is prevalent together with the presence of mainly liquid-origin ice particles. Within in situ cirrus near the cold point tropopause, recent NPF or intense events with mixing ration nnm larger than 5000 mg−1 were observed only in about 6 % of the in-cloud NPF data. In determining whether the cloud-internal NPF is attenuated or prevented by the microphysical properties of cloud elements, the integral radius (IR) of the ice cloud population turned out to be indicative. Neither the number of ice particles nor the free distance between the ice particles is clearly related to the NPF rate detected. While the increase in ice particles' mass per time dmdt is proportional to the IR and mainly due to the condensation of water vapour, additional condensation of NPF precursors proceeds at the expense of the NPF rate as the precursor's saturation ratio declines. Numerical simulations show the impact of the IR on the supersaturation of a condensable vapour, such as sulfuric acid, and furthermore illustrate that the IR of the cloud ice determines the effective limitation of NPF rates.

We present high spatial resolution (up to 2.2×2.2 km2) simulations focussed over south-west Germany using the online coupled regional atmospheric chemistry model system MECO(n) (MESSy-fied ECHAM and COSMO models nested n times). Numerical simulation of nitrogen dioxide (NO2) surface volume mixing ratios (VMRs) are compared to in situ measurements from a network with 193 locations including background, traffic-adjacent and industrial stations to investigate the model's performance in simulating the spatial and temporal variability of short-lived chemical species. We show that the use of a high-resolution and up-to-date emission inventory is crucial for reproducing the spatial variability and resulted in good agreement with the measured VMRs at the background and industrial locations with an overall bias of less than 10 %. We introduce a computationally efficient approach that simulates diurnal and daily variability in monthly-resolved anthropogenic emissions to resolve the temporal variability of NO2. MAX-DOAS (Multiple AXis Differential Optical Absorption Spectroscopy) measurements performed at Mainz (49.99∘ N, 8.23∘ E) were used to evaluate the simulated tropospheric vertical column densities (VCDs) of NO2. We propose a consistent and robust approach to evaluate the vertical distribution of NO2 in the boundary layer by comparing the individual differential slant column densities (dSCDs) at various elevation angles. This approach considers details of the spatial heterogeneity and sensitivity volume of the MAX-DOAS measurements while comparing the measured and simulated dSCDs. The effects of clouds on the agreement between MAX-DOAS measurements and simulations have also been investigated. For low elevation angles (≤8∘), small biases in the range of −14 % to +7 % and Pearson correlation coefficients in the range of 0.5 to 0.8 were achieved for different azimuth directions in the cloud-free cases, indicating good model performance in the layers close to the surface. Accounting for diurnal and daily variability in the monthly-resolved anthropogenic emissions was found to be crucial for the accurate representation of time series of measured NO2 VMR and dSCDs and is particularly critical when vertical mixing is suppressed, and the atmospheric lifetime of NO2 is relatively long.

Microphysical processes in cold clouds which act as sources or sinks of hydrometeors below 0 ∘C control the ice crystal number concentrations (ICNCs) and in turn the cloud radiative effects. Estimating the relative importance of the cold cloud microphysical process rates is of fundamental importance to underpin the development of cloud parameterizations for weather, atmospheric chemistry, and climate models and to compare the output with observations at different temporal resolutions. This study quantifies and investigates the ICNC rates of cold cloud microphysical processes by means of the chemistry–climate model EMAC (ECHAM/MESSy Atmospheric Chemistry) and defines the hierarchy of sources and sinks of ice crystals. Both microphysical process rates, such as ice nucleation, aggregation, and secondary ice production, and unphysical correction terms are presented. Model ICNCs are also compared against a satellite climatology. We found that model ICNCs are in overall agreement with satellite observations in terms of spatial distribution, although the values are overestimated, especially around high mountains. The analysis of ice crystal rates is carried out both at global and at regional scales. We found that globally the freezing of cloud droplets and convective detrainment over tropical land masses are the dominant sources of ice crystals, while aggregation and accretion act as the largest sinks. In general, all processes are characterized by highly skewed distributions. Moreover, the influence of (a) different ice nucleation parameterizations and (b) a future global warming scenario on the rates has been analysed in two sensitivity studies. In the first, we found that the application of different parameterizations for ice nucleation changes the hierarchy of ice crystal sources only slightly. In the second, all microphysical processes follow an upward shift in altitude and an increase by up to 10 % in the upper troposphere towards the end of the 21st century.

A new module has been implemented in the fifth generation of the ECMWF/Hamburg (ECHAM5)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) model that simulates cloud-related processes on a much smaller grid. This so-called superparameterisation acts as a replacement for the convection parameterisation and large-scale cloud scheme. The concept of embedding a cloud-resolving model (CRM) inside of each grid box of a general circulation model leads to an explicit representation of cloud dynamics. The new model component is evaluated against observations and the conventional usage of EMAC using a convection parameterisation. In particular, effects of applying different configurations of the superparameterisation are analysed in a systematical way. Consequences of changing the CRM's orientation, cell size and number of cells range from regional differences in cloud amount up to global impacts on precipitation distribution and its variability. For some edge case setups, the analysed climate state of superparameterised simulations even deteriorates from the mean observed energy budget. In the current model configuration, different climate regimes can be formed that are mainly driven by some of the parameters of the CRM. Presently, the simulated total cloud cover is at the lower edge of the CMIP5 model ensemble. However, certain “tuning” of the current model configuration could improve the slightly underestimated cloud cover, which will result in a shift of the simulated climate. The simulation results show that especially tropical precipitation is better represented with the superparameterisation in the EMAC model configuration. Furthermore, the diurnal cycle of precipitation is heavily affected by the choice of the CRM parameters. However, despite an improvement of the representation of the continental diurnal cycle in some configurations, other parameter choices result in a deterioration compared to the reference simulation using a conventional convection parameterisation. The ability of the superparameterisation to represent latent and sensible heat flux climatology is independent of the chosen CRM setup. Evaluation of in-atmosphere cloud amounts depending on the chosen CRM setup shows that cloud development can significantly be influenced on the large scale using a too-small CRM domain size. Therefore, a careful selection of the CRM setup is recommended using 32 or more CRM cells to compensate for computational expenses.

Central to the development of Earth system models (ESMs) has been the coupling of previously separate model types, such as ocean, atmospheric, and vegetation models, to address interactive feedbacks between the system components. A modelling framework which combines a detailed representation of these components, including vegetation and other land surface processes, enables the study of land–atmosphere feedbacks under global climate change. Here we present the initial steps of coupling LPJ-GUESS, a dynamic global vegetation model, to the atmospheric chemistry-enabled atmosphere–ocean general circulation model EMAC. The LPJ-GUESS framework is based on ecophysiological processes, such as photosynthesis; plant and soil respiration; and ecosystem carbon, nitrogen, and water cycling, and it includes a comparatively detailed individual-based representation of resource competition, plant growth, and vegetation dynamics as well as fire disturbance. Although not enabled here, the model framework also includes a crop and managed-land scheme, a representation of arctic methane and permafrost, and a choice of fire models; and hence it represents many important terrestrial biosphere processes and provides a wide range of prognostic trace-gas emissions from vegetation, soil, and fire. We evaluated an online one-way-coupled model configuration (with climate variable being passed from EMAC to LPJ-GUESS but no return information flow) by conducting simulations at three spatial resolutions (T42, T63, and T85). These were compared to an expert-derived map of potential natural vegetation and four global gridded data products: tree cover, biomass, canopy height, and gross primary productivity (GPP). We also applied a post hoc land use correction to account for human land use. The simulations give a good description of the global potential natural vegetation distribution, although there are some regional discrepancies. In particular, at the lower spatial resolutions, a combination of low-temperature and low-radiation biases in the growing season of the EMAC climate at high latitudes causes an underestimation of vegetation extent. Quantification of the agreement with the gridded datasets using the normalised mean error (NME) averaged over all datasets shows that increasing the spatial resolution from T42 to T63 improved the agreement by 10 %, and going from T63 to T85 improved the agreement by a further 4 %. The highest-resolution simulation gave NME scores of 0.63, 0.66, 0.84, and 0.53 for tree cover, biomass, canopy height, and GPP, respectively (after correcting tree cover and biomass for human-caused deforestation which was not present in the simulations). These scores are just 4 % worse on average than an offline LPJ-GUESS simulation using observed climate data and corrected for deforestation by the same method. However, it should be noted that the offline LPJ-GUESS simulation used a higher spatial resolution, which makes the evaluation more rigorous, and that excluding GPP from the datasets (which was anomalously better in the EMAC simulations) gave 10 % worse agreement for the EMAC simulation than the offline simulation. Gross primary productivity was best simulated by the coupled simulations, and canopy height was the worst. Based on this first evaluation, we conclude that the coupled model provides a suitable means to simulate dynamic vegetation processes in EMAC.

The hydroxyl radical (OH) plays critical roles within the troposphere, such as determining the lifetime of methane (CH4), yet is challenging to model due to its fast cycling and dependence on a multitude of sources and sinks. As a result, the reasons for variations in OH and the resulting methane lifetime (τCH4), both between models and in time, are difficult to diagnose. We apply a neural network (NN) approach to address this issue within a group of models that participated in the Chemistry-Climate Model Initiative (CCMI). Analysis of the historical specified dynamics simulations performed for CCMI indicates that the primary drivers of τCH4 differences among 10 models are the flux of UV light to the troposphere (indicated by the photolysis frequency JO1D), the mixing ratio of tropospheric ozone (O3), the abundance of nitrogen oxides (NOx≡NO+NO2), and details of the various chemical mechanisms that drive OH. Water vapour, carbon monoxide (CO), the ratio of NO:NOx, and formaldehyde (HCHO) explain moderate differences in τCH4, while isoprene, methane, the photolysis frequency of NO2 by visible light (JNO2), overhead ozone column, and temperature account for little to no model variation in τCH4. We also apply the NNs to analysis of temporal trends in OH from 1980 to 2015. All models that participated in the specified dynamics historical simulation for CCMI demonstrate a decline in τCH4 during the analysed timeframe. The significant contributors to this trend, in order of importance, are tropospheric O3, JO1D, NOx, and H2O, with CO also causing substantial interannual variability in OH burden. Finally, the identified trends in τCH4 are compared to calculated trends in the tropospheric mean OH concentration from previous work, based on analysis of observations. The comparison reveals a robust result for the effect of rising water vapour on OH and τCH4, imparting an increasing and decreasing trend of about 0.5 % decade−1, respectively. The responses due to NOx, ozone column, and temperature are also in reasonably good agreement between the two studies.

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.

The new submodel SVOC for the Modular Earth Submodel System (MESSy) was developed and applied within the ECHAM5/MESSy Atmospheric Chemistry (EMAC) model to simulate the atmospheric cycling and air–surface exchange processes of semivolatile organic pollutants. Our focus is on four polycyclic aromatic hydrocarbons (PAHs) of largely varying properties. Some new features in input and physics parameterizations of tracers were tested: emission seasonality, the size discretization of particulate-phase tracers, the application of poly-parameter linear free-energy relationships in gas–particle partitioning, and re-volatilization from land and sea surfaces. The results indicate that the predicted global distribution of the 3-ring PAH phenanthrene is sensitive to the seasonality of its emissions, followed by the effects of considering re-volatilization from surfaces. The predicted distributions of the 4-ring PAHs fluoranthene and pyrene and the 5-ring PAH benzo(a)pyrene are found to be sensitive to the combinations of factors with their synergistic effects being stronger than the direct effects of the individual factors. The model was validated against observations of PAH concentrations and aerosol particulate mass fraction. The annual mean concentrations are simulated to the right order of magnitude for most cases and the model well captures the species and regional variations. However, large underestimation is found over the ocean. It is found that the particulate mass fraction of the benzo(a)pyrene is well simulated, whereas those of other species are lower than observed.

Recently, the aerosol microphysics submodel MADE3 (Modal Aerosol Dynamics model for Europe, adapted for global applications, third generation) was introduced as a successor to MADE and MADE-in. It includes nine aerosol species and nine lognormal modes to represent aerosol particles of three different mixing states throughout the aerosol size spectrum. Here, we describe the implementation of the most recent version of MADE3 into the ECHAM/MESSy Atmospheric Chemistry (EMAC) general circulation model, including a detailed evaluation of a 10-year aerosol simulation with MADE3 as part of EMAC.We compare simulation output to station network measurements of near-surface aerosol component mass concentrations, to airborne measurements of aerosol mass mixing ratio and number concentration vertical profiles, to ground-based and airborne measurements of particle size distributions, and to station network and satellite measurements of aerosol optical depth. Furthermore, we describe and apply a new evaluation method, which allows a comparison of model output to size-resolved electron microscopy measurements of particle composition. Although there are indications that fine-mode particle deposition may be underestimated by the model, we obtained satisfactory agreement with the observations. Remaining deviations are of similar size to those identified in other global aerosol model studies.Thus, MADE3 can be considered ready for application within EMAC. Due to its detailed representation of aerosol mixing state, it is especially useful for simulating wet and dry removal of aerosol particles, aerosol-induced formation of cloud droplets and ice crystals as well as aerosol–radiation interactions. Besides studies on these fundamental processes, we also plan to use MADE3 for a reassessment of the climate effects of anthropogenic aerosol perturbations.

A comprehensive ice nucleation parameterization has been implemented in the global chemistry-climate model EMAC to improve the representation of ice crystal number concentrations (ICNCs). The parameterization of Barahona and Nenes (2009, hereafter BN09) allows for the treatment of ice nucleation taking into account the competition for water vapour between homogeneous and heterogeneous nucleation in cirrus clouds. Furthermore, the influence of chemically heterogeneous, polydisperse aerosols is considered by applying one of the multiple ice nucleating particle parameterizations which are included in BN09 to compute the heterogeneously formed ice crystals. BN09 has been modified in order to consider the pre-existing ice crystal effect and implemented to operate both in the cirrus and in the mixed-phase regimes. Compared to the standard EMAC parameterizations, BN09 produces fewer ice crystals in the upper troposphere but higher ICNCs in the middle troposphere, especially in the Northern Hemisphere where ice nucleating mineral dust particles are relatively abundant. Overall, ICNCs agree well with the observations, especially in cold cirrus clouds (at temperatures below 205 K), although they are underestimated between 200 and 220 K. As BN09 takes into account processes which were previously neglected by the standard version of the model, it is recommended for future EMAC simulations.

We present a sensitivity study on transatlantic dust transport, a process which has many implications for the atmosphere, the ocean and the climate. We investigate the impact of key processes that control the dust outflow, i.e., the emission flux, convection schemes and the chemical aging of mineral dust, by using the EMAC model following Abdelkader et al. (2015). To characterize the dust outflow over the Atlantic Ocean, we distinguish two geographic zones: (i) dust interactions within the Intertropical Convergence Zone (ITCZ), or the dust–ITCZ interaction zone (DIZ), and (ii) the adjacent dust transport over the Atlantic Ocean (DTA) zone. In the latter zone, the dust loading shows a steep and linear gradient westward over the Atlantic Ocean since particle sedimentation is the dominant removal process, whereas in the DIZ zone aerosol–cloud interactions, wet deposition and scavenging processes determine the extent of the dust outflow. Generally, the EMAC simulated dust compares well with CALIPSO observations; however, our reference model configuration tends to overestimate the dust extinction at a lower elevation and underestimates it at a higher elevation. The aerosol optical depth (AOD) over the Caribbean responds to the dust emission flux only when the emitted dust mass is significantly increased over the source region in Africa by a factor of 10. These findings point to the dominant role of dust removal (especially wet deposition) in transatlantic dust transport. Experiments with different convection schemes have indeed revealed that the transatlantic dust transport is more sensitive to the convection scheme than to the dust emission flux parameterization. To study the impact of dust chemical aging, we focus on a major dust outflow in July 2009. We use the calcium cation as a proxy for the overall chemical reactive dust fraction and consider the uptake of major inorganic acids (i.e., H2SO4, HNO3 and HCl) and their anions, i.e., sulfate (SO42−), bisulfate (HSO4−), nitrate (NO3−) and chloride (Cl−), on the surface of mineral particles. The subsequent neutralization reactions with the calcium cation form various salt compounds that cause the uptake of water vapor from the atmosphere, i.e., through the chemical aging of dust particles leading to an increase of 0.15 in the AOD under subsaturated conditions (July 2009 monthly mean). As a result of the radiative feedback on surface winds, dust emissions increased regionally. On the other hand, the aged dust particles, compared to the non-aged particles, are more efficiently removed by both wet and dry deposition due to the increased hygroscopicity and particle size (mainly due to water uptake). The enhanced removal of aged particles decreases the dust burden and lifetime, which indirectly reduces the dust AOD by 0.05 (monthly mean). Both processes can be significant (major dust outflow, July 2009), but the net effect depends on the region and level of dust chemical aging.

Lightning represents one of the dominant emission sources for NOx in the troposphere. The direct release of oxidised nitrogen in the upper troposphere does not only affect ozone formation, but also chemical and microphysical properties of aerosol particles in this region. This study investigates the direct impact of LNOx emissions on upper-tropospheric nitrate using a global chemistry climate model. The simulation results show a substantial influence of the lightning emissions on the mixing ratios of nitrate aerosol in the upper troposphere of more than 50 %. In addition to the impact on nitrate, lightning substantially affects the oxidising capacity of the atmosphere with substantial implications for gas-phase sulfate formation and new particle formation in the upper troposphere. In conjunction with the condensation of nitrates, substantial differences in the aerosol size distribution occur in the upper troposphere as a consequence of lightning. This has implications for the extinction properties of the aerosol particles and for the cloud optical properties. While the extinction is generally slightly enhanced due to the LNOx emissions, the response of the clouds is ambiguous due to compensating effects in both liquid and ice clouds. Resulting shortwave flux perturbations are of ∼ −100 mW m−2 as determined from several sensitivity scenarios, but an uncertainty range of almost 50 % has to be defined due to the large internal variability of the system and the uncertainties in the multitude of involved processes. Despite the clear statistical significance of the influence of lightning on the nitrate concentrations, the robustness of the findings gradually decreases towards the determination of the radiative flux perturbations.

For the first time, a simulation incorporating tropospheric and stratospheric chemistry using the newly developed MECO(n) model system is performed. MECO(n) is short for MESSy-fied ECHAM and COSMO models nested n times. It features an online coupling of the COSMO-CLM model, equipped with the Modular Earth Submodel System (MESSy) interface (called COSMO/MESSy), with the global atmospheric chemistry model ECHAM5/MESSy for Atmospheric Chemistry (EMAC). This online coupling allows a consistent model chain with respect to chemical and meteorological boundary conditions from the global scale down to the regional kilometre scale. A MECO(2) simulation incorporating one regional instance over Europe with 50 km resolution and one instance over Germany with 12 km resolution is conducted for the evaluation of MECO(n) with respect to tropospheric gas-phase chemistry. The main goal of this evaluation is to ensure that the chemistry-related MESSy submodels and the online coupling with respect to the chemistry are correctly implemented. This evaluation is a prerequisite for the further usage of MECO(n) in atmospheric chemistry-related studies. Results of EMAC and the two COSMO/MESSy instances are compared with satellite, ground-based and aircraft in situ observations, focusing on ozone, carbon monoxide and nitrogen dioxide. Further, the methane lifetimes in EMAC and the two COSMO/MESSy instances are analysed in view of the tropospheric oxidation capacity. From this evaluation, we conclude that the chemistry-related submodels and the online coupling with respect to the chemistry are correctly implemented. In comparison with observations, both EMAC and COSMO/MESSy show strengths and weaknesses. Especially in comparison to aircraft in situ observations, COSMO/MESSy shows very promising results. However, the amplitude of the diurnal cycle of ground-level ozone measurements is underestimated. Most of the differences between COSMO/MESSy and EMAC can be attributed to differences in the dynamics of both models, which are subject to further model developments.

The Modular Earth Submodel System (MESSy) provides an interface to couple submodels to a base model via a highly flexible data management facility (Jöckel et al., 2010). In the present paper we present the four new radiation related submodels RAD, AEROPT, CLOUDOPT, and ORBIT. The submodel RAD (including the shortwave radiation scheme RAD_FUBRAD) simulates the radiative transfer, the submodel AEROPT calculates the aerosol optical properties, the submodel CLOUDOPT calculates the cloud optical properties, and the submodel ORBIT is responsible for Earth orbit calculations. These submodels are coupled via the standard MESSy infrastructure and are largely based on the original radiation scheme of the general circulation model ECHAM5, however, expanded with additional features. These features comprise, among others, user-friendly and flexibly controllable (by namelists) online radiative forcing calculations by multiple diagnostic calls of the radiation routines. With this, it is now possible to calculate radiative forcing (instantaneous as well as stratosphere adjusted) of various greenhouse gases simultaneously in only one simulation, as well as the radiative forcing of cloud perturbations. Examples of online radiative forcing calculations in the ECHAM/MESSy Atmospheric Chemistry (EMAC) model are presented.

Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (137Cs) and xenon-133 (133Xe) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. 137Cs size distribution measurements taken close to the power plant suggested that accumulation-mode (AM) sulfate aerosols were the main carriers of cesium. Hence, 137Cs can be used as a proxy tracer for the AM sulfate aerosol's fate in the atmosphere. In contrast, the noble gas 133Xe behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of 137Cs that were assigned to an aerosol tracer with each model's default properties of AM sulfate, and 133Xe emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulfate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled 137Cs and 133Xe concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime τe, calculated from station measurement data taken between 2 and 9 weeks after the start of the emissions, is 14.3 days (95 % confidence interval 13.1–15.7 days). The equivalent modelled τe lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.4 ± 2.3 days, indicating too fast a removal in most models. Because sufficient measurement data were only available from about 2 weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first 2 weeks was quicker (lifetimes between 1 and 5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer (133Xe) concentrations in the Arctic as well but to a smaller extent than for the aerosol (137Cs) tracer. This indicates that in addition to too fast an aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the underestimation of the Arctic aerosol concentrations.

Three types of reference simulations, as recommended by the Chemistry–Climate Model Initiative (CCMI), have been performed with version 2.51 of the European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) model: hindcast simulations (1950–2011), hindcast simulations with specified dynamics (1979–2013), i.e. nudged towards ERA-Interim reanalysis data, and combined hindcast and projection simulations (1950–2100). The manuscript summarizes the updates of the model system and details the different model set-ups used, including the on-line calculated diagnostics. Simulations have been performed with two different nudging set-ups, with and without interactive tropospheric aerosol, and with and without a coupled ocean model. Two different vertical resolutions have been applied. The on-line calculated sources and sinks of reactive species are quantified and a first evaluation of the simulation results from a global perspective is provided as a quality check of the data. The focus is on the intercomparison of the different model set-ups. The simulation data will become publicly available via CCMI and the Climate and Environmental Retrieval and Archive (CERA) database of the German Climate Computing Centre (DKRZ). This manuscript is intended to serve as an extensive reference for further analyses of the Earth System Chemistry integrated Modelling (ESCiMo) simulations.

The Community Earth System Model (CESM1), maintained by the United States National Centre for Atmospheric Research (NCAR) is connected with the Modular Earth Submodel System (MESSy). For the MESSy user community, this offers many new possibilities. The option to use the Community Atmosphere Model (CAM) atmospheric dynamical cores, especially the state-of-the-art spectral element (SE) core, as an alternative to the ECHAM5 spectral transform dynamical core will provide scientific and computational advances for atmospheric chemistry and climate modelling with MESSy. The well-established finite volume core from CESM1(CAM) is also made available. This offers the possibility to compare three different atmospheric dynamical cores within MESSy. Additionally, the CESM1 land, river, sea ice, glaciers and ocean component models can be used in CESM1/MESSy simulations, allowing the use of MESSy as a comprehensive Earth system model (ESM). For CESM1/MESSy set-ups, the MESSy process and diagnostic submodels for atmospheric physics and chemistry are used together with one of the CESM1(CAM) dynamical cores; the generic (infrastructure) submodels support the atmospheric model component. The other CESM1 component models, as well as the coupling between them, use the original CESM1 infrastructure code and libraries; moreover, in future developments these can also be replaced by the MESSy framework. Here, we describe the structure and capabilities of CESM1/MESSy, document the code changes in CESM1 and MESSy, and introduce several simulations as example applications of the system. The Supplements provide further comparisons with the ECHAM5/MESSy atmospheric chemistry (EMAC) model and document the technical aspects of the connection in detail.

The convective transport module, CVTRANS, of the ECHAM/MESSy Atmospheric Chemistry (EMAC) model has been revised to better represent the physical flows and incorporate recent findings on the properties of the convective plumes. The modifications involve (i) applying intermediate time stepping based on a settable criterion, (ii) using an analytic expression to account for the intra-time-step mixing ratio evolution below cloud base, and (iii) implementing a novel expression for the mixing ratios of atmospheric compounds at the base of an updraft. Even when averaged over a year, the predicted mixing ratios of atmospheric compounds are affected considerably by the intermediate time stepping. For example, for an exponentially decaying atmospheric tracer with a lifetime of 1 day, the zonal averages can locally differ by more than a factor of 6 and the induced root mean square deviation from the original code is, weighted by the air mass, higher than 40 % of the average mixing ratio. The other modifications result in smaller differences. However, since they do not require additional computational time, their application is also recommended.

The aerosol optical depth (AOD) trend between 2001 and 2010 is estimated globally and regionally from observations and results from simulations with the EMAC (ECHAM5/MESSy Atmospheric Chemistry) model. Although interannual variability is applied only to anthropogenic and biomass-burning emissions, the model is able to quantitatively reproduce the AOD trends as observed by the MODIS (Moderate Resolution Imaging Spectroradiometer) satellite sensor, while some discrepancies are found when compared to MISR (Multi-angle Imaging SpectroRadiometer) and SeaWIFS (Sea-viewing Wide Field-of-view Sensor) observations. Thanks to an additional simulation without any change in emissions, it is shown that decreasing AOD trends over the US and Europe are due to the decrease in the emissions, while over the Sahara Desert and the Middle East region, the meteorological changes play a major role. Over Southeast Asia, both meteorology and emissions changes are equally important in defining AOD trends. Additionally, decomposing the regional AOD trends into individual aerosol components reveals that the soluble components are the most dominant contributors to the total AOD, as their influence on the total AOD is enhanced by the aerosol water content.

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.

This paper evaluates the current status of global modeling of the organic aerosol (OA) in the troposphere and analyzes the differences between models as well as between models and observations. Thirty-one global chemistry transport models (CTMs) and general circulation models (GCMs) have participated in this intercomparison, in the framework of AeroCom phase II. The simulation of OA varies greatly between models in terms of the magnitude of primary emissions, secondary OA (SOA) formation, the number of OA species used (2 to 62), the complexity of OA parameterizations (gas-particle partitioning, chemical aging, multiphase chemistry, aerosol microphysics), and the OA physical, chemical and optical properties. The diversity of the global OA simulation results has increased since earlier AeroCom experiments, mainly due to the increasing complexity of the SOA parameterization in models, and the implementation of new, highly uncertain, OA sources. Diversity of over one order of magnitude exists in the modeled vertical distribution of OA concentrations that deserves a dedicated future study. Furthermore, although the OA / OC ratio depends on OA sources and atmospheric processing, and is important for model evaluation against OA and OC observations, it is resolved only by a few global models. The median global primary OA (POA) source strength is 56 Tg a−1 (range 34–144 Tg a−1) and the median SOA source strength (natural and anthropogenic) is 19 Tg a−1 (range 13–121 Tg a−1). Among the models that take into account the semi-volatile SOA nature, the median source is calculated to be 51 Tg a−1 (range 16–121 Tg a−1), much larger than the median value of the models that calculate SOA in a more simplistic way (19 Tg a−1; range 13–20 Tg a−1, with one model at 37 Tg a−1). The median atmospheric burden of OA is 1.4 Tg (24 models in the range of 0.6–2.0 Tg and 4 between 2.0 and 3.8 Tg), with a median OA lifetime of 5.4 days (range 3.8–9.6 days). In models that reported both OA and sulfate burdens, the median value of the OA/sulfate burden ratio is calculated to be 0.77; 13 models calculate a ratio lower than 1, and 9 models higher than 1. For 26 models that reported OA deposition fluxes, the median wet removal is 70 Tg a−1 (range 28–209 Tg a−1), which is on average 85% of the total OA deposition. Fine aerosol organic carbon (OC) and OA observations from continuous monitoring networks and individual field campaigns have been used for model evaluation. At urban locations, the model–observation comparison indicates missing knowledge on anthropogenic OA sources, both strength and seasonality. The combined model–measurements analysis suggests the existence of increased OA levels during summer due to biogenic SOA formation over large areas of the USA that can be of the same order of magnitude as the POA, even at urban locations, and contribute to the measured urban seasonal pattern. Global models are able to simulate the high secondary character of OA observed in the atmosphere as a result of SOA formation and POA aging, although the amount of OA present in the atmosphere remains largely underestimated, with a mean normalized bias (MNB) equal to −0.62 (−0.51) based on the comparison against OC (OA) urban data of all models at the surface, −0.15 (+0.51) when compared with remote measurements, and −0.30 for marine locations with OC data. The mean temporal correlations across all stations are low when compared with OC (OA) measurements: 0.47 (0.52) for urban stations, 0.39 (0.37) for remote stations, and 0.25 for marine stations with OC data. The combination of high (negative) MNB and higher correlation at urban stations when compared with the low MNB and lower correlation at remote sites suggests that knowledge about the processes that govern aerosol processing, transport and removal, on top of their sources, is important at the remote stations. There is no clear change in model skill with increasing model complexity with regard to OC or OA mass concentration. However, the complexity is needed in models in order to distinguish between anthropogenic and natural OA as needed for climate mitigation, and to calculate the impact of OA on climate accurately.

In the last decades several convection parameterisations have been developed to consider the impact of small-scale unresolved processes in Earth System Models associated with convective clouds. Global model simulations, which have been performed under current climate conditions with different convection schemes, significantly differ among each other in the simulated transport of trace gases and precipitation patterns due to the parameterisation assumptions and formulations, e.g. the computation of convective rainfall rates, calculation of entrainment and detrainment rates etc. Here we address sensitivity studies comparing four different convection schemes under alternative climate conditions (with doubling of the CO2 concentrations) to identify uncertainties related to convective processes. The increase in surface temperature reveals regional differences up to 4 K dependent on the chosen convection parameterisation. These differences are statistically significant almost everywhere in the troposphere of the intertropical convergence zone. The increase in upper tropospheric temperature affects the amount of water vapour transported to the lower stratosphere, leading to enhanced water vapour contents between 40% and 60% at the cold point temperature in the Tropics. Furthermore, the change in transporting short-lived pollutants within the atmosphere is highly ambiguous for the lower and upper troposphere. These results reflect that different approaches to compute mass fluxes, detrainment levels or trigger functions determine the transport of short-lived trace gases from the planetary boundary layer to lower, middle or upper tropospheric levels. Finally, cloud radiative effects have been analysed, uncovering a shift in different cloud types in the Tropics, especially for cirrus and deep convective clouds. These cloud types induce a change in net cloud radiative forcing varying from 0.5 W m−2 to 2.0 W m−2.

Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network of aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the multi-model-mean data set simulates the global variation of the particle size distribution with a good degree of skill, suggesting that most of the individual global aerosol microphysics models are performing well, although the large model diversity indicates that some models are in poor agreement with the observations. Further work is required to better constrain size-resolved primary and secondary particle number sources, and an improved understanding of nucleation and growth (e.g. the role of nitrate and secondary organics) will improve the fidelity of simulated particle size distributions.

We apply a cloud slicing technique (CST), originally developed for Total Ozone Mapping Spectrometer (TOMS) ozone observations, to CO vertical column densities retrieved from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY). CST makes use of the shielding effect of clouds and combines trace gas column measurements of cloudy pixels with different cloud heights to retrieve fractional columns aloft. Here we determine seasonal mean tropospheric CO profiles at a vertical resolution of about 1 km, which is much finer than what can be obtained from thermal infrared (IR) instruments. However, since both the atmospheric CO profiles and the effective cloud heights depend systematically on meteorology, and in addition part of the retrieved signal originates from the clear part of the satellite ground pixel, the profiles retrieved from the CST have to be interpreted with care. We compare the seasonal mean SCIAMACHY CO profiles with the output from two atmospheric models sampled in the same way as the satellite observations. We find in general good agreement of the spatial patterns, but systematic differences in the absolute values are observed in both hemispheres (more strongly in the Northern Hemisphere), indicating that the source strengths in the emission inventories are probably underestimated.

Recently, realistic simulation of nitrous acid (HONO) based on the HONO / NOx ratio of 0.02 was found to have a significant impact on the global budgets of HOx (OH + HO2) and gas phase oxidation products in polluted regions, especially in winter when other photolytic sources are of minor importance. It has been reported that chemistry-transport models underestimate sulphate concentrations, mostly during winter. Here we show that simulating realistic HONO levels can significantly enhance aerosol sulphate (S(VI)) due to the increased formation of H2SO4. Even though in-cloud aqueous phase oxidation of dissolved SO2 (S(IV)) is the main source of S(VI), it appears that HONO related enhancement of H2O2 does not significantly affect sulphate because of the predominantly S(IV) limited conditions, except over eastern Asia. Nitrate is also increased via enhanced gaseous HNO3 formation and N2O5 hydrolysis on aerosol particles. Ammonium nitrate is enhanced in ammonia-rich regions but not under ammonia-limited conditions. Furthermore, particle number concentrations are also higher, accompanied by the transfer from hydrophobic to hydrophilic aerosol modes. This implies a significant impact on the particle lifetime and cloud nucleating properties. The HONO induced enhancements of all species studied are relatively strong in winter though negligible in summer. Simulating realistic HONO levels is found to improve the model-measurement agreement of sulphate aerosols, most apparent over the US. Our results underscore the importance of HONO for the atmospheric oxidizing capacity and corroborate the central role of cloud chemical processing in S(IV) formation.

Major population centers (MPCs), or megacities, represent the largest of growing urban agglomerations with major societal and environmental implications. In terms of air quality, they are seen as localized but strong emission sources of aerosols and trace gases which in turn affect air pollution levels in the city or in downwind regions. In the state-of-the-art atmospheric chemistry general circulation model EMAC, generic aerosol and gas-phase tracers with equal emission source strengths at 46 MPC locations are used to study the balance between local pollution build-up and pollution export, either vertically into the upper troposphere or horizontally in the lower troposphere. The insoluble gas-phase tracers with fixed lifetimes are transported with the atmospheric circulation, while the aerosol tracers also undergo gravitational sedimentation as well as dry and wet deposition processes. The strength of low-level tracer export depends on the location of the emission source and prevailing meteorology, in particular on atmospheric stability and the height of the boundary layer and the mixing out of this layer. In contrast, vertical transport of tracer mass depends on the tracer's solubility: the more soluble a tracer is, the less mass reaches altitudes above five kilometers. Hence, the mass of insoluble gas-phase tracer above five kilometers can be up to ten times higher than the hydrophilic aerosol mass from the same source. In the case of aerosol tracers, pollution build-up around the source is determined by meteorological factors which have only indirect effects on tracer lifetime, like surface wind, boundary layer height, and turbulent mixing, as well as those which affect the lifetime of the tracers such as precipitation. The longer a tracer stays in the atmosphere, the lower is the relative importance of the location of the source to the atmospheric mass, and thus the lower is the relative local pollution build-up. We further use aerosol deposition fields to estimate regions with high deposition, that is more than 1% or more than 5% of the corresponding tracer emission deposited in this region. In doing so, we find that the high deposition areas are larger for aerosols with diameters of 10.0 μm, and these differ less between the MPCs than for aerosols with diameters smaller than 2.5 μm due to faster deposition. Furthermore, cities in regions with high precipitation rates or unfavorable geographic locations, e.g., in a basin, suffer most of this high deposition. Most of the high deposition occurs over land, although about 50% of the MPCs are located along coastlines. By folding the aerosol deposition fields with geographical distributions of cropland, pasture, and forest, the impact on different land ecosystems is assessed. In general, forest is exposed most to deposition from MPCs while pastureland is least affected. Moreover, the impact on humans, measured with a threshold exceedance of pollutant surface mixing ratios, is more dependent on population densities than on the size of the area with a certain mixing ratio.

Artificially increasing the albedo of marine boundary layer clouds by the mechanical emission of sea spray aerosol has been proposed as a geoengineering technique to slow the warming caused by anthropogenic greenhouse gases. A previous global model study (Korhonen et al., 2010) found that only modest increases (< 20%) and sometimes even decreases in cloud drop number (CDN) concentrations would result from emission scenarios calculated using a windspeed dependent geoengineering flux parameterisation. Here we extend that work to examine the conditions under which decreases in CDN can occur, and use three independent global models to quantify maximum achievable CDN changes. We find that decreases in CDN can occur when at least three of the following conditions are met: the injected particle number is < 100 cm−3, the injected diameter is > 250–300 nm, the background aerosol loading is large (≥ 150 cm−3) and the in-cloud updraught velocity is low (< 0.2 m s−1). With lower background loadings and/or increased updraught velocity, significant increases in CDN can be achieved. None of the global models predict a decrease in CDN as a result of geoengineering, although there is considerable diversity in the calculated efficiency of geoengineering, which arises from the diversity in the simulated marine aerosol distributions. All three models show a small dependence of geoengineering efficiency on the injected particle size and the geometric standard deviation of the injected mode. However, the achievability of significant cloud drop enhancements is strongly dependent on the cloud updraught speed. With an updraught speed of 0.1 m s−1 a global mean CDN of 375 cm−3 (previously estimated to cancel the forcing caused by CO2 doubling) is achievable in only about 50% of grid boxes which have > 50% cloud cover, irrespective of the amount of aerosol injected. But at stronger updraft speeds (0.2 m s−1), higher values of CDN are achievable due to the elevated in-cloud supersaturations. Achieving a value of 375 cm−3 in regions dominated by stratocumulus clouds with relatively weak updrafts cannot be attained regardless of the number of injected particles, thereby limiting the efficacy of sea spray geoengineering.

We present a numerical modelling study investigating the impact of mineral dust on cloud formation over the Eastern Mediterranean for two case studies: (i) 25 September 2008 and (ii) 28/29 January 2003. In both cases dust plumes crossed the Mediterranean and interacted with clouds forming along frontal systems. For our investigation we used the fully online coupled model WRF-chem. The results show that increased aerosol concentrations due to the presence of mineral dust can enhance the formation of ice crystals. This leads to slight shifts of the spatial and temporal precipitation patterns compared to scenarios where dust was not considered to act as ice nuclei. However, the total amount of precipitation did not change significantly. The only exception occurred when dust entered into an area of orographic ascent, causing glaciation of the clouds, leading to a local enhancement of rainfall. The impact of dust particles acting as giant cloud condensation nuclei on precipitation formation was found to be small. Based on our simulations the contribution of dust to the CCN population is potentially significant only for warm phase clouds. Nevertheless, the dust-induced differences in the microphysical structure of the clouds can contribute to a significant radiative forcing, which is important from a climate perspective.

Organics dominate the composition of the atmospheric aerosol, especially in the fine mode, influencing some of its characteristics such as the hygroscopicity, which is of climatic relevance for the Earth system. This study targets an improvement in the description of organic aerosols suitable for large-scale modelling, making use of recent developments based on laboratory and field measurements. In addition to the organic mass and particle number distribution, the proposed method keeps track of the oxidation state of the aerosol based on the OH exposure time, describing some of its chemical characteristics. This study presents the application of the method in a global chemistry climate model, investigates the sensitivity to process formulations and emission assignments, provides a comparison with observations and analyses the climate impact. Even though the organic aerosol mass distribution is hardly affected by the new formulation, it shows impacts (regionally of the order of 10 % to 20 %) on parameters directly influencing climate via the direct and indirect aerosol effects. Furthermore, the global distribution of the organic O:C ratio is analysed in detail, leading to different regimes in the oxidation state: low O:C ratios over the tropical continents due to small OH concentrations caused by OH depletion in chemical reactions, and enhanced oxidation states over the tropical oceans based on less OH scavengers and at high altitudes due to longer atmospheric residence time. Due to the relation between O:C ratio and the aerosol hygroscopicity the ageing results in a more physically and chemically consistent description of aerosol water uptake by the organic aerosol. In comparison with observations reasonable agreement for the O:C ratio within the limits of a global model of the simulations is achieved.

The atmospheric chemistry general circulation model EMAC has been used to estimate the impact of anthropogenic emission changes on global and regional air quality in recent and future years (2005, 2010, 2025 and 2050). The emission scenario assumes that population and economic growth largely determine energy and food consumption and consequent pollution sources with the current technologies ("business as usual"). This scenario is chosen to show the effects of not implementing legislation to prevent additional climate change and growing air pollution, other than what is in place for the base year 2005, representing a pessimistic (but plausible) future. By comparing with recent observations, it is shown that the model reproduces the main features of regional air pollution distributions though with some imprecisions inherent to the coarse horizontal resolution (~100 km) and simplified bottom-up emission input. To identify possible future hot spots of poor air quality, a multi pollutant index (MPI), suited for global model output, has been applied. It appears that East and South Asia and the Middle East represent such hotspots due to very high pollutant concentrations, while a general increase of MPIs is observed in all populated regions in the Northern Hemisphere. In East Asia a range of pollutant gases and fine particulate matter (PM2.5) is projected to reach very high levels from 2005 onward, while in South Asia air pollution, including ozone, will grow rapidly towards the middle of the century. Around the Persian Gulf, where natural PM2.5 concentrations are already high (desert dust), ozone levels are expected to increase strongly. The population weighted MPI (PW-MPI), which combines demographic and pollutant concentration projections, shows that a rapidly increasing number of people worldwide will experience reduced air quality during the first half of the 21st century. Following this business as usual scenario, it is projected that air quality for the global average citizen in 2050 would be almost comparable to that for the average citizen in East Asia in the year 2005, which underscores the need to pursue emission reductions.

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 new global anthropogenic emission inventory (EDGAR-CIRCE) of gas and aerosol pollutants has been incorporated in the chemistry general circulation model EMAC (ECHAM5/MESSy Atmospheric Chemistry). A relatively high horizontal resolution simulation is performed for the years 2005–2008 to evaluate the capability of the model and the emissions to reproduce observed aerosol concentrations and aerosol optical depth (AOD) values. Model output is compared with observations from different measurement networks (CASTNET, EMEP and EANET) and AODs from remote sensing instruments (MODIS and MISR). A good spatial agreement of the distribution of sulfate and ammonium aerosol is found when compared to observations, while calculated nitrate aerosol concentrations show some discrepancies. The simulated temporal development of the inorganic aerosols is in line with measurements of sulfate and nitrate aerosol, while for ammonium aerosol some deviations from observations occur over the USA, due to the wrong temporal distribution of ammonia gas emissions. The calculated AODs agree well with the satellite observations in most regions, while negative biases are found for the equatorial area and in the dust outflow regions (i.e. Central Atlantic and Northern Indian Ocean), due to an underestimation of biomass burning and aeolian dust emissions, respectively. Aerosols and precursors budgets for five different regions (North America, Europe, East Asia, Central Africa and South America) are calculated. Over East-Asia most of the emitted aerosols (precursors) are also deposited within the region, while in North America and Europe transport plays a larger role. Further, it is shown that a simulation with monthly varying anthropogenic emissions typically improves the temporal correlation by 5–10% compared to one with constant annual emissions.

In this study we report measurements of hydrogen peroxide (H2O2), methyl hydroperoxide* (MHP* as a proxy of MHP based on an unspecific measurement of total organic peroxides) and formaldehyde (HCHO) from the HOx OVer EuRope (HOOVER) project (HOx = OH+HO2). HOOVER included two airborne field campaigns, in October 2006 and July 2007. Measurement flights were conducted from the base of operation Hohn (Germany, 54° N, 9° E) towards the Mediterranean and to the subpolar regions over Norway. We find negative concentration gradients with increasing latitude throughout the troposphere for H2O2 and CH3OOH*. In contrast, observed HCHO is almost homogeneously distributed over central and northern Europe and is elevated over the Mediterranean. In general, the measured gradients tend to be steepest entering the Mediterranean region, where we also find the highest abundances of the 3 species. Mixing ratios of these tracers generally decrease with altitude. H2O2 and CH3OOH* show maxima above the boundary layer at 2–5 km, being more distinct over southern than over northern Europe. We also present a comparison of our data with simulations by two global 3-D-models, MATCH-MPIC and EMAC, and with the box model CAABA. The models realistically represent altitude and latitude gradients for both HCHO and hydroperoxides (ROOH). In contrast, the models have problems reproducing the absolute mixing ratios, in particular of H2O2. Large uncertainties about retention coefficients and cloud microphysical parameters suggest that cloud scavenging might be a large source of error for the simulation of H2O2. A sensitivity study with EMAC shows a strong influence of cloud and precipitation scavenging on the budget of H2O2 as simulations improve significantly with this effect switched off.

We present version 3.0 of the atmospheric chemistry box model CAABA/MECCA. In addition to a complete update of the rate coefficients to the most recent recommendations, a number of new features have been added: chemistry in multiple aerosol size bins; automatic multiple simulations reaching steady-state conditions; Monte-Carlo simulations with randomly varied rate coefficients within their experimental uncertainties; calculations along Lagrangian trajectories; mercury chemistry; more detailed isoprene chemistry; tagging of isotopically labeled species. Further changes have been implemented to make the code more user-friendly and to facilitate the analysis of the model results. Like earlier versions, CAABA/MECCA-3.0 is a community model published under the GNU General Public License.

The Modular Earth Submodel System (MESSy) is an open, multi-institutional project providing a strategy for developing comprehensive Earth System Models (ESMs) with highly flexible complexity. The first version of the MESSy infrastructure and process submodels, mainly focusing on atmospheric chemistry, has been successfully coupled to an atmospheric General Circulation Model (GCM) expanding it into an Atmospheric Chemistry GCM (AC-GCM) for nudged simulations and into a Chemistry Climate Model (CCM) for climate simulations. Here, we present the second development cycle of MESSy, which comprises (1) an improved and extended infrastructure for the basemodel independent coupling of process-submodels, (2) new, highly valuable diagnostic capabilities for the evaluation with observational data and (3) an improved atmospheric chemistry setup. With the infrastructural changes, we place the headstone for further model extensions from a CCM towards a comprehensive ESM. The new diagnostic submodels will be used for regular re-evaluations of the continuously further developing model system. The updates of the chemistry setup are briefly evaluated.

We present a new aerosol microphysics and gas aerosol partitioning submodel (Global Modal-aerosol eXtension, GMXe) implemented within the ECHAM/MESSy Atmospheric Chemistry model (EMAC, version 1.8). The submodel is computationally efficient and is suitable for medium to long term simulations with global and regional models. The aerosol size distribution is treated using 7 log-normal modes and has the same microphysical core as the M7 submodel (Vignati et al., 2004). The main developments in this work are: (i) the extension of the aerosol emission routines and the M7 microphysics, so that an increased (and variable) number of aerosol species can be treated (new species include sodium and chloride, and potentially magnesium, calcium, and potassium), (ii) the coupling of the aerosol microphysics to a choice of treatments of gas/aerosol partitioning to allow the treatment of semi-volatile aerosol, and, (iii) the implementation and evaluation of the developed submodel within the EMAC model of atmospheric chemistry. Simulated concentrations of black carbon, particulate organic matter, dust, sea spray, sulfate and ammonium aerosol are shown to be in good agreement with observations (for all species at least 40% of modeled values are within a factor of 2 of the observations). The distribution of nitrate aerosol is compared to observations in both clean and polluted regions. Concentrations in polluted continental regions are simulated quite well, but there is a general tendency to overestimate nitrate, particularly in coastal regions (geometric mean of modelled values/geometric mean of observed data ≈2). In all regions considered more than 40% of nitrate concentrations are within a factor of two of the observations. Marine nitrate concentrations are well captured with 96% of modeled values within a factor of 2 of the observations.

In this study we use the ECHAM/MESSy Atmospheric Chemistry (EMAC) model to simulate global fields of the effective hygroscopicity parameter κ which approximately describes the influence of chemical composition on the cloud condensation nucleus (CCN) activity of aerosol particles. The obtained global mean values of κ at the Earth's surface are 0.27±0.21 for continental and 0.72±0.24 for marine regions (arithmetic mean ± standard deviation). These values are the internally mixed κ calculated across the Aitken and accumulation modes. The mean κ values are in good agreement with previous estimates based on observational data, but the model standard deviation for continental regions is higher. Over the continents, the regional distribution appears fairly uniform, with κ values mostly in the range of 0.1–0.4. Lower values over large arid regions and regions of high organic loading lead to reduced continental average values for Africa and South America (0.15–0.17) compared to the other continents (0.21–0.36). Marine regions show greater variability with κ values ranging from 0.9–1.0 in remote regions to 0.4–0.6 in continental outflow regions where the highly hygroscopic sea spray aerosol mixes with less hygroscopic continental aerosol. Marine κ values as low as 0.2–0.3 are simulated in the outflow from the Sahara desert. At the top of the planetary boundary layer the κ values can deviate substantially from those at the surface (up to 30%) – especially in marine and coastal regions. In moving from the surface to the height of the planetary boundary layer, the global average marine κ value reduces by 20%. Thus, surface observations may not always be representative for the altitudes where cloud formation mostly occurs. In a pre-industrial model scenario, the κ values tend to be higher over marine regions and lower over the continents, because the anthropogenic particulate matter is on average less hygroscopic than sea-spray but more hygroscopic than the natural continental background aerosol (dust and organic matter). In regions influenced by desert dust the particle hygroscopicity has increased strongly as the mixing of air pollutants with mineral particles typically enhances the κ values by a factor of 2–3 above the initial value of ≈0.005.

The atmospheric chemistry general circulation model ECHAM5/MESSy (EMAC) and the atmospheric chemistry box model CAABA are extended by a computationally very efficient submodel for atmospheric chemistry, E4CHEM. It focuses on stratospheric chemistry but also includes background tropospheric chemistry. It is based on the chemistry of MAECHAM4-CHEM and is intended to serve as a simple and fast alternative to the flexible but also computationally more demanding submodel MECCA. In a model setup with E4CHEM, EMAC is now also suitable for simulations of longer time scales. The reaction mechanism contains basic O3, CH4, CO, HOx, NOx, and ClOx gas phase chemistry. In addition, E4CHEM includes optional fast routines for heterogeneous reactions on sulphate aerosols and polar stratospheric clouds (substituting the existing submodels PSC and HETCHEM), and scavenging (substituting the existing submodel SCAV). We describe the implementation of E4CHEM into the MESSy structure of CAABA and EMAC. For some species the steady state in the box model differs by up to 100% when compared to results from CAABA/MECCA due to different reaction rates. After an update of the reaction rates in E4CHEM the mixing ratios in both boxmodel and 3-D model simulations are in satisfactory agreement with the results from a simulation where MECCA with a similar chemistry scheme was employed. Finally, a comparison against a simulation with a more complex and already evaluated chemical mechanism is presented in order to discuss shortcomings associated with the simplification of the chemical mechanism.

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.