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A mineralogical database is included in the simulation of mineral dust atmospheric life cycle for the chemistry and transport model COSMO5.05-MUSCAT. Evaluation of the ability of the model to reproduce the atmospheric drivers and the spatial-temporal resolution of mineral dust in the atmosphere is done through comparisons with remote sensing measurements in the Sahara Desert region for January-February 2022. Results show simultaneously good agreements and suggest that discrepancies could be explained due to the methods used for calculating mineral dust in the atmosphere not considering compositional differences.

Mineral dust aerosols are composed of a complex assemblage of various minerals depending on the region in which they originated. Given the different mineral composition of desert dust aerosols, different physicochemical properties and therefore varying climate effects are expected. Despite the known regional variations in mineral composition, chemical transport models typically assume that mineral dust aerosols have uniform composition. This study adds, for the first time, mineralogical information to the mineral dust emission scheme used in the chemical transport model COSMO–MUSCAT. We provide a detailed description of the implementation of the mineralogical database, GMINER (), together with a specific set of physical parameterizations in the model's mineral dust emission module, which led to a general improvement of the model performance when comparing the simulated mineral dust aerosols with measurements over the Sahara region for January–February 2022. The simulated mineral dust aerosol vertical distribution is tested by a comparison with aerosol lidar measurements from the lidar system PollyXT , located at Cape Verde. For a lofted mineral dust aerosol layer on 2 February at 05:00 UTC the lidar retrievals yield a dust mass concentration peak of 156 µgm-3 , while the model calculates the mineral dust peak at 136 µgm-3. The results highlight the possibility of using the model with resolved mineral dust composition for interpretation of the lidar measurements since a higher absorption in the UV–Vis wavelengths is correlated with particles having a higher hematite content. Additionally, the comparison with in situ mineralogical measurements of dust aerosol particles shows that more of them are needed for model evaluation. [ABSTRACT FROM AUTHOR]

Mineral dust aerosols are composed from a complex assemblage of various minerals depending on the region they originated. Giving the different mineral composition of desert dust aerosols, different physico-chemical properties and therefore varying climate effects are expected. Despite the known regional variations in mineral composition, chemical transport models typically assume that mineral dust aerosol have uniform composition. This study adds, for the first time, mineralogical information to the mineral dust emission scheme used in the chemical transport model COSMO-MUSCAT. We provide a detailed description of the implementation of the mineralogical database, GMINER (Nickovic et al., 2012), together with a specific set of physical parametrizations in the model's mineral dust emission module. These changes lead to a general improvement of the model performance when comparing the simulated mineral dust aerosols with measurements over the Sahara Desert region for January–February 2022. The simulated mineral dust aerosol vertical distribution is tested by a comparison with aerosol lidar measurements from the lidar system PollyXT, located at Cape Verde. For a lofted mineral dust aerosol layer on the 2 February 5:00 UTC the lidar retrievals yield on a dust mass concentration peak of 156 μg/m3 while the model calculates the mineral dust peak at 136 μg/m3. The results highlight the possibility of using the model with resolved mineral dust composition for interpretation of the lidar measurements since higher absorption the UV-VIS wavelength is correlated to particles having higher hematite content. Additionally, the comparison with in-situ mineralogical measurements of dust aerosol particles show how important they are, but also that more of them are needed for model evaluation. [ABSTRACT FROM AUTHOR]

Mineral dust aerosols are composed from a complex assemblage of various minerals depending on the region they originated. Giving the different mineral composition of desert dust aerosols, different physico-chemical properties and therefore varying climate effects are expected. Despite the known regional variations in mineral composition, chemical transport models typically assume that mineral dust 5 aerosols have uniform composition. This study adds, for the first time, mineralogical information to the mineral dust emission scheme used in the chemical transport model COSMO-MUSCAT. We provide a detailed description of the implementation of the mineralogical database, GMINER (Nickovic et al., 2012), together with a specific set of physical parametrizations in the model's mineral dust emission module. These changes lead to a general improvement of the model performance when comparing the simulated mineral dust aerosols with measurements over the Sahara Desert region for January - February 2022 . 10 The simulated mineral dust aerosol vertical distribution is tested by a comparison with aerosol lidar measurements from the lidar system PollyXT, located at Cape Verde. For a lofted mineral dust aerosol layer on the 2 February 5:00 UTC the lidar retrievals yield on a dust mass concentration peak of 156 µg/m³ while the model calculates the mineral dust peak at 136 µg/m³. The results highlight the possibility of using the model with resolved mineral dust composition for interpretation of the lidar measurements since higher absorption the UV-VIS wavelength is correlated to particles having higher hematite 15 content. Additionally, the comparison with in-situ mineralogical measurements of dust aerosol particles show how important they are, but also that more of them are needed for model evaluation. [ABSTRACT FROM AUTHOR]

Wildfires are a significant source of absorbing aerosols in the atmosphere. Extreme fires in particular, such as those during the 2019–2020 Australian wildfire season (Black Summer fires), can have considerable large-scale effects. In this context, the climate impact of extreme wildfires unfolds not only because of the emitted carbon dioxide but also due to smoke aerosol released up to an altitude of 17 km. The overall aerosol effects depend on a variety of factors, such as the amount emitted, the injection height, and the composition of the burned material, and is therefore subject to considerable uncertainty. In the present study, we address the global impact caused by the exceptionally strong and high-reaching smoke emissions from the Australian wildfires using simulations with a global aerosol–climate model. We show that the absorption of solar radiation by the black carbon contained in the emitted smoke led to a shortwave radiative forcing of more than +5 Wm-2 in the southern mid-latitudes of the lower stratosphere. Subsequent adjustment processes in the stratosphere slowed down the diabatically driven meridional circulation, thus redistributing the heating perturbation on a global scale. As a result of these stratospheric adjustments, a positive temperature perturbation developed in both hemispheres, leading to additional longwave radiation emitted back to space. According to the model results, this adjustment occurred in the stratosphere within the first 2 months after the event. At the top of the atmosphere (TOA), the net effective radiative forcing (ERF) averaged over the Southern Hemisphere was initially dominated by the instantaneous positive radiative forcing of about +0.5 Wm-2 , for which the positive sign resulted mainly from the presence of clouds above the Southern Ocean. The longwave adjustments led to a compensation of the initially net positive TOA ERF, which is seen in the Southern Hemisphere, the tropics, and the northern mid-latitudes. The simulated changes in the lower stratosphere also affected the upper troposphere through a thermodynamic downward coupling. Subsequently, increased temperatures were also obtained in the upper troposphere, causing a global decrease in relative humidity, cirrus amount, and the ice water path of about 0.2 %. As a result, surface precipitation also decreased by a similar amount, which was accompanied by a weakening of the tropospheric circulation due to the given energetic constraints. In general, it appears that the radiative effects of smoke from single extreme wildfire events can lead to global impacts that affect the interplay of tropospheric and stratospheric budgets in complex ways. This emphasizes that future changes in extreme wildfires need to be included in projections of aerosol radiative forcing. [ABSTRACT FROM AUTHOR]

In Central Asia, climate and air quality are largely affected by local and long-travelled mineral dust. For the last century, the area has experienced severe land-use changes and water exploitation producing new dust sources. Today global warming causes rapid shrinking of mountain glaciers with yet unknow consequences for dust and its climate effects. Despite the importance for a growing population, only little is known about sources, transport pathways and properties of Central Asian dust. A transport study with a global aerosol-climate model is undertaken to investigate the life cycle of mineral dust in Central Asia for the period of a remote-sensing campaign in Tajikistan in 2015–2016. An initial evaluation with sun photometer measurements shows reasonable agreement for the average amount of dust, but a significant weakness of the model in reproducing the seasonality of local dust with maximum activity in summer. Source apportionment reveals a major contribution from Arabia throughout the year in accordance with observations. In the model, local sources mainly contribute in spring and autumn while summer-time dust production is underestimated. The results underline the importance of considering long-range transport and, locally, a detailed representation of atmospheric dynamics and surface characteristics for modelling dust in Central Asia.

The radiative effect of mineral dust and black carbon aerosol are investigated with aerosolclimate model simulations with fixed sea surface temperatures as boundary condition. The semi-direct effects of the absorbing aerosol are assessed as the residual between the total direct radiative effect and the instantaneous direct radiative effect of the aerosol species. For Central Asia the presence of mineral dust aerosol below a black carbon aerosol layer enhances the positive radiative effect of the black carbon aerosol.

More than 1 Tg smoke aerosol was emitted into the atmosphere by the exceptional 2019–2020 southeastern Australian wildfires. Triggered by the extreme fire heat, several deep pyroconvective events carried the smoke directly into the stratosphere. Once there, smoke aerosol remained airborne considerably longer than in lower atmospheric layers. The thick plumes traveled eastward, thereby being distributed across the high and mid-latitudes in the Southern Hemisphere, enhancing the atmospheric opacity. Due to the increased atmospheric lifetime of the smoke plume, its radiative effect increased compared to smoke that remains in lower altitudes. Global models describing aerosol-climate impacts lack adequate descriptions of the emission height of aerosols from intense wildfires. Here, we demonstrate, by a combination of aerosol-climate modeling and lidar observations, the importance of the representation of those high-altitude fire smoke layers for estimating the atmospheric energy budget. Through observation-based input into the simulations, the Australian wildfire emissions by pyroconvection are explicitly prescribed to the lower stratosphere in different scenarios. Based on our simulations, the 2019–2020 Australian fires caused a significant top-of-atmosphere (TOA) hemispheric instantaneous direct radiative forcing signal that reached a magnitude comparable to the radiative forcing induced by anthropogenic absorbing aerosol. Up to + 0.50 Wm-2 instantaneous direct radiative forcing was modeled at TOA, averaged for the Southern Hemisphere (+ 0.25 Wm-2 globally) from January to March 2020 under all-sky conditions. At the surface, on the other hand, an instantaneous solar radiative forcing of up to - 0.81 Wm-2 was found for clear-sky conditions, with the respective estimates depending on the model configuration and subject to the model uncertainties in the smoke optical properties. Since extreme wildfires are expected to occur more frequently in the rapidly changing climate, our findings suggest that high-altitude wildfire plumes must be adequately considered in climate projections in order to obtain reasonable estimates of atmospheric energy budget changes. [ABSTRACT FROM AUTHOR]

Enough of silos: develop a joint scientific agenda to understand the intertwined global crises of the Earth system. [ABSTRACT FROM AUTHOR]

More than 1 Tg smoke aerosol was emitted into the atmosphere by the exceptional 2019-2020 Southeast Australian wildfires. Triggered by the extreme fire heat, several deep pyroconvective events carried the smoke directly into the stratosphere. Once there, smoke aerosol remained airborne considerably longer than in lower atmospheric layers. The thick plumes traveled eastward thereby being distributed across the high and mid-latitude Southern Hemisphere enhancing the atmospheric opacity. Due to the increased atmospheric lifetime of the smoke plume its radiative effect increased compared to smoke that remains lower altitudes. Global models describing aerosol-climate impacts show significant uncertainties regarding the emission height of aerosols from intense wildfires. Here, we demonstrate by combination of aerosol-climate modeling and lidar observations the importance of the representation of those high-altitude fire smoke layers for estimating the atmospheric energy budget. In this observation-based approach, the Australian wildfire emissions by pyroconvection are explicitly prescribed to the lower stratosphere in different scenarios. The 2019-2020 Australian fires caused a significant top-of-atmosphere hemispheric instantaneous direct radiative forcing signal that reached a magnitude comparable to the radiative forcing induced by anthropogenic absorbing aerosol. Up to +0.50 W m-2 instantaneous direct radiative forcing was modeled at top of the atmosphere, averaged for the Southern Hemisphere for January to March 2020 under all-sky conditions. While at the surface, an instantaneous solar radiative forcing of up to -0.81 W m-2 was found for clear-sky conditions, depending on the model configuration. Since extreme wildfires are expected to occur more frequently in the rapidly changing climate, our findings suggest that deep wildfire plumes must be adequately considered in climate projections in order to obtain reasonable estimates of atmospheric energy budget changes. [ABSTRACT FROM AUTHOR]

The oxidation of dimethyl sulfide (DMS) is key for the natural sulfate aerosol formation and its climate impact. Multiphase chemistry is an important oxidation pathway but neglected in current chemistry‐climate models. Here, the DMS chemistry in the aerosol‐chemistry‐climate model ECHAM‐HAMMOZ is extended to include multiphase methane sulfonic acid (MSA) formation in deliquesced aerosol particles, parameterized by reactive uptake. First simulations agree well with observed gas‐phase MSA concentrations. The implemented formation pathways are quantified to contribute up to 60% to the sulfate aerosol burden over the Southern Ocean and Arctic/Antarctic regions. While globally the impact on the aerosol radiative forcing almost levels off, a significantly more positive solar radiative forcing of up to +0.1 W m−2 is computed in the Arctic (>60°N). The findings imply the need of both further laboratory and model studies on the atmospheric multiphase oxidation of DMS. Plain Language Summary: The emission of dimethyl sulfide (DMS) represents the largest natural reduced sulfur source into the atmosphere. There, DMS can be oxidized to sulfur dioxide, sulfuric acid, or methane sulfonic acid modifying the radiative properties of aerosol particles and clouds. DMS oxidation is represented in chemistry‐climate models by a limited number of very simplified reactions. Small changes in the parameter settings can have large effects, that's why these should be as accurate as possible. In this study, the DMS chemistry in ECHAM‐HAMMOZ was upgraded. Sensitivity simulations show variations in the natural aerosol radiative forcing due to the different schemes tested in this study. Further laboratory and process studies with models are therefore essential. Key Points: Dimethyl sulfide (DMS) chemistry in chemistry‐climate simulations extended by multiphase methane sulfonic acid (MSA) formation provides more realistic MSA gas‐phase concentrationsFormation of MSA is very sensitive toward reactive uptake on deliquesced aerosol particlesIn the Arctic, the extended DMS chemistry leads to a significantly less negative effective radiative forcing of sulfate aerosol [ABSTRACT FROM AUTHOR]

Despite advances in our understanding of ice-nucleating particles, the effect of cloud glaciation on the Earth's radiation balance has remained poorly constrained. Particularly, dust ice nuclei are believed to enhance cloud glaciation in the Northern Hemisphere. We used satellite observations of the hemispheric and seasonal contrast in cloud top phase to assess the dust-driven droplet freezing in a climate model. The required freezing efficiency for dust ice nuclei suggests that climate models glaciate too few clouds through immersion droplet freezing. After tuning, the model leads to more realistic cloudtop-phase contrasts and a dust-driven glaciation effect of 0.14 ± 0.13 W m-2 between 30°N and 60°N. Observations of cloud-top-phase contrasts provide a strong constraint for ice formation in mixed-phase clouds and may provide a weak constraint for the associated impact on radiation and precipitation. Future studies should therefore consider both the mean-state cloud-phase partitioning and cloud-phase contrasts to achieve a more accurate simulation of dust-driven cloud glaciation. Plain Language Summary Between 0°C and -38°C, clouds can be composed of cloud droplets (water), ice crystals, or some combination of the two. Water clouds reflect much more sunshine back to space compared to ice clouds and therefore have a larger cooling effect on climate. Some atmospheric particles like dust can transform water clouds into ice clouds. The Northern Hemisphere contains more of such particles, which leads to more ice clouds, as confirmed by satellite observations. We such satellite observations to constrain the effect of cloud freezing in climate models and its impact on climate. This helps make climate models and their projections of future climate more realistic. [ABSTRACT FROM AUTHOR]

Aerosol‐cloud interactions are an important source of uncertainty in current climate models. To understand and quantify the influence of ice‐nucleating particles in cloud glaciation, it is crucial to have a reliable estimation of the hemispheric and seasonal contrast in cloud top phase, which is believed to result from the higher dust aerosol loading in boreal spring. For this reason, we locate and quantify these contrasts by combining three different A‐Train cloud‐phase products for the period 2007–2010. These products rely on a spaceborne lidar, a lidar‐radar synergy, and a radiometer‐polarimeter synergy. We show that the cloud‐phase from the product combination is more reliable and that the estimation of the hemispheric and seasonal contrast has a lower error compared to the individual products. To quantify the contrast in cloud‐phase, we use the hemispheric difference in ice cloud frequency normalized by the liquid cloud frequency in the southern hemisphere between −42 °C and 0 °C. In the midlatitudes, from −15 to −30 °C, the hemispheric contrasts increase with decreasing temperature. At −30 °C, the hemispheric contrast varies from 29% to 39% for the individual cloud‐phase products and from 52% to 73% for the product combination. Similarly, in the northern hemisphere, we assess the seasonal contrast between spring and fall normalized by the liquid cloud frequency during fall. At −30 °C, the seasonal contrast ranges from 21% to 39% for the individual cloud‐phase products and from 54% to 75% for the product combination. Plain Language Summary: The influence of atmospheric particles on clouds is one of the main unknowns in climate predictions. Particularly, the cloud glaciation process and its dependence on desert dust and soot particles are not well‐understood. To better understand the differences in cloud glaciation between hemispheres, we counted liquid and ice cloud tops, as observed from four different satellites, during 4 years. Combining these observations, we could confirm a higher frequency of ice cloud tops during spring in the northern hemisphere. We found that the contrast between hemispheres is higher than previously thought. These results will help to improve our understanding of cloud glaciation processes, which can be valuable for future climate predictions and for understanding the impact of aerosols on radiation and precipitation. Key Points: A satellite product ensemble was used to locate and quantify the hemispheric and seasonal contrast in cloud top thermodynamic phaseAt −30 °C, half of the liquid cloud tops observed in the southern hemisphere would glaciate in the northern hemisphereThe new product ensemble is more reliable than the individual products and suggests a previous underestimation of the cloud‐phase contrasts [ABSTRACT FROM AUTHOR]

It was hypothesized that using mineral dust emission climatologies in global chemistry climate models (GCCMs), i.e. prescribed monthly-mean dust emissions representative of a specific year, may lead to misrepresentations of strong dust burst events. This could result in a negative bias of model dust concentrations compared to observations for these episodes. Here, we apply the aerosol microphysics submodel MADE3 (Modal Aerosol Dynamics model for Europe, adapted for global applications, third generation) as part of the ECHAM/MESSy Atmospheric Chemistry (EMAC) general circulation model. We employ two different representations of mineral dust emissions for our model simulations: (i) a prescribed monthly-mean climatology of dust emissions representative of the year 2000 and (ii) an online dust parametrization which calculates wind-driven mineral dust emissions at every model time step. We evaluate model results for these two dust representations by comparison with observations of aerosol optical depth from ground-based station data. The model results show a better agreement with the observations for strong dust burst events when using the online dust representation compared to the prescribed dust emissions setup. Furthermore, we analyse the effect of increasing the vertical and horizontal model resolution on the mineral dust properties in our model. We compare results from simulations with T42L31 and T63L31 model resolution (2.8∘×2.8∘ and 1.9∘×1.9∘ in latitude and longitude, respectively; 31 vertical levels) with the reference setup (T42L19). The different model versions are evaluated against airborne in situ measurements performed during the SALTRACE mineral dust campaign (Saharan Aerosol Long-range Transport and Aerosol-Cloud Interaction Experiment, June–July 2013), i.e. observations of dust transported from the Sahara to the Caribbean. Results show that an increased horizontal and vertical model resolution is able to better represent the spatial distribution of airborne mineral dust, especially in the upper troposphere (above 400 hPa). Additionally, we analyse the effect of varying assumptions for the size distribution of emitted dust but find only a weak sensitivity concerning these changes. The results of this study will help to identify the model setup best suited for future studies and to further improve the representation of mineral dust particles in EMAC-MADE3. [ABSTRACT FROM AUTHOR]

Atmospheric aerosol particles are the precondition for the formation of cloud droplets and therefore have large influence on the microphysical and radiative properties of clouds. In this work, four different methods to derive or measure number concentrations of cloud condensation nuclei (CCN) were analyzed and compared for present-day aerosol conditions: (i) a model parameterization based on simulated particle concentrations, (ii) the same parameterization based on gravimetrical particle measurements, (iii) direct CCN measurements with a CCN counter, and (iv) lidar-derived and in situ measured vertical CCN profiles. In order to allow for sensitivity studies of the anthropogenic impact, a scenario to estimate the maximum CCN concentration under peak aerosol conditions of the mid-1980s in Europe was developed as well. In general, the simulations are in good agreement with the observations. At ground level, average values between 0.7 and 1.5×109 CCNm-3 at a supersaturation of 0.2 % were found with the different methods under present-day conditions. The discrimination of the chemical species revealed an almost equal contribution of ammonium sulfate and ammonium nitrate to the total number of CCN for present-day conditions. This was not the case for the peak aerosol scenario, in which it was assumed that no ammonium nitrate was formed while large amounts of sulfate were present, consuming all available ammonia during ammonium sulfate formation. The CCN number concentration at five different supersaturation values has been compared to the measurements. The discrepancies between model and in situ observations were lowest for the lowest (0.1 %) and highest supersaturations (0.7 %). For supersaturations between 0.3 % and 0.5 %, the model overestimated the potentially activated particle fraction by around 30 %. By comparing the simulation with observed profiles, the vertical distribution of the CCN concentration was found to be overestimated by up to a factor of 2 in the boundary layer. The analysis of the modern (year 2013) and the peak aerosol scenario (expected to be representative of the mid-1980s over Europe) resulted in a scaling factor, which was defined as the quotient of the average vertical profile of the peak aerosol and present-day CCN concentration. This factor was found to be around 2 close to the ground, increasing to around 3.5 between 2 and 5 km and approaching 1 (i.e., no difference between present-day and peak aerosol conditions) with further increasing height. [ABSTRACT FROM AUTHOR]

The spatial distribution and properties of submicron organic aerosol (OA) are among the key sources of uncertainty in our understanding of aerosol effects on climate. Uncertainties are particularly large over remote regions of the free troposphere and Southern Ocean, where very few data have been available and where OA predictions from AeroCom Phase II global models span 2 to 3 orders of magnitude, greatly exceeding the model spread over source regions. The (nearly) pole-to-pole vertical distribution of non-refractory aerosols was measured with an aerosol mass spectrometer onboard the NASA DC-8 aircraft as part of the Atmospheric Tomography (ATom) mission during the Northern Hemisphere summer (August 2016) and winter (February 2017). This study presents the first extensive characterization of OA mass concentrations and their level of oxidation in the remote atmosphere. OA and sulfate are the major contributors by mass to submicron aerosols in the remote troposphere, together with sea salt in the marine boundary layer. Sulfate was dominant in the lower stratosphere. OA concentrations have a strong seasonal and zonal variability, with the highest levels measured in the lower troposphere in the summer and over the regions influenced by biomass burning from Africa (up to 10 µgsm-3). Lower concentrations (∼0.1 –0.3 µgsm-3) are observed in the northern middle and high latitudes and very low concentrations (<0.1 µgsm-3) in the southern middle and high latitudes. The ATom dataset is used to evaluate predictions of eight current global chemistry models that implement a variety of commonly used representations of OA sources and chemistry, as well as of the AeroCom-II ensemble. The current model ensemble captures the average vertical and spatial distribution of measured OA concentrations, and the spread of the individual models remains within a factor of 5. These results are significantly improved over the AeroCom-II model ensemble, which shows large overestimations over these regions. However, some of the improved agreement with observations occurs for the wrong reasons, as models have the tendency to greatly overestimate the primary OA fraction and underestimate the secondary fraction. Measured OA in the remote free troposphere is highly oxygenated, with organic aerosol to organic carbon (OA / OC) ratios of ∼2.2 –2.8, and is 30 %–60 % more oxygenated than in current models, which can lead to significant errors in OA concentrations. The model–measurement comparisons presented here support the concept of a more dynamic OA system as proposed by Hodzic et al. (2016), with enhanced removal of primary OA and a stronger production of secondary OA in global models needed to provide better agreement with observations. [ABSTRACT FROM AUTHOR]

Mineral dust particles play an important role in the climate system, by e.g. interacting with solar and terrestrial radiation or facilitating the formation of cloud droplets. Additionally, dust particles can act as very efficient ice nuclei in cirrus clouds. Many Global Chemistry Climate Models (GCCMs) use prescribed monthly mean mineral dust emissions representative of a specific year, based on a climatology. It was hypothesized that using dust emission climatologies may lead to misrepresentations of strong dust burst episodes, resulting in a negative bias of model dust concentrations compared to observations for these episodes. Here, we apply the aerosol microphysics submodel MADE3 (Modal Aerosol Dynamics model for Europe, adapted for global applications, third generation) as part of the ECHAM/MESSy Atmospheric Chemistry (EMAC) general circulation model. We employ two different representations of mineral dust for our model simulations: i) a prescribed monthly-mean climatology of dust emissions representative of the year 2000; ii) an online dust parametrization which calculates wind-driven mineral dust emissions at every model time-step. We evaluate model results for these two dust representations by comparison with observations of aerosol optical depth from ground-based station data. The model results show a better agreement with the observations for strong dust burst events when using the online dust representation compared to the prescribed dust emissions setup. Furthermore, we analyse the effect of increasing the vertical and horizontal model resolution on mineral dust properties in our model. The model is evaluated against airborne in situ measurements performed during the SALTRACE mineral dust campaign (Saharan Aerosol Long-range Transport and Aerosol-Cloud Interaction Experiment, June/July 2013), i.e. observations of dust transported from the Sahara to the Caribbean. Results show that an increased horizontal and vertical model resolution is able to better represent the spatial distribution of airborne mineral dust, especially in the upper troposphere (above 400 hPa). Additionally, we analyse the effect of varying assumptions for the size distribution of emitted dust. The results of this study will help to identify the model setup best suited for future studies and to further improve the representation of mineral dust particles in EMAC-MADE3. [ABSTRACT FROM AUTHOR]

A new cloud microphysical scheme including a detailed parameterization for aerosol-driven ice formation in cirrus clouds is implemented in the global ECHAM/MESSy Atmospheric Chemistry (EMAC) chemistry–climate model and coupled to the third generation of the Modal Aerosol Dynamics model for Europe adapted for global applications (MADE3) aerosol submodel. The new scheme is able to consistently simulate three regimes of stratiform clouds – liquid, mixed-, and ice-phase (cirrus) clouds – considering the activation of aerosol particles to form cloud droplets and the nucleation of ice crystals. In the cirrus regime, it allows for the competition between homogeneous and heterogeneous freezing for the available supersaturated water vapor, taking into account different types of ice-nucleating particles, whose specific ice-nucleating properties can be flexibly varied in the model setup. The new model configuration is tuned to find the optimal set of parameters that minimizes the model deviations with respect to observations. A detailed evaluation is also performed comparing the model results for standard cloud and radiation variables with a comprehensive set of observations from satellite retrievals and in situ measurements. The performance of EMAC-MADE3 in this new coupled configuration is in line with similar global coupled models and with other global aerosol models featuring ice cloud parameterizations. Some remaining discrepancies, namely a high positive bias in liquid water path in the Northern Hemisphere and overestimated (underestimated) cloud droplet number concentrations over the tropical oceans (in the extratropical regions), which are both a common problem in these kinds of models, need to be taken into account in future applications of the model. To further demonstrate the readiness of the new model system for application studies, an estimate of the anthropogenic aerosol effective radiative forcing (ERF) is provided, showing that EMAC-MADE3 simulates a relatively strong aerosol-induced cooling but within the range reported in the Intergovernmental Panel on Climate Change (IPCC) assessments. [ABSTRACT FROM AUTHOR]

To estimate the global co-variability between mineral dust aerosol and cloud glaciation, we combined an aerosol model reanalysis with satellite retrievals of cloud thermodynamic phase. We used the CALIPSO-GOCCP product from the A-Train satellite constellation to assess whether clouds are composed of liquid or ice and the MACC reanalysis to estimate the dust mixing ratio in the atmosphere. Night-time retrievals within a temperature range from +3 to −42 ∘ C for the period 2007–2010 were included. The results confirm that the cloud thermodynamic phase is highly dependent on temperature and latitude. However, at middle and high latitudes, at equal temperature and within narrow constraints for humidity and static stability, the average frequency of fully glaciated clouds increases by +5 to +10% for higher mineral dust mixing ratios. The discrimination between humidity and stability regimes reduced the confounding influence of meteorology on the observed relationship between dust and cloud ice. Furthermore, for days with similar mixing ratios of mineral dust, the cloud ice occurrence frequency in the Northern Hemisphere was found to be higher than in the Southern Hemisphere at −30 ∘ C but lower at −15 ∘ C. This contrast may suggest a difference in the susceptibility of cloud glaciation to the presence of dust. Based on previous studies, the differences at −15 ∘ C could be explained by higher feldspar fractions in the Southern Hemisphere, while the higher freezing efficiency of clay minerals in the Northern Hemisphere may explain the differences at −30 ∘ C. [ABSTRACT FROM AUTHOR]

Natural sea-salt aerosols, when interacting with anthropogenic emissions, can enhance the formation of particulate nitrate. This enhancement has been suggested to increase the direct radiative forcing of nitrate, called the "mass-enhancement effect". Through a size-resolved dynamic mass transfer modeling approach, we show that interactions with sea salt shift the nitrate from sub- to super-micron-sized particles ("redistribution effect"), and hence this lowers its efficiency for light extinction and reduces its lifetime. The redistribution effect overwhelms the mass-enhancement effect and significantly moderates nitrate cooling; e.g., the nitrate-associated aerosol optical depth can be reduced by 10 %–20 % over European polluted regions during a typical sea-salt event, in contrast to an increase by ∼10 % when only accounting for the mass-enhancement effect. Global model simulations indicate significant redistribution over coastal and offshore regions worldwide. Our study suggests a strong buffering by natural sea-salt aerosols that reduces the climate forcing of anthropogenic nitrate, which had been expected to dominate the aerosol cooling by the end of the century. Comprehensive considerations of this redistribution effect foster better understandings of climate change and nitrogen deposition. [ABSTRACT FROM AUTHOR]

A new cloud microphysical scheme including a detailed parameterization for aerosol-driven ice formation in cirrus clouds is implemented in the global chemistry climate model EMAC and coupled to the aerosol submodel MADE3. The new scheme is able to consistently simulate three regimes of stratiform clouds (liquid, mixed- and ice-phase (cirrus) clouds), considering the impact of aerosol on the activation of cloud droplets and the nucleation of ice crystals. In the cirrus regime, it accounts for the competition between homogeneous and heterogeneous freezing for the available supersaturated water vapor, taking into account different types of ice-nucleating particles, whose specific ice-nucleating properties can be flexibly varied in the model setup. The new model configuration was tuned using satellite data to find the optimal set of parameters that reproduces the observations. A detailed evaluation is also performed comparing the model results for standard cloud and radiation variables with a comprehensive set of observations from satellite retrievals and in situ measurements. The performance of EMAC-MADE3 in this new coupled configuration is in line with similar global coupled models and with other global aerosol models featuring ice cloud parameterizations. Some remaining discrepancies, especially with regard to ice crystal number concentrations in cirrus, which are a common problem of this kind of models, need to be the subject of future investigations. To further demonstrate the readiness of the new model system for application studies, an estimate of the global anthropogenic aerosol radiative forcing is provided and discussed in the context of the CMIP5 results for the IPCC. [ABSTRACT FROM AUTHOR]

Aerosol particles can contribute to the Arctic amplification (AA) by direct and indirect radiative effects. Specifically, black carbon (BC) in the atmosphere, and when deposited on snow and sea ice, has a positive warming effect on the top-of-atmosphere (TOA) radiation balance during the polar day. Current climate models, however, are still struggling to reproduce Arctic aerosol conditions. We present an evaluation study with the global aerosol-climate model ECHAM6.3-HAM2.3 to examine emission-related uncertainties in the BC distribution and the direct radiative effect of BC. The model results are comprehensively compared against the latest ground and airborne aerosol observations for the period 2005–2017, with a focus on BC. Four different setups of air pollution emissions are tested. The simulations in general match well with the observed amount and temporal variability in near-surface BC in the Arctic. Using actual daily instead of fixed biomass burning emissions is crucial for reproducing individual pollution events but has only a small influence on the seasonal cycle of BC. Compared with commonly used fixed anthropogenic emissions for the year 2000, an up-to-date inventory with transient air pollution emissions results in up to a 30 % higher annual BC burden locally. This causes a higher annual mean all-sky net direct radiative effect of BC of over 0.1 W m -2 at the top of the atmosphere over the Arctic region (60–90 ∘ N), being locally more than 0.2 W m -2 over the eastern Arctic Ocean. We estimate BC in the Arctic as leading to an annual net gain of 0.5 W m -2 averaged over the Arctic region but to a local gain of up to 0.8 W m -2 by the direct radiative effect of atmospheric BC plus the effect by the BC-in-snow albedo reduction. Long-range transport is identified as one of the main sources of uncertainties for ECHAM6.3-HAM2.3, leading to an overestimation of BC in atmospheric layers above 500 hPa, especially in summer. This is related to a misrepresentation in wet removal in one identified case at least, which was observed during the ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) summer aircraft campaign. Overall, the current model version has significantly improved since previous intercomparison studies and now performs better than the multi-model average in the Aerosol Comparisons between Observation and Models (AEROCOM) initiative in terms of the spatial and temporal distribution of Arctic BC. [ABSTRACT FROM AUTHOR]

The spatial distribution and properties of submicron organic aerosols (OA) are among the key sources of uncertainty in our understanding of aerosol effects on climate. Uncertainties are particularly large over remote regions of the free troposphere and Southern Ocean, where very little data has been available, and where OA predictions from AeroCom Phase II global models span a factor of 400–1000, greatly exceeding the model spread over source regions. The (nearly) pole-to-pole vertical distribution of non-refractory aerosols was measured with an aerosol mass spectrometer onboard the NASA DC8 aircraft as part of the Atmospheric Tomography (ATom) mission during the northern hemisphere summer (August 2016) and winter (February 2017). This study presents the first extensive characterization of OA mass concentrations and their level of oxidation in the remote atmosphere. OA and sulfate are the major contributors by mass to submicron aerosols in the remote troposphere, together with sea salt in the marine boundary layer. Sulfate was dominant in the lower stratosphere. OA concentrations have a strong seasonal and zonal variability, with the highest levels measured in the summer and over the regions influenced by the biomass burning from Africa (up to 10 μg sm−3). Lower concentrations (~ 0.1–0.3 μg sm−3) are observed in the northern mid- and high-latitudes and very low concentrations (< 0.1 μg sm−3) in the southern mid- and high-latitudes. The ATom dataset is used to evaluate predictions of eight current global chemistry models that implement a variety of commonly used representations of OA sources and chemistry, as well as of the AeroCom-II ensemble. The current model ensemble captures the average vertical and spatial distribution of measured OA concentrations, and the spread of the individual models remains within a factor of 5. These results are significantly improved over the AeroCom-II model ensemble, which shows large overestimations over these regions. However, some of the improved agreement with observations occurs for the wrong reasons, as models have the tendency to greatly overestimate the primary OA fraction, and underestimate the secondary fraction. Measured OA in the remote free troposphere are highly oxygenated with organic aerosol to organic carbon (OA / OC) ratios of ~ 2.2–2.8 and are 30–60 % more oxygenated than in current models, which can lead to significant errors in OA concentrations. The model/measurement comparisons presented here support the concept of a more dynamic OA system as proposed by Hodzic et al. (2016), with enhanced removal of primary OA, and a stronger production of secondary OA in global models needed to provide a better agreement with observations. [ABSTRACT FROM AUTHOR]

Atmospheric aerosols are the precondition for the formation of cloud droplets and have thus large influence on the microphysical and radiative properties of clouds. In this work four different methods to derive potential cloud condensation nuclei (CCN) number concentrations were analyzed and compared: A model parameterization based on simulated particle concentrations, the same parameterization based on gravimetrical particle measurements, direct CCN measurements with a CCN counter at a certain observation site and lidar derived CCN profiles. In order to allow for sensitivity studies of the anthropogenic impact, a scenario for the maximum CCN concentration under peak aerosol conditions (1985) was estimated as well. In general, the simulations are in good agreement with the observation. At ground level, an average value of around 1 × 109 CCN/m³ at a supersaturation of 0.2 % was found with all methods. The discrimination of the chemical species revealed an almost equal contribution of ammonium sulfate and ammonium nitrate to the total number of potential CCN. This was not the case for the peak aerosol scenario, where almost no nitrate particles were formed. The potential activation at five different supersaturation values has been compared to the measurements. The discrepancies were lowest for the lowest and highest supersaturations, since chemical composition and the size distribution of the particles are less important in this range. In the mid supersaturation regime, the model overestimated the potentially activated particle fraction by around 30 %. The analysis of the modern (2013) and the peak aerosol scenario (1985) resulted in a scaling factor, which was defined as the quotient of the average vertical profile of the peak aerosol and present day CCN concentration. This factor was found to be around 2 close to the ground, increasing to around 3.5 between 2 and 5 km and approaching 1 (i.e., no difference between present day and peak aerosol conditions) with increasing height. By comparing the simulation with observed profiles, the vertical distribution of the potential CCN was found to be reasonable. [ABSTRACT FROM AUTHOR]

The global aerosol–climate model ECHAM6.3–HAM2.3 (E63H23) as well as the previous model versions ECHAM5.5–HAM2.0 (E55H20) and ECHAM6.1–HAM2.2 (E61H22) are evaluated using global observational datasets for clouds and precipitation. In E63H23, the amount of low clouds, the liquid and ice water path, and cloud radiative effects are more realistic than in previous model versions. E63H23 has a more physically based aerosol activation scheme, improvements in the cloud cover scheme, changes in the detrainment of convective clouds, changes in the sticking efficiency for the accretion of ice crystals by snow, consistent ice crystal shapes throughout the model, and changes in mixed-phase freezing; an inconsistency in ice crystal number concentration (ICNC) in cirrus clouds was also removed. Common biases in ECHAM and in E63H23 (and in previous ECHAM–HAM versions) are a cloud amount in stratocumulus regions that is too low and deep convective clouds over the Atlantic and Pacific oceans that form too close to the continents (while tropical land precipitation is underestimated). There are indications that ICNCs are overestimated in E63H23. Since clouds are important for effective radiative forcing due to aerosol–radiation and aerosol–cloud interactions (ERF ari+aci) and equilibrium climate sensitivity (ECS), differences in ERF ari+aci and ECS between the model versions were also analyzed. ERF ari+aci is weaker in E63H23 (-1.0 W m -2) than in E61H22 (-1.2 W m -2) (or E55H20; -1.1 W m -2). This is caused by the weaker shortwave ERF ari+aci (a new aerosol activation scheme and sea salt emission parameterization in E63H23, more realistic simulation of cloud water) overcompensating for the weaker longwave ERF ari+aci (removal of an inconsistency in ICNC in cirrus clouds in E61H22). The decrease in ECS in E63H23 (2.5 K) compared to E61H22 (2.8 K) is due to changes in the entrainment rate for shallow convection (affecting the cloud amount feedback) and a stronger cloud phase feedback. Experiments with minimum cloud droplet number concentrations (CDNCmin) of 40 cm -3 or 10 cm -3 show that a higher value of CDNCmin reduces ERF ari+aci as well as ECS in E63H23. [ABSTRACT FROM AUTHOR]

To estimate the global co-variability between mineral dust aerosol and cloud glaciation, an aerosol model reanalysis was combined with satellite retrievals of cloud thermodynamic phase. We used the CALIPSO-GOCCP and DARDAR products from the A-Train satellite constellation to obtain the cloud phase and the MACC reanalysis to estimate the dust mixing-ratio in the atmosphere. Night-time retrievals within a temperature range from +3 °C to -42 °C for the period 2007-2010 were included. The results confirm that the cloud thermodynamic phase is highly dependent on temperature and latitude. However, at mid- and high latitudes, at equal temperature and within narrow constrains for humidity and static stability the average frequency of fully glaciated clouds increase by +5 to +10 % for higher mineral dust mixing-ratios. The differentiation between humidity-stability regimes reduced the confounding influence of meteorology on the observed relationship between dust and cloud ice. Furthermore, for similar mixing-ratios of mineral dust the cloud ice occurrence-frequency in the Northern Hemisphere was found to be higher than in the Southern Hemisphere at -30 °C but lower at -15 °C. This may suggest a difference in the susceptibility of cloud glaciation to the presence of dust. Based on previous studies, the differences at -15 °C could be explained by higher feldspar fractions in the Southern Hemisphere, while the differences at -30 °C may be explained by the higher freezing efficiency of clay minerals in the Northern Hemisphere. [ABSTRACT FROM AUTHOR]

Natural sea-salt aerosols, when interacting with anthropogenic emissions, can enhance the formation of particulate nitrate. This enhancement has been suggested to increase the direct radiative forcing of nitrate, called mass-enhancement effect. Through a size-resolved dynamic mass transfer modelling approach, we show that interactions with sea-salt shift the nitrate from sub- to super-micron sizes (re-distribution effect), and hence lower its efficiency for light extinction and reduce its lifetime. The re-distribution effect overwhelms the mass-enhancement effect and significantly moderates nitrate cooling; e.g., the nitrate associated aerosol optical depth can be reduced by 10-20 % over European polluted regions during a typical sea-salt event, in contrast to an increase by ~ 10 % when only accounting for the mass-enhancement effect. Global model simulations indicate significant re-distribution over coastal and offshore regions world-wide. Our study suggests a strong buffering by natural sea-salt aerosols that reduces the climate forcing of anthropogenic nitrate, which had been expected to dominate the aerosol cooling by the end of the century. Comprehensive considerations of this re-distribution effect foster better understandings of climate change and nitrogen deposition. [ABSTRACT FROM AUTHOR]

A regional modeling study on the impact of desert dust on cloud formation is presented for a major Saharan dust outbreak over Europe from 2 to 5 April 2014. The dust event coincided with an extensive and dense cirrus cloud layer, suggesting an influence of dust on atmospheric ice nucleation. Using interactive simulation with the regional dust model COSMO-MUSCAT, we investigate cloud and precipitation representation in the model and test the sensitivity of cloud parameters to dust–cloud and dust–radiation interactions of the simulated dust plume. We evaluate model results with ground-based and spaceborne remote sensing measurements of aerosol and cloud properties, as well as the in situ measurements obtained during the ML-CIRRUS aircraft campaign. A run of the model with single-moment bulk microphysics without online dust feedback considerably underestimated cirrus cloud cover over Germany in the comparison with infrared satellite imagery. This was also reflected in simulated upper-tropospheric ice water content (IWC), which accounted for only 20 % of the observed values. The interactive dust simulation with COSMO-MUSCAT, including a two-moment bulk microphysics scheme and dust–cloud as well as dust–radiation feedback, in contrast, led to significant improvements. The modeled cirrus cloud cover and IWC were by at least a factor of 2 higher in the relevant altitudes compared to the noninteractive model run. We attributed these improvements mainly to enhanced deposition freezing in response to the high mineral dust concentrations. This was corroborated further in a significant decrease in ice particle radii towards more realistic values, compared to in situ measurements from the ML-CIRRUS aircraft campaign. By testing different empirical ice nucleation parameterizations, we further demonstrate that remaining uncertainties in the ice-nucleating properties of mineral dust affect the model performance at least as significantly as including the online representation of the mineral dust distribution. Dust–radiation interactions played a secondary role for cirrus cloud formation, but contributed to a more realistic representation of precipitation by suppressing moist convection in southern Germany. In addition, a too-low specific humidity in the 7 to 10 km altitude range in the boundary conditions was identified as one of the main reasons for misrepresentation of cirrus clouds in this model study. [ABSTRACT FROM AUTHOR]

Two different A-Train satellite cloud phase products were analysed together with an aerosol model reanalysis to assess the global day-to-day variability of cloud thermodynamic phase. This variability was analysed for different mixing-ratios of fine and coarse mineral dust during the period 2007–2010 and within a temperature range from +3°C to −42°C. Night‑time stratiform clouds were analysed, including stratocumulus, altocumulus, altostratus and cirrus clouds. This analysis showed that the phase of stratiform clouds is highly dependent on temperature and latitude. However, at equal temperature the average occurrence of fully glaciated stratiform clouds was found to increase for higher dust mixing-ratios on a day-to-day basis at mid- and high latitudes. At −15°C, the increment of ice cloud occurrence between the lowest and highest mixing-ratio was found to be higher for fine dust (+10% to +18% occurrence) than for coarse dust (+5% to +10%). Surprisingly, the increments were higher in remote regions (e.g. southern high latitudes) where the average dust-mixing ratios are low. [ABSTRACT FROM AUTHOR]

We introduce and evaluate the aerosol simulations with the global aerosol-climate model ECHAM6.3-HAM2.3, which is the aerosol component of the fully coupled aerosol-chemistry-climate model ECHAM-HAMMOZ. Both the host atmospheric climate model ECHAM6.3 and the aerosol model HAM2.3 were updated from previous versions. The updated version of the HAM aerosol model contains improved parameterizations of aerosol processes such as cloud activation, as well as updated emission fields for anthropogenic aerosol species and modifications in the online computation of sea salt and mineral dust aerosol emissions. Aerosol results from nudged and free running simulations for the 10-year period 2003 to 2012 are compared to various measurements of aerosol properties. While there are regional deviations between model and observations, the model performs well overall in terms of aerosol optical thickness, but may underestimate coarse mode aerosol concentrations to some extent, so that the modeled particles are smaller than indicated by the observations. Sulfate aerosol measurements in the US and Europe are reproduced well by the model, while carbonaceous aerosol species are biased low. Both mineral dust and sea salt aerosol concentrations are improved compared to previous versions of ECHAM-HAM. The evaluation of the simulated aerosol distributions serves as a basis for the suitability of the model for simulating aerosol-climate interactions in a changing climate. [ABSTRACT FROM AUTHOR]

In this paper, we present the implementation and evaluation of the aerosol microphysics module SALSA2.0 in the framework of the aerosol-chemistry-climate model ECHAM-HAMMOZ. It is an alternative microphysics module to the default modal microphysics scheme M7 in ECHAM-HAMMOZ. The SALSA2.0 implementation within ECHAM-HAMMOZ is evaluated against observations of aerosol optical properties, aerosol mass, and size distributions, comparing also to the skill of the M7 implementation. The largest differences between the implementation of SALSA2.0 and M7 are in the methods used for calculating microphysical processes, i.e., nucleation, condensation, coagulation, and hydration. These differences in the microphysics are reflected in the results so that the largest differences between SALSA2.0 and M7 are evident over regions where the aerosol size distribution is heavily modified by the microphysical processing of aerosol particles. Such regions are, for example, highly polluted regions and regions strongly affected by biomass burning. In addition, in a simulation of the 1991 Mt. Pinatubo eruption in which a stratospheric sulfate plume was formed, the global burden and the effective radii of the stratospheric aerosol are very different in SALSA2.0 and M7. While SALSA2.0 was able to reproduce the observed time evolution of the global burden of sulfate and the effective radii of stratospheric aerosol, M7 strongly overestimates the removal of coarse stratospheric particles and thus underestimates the effective radius of stratospheric aerosol. As the mode widths of M7 have been optimized for the troposphere and were not designed to represent stratospheric aerosol, the ability of M7 to simulate the volcano plume was improved by modifying the mode widths, decreasing the standard deviations of the accumulation and coarse modes from 1.59 and 2.0, respectively, to 1.2 similar to what was observed after the Mt. Pinatubo eruption. Overall, SALSA2.0 shows promise in improving the aerosol description of ECHAM-HAMMOZ and can be further improved by implementing methods for aerosol processes that are more suitable for the sectional method, e.g., size-dependent emissions for aerosol species and size-resolved wet deposition. [ABSTRACT FROM AUTHOR]

Ice nucleating particles (INPs) increase the temperature at which supercooled droplets start to freeze. They are therefore of particular interest in mixed-phase cloud temperature regimes, where supercooled liquid droplets can persist for extended periods of time in the absence of INPs. When INPs are introduced to such an environment, the cloud can quickly glaciate following ice multiplication processes and the Wegener--Bergeron--Findeisen (WBF) process. The WBF process can also cause the ice to grow to precipitation size and precipitate out. All of these processes alter the radiative properties. Despite their potential influence on climate, the ice nucleation ability and importance of different aerosol species is still not well understood and is a field of active research. In this study, we use the aerosol--climate model ECHAM6-HAM2 to examine the global relevance of marine organic aerosol (MOA), which has drawn much interest in recent years as a potentially important INPs in remote marine regions. We address the uncertainties in emissions and ice nucleation activity of MOA with a range of reasonable set-ups and find a wide range of resultingMOA burdens. The relative importance of MOA as an INP compared to dust is investigated and found to depend strongly on the type of ice nucleation parameterisation scheme chosen. On the zonal mean, freezing due to MOA leads to relative increases in the cloud ice occurrence and in-cloud number concentration close to the surface in the polar regions during summer. Slight but consistent decreases in the in-cloud ice crystal effective radius can also be observed over the same regions during all seasons. Regardless, MOA was not found to affect the radiative balance significantly on the global scale, due to its relatively weak ice activity and a low sensitivity of cloud ice properties to heterogeneous ice nucleation in our model. [ABSTRACT FROM AUTHOR]