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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 cloud-top-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., Geophysical Research Letters, 48 (11), ISSN:0094-8276, ISSN:1944-8007

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.

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.

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. ISSN:1991-9603 ISSN:1991-959X

We introduce and evaluate 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 the 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., Geoscientific Model Development, 12 (4), ISSN:1991-9603, ISSN:1991-959X

We introduce and evaluate 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 the 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.

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 resulting MOA 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. ISSN:1680-7375 ISSN:1680-7367

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.

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 April 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 space-borne remote sensings of aerosol and cloud properties, as well as the in situ measurements obtained during the ML-CIRRUS aircraft campaign.

A new German research consortium is investigating the causes and effects of the rapid rise of near-surface air temperatures in the Artic. Within the last 25 years a remarkable increase of the Arctic near-surface air temperature exceeding the global warming by a factor of two to three has been observed. The phenomenon is commonly referred to as Arctic Amplification. The warming results in rather drastic changes of a variety of climate parameters. For example, the Arctic sea ice has declined significantly. This ice retreat has been well identified by satellite measurements. However, coupled regional and global climate models still fail to reproduce it adequately; they tend to systematically underestimate the observed sea ice decline. This model observation difference implies that the underlying physical processes and feedback mechanisms are not appropriately represented in Arctic climate models. Thus, the predictions of these models are also likely to be inadequate. It is mandatory to identify the origin of this disagreement. Ein neu geschaffenes deutsches Forschungskonsortium untersucht die Ursachen und Effekte des rapiden Anstiegs der bodennahen Lufttemperatur in der Arktis. Innerhalb der letzten 25 Jahre wurde ein bemerkenswerter Anstieg der Bodenlufttemperatur in der Arktis beobachtet, welcher die globale Erwärmung um den Faktor 2 bis 3 übersteigt. Dieses Phänomen wird als arktische Verstärkung bezeichnet. Diese Erwärmung resultiert vielmehr in einer drastischen Änderung einer Vielzahl von Klimarparametern. Beispielsweise ist das arktische Meereis deutlich zurückgegangen. Dieser Eisrückgang wurde durch Satellitenbeobachtungen gut beobachtet. Dagegen haben regionale und globale Klimamodelle immer noch Probleme, den Rückgang entsprechend zu reproduzieren. Sie tendieren dazu, den Meereisrückgang systematisch zu unterschätzen. Die Unterschiede zwischen Modell und Beobachtungen legen nahe, dass die grundlegenden physikalischen Prozesse und Rückkopplungsmechanismen nicht entsprechend in arktischen Klimamodellen repräsentiert werden. Somit sind wahrscheinlich auch die Vorhersagen der Modelle unzureichend. Es ist notwendig, den Ursprung dieser Unstimmigkeit zu identifizieren.

The regional atmospheric model Consortium for Small-scale Modeling (COSMO) coupled to the Multi-Scale Chemistry Aerosol Transport model (Muscat) is extended in this work to represent aerosol-cloud interactions. Previously, only one-way interactions (scavenging of aerosol and in-cloud chemistry) and aerosol-radiation interactions were included in this model. The new version allows for a microphysical aerosol effect on clouds. For this, we use the optional two-moment cloud microphysical scheme in COSMO and the online-computed aerosol information for cloud condensation nuclei concentrations (Cccn), replacing the constant Cccn profile. In the radiation scheme, we have implemented a droplet-size-dependent cloud optical depth, allowing now for aerosol-cloud-radiation interactions. To evaluate the models with satellite data, the Cloud Feedback Model Intercomparison Project Observation Simulator Package (COSP) has been implemented. A case study has been carried out to understand the effects of the modifications, where the modified modeling system is applied over the European domain with a horizontal resolution of 0.25°g × g0.25°. To reduce the complexity in aerosol-cloud interactions, only warm-phase clouds are considered. We found that the online-coupled aerosol introduces significant changes for some cloud microphysical properties. The cloud effective radius shows an increase of 9.5g%, and the cloud droplet number concentration is reduced by 21.5g%.

An aerosol model was used to simulate the generation and transport of aerosols over Germany during the HD(CP)2 Observational Prototype Experiment (HOPE) field campaign of 2013. The aerosol number concentrations and size distributions were evaluated against observations, which shows satisfactory agreement in the magnitude and temporal variability of the main aerosol contributors to cloud condensation nuclei (CCN) concentrations. From the modelled aerosol number concentrations, number concentrations of CCN were calculated as a function of vertical velocity using a comprehensive aerosol activation scheme which takes into account the influence of aerosol chemical and physical properties on CCN formation. There is a large amount of spatial variability in aerosol concentrations; however the resulting CCN concentrations vary significantly less over the domain. Temporal variability is large in both aerosols and CCN. A parameterization of the CCN number concentrations is developed for use in models. The technique involves defining a number of best fit functions to capture the dependence of CCN on vertical velocity at different pressure levels. In this way, aerosol chemical and physical properties as well as thermodynamic conditions are taken into account in the new CCN parameterization. A comparison between the parameterization and the CCN estimates from the model data shows excellent agreement. This parameterization may be used in other regions and time periods with a similar aerosol load; furthermore, the technique demonstrated here may be employed in regions dominated by different aerosol species.

Since iron is an important micronutrient, deposition of iron in mineral aerosols can impact the carbon cycle and atmospheric CO2. This paper reviews our current understanding of the global dust cycle and identifies future research needs. The global distribution of desert dust is estimated from a combination of observations of dust from in situ concentration, optical depth, and deposition data; observations from satellite; and global atmospheric models. The anthropogenically influenced portion of atmospheric desert dust flux is thought to be smaller than the natural portion, but is difficult to quantify due to the poorly understood response of desert dust to changes in climate, land use, and water use. The iron content of aerosols is thought to vary by a factor of 2, while the uncertainty in dust deposition is at least a factor of 10 in some regions due to the high spatial and temporal variability and limited observations. Importantly, we have a limited understanding of the processes by which relatively insoluble soil iron (typically similar to 0.5% is soluble) becomes more soluble (1-80%) during atmospheric transport, but these processes could be impacted by anthropogenic emissions of sulfur or organic acids. In order to understand how humans will impact future iron deposition to the oceans, we need to improve our understanding of: iron deposition to remote oceans, iron chemistry in aerosols, how desert dust sources will respond to climate change, and how humans will impact the transport of bioavailable fraction of iron to the oceans. [References: 172]

It is important to understand how future environmental policies will impact both climate change and air pollution. Although targeting near-term climate forcers (NTCFs), defined here as aerosols, tropospheric ozone, and precursor gases, should improve air quality, NTCF reductions will also impact climate. Prior assessments of the impact of NTCF mitigation on air quality and climate have been limited. This is related to the idealized nature of some prior studies, simplified treatment of aerosols and chemically reactive gases, as well as a lack of a sufficiently large number of models to quantify model diversity and robust responses. Here, we quantify the 2015–2055 climate and air quality effects of non-methane NTCFs using nine state-of-the-art chemistry–climate model simulations conducted for the Aerosol and Chemistry Model Intercomparison Project (AerChemMIP). Simulations are driven by two future scenarios featuring similar increases in greenhouse gases (GHGs) but with “weak” (SSP3-7.0) versus “strong” (SSP3-7.0-lowNTCF) levels of air quality control measures. As SSP3-7.0 lacks climate policy and has the highest levels of NTCFs, our results (e.g., surface warming) represent an upper bound. Unsurprisingly, we find significant improvements in air quality under NTCF mitigation (strong versus weak air quality controls). Surface fine particulate matter (PM2.5) and ozone (O3) decrease by −2.2±0.32 µg m−3 and −4.6±0.88 ppb, respectively (changes quoted here are for the entire 2015–2055 time period; uncertainty represents the 95 % confidence interval), over global land surfaces, with larger reductions in some regions including south and southeast Asia. Non-methane NTCF mitigation, however, leads to additional climate change due to the removal of aerosol which causes a net warming effect, including global mean surface temperature and precipitation increases of 0.25±0.12 K and 0.03±0.012 mm d−1, respectively. Similarly, increases in extreme weather indices, including the hottest and wettest days, also occur. Regionally, the largest warming and wetting occurs over Asia, including central and north Asia (0.66±0.20 K and 0.03±0.02 mm d−1), south Asia (0.47±0.16 K and 0.17±0.09 mm d−1), and east Asia (0.46±0.20 K and 0.15±0.06 mm d−1). Relatively large warming and wetting of the Arctic also occur at 0.59±0.36 K and 0.04±0.02 mm d−1, respectively. Similar surface warming occurs in model simulations with aerosol-only mitigation, implying weak cooling due to ozone reductions. Our findings suggest that future policies that aggressively target non-methane NTCF reductions will improve air quality but will lead to additional surface warming, particularly in Asia and the Arctic. Policies that address other NTCFs including methane, as well as carbon dioxide emissions, must also be adopted to meet climate mitigation goals., Atmospheric Chemistry and Physics, 20 (16), ISSN:1680-7375, ISSN:1680-7367

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., Geoscientific Model Development, 13 (3), ISSN:1991-9603, ISSN:1991-959X

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 (ERFari+aci) and equilibrium climate sensitivity (ECS), differences in ERFari+aci and ECS between the model versions were also analyzed. ERFari+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 ERFari+aci (a new aerosol activation scheme and sea salt emission parameterization in E63H23, more realistic simulation of cloud water) overcompensating for the weaker longwave ERFari+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 ERFari+aci as well as ECS in E63H23., Geoscientific Model Development, 12 (8), ISSN:1991-9603, ISSN:1991-959X

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 resulting MOA 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., Atmospheric Chemistry and Physics, 18 (15), ISSN:1680-7375, ISSN:1680-7367

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., Atmospheric Chemistry and Physics, 19 (17), ISSN:1680-7375, ISSN:1680-7367

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 phase. At −30 °C, half of the liquid cloud tops observed in the southern hemisphere would glaciate in the northern hemisphere. The new product ensemble is more reliable than the individual products and suggests a previous underestimation of the cloud‐phase contrasts.

Die Entwicklung eines Emissionsmoduls für primäres marines Aerosol (PMA; bestehend aus Meersalz und organischem Material) war Hauptgegenstand der vorliegenden Arbeit. Dieses wurde in das Chemie-Transportmodell „COSMO-MUSCAT“ eingebaut und löste dort das vorherige einfach gehaltene Modul (nur Meersalz) ab, welches entsprechend früherer Studien zu hohe Meersalzkonzentrationen berechnete. Das neue Emissionsmodul wurde umfangreich getestet und gegen die Messdaten von verschiedenen Stationen in Europa, einem Bernerimpaktor auf São Vicente (Kap Verden) und einem Aerosolmassenspektrometer sowie einem Digitelfilter während der Fahrt ANT-XXVII/4 des Forschungsschiffes Polarstern validiert. Bei den Untersuchungen kristallisierte sich die Emissionsparametrisierung von Long et al. (2011) als die am Besten geeignete für COSMO-MUSCAT heraus. Weiterhin wurde der Einfluss der Wassertemperatur an der Meeresoberfläche auf die PMA-Emission untersucht. Dabei konnte gezeigt werden, dass dieser Effekt insbesondere für größere Aerosolpartikel (2,5 µm < Dp) relevant ist. Die Nichtbeachtung der Temperaturkorrektur würde in diesem Größenbereich zu einer Überschätzung der Emissionsflüsse und folgend der Konzentration von PMA über kalten Gewässern führen. Beim erstmaligen Vergleich verschiedener Funktionen zur Beachtung des Temperatureffektes erzielte die Funktion von Sofiev et al. (2011) die besten Ergebnisse. Als weitere Neuerung wurde das mit dem PMA emittierte organische Material in das Emissionsmodul eingebaut. Auch hierfür erfolgten Vergleichsstudien verschiedener Parametrisierungen und Ansätze. Allerdings standen nur unzureichende Messungen zur Verfügung, da sie keine Aufteilung in primäres (mit PMA emittiert) und sekundäres (in Gasphase gebildet) organisches Material lieferten. Daher war eine Aussage zur Güte der Funktionen kaum möglich. Die Simulationen zeigten jedoch die Bedeutung der verschiedenen Ansätze zur Berechnung der Emissionsflüsse von organischem Material. So kann bspw. der Einfluss der Emissionsfunktion den Einfluss der Parametrisierung zur Aufteilung in Meersalz und organisches Material deutlich übersteigen. Letztlich bleibt die Frage der richtigen Eingangsdaten für die Emission von primärem organischen Material offen. Es zeigte sich, dass die Abhängigkeit der Anreicherung von organischem Material im PMA von der Chlorophyll a-Konzentration im Oberflächenwasser nicht zwingend gegeben sein muss. Daher ist es notwendig sie in der Berechnung der Emissionsflüsse durch weitere/andere Parameter zu ergänzen/ersetzen. Dies ist Gegenstand eines neuen Forschungsprojektes, bei dem das neue Emissionsmodul angewendet und weiterentwickelt wird.

In dieser Dissertation wird das kompressible, nicht-hydrostatische und dreidimensionale Modell All Scale Atmospheric Model (ASAM) für Grobstruktur- bzw. Large-Eddy-Simulationen (LES) angewendet, um lokale Inseleffekte in der karibischen Passatwindzone zu untersuchen. Da das Modell bis dato noch keine Anwendung im Bereich von LES feuchter atmosphärischer Grenzschichten und heterogener Oberflächen fand, wurden einige Bestandteile zum Modellcode hinzugefügt oder überarbeitet. Ein Hauptaugenmerk liegt dabei auf das Einbeziehen orographischer Strukturen mittels angeschnittener Zellen (engl. cut cells). Sowohl die räumliche und zeitliche Diskretisierung der Modellgleichungen als auch die nötigen physikalischen Parameterisierungen werden in einer umfassenden Modellbeschreibung zusammengefasst. Die Robustheit und Stabilität der Modellformulierung wird durch eine Reihe von Simulationen idealisierter Testfälle bestätigt. Large-Eddy-Simulationen werden für das Gebiet der Karibikinsel Barbados zur Untersuchung von Inseleffekten bezüglich Grenzschichtmodifikation, Wolkenbildung und vertikaler Durchmischung von Aerosolen durchgeführt. Durch das Vorhandensein einer topographisch strukturierten Inseloberfläche in der Mitte des Modellgebietes muss das Modellsetup offene seitliche Randbedingungen beinhalten. Damit das einströmende Windfeld konsistent mit der Dynamik einer turbulenten, marinen Grenzschicht ist, wird eine neue Methode implementiert und angewendet, welche auf Störungen des potentiellen Temperaturfeldes mittels finiter Amplituden basiert. Beobachtungen aus der SALTRACE-Messkampagne werden benutzt, um die Modellläufe anzutreiben. Die Ergebnisse einiger Sensitivitätstests zeigen Probleme der Modellierung im Bereich der \"Terra incognita\" auf. Dabei handelt es sich um die Modellierung auf räumlichen Skalen, welche zwischen denen von LES und wolkenauflösenden Modellen liegen. Außerdem werden Auswirkungen von entweder turbulent oder laminar anströmenden Windfeldern auf die Simulationsergebnisse untersucht. Besonders die Wolkeneigenschaften im Lee von Barbados werden in diesen Simulationen merklich beeinflusst. Ergebnisse einer weiteren Simulation mit einer sehr starken Passatinversion bringt deren Einfluss auf die Dicke und Höhe der simulierten Wolkenschichten zum Vorschein. Die Veränderung von Saharastaubschichten, welche Barbados über weiträumigen Transport über den Atlantik erreichen, wird analysiert. Die Auswirkungen beinhalten sowohl eine Ausdünnung und ein Absinken dieser Schichten als auch turbulenter Transport in Richtung Erdoberfläche. Die genaue Position der beeinflussten Schichten und die Stärke des turbulenten Mischens werden hauptsächlich von der atmosphärischen Schichtung, der Inversionsstärke und Windscherung gesteuert. Vergleiche zwischen den LES-Modellergebnissen und Daten aus Doppler-Windlidarmessungen zeigen gute Übereinstimmungen in der Formierung der konvektiven Strukturen tagsüber und des Vertikalwindfeldes. In this thesis, the fully compressible, three-dimensional, nonhydrostatic atmospheric model called All Scale Atmospheric Model (ASAM) is utilized for large eddy simulations (LES) to investigate local island effects at the Caribbean. Since the model has not been applied to LES for moist boundary layers and heterogeneous surfaces so far, several parts are added to the model code or reworked. A special focus lies on the inclusion of orographical structures via the cut cell method. Spatial and temporal discretization as well as necessary physical parameterizations are summarized in a thorough model description. The robustness of the model formulation is confirmed by a set of idealized test case simulations. Large eddy simulations are performed for the area of the Caribbean island Barbados to investigate island effects on boundary layer modification, cloud generation and vertical mixing of aerosols. Due to the presence of a topographically structured island surface in the domain center, the model setup has to be designed with open lateral boundaries. In order to generate inflow turbulence consistent with the upstream marine boundary layer forcing, the newly developed cell perturbation method based on finite amplitude perturbations is applied. Observations from the SALTRACE field campaign are used to initialize the model runs. Several numerical sensitivity tests are carried out to demonstrate the problems related to \"gray zone modeling\" beyond LES scales or when the turbulent marine boundary layer flow is replaced by laminar winds. Especially cloud properties west of Barbados (downwind) are markedly affected in these simulations. Results of an additional simulation with a strong trade-wind inversion reveal its effect on cloud layer depth and height. The modification of Saharan dust layers reaching Barbados via long-range transport over the North Atlantic is analyzed. Effects of layer thinning, subsidence and turbulent downward transport near the layer bottom become apparent. The position of these layers and strength of downward mixing is found to be mainly controlled atmospheric stability, inversion strength and wind shear. Comparisons of LES model output with wind lidar data show similarities in the formation of the daytime convective plume and the vertical wind structure.

In this thesis the occurrence and the properties of atmospheric particles within Europe are studied by means of the regional transport model COSMO-MUSCAT (Consortium for Small-scale Modeling - MultiScale Atmospheric Transport Model). The model is used to perform calculations for a summer (19-26 July 2006) and a winter (16-26 February 2007) period. Individual extinction coefficients are computed taking into account hygroscopic growth and mass extinction efficiencies of specific chemical compounds. The model study focuses on vertical backscatter profiles, aerosol optical depths, particle surface concentrations and radiative effects. Different descriptions of the vertical distribution of chemical compounds at the lateral model boundaries are tested. The results show that for the tested model setup the influence of the aerosol distribution at the model boundaries on European aerosol is limited. Information from lidar profiles may improve the description at the lateral model boundaries. This may be more important for smaller model domains. Space-based lidar (light detection and ranging) observations (CALIOP - Cloud-Aerosol Lidar with Orthogonal Polarization) observations are compared to the simulated backscatter profiles caused by the simulated anthropogenic aerosol. The model reproduces the shape and magnitude of the vertical backscatter profiles well for both time periods. Better agreements are found for night-time observations compared to day-time data. Satisfying agreements between the model results and experimental observations of ground-based vertical backscatter profiles, aerosol optical depths and particle surface concentrations are also found for the two time periods in Europe. Discrepancies between measurement and simulation highlight the difficulties to describe horizontal and vertical aerosol properties properly. The direct and semi-direct radiative effects of the absorbing aerosol are studied for both summer and winter period. For both periods, an increase of the solar heating rate due to the aerosol forcing is determined. This heating leads to an average decrease of the total cloud cover of 1.0% (summer) and of 0.7% (winter). This semi-direct radiative effect causes a positive forcing at the surface and at the top-of-atmosphere in the European domain.

The PhD-thesis aims to characterise the Saharan dust cycle at diffent seasons using satellite remote sensing techniques and regional modelling studies. A dust index based on 15-minute infrared satellite measurements provided by the SEVIRI instrument onboard the Meteosat Second Generation (MSG) satellite is used to infer spatio-temporal charcteristics of dust sources north of 5°N over Africa since March 2006. The spatial distribution of dust sources points towards the importance of endorehic drainage systems in mountain areas. The temporal distribution of the time-of-day when dust mobilisation starts shows maximum activity during local morning hours, pointing towards the role of the breakdown of the nocturnal low-level jet. Details of the role and ability of the low-level jet breakdown for dust entrainment were studied using regional modelling. Furthermore, the seasonal dust export towards the tropical North Atlantic is considered using regional modelling. Die Arbeit beschäftigt sich mit der Charakterisierung des atmosphärischen Kreislaufs von nordafrikanischen Wüstenstaub. Dazu wurde Satellitendaten auf einer zeitlichen Auflösung von 15 Minuten hinsichtlich der Aktivierung von Staubquellen nördlich von 5°N über Afrika ausgewertet. Der Auswertezeitraum beginnt im März 2006. Der erstellte Datensatz wurde hinsichtlich der raum-zeitlichen Verteilung aktiver Staubquellen untersucht. Die räumlich Verteilung der Staubquellen zeigt die Bedeutung von Trockentälern im Zuge der Staubmobilisierung auf. Die zeitliche Verteilung einsetzender Staubmobilisierung zeigt ein Maximum während der lokalen Morgenstunden. Mit Hilfe von regionaler Modellierung wurden diese Ereignisse im Zusammenhang mit dem Heruntermischen des nächtlichen Grenzschichtstrahlstroms untersucht. Im Weiteren wurde der saisonale Staubexport Richtung tropischen Atlantik mit untersucht.