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- ItemCharacterization of organic aerosol across the global remote troposphere: A comparison of ATom measurements and global chemistry models(Katlenburg-Lindau : EGU, 2020) Hodzic, Alma; Campuzano-Jost, Pedro; Bian, Huisheng; Chin, Mian; Colarco, Peter R.; Day, Douglas A.; Froyd, Karl D.; Heinold, Bernd; Katich, Joseph M.; Jo, Duseong S.; Kodros, John K.; Nault, Benjamin A.; Pierce, Jeffrey R.; Ray, Eric; Schacht, Jacob; Schill, Gregory P.; Schroder, Jason C.; Schwarz, Joshua P.; Sueper, Donna T.; Tegen, Ina; Tilmes, Simone; Tsigaridis, Kostas; Yu, Pengfei; Jimenez, Jose L.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 nonrefractory 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 sec-ondary 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. © 2020 IEEE Computer Society. All rights reserved.
- ItemCombining atmospheric and snow radiative transfer models to assess the solar radiative effects of black carbon in the Arctic(Katlenburg-Lindau : EGU, 2020) Donth, Tobias; Jäkel, Evelyn; Ehrlich, André; Heinold, Bernd; Schacht, Jacob; Herber, Andreas; Zanatta, Marco; Wendisch, ManfredThe magnitude of solar radiative effects (cooling or warming) of black carbon (BC) particles embedded in the Arctic atmosphere and surface snow layer was explored on the basis of case studies. For this purpose, combined atmospheric and snow radiative transfer simulations were performed for cloudless and cloudy conditions on the basis of BC mass concentrations measured in pristine early summer and more polluted early spring conditions. The area of interest is the remote sea-ice-covered Arctic Ocean in the vicinity of Spitsbergen, northern Greenland, and northern Alaska typically not affected by local pollution. To account for the radiative interactions between the black-carbon-containing snow surface layer and the atmosphere, an atmospheric and snow radiative transfer model were coupled iteratively. For pristine summer conditions (no atmospheric BC, minimum solar zenith angles of 55 ) and a representative BC particle mass concentration of 5 ng g-1 in the surface snow layer, a positive daily mean solar radiative forcing of +0.2 W m-2 was calculated for the surface radiative budget. A higher load of atmospheric BC representing early springtime conditions results in a slightly negative mean radiative forcing at the surface of about -0.05 W m-2, even when the low BC mass concentration measured in the pristine early summer conditions was embedded in the surface snow layer. The total net surface radiative forcing combining the effects of BC embedded in the atmosphere and in the snow layer strongly depends on the snow optical properties (snow specific surface area and snow density). For the conditions over the Arctic Ocean analyzed in the simulations, it was found that the atmospheric heating rate by water vapor or clouds is 1 to 2 orders of magnitude larger than that by atmospheric BC. Similarly, the daily mean total heating rate (6 K d-1) within a snowpack due to absorption by the ice was more than 1 order of magnitude larger than that of atmospheric BC (0.2 K d-1). Also, it was shown that the cooling by atmospheric BC of the near-surface air and the warming effect by BC embedded in snow are reduced in the presence of clouds. © 2020 Copernicus GmbH. All rights reserved.
- ItemModelling mineral dust emissions and atmospheric dispersion with MADE3 in EMAC v2.54(Katlenburg-Lindau : Copernicus, 2020) Beer, Christof G.; Hendricks, Johannes; Righi, Mattia; Heinold, Bernd; Tegen, Ina; Groß, Silke; Sauer, Daniel; Walser, Adrian; Weinzierl, BernadettIt 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.
- ItemCoupling aerosols to (cirrus) clouds in the global EMAC-MADE3 aerosol–climate model(Katlenburg-Lindau : Copernicus, 2020) Righi, Mattia; Hendricks, Johannes; Lohmann, Ulrike; Beer, Christof Gerhard; Hahn, Valerian; Heinold, Bernd; Heller, Romy; Krämer, Martina; Ponater, Michael; Rolf, Christian; Tegen, Ina; Voigt, ChristianeA 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.
- ItemThe impact of COVID-19 lockdown measures on the Indian summer monsoon(Bristol : IOP Publ., 2021-7-16) Fadnavis, Suvarna; Sabin, T. P.; Rap, Alexandru; Müller, Rolf; Kubin, Anne; Heinold, BerndAerosol concentrations over Asia play a key role in modulating the Indian summer monsoon (ISM) rainfall. Lockdown measures imposed to prevent the spread of the COVID-19 pandemic led to substantial reductions in observed Asian aerosol loadings. Here, we use bottom-up estimates of anthropogenic emissions based on national mobility data from Google and Apple, along with simulations from the ECHAM6-HAMMOZ state-of-the-art aerosol-chemistry-climate model to investigate the impact of the reduced aerosol and gases pollution loadings on the ISM. We show that the decrease in anthropogenic emissions led to a 4 W m−2 increase in surface solar radiation over parts of South Asia, which resulted in a strengthening of the ISM. Simultaneously, while natural emission parameterizations are kept the same in all our simulations, the anthropogenic emission reduction led to changes in the atmospheric circulation, causing accumulation of dust over the Tibetan plateau (TP) during the pre-monsoon and monsoon seasons. This accumulated dust has intensified the warm core over the TP that reinforced the intensification of the Hadley circulation. The associated cross-equatorial moisture influx over the Indian landmass led to an enhanced amount of rainfall by 4% (0.2 mm d−1) over the Indian landmass and 5%–15% (0.8–3 mm d−1) over central India. These estimates may vary under the influence of large-scale coupled atmosphere–ocean oscillations (e.g. El Nino Southern Oscillation, Indian Ocean Dipole). Our study indicates that the reduced anthropogenic emissions caused by the unprecedented COVID-19 restrictions had a favourable effect on the hydrological cycle over South Asia, which has been facing water scarcity during the past decades. This emphasizes the need for stringent measures to limit future anthropogenic emissions in South Asia for protecting one of the world's most densely populated regions.
- ItemICONGETM v1.0 – flexible NUOPC-driven two-way coupling via ESMF exchange grids between the unstructured-grid atmosphere model ICON and the structured-grid coastal ocean model GETM(Katlenburg-Lindau : Copernicus, 2021) Bauer, Tobias Peter; Holtermann, Peter; Heinold, Bernd; Radtke, Hagen; Knoth, Oswald; Klingbeil, KnutTwo-way model coupling is important for representing the mutual interactions and feedbacks between atmosphere and ocean dynamics. This work presents the development of the two-way coupled model system ICONGETM, consisting of the atmosphere model ICON and the ocean model GETM. ICONGETM is built on the latest NUOPC coupling software with flexible data exchange and conservative interpolation via ESMF exchange grids. With ICON providing a state-of-the-art kernel for numerical weather prediction on an unstructured mesh and GETM being an established coastal ocean model, ICONGETM is especially suited for high-resolution studies. For demonstration purposes the newly developed model system has been applied to a coastal upwelling scenario in the central Baltic Sea.
- ItemThe day-to-day co-variability between mineral dust and cloud glaciation: a proxy for heterogeneous freezing(Katlenburg-Lindau : EGU, 2020) Villanueva, Diego; Heinold, Bernd; Seifert, Patric; Deneke, Hartwig; Radenz, Martin; Tegen, InaTo 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.
- ItemEstimation of cloud condensation nuclei number concentrations and comparison to in situ and lidar observations during the HOPE experiments(Katlenburg-Lindau : EGU, 2020) Genz, Christa; Schrödner, Roland; Heinold, Bernd; Henning, Silvia; Baars, Holger; Spindler, Gerald; Tegen, InaAtmospheric 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 presentday 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) lidarderived 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. © 2020 Author(s).
- ItemThe Importance of the Representation of DMS Oxidation in Global Chemistry‐Climate Simulations(Hoboken, NJ : Wiley, 2021) Hoffmann, Erik Hans; Heinold, Bernd; Kubin, Anne; Tegen, Ina; Herrmann, HartmutThe 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.
- ItemKnowledge Transfer with Citizen Science: Luft-Leipzig Case Study(Basel : MDPI, 2021) Tõnisson, Liina; Voigtländer, Jens; Weger, Michael; Assmann, Denise; Käthner, Ralf; Heinold, Bernd; Macke, AndreasCommunity-based participatory research initiatives such as “hackAir”, “luftdaten.info”, “senseBox”, “CAPTOR”, “CurieuzeNeuzen Vlaanderen”, “communityAQ”, and “Healthy Air, Healthier Children” campaign among many others for mitigating short-lived climate pollutants (SLCPs) and improving air quality have reported progressive knowledge transfer results. These research initiatives provide the research community with the practical four-element state-of-the-art method for citizen science. For the preparation-, measurements-, data analysis-, and scientific support-elements that collectively present the novel knowledge transfer method, the Luft-Leipzig project results are presented. This research contributes to science by formulating a novel method for SLCP mitigation projects that employ citizen scientists. The Luft-Leipzig project results are presented to validate the four-element state-of-the-art method. The method is recommended for knowledge transfer purposes beyond the scope of mitigating short-lived climate pollutants (SLCPs) and improving air quality.