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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.
- ItemHow the extreme 2019-2020 Australian wildfires affected global circulation and adjustments(Katlenburg-Lindau : EGU, 2023) Senf, Fabian; Heinold, Bernd; Kubin, Anne; Müller, Jason; Schrödner, Roland; Tegen, InaWildfires 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 17ĝ€¯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 +5ĝ€¯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 +0.5ĝ€¯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 0.2ĝ€¯%. 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.
- ItemAir pollution trapping in the Dresden Basin from gray-zone scale urban modeling(Katlenburg-Lindau : EGU, 2023) Weger, Michael; Heinold, BerndThe microscale variability of urban air pollution is essentially driven by the interaction between meteorology and urban topography, which remains challenging to represent spatially accurately and computationally efficiently in urban dispersion models. Natural topography can additionally exert a considerable amplifying effect on urban background pollution, depending on atmospheric stability. This requires an equally important representation in models, as even subtle terrain-height variations can enforce characteristic local flow regimes. In this model study, the effects of urban and natural topography on the local winds and air pollution dispersion in the Dresden Basin in the Eastern German Elbe valley are investigated. A new, efficient urban microscale model is used within a multiscale air quality modeling framework. The simulations that consider real meteorological and emission conditions focus on two periods in late winter and early summer, respectively, as well as on black carbon (BC), a key air pollutant mainly emitted from motorized traffic. As a complement to the commonly used mass concentrations, the particle age content (age concentration) is simulated. This concept, which was originally developed to study hydrological reservoir flows in a Eulerian framework, is adapted here for the first time for atmospheric boundary-layer modeling. The approach is used to identify stagnant or recirculating orographic air flows and resulting air pollution trapping. An empirical orthogonal function (EOF) analysis is applied to the simulation results to attribute the air pollution modes to specific weather patterns and quantify their significance. Air quality monitoring data for the region are used for model evaluation. The model results show a strong sensitivity to atmospheric conditions, but generally confirm increased BC levels in Dresden due to the valley location. The horizontal variability of mass concentrations is dominated by the patterns of traffic emissions, which overlay potential orography-driven pollutant accumulations. Therefore, an assessment of the orographic impact on air pollution is usually inconclusive. However, using the age-concentration metric, which filters out direct emission effects, previously undetected spatial patterns are discovered that are largely modulated by the surface orography. The comparison with a dispersion simulation assuming spatially homogeneous emissions also proves the robustness of the orographic flow information contained in the age-concentration distribution and shows it to be a suitable metric for assessing orographic air pollution trapping. The simulation analysis indicates several air quality hotspots on the southwestern slopes of the Dresden Basin and in the southern side valley, the Döhlen Basin, depending on the prevailing wind direction.
- ItemImportant role of stratospheric injection height for the distribution and radiative forcing of smoke aerosol from the 2019–2020 Australian wildfires(Katlenburg-Lindau : EGU, 2022) Heinold, Bernd; Baars, Holger; Barja, Boris; Christensen, Matthew; Kubin, Anne; Ohneiser, Kevin; Schepanski, Kerstin; Schutgens, Nick; Senf, Fabian; Schrödner, Roland; Villanueva, Diego; Tegen, InaMore 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 W m−2 instantaneous direct radiative forcing was modeled at TOA, averaged for the Southern Hemisphere (+0.25 W m−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 W m−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.
- 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.