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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.
- ItemClimate and air quality impacts due to mitigation of non-methane near-term climate forcers(Katlenburg-Lindau : EGU, 2020) Allen, Robert J.; Turnock, Steven; Nabat, Pierre; Neubauer, David; Lohmann, Ulrike; Olivié, Dirk; Oshima, Naga; Michou, Martine; Wu, Tongwen; Zhang, Jie; Takemura, Toshihiko; Schulz, Michael; Tsigaridis, Kostas; Bauer, Susanne E.; Emmons, Louisa; Horowitz, Larry; Naik, Vaishali; van Noije, Twan; Bergman, Tommi; Lamarque, Jean-Francois; Zanis, Prodromos; Tegen, Ina; Westervelt, Daniel M.; Le Sager, Philippe; Good, Peter; Shim, Sungbo; O’Connor, Fiona; Akritidis, Dimitris; Georgoulias, Aristeidis K.; Deushi, Makoto; Sentman, Lori T.; John, Jasmin G.; Fujimori, Shinichiro; Collins, William J.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 2:20:32 ugm3 and 4:60:88 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 0:250:12K and 0:030:012mmd1, 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 (0:660:20K and 0:030:02mmd1), south Asia (0:470:16K and 0:170:09mmd1), and east Asia (0:460:20K and 0:150:06mmd1). Relatively large warming and wetting of the Arctic also occur at 0:590:36K and 0:040:02mmd1, 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. © Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.
- 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.
- ItemAtmospheric Dynamics and Numerical Simulations of Six Frontal Dust Storms in the Middle East Region(Basel : MDPI, 2021) Hamzeh, Nasim Hossein; Karami, Sara; Kaskaoutis, Dimitris G.; Tegen, Ina; Moradi, Mohamad; Opp, ChristianThis study analyzes six frontal dust storms in the Middle East during the cold period (October–March), aiming to examine the atmospheric circulation patterns and force dynamics that triggered the fronts and the associated (pre-or post-frontal) dust storms. Cold troughs mostly located over Turkey, Syria and north Iraq played a major role in the front propagation at the surface, while cyclonic conditions and strong winds facilitated the dust storms. The presence of an upper-atmosphere (300 hPa) sub-tropical jet stream traversing from Egypt to Iran constitutes also a dynamic force accompanying the frontal dust storms. Moderate-Resolution Imaging Spectroradiometer (MODIS) and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) observations are used to monitor the spatial and vertical extent of the dust storms, while model (Weather Research and Forecasting model coupled with Chemistry (WRF-Chem), Copernicus Atmospheric Monitoring Service (CAMS), Regional Climate Model-4 (RegCM4)) simulations are also analyzed. The WRF-Chem outputs were in better agreement with the MODIS observations compared to those of CAMS and RegCM4. The fronts were identified by WRF-Chem simulations via gradients in the potential temperature and sudden changes of wind direction in vertical cross-sections. Overall, the uncertainties in the simulations and the remarkable differences between the model outputs indicate that modelling of dust storms in the Middle East is really challenging due to the complex terrain, incorrect representation of the dust sources and soil/surface characteristics, and uncertainties in simulating the wind speed/direction and meteorological dynamics. Given the potential threat by dust storms, more attention should be directed to the dust model development in this region. © 2021 by the authors. Licensee MDPI, Basel, Switzerland.
- 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.
- ItemDetection and attribution of aerosol-cloud interactions in large-domain large-eddy simulations with the ICOsahedral Non-hydrostatic model(Katlenburg-Lindau : EGU, 2020) Costa-Surós, Montserrat; Sourdeval, Odran; Acquistapace, Claudia; Baars, Holger; Carbajal Henken, Cintia; Genz, Christa; Hesemann, Jonas; Jimenez, Cristofer; König, Marcel; Kretzschmar, Jan; Madenach, Nils; Meyer, Catrin I.; Schrödner, Roland; Seifert, Patric; Senf, Fabian; Brueck, Matthias; Cioni, Guido; Engels, Jan Frederik; Fieg, Kerstin; Gorges, Ksenia; Heinze, Rieke; Kumar Siligam, Pavan; Burkhardt, Ulrike; Crewell, Susanne; Hoose, Corinna; Seifert, Axel; Tegen, Ina; Quaas, JohannesClouds and aerosols contribute the largest uncertainty to current estimates and interpretations of the Earth's changing energy budget. Here we use a new-generation large-domain large-eddy model, ICON-LEM (ICOsahedral Non-hydrostatic Large Eddy Model), to simulate the response of clouds to realistic anthropogenic perturbations in aerosols serving as cloud condensation nuclei (CCN). The novelty compared to previous studies is that (i) the LEM is run in weather prediction mode and with fully interactive land surface over a large domain and (ii) a large range of data from various sources are used for the detection and attribution. The aerosol perturbation was chosen as peak-aerosol conditions over Europe in 1985, with more than fivefold more sulfate than in 2013. Observational data from various satellite and ground-based remote sensing instruments are used, aiming at the detection and attribution of this response. The simulation was run for a selected day (2 May 2013) in which a large variety of cloud regimes was present over the selected domain of central Europe. It is first demonstrated that the aerosol fields used in the model are consistent with corresponding satellite aerosol optical depth retrievals for both 1985 (perturbed) and 2013 (reference) conditions. In comparison to retrievals from groundbased lidar for 2013, CCN profiles for the reference conditions were consistent with the observations, while the ones for the 1985 conditions were not. Similarly, the detection and attribution process was successful for droplet number concentrations: the ones simulated for the 2013 conditions were consistent with satellite as well as new ground-based lidar retrievals, while the ones for the 1985 conditions were outside the observational range. For other cloud quantities, including cloud fraction, liquid water path, cloud base altitude and cloud lifetime, the aerosol response was small compared to their natural vari ability. Also, large uncertainties in satellite and ground-based observations make the detection and attribution difficult for these quantities. An exception to this is the fact that at a large liquid water path value (LWP > 200 g m-2), the control simulation matches the observations, while the perturbed one shows an LWP which is too large. The model simulations allowed for quantifying the radiative forcing due to aerosol-cloud interactions, as well as the adjustments to this forcing. The latter were small compared to the variability and showed overall a small positive radiative effect. The overall effective radiative forcing (ERF) due to aerosol-cloud interactions (ERFaci) in the simulation was dominated thus by the Twomey effect and yielded for this day, region and aerosol perturbation-2:6 W m-2. Using general circulation models to scale this to a global-mean present-day vs. pre-industrial ERFaci yields a global ERFaci of-0:8 W m-2 © 2020 Author(s).
- ItemHemispheric and Seasonal Contrast in Cloud Thermodynamic Phase From A‐Train Spaceborne Instruments(Hoboken, NJ : Wiley, 2021) Villanueva, Diego; Senf, Fabian; Tegen, InaAerosol-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.
- 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.
- ItemNatural sea-salt emissions moderate the climate forcing of anthropogenic nitrate(Katlenburg-Lindau : EGU, 2020) Chen, Ying; Cheng, Yafang; Ma, Nan; Wei, Chao; Ran, Liang; Wolke, Ralf; Größ, Johannes; Wang, Qiaoqiao; Denier van der Gon, Hugo A.C.; Spindler, Gerald; Lelieveld, Jos; Tegen, Ina; Su, Hang; Wiedensohler, AlfredNatural 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.
- 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).