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- ItemLong-term measurements of aerosol and carbon monoxide at the ZOTTO tall tower to characterize polluted and pristine air in the Siberian taiga(München : European Geopyhsical Union, 2013) Chi, X.; Winderlich, J.; Mayer, J.-C.; Panov, A.V.; Heimann, M.; Birmili, W.; Heintzenberg, J.; Cheng, Y.; Andreae, M.O.Siberia is one of few continental regions in the Northern Hemisphere where the atmosphere may sometimes approach pristine background conditions. We present the time series of aerosol and carbon monoxide (CO) measurements between September 2006 and December 2011 at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E). We investigate the seasonal, weekly and diurnal variations of aerosol properties (including absorption and scattering coefficients and derived parameters, such as equivalent black carbon (BCe), Ångström exponent, single scattering albedo, and backscattering ratio) and the CO mixing ratios. Criteria were established to distinguish polluted from near-pristine air masses, providing quantitative characteristics for each type. Depending on the season, 23–36% of the sampling time at ZOTTO was found to be representative of a clean atmosphere. The summer pristine data indicate that primary biogenic and secondary organic aerosol formation are quite strong particle sources in the Siberian taiga. The summer seasons 2007–2008 were dominated by an Aitken mode around 80 nm size, whereas the summer 2009 with prevailing easterly winds produced particles in the accumulation mode around 200 nm size. We found these differences to be mainly related to air temperature, through its effect on the production rates of biogenic volatile organic compounds (VOC) precursor gases. In winter, the particle size distribution peaked at 160 nm, and the footprint of clean background air was characteristic for aged particles from anthropogenic sources at great distances from ZOTTO and diluted biofuel burning emissions from domestic heating. The wintertime polluted air originates mainly from large cities south and southwest of the site; these particles have a dominant mode around 100 nm, and the ΔBCe / ΔCO ratio of 7–11 ng m−3 ppb−1 suggests dominant contributions from coal and biofuel burning for heating. During summer, anthropogenic emissions are the dominant contributor to the pollution particles at ZOTTO, while only 12% of the polluted events are classified as biomass-burning-dominated, but then often associated with extremely high CO concentrations and aerosol absorption coefficients. Two biomass-burning case studies revealed different ΔBCe / ΔCO ratios from different fire types, with the agricultural fires in April~2008 yielding a very high ratio of 21 ng m−3 ppb−1. Overall, we find that anthropogenic sources dominate the aerosol population at ZOTTO most of the time, even during nominally clean episodes in winter, and that near-pristine conditions are encountered only in the growing season and then only episodically.
- ItemCharacterization of submicron particles influenced by mixed biogenic and anthropogenic emissions using high-resolution aerosol mass spectrometry: Results from CARES(München : European Geopyhsical Union, 2012) Setyan, A.; Zhang, Q.; Merkel, M.; Knighton, W.B.; Sun, Y.; Song, C.; Shilling, J.E.; Onasch, T.B.; Herndon, S.C.; Worsnop, D.R.; Fast, J.D.; Zaveri, R.A.; Berg, L.K.; Wiedensohler, A.; Flowers, B.A.; Dubey, M.K.; Subramanian, R.An Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed during the Carbonaceous Aerosols and Radiative Effects Study (CARES) that took place in northern California in June 2010. We present results obtained at Cool (denoted as the T1 site of the project) in the foothills of the Sierra Nevada Mountains, where intense biogenic emissions are periodically mixed with urban outflow transported by daytime southwesterly winds from the Sacramento metropolitan area. During this study, the average mass loading of submicrometer particles (PM1) was 3.0 μg m−3, dominated by organics (80%) and sulfate (9.9%). The organic aerosol (OA) had a nominal formula of C1H1.38N0.004OM0.44, thus an average organic mass-to-carbon (OM/OC) ratio of 1.70. Two distinct oxygenated OA factors were identified via Positive matrix factorization (PMF) of the high-resolution mass spectra of organics. The more oxidized MO-OOA (O/C = 0.54) was interpreted as a surrogate for secondary OA (SOA) influenced by biogenic emissions whereas the less oxidized LO-OOA (O/C = 0.42) was found to represent SOA formed in photochemically processed urban emissions. LO-OOA correlated strongly with ozone and MO-OOA correlated well with two 1st generation isoprene oxidation products (methacrolein and methyl vinyl ketone), indicating that both SOAs were relatively fresh. A hydrocarbon like OA (HOA) factor was also identified, representing primary emissions mainly due to local traffic. On average, SOA (= MO-OOA + LO-OOA) accounted for 91% of the total OA mass and 72% of the PM1 mass observed at Cool. Twenty three periods of urban plumes from T0 (Sacramento) to T1 (Cool) were identified using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). The average PM1 mass loading was considerably higher in urban plumes than in air masses dominated by biogenic SOA. The change in OA mass relative to CO (ΔOA/ΔCO) varied in the range of 5-196 μg m−3 ppm−1, reflecting large variability in SOA production. The highest ΔOA/ΔCO was reached when air masses were dominated by anthropogenic emissions in the presence of a high concentration of biogenic volatile organic compounds (BVOCs). This ratio, which was 97 μg m−3 ppm−1 on average, was much higher than when urban plumes arrived in a low BVOC environment (~36 μg m−3 ppm−1) or during other periods dominated by biogenic SOA (35 μg m−3 ppm−1). These results demonstrate that SOA formation is enhanced when anthropogenic emissions interact with biogenic precursors.
- ItemProfiling of Saharan dust from the Caribbean to western Africa - Part 2: Shipborne lidar measurements versus forecasts(Katlenburg-Lindau : EGU, 2017) Ansmann, Albert; Rittmeister, Franziska; Engelmann, Ronny; Basart, Sara; Jorba, Oriol; Spyrou, Christos; Remy, Samuel; Skupin, Annett; Baars, Holger; Seifert, Patric; Senf, Fabian; Kanitz, ThomasA unique 4-week ship cruise from Guadeloupe to Cabo Verde in April-May 2013 see part 1, Rittmeister et al. (2017) is used for an in-depth comparison of dust profiles observed with a polarization/Raman lidar aboard the German research vessel Meteor over the remote tropical Atlantic and respective dust forecasts of a regional (SKIRON) and two global atmospheric (dust) transport models (NMMB/BSC-Dust, MACC/CAMS). New options of model-observation comparisons are presented. We analyze how well the modeled fine dust (submicrometer particles) and coarse dust contributions to light extinction and mass concentration match respective lidar observations, and to what extent models, adjusted to aerosol optical thickness observations, are able to reproduce the observed layering and mixing of dust and non-dust (mostly marine) aerosol components over the remote tropical Atlantic. Based on the coherent set of dust profiles at well-defined distances from Africa (without any disturbance by anthropogenic aerosol sources over the ocean), we investigate how accurately the models handle dust removal at distances of 1500g km to more than 5000g km west of the Saharan dust source regions. It was found that (a) dust predictions are of acceptable quality for the first several days after dust emission up to 2000g km west of the African continent, (b) the removal of dust from the atmosphere is too strong for large transport paths in the global models, and (c) the simulated fine-to-coarse dust ratio (in terms of mass concentration and light extinction) is too high in the models compared to the observations. This deviation occurs initially close to the dust sources and then increases with distance from Africa and thus points to an overestimation of fine dust emission in the models.
- ItemFormation of organic aerosol in the Paris region during the MEGAPOLI summer campaign: Evaluation of the volatility-basis-set approach within the CHIMERE model(Göttingen : Copernicus, 2013) Zhang, Q.J.; Beekmann, M.; Drewnick, F.; Freutel, F.; Schneider, J.; Crippa, M.; Prevot, A.S.H.; Baltensperger, U.; Poulain, L.; Wiedensohler, A.; Sciare, J.; Gros, V.; Borbon, A.; Colomb, A.; Michoud, V.; Doussin, J.-F.; Denier Van Der Gon, H.A.C.; Haeffelin, M.; Dupont, J.-C.; Siour, G.; Petetin, H.; Bessagnet, B.; Pandis, S.N.; Hodzic, A.; Sanchez, O.; Honoré, C.; Perrussel, O.Simulations with the chemistry transport model CHIMERE are compared to measurements performed during the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) summer campaign in the Greater Paris region in July 2009. The volatility-basis-set approach (VBS) is implemented into this model, taking into account the volatility of primary organic aerosol (POA) and the chemical aging of semi-volatile organic species. Organic aerosol is the main focus and is simulated with three different configurations with a modified treatment of POA volatility and modified secondary organic aerosol (SOA) formation schemes. In addition, two types of emission inventories are used as model input in order to test the uncertainty related to the emissions. Predictions of basic meteorological parameters and primary and secondary pollutant concentrations are evaluated, and four pollution regimes are defined according to the air mass origin. Primary pollutants are generally overestimated, while ozone is consistent with observations. Sulfate is generally overestimated, while ammonium and nitrate levels are well simulated with the refined emission data set. As expected, the simulation with non-volatile POA and a single-step SOA formation mechanism largely overestimates POA and underestimates SOA. Simulation of organic aerosol with the VBS approach taking into account the aging of semi-volatile organic compounds (SVOC) shows the best correlation with measurements. High-concentration events observed mostly after long-range transport are well reproduced by the model. Depending on the emission inventory used, simulated POA levels are either reasonable or underestimated, while SOA levels tend to be overestimated. Several uncertainties related to the VBS scheme (POA volatility, SOA yields, the aging parameterization), to emission input data, and to simulated OH levels can be responsible for this behavior. Despite these uncertainties, the implementation of the VBS scheme into the CHIMERE model allowed for much more realistic organic aerosol simulations for Paris during summertime. The advection of SOA from outside Paris is mostly responsible for the highest OA concentration levels. During advection of polluted air masses from northeast (Benelux and Central Europe), simulations indicate high levels of both anthropogenic and biogenic SOA fractions, while biogenic SOA dominates during periods with advection from Southern France and Spain.
- ItemImportance of secondary organic aerosol formation of iα/i-pinene, limonene, and im/i-cresol comparing day- And nighttime radical chemistry(Katlenburg-Lindau : European Geosciences Union, 2021) Mutzel, Anke; Zhang, Yanli; Böge, Olaf; Rodigast, Maria; Kolodziejczyk, Agata; Wang, Xinming; Herrmann, HartmutThe oxidation of biogenic and anthropogenic compounds leads to the formation of secondary organic aerosol mass (SOA). The present study aims to investigate span classCombining double low line"inline-formula"iα/i/span-pinene, limonene, and span classCombining double low line"inline-formula"im/i/span-cresol with regards to their SOA formation potential dependent on relative humidity (RH) under night- (NOspan classCombining double low line"inline-formula"3/span radicals) and daytime conditions (OH radicals) and the resulting chemical composition. It was found that SOA formation potential of limonene with NOspan classCombining double low line"inline-formula"3/span under dry conditions significantly exceeds that of the OH-radical reaction, with SOA yields of 15-30 % and 10-21 %, respectively. Additionally, the nocturnal SOA yield was found to be very sensitive towards RH, yielding more SOA under dry conditions. In contrast, the SOA formation potential of span classCombining double low line"inline-formula"iα/i/span-pinene with NOspan classCombining double low line"inline-formula"3/span slightly exceeds that of the OH-radical reaction, independent from RH. On average, span classCombining double low line"inline-formula"iα/i/span-pinene yielded SOA with about 6-7 % from NOspan classCombining double low line"inline-formula"3/span radicals and 3-4 % from OH-radical reaction. Surprisingly, unexpectedly high SOA yields were found for span classCombining double low line"inline-formula"im/i/span-cresol oxidation with OH radicals (3-9 %), with the highest yield under elevated RH (9 %), which is most likely attributable to a higher fraction of 3-methyl-6-nitro-catechol (MNC). While span classCombining double low line"inline-formula"iα/i/span-pinene and span classCombining double low line"inline-formula"im/i/span-cresol SOA was found to be mainly composed of water-soluble compounds, 50-68 % of nocturnal SOA and 22-39 % of daytime limonene SOA are water-insoluble. The fraction of SOA-bound peroxides which originated from span classCombining double low line"inline-formula"iα/i/span-pinene varied between 2 and 80 % as a function of RH./p pFurthermore, SOA from span classCombining double low line"inline-formula"iα/i/span-pinene revealed pinonic acid as the most important particle-phase constituent under day- and nighttime conditions with a fraction of 1-4 %. Other compounds detected are norpinonic acid (0.05-1.1 % mass fraction), terpenylic acid (0.1-1.1 % mass fraction), pinic acid (0.1-1.8 % mass fraction), and 3-methyl-1,2,3-tricarboxylic acid (0.05-0.5 % mass fraction). All marker compounds showed higher fractions under dry conditions when formed during daytime and showed almost no RH effect when formed during night./p © 2021 Copernicus GmbH. All rights reserved.
- ItemThe shared socio-economic pathway (SSP) greenhouse gas concentrations and their extensions to 2500(Katlenburg-Lindau : Copernicus, 2020) Meinshausen, Malte; Nicholls, Zebedee R. J.; Lewis, Jared; Gidden, Matthew J.; Vogel, Elisabeth; Freund, Mandy; Beyerle, Urs; Gessner, Claudia; Nauels, Alexander; Bauer, Nico; Canadell, Josep G.; Daniel, John S.; John, Andrew; Krummel, Paul B.; Luderer, Gunnar; Meinshausen, Nicolai; Montzka, Stephen A.; Rayner, Peter J.; Reimann, Stefan; Smith, Steven J.; van den Berg, Marten; Velders, Guus J. M.; Vollmer, Martin K.; Wang, Ray H. J.Anthropogenic increases in atmospheric greenhouse gas concentrations are the main driver of current and future climate change. The integrated assessment community has quantified anthropogenic emissions for the shared socio-economic pathway (SSP) scenarios, each of which represents a different future socio-economic projection and political environment. Here, we provide the greenhouse gas concentrations for these SSP scenarios – using the reduced-complexity climate–carbon-cycle model MAGICC7.0. We extend historical, observationally based concentration data with SSP concentration projections from 2015 to 2500 for 43 greenhouse gases with monthly and latitudinal resolution. CO2 concentrations by 2100 range from 393 to 1135 ppm for the lowest (SSP1-1.9) and highest (SSP5-8.5) emission scenarios, respectively. We also provide the concentration extensions beyond 2100 based on assumptions regarding the trajectories of fossil fuels and land use change emissions, net negative emissions, and the fraction of non-CO2 emissions. By 2150, CO2 concentrations in the lowest emission scenario are approximately 350 ppm and approximately plateau at that level until 2500, whereas the highest fossil-fuel-driven scenario projects CO2 concentrations of 1737 ppm and reaches concentrations beyond 2000 ppm by 2250. We estimate that the share of CO2 in the total radiative forcing contribution of all considered 43 long-lived greenhouse gases increases from 66 % for the present day to roughly 68 % to 85 % by the time of maximum forcing in the 21st century. For this estimation, we updated simple radiative forcing parameterizations that reflect the Oslo Line-By-Line model results. In comparison to the representative concentration pathways (RCPs), the five main SSPs (SSP1-1.9, SSP1-2.6, SSP2-4.5, SSP3-7.0, and SSP5-8.5) are more evenly spaced and extend to lower 2100 radiative forcing and temperatures. Performing two pairs of six-member historical ensembles with CESM1.2.2, we estimate the effect on surface air temperatures of applying latitudinally and seasonally resolved GHG concentrations. We find that the ensemble differences in the March–April–May (MAM) season provide a regional warming in higher northern latitudes of up to 0.4 K over the historical period, latitudinally averaged of about 0.1 K, which we estimate to be comparable to the upper bound (∼5 % level) of natural variability. In comparison to the comparatively straight line of the last 2000 years, the greenhouse gas concentrations since the onset of the industrial period and this studies' projections over the next 100 to 500 years unequivocally depict a “hockey-stick” upwards shape. The SSP concentration time series derived in this study provide a harmonized set of input assumptions for long-term climate science analysis; they also provide an indication of the wide set of futures that societal developments and policy implementations can lead to – ranging from multiple degrees of future warming on the one side to approximately 1.5 ∘C warming on the other.
- ItemGlobal emissions pathways under different socioeconomic scenarios for use in CMIP6: a dataset of harmonized emissions trajectories through the end of the century(Katlenburg-Lindau : Copernicus, 2019) Gidden, Matthew J.; Riahi, Keywan; Smith, Steven J.; Fujimori, Shinichiro; Luderer, Gunnar; Kriegler, Elmar; van Vuuren, Detlef P.; van den Berg, Maarten; Feng, Leyang; Klein, David; Calvin, Katherine; Doelman, Jonathan C.; Frank, Stefan; Fricko, Oliver; Harmsen, Mathijs; Hasegawa, Tomoko; Havlik, Petr; Hilaire, Jérôme; Hoesly, Rachel; Horing, Jill; Popp, Alexander; Stehfest, Elke; Takahashi, KiyoshiWe present a suite of nine scenarios of future emissions trajectories of anthropogenic sources, a key deliverable of the ScenarioMIP experiment within CMIP6. Integrated assessment model results for 14 different emissions species and 13 emissions sectors are provided for each scenario with consistent transitions from the historical data used in CMIP6 to future trajectories using automated harmonization before being downscaled to provide higher emissions source spatial detail. We find that the scenarios span a wide range of end-of-century radiative forcing values, thus making this set of scenarios ideal for exploring a variety of warming pathways. The set of scenarios is bounded on the low end by a 1.9 W m−2 scenario, ideal for analyzing a world with end-of-century temperatures well below 2 ∘C, and on the high end by a 8.5 W m−2 scenario, resulting in an increase in warming of nearly 5 ∘C over pre-industrial levels. Between these two extremes, scenarios are provided such that differences between forcing outcomes provide statistically significant regional temperature outcomes to maximize their usefulness for downstream experiments within CMIP6. A wide range of scenario
- 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.
- ItemInfrequent new particle formation over the remote boreal forest of Siberia(Amsterdam [u.a.] : Elsevier Science, 2018) Wiedensohler, A.; Ma, N.; Birmili, W.; Heintzenberg, J.; Ditas, F.; Andreae, M.O.; Panov, A.Aerosol particle number size distributions (PNSD) were investigated to verify, if extremely low-volatility organic vapors (ELVOC) from natural sources alone could induce new particle formation and growth events over the remote boreal forest region of Siberia, hundreds of kilometers away from significant anthropogenic sources. We re-evaluated observations determined at a height of 300 m of the remote observatory ZOTTO (Zotino Tall Tower Observatory, http://www.zottoproject.org). We found that new particle formation events occurred only on 11 days in a 3-year period, suggesting that homogeneous nucleation with a subsequent condensational growth could not be the major process, maintaining the particle number concentration in the planetary boundary layer of the remote boreal forest area of Siberia. © 2018 Elsevier Ltd
- ItemGeochemistry of PM10 over Europe during the EMEP intensive measurement periods in summer 2012 and winter 2013(München : European Geopyhsical Union, 2016) Alastuey, Andrés; Querol, Xavier; Aas, Wenche; Lucarelli, Franco; Pérez, Noemí; Moreno, Teresa; Cavalli, Fabrizia; Areskoug, Hans; Balan, Violeta; Catrambone, Maria; Ceburnis, Darius; Cerro, José C.; Conil, Sébastien; Gevorgyan, Lusine; Hueglin, Christoph; Imre, Kornelia; Jaffrezo, Jean-Luc; Leeson, Sarah R.; Mihalopoulos, Nikolaos; Mitosinkova, Marta; O'Dowd, Colin D.; Pey, Jorge; Putaud, Jean-Philippe; Riffault, Véronique; Ripoll, Anna; Sciare, Jean; Sellegri, Karine; Spindler, Gerald; Yttri, Karl EspenThe third intensive measurement period (IMP) organised by the European Monitoring and Evaluation Programme (EMEP) under the UNECE CLTRAP took place in summer 2012 and winter 2013, with PM10 filter samples concurrently collected at 20 (16 EMEP) regional background sites across Europe for subsequent analysis of their mineral dust content. All samples were analysed by the same or a comparable methodology. Higher PM10 mineral dust loadings were observed at most sites in summer (0.5–10 µg m−3) compared to winter (0.2–2 µg m−3), with the most elevated concentrations in the southern- and easternmost countries, accounting for 20–40 % of PM10. Saharan dust outbreaks were responsible for the high summer dust loadings at western and central European sites, whereas regional or local sources explained the elevated concentrations observed at eastern sites. The eastern Mediterranean sites experienced elevated levels due to African dust outbreaks during both summer and winter. The mineral dust composition varied more in winter than in summer, with a higher relative contribution of anthropogenic dust during the former period. A relatively high contribution of K from non-mineral and non-sea-salt sources, such as biomass burning, was evident in winter at some of the central and eastern European sites. The spatial distribution of some components and metals reveals the influence of specific anthropogenic sources on a regional scale: shipping emissions (V, Ni, and SO42−) in the Mediterranean region, metallurgy (Cr, Ni, and Mn) in central and eastern Europe, high temperature processes (As, Pb, and SO42−) in eastern countries, and traffic (Cu) at sites affected by emissions from nearby cities.