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- 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
- ItemEURODELTA III exercise: An evaluation of air quality models’ capacity to reproduce the carbonaceous aerosol(Amsterdam : Elsevier, 2019) Mircea, Mihaela; Bessagnet, Bertrand; D'Isidoro, Massimo; Pirovano, Guido; Aksoyoglu, Sebnem; Ciarelli, Giancarlo; Tsyro, Svetlana; Manders, Astrid; Bieser, Johannes; Stern, Rainer; Vivanco, Marta García; Cuvelier, Cornelius; Aas, Wenche; Prévôt, André S.H.; Aulinger, Armin; Briganti, Gino; Calori, Giuseppe; Cappelletti, Andrea; Colette, Augustin; Couvidat, Florian; Fagerli, Hilde; Finardi, Sandro; Kranenburg, Richard; Rouïl, Laurence; Silibello, Camillo; Spindler, Gerald; Poulain, Laurent; Herrmann, Hartmut; Jimenez, Jose L.; Day, Douglas A.; Tiitta, Petri; Carbone, SamaraThe carbonaceous aerosol accounts for an important part of total aerosol mass, affects human health and climate through its effects on physical and chemical properties of the aerosol, yet the understanding of its atmospheric sources and sinks is still incomplete. This study shows the state-of-the-art in modelling carbonaceous aerosol over Europe by comparing simulations performed with seven chemical transport models (CTMs) currently in air quality assessments in Europe: CAMx, CHIMERE, CMAQ, EMEP/MSC-W, LOTOS-EUROS, MINNI and RCGC. The simulations were carried out in the framework of the EURODELTA III modelling exercise and were evaluated against field measurements from intensive campaigns of European Monitoring and Evaluation Programme (EMEP) and the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI). Model simulations were performed over the same domain, using as much as possible the same input data and covering four seasons: summer (1–30 June 2006), winter (8 January – 4 February 2007), autumn (17 September- 15 October 2008) and spring (25 February - 26 March 2009). The analyses of models’ performances in prediction of elemental carbon (EC) for the four seasons and organic aerosol components (OA) for the last two seasons show that all models generally underestimate the measured concentrations. The maximum underestimation of EC is about 60% and up to about 80% for total organic matter (TOM). The underestimation of TOM outside of highly polluted area is a consequence of an underestimation of secondary organic aerosol (SOA), in particular of its main contributor: biogenic secondary aerosol (BSOA). This result is independent on the SOA modelling approach used and season. The concentrations and daily cycles of total primary organic matter (TPOM) are generally better reproduced by the models since they used the same anthropogenic emissions. However, the combination of emissions and model formulation leads to overestimate TPOM concentrations in 2009 for most of the models. All models capture relatively well the SOA daily cycles at rural stations mainly due to the spatial resolution used in the simulations. For the investigated carbonaceous aerosol compounds, the differences between the concentrations simulated by different models are lower than the differences between the concentrations simulated with a model for different seasons. © 2019 The Authors
- ItemThe RCP greenhouse gas concentrations and their extensions from 1765 to 2300(Dordrecht [u.a.] : Springer, 2011) Meinshausen, M.; Smith, S.J.; Calvin, K.; Daniel, J.S.; Kainuma, M.L.T.; Lamarque, J.; Matsumoto, K.; Montzka, S.A.; Raper, S.C.B.; Riahi, K.; Thomson, A.; Velders, G.J.M.; van Vuuren, D.P.P.We present the greenhouse gas concentrations for the Representative Concentration Pathways (RCPs) and their extensions beyond 2100, the Extended Concentration Pathways (ECPs). These projections include all major anthropogenic greenhouse gases and are a result of a multi-year effort to produce new scenarios for climate change research. We combine a suite of atmospheric concentration observations and emissions estimates for greenhouse gases (GHGs) through the historical period (1750-2005) with harmonized emissions projected by four different Integrated Assessment Models for 2005-2100. As concentrations are somewhat dependent on the future climate itself (due to climate feedbacks in the carbon and other gas cycles), we emulate median response characteristics of models assessed in the IPCC Fourth Assessment Report using the reduced-complexity carbon cycle climate model MAGICC6. Projected 'best-estimate' global-mean surface temperature increases (using inter alia a climate sensitivity of 3°C) range from 1.5°C by 2100 for the lowest of the four RCPs, called both RCP3-PD and RCP2. 6, to 4.5°C for the highest one, RCP8. 5, relative to pre-industrial levels. Beyond 2100, we present the ECPs that are simple extensions of the RCPs, based on the assumption of either smoothly stabilizing concentrations or constant emissions: For example, the lower RCP2. 6 pathway represents a strong mitigation scenario and is extended by assuming constant emissions after 2100 (including net negative CO2 emissions), leading to CO2 concentrations returning to 360 ppm by 2300. We also present the GHG concentrations for one supplementary extension, which illustrates the stringent emissions implications of attempting to go back to ECP4. 5 concentration levels by 2250 after emissions during the 21st century followed the higher RCP6 scenario. Corresponding radiative forcing values are presented for the RCP and ECPs.
- ItemThe EMEP Intensive Measurement Period campaign, 2008-2009: Characterizing carbonaceous aerosol at nine rural sites in Europe(Katlenburg-Lindau : EGU, 2019) Yttri, Karl Espen; Simpson, David; Bergström, Robert; Kiss, Gyula; Szidat, Sönke; Ceburnis, Darius; Eckhardt, Sabine; Hueglin, Christoph; Nøjgaard, Jacob Klenø; Perrino, Cinzia; Pisso, Ignazio; Prevot, Andre Stephan Henry; Putaud, Jean-Philippe; Spindler, Gerald; Vana, Milan; Zhang, Yan-Lin; Aas, WencheCarbonaceous aerosol (total carbon, TCp) was source apportioned at nine European rural background sites, as part of the European Measurement and Evaluation Programme (EMEP) Intensive Measurement Periods in fall 2008 and winter/spring 2009. Five predefined fractions were apportioned based on ambient measurements: elemental and organic carbon, from combustion of biomass (ECbb and OCbb) and from fossil-fuel (ECff and OCff) sources, and remaining non-fossil organic carbon (OCrnf), dominated by natural sources.OCrnf made a larger contribution to TCp than anthropogenic sources (ECbb, OCbb, ECff, and OCff) at four out of nine sites in fall, reflecting the vegetative season, whereas anthropogenic sources dominated at all but one site in winter/spring. Biomass burning (OCbb + ECbb) was the major anthropogenic source at the central European sites in fall, whereas fossil-fuel (OCff + ECff) sources dominated at the southernmost and the two northernmost sites. Residential wood burning emissions explained 30 %-50 % of TCp at most sites in the first week of sampling in fall, showing that this source can be the dominant one, even outside the heating season. In winter/spring, biomass burning was the major anthropogenic source at all but two sites, reflecting increased residential wood burning emissions in the heating season. Fossil-fuel sources dominated EC at all sites in fall, whereas there was a shift towards biomass burning for the southernmost sites in winter/spring.Model calculations based on base-case emissions (mainly officially reported national emissions) strongly underpredicted observational derived levels of OCbb and ECbb outside Scandinavia. Emissions based on a consistent bottom-up inventory for residential wood burning (and including intermediate volatility compounds, IVOCs) improved model results compared to the base-case emissions, but modeled levels were still substantially underestimated compared to observational derived OCbb and ECbb levels at the southernmost sites.Our study shows that natural sources are a major contributor to carbonaceous aerosol in Europe, even in fall and in winter/spring, and that residential wood burning emissions are equally as large as or larger than that of fossil-fuel sources, depending on season and region. The poorly constrained residential wood burning emissions for large parts of Europe show the obvious need to improve emission inventories, with harmonization of emission factors between countries likely being the most important step to improve model calculations for biomass burning emissions, and European PM2.5 concentrations in general. © Author(s) 2019.