2021, Brugger, Julia, Feulner, Georg, Hofmann, Matthias, Petri, Stefan

There is increasing evidence linking the mass-extinction event at the Cretaceous-Paleogene boundary to an asteroid impact near Chicxulub, Mexico. Here we use model simulations to explore the combined effect of sulfate aerosols, carbon dioxide and dust from the impact on the oceans and the marine biosphere in the immediate aftermath of the impact. We find a strong temperature decrease, a brief algal bloom caused by nutrients from both the deep ocean and the projectile, and moderate surface ocean acidification. Comparing the modeled longer-term post-impact warming and changes in carbon isotopes with empirical evidence points to a substantial release of carbon from the terrestrial biosphere. Overall, our results shed light on the decades to centuries after the Chicxulub impact which are difficult to resolve with proxy data.

2016, Kohn, Monika, Lohmann, Ulrike, Welti, André, Kanji, Zamin A.

The new Portable Immersion Mode Cooling chAmber (PIMCA) has been developed for online immersion freezing of single-immersed aerosol particles. PIMCA is a vertical extension of the established Portable Ice Nucleation Chamber (PINC). PIMCA immerses aerosol particles into cloud droplets before they enter PINC. Immersion freezing experiments on cloud droplets with a radius of 5–7 μm at a prescribed supercooled temperature (T) and water saturation can be conducted, while other ice nucleation mechanisms (deposition, condensation, and contact mode) are excluded. Validation experiments on reference aerosol (kaolinite, ammonium sulfate, and ammonium nitrate) showed good agreement with theory and literature. The PIMCA-PINC setup was tested in the field during the Zurich AMBient Immersion freezing Study (ZAMBIS) in spring 2014 in Zurich, Switzerland. Significant concentrations of submicron ambient aerosol triggering immersion freezing at T > 236 K were rare. The mean frozen cloud droplet number concentration was estimated to be 7.22·105 L−1 for T < 238 K and determined from the measured frozen fraction and cloud condensation nuclei (CCN) concentrations predicted for the site at a typical supersaturation of SS = 0.3%. This value should be considered as an upper limit of cloud droplet freezing via immersion and homogeneous freezing processes. The predicted ice nucleating particle (INP) concentration based on measured total aerosol larger than 0.5 μm and the parameterization by DeMott et al. (2010) at T = 238 K is INPD10=54 ± 39 L−1. This is a lower limit as supermicron particles were not sampled with PIMCA-PINC during ZAMBIS.

2020, Hoffmann, Erik H., Schrödner, Roland, Tilgner, Andreas, Wolke, Ralf, Herrmann, Hartmut

A condensed multiphase halogen and dimethyl sulfide (DMS) chemistry mechanism for application in chemistry transport models is developed by reducing the CAPRAM DMS module 1.0 (CAPRAM-DM1.0) and the CAPRAM halogen module 3.0 (CAPRAM-HM3.0). The reduction is achieved by determining the main oxidation pathways from analysing the mass fluxes of complex multiphase chemistry simulations with the air parcel model SPACCIM (SPectral Aerosol Cloud Chemistry Interaction Model). These simulations are designed to cover both pristine and polluted marine boundary layer conditions. Overall, the reduced CAPRAM-DM1.0 contains 32 gas-phase reactions, 5 phase transfers, and 12 aqueous-phase reactions, of which two processes are described as equilibrium reactions. The reduced CAPRAM-HM3.0 contains 199 gas-phase reactions, 23 phase transfers, and 87 aqueous-phase reactions. For the aqueous-phase chemistry, 39 processes are described as chemical equilibrium reactions. A comparison of simulations using the complete CAPRAM-DM1.0 and CAPRAM-HM3.0 mechanisms against the reduced ones indicates that the relative deviations are below 5 % for important inorganic and organic air pollutants and key reactive species under pristine ocean and polluted conditions. The reduced mechanism has been implemented into the chemical transport model COSMO-MUSCAT and tested by performing 2D simulations under prescribed meteorological conditions that investigate the effect of stable (stratiform cloud) and more unstable meteorological conditions (convective clouds) on marine multiphase chemistry. The simulated maximum concentration of HCl is of the order of 109 molecules cm−3 and that of BrO is around 1×107 molecules cm−3, reproducing the range of ambient measurements. Afterwards, the oxidation pathways of DMS in a cloudy marine atmosphere have been investigated in detail. The simulations demonstrate that clouds have both a direct and an indirect photochemical effect on the multiphase processing of DMS and its oxidation products. The direct photochemical effect is related to in-cloud chemistry that leads to high dimethyl sulfoxide (DMSO) oxidation rates and a subsequently enhanced formation of methane sulfonic acid compared to aerosol chemistry. The indirect photochemical effect is characterized by cloud shading, which occurs particularly in the case of stratiform clouds. The lower photolysis rate affects the activation of Br atoms and consequently lowers the formation of BrO radicals. The corresponding DMS oxidation flux is lowered by up to 30 % under thick optical clouds. Moreover, high updraught velocities lead to a strong vertical mixing of DMS into the free troposphere predominately under cloudy conditions. The photolysis of hypohalous acids (HOX, X = Cl, Br, or I) is reduced as well, resulting in higher HOX-driven sulfite-to-sulfate oxidation in aerosol particles below stratiform clouds. Altogether, the present model simulations have demonstrated the ability of the reduced mechanism to be applied in studying marine aerosol–cloud processing effects in regional models such as COSMO-MUSCAT. The reduced mechanism can be used also by other regional models for more adequate interpretations of complex marine field measurement data.

2009, Bierwirth, E., Wendisch, M., Ehrlich, A., Heese, B., Tesche, M., Althausen, D., Schladitz, A., Müller, D., Otto, S., Trautmann, T., Dinter, T., Von Hoyningen-Huene, W., Kahn, R.

In May-June 2006, airborne and ground-based solar (0.3-2.2 μm) and thermal infrared (4-42 μm) radiation measurements have been performed in Morocco within the Saharan Mineral Dust Experiment (SAMUM). Upwelling and downwelling solar irradiances have been measured using the Spectral Modular Airborne Radiation Measurement System (SMART)-Albedometer. With these data, the areal spectral surface albedo for typical surface types in southeastern Morocco was derived from airborne measurements for the first time. The results are compared to the surface albedo retrieved from collocated satellite measurements, and partly considerable deviations are observed. Using measured surface and atmospheric properties, the spectral and broad-band dust radiative forcing at top-of-atmosphere (TOA) and at the surface has been estimated. The impact of the surface albedo on the solar radiative forcing of Saharan dust is quantified. In the SAMUM case of 19 May 2006, TOA solar radiative forcing varies by 12 W m-2 per 0.1 surface-albedo change. For the thermal infrared component, values of up to +22 W m-2 were derived. The net (solar plus thermal infrared) TOA radiative forcing varies between -19 and +24 W m-2 for a broad-band solar surface albedo of 0.0 and 0.32, respectively. Over the bright surface of southeastern Morocco, the Saharan dust always has a net warming effect. © 2008 The Author Journal compilation © 2008 Blackwell Munksgaard.

2017, Gordon, Hamish, Kirkby, Jasper, Baltensperger, Urs, Bianchi, Federico, Breitenlechner, Martin, Curtius, Joachim, Dias, Antonio, Dommen, Josef, Donahue, Neil M., Dunne, Eimear M., Duplissy, Jonathan, Ehrhart, Sebastian, Flagan, Richard C., Frege, Carla, Fuchs, Claudia, Hansel, Armin, Hoyle, Christopher R., Kulmala, Markku, Kürten, Andreas, Lehtipalo, Katrianne, Makhmutov, Vladimir, Molteni, Ugo, Rissanen, Matti P., Stozkhov, Yuri, Tröstl, Jasmin, Tsagkogeorgas, Georgios, Wagner, Robert, Williamson, Christina, Wimmer, Daniela, Winkler, Paul M., Yan, Chao, Carslaw, Ken S.

New particle formation has been estimated to produce around half of cloud-forming particles in the present-day atmosphere, via gas-to-particle conversion. Here we assess the importance of new particle formation (NPF) for both the present-day and the preindustrial atmospheres. We use a global aerosol model with parametrizations of NPF from previously published CLOUD chamber experiments involving sulfuric acid, ammonia, organic molecules, and ions. We find that NPF produces around 67% of cloud condensation nuclei at 0.2% supersaturation (CCN0.2%) at the level of low clouds in the preindustrial atmosphere (estimated uncertainty range 45–84%) and 54% in the present day (estimated uncertainty range 38–66%). Concerning causes, we find that the importance of biogenic volatile organic compounds (BVOCs) in NPF and CCN formation is greater than previously thought. Removing BVOCs and hence all secondary organic aerosol from our model reduces low-cloud-level CCN concentrations at 0.2% supersaturation by 26% in the present-day atmosphere and 41% in the preindustrial. Around three quarters of this reduction is due to the tiny fraction of the oxidation products of BVOCs that have sufficiently low volatility to be involved in NPF and early growth. Furthermore, we estimate that 40% of preindustrial CCN0.2% are formed via ion-induced NPF, compared with 27% in the present day, although we caution that the ion-induced fraction of NPF involving BVOCs is poorly measured at present. Our model suggests that the effect of changes in cosmic ray intensity on CCN is small and unlikely to be comparable to the effect of large variations in natural primary aerosol emissions.

2008, Bauer, E., Petoukhov, V., Ganopolski, A., Eliseev, A.V.

The Earth system model CLIMBER-2 is extended by a scheme for calculating the climatic response to anthropogenic sulphur dioxide emissions. The scheme calculates the direct radiative forcing, the first indirect cloud albedo effect, and the second indirect cloud lifetime effect induced by geographically resolved sulphate aerosol burden. The simulated anthropogenic sulphate aerosol burden in the year 2000 amounts to 0.47 TgS. The best guesses for the radiative forcing due to the direct effect are -0.4 W m-2 and for the decrease in short-wave radiation due to all aerosol effects -0.8 W m-2. The simulated global warming by 1 K from 1850 to 2000 caused by anthropogenic greenhouse gases reduces to 0.6 K when the sulphate aerosol effects are included. The model's hydrological sensitivity of 4%/K is decreased by the second indirect effect to 0.8%/K. The quality of the geographically distributed climatic response to the historic emissions of sulphur dioxide and greenhouse gases makes the extended model relevant to computational efficient investigations of future climate change scenarios.

2017, Schmale, Julia, Henning, Silvia, Henzing, Bas, Keskinen, Helmi, Sellegri, Karine, Ovadnevaite, Jurgita, Bougiatioti, Aikaterini, Kalivitis, Nikos, Stavroulas, Iasonas, Jefferson, Anne, Park, Minsu, Schlag, Patrick, Kristensson, Adam, Iwamoto, Yoko, Pringle, Kirsty, Reddington, Carly, Aalto, Pasi, Äijälä, Mikko, Baltensperger, Urs, Bialek, Jakub, Birmili, Wolfram, Bukowiecki, Nicolas, Ehn, Mikael, Fjæraa, Ann Mari, Fiebig, Markus, Frank, Göran, Fröhlich, Roman, Frumau, Arnoud, Furuya, Masaki, Hammer, Emanuel, Heikkinen, Liine, Herrmann, Erik, Holzinger, Rupert, Hyono, Hiroyuki, Kanakidou, Maria, Kiendler-Scharr, Astrid, Kinouchi, Kento, Kos, Gerard, Kulmala, Markku, Mihalopoulos, Nikolaos, Motos, Ghislain, Nenes, Athanasios, O’Dowd, Colin, Paramonov, Mikhail, Petäjä, Tuukka, Picard, David, Poulain, Laurent, Prévôt, André Stephan Henry, Slowik, Jay, Sonntag, Andre, Swietlicki, Erik, Svenningsson, Birgitta, Tsurumaru, Hiroshi, Wiedensohler, Alfred, Wittbom, Cerina, Ogren, John A., Matsuki, Atsushi, Yum, Seong Soo, Myhre, Cathrine Lund, Carslaw, Ken, Stratmann, Frank, Gysel, Martin

Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment.

2017, Dipu, Sudhakar, Quaas, Johannes, Wolke, Ralf, Stoll, Jens, Mühlbauer, Andreas, Sourdeval, Odran, Salzmann, Marc, Heinold, Bernd, Tegen, Ina

The regional atmospheric model Consortium for Small-scale Modeling (COSMO) coupled to the Multi-Scale Chemistry Aerosol Transport model (Muscat) is extended in this work to represent aerosol-cloud interactions. Previously, only one-way interactions (scavenging of aerosol and in-cloud chemistry) and aerosol-radiation interactions were included in this model. The new version allows for a microphysical aerosol effect on clouds. For this, we use the optional two-moment cloud microphysical scheme in COSMO and the online-computed aerosol information for cloud condensation nuclei concentrations (Cccn), replacing the constant Cccn profile. In the radiation scheme, we have implemented a droplet-size-dependent cloud optical depth, allowing now for aerosol-cloud-radiation interactions. To evaluate the models with satellite data, the Cloud Feedback Model Intercomparison Project Observation Simulator Package (COSP) has been implemented. A case study has been carried out to understand the effects of the modifications, where the modified modeling system is applied over the European domain with a horizontal resolution of 0.25°g × g0.25°. To reduce the complexity in aerosol-cloud interactions, only warm-phase clouds are considered. We found that the online-coupled aerosol introduces significant changes for some cloud microphysical properties. The cloud effective radius shows an increase of 9.5g%, and the cloud droplet number concentration is reduced by 21.5g%.

2021-9-13, van Noije, Twan, Bergman, Tommi, Le Sager, Philippe, O'Donnell, Declan, Makkonen, Risto, Gonçalves-Ageitos, María, Döscher, Ralf, Fladrich, Uwe, von Hardenberg, Jost, Keskinen, Jukka-Pekka, Korhonen, Hannele, Laakso, Anton, Myriokefalitakis, Stelios, Ollinaho, Pirkka, Pérez García-Pando, Carlos, Reerink, Thomas, Schrödner, Roland, Wyser, Klaus, Yang, Shuting

This paper documents the global climate model EC-Earth3-AerChem, one of the members of the EC-Earth3 family of models participating in the Coupled Model Intercomparison Project Phase 6 (CMIP6). EC-Earth3-AerChem has interactive aerosols and atmospheric chemistry and contributes to the Aerosols and Chemistry Model Intercomparison Project (AerChemMIP). In this paper, we give an overview of the model, describe in detail how it differs from the other EC-Earth3 configurations, and outline the new features compared with the previously documented version of the model (EC-Earth 2.4). We explain how the model was tuned and spun up under preindustrial conditions and characterize the model's general performance on the basis of a selection of coupled simulations conducted for CMIP6. The net energy imbalance at the top of the atmosphere in the preindustrial control simulation is on average −0.09 W m−2 with a standard deviation due to interannual variability of 0.25 W m−2, showing no significant drift. The global surface air temperature in the simulation is on average 14.08 ∘C with an interannual standard deviation of 0.17 ∘C, exhibiting a small drift of 0.015 ± 0.005 ∘C per century. The model's effective equilibrium climate sensitivity is estimated at 3.9 ∘C, and its transient climate response is estimated at 2.1 ∘C. The CMIP6 historical simulation displays spurious interdecadal variability in Northern Hemisphere temperatures, resulting in a large spread across ensemble members and a tendency to underestimate observed annual surface temperature anomalies from the early 20th century onwards. The observed warming of the Southern Hemisphere is well reproduced by the model. Compared with the ECMWF (European Centre for Medium-Range Weather Forecasts) Reanalysis version 5 (ERA5), the surface air temperature climatology for 1995–2014 has an average bias of −0.86 ± 0.05 ∘C with a standard deviation across ensemble members of 0.35 ∘C in the Northern Hemisphere and 1.29 ± 0.02 ∘C with a corresponding standard deviation of 0.05 ∘C in the Southern Hemisphere. The Southern Hemisphere warm bias is largely caused by errors in shortwave cloud radiative effects over the Southern Ocean, a deficiency of many climate models. Changes in the emissions of near-term climate forcers (NTCFs) have significant effects on the global climate from the second half of the 20th century onwards. For the SSP3-7.0 Shared Socioeconomic Pathway, the model gives a global warming at the end of the 21st century (2091–2100) of 4.9 ∘C above the preindustrial mean. A 0.5 ∘C stronger warming is obtained for the AerChemMIP scenario with reduced emissions of NTCFs. With concurrent reductions of future methane concentrations, the warming is projected to be reduced by 0.5 ∘C.

2011, Jones, C.D., Hughes, J.K., Bellouin, N., Hardiman, S.C., Jones, G.S., Knight, J., Liddicoat, S., O'Connor, F.M., Andres, R.J., Bell, C., Boo, K.-O., Bozzo, A., Butchart, N., Cadule, P., Corbin, K.D., Doutriaux-Boucher, M., Friedlingstein, P., Gornall, J., Gray, L., Halloran, P.R., Hurtt, G., Ingram, W.J., Lamarque, J.-F., Law, R.M., Meinshausen, M., Osprey, S., Palin, E.J., Parsons, Chini, L., Raddatz, T., Sanderson, M.G., Sellar, A.A., Schurer, A., Valdes, P., Wood, N., Woodward, S., Yoshioka, M., Zerroukat, M.

The scientific understanding of the Earth's climate system, including thecentral question of how the climate system is likely to respond tohuman-induced perturbations, is comprehensively captured in GCMs and EarthSystem Models (ESM). Diagnosing the simulated climate response, andcomparing responses across different models, is crucially dependent ontransparent assumptions of how the GCM/ESM has been driven - especiallybecause the implementation can involve subjective decisions and may differbetween modelling groups performing the same experiment. This paper outlinesthe climate forcings and setup of the Met Office Hadley Centre ESM, HadGEM2-ES for the CMIP5 set of centennial experiments. We document theprescribed greenhouse gas concentrations, aerosol precursors, stratosphericand tropospheric ozone assumptions, as well as implementation of land-usechange and natural forcings for the HadGEM2-ES historical and futureexperiments following the Representative Concentration Pathways. Inaddition, we provide details of how HadGEM2-ES ensemble members wereinitialised from the control run and how the palaeoclimate and AMIPexperiments, as well as the "emission-driven" RCP experiments wereperformed.