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- ItemCharacterization of Saharan dust, marine aerosols and mixtures of biomass-burning aerosols and dust by means of multi-wavelength depolarization and Raman lidar measurements during SAMUM 2(Milton Park : Taylor & Francis, 2017) Groß, Silke; Tesche, Matthias; Freudenthaler, Volker; Toledano, Carlos; Wiegner, Matthias; Ansmann, Albert; Althausen, Dietrich; Seefeldner, MeinhardThe particle linear depolarization ratio δp of Saharan dust, marine aerosols and mixtures of biomass-burning aerosols from southern West Africa and Saharan dust was determined at three wavelengths with three lidar systems during the SAharan Mineral dUst experiMent 2 at the airport of Praia, Cape Verde, between 22 January and 9 February 2008. The lidar ratio Sp of these major types of tropospheric aerosols was analysed at two wavelengths. For Saharan dust, we find wavelength dependent mean particle linear depolarization ratios δp of 0.24–0.27 at 355 nm, 0.29–0.31 at 532 nm and 0.36–0.40 at 710 nm, and wavelength independent mean lidar ratios Sp of 48–70 sr. Mixtures of biomass-burning aerosols and dust show wavelength independent values of δp and Sp between 0.12–0.23 and 57–98 sr, respectively. The mean values of marine aerosols range independent of wavelength for δp from 0.01 to 0.03 and for Sp from 14 to 24 sr.
- ItemDust mobilization and aerosol transport from West Africa to Cape Verde - a meteorological overview of SAMUM-2(Milton Park : Taylor & Francis, 2017) Knippertz, Peter; Tesche, Matthias; Heinold, Bernd; Kandler, Konrad; Toledano, Carlos; Esselborn, MichaelThe second field campaign of the SAharan Mineral dUst experiMent (SAMUM-2) was performed between 15 January and 14 February 2008 at the airport of Praia, Cape Verde, and provided valuable information to study the westward transport of Saharan dust and the mixing with biomass-burning smoke and sea-salt aerosol. Here lidar, meteorological, and particle measurements at Praia, together with operational analyses, trajectories, and satellite and synoptic station data are used to give an overview of the meteorological conditions and to place other SAMUM-2 measurements into a large-scale context. It is demonstrated that wintertime dust conditions at Cape Verde are closely related to the movement and intensification of mid-latitude high-pressure systems and the associated pressure gradients at their southern flanks. These cause dust emission over Mauritania, Mali, and Niger, and subsequent westward transport to Cape Verde within about 1–5 d. Dust emissions often peak around midday, suggesting a relation to daytime mixing of momentum from nocturnal low-level jets to the surface. The dust layer over Cape Verde is usually restricted to the lowest 1.5 km of the atmosphere. During periods with near-surface wind speeds about 5.5 ms−1, a maritime aerosol layer develops which often mixes with dust from above. On most days, the middle levels up to about 5 km additionally contain smoke that can be traced back to sources in southernWest Africa. Above this layer, clean air masses are transported to Cape Verde with the westerly flow at the southern side of the subtropical jet. The penetration of extra-tropical disturbances to low latitudes can bring troposphere-deep westerly flow and unusually clean conditions to the region.
- ItemTreatment of non-ideality in the SPACCIM multiphase model - Part 1: Model development(München : European Geopyhsical Union, 2016) Rusumdar, A.J.; Wolke, R.; Tilgner, A.; Herrmann, H.Ambient tropospheric deliquesced particles generally comprise a complex mixture of electrolytes, organic compounds, and water. Dynamic modeling of physical and chemical processes in this complex matrix is challenging. Thus, up-to-date multiphase chemistry models generally do not consider non-ideal solution effects. Therefore, the present study was aimed at presenting further development of the SPACCIM (Spectral Aerosol Cloud Chemistry Interaction Model) through treatment of solution non-ideality, which has not been considered before. The present paper firstly describes the model developments including (i) the implementation of solution non-ideality in aqueous-phase reaction kinetics in the SPACCIM framework, (ii) the advancements in the coupling scheme of microphysics and multiphase chemistry and (iii) the required adjustments of the numerical schemes, especially in the sparse linear solver and the calculation of the Jacobian. Secondly, results of sensitivity investigations are outlined, aiming at the evaluation of different activity coefficient modules and the examination of the contributions of different intermolecular forces to the overall activity coefficients. Finally, first results obtained with the new model framework are presented. The SPACCIM parcel model was developed and, so far, applied for the description of aerosol–cloud interactions. To advance SPACCIM also for modeling physical and chemical processes in deliquesced particles, the solution non-ideality has to be taken into account by utilizing activities in reaction terms instead of aqueous concentrations. The main goal of the extended approach was to provide appropriate activity coefficients for solved species. Therefore, an activity coefficient module was incorporated into the kinetic model framework of SPACCIM. Based on an intercomparison of different activity coefficient models and the comparison with experimental data, the AIOMFAC approach was implemented and extended by additional interaction parameters from the literature for mixed organic–inorganic systems. Moreover, the performance and the capability of the applied activity coefficient module were evaluated by means of water activity measurements, literature data and results of other activity coefficient models. Comprehensive comparison studies showed that the SpactMod (SPACCIM activity coefficient module) is valuable for predicting the thermodynamic behavior of complex mixtures of multicomponent atmospheric aerosol particles. First simulations with a detailed chemical mechanism have demonstrated the applicability of SPACCIM-SpactMod. The simulations indicate that the treatment of solution non-ideality might be needed for modeling multiphase chemistry processes in deliquesced particles. The modeled activity coefficients imply that chemical reaction fluxes of chemical processes in deliquesced particles can be both decreased and increased depending on the particular species involved in the reactions. For key ions, activity coefficients on the order of 0.1–0.8 and a strong dependency on the charge state as well as the RH conditions are modeled, implying a lowered chemical processing of ions in concentrated solutions. In contrast, modeled activity coefficients of organic compounds are in some cases larger than 1 under deliquesced particle conditions and suggest the possibility of an increased chemical processing of organic compounds. Moreover, the model runs have shown noticeable differences in the pH values calculated with and without consideration of solution non-ideality. On average, the predicted pH values of the simulations considering solution non-ideality are −0.27 and −0.44 pH units lower under 90 and 70 % RH conditions, respectively. More comprehensive results of detailed SPACCIM-SpactMod studies on the multiphase processing in organic–inorganic mixtures of deliquesced particles are described in a companion paper.
- ItemNear-global aerosol mapping in the upper troposphere and lowermost stratosphere with data from the CARIBIC project(Milton Park : Taylor & Francis, 2017) Heintzenberg, Jost; Hermann, Markus; Weigelt, Andreas; Kapustin, Vladimir; Anderson, Bruce; Thornhill, Kenneth; Van Velthoven, Peter; Zahn, Andreas; Brenninkmeijer, CarlThis study extrapolates aerosol data of the CARIBIC project from 1997 until June 2008 in along trajectories to compose large-scale maps and vertical profiles of submicrometre particle concentrations in the upper troposphere and lowermost stratosphere (UT/LMS). The extrapolation was validated by comparing extrapolated values with CARIBIC data measured near the respective trajectory position and by comparing extrapolated CARIBIC data to measurements by other experiments near the respective trajectory positions. Best agreement between extrapolated and measured data is achieved with particle lifetimes longer than the maximum length of used trajectories. The derived maps reveal regions of strong and frequent new particle formation, namely the Tropical Central and Western Africa with the adjacent Atlantic, South America, the Caribbean and Southeast Asia. These regions of particle formation coincide with those of frequent deep convective clouds. Vertical particle concentration profiles for the troposphere and the stratosphere confirm statistically previous results indicating frequent new particle formation in the tropopause region. There was no statistically significant increase in Aitken mode particle concentration between the first period of CARIBIC operation, 1997–2002, and the second period, 2004–2009. However, a significant increase in concentration occurred within the latter period when considering it in isolation.
- ItemSubmicrometer aerosol particle distributions in the upper troposphere over the mid-latitude North Atlantic - Results from the third route of 'CARIBIC'(Milton Park : Taylor & Francis, 2017) Hermann, M.; Brenninkmeijer, C.A.M.; Slemr, F.; Heintzenberg, J.; Martinsson, B.G.; Schlager, H.; Van Velthoven, P.F.J.; Wiedensohler, A.; Zahn, A.; Ziereis, H.Particle number and mass concentrations of submicrometer aerosol particles were determined for the upper troposphere over the mid-latitude North Atlantic within the Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container project (CARIBIC, http://www.caribic-atmospheric.com). Between May 2001 and April 2002, 22 flights from Germany to the Caribbean were conducted using an automated measurement container on a B767 passenger aircraft. Spatial and seasonal probability distributions for ultrafine and Aitken mode particles as well as mass concentrations of particulate sulphur in 8–12 km altitude are presented. High particle number concentrations (mostly 2500–15 000 particles cm-3 STP) are particularly found in summer over the western North Atlantic Ocean close to the North American continent. The distributions together with an analysis of particle source processes show that deep vertical transport is the dominant process leading to most of the events with high particle number concentrations (8000 particles cm-3 STP) for ultrafine particles as well as for Aitken mode particles. This study emphasizes the importance of deep vertical transport and cloud processing for the concentration of aerosol particles in the upper troposphere.
- ItemThe HadGEM2-ES implementation of CMIP5 centennial simulations(Göttingen : Copernicus, 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.