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- ItemComplex refractive indices of Saharan dust samples at visible and near UV wavelengths: A laboratory study(München : European Geopyhsical Union, 2012) Wagner, R.; Ajtai, T.; Kandler, K.; Lieke, K.; Linke, C.; Müller, T.; Schnaiter, M.; Vragel, M.We have retrieved the wavelength-dependent imaginary parts of the complex refractive index for five different Saharan dust aerosol particles of variable mineralogical composition at wavelengths between 305 and 955 nm. The dust particles were generated by dispersing soil samples into a laboratory aerosol chamber, typically yielding particle sizes with mean diameters ranging from 0.3 to 0.4 μm and maximum diameters from 2 to 4 μm. The extinction and absorption coefficients as well as the number size distribution of the dust particles were simultaneously measured by various established techniques. An inversion scheme based on a spheroidal dust model was employed to deduce the refractive indices. The retrieved imaginary parts of the complex refractive index were in the range from 0.003 to 0.005, 0.005 to 0.011, and 0.016 to 0.050 at the wavelengths 955, 505, and 305 nm. The hematite content of the dust particles was determined by electron-microscopical single particle analysis. Hematite volume fractions in the range from 1.1 to 2.7% were found for the different dusts, a range typical for atmospheric mineral dust. We have performed a sensitivity study to assess how accurately the retrieved imaginary refractive indices could be reproduced by calculations with mixing rule approximations using the experimentally determined hematite contents as input.
- ItemNumerical simulations of mixing conditions and aerosol dynamics in the CERN CLOUD chamber(München : European Geopyhsical Union, 2012) Voigtländer, J.; Duplissy, J.; Rondo, L.; Kürten, A.; Stratmann, F.To study the effect of galactic cosmic rays on aerosols and clouds, the Cosmics Leaving OUtdoor Droplets (CLOUD) project was established. Experiments are carried out at a 26.1 m3 tank at CERN (Switzerland). In the experiments, the effect of ionizing radiation on H2SO4 particle formation and growth is investigated. To evaluate the experimental configuration, the experiment was simulated using a coupled multidimensional computational fluid dynamics (CFD) – particle model. In the model the coupled fields of gas/vapor species, temperature, flow velocity and particle properties were computed to investigate mixing state and mixing times of the CLOUD tank's contents. Simulation results show that a 1-fan configuration, as used in first experiments, may not be sufficient to ensure a homogeneously mixed chamber. To mix the tank properly, two fans and sufficiently high fan speeds are necessary. The 1/e response times for instantaneous changes of wall temperature and saturation ratio were found to be in the order of few minutes. Particle nucleation and growth was also simulated and particle number size distribution properties of the freshly nucleated particles (particle number, mean size, standard deviation of the assumed log-normal distribution) were found to be distributed over the tank's volume similar to the gas species.
- ItemColumnar modelling of nucleation burst evolution in the convective boundary layer - First results from a feasibility study, Part I: Modelling approach(München : European Geopyhsical Union, 2006) Hellmuth, O.A high-order modelling approach to interpret "continental-type" particle formation bursts in the anthropogenically influenced convective boundary layer (CBL) is proposed. The model considers third-order closure for planetary boundary layer turbulence, sulphur and ammonia chemistry as well as aerosol dynamics. In Paper I of four papers, previous observations of ultrafine particle evolution are reviewed, model equations are derived, the model setup for a conceptual study on binary and ternary homogeneous nucleation is defined and shortcomings of process parameterisation are discussed. In the subsequent Papers II, III and IV simulation results, obtained within the framework of a conceptual study on the CBL evolution and new particle formation (NPF), will be presented and compared with observational findings.
- ItemA parameterization of the heterogeneous hydrolysis of N2O5 for mass-based aerosol models: Improvement of particulate nitrate prediction(Katlenburg-Lindau : EGU, 2018) Chen, Ying; Wolke, Ralf; Ran, Liang; Birmili, Wolfram; Spindler, Gerald; Schröder, Wolfram; Su, Hang; Cheng, Yafang; Tegen, Ina; Wiedensohler, AlfredThe heterogeneous hydrolysis of N2O5 on the surface of deliquescent aerosol leads to HNO3 formation and acts as a major sink of NOx in the atmosphere during night-time. The reaction constant of this heterogeneous hydrolysis is determined by temperature (T), relative humidity (RH), aerosol particle composition, and the surface area concentration (S). However, these parameters were not comprehensively considered in the parameterization of the heterogeneous hydrolysis of N2O5 in previous mass-based 3-D aerosol modelling studies. In this investigation, we propose a sophisticated parameterization (NewN2O5) of N2O5 heterogeneous hydrolysis with respect to T, RH, aerosol particle compositions, and S based on laboratory experiments. We evaluated closure between NewN2O5 and a state-of-the-art parameterization based on a sectional aerosol treatment. The comparison showed a good linear relationship (R Combining double low line 0.91) between these two parameterizations. NewN2O5 was incorporated into a 3-D fully online coupled model, COSMO-Muscat, with the mass-based aerosol treatment. As a case study, we used the data from the HOPE Melpitz campaign (10-25 September 2013) to validate model performance. Here, we investigated the improvement of nitrate prediction over western and central Europe. The modelled particulate nitrate mass concentrations ([NO3-]) were validated by filter measurements over Germany (Neuglobsow, Schmücke, Zingst, and Melpitz). The modelled [NO3-] was significantly overestimated for this period by a factor of 5-19, with the corrected NH3 emissions (reduced by 50 %) and the original parameterization of N2O5 heterogeneous hydrolysis. The NewN2O5 significantly reduces the overestimation of [NO3-] by ∼ 35 %. Particularly, the overestimation factor was reduced to approximately 1.4 in our case study (12, 17-18 and 25 September 2013) when [NO3-] was dominated by local chemical formations. In our case, the suppression of organic coating was negligible over western and central Europe, with an influence on [NO3-] of less than 2 % on average and 20 % at the most significant moment. To obtain a significant impact of the organic coating effect, N2O5, SOA, and NH3 need to be present when RH is high and T is low. However, those conditions were rarely fulfilled simultaneously over western and central Europe. Hence, the organic coating effect on the reaction probability of N2O5 may not be as significant as expected over western and central Europe.
- 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.
- 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.
- ItemEvaluation of a three-dimensional chemical transport model (PMCAMx) in the European domain during the EUCAARI May 2008 campaign(München : European Geopyhsical Union, 2011) Fountoukis, C.; Racherla, P.N.; Denier van der Gon, H.A.C.; Polymeneas, P.; Charalampidis, P.E.; Pilinis, C.; Wiedensohler, A.; Dall'Osto, M.; O'Dowd, C.; Pandis, S.N.Sea salt aerosol can significantly affect the air quality. Sea salt can cause enhanced concentrations of particulate matter and change particle chemical composition, in particular in coastal areas, and therefore should be accounted for in air quality modelling. We have used an EMEP Unified model to calculate sea salt concentrations and depositions over Europe, focusing on studying the effects of uncertainties in sea salt production and lifetime on calculation results. Model calculations of sea salt have been compared with EMEP observations of sodium concentrations in air and precipitation for a four year period, from 2004 to 2007, including size (fine/coarse) resolved EMEP intensive measurements in 2006 and 2007. In the presented calculations, sodium air concentrations are between 8% and 46% overestimated, whereas concentrations in precipitation are systematically underestimated by 65–70% for years 2004–2007. A series of model tests have been performed to investigate the reasons for this underestimation, but further studies are needed. The model is found to reproduce the spatial distribution of Na+ in air and precipitation over Europe fairly well, and to capture most of sea salt episodes. The paper presents the main findings from a series of tests in which we compare several different sea spray source functions and also look at the effects of meteorological input and the efficiency of removal processes on calculated sea salt concentrations. Finally, sea salt calculations with the EMEP model have been compared with results from the SILAM model and observations for 2007. While the models produce quite close results for Na+ at the majority of 26 measurement sites, discrepancies in terms of bias and temporal correlation are also found. Those differences are believed to occur due to differences in the representation of source function and size distribution of sea salt aerosol, different meteorology used for model runs and the different models' resolution. This study contributes to getting a better insight on uncertainties associated with sea salt calculations and thus facilitates further improvement of aerosol modelling on both regional and global scales.
- ItemAtmospheric dust modeling from meso to global scales with the online NMMB/BSC-Dust model – Part 2: Experimental campaigns in Northern Africa(München : European Geopyhsical Union, 2012) Haustein, K.; Pérez, C.; Baldasano, J.M.; Jorba, O.; Basart, S.; Miller, R.L.; Janjic, Z.; Black, T.; Nickovic, S.; Todd, M.C.; Washington, R.; Müller, D.; Tesche, M.; Weinzierl, B.; Esselborn, M.; Schladitz, A.The new NMMB/BSC-Dust model is intended to provide short to medium-range weather and dust forecasts from regional to global scales. It is an online model in which the dust aerosol dynamics and physics are solved at each model time step. The companion paper (Pérez et al., 2011) develops the dust model parameterizations and provides daily to annual evaluations of the model for its global and regional configurations. Modeled aerosol optical depth (AOD) was evaluated against AERONET Sun photometers over Northern Africa, Middle East and Europe with correlations around 0.6–0.7 on average without dust data assimilation. In this paper we analyze in detail the behavior of the model using data from the Saharan Mineral dUst experiment (SAMUM-1) in 2006 and the Bodélé Dust Experiment (BoDEx) in 2005. AOD from satellites and Sun photometers, vertically resolved extinction coefficients from lidars and particle size distributions at the ground and in the troposphere are used, complemented by wind profile data and surface meteorological measurements. All simulations were performed at the regional scale for the Northern African domain at the expected operational horizontal resolution of 25 km. Model results for SAMUM-1 generally show good agreement with satellite data over the most active Saharan dust sources. The model reproduces the AOD from Sun photometers close to sources and after long-range transport, and the dust size spectra at different height levels. At this resolution, the model is not able to reproduce a large haboob that occurred during the campaign. Some deficiencies are found concerning the vertical dust distribution related to the representation of the mixing height in the atmospheric part of the model. For the BoDEx episode, we found the diurnal temperature cycle to be strongly dependant on the soil moisture, which is underestimated in the NCEP analysis used for model initialization. The low level jet (LLJ) and the dust AOD over the Bodélé are well reproduced. The remaining negative AOD bias (due to underestimated surface wind speeds) can be substantially reduced by decreasing the threshold friction velocity in the model.
- ItemNumerical simulations of optical properties of Saharan dust aerosols with emphasis on lidar applications(Milton Park : Taylor & Francis, 2017) Wiegner, M.; Gasteiger, J.; Kandler, K.; Weinzierl, B.; Rasp, K.; Esselborn, M.; Freudenthaler, V.; Heese, B.; Toledano, C.; Tesche, M.; Althausen, D.In the framework of the Saharan Mineral Dust Experiment (SAMUM) for the first time the spectral dependence of particle linear depolarization ratios was measured by combining four lidar systems. In this paper these measurements are compared with results from scattering theory based on the T-matrix method. For this purpose, in situ measurements—size distribution, shape distribution and refractive index—were used as input parameters; particle shape was approximated by spheroids. A sensitivity study showed that lidar-related parameters—lidar ratio Sp and linear depolarization ratio δp—are very sensitive to changes of all parameters. The simulated values of the δp are in the range of 20% and 31% and thus in the range of the measurements. The spectral dependence is weak, so that it could not be resolved by the measurements. Calculated lidar ratios based on the measured microphysics and considering equivalent radii up to 7.5μm show a range of possible values between 29 and 50 sr at λ = 532 nm. Larger Sp might be possible if the real part of the refractive index is small and the imaginary part is large. A strict validation was however not possible as too many microphysical parameters influence Sp and δp that could not be measured with the required accuracy.
- ItemStatus and future of numerical atmospheric aerosol prediction with a focus on data requirements(Katlenburg-Lindau : EGU, 2018) Benedetti, Angela; Reid, Jeffrey S.; Knippertz, Peter; Marsham, John H.; Di Giuseppe, Francesca; Rémy, Samuel; Basart, Sara; Boucher, Olivier; Brooks, Ian M.; Menut, Laurent; Mona, Lucia; Laj, Paolo; Pappalardo, Gelsomina; Wiedensohler, Alfred; Baklanov, Alexander; Brooks, Malcolm; Colarco, Peter R.; Cuevas, Emilio; da Silva, Arlindo; Escribano, Jeronimo; Flemming, Johannes; Huneeus, Nicolas; Jorba, Oriol; Kazadzis, Stelios; Kinne, Stefan; Popp, Thomas; Quinn, Patricia K.; Sekiyama, Thomas T.; Tanaka, Taichu; Terradellas, EnricNumerical prediction of aerosol particle properties has become an important activity at many research and operational weather centers. This development is due to growing interest from a diverse set of stakeholders, such as air quality regulatory bodies, aviation and military authorities, solar energy plant managers, climate services providers, and health professionals. Owing to the complexity of atmospheric aerosol processes and their sensitivity to the underlying meteorological conditions, the prediction of aerosol particle concentrations and properties in the numerical weather prediction (NWP) framework faces a number of challenges. The modeling of numerous aerosol-related parameters increases computational expense. Errors in aerosol prediction concern all processes involved in the aerosol life cycle including (a) errors on the source terms (for both anthropogenic and natural emissions), (b) errors directly dependent on the meteorology (e.g., mixing, transport, scavenging by precipitation), and (c) errors related to aerosol chemistry (e.g., nucleation, gas-aerosol partitioning, chemical transformation and growth, hygroscopicity). Finally, there are fundamental uncertainties and significant processing overhead in the diverse observations used for verification and assimilation within these systems. Indeed, a significant component of aerosol forecast development consists in streamlining aerosol-related observations and reducing the most important errors through model development and data assimilation. Aerosol particle observations from satellite- and ground-based platforms have been crucial to guide model development of the recent years and have been made more readily available for model evaluation and assimilation. However, for the sustainability of the aerosol particle prediction activities around the globe, it is crucial that quality aerosol observations continue to be made available from different platforms (space, near surface, and aircraft) and freely shared. This paper reviews current requirements for aerosol observations in the context of the operational activities carried out at various global and regional centers. While some of the requirements are equally applicable to aerosol-climate, the focus here is on global operational prediction of aerosol properties such as mass concentrations and optical parameters. It is also recognized that the term "requirements" is loosely used here given the diversity in global aerosol observing systems and that utilized data are typically not from operational sources. Most operational models are based on bulk schemes that do not predict the size distribution of the aerosol particles. Others are based on a mix of "bin" and bulk schemes with limited capability of simulating the size information. However the next generation of aerosol operational models will output both mass and number density concentration to provide a more complete description of the aerosol population. A brief overview of the state of the art is provided with an introduction on the importance of aerosol prediction activities. The criteria on which the requirements for aerosol observations are based are also outlined. Assimilation and evaluation aspects are discussed from the perspective of the user requirements.