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- ItemOrganic aerosol concentration and composition over Europe: Insights from comparison of regional model predictions with aerosol mass spectrometer factor analysis(München : European Geopyhsical Union, 2014) Fountoukis, C.; Megaritis, A.G.; Skyllakou, K.; Charalampidis, P.E.; Pilinis, C.; van der Gon, H.A.C. Denier; Crippa, M.; Canonaco, F.; Mohr, C.; Prévôt, A.S.H.; Allan, J.D.; Poulain, L.; Petäjä, T.; Tiitta, P.; Carbone, S.; Kiendler-Scharr, A.; Nemitz, E.; O'Dowd, C.; Swietlicki, E.; Pandis, S.N.A detailed three-dimensional regional chemical transport model (Particulate Matter Comprehensive Air Quality Model with Extensions, PMCAMx) was applied over Europe, focusing on the formation and chemical transformation of organic matter. Three periods representative of different seasons were simulated, corresponding to intensive field campaigns. An extensive set of AMS measurements was used to evaluate the model and, using factor-analysis results, gain more insight into the sources and transformations of organic aerosol (OA). Overall, the agreement between predictions and measurements for OA concentration is encouraging, with the model reproducing two-thirds of the data (daily average mass concentrations) within a factor of 2. Oxygenated OA (OOA) is predicted to contribute 93% to total OA during May, 87% during winter and 96% during autumn, with the rest consisting of fresh primary OA (POA). Predicted OOA concentrations compare well with the observed OOA values for all periods, with an average fractional error of 0.53 and a bias equal to −0.07 (mean error = 0.9 μg m−3, mean bias = −0.2 μg m−3). The model systematically underpredicts fresh POA at most sites during late spring and autumn (mean bias up to −0.8 μg m−3). Based on results from a source apportionment algorithm running in parallel with PMCAMx, most of the POA originates from biomass burning (fires and residential wood combustion), and therefore biomass burning OA is most likely underestimated in the emission inventory. The sensitivity of POA predictions to the corresponding emissions' volatility distribution is discussed. The model performs well at all sites when the Positive Matrix Factorization (PMF)-estimated low-volatility OOA is compared against the OA with saturation concentrations of the OA surrogate species C* ≤ 0.1 μg m−3 and semivolatile OOA against the OA with C* > 0.1 μg m−3.
- ItemSimulating ultrafine particle formation in Europe using a regional CTM: Contribution of primary emissions versus secondary formation to aerosol number concentrations(München : European Geopyhsical Union, 2012) Fountoukis, C.; Riipinen, I.; Denier van der Gon, H.A.C.; Charalampidis, P.E.; Pilinis, C.; Wiedensohler, A.; O'Dowd, C.; Putaud, J.P.; Moerman, M.; Pandis, S.N.A three-dimensional regional chemical transport model (CTM) with detailed aerosol microphysics, PMCAMx-UF, was applied to the European domain to simulate the contribution of direct emissions and secondary formation to total particle number concentrations during May 2008. PMCAMx-UF uses the Dynamic Model for Aerosol Nucleation and the Two-Moment Aerosol Sectional (TOMAS) algorithm to track both aerosol number and mass concentration using a sectional approach. The model predicts nucleation events that occur over scales of hundreds up to thousands of kilometers especially over the Balkans and Southeast Europe. The model predictions were compared against measurements from 7 sites across Europe. The model reproduces more than 70% of the hourly concentrations of particles larger than 10 nm (N10) within a factor of 2. About half of these particles are predicted to originate from nucleation in the lower troposphere. Regional nucleation is predicted to increase the total particle number concentration by approximately a factor of 3. For particles larger than 100 nm the effect varies from an increase of 20% in the eastern Mediterranean to a decrease of 20% in southern Spain and Portugal resulting in a small average increase of around 1% over the whole domain. Nucleation has a significant effect in the predicted N50 levels (up to a factor of 2 increase) mainly in areas where there are condensable vapors to grow the particles to larger sizes. A semi-empirical ternary sulfuric acid-ammonia-water parameterization performs better than the activation or the kinetic parameterizations in reproducing the observations. Reducing emissions of ammonia and sulfur dioxide affects certain parts of the number size distribution.
- ItemThree-dimensional evolution of Saharan dust transport towards Europe based on a 9-year EARLINET-optimized CALIPSO dataset(Katlenburg-Lindau : EGU, 2017) Marinou, Eleni; Amiridis, Vassilis; Binietoglou, Ioannis; Tsikerdekis, Athanasios; Solomos, Stavros; Proestakis, Emannouil; Konsta, Dimitra; Papagiannopoulos, Nikolaos; Tsekeri, Alexandra; Vlastou, Georgia; Zanis, Prodromos; Balis, Dimitrios; Wandinger, Ulla; Ansmann, AlbertIn this study we use a new dust product developed using CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation) observations and EARLINET (European Aerosol Research Lidar Network) measurements and methods to provide a 3-D multiyear analysis on the evolution of Saharan dust over North Africa and Europe. The product uses a CALIPSO L2 backscatter product corrected with a depolarization-based method to separate pure dust in external aerosol mixtures and a Saharan dust lidar ratio (LR) based on long-term EARLINET measurements to calculate the dust extinction profiles. The methodology is applied on a 9-year CALIPSO dataset (2007-2015) and the results are analyzed here to reveal for the first time the 3-D dust evolution and the seasonal patterns of dust over its transportation paths from the Sahara towards the Mediterranean and Continental Europe. During spring, the spatial distribution of dust shows a uniform pattern over the Sahara desert. The dust transport over the Mediterranean Sea results in mean dust optical depth (DOD) values up to 0.1. During summer, the dust activity is mostly shifted to the western part of the desert where mean DOD near the source is up to 0.6. Elevated dust plumes with mean extinction values between 10 and 75 Mm-1 are observed throughout the year at various heights between 2 and 6 km, extending up to latitudes of 40° N. Dust advection is identified even at latitudes of about 60° N, but this is due to rare events of episodic nature. Dust plumes of high DOD are also observed above the Balkans during the winter period and above northwest Europe during autumn at heights between 2 and 4 km, reaching mean extinction values up to 50 Mm-1. The dataset is considered unique with respect to its potential applications, including the evaluation of dust transport models and the estimation of cloud condensation nuclei (CCN) and ice nuclei (IN) concentration profiles. Finally, the product can be used to study dust dynamics during transportation, since it is capable of revealing even fine dynamical features such as the particle uplifting and deposition on European mountainous ridges such as the Alps and Carpathian Mountains.
- ItemSimulating the formation of carbonaceous aerosol in a European Megacity (Paris) during the MEGAPOLI summer and winter campaigns(München : European Geopyhsical Union, 2016) Fountoukis, Christos; Megaritis, Athanasios G.; Skyllakou, Ksakousti; Charalampidis, Panagiotis E.; van der Gon, Hugo A.C.Denier; Crippa, Monica; Prévôt, André S.H.; Fachinger, Friederike; Wiedensohler, Alfred; Pilinis, Christodoulos; Pandis, Spyros N.We use a three-dimensional regional chemical transport model (PMCAMx) with high grid resolution and high-resolution emissions (4 × 4 km2) over the Paris greater area to simulate the formation of carbonaceous aerosol during a summer (July 2009) and a winter (January/February 2010) period as part of the MEGAPOLI (megacities: emissions, urban, regional, and global atmospheric pollution and climate effects, and Integrated tools for assessment and mitigation) campaigns. Model predictions of carbonaceous aerosol are compared against Aerodyne aerosol mass spectrometer and black carbon (BC) high time resolution measurements from three ground sites. PMCAMx predicts BC concentrations reasonably well reproducing the majority (70 %) of the hourly data within a factor of two during both periods. The agreement for the summertime secondary organic aerosol (OA) concentrations is also encouraging (mean bias = 0.1 µg m−3) during a photochemically intense period. The model tends to underpredict the summertime primary OA concentrations in the Paris greater area (by approximately 0.8 µg m−3) mainly due to missing primary OA emissions from cooking activities. The total cooking emissions are estimated to be approximately 80 mg d−1 per capita and have a distinct diurnal profile in which 50 % of the daily cooking OA is emitted during lunch time (12:00–14:00 LT) and 20 % during dinner time (20:00–22:00 LT). Results also show a large underestimation of secondary OA in the Paris greater area during wintertime (mean bias = −2.3 µg m−3) pointing towards a secondary OA formation process during low photochemical activity periods that is not simulated in the model.
- ItemASAMgpu V1.0 - A moist fully compressible atmospheric model using graphics processing units (GPUs)(München : European Geopyhsical Union, 2012) Horn, S.In this work the three dimensional compressible moist atmospheric model ASAMgpu is presented. The calculations are done using graphics processing units (GPUs). To ensure platform independence OpenGL and GLSL are used, with that the model runs on any hardware supporting fragment shaders. The MPICH2 library enables interprocess communication allowing the usage of more than one GPU through domain decomposition. Time integration is done with an explicit three step Runge-Kutta scheme with a time-splitting algorithm for the acoustic waves. The results for four test cases are shown in this paper. A rising dry heat bubble, a cold bubble induced density flow, a rising moist heat bubble in a saturated environment, and a DYCOMS-II case.
- ItemEvaluation of long-range transport and deposition of desert dust with the CTM MOCAGE(Milton Park : Taylor & Francis, 2017) Martet, M.; Peuch, V-H.; Laurent, B.; Marticorena, B.; Bergametti, G.Desert dust modelling and forecasting attract growing interest, due to the numerous impacts of dusts on climate, numerical weather prediction, health, ecosystems, transportation, as well as on many industrial activities. The validation of numerical tools is a very important activity in this context, and we present here an example of such an effort, combining in situ (horizontal visibility in SYNOP messages, IMPROVE database) and remote-sensing data (satellite imagery, AERONET aerosol optical thickness data). Interestingly, these measurements are available routinely, and not only in the context of dedicated measurements campaign; thus, they can be used in an operational context to monitor the performances of operational forecasting systems. MOCAGE is the chemistry-transport model of Météo-France, used operationally to forecast the three-dimensional transport of dusts and their deposition. Two very long-range transport episodes of dust have been studied: one case of Saharan dust transported to East America through Asia and Pacific observed in November 2004 and one case of Saharan dust transported from West Africa to Caribbean Islands in May 2007. Episodes of geographical extension had seldom been studied, and they provide a very selective reference to compare the modelled desert dusts with. The representation of dusts in MOCAGE appears to be realistic in these two very different cases. In turn, the model simulations are used to make the link between the complementary information provided by the different measurements tools, providing a fully consistent picture of the entire episodes. The evolution of the aerosol size distribution during the episodes has also been studied. With no surprise, our study underlines that deposition processes are very sensitive to the size of dust particles. If the atmospheric cycle, in terms of mass, is very much under the influence of larger particles (some micrometres and above), only the finer particles actually travel over thousands of kilometres. This illustrates the need for an accurate representation of size distributions for this aerosol component in numerical models and advocates for using a size-resolved (bin) approach as sinks, and particularly, deposition do not affect the emitted log-normal distributions symmetrically on both sides of the median diameter. Overall, the results presented in this study provide an evaluation of Météo-France operational dust forecasting system MOCAGE.