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- ItemDiurnal variations of ambient particulate wood burning emissions and their contribution to the concentration of Polycyclic Aromatic Hydrocarbons (PAHs) in Seiffen, Germany(München : European Geopyhsical Union, 2011) Poulain, L.; Iinuma, Y.; Müller, K.; Birmili, W.; Weinhold, K.; Brüggemann, E.; Gnauk, T.; Hausmann, A.; Löschau, G.; Wiedensohler, A.; Herrmann, H.Residential wood burning is becoming an increasingly important cause of air quality problems since it has become a popular source of alternative energy to fossil fuel. In order to characterize the contribution of residential wood burning to local particle pollution, a field campaign was organized at the village of Seiffen (Saxony, Germany). During this campaign, an Aerosol Mass Spectrometer (AMS) was deployed in parallel to a PM1 high volume filter sampler. The AMS mass spectra were analyzed using Positive Matrix Factorization (PMF) to obtain detailed information about the organic aerosol (OA). Biomass-burning organic aerosol (BBOA), Hydrocarbon-like organic aerosol (HOA), and Oxygenated Organic Aerosol (OOA) were identified and represented 20%, 17% and 62% of total OA, respectively. Additionally, Polycyclic Aromatic Hydrocarbons (PAH) were measured by the AMS with an average concentration of 10 ng m−3 and short term events of extremely high PAH concentration (up to 500 ng m−3) compared to the mean PAH value were observed during the whole measurement period. A comparison with the results from PM1 filter samples showed that the BBOA factor and the AMS PAH are good indicators of the total concentration of the different monosaccharide anhydrides and PAH measured on the filter samples. Based on its low correlation with CO and the low car traffic, the HOA factor was considered to be related to residential heating using liquid fuel. An influence of the time of the week (week vs. weekend) on the diurnal profiles of the different OA components was observed. The weekdays were characterized by two maxima; a first one early in the morning and a stronger one in the evening. During the weekend days, the different OA components principally reached only one maximum in the afternoon. Finally, the PAH emitted directly from residential wood combustion was estimated to represent 1.5% of the total mass of the BBOA factor and around 62% of the total PAH concentration measured at Seiffen. This result highlights the important contribution of residential wood combustion to air quality and PAH emissions at the sampling place, which might have a significant impact on human health. Moreover, it also emphasizes the need for a better time resolution of the chemical characterization of toxic particulate compounds in order to provide more information on variations of the different sources through the days as well as to better estimate the real human exposure.
- ItemAtmospheric black carbon and warming effects influenced by the source and absorption enhancement in central Europe(München : European Geopyhsical Union, 2014) Nordmann, S.; Cheng, Y.F.; Carmichael, G.R.; Yu, M.; van der Gon, H.A.C.Denier; Zhang, Q.; Saide, P.E.; Pöschl, U.; Su, H.; Birmili, W.; Wiedensohler, A.Particles containing black carbon (BC), a strong absorbing substance, exert a rather uncertain direct and indirect radiative forcing in the atmosphere. To investigate the mass concentration and absorption properties of BC particles over central Europe, the model WRF-Chem was used at a resolution of 12 km in conjunction with a high-resolution BC emission inventory (EUCAARI 42-Pan-European Carbonaceous Aerosol Inventory; 1/8° × 1/16°). The model simulation was evaluated using measurements of equivalent soot carbon, absorption coefficients and particle number concentrations at seven sites within the German Ultrafine Aerosol Network, PM mass concentrations from the dense measurement network of the German Federal Environmental Agency at 392 monitoring stations, and aerosol optical depth from MODIS and AERONET. A distinct time period (25 March to 10 April 2009) was chosen, during which the clean marine air mass prevailed in the first week and afterwards the polluted continental air mass mainly from the southeast dominated with elevated daily average BC concentration of up to 4 μ g m−3. The simulated PM mass concentration, aerosol number concentration and optical depth were in good agreement with the observations, while the modelled BC mass concentrations were found to be a factor of 2 lower than the observations. Together with back trajectories, detailed model bias analyses suggested that the current BC emission in countries to the east and south of Germany might be underestimated by a factor of 5, at least for the simulation period. Running the model with upscaled BC emissions in these regions led to a smaller model bias and a better correlation between model and measurement. In contrast, the particle absorption coefficient was positively biased by about 20% even when the BC mass concentration was underestimated by around 50%. This indicates that the internal mixture treatment of BC in the WRF-Chem optical calculation is unrealistic in our case, which overamplifies the light absorption by BC-containing particles. By adjusting the modelled mass absorption cross-section towards the measured values, the simulation of particle light absorption of BC was improved as well. Finally, the positive direct radiative forcing of BC particles at the top of the atmosphere was estimated to be in the range of 0 to +4 W m−2 over Germany for the model run with improved BC mass concentration and adjusted BC light absorption cross-section. This adjustment lowered the positive forcing of BC by up to 70%, compared with the internal mixing treatment of BC in the model simulation.
- 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.