Browsing by Author "Pandis, Spyros N."
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- 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.
- ItemSimulation of atmospheric organic aerosol using its volatility-oxygen-content distribution during the PEGASOS 2012 campaign(Katlenburg-Lindau : EGU, 2018) Karnezi, Eleni; Murphy, Benjamin N.; Poulain, Laurent; Herrmann, Hartmut; Wiedensohler, Alfred; Rubach, Florian; Kiendler-Scharr, Astrid; Mentel, Thomas F.; Pandis, Spyros N.A lot of effort has been made to understand and constrain the atmospheric aging of the organic aerosol (OA). Different parameterizations of the organic aerosol formation and evolution in the two-dimensional volatility basis set (2D-VBS) framework are evaluated using ground and airborne measurements collected in the 2012 Pan-European Gas AeroSOls-climate interaction Study (PEGASOS) field campaign in the Po Valley (Italy). A number of chemical aging schemes are examined, taking into account various functionalization and fragmentation pathways for biogenic and anthropogenic OA components. Model predictions and measurements, both at the ground and aloft, indicate a relatively oxidized OA with little average diurnal variation. Total OA concentration and O: C ratios are reproduced within experimental error by a number of chemical aging schemes. Anthropogenic secondary OA (SOA) is predicted to contribute 15-25% of the total OA, while SOA from intermediate volatility compound oxidation contributes another 20-35%. Biogenic SOA (bSOA) contributions varied from 15 to 45% depending on the modeling scheme. Primary OA contributed around 5% for all schemes and was comparable to the hydrocarbon-like OA (HOA) concentrations derived from the positive matrix factorization of the aerosol mass spectrometer (PMF-AMS) ground measurements. The average OA and O: C diurnal variation and their vertical profiles showed a surprisingly modest sensitivity to the assumed vaporization enthalpy for all aging schemes. This can be explained by the interplay between the partitioning of the semi-volatile compounds and their gas-phase chemical aging reactions.