Auflistung nach Autor:in "DeCarlo, Peter F."
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- PublikationA new method to discriminate secondary organic aerosols from different sources using high-resolution aerosol mass spectra(Copernicus, 2012) Heringa, Maarten F.; DeCarlo, Peter F.; Chirico, Roberto; Tritscher, Torsten; Clairotte, Michael; Mohr, Christine; Crippa, Monica; Slowik, Jay Gates; Pfaffenberger, Lisa; Dommen, Josef; Weingartner, Ernest; Prévôt, André; Baltensperger, Urs [in: Atmospheric Chemistry and Physics]Abstract. Organic aerosol (OA) represents a significant and often major fraction of the non-refractory PM1 (particulate matter with an aerodynamic diameter da < 1 μm) mass. Secondary organic aerosol (SOA) is an important contributor to the OA and can be formed from biogenic and anthropogenic precursors. Here we present results from the characterization of SOA produced from the emissions of three different anthropogenic sources. SOA from a log wood burner, a Euro 2 diesel car and a two-stroke Euro 2 scooter were characterized with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and compared to SOA from α-pinene. The emissions were sampled from the chimney/tailpipe by a heated inlet system and filtered before injection into a smog chamber. The gas phase emissions were irradiated by xenon arc lamps to initiate photo-chemistry which led to nucleation and subsequent particle growth by SOA production. Duplicate experiments were performed for each SOA type, with the averaged organic mass spectra showing Pearson's r values >0.94 for the correlations between the four different SOA types after five hours of aging. High-resolution mass spectra (HR-MS) showed that the dominant peaks in the MS, m/z 43 and 44, are dominated by the oxygenated ions C2H3O+ and CO2+, respectively, similarly to the relatively fresh semi-volatile oxygenated OA (SV-OOA) observed in the ambient aerosol. The atomic O:C ratios were found to be in the range of 0.25–0.55 with no major increase during the first five hours of aging. On average, the diesel SOA showed the lowest O:C ratio followed by SOA from wood burning, α-pinene and the scooter emissions. Grouping the fragment ions revealed that the SOA source with the highest O:C ratio had the largest fraction of small ions. The HR data of the four sources could be clustered and separated using principal component analysis (PCA). The model showed a significant separation of the four SOA types and clustering of the duplicate experiments on the first two principal components (PCs), which explained 79% of the total variance. Projection of ambient SV-OOA spectra resolved by positive matrix factorization (PMF) showed that this approach could be useful to identify large contributions of the tested SOA sources to SV-OOA. The first results from this study indicate that the SV-OOA in Barcelona is strongly influenced by diesel emissions in winter while in summer at SIRTA at the southwestern edge of Paris SV-OOA is more similar to alpha-pinene SOA. However, contributions to the ambient SV-OOA from SOA sources that are not covered by the model can cause major interference and therefore future expansions of the PCA model with additional SOA sources is recommended.01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationAerosol and trace gas vehicle emission factors measured in a tunnel using an Aerosol Mass Spectrometer and other on-line instrumentation(Elsevier, 04/2011) Chirico, Roberto; Prevot, Andre S.H.; DeCarlo, Peter F.; Heringa, Maarten F.; Richter, Rene; Weingartner, Ernest; Baltensperger, Urs [in: Atmospheric Environment]In this study we present measurements of gas and aerosol phase composition for a mixed vehicle fleet in the Gubrist tunnel (Switzerland) in June 2008. PM1 composition measurements were made with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (AMS) and a Multi Angle Absorption Photometer (MAAP). Gas-phase measurements of CO, CO2, NOx and total hydrocarbons (THC) were performed with standard instrumentation. Weekdays had a characteristic diurnal pattern with 2 peaks in concentrations for all traffic related species corresponding to high vehicle density (∼300 ± 30 vehicles per 5 min) in the morning rush hour between 06:00 and 09:00 and in the afternoon rush hours from approximately 15:30 to 18:30. The emission factors (EF) of OA were heavily influenced by the OA mass loading. To exclude this partitioning effect, only organic aerosol mass concentrations from 60 μg m−3 to 90 μg m−3 were considered and for these conditions the EF(OA) value for HDV was 33.7 ± 2.3 mg km−1 for a temperature inside the tunnel of 20–25 °C. This value is not directly applicable to ambient conditions because it is derived from OA mass concentrations that are roughly a factor of 10 higher than typical ambient concentrations. An even higher EF(OA)HDV value of 47.4 ± 1.6 mg km−1 was obtained when the linear fit was applied to all data points including OA concentrations up to 120 μg m−3. Similar to the increasing EF, the OA/BC ratio in the tunnel was also affected by the organic loading and it increased by a factor of ∼3 over the OA range 10–120 μg m−3. This means that also the OA emission factors at ambient concentrations of around 5–10 μg m−3 would be 2–3 times lower than the emission factor given above. For OA concentrations lower than 40 μg m−3 the OA/BC mass ratio was below 1, while at an OA concentration of 100–120 μg m−3 the OA/BC ratio was ∼1.5. The AMS mass spectra (MS) acquired in the tunnel were highly correlated with the primary organic aerosol (POA) MS from a EURO 3 diesel vehicle with a speed similar to the average tunnel speed.01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationChanges of hygroscopicity and morphology during ageing of diesel soot(Institute of Physics Publishing, 2011) Tritscher, Torsten; Jurányi, Zsófia; Martin, Maria; Chirico, Roberto; Gysel, Martin; Heringa, Maarten F.; DeCarlo, Peter F.; Sierau, Berko; Prévôt, André S. H.; Weingartner, Ernest; Baltensperger, Urs [in: Environmental Research Letters]01A - Beitrag in wissenschaftlicher Zeitschrift