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- ItemHygroscopic properties of the Paris urban aerosol in relation to its chemical composition(München : European Geopyhsical Union, 2014) Kamilli, K.A.; Poulain, L.; Held, A.; Nowak, A.; Birmili, W.; Wiedensohler, A.Aerosol hygroscopic growth factors and chemical properties were measured as part of the MEGAPOLI "Megacities Plume Case Study" at the urban site Laboratoire d'Hygiène de la Ville de Paris (LHVP) in the city center of Paris from June to August 2009, and from January to February 2010. Descriptive hygroscopic growth factors (DGF) were derived in the diameter range from 25 to 350 nm at relative humidities of 30, 55, 75, and 90% by applying the summation method on humidified and dry aerosol size distributions measured simultaneously with a humidified differential mobility particle sizer (HDMPS) and a twin differential mobility particle sizer (TDMPS). For 90% relative humidity, the DGF varied from 1.06 to 1.46 in summer, and from 1.06 to 1.66 in winter. Temporal variations in the observed mean DGF could be well explained with a simple growth model based on the aerosol chemical composition measured by aerosol mass spectrometry (AMS) and black carbon photometry (MAAP). In particular, good agreement was observed when sulfate was the predominant inorganic factor. A clear overestimation of the predicted growth factor was found when the nitrate mass concentration exceeded values of 10 μg m−3, e.g., during winter.
- ItemACTRIS ACSM intercomparison - Part 1: Reproducibility of concentration and fragment results from 13 individual Quadrupole Aerosol Chemical Speciation Monitors (Q-ACSM) and consistency with co-located instruments(München : European Geopyhsical Union, 2015) Crenn, V.; Sciare, J.; Croteau, P.L.; Verlhac, S.; Fröhlich, R.; Belis, C.A.; Aas, W.; Äijälä, M.; Alastuey, A.; Artiñano, B.; Baisnée, D.; Bonnaire, N.; Bressi, M.; Canagaratna, M.; Canonaco, F.; Carbone, C.; Cavalli, F.; Coz, E.; Cubison, M.J.; Esser-Gietl, J.K.; Green, D.C.; Gros, V.; Heikkinen, L.; Herrmann, H.; Lunder, C.; Minguillón, M.C.; Močnik, G.; O'Dowd, C.D.; Ovadnevaite, J.; Petit, J.-E.; Petralia, E.; Poulain, L.; Priestman, M.; Riffault, V.; Ripoll, A.; Sarda-Estève, R.; Slowik, J.G.; Setyan, A.; Wiedensohler, A.; Baltensperger, U.; Prévôt, A.S.H.; Jayne, J.T.; Favez, O.As part of the European ACTRIS project, the first large Quadrupole Aerosol Chemical Speciation Monitor (Q-ACSM) intercomparison study was conducted in the region of Paris for 3 weeks during the late-fall – early-winter period (November–December 2013). The first week was dedicated to the tuning and calibration of each instrument, whereas the second and third were dedicated to side-by-side comparison in ambient conditions with co-located instruments providing independent information on submicron aerosol optical, physical, and chemical properties. Near real-time measurements of the major chemical species (organic matter, sulfate, nitrate, ammonium, and chloride) in the non-refractory submicron aerosols (NR-PM1) were obtained here from 13 Q-ACSM. The results show that these instruments can produce highly comparable and robust measurements of the NR-PM1 total mass and its major components. Taking the median of the 13 Q-ACSM as a reference for this study, strong correlations (r2 > 0.9) were observed systematically for each individual Q-ACSM across all chemical families except for chloride for which three Q-ACSMs showing weak correlations partly due to the very low concentrations during the study. Reproducibility expanded uncertainties of Q-ACSM concentration measurements were determined using appropriate methodologies defined by the International Standard Organization (ISO 17025, 1999) and were found to be 9, 15, 19, 28, and 36 % for NR-PM1, nitrate, organic matter, sulfate, and ammonium, respectively. However, discrepancies were observed in the relative concentrations of the constituent mass fragments for each chemical component. In particular, significant differences were observed for the organic fragment at mass-to-charge ratio 44, which is a key parameter describing the oxidation state of organic aerosol. Following this first major intercomparison exercise of a large number of Q-ACSMs, detailed intercomparison results are presented, along with a discussion of some recommendations about best calibration practices, standardized data processing, and data treatment.
- ItemSingle particle diversity and mixing state measurements(München : European Geopyhsical Union, 2014) Healy, R.M.; Riemer, N.; Wenger, J.C.; Murphy, M.; West, M.; Poulain, L.; Wiedensohler, A.; O'Connor, I.P.; McGillicuddy, E.; Sodeau, J.R.; Evans, G.J.A newly developed framework for quantifying aerosol particle diversity and mixing state based on information-theoretic entropy is applied for the first time to single particle mass spectrometry field data. Single particle mass fraction estimates for black carbon, organic aerosol, ammonium, nitrate and sulfate, derived using single particle mass spectrometer, aerosol mass spectrometer and multi-angle absorption photometer measurements are used to calculate single particle species diversity (Di). The average single particle species diversity (Dα) is then related to the species diversity of the bulk population (Dγ) to derive a mixing state index value (χ) at hourly resolution. The mixing state index is a single parameter representation of how internally/externally mixed a particle population is at a given time. The index describes a continuum, with values of 0 and 100% representing fully external and internal mixing, respectively. This framework was applied to data collected as part of the MEGAPOLI winter campaign in Paris, France, 2010. Di values are low (~ 2) for fresh traffic and wood-burning particles that contain high mass fractions of black carbon and organic aerosol but low mass fractions of inorganic ions. Conversely, Di values are higher (~ 4) for aged carbonaceous particles containing similar mass fractions of black carbon, organic aerosol, ammonium, nitrate and sulfate. Aerosol in Paris is estimated to be 59% internally mixed in the size range 150–1067 nm, and mixing state is dependent both upon time of day and air mass origin. Daytime primary emissions associated with vehicular traffic and wood-burning result in low χ values, while enhanced condensation of ammonium nitrate on existing particles at night leads to higher χ values. Advection of particles from continental Europe containing ammonium, nitrate and sulfate leads to increases in Dα, Dγ and χ. The mixing state index represents a useful metric by which to compare and contrast ambient particle mixing state at other locations globally.
- ItemWintertime aerosol chemical composition and source apportionment of the organic fraction in the metropolitan area of Paris(München : European Geopyhsical Union, 2013) Crippa, M.; DeCarlo, P.F.; Slowik, J.G.; Mohr, C.; Heringa, M.F.; Chirico, R.; Poulain, L.; Freutel, F.; Sciare, J.; Cozic, J.; Di Marco, C.F.; Elsasser, M.; Nicolas, B.; Marchand, N.; Abidi, E.; Wiedensohler, A.; Drewnick, F.; Schneider, J.; Borrmann, S.; Nemitz, E.; Zimmermann, R.; Jaffrezo, J.-L.; Prévôt, A.S.H.; Baltensperger, U.The effect of a post-industrial megacity on local and regional air quality was assessed via a month-long field measurement campaign in the Paris metropolitan area during winter 2010. Here we present source apportionment results from three aerosol mass spectrometers and two aethalometers deployed at three measurement stations within the Paris region. Submicron aerosol composition is dominated by the organic fraction (30–36%) and nitrate (28–29%), with lower contributions from sulfate (14–16%), ammonium (12–14%) and black carbon (7–13%). Organic source apportionment was performed using positive matrix factorization, resulting in a set of organic factors corresponding both to primary emission sources and secondary production. The dominant primary sources are traffic (11–15% of organic mass), biomass burning (13–15%) and cooking (up to 35% during meal hours). Secondary organic aerosol contributes more than 50% to the total organic mass and includes a highly oxidized factor from indeterminate and/or diverse sources and a less oxidized factor related to wood burning emissions. Black carbon was apportioned to traffic and wood burning sources using a model based on wavelength-dependent light absorption of these two combustion sources. The time series of organic and black carbon factors from related sources were strongly correlated. The similarities in aerosol composition, total mass and temporal variation between the three sites suggest that particulate pollution in Paris is dominated by regional factors, and that the emissions from Paris itself have a relatively low impact on its surroundings.