J. P. Putaud

European Commission - Joint Research Centre, Bruxelles, Brussels Capital Region, Italy

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Publications (97)206 Total impact

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    ABSTRACT: This paper analyses elemental (EC), organic (OC) and total carbon (TC) concentration in PM2.5 and PM10 samples collected over the last few years within several national and European projects at 37 remote, rural, urban, and traffic sites across the Italian peninsula. The purpose of the study is to obtain a picture of the spatial and seasonal variability of these aerosol species in Italy, and an insight into sources, processes and effects of meteorological conditions. OC and EC showed winter maxima and summer minima at urban and rural locations and an opposite behaviour at remote high altitude sites, where they increase during the warm period due to the rising of the Planetary Boundary Layer (PBL). The seasonal averages of OC are higher during winter compared to summer at the rural sites in the Po Valley (from 1.4 to 3.5 times), opposite to what usually occurs at rural locations, where OC increases during the warm period. This denotes the marked influence of urban areas on the surrounding rural environment in this densely populated region. The different types of sites exhibit marked differences in the average concentrations of carbonaceous aerosol and OC/EC ratio. This ratio is less sensitive to atmospheric processing than OC and EC concentrations, and hence more representative of different source types. Remote locations are characterised by the lowest levels of OC and especially EC, with OC/EC ratios ranging from 13 to 20, while the maximum OC and EC concentrations are observed at road-traffic influenced urban sites, where the OC/EC ratio ranges between 1 and 3. The highest urban impacts of OC and EC relative to remote and rural background sites occur in the Po Valley, especially in the city of Milan, which has the highest concentrations of PM and TC and low values of the OC/EC ratio.
    Atmospheric Environment 10/2014; 99:587-598. · 3.11 Impact Factor
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    ABSTRACT: Along with some research networking programmes, the European Directive 2008/50/CE requires chemical speciation of fine aerosol (PM2.5), including elemental (EC) and organic carbon (OC), at a few rural sites in European countries. Meanwhile, the thermal-optical technique is considered by the European and US networking agencies and normalisation bodies as a reference method to quantify EC–OC collected on filters. Although commonly used for many years, this technique still suffers from a lack of information on the comparability of the different analytical protocols (temperature protocols, type of optical correction) currently applied in the laboratories. To better evaluate the EC–OC data set quality and related uncertainties, the French National Reference Laboratory for Ambient Air Quality Monitoring (LCSQA) organised an EC–OC comparison exercise for French laboratories using different thermaloptical methods (five laboratories only). While there is good agreement on total carbon (TC) measurements among all participants, some differences can be observed on the EC / TC ratio, even among laboratories using the same thermal protocol. These results led to further tests on the influence of the optical correction: results obtained from different European laboratories confirmed that there were higher differences between OCTOT and OCTOR measured with NIOSH 5040 in comparison to EUSAAR-2. Also, striking differences between ECTOT / ECTOR ratios can be observed when comparing results obtained for rural and urban samples, with ECTOT being 50% lower than ECTOR at rural sites whereas it is only 20% lower at urban sites. The PM chemical composition could explain these differences but the way it influences the EC–OC measurement is not clear and needs further investigation. Meanwhile, some additional tests seem to indicate an influence of oven soiling on the EC–OC measurement data quality. This highlights the necessity to follow the laser signal decrease with time and its impact on measurements. Nevertheless, this should be confirmed by further experiments, involving more samples and various instruments, to enable statistical processing. All these results provide insights to determine the quality of EC–OC analytical methods and may contribute to the work toward establishing method standardisation.
    Atmospheric Measurement Techniques 06/2014; 7:1649-1661. · 3.21 Impact Factor
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    ABSTRACT: Cluster analysis of particle number size distributions from background sites across Europe is presented. This generated a total of nine clusters of particle size distributions which could be further combined into two main groups, namely: a south-to-north category (four clusters) and a west-to-east category (five clusters). The first group was identified as most frequently being detected inside and around northern Germany and neighbouring countries, showing clear evidence of local afternoon nucleation and growth events that could be linked to movement of air masses from south to north arriving ultimately at the Arctic contributing to Arctic haze. The second group of particle size spectra proved to have narrower size distributions and collectively showed a dependence of modal diameter upon the longitude of the site (west to east) at which they were most frequently detected. These clusters indicated regional nucleation (at the coastal sites) growing to larger modes further inland. The apparent growth rate of the modal diameter was around 0.6–0.9 nm* h^(−1) . Four specific air mass back-trajectories were successively taken as case studies to examine in real time the evolution of aerosol size distributions across Europe. While aerosol growth processes can be observed as aerosol traverses Europe, the processes are often obscured by the addition of aerosol by emissions en route. This study revealed that some of the 24 stations exhibit more complex behaviour than others, especially when impacted by local sources or a variety of different air masses. Overall, the aerosol size distribution clustering analysis greatly simplifies the complex data set and allows a description of aerosol aging processes, which reflects the longer-term average development of particle number size distributions as air masses advect across Europe.
    ATMOSPHERIC CHEMISTRY AND PHYSICS 04/2014; Atmos. Chem. Phys., 14, 4327-4348, 2014(14):4327-4348. · 5.51 Impact Factor
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    ABSTRACT: Aerosols properties have been monitored by ground-based in situ and remote sensing measurements at the station for atmospheric research located in Ispra on the edge of the Po Valley for almost one decade. In-situ measurements are performed according to Global Atmosphere Watch recommendations, and quality is assured through the participation in regular inter-laboratory comparisons. Sunphotometer data are produced by AERONET. Data show significant decreasing trends over 2004-2010 for a number of variables including particulate matter (PM) mass concentration, aerosol scattering, backscattering and absorption coefficients, and aerosol optical thickness (AOT). In-situ measurement data show no significant trend in the aerosol backscatter ratio, but a significant decreasing trend of about -0.7 ± 0.3% in the aerosol single scattering albedo in the visible light range. Similar trends are observed in the aerosol single scattering albedo retrieved from sunphotometer measurements. Correlations appear between in situ PM mass concentration and aerosol scattering coefficient on the one hand, and elemental carbon (EC) and aerosol absorption coefficient on the other hand, however, no increase in the EC / PM ratio was observed, which could have explained the decrease in SSA. The application of a simple approximation to calculate the direct radiative forcing by aerosols suggests a significant diminution in their cooling effect, mainly due to the decrease in AOT. Applying the methodology we present to those sites where the necessary suite of measurements is available would provide important information to inform future policies for air quality enhancement and fast climate change mitigation.
    Atmospheric Chemistry and Physics 03/2014; 14(7). · 5.51 Impact Factor
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    ABSTRACT: Along with some research networking programs, the European Directive 2008/50/CE requires chemical speciation of fine aerosol (PM2.5), including elemental (EC) and organic carbon (OC), at a few rural sites in European countries. Meanwhile, the thermal-optical technique is considered by the European and US networking agencies and normalization bodies as a reference method to quantify EC-OC collected on filters. Although commonly used for many years, this technique is still suffering from a lack of information on the comparability of the different analytical protocols (temperature protocols, type of optical correction) currently applied in the laboratories. To better evaluate the EC-OC data set quality and related uncertainties, the French National Reference Laboratory for Ambient Air Quality Monitoring (LCSQA) has organized an EC-OC comparison exercise for French laboratories using different thermal-optical methods. While there is good agreement on total carbon (TC) measurements among all participants, some discrepancies can be observed on the EC/TC ratio, even among laboratories using the same thermal protocol. These results led to further tests on the influence of the optical correction: results obtained from different European Laboratories, confirming that there are higher differences between OCTOT and OCTOR measured with NIOSH 5040 in comparison to EUSAAR-2. Also, striking differences between ECTOT/ECTOT ratios can be observed when comparing rural and urban results whatever the thermal protocol ECTOT being 50% lower than ECTOT at rural sites whereas it is only 20% lower at urban sites. The PM chemical composition could explain these differences but the way it influences the EC-OC measurement is not clear and needs further investigations. Meanwhile, some additional tests seem to indicate an influence of the oven soiling on the EC-OC measurement data quality. This enlightens the necessity to follow the laser signal decrease with time and its impact on measurements. Nevertheless, this should be confirmed by further experiments, involving more samples and various instruments, to enable statistical processing. All these results provide insights to determine the quality of EC-OC analytical methods and may contribute to the work toward establishing method standardisation.
    Atmospheric Measurement Techniques Discussions. 11/2013; 6(6):10231-10268.
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    ABSTRACT: The chemical composition of the plumes of seagoing ships was investigated during a two weeks long measurement campaign in the port of Rotterdam, Hoek van Holland, The Netherlands, in September 2009. Altogether, 497 ships were monitored and a statistical evaluation of emission factors (g kg-1 fuel) was provided. The concerned main atmospheric components were SO2, NO2, NOx and the aerosol particle number. In addition, the elemental and water-soluble ionic composition of the emitted particulate matter was determined. Emission factors were expressed as a function of ship type, power and crankshaft rotational speed. The average SO2 emission factor was found to be roughly half of what is allowed in sulphur emission control areas (16 vs. 30 g kg-1 fuel), and exceedances of this limit were rarely registered. A significant linear relationship was observed between the SO2 and particle number emission factor. The intercept of the regression line, 0.5 × 1016 (kg fuel)-1, gives the average number of particles formed during the burning of 1 kg zero sulphur content fuel, while the slope, 2 × 1018, provides the average number of particles formed with 1 kg sulphur burnt with the fuel. Water-soluble ionic composition analysis of the aerosol samples from the plumes showed that ~144 g of particulate sulphate was emitted from 1 kg sulphur burnt with the fuel. The mass median diameter of sulphate particles estimated from the measurements was ~42 nm.
    Atmospheric Measurement Techniques 12/2012; 5(6):8925-8967. · 3.21 Impact Factor
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    ABSTRACT: 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.
    Atmospheric Chemistry and Physics 09/2012; 12:8663–8677. · 4.88 Impact Factor
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    ABSTRACT: The first EMEP intensive measurement periods were held in June 2006 and January 2007. The measurements aimed to characterize the aerosol chemical compositions, including the gas/aerosol partitioning of inorganic compounds. The measurement program during these periods included daily or hourly measurements of the secondary inorganic components, with additional measurements of elemental- and organic carbon (EC and OC) and mineral dust in PM1, PM2.5 and PM10. These measurements have provided extended knowledge regarding the composition of particulate matter and the temporal and spatial variability of PM, as well as an extended database for the assessment of chemical transport models. This paper summarise the first experiences of making use of measurements from the first EMEP intensive measurement periods along with EMEP model results from the updated model version to characterise aerosol composition. We investigated how the PM chemical composition varies between the summer and the winter month and geographically. The observation and model data are in general agreement regarding the main features of PM10 and PM2.5 composition and the relative contribution of different components, though the EMEP model tends to give slightly lower estimates of PM10 and PM2.5 compared to measurements. The intensive measurement data has identified areas where improvements are needed. Hourly concurrent measurements of gaseous and particulate components for the first time facilitated testing of modelled diurnal variability of the gas/aerosol partitioning of nitrogen species. In general, the modelled diurnal cycles of nitrate and ammonium aerosols are in fair agreement with the measurements, but the diurnal variability of ammonia is not well captured. The largest differences between model and observations of aerosol mass are seen in Italy during winter, which to a large extent may be explained by an underestimation of residential wood burning sources. It should be noted that both primary and secondary OC has been included in the calculations for the first time, showing promising results. Mineral dust is important, especially in southern Europe, and the model seems to capture the dust episodes well. The lack of measurements of mineral dust hampers the possibility for model evaluation for this highly uncertain PM component. There are also lessons learnt regarding improved measurements for future intensive periods. There is a need for increased comparability between the measurements at different sites. For the nitrogen compounds it is clear that more measurements using artefact free methods based on continuous measurement methods and/or denuders are needed. For EC/OC, a reference methodology (both in field and laboratory) was lacking during these periods giving problems with comparability, though measurement protocols have recently been established and these should be followed by the Parties to the EMEP Protocol. For measurements with no defined protocols, it might be a good solution to use centralised laboratories to ensure comparability across the network. To cope with the introduction of these new measurements, new reporting guidelines have been developed to ensure that all proper information about the methodologies and data quality is given.
    ATMOSPHERIC CHEMISTRY AND PHYSICS 09/2012; 12(17):8073-8094. · 5.51 Impact Factor
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    ABSTRACT: This study focuses on the aerosol hygroscopic properties as determined from ground-based measurements and Mie theory. Usually, aerosol ground-based measurements are taken in dry conditions in order to have a consistency within networks. The dependence of the various aerosol optical characteristics (e.g. aerosol absorption, scattering, backscattering or extinction coefficients) on relative humidity has therefore to be established in order to determine their values in the atmosphere, where relative humidity can reach high values. We calculated mean monthly diurnal values of the aerosol hygroscopic growth factor at 90% relative humidity GF(90) based on measurements performed at the atmospheric research station in Ispra (Italy) with a Hygroscopicity Tandem Differential Mobility Analyzer over eight months in 2008 and 2009. Particle hygroscopicity increases with particle dry diameter ranging from 35 to 165 nm for all seasons. We observed a clear seasonal variation in GF(90) for particles larger than 75 nm, and a diurnal cycle in spring and winter for all sizes. For 165 nm particles, GF(90) averages 1.32 ± 0.06. The effect of the particle hygroscopic growth on the aerosol optical properties (scattering, extinction, absorption and backscatter coefficients, asymmetry parameter and backscatter faction) was computed using the Mie theory, based on data obtained from a series of instruments running at our station. We found median enhancement factors (defined as ratios between the values of optical variables at 90% and 0% relative humidity) equal to 1.1, 2.1, 1.7, and 1.8, for the aerosol absorption, scattering, backscattering, and extinction coefficients, respectively. All except the absorption enhancement factors show a strong correlation with the hygroscopic growth factor. The enhancement factors observed at our site are among the lowest observed across the world for the aerosol scattering coefficient, and among the highest for the aerosol backscatter fraction.
    ATMOSPHERIC CHEMISTRY AND PHYSICS 07/2012; 12(13):5703-5717. · 5.51 Impact Factor
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    ABSTRACT: This study focuses on the aerosol hygroscopic properties as determined from ground-based measurements and Mie theory. Usually, aerosol ground-based measurements are taken in dry conditions to ensure data consistency within networks. The dependence of the various aerosol optical characteristics (e.g. aerosol absorption, scattering, backscattering or extinction coefficients) on relative humidity has therefore to be established in order to determine their values in the atmosphere, where relative humidity can reach high values. We calculated mean monthly diurnal values of the aerosol hygroscopic growth factor at 90% relative humidity GF(90) based on measurements performed at EMEP-GAW station of Ispra with a Hygroscopicity Tandem Differential Mobility Analyzer over eight months in 2008 and 2009. Particle hygroscopicity increases with particle dry diameter ranging from 35 to 165 nm for all seasons. We observed a clear seasonal variation in GF(90) for particles larger than 75 nm, and a diurnal cycle in spring and winter for all sizes. For 165 nm particles, GF(90) averages 1.32 ± 0.06. The effect of the particle hygroscopic growth on the aerosol optical properties (scattering, extinction, absorption and backscatter coefficients, asymmetry parameter and backscatter faction) was computed using the Mie theory, based on data obtained from a series of instruments running at our station. We found median enhancement factors (defined as ratios between the values of optical variables at 90% and 0% relative humidity) equal to 1.1, 2.1, 1.7, and 1.8, for the aerosol absorption, scattering, backscattering, and extinction coefficients, respectively. All except the absorption enhancement factor show a strong correlation with the hygroscopic growth factor. The enhancement factors observed at our site are among the lowest observed across the world for the aerosol scattering coefficient, and among the highest for the aerosol backscatter fraction.
    Atmospheric Chemistry and Physics 02/2012; 12(2):5293-5340. · 4.88 Impact Factor
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    ABSTRACT: Abstract. The lack of standard reference materials for calibrating, troubleshooting and intercomparing techniques that measure the composition of black carbon, commonly referred to as soot, has been a major obstacle that hinders improved understanding of how climate and health is impacted by this ubiquitous component of the atmosphere. A different approach is offered here as a means of constructing precisely controlled material with fractions of organic carbon (OC) on the surface of elemental carbon (EC) whose structure reflects that of the combustion produced particles found in the atmosphere. The proposed soot reference material (SRM) uses EC as a basis substrate for surface coatings of organic compounds that are representative of the main classes of organics identified in the coverage of soot produced by fossil fuel burning. A number of methods are used to demonstrate the quality and stability of the reference EC and SRM. Comparison of the nominal fraction of OC deposited on the EC substrate with the fraction measured with thermal/optical analysis (TOA) shows excellent agreement. Application of this type of reference material for evaluating the different methods of carbon analysis may help resolve differences that currently exist between comparable measurement techniques when trying to separate OC and EC from ambient samples.
    Atmos. Meas. Tech. Discus. 01/2012; 5:2315-2362.
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    ABSTRACT: Soot, which is produced from biomass burning and the incomplete combustion of fossil and biomass fuels, has been linked to regional and global climate change and to negative health problems. Scientists measure the properties of soot using a variety of methods in order to quantify source emissions and understand its atmospheric chemistry, reactivity under emission conditions, interaction with solar radiation, influence on clouds, and health impacts. A major obstacle currently limiting progress is the absence of established standards or reference materials for calibrating the many instruments used to measure the various properties of soot. The current state of availability and practicability of soot standard reference materials (SRMs) was reviewed by a group of 50 international experts during a workshop in June of 2011. The workshop was convened to summarize the current knowledge on soot measurement techniques, identify the measurement uncertainties and limitations related to the lack of soot SRMs, and identify attributes of SRMs that, if developed, would reduce measurement uncertainties. The workshop established that suitable SRMs are available for calibrating some, but not all, measurement methods. The community of users of the single-particle soot-photometer (SP2), an instrument using laser-induced incandescence, identified a suitable SRM, fullerene soot, but users of instruments that measure light absorption by soot collected on filters did not. Similarly, those who use thermal optical analysis (TOA) to analyze the organic and elemental carbon components of soot were not satisfied with current SRMs. The workshop, and subsequent, interactive discussions, produced a number of recommendations for the development of new SRMs, and their implementation, that would be suitable for the different soot measurement methods.
    Atmospheric Measurement Techniques 01/2012; 5(8):1869-1887. · 3.21 Impact Factor
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    ABSTRACT: The source contributions to carbonaceous PM2.5 aerosol were investigated at a European background site at the edge of the Po Valley, in Northern Italy, during the period January–December 2007. Carbonaceous aerosol was described as the sum of eight source components: primary (1) and secondary (2) biomass burning organic carbon, biomass burning elemental carbon (3), primary (4) and secondary (5) fossil fuel burning organic carbon, fossil fuel burning elemental carbon (6), primary (7) and secondary (8) biogenic organic carbon. The concentration of each component was quantified using a set of macro tracers (organic carbon OC, elemental carbon EC, and levoglucosan), micro tracers (arabitol and mannitol), and 14C measurements. This was the first time that 14C measurements were performed on a long time series of data able to represent the entire annual cycle. This set of 6 tracers, together with assumed uncertainty ranges of the ratios of OC-to-EC, and the fraction of modern carbon in the 8 source categories, provides strong constraints to the source contributions to carbonaceous aerosol. The uncertainty of contributions was assessed with a Quasi-Monte Carlo (QMC) method accounting for the variability of OC and EC emission factors, and the uncertainty of reference fractions of modern carbon. During winter biomass burning composed 50% of the total carbon (TC) concentration, while in summer secondary biogenic OC accounted for 45% of TC. The contribution of primary biogenic aerosol particles was negligible during the entire year. Moreover, aerosol associated with fossil fuel burning represented 26% and 43% of TC in winter and summer, respectively. The comparison of source apportionment results in different urban and rural areas showed that the sampling site was mainly affected by local aerosol sources during winter and regional air masses from the nearby Po Valley in summer. This observation was further confirmed by back-trajectory analysis applying the Potential Source Contribution Function method to identify potential source regions. The contribution of secondary organic aerosol (SOA) to the organic mass (OM) was significant during the entire year. SOA accounted for 23% and 83% of OM during winter and summer, respectively. While the summer SOA was dominated by biogenic sources, winter SOA was mainly due to biomass and fossil fuel burning. This indicates that the oxidation of intermediate volatility organic compounds co-emitted with primary organics is a significant source of SOA, as suggested by recent model results and Aerosol Mass Spectrometer measurements in urban regions. Comparison with previous global model simulations, indicates a strong underestimate of wintertime primary aerosol emissions in this region.
    Atmospheric Chemistry and Physics 01/2011; · 4.88 Impact Factor
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    ABSTRACT: The source contributions to carbonaceous PM 2.5 aerosol were investigated at a European background site at the edge of the Po Valley, in Northern Italy, during the pe-riod January–December 2007. Carbonaceous aerosol was described as the sum of 8 source components: primary (1) and secondary (2) biomass burning organic carbon, biomass burning elemental carbon (3), primary (4) and secondary (5) fossil organic carbon, fossil fuel burning elemental carbon (6), primary (7) and secondary (8) biogenic organic carbon. The mass concentration of each component was quantified using a set of macro tracers (organic carbon OC, elemen-tal carbon EC, and levoglucosan), micro tracers (arabitol and mannitol), and 14 C measurements. This was the first time that 14 C measurements covered a full annual cycle with daily resolution. This set of 6 tracers, together with assumed un-certainty ranges of the ratios of OC-to-EC, and the reference fraction of modern carbon in the 8 source categories, pro-vides strong constraints to the source contributions to car-bonaceous aerosol. The uncertainty of contributions was as-sessed with a Quasi-Monte Carlo (QMC) method accounting for the variability of OC and EC emission factors, the un-certainty of reference fractions of modern carbon, and the measurement uncertainty. During winter, biomass burning composed 64 % (±15 %) of the total carbon (TC) concentration, while in summer sec-ondary biogenic OC accounted for 50 % (±16 %) of TC. The contribution of primary biogenic aerosol particles was Correspondence to: E. Vignati (elisabetta.vignati@jrc.ec.europa.eu) negligible during the entire year. Moreover, aerosol associ-ated with fossil sources represented 27 % (±16 %) and 41 % (±26 %) of TC in winter and summer, respectively. The con-tribution of secondary organic aerosol (SOA) to the organic mass (OM) was significant during the entire year. SOA ac-counted for 30 % (±16 %) and 85 % (±12 %) of OM during winter and summer, respectively. While the summer SOA was dominated by biogenic sources, winter SOA was mainly due to biomass burning and fossil sources. This indicates that the oxidation of semi-volatile and intermediate volatility or-ganic compounds co-emitted with primary organics is a sig-nificant source of SOA, as suggested by recent model results and Aerosol Mass Spectrometer measurements. Comparison with previous global model simulations, indicates a strong underestimate of wintertime primary aerosol emissions in this region. The comparison of source apportionment results in different urban and rural areas showed that the sampling site was mainly affected by local aerosol sources during win-ter and regional air masses from the nearby Po Valley in summer. This observation was further confirmed by back-trajectory analysis applying the Potential Source Contribu-tion Function method to identify potential source regions.
    Atmospheric Chemistry and Physics 01/2011; 11:5685-5700. · 5.51 Impact Factor
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    ABSTRACT: Two years of harmonized aerosol number size distribution data from 24 European field monitoring sites have been analysed. The results give a comprehensive overview of the European near surface aerosol particle number concentrations and number size distributions between 30 and 500 nm of dry particle diameter. Spatial and temporal distribution of aerosols in the particle sizes most important for climate applications are presented. We also analyse the annual, weekly and diurnal cycles of the aerosol number concentrations, provide log-normal fitting parameters for median number size distributions, and give guidance notes for data users. Emphasis is placed on the usability of results within the aerosol modelling community. We also show that the aerosol number concentrations of Aitken and accumulation mode particles (with 100 nm dry diameter as a cut-off between modes) are related, although there is significant variation in the ratios of the modal number concentrations. Different aerosol and station types are distinguished from this data and this methodology has potential for further categorization of stations aerosol number size distribution types. The European submicron aerosol was divided into characteristic types: Central European aerosol, characterized by single mode median size distributions, unimodal number concentration histograms and low variability in CCN-sized aerosol number concentrations; Nordic aerosol with low number concentrations, although showing pronounced seasonal variation of especially Aitken mode particles; Mountain sites (altitude over 1000 m a.s.l.) with a strong seasonal cycle in aerosol number concentrations, high variability, and very low median number concentrations. Southern and Western European regions had fewer stations, which decreases the regional representativeness of these results. Aerosol number concentrations over the Britain and Ireland had very high variance and there are indications of mixed air masses from several source regions; the Mediterranean aerosol exhibit high seasonality, and a strong accumulation mode in the summer. The highest concentrations were observed at the JRC station in Northern Italy with high accumulation mode number concentrations in the winter. The aerosol number concentrations at the Arctic station Zeppelin in Ny-Ålesund in Svalbard have also a strong seasonal cycle, with higher concentrations of accumulation mode particles in winter, and dominating summer Aitken mode indicating more recently formed particles. Observed particles did not show any statistically significant regional work-week or weekday related variation in number concentrations studied. Analysis products are made for open-access to the research community, available in a freely accessible internet site. The results give to the modelling community a reliable, easy-to-use and freely available comparison dataset of aerosol size distributions.
    Atmospheric Chemistry and Physics Discussions. 01/2011; 11:8893-8976.
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    ABSTRACT: It is important to understand the relative contribution of primary and secondary particles to regional and global aerosol so that models can attribute aerosol radiative forcing to different sources. In large-scale models, there is considerable uncertainty associated with treatments of particle formation (nucleation) in the boundary layer (BL) and in the size distribution of emitted primary particles, leading to uncertainties in predicted cloud condensation nuclei (CCN) concentrations. Here we quantify how primary particle emissions and secondary particle formation influence size-resolved particle number concentrations in the BL using a global aerosol microphysics model and aircraft and ground site observations made during the May 2008 campaign of the European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI). We tested four different parameterisations for BL nucleation and two assumptions for the emission size distribution of anthropogenic and wildfire carbonaceous particles. When we emit carbonaceous particles at small sizes (as recommended by the Aerosol Intercomparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with diameter >50 nm (N50) and >100 nm (N100) were well captured by the model (R2≥0.8) and the normalised mean bias (NMB) was also small (−18% for N50 and −1% for N100). Emission of carbonaceous particles at larger sizes, which we consider to be more realistic for low spatial resolution global models, results in equally good correlation but larger bias (R2≥0.8, NMB = −52% and −29%), which could be partly but not entirely compensated by BL nucleation. Within the uncertainty of the observations and accounting for the uncertainty in the size of emitted primary particles, BL nucleation makes a statistically significant contribution to CCN-sized particles at less than a quarter of the ground sites. Our results show that a major source of uncertainty in CCN-sized particles in polluted European air is the emitted size of primary carbonaceous particles. New information is required not just from direct observations, but also to determine the "effective emission size" and composition of primary particles appropriate for different resolution models.
    Atmospheric Chemistry and Physics 01/2011; 11(2011-12-05):12007-12036. · 4.88 Impact Factor
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    ATMOSPHERIC CHEMISTRY AND PHYSICS 01/2011; 11:5505-5538. · 5.51 Impact Factor
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    ABSTRACT: Remote sensing represents a prospective tool to complement in situ measurements for monitoring particulate matter air pollution. The remotely sensed aerosol metric which is generally related to the in situ measured particulate matter mass concentration (PM) is the aerosol optical thickness (AOT), the vertically integrated aerosol extinction that optically quantifies the aerosol load in the whole atmospheric column. Annual variations in AOT and PM can follow very different patterns, indicating that the AOT-to-PM conversion is not straightforward. In the Po Valley, northern Italy, AOT and PM seasonal cycles exhibit a marked phase shift. Making use of aerosol extinction vertical profiles derived from continuous aerosol lidar measurements, we further searched through the AOT-to-PM10 relationship in this region. On the basis of a 2-year (2006–2007) multisensor database, including remote sensing observations from ground and space and in situ measurements, this study: (1) discloses for the first time the height-resolved seasonal variability of the aerosol optical properties in the Po Valley, (2) demonstrates and quantifies the crucial role of the aerosol vertical distribution in the AOT-to-PM relationship in this region, (3) suggests a methodology to rescale AOT to ground-level aerosol extinction values that correlate with PM concentration and from which PM10 annual average and exceedances frequency of daily limit value can be retrieved within a few percentage points, and (4) highlights that the hygroscopic growth of the particles in the atmosphere is a critical factor for comparing in situ-measured to remotely sensed aerosol properties.
    Journal of Geophysical Research Atmospheres 10/2010; 115(D19):1-22. · 3.44 Impact Factor

Publication Stats

3k Citations
206.00 Total Impact Points

Institutions

  • 2001–2007
    • European Commission - Joint Research Centre
      • Institute for Environment and Sustainability
      Bruxelles, Brussels Capital Region, Italy
    • University of Bologna
      • "Giacomo Ciamician" Department of Chemistry CHIM
      Bologna, Emilia-Romagna, Italy
  • 2003
    • Université du Littoral Côte d'Opale (ULCO)
      Dunkirk, Nord-Pas-de-Calais, France
  • 2002
    • Klinikum Garmisch-Partenkirchen
      Markt Garmisch-Partenkirchen, Bavaria, Germany
    • Institute for Environmental Protection and Research (ISPRA)
      Roma, Latium, Italy