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- ItemSource apportionment of the organic aerosol over the Atlantic Ocean from 53° N to 53° S: Significant contributions from marine emissions and long-range transport(Katlenburg-Lindau : EGU, 2018) Huang, Shan; Wu, Zhijun; Poulain, Laurent; van Pinxteren, Manuela; Merkel, Maik; Assmann, Denise; Herrmann, Hartmut; Wiedensohler, AlfredMarine aerosol particles are an important part of the natural aerosol systems and might have a significant impact on the global climate and biological cycle. It is widely accepted that truly pristine marine conditions are difficult to find over the ocean. However, the influence of continental and anthropogenic emissions on the marine boundary layer (MBL) aerosol is still less understood and non-quantitative, causing uncertainties in the estimation of the climate effect of marine aerosols. This study presents a detailed chemical characterization of the MBL aerosol as well as the source apportionment of the organic aerosol (OA) composition. The data set covers the Atlantic Ocean from 53∘ N to 53∘ S, based on four open-ocean cruises in 2011 and 2012. The aerosol particle composition was measured with a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), which indicated that sub-micrometer aerosol particles over the Atlantic Ocean are mainly composed of sulfates (50 % of the particle mass concentration), organics (21 %) and sea salt (12 %). OA has been apportioned into five factors, including three factors linked to marine sources and two with continental and/or anthropogenic origins. The marine oxygenated OA (MOOA, 16 % of the total OA mass) and marine nitrogen-containing OA (MNOA, 16 %) are identified as marine secondary products with gaseous biogenic precursors dimethyl sulfide (DMS) or amines. Marine hydrocarbon-like OA (MHOA, 19 %) was attributed to the primary emissions from the Atlantic Ocean. The factor for the anthropogenic oxygenated OA (Anth-OOA, 19 %) is related to continental long-range transport. Represented by the combustion oxygenated OA (Comb-OOA), aged combustion emissions from maritime traffic and wild fires in Africa contributed, on average, a large fraction to the total OA mass (30 %). This study provides the important finding that long-range transport was found to contribute averagely 49 % of the submicron OA mass over the Atlantic Ocean. This is almost equal to that from marine sources (51 %). Furthermore, a detailed latitudinal distribution of OA source contributions showed that DMS oxidation contributed markedly to the OA over the South Atlantic during spring, while continental-related long-range transport largely influenced the marine atmosphere near Europe and western and central Africa (15∘ N to 15∘ S). In addition, supported by a solid correlation between marine tracer methanesulfonic acid (MSA) and the DMS-oxidation OA (MOOA, R2>0.85), this study suggests that the DMS-related secondary organic aerosol (SOA) over the Atlantic Ocean could be estimated by MSA and a scaling factor of 1.79, especially in spring.
- ItemSource apportionment and impact of long-range transport on carbonaceous aerosol particles in central Germany during HCCT-2010(Katlenburg-Lindau : EGU, 2021) Poulain, Laurent; Fahlbusch, Benjamin; Spindler, Gerald; Mueller, Konrad; van Pinxteren, Dominik; Wu, Zhijun; Iinuma, Yoshiteru; Birmili, Wolfram; Wiedensohler, Alfred; Herrmann, HartmutThe identification of different sources of the carbonaceous aerosol (organics and black carbon) was investigated at a mountain forest site located in central Germany from September to October 2010 to characterize incoming air masses during the Hill Cap Cloud Thuringia 2010 (HCCT-2010) experiment. The near-PM1 chemical composition, as measured by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), was dominated by organic aerosol (OA; 41 %) followed by sulfate (19 %) and nitrate (18 %). Source apportionment of the OA fraction was performed using the multilinear engine (ME-2) approach, resulting in the identification of the following five factors: hydrocarbon-like OA (HOA; 3 % of OA mass), biomass burning OA (BBOA; 13 %), semi-volatile-like OA (SV-OOA; 19 %), and two oxygenated OA (OOA) factors. The more oxidized OOA (MO-OOA, 28 %) was interpreted as being influenced by aged, polluted continental air masses, whereas the less oxidized OOA (LO-OOA, 37 %) was found to be more linked to aged biogenic sources. Equivalent black carbon (eBC), measured by a multi-angle absorption photometer (MAAP) represented 10 % of the total particulate matter (PM). The eBC was clearly associated with HOA, BBOA, and MO-OOA factors (all together R2=0.83). Therefore, eBC's contribution to each factor was achieved using a multi-linear regression model. More than half of the eBC (52 %) was associated with long-range transport (i.e., MO-OOA), whereas liquid fuel eBC (35 %) and biomass burning eBC (13 %) were associated with local emissions, leading to a complete apportionment of the carbonaceous aerosol. The separation between local and transported eBC was well supported by the mass size distribution of elemental carbon (EC) from Berner impactor samples. Air masses with the strongest marine influence, based on back trajectory analysis, corresponded with a low particle mass concentration (6.4–7.5 µg m−3) and organic fraction (≈30 %). However, they also had the largest contribution of primary OA (HOA ≈ 4 % and BBOA 15 %–20 %), which was associated with local emissions. Continental air masses had the highest mass concentration (11.4–12.6 µg m−3), and a larger fraction of oxygenated OA (≈45 %) indicated highly processed OA. The present results emphasize the key role played by long-range transport processes not only in the OA fraction but also in the eBC mass concentration and the importance of improving our knowledge on the identification of eBC sources.
- ItemDevelopment of a protocol for the auto-generation of explicit aqueous-phase oxidation schemes of organic compounds(Katlenburg-Lindau : EGU, 2019) Bräuer, Peter; Mouchel-Vallon, Camille; Tilgner, Andreas; Mutzel, Anke; Böge, Olaf; Rodigast, Maria; Poulain, Laurent; van Pinxteren, Dominik; Wolke, Ralf; Aumont, Bernard; Herrmann, HartmutThis paper presents a new CAPRAM-GECKOA protocol for mechanism auto-generation of aqueous-phase organic processes. For the development, kinetic data in the literature were reviewed and a database with 464 aqueousphase reactions of the hydroxyl radical with organic compounds and 130 nitrate radical reactions with organic compounds has been compiled and evaluated. Five different methods to predict aqueous-phase rate constants have been evaluated with the help of the kinetics database: gas-aqueous phase correlations, homologous series of various compound classes, radical reactivity comparisons, Evans-Polanyi-type correlations, and structure-activity relationships (SARs). The quality of these prediction methods was tested as well as their suitability for automated mechanism construction. Based on this evaluation, SARs form the basis of the new CAPRAM-GECKO-A protocol. Evans-Polanyi-type correlations have been advanced to consider all available H atoms in a molecule besides the H atoms with only the weakest bond dissociation enthalpies (BDEs). The improved Evans- Polanyi-type correlations are used to predict rate constants for aqueous-phase NO3 and organic compounds reactions. Extensive tests have been performed on essential parameters and on highly uncertain parameters with limited experimental data. These sensitivity studies led to further improvements in the new CAPRAM-GECKO-A protocol but also showed current limitations. Biggest uncertainties were observed in uptake processes and the estimation of Henry's law coefficients as well as radical chemistry, in particular the degradation of alkoxy radicals. Previous estimation methods showed several deficits, which impacted particle growth. For further evaluation, a 1,3,5-trimethylbenzene oxidation experiment has been performed in the aerosol chamber "Leipziger Aerosolkammer" (LEAK) at high relative humidity conditions and compared to a multiphase mechanism using the Master Chemical Mechanism (MCMv3.2) in the gas phase and using a methylglyoxal oxidation scheme of about 600 reactions generated with the new CAPRAM-GECKO-A protocol in the aqueous phase. While it was difficult to evaluate single particle constituents due to concentrations close to the detection limits of the instruments applied, the model studies showed the importance of aqueous-phase chemistry in respect to secondary organic aerosol (SOA) formation and particle growth. The new protocol forms the basis for further CAPRAM mechanism development towards a new version 4.0. Moreover, it can be used as a supplementary tool for aerosol chambers to design and analyse experiments of chemical complexity and help to understand them on a molecular level. © 2019 Author(s).
- 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.
- ItemThe impact of biomass burning and aqueous-phase processing on air quality: A multi-year source apportionment study in the Po Valley, Italy(Katlenburg-Lindau : EGU, 2020) Paglione, Marco; Gilardoni, Stefania; Rinaldi, Matteo; Decesari, Stefano; Zanca, Nicola; Sandrini, Silvia; Giulianelli, Lara; Bacco, Dimitri; Ferrari, Silvia; Poluzzi, Vanes; Scotto, Fabiana; Trentini, Arianna; Poulain, Laurent; Herrmann, Hartmut; Wiedensohler, Alfred; Canonaco, Francesco; Prévôt, André S.H.; Massoli, Paola; Carbone, Claudio; Facchini, Maria Cristina; Fuzzi, SandroThe Po Valley (Italy) is a well-known air quality hotspot characterized by particulate matter (PM) levels well above the limit set by the European Air Quality Directive and by the World Health Organization, especially during the colder season. In the framework of Emilia-Romagna regional project "Supersito", the southern Po Valley submicron aerosol chemical composition was characterized by means of high-resolution aerosol mass spectroscopy (HR-AMS) with the specific aim of organic aerosol (OA) characterization and source apportionment. Eight intensive observation periods (IOPs) were carried out over 4 years (from 2011 to 2014) at two different sites (Bologna, BO, urban background, and San Pietro Capofiume, SPC, rural background), to characterize the spatial variability and seasonality of the OA sources, with a special focus on the cold season. On the multi-year basis of the study, the AMS observations show that OA accounts for averages of 45 ± 8 % (ranging from 33 % to 58 %) and 46 ± 7 % (ranging from 36 % to 50 %) of the total non-refractory submicron particle mass (PM1-NR) at the urban and rural sites, respectively. Primary organic aerosol (POA) comprises biomass burning (23±13 % of OA) and fossil fuel (12±7 %) contributions with a marked seasonality in concentration. As expected, the biomass burning contribution to POA is more significant at the rural site (urban / rural concentration ratio of 0.67), but it is also an important source of POA at the urban site during the cold season, with contributions ranging from 14 % to 38 % of the total OA mass. Secondary organic aerosol (SOA) contributes to OA mass to a much larger extent than POA at both sites throughout the year (69 ± 16 % and 83 ± 16 % at the urban and rural sites, respectively), with important implications for public health. Within the secondary fraction of OA, the measurements highlight the importance of biomass burning aging products during the cold season, even at the urban background site. This biomass burning SOA fraction represents 14 %-44 % of the total OA mass in the cold season, indicating that in this region a major contribution of combustion sources to PM mass is mediated by environmental conditions and atmospheric reactivity. © 2020 Author(s).
- ItemAir quality in the German–Czech border region: A focus on harmful fractions of PM and ultrafine particles(Amsterdam : Elsevier, 2015) Schladitz, Alexander; Leníček, Jan; Beneš, Ivan; Kováč, Martin; Skorkovský, Jiří; Soukup, Aleš; Jandlová, Jana; Poulain, Laurent; Plachá, Helena; Löschau, Gunter; Wiedensohler, AlfredA comprehensive air quality study has been carried out at two urban background sites in Annaberg-Buchholz (Germany) and Ústí nad Labem (Czech Republic) in the German–Czech border region between January 2012 and June 2014. Special attention was paid to quantify harmful fractions of particulate matter (PM) and ultrafine particle number concentration (UFP) from solid fuel combustion and vehicular traffic. Source type contributions of UFP were quantified by using the daily concentration courses of UFP and nitrogen oxide. Two different source apportionment techniques were used to quantify relative and absolute mass contributions: positive matrix factorization for total PM2.5 and elemental carbon in PM2.5 and chemical mass balance for total PM1 and organic carbon in PM1. Contributions from solid fuel combustion strongly differed between the non-heating period (April–September) and the heating period (October–March). Major sources of solid fuel combustion in this study were wood and domestic coal combustion, while the proportion of industrial coal combustion was low (<3%). In Ústí nad Labem combustion of domestic brown coal was the most important source of organic carbon ranging from 34% to 43%. Wood combustion was an important source of organic carbon in Annaberg-Buchholz throughout the year. Heavy metals and less volatile polycyclic aromatic hydrocarbons (PAH) in the accumulation mode were related to solid fuel combustion with enhanced concentrations during the heating period. In contrast, vehicular PAH emissions were allocated to the Aitken mode. Only in Ústí nad Labem a significant contribution of photochemical new particle formation (e.g. from sulfur dioxide) to UFP of almost 50% was observed during noontime. UFPs from traffic emissions (nucleation particles) and primary emitted soot particles dominated at both sites during the rest of the day. The methodology of a combined source apportionment of UFP and PM can be adapted to other regions of the world with similar problems of atmospheric pollution to calculate the relative risk in epidemiological health studies for different sub-fractions of PM and UFP. This will enhance the meaningfulness of published relative risks in health studies based on total PM and UFP number concentrations..
- ItemModelling winter organic aerosol at the European scale with CAMx: Evaluation and source apportionment with a VBS parameterization based on novel wood burning smog chamber experiments(Katlenburg-Lindau : EGU, 2017) Ciarelli, Giancarlo; Aksoyoglu, Sebnem; El Haddad, Imad; Bruns, Emily A.; Crippa, Monica; Poulain, Laurent; Äijälä, Mikko; Carbone, Samara; Freney, Evelyn; O'Dowd, Colin; Baltensperger, Urs; Prévôt, André S. H.We evaluated a modified VBS (volatility basis set) scheme to treat biomass-burning-like organic aerosol (BBOA) implemented in CAMx (Comprehensive Air Quality Model with extensions). The updated scheme was parameterized with novel wood combustion smog chamber experiments using a hybrid VBS framework which accounts for a mixture of wood burning organic aerosol precursors and their further functionalization and fragmentation in the atmosphere. The new scheme was evaluated for one of the winter EMEP intensive campaigns (February-March 2009) against aerosol mass spectrometer (AMS) measurements performed at 11 sites in Europe. We found a considerable improvement for the modelled organic aerosol (OA) mass compared to our previous model application with the mean fractional bias (MFB) reduced from -61 to -29 %. We performed model-based source apportionment studies and compared results against positive matrix factorization (PMF) analysis performed on OA AMS data. Both model and observations suggest that OA was mainly of secondary origin at almost all sites. Modelled secondary organic aerosol (SOA) contributions to total OA varied from 32 to 88% (with an average contribution of 62 %) and absolute concentrations were generally under-predicted. Modelled primary hydrocarbon-like organic aerosol (HOA) and primary biomass-burning-like aerosol (BBPOA) fractions contributed to a lesser extent (HOA from 3 to 30 %, and BBPOA from 1 to 39 %) with average contributions of 13 and 25 %, respectively. Modelled BBPOA fractions were found to represent 12 to 64% of the total residential-heating-related OA, with increasing contributions at stations located in the northern part of the domain. Source apportionment studies were performed to assess the contribution of residential and non-residential combustion precursors to the total SOA. Non-residential combustion and road transportation sector contributed about 30-40% to SOA formation (with increasing contributions at urban and near industrialized sites), whereas residential combustion (mainly related to wood burning) contributed to a larger extent, around 60-70 %. Contributions to OA from residential combustion precursors in different volatility ranges were also assessed: our results indicate that residential combustion gas-phase precursors in the semivolatile range (SVOC) contributed from 6 to 30 %, with higher contributions predicted at stations located in the southern part of the domain. On the other hand, the oxidation products of higher-volatility precursors (the sum of intermediate-volatility compounds (IVOCs) and volatile organic compounds (VOCs)) contribute from 15 to 38% with no specific gradient among the stations. Although the new parameterization leads to a better agreement between model results and observations, it still underpredicts the SOA fraction, suggesting that uncertainties in the new scheme and other sources and/or formation mechanisms remain to be elucidated. Moreover, a more detailed characterization of the semivolatile components of the emissions is needed.
- ItemMulti-year ACSM measurements at the central European research station Melpitz (Germany)-Part 1: Instrument robustness, quality assurance, and impact of upper size cutoff diameter(Katlenburg-Lindau : Copernicus, 2020) Poulain, Laurent; Spindler, Gerald; Grüner, Achim; Tuch, Thomas; Stieger, Bastian; van Pinxteren, Dominik; Petit, Jean-Eudes; Favez, Olivier; Herrmann, Hartmut; Wiedensohler, AlfredThe aerosol chemical speciation monitor (ACSM) is nowadays widely used to identify and quantify the main components of fine particles in ambient air. As such, its deployment at observatory platforms is fully incorporated within the European Aerosol, Clouds and Trace Gases Research Infrastructure (ACTRIS). Regular intercomparisons are organized at the Aerosol Chemical Monitoring Calibration Center (ACMCC; part of the European Center for Aerosol Calibration, Paris, France) to ensure the consistency of the dataset, as well as instrumental performance and variability. However, in situ quality assurance remains a fundamental aspect of the instrument's stability. Here, we present and discuss the main outputs of long-term quality assurance efforts achieved for ACSM measurements at the research station Melpitz (Germany) since 2012 onwards. In order to validate the ACSM measurements over the years and to characterize seasonal variations, nitrate, sulfate, ammonium, organic, and particle mass concentrations were systematically compared against the collocated measurements of daily offline high-volume PM1 and PM2:5 filter samples and particle number size distribution (PNSD) measurements. Mass closure analysis was made by comparing the total particle mass (PM) concentration obtained by adding the mass concentration of equivalent black carbon (eBC) from the multi-angle absorption photometer (MAAP) to the ACSM chemical composition, to that of PM1 and PM2:5 during filter weighing, as well as to the derived mass concentration of PNSD. A combination of PM1 and PM2:5 filter samples helped identifying the critical importance of the upper size cutoff of the ACSM during such exercises. The ACSM-MAAP-derived mass concentrations systematically deviated from the PM1 mass when the mass concentration of the latter represented less than 60% of PM2:5, which was linked to the transmission efficiency of the aerodynamic lenses of the ACSM. The best correlations are obtained for sulfate (slopeD 0:96; R2 D 0:77) and total PM (slopeD 1:02; R2 D 0:90). Although, sulfate did not exhibit a seasonal dependency, total PM mass concentration revealed a small seasonal variability linked to the increase in non-water-soluble fractions. The nitrate suffers from a loss of ammonium nitrate during filter collection, and the contribution of organo-nitrate compounds to the ACSM nitrate signal make it difficult to directly compare the two methods. The contribution of m=z 44 (f44) to the total organic mass concentration was used to convert the ACSM organic mass (OM) to organic carbon (OC) by using a similar approach as for the aerosol mass spectrometer (AMS). The resulting estimated OCACSM was compared with the measured OCPM1 (slopeD 0:74; R2 D 0:77), indicating that the f44 signal was relatively free of interferences during this period. The PM2:5 filter samples use for the ACSM data quality might suffer from a systematic bias due to a size truncation effect as well as to the presence of chemical species that cannot be detected by the ACSM in coarse mode (e.g., sodium nitrate and sodium sulfate). This may lead to a systematic underestimation of the ACSM particle mass concentration and/or a positive artifact that artificially decreases the discrepancies between the two methods. Consequently, ACSM data validation using PM2:5 filters has to be interpreted with extreme care. The particle mass closure with the PNSD was satisfying (slopeD 0:77; R2 D 0:90 over the entire period), with a slight overestimation of the mobility particle size spectrometer (MPSS)-derived mass concentration in winter. This seasonal variability was related to a change on the PNSD and a larger contribution of the supermicrometer particles in winter. This long-term analysis between the ACSM and other collocated instruments confirms the robustness of the ACSM and its suitability for long-term measurements. Particle mass closure with the PNSD is strongly recommended to ensure the stability of the ACSM. A near-real-time mass closure procedure within the entire ACTRIS-ACSM network certainly represents an optimal quality control and assurance of both warranting the quality assurance of the ACSM measurements as well as identifying cross-instrumental biases. © Author(s) 2020.
- ItemSize-resolved aerosol composition at an urban and a rural site in the Po Valley in summertime: implications for secondary aerosol formation(München : European Geopyhsical Union, 2016) Sandrini, Silvia; van Pinxteren, Dominik; Giulianelli, Lara; Herrmann, Hartmut; Poulain, Laurent; Facchini, Maria Cristina; Gilardoni, Stefania; Rinaldi, Matteo; Paglione, Marco; Turpin, Barbara J.; Pollini, Francesca; Bucci, Silvia; Zanca, Nicola; Decesari, StefanoThe aerosol size-segregated chemical composition was analyzed at an urban (Bologna) and a rural (San Pietro Capofiume) site in the Po Valley, Italy, during June and July 2012, by ion-chromatography (major water-soluble ions and organic acids) and evolved gas analysis (total and water-soluble carbon), to investigate sources and mechanisms of secondary aerosol formation during the summer. A significant enhancement of secondary organic and inorganic aerosol mass was observed under anticyclonic conditions with recirculation of planetary boundary layer air but with substantial differences between the urban and the rural site. The data analysis, including a principal component analysis (PCA) on the size-resolved dataset of chemical concentrations, indicated that the photochemical oxidation of inorganic and organic gaseous precursors was an important mechanism of secondary aerosol formation at both sites. In addition, at the rural site a second formation process, explaining the largest fraction (22 %) of the total variance, was active at nighttime, especially under stagnant conditions. Nocturnal chemistry in the rural Po Valley was associated with the formation of ammonium nitrate in large accumulation-mode (0.42–1.2 µm) aerosols favored by local thermodynamic conditions (higher relative humidity and lower temperature compared to the urban site). Nocturnal concentrations of fine nitrate were, in fact, on average 5 times higher at the rural site than in Bologna. The water uptake by this highly hygroscopic compound under high RH conditions provided the medium for increased nocturnal aerosol uptake of water-soluble organic gases and possibly also for aqueous chemistry, as revealed by the shifting of peak concentrations of secondary compounds (water-soluble organic carbon (WSOC) and sulfate) toward the large accumulation mode (0.42–1.2 µm). Contrarily, the diurnal production of WSOC (proxy for secondary organic aerosol) by photochemistry was similar at the two sites but mostly affected the small accumulation mode of particles (0.14–0.42 µm) in Bologna, while a shift to larger accumulation mode was observed at the rural site. A significant increment in carbonaceous aerosol concentration (for both WSOC and water-insoluble carbon) at the urban site was recorded mainly in the quasi-ultrafine fraction (size range 0.05–0.14 µm), indicating a direct influence of traffic emissions on the mass concentrations of this range of particles.
- ItemEURODELTA III exercise: An evaluation of air quality models’ capacity to reproduce the carbonaceous aerosol(Amsterdam : Elsevier, 2019) Mircea, Mihaela; Bessagnet, Bertrand; D'Isidoro, Massimo; Pirovano, Guido; Aksoyoglu, Sebnem; Ciarelli, Giancarlo; Tsyro, Svetlana; Manders, Astrid; Bieser, Johannes; Stern, Rainer; Vivanco, Marta García; Cuvelier, Cornelius; Aas, Wenche; Prévôt, André S.H.; Aulinger, Armin; Briganti, Gino; Calori, Giuseppe; Cappelletti, Andrea; Colette, Augustin; Couvidat, Florian; Fagerli, Hilde; Finardi, Sandro; Kranenburg, Richard; Rouïl, Laurence; Silibello, Camillo; Spindler, Gerald; Poulain, Laurent; Herrmann, Hartmut; Jimenez, Jose L.; Day, Douglas A.; Tiitta, Petri; Carbone, SamaraThe carbonaceous aerosol accounts for an important part of total aerosol mass, affects human health and climate through its effects on physical and chemical properties of the aerosol, yet the understanding of its atmospheric sources and sinks is still incomplete. This study shows the state-of-the-art in modelling carbonaceous aerosol over Europe by comparing simulations performed with seven chemical transport models (CTMs) currently in air quality assessments in Europe: CAMx, CHIMERE, CMAQ, EMEP/MSC-W, LOTOS-EUROS, MINNI and RCGC. The simulations were carried out in the framework of the EURODELTA III modelling exercise and were evaluated against field measurements from intensive campaigns of European Monitoring and Evaluation Programme (EMEP) and the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI). Model simulations were performed over the same domain, using as much as possible the same input data and covering four seasons: summer (1–30 June 2006), winter (8 January – 4 February 2007), autumn (17 September- 15 October 2008) and spring (25 February - 26 March 2009). The analyses of models’ performances in prediction of elemental carbon (EC) for the four seasons and organic aerosol components (OA) for the last two seasons show that all models generally underestimate the measured concentrations. The maximum underestimation of EC is about 60% and up to about 80% for total organic matter (TOM). The underestimation of TOM outside of highly polluted area is a consequence of an underestimation of secondary organic aerosol (SOA), in particular of its main contributor: biogenic secondary aerosol (BSOA). This result is independent on the SOA modelling approach used and season. The concentrations and daily cycles of total primary organic matter (TPOM) are generally better reproduced by the models since they used the same anthropogenic emissions. However, the combination of emissions and model formulation leads to overestimate TPOM concentrations in 2009 for most of the models. All models capture relatively well the SOA daily cycles at rural stations mainly due to the spatial resolution used in the simulations. For the investigated carbonaceous aerosol compounds, the differences between the concentrations simulated by different models are lower than the differences between the concentrations simulated with a model for different seasons. © 2019 The Authors
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