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Volume 17, issue 12 | Copyright
Atmos. Chem. Phys., 17, 7653-7669, 2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.

Research article 23 Jun 2017

Research article | 23 Jun 2017

Modelling 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

Giancarlo Ciarelli1,a, Sebnem Aksoyoglu1, Imad El Haddad1, Emily A. Bruns1, Monica Crippa2, Laurent Poulain3, Mikko Äijälä4, Samara Carbone5, Evelyn Freney6, Colin O'Dowd7, Urs Baltensperger1, and André S. H. Prévôt1 Giancarlo Ciarelli et al.
  • 1Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
  • 2European Commission, Joint Research Centre (JRC), Directorate for Energy, Transport and Climate, Air and Climate Unit, Via E. Fermi 2749, 21027 Ispra (VA), Italy
  • 3Leibniz Institute for Tropospheric Research (TROPOS), Permoserstr. 15, 04318 Leipzig, Germany
  • 4Department of Physics, University of Helsinki, Helsinki, Finland
  • 5Institute of Physics, University of São Paulo, Rua do Matão Travessa R, 187, 05508-090 São Paulo, S.P., Brazil
  • 6Laboratoire de Météorologie Physique (LaMP), CNRS/Université Blaise Pascal, Clermont-Ferrand, France
  • 7School of Physics and Centre for Climate & Air Pollution Studies, Ryan Institute, National University of Ireland Galway, University Road, Galway, Ireland
  • anow at: Laboratoire Inter-Universitaire des Systèmes Atmosphériques (LISA), UMR CNRS 7583, Université Paris Est Créteil et Université Paris Diderot, Institut Pierre Simon Laplace, Créteil, France

Abstract. 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 under-predicts 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.

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Short summary
Organic aerosol (OA) comprises the main fraction of fine particulate matter (PM1). Using a new VBS parameterization, we performed model-based source apportionment studies to assess the importance of different emission sources to the total OA loads in Europe during winter periods. Our results indicate that residential wood burning emissions represent the major source of OA, followed by non-residential emission sources (i.e. traffic and industries).
Organic aerosol (OA) comprises the main fraction of fine particulate matter (PM1). Using a new...