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Discussion papers
https://doi.org/10.5194/gmd-2019-70
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/gmd-2019-70
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.

Model evaluation paper 03 Apr 2019

Model evaluation paper | 03 Apr 2019

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This discussion paper is a preprint. It is a manuscript under review for the journal Geoscientific Model Development (GMD).

Trends of inorganic and organic aerosols and precursor gases in Europe: insights from the EURODELTA multi-model experiment over the 1990–2010 period

Giancarlo Ciarelli1,2,a, Mark R. Theobald3, Marta G. Vivanco3, Matthias Beekmann1, Wenche Aas4, Camilla Andersson5, Robert Bergström5,6, Astrid Manders-Groot7, Florian Couvidat2, Mihaela Mircea8, Svetlana Tsyro9, Hilde Fagerli9, Kathleen Mar10, Valentin Raffort11, Yelva Roustan11, Maria-T. Pay12, Martijn Schaap7, Richard Kranenburg7, Mario Adani8, Gino Briganti8, Andrea Cappelletti8, Massimo D'Isidoro8, Cornelis Cuvelier13, Arineh Cholakian1,2, Bertrand Bessagnet2,b, Peter Wind9,14, and Augustin Colette2 Giancarlo Ciarelli et al.
  • 1Laboratoire Inter-Universitaire des Systèmes Atmosphériques (LISA), UMR CNRS 7583, Université Paris Est Créteil et Université Paris Diderot, Institut Pierre Simon Laplace, Créteil, France
  • 2National Institute for Industrial Environment and Risks (INERIS), Parc Technologique ALATA, 60550 Verneuil-en-Halatte, France
  • 3CIEMAT, Research Centre for Energy, Environment and Technology, Madrid, Spain
  • 4Norwegian Institute for Air Research (NILU), Box 100, 2027 Kjeller, Norway
  • 5Swedish Meteorological and Hydrological Institute, 60176 Norrköping, Sweden
  • 6Department of Space, Earth and Environment, Chalmers University of Technology, 41296 Gothenburg, Sweden
  • 7Netherlands Organisation for applied scientific research (TNO), P.O. Box 80015, 3508 TA Utrecht, the Netherlands
  • 8Italian National Agency for New Technologies, Energy and Sustainable Economic Development (ENEA), Via Martiri di Monte Sole 4, 40129 Bologna, Italy
  • 9Climate Modelling and Air Pollution Division, Research and Development Department, Norwegian Meteorological Institute (MET Norway), Blindern, 0313 Oslo, Norway
  • 10Institute for Advanced Sustainability Studies (IASS), Postdam, Germany
  • 11CEREA, Joint Laboratory Ecole des Ponts ParisTech – EDF R&D, Champs-Sur-Marne, France
  • 12Barcelona Supercomputing Center, Centro Nacional de Supercomputación, Jordi Girona, 29, 08034 Barcelona, Spain
  • 13ex European Commission - JRC, Ispra, Italy
  • 14Faculty of Science and Technology, University of Tromsø, Tromsø, Norway
  • anow at: Department of Chemical Engineering, Carnegie Mellon University, Pittsburgh, USA
  • bnow at: Hangzhou Futuris Environmental Technology Co. Ltd, Zhejiang Overseas High-Level Talent Innovation Park, No. 998 WenYi Road, 311121, Hangzhou, Zhejiang, China

Abstract. In the framework of the EURODELTA-Trends (EDT) modeling experiment, several chemical transport models (CTMs) were applied for the 1990–2010 period to investigate air quality changes in Europe as well as the capability of the models to reproduce observed long-term air quality trends. Five CTMs have provided modeled air quality data for twenty-one continuous years in Europe using emission scenarios prepared by IIASA/GAINS and corresponding year-by-year meteorology derived from ERA-interim global reanalysis. For this study, long-term observations of particle sulfate (SO42−), total nitrate (TNO3), total ammonium (TNHx) as well as sulfur dioxide (SO2) and nitrogen dioxide (NO2) for multiple sites in Europe were used to validate the model results. The trends analysis was performed for the full twenty-one years (referred to as PT), but also for two 11-year sub-periods: 1990–2000 (referred to as P1) and 2000–2010 (referred to as P2).

The experiment revealed that the models were able to reproduce the faster decline in observed SO2 concentrations during the first decade, i.e. 1990–2000, with a 64–76 % mean relative reduction in SO2 concentrations indicated by the EDT experiment (range of all the models) versus an 82 % mean relative reduction in observed concentrations. During the second decade, P2, the models estimated a mean relative reduction in SO2 concentrations of about 34–54 %, which was also in line with that observed (47 %). Comparisons of observed and modeled NO2 trends revealed a mean relative decrease of 25 % and between 19–23 % (range of all the models) during the P1 period, and 12 % and between 22–26 % (range of all the models) during the P2 period, respectively.

Comparisons of observed and modeled trends in SO42− concentrations during the P1 period indicated that the models were able to reproduce the observed trends at most of the sites, with a 42–54 % mean relative reduction indicated by the EDT experiment (range of all models) versus a 57 % mean relative reduction in observed concentrations, and with good performances also during the P2 and PT periods. Moreover, especially during the P1 period, both modeled and observational data indicated smaller reductions in SO42− concentrations compared with its gas-phase precursor (i.e. SO2), which could be mainly attributed to increased oxidant levels and pH-dependent cloud chemistry. An analysis of the trends in TNO3 concentrations indicated a 28–39 % and 29 % mean relative reduction in TNO3 concentrations for the full period for model data (range of all the models) and observations, respectively. Further analysis of the trends in modeled HNO3 and particle nitrate (NO3) concentrations revealed that the relative reduction in HNO3 was larger than that for NO3 during the P1 period, which was mainly attributed to an increased availability of “free-ammonia”. By contrast, trends in modeled HNO3 and NO3 concentrations were more comparable during the P2 period. Also, trends of TNHx concentrations were, in general, under-predicted by all models, with worst performance for the P1 period than for P2.

Trends in modeled anthropogenic and biogenic secondary organic aerosol (ASOA and BSOA) concentrations together with the trends in available emissions of biogenic volatile organic compounds (BVOCs) were also investigated. A strong decrease in ASOA was indicated by all the models, following the reduction in anthropogenic NMVOCs precursors. Biogenic emission data provided by the modeling teams indicated a few areas with statistically significant increase in isoprene emission and monoterpene emissions during the 1990–2010 period over Fennoscandia and Eastern European regions (i.e. around 14–27 %), which was mainly attributed to the increase of surface temperature. However, the modeled BSOA concentrations did not linearly follow the increase in biogenic emissions. Finally, a comprehensive evaluation against positive matrix factorization (PMF) data, available during the second period (P2) at various European sites, revealed a systematic under-estimation of the modeled SOA fractions of between a factor of 3 to 11, on average, most likely because of missing SOA precursors and formation pathways, with reduced biases for the models that accounted for chemical aging of semi-volatile SOA components in the atmosphere.

Giancarlo Ciarelli et al.
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Short summary
The novel multi-model EURODELTA-Trends exercise provided 21-year of continuous PM components and their gas-phase precursors concentrations over Europe from the year 1990. The models’ capabilities to reproduce PM components and gas-phase PM precursors trends over the 1990–2010 period is the key focus of this study. The models were able to reproduce the observed trends relatively well, indicating a possible shift in the thermodynamic equilibrium between gas and particle phase.
The novel multi-model EURODELTA-Trends exercise provided 21-year of continuous PM components and...
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