Abstract

Abstract. A new aerosol module was developed and integrated in the air quality model CHIMERE. Developments include the use of the Model of Emissions and Gases and Aerosols from Nature (MEGAN) 2.1 for biogenic emissions, the implementation of the inorganic thermodynamic model ISORROPIA 2.1, revision of wet deposition processes and of the algorithms of condensation/evaporation and coagulation and the implementation of the secondary organic aerosol (SOA) mechanism H2O and the thermodynamic model SOAP. Concentrations of particles over Europe were simulated by the model for the year 2013. Model concentrations were compared to the European Monitoring and Evaluation Programme (EMEP) observations and other observations available in the EBAS database to evaluate the performance of the model. Performances were determined for several components of particles (sea salt, sulfate, ammonium, nitrate, organic aerosol) with a seasonal and regional analysis of results. The model gives satisfactory performance in general. For sea salt, the model succeeds in reproducing the seasonal evolution of concentrations for western and central Europe. For sulfate, except for an overestimation of sulfate in northern Europe, modeled concentrations are close to observations and the model succeeds in reproducing the seasonal evolution of concentrations. For organic aerosol, the model reproduces with satisfactory results concentrations for stations with strong modeled biogenic SOA concentrations. However, the model strongly overestimates ammonium nitrate concentrations during late autumn (possibly due to problems in the temporal evolution of emissions) and strongly underestimates summer organic aerosol concentrations over most of the stations (especially in the northern half of Europe). This underestimation could be due to a lack of anthropogenic SOA or biogenic emissions in northern Europe. A list of recommended tests and developments to improve the model is also given.

Highlights

  • Atmospheric particulate matter (PM) contributes to adverse effects on health and ecosystems

  • VOC emissions (based on the European Monitoring and Evaluation Programme (EMEP) inventory in this study) are used as in Menut et al (2013); volatile organic compounds are split into CHIMERE model species according to a speciation database depending on the emission sector

  • A similar feature is obtained with PM10 but with lower mean fractional bias (MFB) in March, November and December, which is probably due to some compensation effects and an underestimation of the coarse fraction of PM

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Summary

Introduction

Atmospheric particulate matter (PM) contributes to adverse effects on health and ecosystems. PM consists of various chemical species: organic matter (OM), elemental carbon (EC) mainly originating from anthropogenic sources, major inorganic components (ammonium, nitrate and sulfate), sea salt, mineral dust and other crustal compounds. To simulate PM concentrations, models have to take into account the microphysics of particles (condensation/evaporation, coagulation, nucleation), chemical mechanisms for the gas-phase chemistry, aerosol thermodynamics, emissions and deposition processes. The second part focuses on the comparison of modeled concentrations with observations for Cl−, Na+, SO24−, NO−3 , NH+4 , organic carbon, PM2.5 and PM10 with a regional and seasonal analysis of results

Method
Chemical mechanisms
Biogenic emissions
Anthropogenic emissions
Thermodynamic of secondary organic and inorganic aerosols
Computation of the wet diameter and the wet density of particles
Dry deposition of particles and semi-volatile organic species
Wet deposition of particles and semi-volatile species
Coagulation
Nucleation
Simulation setup
Observations
Sea salt
Sulfate
Ammonium and nitrate
Organic aerosol
PM concentrations
The case of the Cyprus station
Perspectives on model improvement
Conclusions
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