A secondary organic aerosol (SOA) model, the Hydrophilic/Hydrophobic Organic model (H2O), is presented and evaluated over Europe. H2O uses surrogate organic molecules to represent the myriad of SOA species and distinguishes two kinds of surrogate species: hydrophilic species (which condense preferentially into an aqueous phase) and hydrophobic species (which condense only into an organic phase). These surrogate species are formed from the oxidation in the atmosphere of volatile organic compounds. H2O includes several important processes, including the effect of nitrogen oxides (NOX) on SOA formation, the dissociation of organic acids in an aqueous phase, the oligomerization of aldehydes, the non‐ideality of the particle phase and the hygroscopicity of organics. Concentrations of organic aerosols were simulated over Europe from July 2002 to July 2003 for comparison with measurements of the European Monitoring Evaluation Program (EMEP). In H2O, primary organic aerosols (POA) are considered as semi‐volatile organic compounds (SVOC) present in both the gas phase and the particle phase. Taking into account the gas‐phase fraction of SVOC increases significantly organic PM concentrations, particularly in winter, in better agreement with observations. The impacts on organic aerosol formation of ideality, of the choice of the parameterization for isoprene SOA formation, and of the OM/OC ratio of the model were also investigated. Assuming ideality in H2O was found to lead to a small decrease in OM. Compared to a two‐product parameterization, the parameterization of Couvidat and Seigneur [2011] for SOA formation from isoprene oxidation leads to a significant increase in isoprene SOA by taking into account their hydrophilic properties and suggests that most models may currently underestimate isoprene SOA.
This paper aims at presenting a validation of multi-pollutants over Europe with a focus on aerosols. Chemistry-Transport Models are now used for forecast and emission reduction studies not only for gas-phase species but also for aerosols. Comprehensive model-to-data comparisons are therefore required. We present in this paper a preliminary validation study of the POLYPHEMUS system applied over Europe for 2001. The aerosol model is the SIze REsolved Aerosol Model (SIREAM). It is a sectional model that describes the temporal evolution of the size/composition distribution of atmospheric particles containing a mix of black carbon, mineral dust, inorganic species, and primary and secondary organics. In addition to a brief model description, we present an overview of the model validation. A comprehensive set of model-to-data statistics is computed with observational data extracted from three European databases (the EMEP, AirBase and BDQA databases). Model performance criteria are verified for ozone and particulate matter (PM) and its inorganic components. Comparisons of correlations and root mean square errors with those generated by other models run over Europe for 2001 indicate a good performance of the POLYPHEMUS system. Modifications of the system configuration and parameterizations may have a significant impact on error statistics, which may question the robustness of such models. Because large differences exist between databases, the robustness of model-to-data error statistics is also investigated.
Abstract. We briefly present in this short paper a new SIze REsolved Aerosol Model (SIREAM) which simulates the evolution of atmospheric aerosol by solving the General Dynamic Equation (GDE). SIREAM segregates the aerosol size distribution into sections and solves the GDE by splitting coagulation and condensation/evaporationnucleation. A quasi-stationary sectional approach is used to describe the size distribution change due to condensation/evaporation, and a hybrid equilibrium/dynamical masstransfer method has been developed to lower the computational burden. SIREAM uses the same physical parameterizations as those used in the Modal Aerosol Model, MAM . It is hosted in the modeling system POLYPHEMUS Mallet et al., 2007, but can be linked to any other three-dimensional Chemistry-Transport Model.
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