Thèse de doctorat en Physique de l'Atmosphère
Soutenue le 18-12-2012
à Clermont-Ferrand 2 , dans le cadre de École doctorale des sciences fondamentales (Clermont-Ferrand) , en partenariat avec Laboratoire de météorologie physique (Clermont-Ferrand) (équipe de recherche) .
Le président du jury était Nadine Chaumerliac.
Modeling of physico-chemical properties of atmospheric aerosols at high altitude
Aerosol particles are ubiquitous in the Earth’s atmosphere. Although a minor constituent of the atmosphere, the aerosol particles are linked to visibility reduction, adverse health effects and heat balance of the Earth. The secondary aerosols which are formed in the atmosphere from the gaseous phase : precursor gases become particles by nucleation and condensation (Seinfeld and Pandis, 1998) represents the largest source in a number concentration of atmospheric particles. The chemical reactions can play an important role by turning high volatility gases into species with low vapor pressure and thus high saturation ratio, i.e. creating favorable conditions for particulate matter formation. In this work the CHIMERE chemical transport model is used to ameliorate our understanding of the governing processes for aerosol formation and to investigate its capability to reproduce the mass and number concentrations and temporal evolution of the aerosols particles at high altitudes (as for example Puy de Dome research station), and in particular, evaluate its capacity to simulate the formation of new particles due to nucleation. For the studied cases it was investigated the impact of : a fine resolution topographical database on the accuracy of simulation of dynamical parameters at high altitude, of the use of different emissions databases in the accuracy of gas-phase and aerosol concentration predictions, what is the most adequate nucleation parameterization scheme for simulating new particle formation at high altitude and what is the influence of the choice of the primary particle size distribution on the prediction of new particle formation. Also the ability of the different theories to reproduce the occurrence or lack of a nucleation event is evaluated.