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Article Dans Une Revue Atmospheric Chemistry and Physics Année : 2018

Modeling the partitioning of organic chemical species in cloud phases with CLEPS (1.1)

Résumé

The new detailed aqueous-phase mechanism Cloud Explicit Physico-chemical Scheme (CLEPS 1.0), which describes the oxidation of isoprene-derived water-soluble organic compounds, is coupled with a warm micro-physical module simulating the activation of aerosol particles into cloud droplets. CLEPS 1.0 was then extended to CLEPS 1.1 to include the chemistry of the newly added di-carboxylic acids dissolved from the particulate phase. The resulting coupled model allows the prediction of the aqueous-phase concentrations of chemical compounds originating from particle scavenging, mass transfer from the gas-phase and in-cloud aqueous chemical reactivity. The aim of the present study was more particularly to investigate the effect of particle scavenging on cloud chemistry. Several simulations were performed to assess the influence of various parameters on model predictions and to interpret long-term measurements conducted at the top of Puy de Dôme (PUY, France) in marine air masses. Specific attention was paid to carboxylic acids, whose predicted concentrations are on average in the lower range of the observations, with the exception of formic acid, which is rather overestimated in the model. The different sensitivity runs highlight the fact that formic and acetic acids mainly originate from the gas phase and have highly variable aqueous-phase reactivity depending on the cloud acidity, whereas C 3-C 4 carboxylic acids mainly originate from the particulate phase and are supersaturated in the cloud.
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Dates et versions

hal-01819360 , version 1 (30-10-2020)

Licence

Paternité - Pas de modifications

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Clémence Rose, Nadine Chaumerliac, Laurent Deguillaume, Hélène Perroux, Camille Mouchel-Vallon, et al.. Modeling the partitioning of organic chemical species in cloud phases with CLEPS (1.1). Atmospheric Chemistry and Physics, 2018, 18 (3), pp.2225 - 2242. ⟨10.5194/acp-18-2225-2018⟩. ⟨hal-01819360⟩
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