Cell Model of In-cloud Scavenging of Highly Soluble Gases

We investigate mass transfer during absorption of highly soluble gases such as HNO_{3}, H_{2}O_{2} by stagnant cloud droplets in the presence of inert admixtures. Thermophysical properties of the gases and liquids are assumed to be constant. Diffusion interactions between droplets, caused by the overlap of depleted of soluble gas regions around the neighboring droplets, are taken into account in the approximation of a cellular model of a gas-droplet suspension whereby a suspension is viewed as a periodic structure consisting of the identical spherical cells with periodic boundary conditions at the cell boundary. Using this model we determined temporal and spatial dependencies of the concentration of the soluble trace gas in a gaseous phase and in a droplet and calculated the dependence of the scavenging coefficient on time. It is shown that scavenging of highly soluble gases by cloud droplets leads to essential decrease of soluble trace gas concentration in the interstitial air. We found that scavenging coefficient for gas absorption by cloud droplets remains constant and sharply decreases only at the final stage of absorption. In the calculations we employed gamma size distribution of cloud droplets. It was shown that despite of the comparable values of Henry's law constants for the hydrogen peroxide (H2O2) and the nitric acid (HNO3), the nitric acid is scavenged more effectively by cloud than the hydrogen peroxide due to a major affect of the dissociation reaction on HNO3 scavenging.Comment: 28 pages, including 11 Figures, 1 Tabl

Numerical quantification of sources and phase partitioning of chemical species in cloud: Application to wintertime anthropogenic air masses at the Puy de Dôme station

International audienceThe Model of Multiphase Cloud Chemistry M2C2 has recently been extended to account for nucleation scavenging of aerosol particles in the cloud water chemical composition. This extended version has been applied to multiphase measurements available at the Puy de Dôme station for typical wintertime anthropogenic air masses. The simulated ion concentrations in cloud water are in reasonable agreement with the experimental data. The analysis of the sources of the chemical species in cloud water shows an important contribution from nucleation scavenging of particles which prevails for nitrate, sulphate and ammonium. Moreover, the simulation shows that iron, which comes only from the dissolution of aerosol particles in cloud water, has a significant contribution in the hydroxyl radical production. Finally, the simulated phase partitioning of chemical species in cloud are compared with measurements. Numerical results show an underestimation of interstitial particulate phase fraction with respect to the measurements, which could be due to an overestimation of activated mass by the model. However, the simulated number scavenging efficiency of particles agrees well with the measured value of 40% of total number of aerosol particles activated in cloud droplets. Concerning the origin of chemical species in cloud water, the model reproduces quite well the contribution of gas and aerosol scavenging estimated from measurements. In addition, the simulation provides the contribution of in-cloud chemical reactivity to cloud water concentrations

Effect of mixed-phase cloud on the chemical budget of trace gases: A modeling approach

International audienceA multiphase cloud chemistry model coupling a detailed chemical reactivity mechanism in gas phase and aqueous phase to a cloud parcel model with a two-moment microphysical scheme has been extended to include ice phase processes. This newly developed model is used to study the influence of the ice phase on HCOOH, HNO3, H2O2 and CH2O in a mixed-phase cloud. Microphysical processes are describing the interactions between the water vapor phase, the liquid phase (cloud and rain water) and the ice phase (pristine ice, snow and graupel) in the cloud and for soluble chemical species, their transfer by mixed-phase microphysical processes has been included. In addition to microphysical transfer between iced hydrometeors, the probable two main processes incorporating soluble chemical species in iced hydrometeors are the retention in ice phase as riming or freezing occurs and the burial in the ice crystal as the crystal grows by vapor diffusion. The model is applied to a cloud event describing a moderate precipitating mixed-phase cloud forming in a continental air mass in winter. The main features of the cloud are described and the evolution of key chemical species as function of time and temperature is discussed. Sensitivity tests are performed: a run without ice to highlight the influence of ice phase on the chemical gas phase composition of the cloud, a run without burial showing that it is a negligible process, a run assuming full retention in ice for all species and a run varying the ice crystal shapes. A detailed analysis of the microphysical rates and chemical rates linked to retention and burial effects show that for this cloud event, the effect of the ice phase on gas phase composition is driven by riming of cloud droplets onto graupels, which leads to retention or not of soluble chemical species in the ice phase. Finally, the impact of crystal geometry on the efficiency of collection is studied together with its impact on the riming of cloud droplets on graupels and also on the retention of chemical species in ice phase

Potential impact of microbial activity on the oxidant capacity and organic carbon budget in clouds

International audienceWithin cloud water, microorganisms are metabolically active and, thus, are expected to contribute to the atmospheric chemistry. This paper investigates the interactions between microorganisms and the reactive oxygenated species that are present in cloud water because these chemical compounds drive the oxidant capacity of the cloud system. Real cloud water samples with contrasting features (marine, continental and urban) were taken from the puy de Dôme mountain (France). The samples exhibited a high microbial biodiversity and complex chemical composition. The media were incubated in the dark and subjected to UV radiation in specifically designed photo-bioreactors. The concentrations of H2O2, organic compounds and the ATP/ADP ratio were monitored during the incubation period. The microorganisms remained metabolically active in the presence of *OH radicals that were photo-produced from H2O2. This oxidant and major carbon compounds (formaldehyde and carboxylic acids) were biodegraded by the endogenous microflora. This work suggests that microorganisms could play a double role in atmospheric chemistry; first, they could directly metabolize organic carbon species, and second, they could reduce the available source of radicals through their oxidative metabolism. Consequently, molecules such as H2O2 would no longer be available for photochemical or other chemical reactions, which would decrease the cloud oxidant capacity

Microbiology and atmospheric processes: chemical interactions of primary biological aerosols

This paper discusses the influence of primary biological aerosols (PBA) on atmospheric chemistry and vice versa through microbiological and chemical properties and processes. Several studies have shown that PBA represent a significant fraction of air particulate matter and hence affect the microstructure and water uptake of aerosol particles. Moreover, airborne micro-organisms, namely fungal spores and bacteria, can transform chemical constituents of the atmosphere by metabolic activity. Recent studies have emphasized the viability of bacteria and metabolic degradation of organic substances in cloud water. On the other hand, the viability and metabolic activity of airborne micro-organisms depend strongly on physical and chemical atmospheric parameters such as temperature, pressure, radiation, pH value and nutrient concentrations. In spite of recent advances, however, our knowledge of the microbiological and chemical interactions of PBA in the atmosphere is rather limited. Further targeted investigations combining laboratory experiments, field measurements, and modelling studies will be required to characterize the chemical feedbacks, microbiological activities at the air/snow/water interface supplied to the atmosphere

Modeling study of strong acids formation and partitioning in a polluted cloud during wintertime

International audienceA multiphase chemistry model coupled with a quasi-spectral microphysical model has been applied to measurements from the European Cloud Ice Mountain Experiment campaign to quantify the formation of the strong acids nitrate and sulfate and to evaluate the role of microphysical processes in redistributing reactive species among the different phases (gas versus cloud and/or rain). Significant formation of nitrate and sulfate are found to be due to the reaction of pernitric acid with the sulfite ion. Moreover, pernitric acid, because of its equilibrium in the gas phase and its high solubility, is always available both in cloud water and in rainwater via mass transfer from the gas phase. The sulfite ion comes from the mass transfer from the gas phase of sulfur dioxide in cloud water. When rain formation begins, it is efficiently transferred to the rainwater by collision/coalescence processes. This leads to an enhancement in strong acid production when microphysics is activated in the model. Modeled results have been compared with experimental data in an effort to retrieve a behavior law related to the partitioning between the gas and aqueous phases of the cloud. In particular, when collision/coalescence processes are considered, an improvement in retrieving the partitioning of soluble species and especially nitrate is observed. A higher production in sulfate could help interpret the discrepancy of global model calculations with observed sulfate concentrations in Europe in wintertime

Le rôle de l’enseignant sur le renforcement ou la réduction des inégalités filles / garçons en EPS

Ce mémoire a pour objectif d’analyser le renforcement ou la réduction des inégalités filles / garçons par l’enseignant. Ma première partie reprend de nombreuses recherches menées montrant que les filles sont souvent désavantagées en éducation physique et sportive. Mes hypothèses s’appuient sur ces études qui évoquent que l’enseignant a son rôle à jouer dans la réduction de ces inégalités. J’ai donc mené des recherches pour vérifier ces hypothèses en gymnastique, activité connotée féminine où les filles sont susceptibles de réussir autant que les garçons. Les résultats présentés montrent que les garçons reçoivent plus de feedbacks que les filles. Ma conclusion m’amène à penser que l’enseignant doit donc réfléchir à ses interventions pédagogiques pour tendre vers la réduction des différences de traitement des élèves selon leur sexe

Modelisation du transport et de la redistribution des especes chimiques tropospheriques: physicochimie humide a moyenne echelle

SIGLEAvailable from INIST (FR), Document Supply Service, under shelf-number : TD 20452 / INIST-CNRS - Institut de l'Information Scientifique et TechniqueFRFranc