A model for particle formation and growth in the atmosphere with molecular resolution in size

International audienceThe formation and growth of atmospheric aerosol particles is considered using an exact discrete method with molecular resolution in size space. The method is immune to numerical diffusion problems that are a nuisance for typical simulation methods using a sectional representation for the particle size distribution. For condensational growth, a slight modification is proposed for the Fuchs-Sutugin expression, which improves the prediction of the growth rate of nano-sized particles by as much as a factor of two. The presented method is applied to particle formation in a Finnish Boreal forest and is shown to capture the essential features of the dynamics quite nicely. Furthermore, it is shown that the growth of the particles is roughly linear, which means that the amount of condensable vapour is constant (of the order 1013 1/m3)

Using discriminant analysis as a nucleation event classification method

More than three years of measurements of aerosol size-distribution and different gas and meteorological parameters made in Po Valley, Italy were analysed for this study to examine which of the meteorological and trace gas variables effect on the emergence of nucleation events. As the analysis method, we used discriminant analysis with non-parametric Epanechnikov kernel, included in non-parametric density estimation method. The best classification result in our data was reached with the combination of relative humidity, ozone concentration and a third degree polynomial of radiation. RH appeared to have a preventing effect on the new particle formation whereas the effects of O₃ and radiation were more conductive. The concentration of SO₂ and NO₂ also appeared to have significant effect on the emergence of nucleation events but because of the great amount of missing observations, we had to exclude them from the final analysis

Multicomponent aerosol dynamics model UHMA: model development and validation

A size-segregated aerosol dynamics model UHMA (University of Helsinki Multicomponent Aerosol model) was developed for studies of multicomponent tropospheric aerosol particles. The model includes major aerosol microphysical processes in the atmosphere with a focus on new particle formation and growth; thus it incorporates particle coagulation and multicomponent condensation, applying a revised treatment of condensation flux onto free molecular regime particles and the activation of nanosized clusters by organic vapours (Nano-Köhler theory), as well as recent parameterizations for binary H₂SO₄-H₂O and ternary H₂SO₄-NH₃-H₂O homogeneous nucleation and dry deposition. The representation of particle size distribution can be chosen from three sectional methods: the hybrid method, the moving center method, and the retracking method in which moving sections are retracked to a fixed grid after a certain time interval. All these methods can treat particle emissions and atmospheric transport consistently, and are therefore suitable for use in large scale atmospheric models. In a test simulation against an accurate high resolution solution, all the methods showed reasonable treatment of new particle formation with 20 size sections although the hybrid and the retracking methods suffered from artificial widening of the distribution. The moving center approach, on the other hand, showed extra dents in the particle size distribution and failed to predict the onset of detectable particle formation. In a separate test simulation of an observed nucleation event, the model captured the key qualitative behaviour of the system well. Furthermore, its prediction of the organic volume fraction in newly formed particles, suggesting values as high as 0.5 for 3–4 nm particles and approximately 0.8 for 10 nm particles, agrees with recent indirect composition measurements

Cluster activation theory as an explanation of the linear dependence between formation rate of 3nm particles and sulphuric acid concentration

International audienceAccording to atmospheric observations new particle formation seems to be a function of sulphuric acid concentration to the power from one to two. The nucleation theorem then predicts that the critical cluster contains one to two sulphuric acid molecules. However, existing nucleation theories predicts that the power is more (or equal) than 2. Here we present an activation theory, which can explain the observed slope. In cluster activation the clusters containing one sulphuric acid molecule will activate for further growth due to heterogeneous nucleation, heterogeneous chemical reactions including polymerization or activation of soluble clusters. In the activation process organic vapours are typically needed as condensing agents

Why formation rate of 3 nm particles depends linearly on sulphuric acid concentration?

International audienceAccording to atmospheric observations new particle formation seems to be a function of sulphuric acid concentration to the power from one to two. The nucleation theorem then predicts that the critical cluster contains one to two sulphuric acid molecules. However, existing nucleation theories predicts that the power is more (or equal) than 2. Here we present an activation theory, which can explain the observed slope. In cluster activation the clusters containing one sulphuric acid molecule will activate for further growth due to heterogeneous nucleation, heterogeneous chemical reactions including polymerization or activation of soluble clusters. In the activation process organic vapours are typically needed as condensing agents

A case study on biomass burning aerosols: effects on aerosol optical properties and surface radiation levels

In spring 2006, biomass burning aerosols from eastern Europe were transported extensively to Finland, and to other parts of northern Europe. They were observed as far as in the European Arctic. In the first part of this paper, temporal and spatial evolution and transport of these biomass burning aerosols are monitored with MODIS retrieved aerosol optical depth (AOD) imagery at visible wavelengths (0.55 μm). Comparison of MODIS and AERONET AOD is conducted at Tõravere, Estonia. Then trajectory analyses, as well as MODIS Fire Mapper products are used to better understand the type and origin of the air masses. During the studied four-week period AOD values ranged from near zero up to 1.2 at 0.55 μm and the linear correlation between MODIS and AERONET was very high (~0.97). Temporal variability observed within this four-week period was also rather well explained by the trajectory analysis in conjunction with the fire detections produced by the MODIS Rapid Response System. In the second part of our study, the surface measurements of global and UV radiation at Jokioinen, Finland are used to study the effect of this haze episode on the levels of surface radiation. We found reductions up to 35% in noon-time surface UV irradiance (at 340 nm) as compared to typical aerosol conditions. For global (total solar) radiation, the reduction was always smaller, in line with the expected wavelength dependence of the aerosol effect

A case study on long-range transported aerosols of biomass burning: effects on aerosol optical properties and surface radiation levels

International audienceIn spring 2006, biomass burning aerosols from eastern Europe were transported extensively to Finland, and to other parts of northern Europe. They were observed as far as in the European Arctic. In the first part of this paper, temporal and spatial evolution and transport of these biomass burning aerosols are monitored with MODIS retrieved aerosol optical depth (AOD) imagery at visible wavelengths (0.55 ?m). Comparison of MODIS and AERONET AOD is conducted at Tõravere, Estonia. Then trajectory analyses, as well as MODIS Fire Mapper products are used to better understand the type and origin of the air masses. During the studied four-week period AOD values ranged from near zero up to 1.2 at 0.55 ?m and the linear correlation between MODIS and AERONET was very high (~0.97). Temporal variability observed within this four-week period was also rather well explained by the trajectory analysis in conjunction with the fire detections produced by the MODIS Rapid Response System. In the second part of our study, the surface measurements of global and UV radiation at Jokioinen, Finland are used to study the effect of this haze episode on the levels of surface radiation. We found reductions up to 35% in surface UV irradiance (at 340 nm) as compared to typical aerosol conditions. For global (total solar) radiation, the reduction was always smaller, in line with the expected wavelength dependence of the aerosol effect

On the hygroscopic growth of ammoniated sulfate particles of non-stoichiometric composition

International audienceThe hygroscopic growth of ammoniated sulfate particles was studied by measurements and model calculations for particles with varying ammonium-to-sulfate ratio. In the measurements, the ammonium-to-sulfate ratio was adjusted by using mixtures of ammonium sulfate and ammonium bisulfate in generating the solid particles. The hygroscopic growth was measured using a tandem differential mobility analyzer. The measurements were simulated using a thermodynamical equilibrium model. The calculations indicated that the solid phases in particle with ammonium-to-sulfate ratio between 1.5?2, were ammonium sulfate and letovicite. Both in the calculations and in the experiments the hygroscopic growth was initiated at relative humidities less than the theoretical deliquescence relative humidity of these particles. This indicates that the particles were multi-phase particles including solids and liquids. The equilibrium model yielded a satisfactory prediction of the hygroscopic growth of particles generated from a solution with 1:1 mass ratio between dissolved ammonium sulfate and ammonium bisulfate. However, for particles with 3:1 and 10:1 mass ratios, the model predictions overestimated the growth at relative humidities between about 60% and the point of complete deliquescence (close to 80% RH). In contrast, a model, in which letovicite was allowed to dissolve only after complete dissolution of ammonium sulfate, reproduced the observations well. This indicates that the dry particles had a letovicite core surrounded by an ammonium sulfate shell

CCN activation and cloud processing in simplified sectional aerosol models with low size resolution

International audienceWe investigate the influence of low size resolution, typical to sectional aerosol models in large scale applications, on cloud droplet activation and cloud processing of aerosol particles. A simplified cloud scheme with five approaches to determine the fraction of activated particles is compared with a detailed reference model under different atmospheric conditions. In general, activation approaches which assume a distribution profile within the critical model size sections predict the cloud droplet concentration most accurately under clean and moderately polluted conditions. In such cases, the deviation from the reference simulations is below 15% except for very low updraft velocities. In highly polluted cases, the concentration of cloud droplets is significantly overestimated due to the inability of the simplified scheme to account for the kinetic limitations of the droplet growth. Of the profiles examined, taking into account the local shape of the particle size distribution is the most accurate although in most cases the shape of the profile has little relevance. While the low resolution cloud model cannot reproduce the details of the out-of-the-cloud aerosol size distribution, it captures well the amount of sulphate produced in aqueous-phase reactions as well as the distribution of the sulphate between the cloud droplets. Overall, the simplified cloud scheme with low size resolution performs well for clean and moderately polluted regions that cover most of the Earth's surface and is therefore suitable for large scale models