The influence of aerosol particle composition on cloud droplet formation

A difference in partitioning between cloud droplets and interstitial air for two chemical species (elemental carbon and sulphur) with different expected behaviour in nucleation scavenging was observed in clouds at Mt. Kleiner Feldberg (825 m asl), near Frankfurt, Germany. The fraction of sulphur incorporated in cloud droplets was always higher than the fraction of elemental carbon. This difference in partitioning has also been observed in fog but under different pollution conditions in the Po Valley, Italy. Both these studies were based on bulk samples. In the present study at Kleiner Feldberg, impactor samples of the particles in the interstitial air and the cloud droplet residuals were taken and a single particle analysis was done on the samples. It was found that, for a given particle size, the majority of particles forming cloud droplets were soluble and that insoluble particles preferentially remained in the interstitial air.     

The Cloud Ice Mountain Experiment (CIME) 1998: experiment overview and modelling of the microphysical processes during the seeding by isentropic gas expansion

The second field campaign of the Cloud Ice Mountain Experiment (CIME) project took place in February 1998 on the mountain Puy de Dôme in the centre of France. The content of residual aerosol particles, of H₂O₂ and NH₃ in cloud droplets was evaluated by evaporating the drops larger than 5 μm in a Counterflow Virtual Impactor (CVI) and by measuring the residual particle concentration and the released gas content. The same trace species were studied behind a round jet impactor for the complementary interstitial aerosol particles smaller than 5 μm diameter. In a second step of experiments, the ambient supercooled cloud was converted to a mixed phase cloud by seeding the cloud with ice particles by the gas release from pressurised gas bottles. A comparison between the physical and chemical characteristics of liquid drops and ice particles allows a study of the fate of the trace constituents during the presence of ice crystals in the cloud.In the present paper, an overview is given of the CIME 98 experiment and the instrumentation deployed. The meteorological situation during the experiment was analysed with the help of a cloud scale model. The microphysics processes and the behaviour of the scavenged aerosol particles before and during seeding are analysed with the detailed microphysical model ExMix. The simulation results agreed well with the observations and confirmed the assumption that the Bergeron–Findeisen process was dominating during seeding and was influencing the partitioning of aerosol particles between drops and ice crystals. The results of the CIME 98 experiment give an insight on microphysical changes, redistribution of aerosol particles and cloud chemistry during the Bergeron–Findeisen process when acting also in natural clouds.     

Behaviour of H2O2, NH3, and black carbon in mixed-phase clouds during CIME

We investigated the partitioning of trace substances during the phase transition from supercooled to mixed-phase cloud induced by artificial seeding. Simultaneous determination of the concentrations of H₂O₂, NH₃ and black carbon (BC) in both condensed and interstitial phases with high time resolution showed that the three species undergo different behaviour in the presence of a mixture of ice crystals and supercooled droplets. Both H₂O₂ and NH₃ are efficiently scavenged by growing ice crystals, whereas BC stayed predominantly in the interstitial phase. In addition, the scavenging of H₂O₂ is driven by co-condensation with water vapour onto ice crystals while NH₃ uptake into the ice phase is more efficient than co-condensation alone. The high solubility of NH₄⁺ in the ice could explain this result. Finally, it appears that the H₂O₂–SO₂ reaction is very slow in the ice phase with respect to the liquid phase. Our results are directly applicable for clouds undergoing limited riming.     

A New Tethered Balloon-Borne Payload for Fine-Scale Observations in the Cloudy Boundary Layer

A new scientific payload is introduced for fine-scale measurements of meteorological (wind vector, static air temperature, humidity, and air pressure) and microphysical (aerosol particles and cloud droplets) properties, suspended below a tethered balloon. The high resolution sensors and the tethered balloon are described. Measurements in a lifted fog layer from a first field campaign are presented.The detailed investigation of the fog/haze and the temperature inversion layer demonstrates the damping influence of the fog on temperature fluctuations, while thewind fluctuations are significantly decreased by theevolving temperature inversion, whichwas about 30 m above the fog layer.From spectral analysis the noise floors of the high-resolution sensors are determined to10^-6 kg m^-3 for the LWC (liquid water content) and 4 mK for the fast temperature sensor (UFT-B). The correlation betweentemperature and LWC structures in shallow haze layers is investigated. The release of latent heat and the corresponding warming in the haze of about 0.1 K could be quantified.     

On the distribution of physical and chemical particle properties in the atmospheric aerosol

Consideration of sources and growth dynamics of aerosols has led to the conclusion that there may be a distribution or variation of chemical composition and physical structure among atmospheric aerosol particles as a function of size, and within a narrow size range as well. A mathematical representation of these particle properties in terms of an additional dimension to the number size distribution is described. Examples of the relevance of this aspect of aerosol characterization for physical and chemical processes in the atmosphere are discussed. A review of the available techniques shows that several methods are available which can and have provided quantitative results on the distribution of particle properties. Examples of data from the literature have been selected and are presented as three-dimensional distributions illustrating the wide range of particle properties which may exist in narrow size intervals. An evaluation of these results reiterates the value of taking the distribution of particle properties in the atmosphere into account for sampling and modeling purposes.     

Phase partitioning of aerosol particles in clouds at Kleiner Feldberg

The partitioning of aerosol particles between cloud droplets and interstitial air by number and volume was determined both in terms of an integral value and as a function of size for clouds on Mt. Kleiner Feldberg (825 m asl), in the Taunus Mountains north-west of Frankfurt am Main, Germany. Differences in the integral values and the size dependent partitioning between two periods during the campaign were observed. Higher number and volume concentrations of aerosol particles in the accumulation mode were observed during Period II compared to Period I. In Period I on average 87±11% (±one standard deviation) and 73±7% of the accumulation mode volume and number were incorporated into cloud droplets. For Period II the corresponding fractions were 42±6% and 12±2% in one cloud event and 64±4% and 18±2% in another cloud event. The size dependent partitioning as a function of time was studied in Period II and found to have little variation. The major processes influencing the partitioning were found to be nucleation scavenging and entrainment.     

Changes of cloud microphysical properties during the transition from supercooled to mixed-phase conditions during CIME

A ground-based seeding experiment using carbon dioxide and propane sprayed from pressurized bottles was carried out under supercooled cloud conditions on a small spatial and short time scale. Water vapor deposition on the artificially generated dry ice and propane ice germs as the main ice formation process (nucleation and growth) is consistent with the experimental results. After nucleation, diffusional growth of the ice particles, partly at the expense of evaporating small droplets, was identified during the mixing of the seeding line with the ambient supercooled cloud. Within the seeding plume, ice water contents up to 80% of the total condensed water are observed, although the size of the formed ice particles did not exceed 25 μm. From the changes of the ice and supercooled liquid phase with time under mixed-phase conditions, liquid water content (LWC) evaporation, ice water content (IWC) formation, and ice crystal growth rates are estimated, which are not affected by the artificial nucleation process. Thus, these rates are assessed to be applicable for a growing ice phase of small ice particles in a young mixed-phase cloud, where other growth mechanisms, like riming or aggregation, are negligible.