A. Hallberg

Hygroscopic growth of aerosol particles and its influence on nucleation scavenging in cloud: Experimental results from Kleiner Feldberg

The hygroscopic growth of individual aerosol particles has been measured with a Tandem Differential Mobility Analyser. The hygroscopic growth spectra were analysed in terms of diameter change with increasing RH from ≤20% to 85%. The measurements were carried out during the GCE cloud experiment at Kleiner Feldberg, Taunus, Germany in October and November 1990.Two groups of particles with different hygroscopic growth were observed. The less-hygroscopic group had average growth factors of 1.11, 1.04 and 1.02 for particle diameters of 50, 150 and 300 nm, respectively. The more-hygroscopic group had average growth factors of 1.34, 1.34, and 1.37 for the same particle diameters. The average fraction of less-hygroscopic particles was about 50%. Estimates of the soluble fractions of the particles belonging to the two groups are reported.Hygroscopic growth spectra for total aerosol, interstitial aerosol and cloud drop residuals were measured. A comparison of these hygroscopic growths of individual aerosol particles provides clear evidence for the importance of hygroscopic growth in nucleation scavenging. The measured scavenged fraction of particles as a function of diameter can be explained by the hygroscopic growth spectra.

The Kleiner Feldberg Cloud Experiment 1990. An overview

An overview is given of the Kleiner Feldberg cloud experiment performed from 27 October until 13 November 1990. The experiment was carried out by numerous European research groups as a joint effort within the EUROTRAC-GCE project in order to study the interaction of cloud droplets with atmospheric trace constituents. After a description of the observational site and the measurements which were performed, the general cloud formation mechanisms encountered during the experiment are discussed. Special attention is given here to the process of moist adiabatic lifting. Furthermore, an overview is given regarding the pollutant levels in the gas phase, the particulate and the liquid phase, and some major findings are presented with respect to the experimental objectives. Finally, a first comparison attempts to put the results obtained during this campaign into perspective with the previous GCE field campaign in the Po Valley.

The great dun fell cloud experiment 1993: An overview

The 1993 Ground-based Cloud Experiment on Great Dun Fell used a wide range of measurements of trace gases, aerosol particles and cloud droplets at five sites to study their sources and sinks especially those in cloud. These measurements have been interpreted using a variety of models. The conclusions add to our knowledge of air pollution, acidification of the atmosphere and the ground, eutrophication and climate change. The experiment is designed to use the hill cap cloud as a flow-through reactor, and was conducted in varying levels of pollution typical of much of the rural temperate continental northern hemisphere in spring-time.

Experimental evidence for in-cloud production of aerosol sulphate

Abstract The modification of physical and chemical properties of aerosols passing through clouds has received considerable attention over recent years. Some of these transformations are related to in-cloud chemical reactions, particularly the oxidation of sulphur dioxide (SO 2 ) to sulphate (SO 4 2− . The Great Dun Fell experiment provided an opportunity to investigate the connection between the chemistry within cloud droplets and the processing of an aerosol population. We have noted significant increases in SO 4 2− in the aerosol population downstream of the cloud compared to the aerosol entering the cloud. These increases are connected to both S(IV) oxidation in the liquid phase and to the entrainment of new air into the cloud, supplying reactants such as H 2 O 2 to the system. The addition of SO 4 2− mass to the aerosol is also associated with changes in the NH 4 + aerosol concentrations, possibly as a result of neutralisation of the acidified cloud droplets by NH 3 . The study was performed taking into account dynamical mixing of air masses as well as possible sampling artefacts.

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.

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.

Multiphase chemistry and acidity of clouds at Kleiner Feldberg

The chemistry of cloud multiphase systems was studied within the Kleiner Feldberg Cloud Experiment 1990. The clouds encountered during this experimental campaign could be divided into two categories according to the origin of air masses in which the clouds formed. From the chemical point of view, clouds passing the sampling site during the first period of the campaign (26 October-4 November) were characterized by lower pollutant loading and higher pH, as compared to clouds during the final period of the experimental campaign (10–13 November). The study of multiphase partitioning of the main chemical constituents of the cloud systems and of atmospheric acidity within the multiphase systems themselves (gas + interstitial aerosol + liquid droplets) are presented in this paper. A general lack of gaseous NH3 was found in these cloud systems, which caused a lack of buffer capacity toward acid addition. Evidence supports the hypothesis that the higher acidity of the cloud systems during this final period of the campaign was due to input of HNO3. Our measurements, however, could not determine whether the observed input was due to scavenging of gaseous HNO3 from the air feeding into the cloud, or to heterogeneous HNO3 formation via NO2 oxidation by O3 to NO3 and N2O5. Sulfate in cloud droplets mainly originated from aerosol SO42− scavenging, since S(IV) to S(VI) liquid phase conversion was inhibited due to both lack of H2O2 and low pH of cloud droplets, which made O3 and metal catalyzed S(IV) oxidation inefficient.

Microphysics of clouds at Kleiner Feldberg

During a field measuring campaign at Kleiner Feldberg (Taunus) in 1990, microphysical characteristics of clouds have been measured by Forward Scattering Spectrometer Probes (FSSP). The aim was to study the influence of aerosol and meteorological factors on droplet size and number. The results are: More mass in the accumulation size range of the aerosol leads to more droplets in stratocumulus clouds and to higher soluble masses in droplets of stratus clouds. However, the aerosol distribution was coarser in the stratus clouds compared to the stratocumulus clouds. Within the first 200 m from cloud base, the droplets grow while their number decreases. The growth results in a stable size of about 14 µm diameter over a large distance from cloud base in many stratocumulus clouds. Two types of mixing processes were observed: processes with reductions in the number of droplets (inhomogeneous mixing) and with reductions in the size of the droplets (homogeneous mixing).

Computer modelling of clouds at Kleiner Feldberg

The airflow, cloud microphysics and gas- and aqueous-phase chemistry on Kleiner Feldberg have been modelled for the case study of the evening of 1 November 1990, in order to calculate parameters that are not easily measured in the cloud and thus to aid the interpretation of the GCE experimental data-set. An airflow model has been used to produce the updraught over complex terrain for the cloud model, with some care required to ensure realistic modelling of the strong stable stratification of the atmosphere. An extensive set of measurements has been made self-consistent and used to calculate gas and aerosol input parameters for the model. A typical run of the cloud model has calculated a peak supersaturation of 0.55% which occurs about 20 s after entering cloud where the updraught is 0.6 m s−1. This figure has been used to calculate the efficiency with which aerosol particles were scavenged; it is higher than that calculated by other methods, and produces a cloud with slightly too many droplets. A broad cloud droplet size spectrum has been produced by varying the model inputs to simulate turbulent mixing and fluctuations in cloud parameters in space and time, and the ability of mixing processes near cloud-base to produce a lower peak supersaturation is discussed. The scavenging of soluble gases by cloud droplets has been observed and departures from Henrys Law in bulk cloud-water samples seen to be caused by variation of pH across the droplet spectrum and the inability of diffusion to adjust initial distributions of highly soluble substances across the spectrum in the time available. Aqueous-phase chemistry has been found to play a minor role in the cloud as modelled, but circumstances in which these processes would be more important are identified.

Microphysics of clouds: Model vs measurements

Abstract In order to study the relation between the initial aerosol particle spectrum at cloud base and the resulting droplet spectrum in cloud for the “Ground-based Cloud Experiment” field campaign at the Great Dun Fell in 1993 numerical model simulations have been performed. The droplet spectra were calculated from a microphysical model coupled to a dynamic air flow model. The resulting droplet spectra were compared with cloud droplet spectra measured with a forward scattering spectrometer probe. The size distribution and chemical composition of the initial aerosol population were derived from a combination of size distribution and size-segregated chemical measurements below cloud base. From this we concluded that the aerosol particles consisted almost entirely of an inorganic salt. As part of the sensitivity studies two different microphysical models were used, as well as the dynamic flow fields from two different air flow models. As in previous studies we found that the measured droplet spectra were broader and contained larger drops than the modelled spectra. From the sensitivity studies we identified fluctuations in the dynamics as the most likely explanation for these differences.