Hans-Christen Hansson

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.

Size distribution of biogenic aerosol particles from the amazon basin

Abstract The size distribution and elemental composition of natural background aerosol particles from the tropical rain forest of the Amazon Basin were measured. A 45 m high tower installed in an undisturbed forest near Manaus was used and aerosol was sampled in three levels of the tower. Single orifice Batelle-type cascade impactors with 5 stages and backup filter were used. A total of 50 complete cascade impactor sets was sampled in April and May 1987, during the wet season, when no forest burning occurs. Particle-induced X-ray emission (PIXE) was used to measure elemental concentrations of 20 elements (Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Br, Rb, Sr, Zr and Pb). Absolute factor analysis was used to interpret the large data set of the trace element concentrations and to obtain quantitative elemental source profiles. The identified components in all size ranges comprise biogenic aerosol naturally released by the forest, mineral dust aerosol particles and sea salt. The elements associated with the biogenic component were potassium, phosphorus, sulphur, zinc, strontium and others in smaller proportions. The mineral dust component comprises most of the concentration of aluminium, silicon, calcium, titanium, manganese and iron. Chlorine was found to be associated with the aeolean dust component because of the long-range transport of Sahara dust over the Atlantic ocean, bringing Cl together with mineral dust particles. The size distribution of the elements associated with the windblown dust (Al, Si, Ca, Ti, Mn, Fe and Cl) shows in the coarse mode, with an average aerodynamic diameter of 4 μm. Two different biogenic aerosol components were observed. A fine mode component (d50 ≈ 0.5 μm), characterised by the the elements S, Zn and Sr and the mode biogenic component (d50 ≈ 3.0 μm) characterised by the presence of P, K, Cl and Sr. The coarse biogenic (P, K, Cl, Sr) component is predominant at ground level under the forest canopy. The fine mode biogenic component (S, Zn, Sr) is higher at the top level of the tower.

Cloud droplet nucleation scavenging in relation to the size and hygroscopic behaviour of aerosol particles

The size distributions and hygroscopic growth spectra of aerosol particles were measured during the GCE cloud experiment at Great Dun Fell in the Pennine Hills in northern England. Hygroscopic growth is defined as the particle diameter at 90% RH divided by the particle diameter at 10% RH. The fraction of the aerosol particles scavenged by cloud droplets as a function of particle size was also measured. The general aerosol type was a mixture of marine and aged anthropogenic aerosols. The Aitken and accumulation mode numbers (average ± 1 S.D.) were 1543 ± 1078 and 1023 ± 682 cm−3 respectively. The mean diameters were in the range 30–100 nm and 100–330 nm. The hygroscopic growth spectra were bimodal about half the time. The less-hygroscopic particles had average growth factors of 1.06, 1.06, 1.03, 1.03, and 1.03 for particle diameters of 50, 75, 110, 165, and 265 nm, respectively. For the more-hygroscopic particles of the same sizes, the average hygroscopic growth was 1.34, 1.37, 1.43, 1.47, and 1.53. The effects of ageing on the aerosol particle size distribution and on hygroscopic behaviour are discussed. The scavenged fraction of aerosol particles was a strong function of particle diameter. The diameter with 50% scavenging was in the range 90–220 nm. No tail of smaller particles activated to cloud drops was observed. A small tail of larger particles that remained in the interstitial aerosol can be explained by there being a small fraction of less-hygroscopic particles. A weak correlation between the integral dry particle diameter and the diameter with 50% scavenging was seen.

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.

Night-time formation and occurrence of new particles associated with orographic clouds

Abstract The formation and occurrence of new ultrafine aerosol particles were studied in association with an orographic cloud during a field experiment at Great Dun Fell (GDF), Northern England. Three size spectrometers to measure submicrometer aerosol particles were located upwind, on top, and downwind of GDF Summit to investigate changes in the aerosol size distribution. During two night-time cloud periods, ultrafine particles were observed downwind of the hill while no particles were detected upwind of the hill. During one cloud event, there was some evidence of entrainment. In this case, the occurrence of ultrafine particles may have been due to entrainment from aloft or by homogenous nucleation downwind of the hill. During the other cloud event, the formation of an ultrafine particle mode (nucleation mode) occurred probably after the cloud passage. There was no evidence of entrainment during this time period. Multicomponent homogeneous nucleation models were used to simulate the formation of new particle downwind of an orographic cloud. Possible homogeneous nucleation processes for this could be the formation of sulphuric acid or ammonium chloride due to outgassing of hydrochloric acid. It was not possible, however, to simulate formation rates of new particles as observed downwind the hill using a model for the binary or ternary homogeneous nucleation process of ammonia and hydrochloric acid. During the first event with high sulphur dioxide concentrations, the formation of new particle via binary homogeneous nucleation of sulphuric acid and water could be only predicted using a high nighttime hydroxyl radical concentration. No formation of sulphuric acid particle could be simulated during the second event with low sulphur dioxide concentrations.

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.

Phase partitioning of aerosol constituents in cloud based on single-particle and bulk analysis

Abstract Single-particle analysis, performed by laser microprobe mass spectrometry and bulk analytical techniques were used to study aerosol-cloud interactions within the third field campaign of the EURO-TRAC subproject “ground-based cloud experiments” at the Great Dun Fell, Cumbria, U.K. in spring 1993. The shape of the ridge made it possible for ground-based instrumentation to sample similar parcels of air before, during and after their transit through the cloud. A single jet five-stage minicascade impactor was used for sampling particles of the interstitial aerosol. A second impactor worked in tandem with a counterflow virtual impactor and collected residues of cloud droplets. Considering marine conditions largest droplets nucleated on sea-salt particles, whereas smaller droplets were formed on sulphate and methane sulphonate containing particles. This clearly indicates chemical inhomogeneities in the droplet phase. Particles, which were disfavoured by droplet formation, often contained the highest amounts of water-insoluble carbonaceous matter. For the submicron size range we found that the carbonaceous matter was always internally mixed with sulphate. The fraction of carbonaceous matter increased with decreasing size. A detectable fraction of particles remained in the cloud interstitial air, although they were in size as well as in composition suitable to form cloud droplets. The findings confirm that nucleation is the most important process affecting phase partitioning in cloud, but that spatial and temporal variations of water vapour supersaturation have also an influence on the observed phase partitioning. Proton induced X-ray emission analysis and light absorption measurements of filter samples showed that the average scavenged fraction was 0.77 for sulphur and 0.57 for soot in clouds formed by continental influenced air and 0.62 and 0.44. respectively, for marine influenced clouds.

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.

The size-dependent chemical composition of cloud droplets

Abstract Size-dependent cloud droplet solute concentrations were measured using a two-stage fog water impactor at the summit station of Great Dun Fell (GDF) in the north of England. The measurements showed mostly higher concentrations in the small-droplet fraction. During one cloud event, however, higher solute concentrations were found in the larger-droplet fraction. In order to identify the factors governing the size dependence of cloud droplet solute concentrations, sensitivity studies by means of a diffusional growth model were performed. The time available for the droplets to grow was identified to be of great importance for the size dependence of solute concentrations. In cases when higher solute concentrations were found in the fraction containing the bigger droplets, the cloud droplets were relatively young having been formed by orographic lifting of the air at the GDF summit. For the other events the evidence indicates that the cloud was already formed far upwind from the summit site. Our experimental and model results imply that, after an initially strong decrease of solute concentrations with droplet size we would observe: • ⊎|increasing solute concentrations with increasing diameters during the initial stage of a cloud, e.g. near cloud base where the droplets have just been formed. The primary factors contributing to this behaviour are high peak supersaturations, large numbers of coarse aerosol particles, and high solubility of the aerosol particles. • ⊎|decreasing solute concentrations with increasing diameters in aged cloud parcels, such as those which can be observed high above the cloud base in cumuliform clouds or are advected to the observation point in the case of stratiform clouds. The primary factors contributing to this behaviour are low peak supersaturations, low numbers of coarse particles, and low solubility of the aerosol particles.

Observations and modelling of the processing of aerosol by a hill cap cloud

Abstract Observations are presented of the aerosol size distribution both upwind and downwind of the Great Dun Fell cap cloud. Simultaneous measurements of the cloud microphysics and cloud chemistry, and of the chemical composition of the aerosol both upwind and downwind of the hill were made along with measurements of sulphur dioxide, hydrogen peroxide and ozone. These observations are used for initialisation of, and for comparison with the predictions of a model of the air flow, cloud microphysics and cloud chemistry of the system. A broad droplet size distribution is often observed near to the hill summit, seemingly produced as a result of a complex supersaturation profile and by mixing between parcels with different ascent trajectories. The model generates several supersaturation peaks as the airstream ascends over the complex terrain, activating increasing numbers of droplets. In conditions where sulphate production in-cloud (due to the oxidation of S(IV) by hydrogen peroxide and ozone) is observed, there is a marked effect on the chemical evolution of the aerosol particles on which the droplets form. When sulphate production occurs, a significant modification of the aerosol size distribution and hygroscopic properties is both predicted and observed. The addition of sulphate mass to those aerosol particles nucleation scavenged by the cloud generally increases the ease with which they are subsequently able to act as cloud condensation nuclei (CCN). Often, this will lead to an increase in the number of CCN available for subsequent cloud formation, although this latter effect is shown to be strongly dependent upon the activation history of the droplets and the concentration of pollutant gases present in the interstitial air. Situations are also identified where cloud processing could lead to a reduction in the capacity of smaller aerosol to act as CCN.