The effect of hygroscopicity on cloud droplet formation

Kulmala, M; Korhonen, P; Vesala, T; Hansson, HC; Noone, K; Svenningsson, B
1996 | Tellus B Chem Phys Meteorol | 48 (3) (347-360)
aerosols , albedo , condensation , growth , nitric acid , parameterization , radiation , scattering , temperature , water

The effects of particle hygroscopicity and the availability of condensable material (other than water) in the gas phase on cloud droplet formation and the radiative properties of clouds have been studied using an adiabatic air parcel model with detailed multicomponent condensation. The pre-existing log-normal particle distribution used is bimodal in size and bimodal in hygroscopicity. To simulate this, four log-normal distributions were used and in each mode particles were assumed to be internally mixed, i.e., they are composed partly of salt and partly of an insoluble substance. The mean diameters, standard deviations, total number of pre-existing particles, the mass fraction of the soluble salt and initial concentration of condensable vapour were varied in the simulations. There is a clear effect of hygroscopicity on the activated fraction of aerosol particles in our simulations. Thus hygroscopicity of pre-existing aerosol particles and concentrations of condensable gases can also influence the optical thickness and reflectance of clouds. The change in optical thickness varies as a function of the number concentration of pre-existing particles, having a maximum (Delta tau/tau = 0.2) near a concentration of 1000/cc.

HYGROSCOPIC GROWTH OF AEROSOL-PARTICLES AND ITS INFLUENCE ON NUCLEATION SCAVENGING IN-CLOUD – EXPERIMENTAL RESULTS FROM KLEINER-FELDBERG

SVENNINGSSON, B; HANSSON, HC; WIEDENSOHLER, A; NOONE, K; OGREN, J; HALLBERG, A; COLVILE, R
1994 | J Atmos Chem | 19 (1-2) (129-152)
aerosol-particles , ccn , cloud , hygroscopic growth , scavenging , tandem differential mobility analyzer , tdma

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 less than or equal to 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.

COMPUTER MODELING OF CLOUDS AT KLEINER-FELDBERG

COLVILE, RN; SANDER, R; CHOULARTON, TW; BOWER, KN; INGLIS, DWF; WOBROCK, W; SCHELL, D; SVENNINGSSON, IB; WIEDENSOHLER, A; HANSSON, HC; HALLBERG, A; OGREN, JA; NOONE, KJ; FACCHINI, MC; FUZZI, S; ORSI, G; ARENDS, BG; WINIWARTER, W; SCHNEIDER, T; BERNER, A
1994 | J Atmos Chem | 19 (1-2) (189-229)
aerosols , air-flow model , cloud chemistry , cloud microphysics , cloud model , cloud water acidity , entrainment , flow , gce , henrys law , hills , kleiner-feldberg , marine , mixing , nitric acid , scavenging , turbulence

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 Henry's 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.

THE KLEINER-FELDBERG CLOUD EXPERIMENT 1990 – AN OVERVIEW

WOBROCK, W; SCHELL, D; MASER, R; JAESCHKE, W; GEORGII, HW; WIEPRECHT, W; ARENDS, BG; MOLS, JJ; KOS, GPA; FUZZI, S; FACCHINI, MC; ORSI, G; BERNER, A; SOLLY, I; KRUISZ, C; SVENNINGSSON, IB; WIEDENSOHLER, A; HANSSON, HC; OGREN, JA; NOONE, KJ; HALLBERG, A; PAHL, S; SCHNEIDER, T; WINKLER, P; WINIWARTER, W; COLVILE, RN; CHOULARTON, TW; FLOSSMANN, AI; BORRMANN, S
1994 | J Atmos Chem | 19 (1-2) (3-35)
chemistry , cloud chemistry and microphysics , dependence , droplets , orographic clouds , particles , size

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.

MICROPHYSICS OF CLOUDS AT KLEINER-FELDBERG

ARENDS, BG; KOS, GPA; MASER, R; SCHELL, D; WOBROCK, W; WINKLER, P; OGREN, JA; NOONE, KJ; HALLBERG, A; SVENNINGSSON, IB; WIEDENSOHLER, A; HANSSON, HC; BERNER, A; SOLLY, I; KRUISZ, C
1994 | J Atmos Chem | 19 (1-2) (59-85)
cloud , cumulus , droplet size distribution , entrainment , microphysics

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 mu m 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).

Small crystals in cirrus clouds: their residue sized distribution, cloud water content and realted cloud properties.

Ström, J.; Heintzenberg, J.; Noone, K.J.; Noone, K.B.; Ogren, J.A.; Albers, F. & Quante
1994 | Atmos. Res. | 32 (125-141)

PHASE PARTITIONING OF AEROSOL-PARTICLES IN CLOUDS AT KLEINER-FELDBERG

HALLBERG, A; NOONE, KJ; OGREN, JA; SVENNINGSSON, IB; FLOSSMANN, A; WIEDENSOHLER, A; HANSSON, HC; HEINTZENBERG, J; ANDERSON, TL; ARENDS, BG; MASER, R
1994 | J Atmos Chem | 19 (1-2) (107-127)
aerosol-particles , cloud , cvi , droplet , efficiency , fog , nucleation , partitioning , scavenging , size , sulfate

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.

In-situ observations of cirrus cloud michrophysical properties using the counterflow virtual impactor.

Noone, K.B.; Noone, K.J.; Heintzenberg, J.; Ström, J.; Ogren
1993 | J. Atmos. Ocean. Technol. | 10 (294-303)

Changes in aerosol size and phase distributions due to physical and chemical processes in fog.

Noone, K.J.; Ogren, J.A.; Hallberg, A.; Heintzenberg, J.; Ström, J.; Hansson, H.-C.; Svenningsson, I.B.; Wiediensohler, A.; Fuzzi, S.; Facchini, M.C.; Arends, B.G.; Berner, A.
1992 | Tellus | 44B (489-504)

THE PO VALLEY FOG EXPERIMENT 1989 – AN OVERVIEW

FUZZI, S; FACCHINI, MC; ORSI, G; LIND, JA; WOBROCK, W; KESSEL, M; MASER, R; JAESCHKE, W; ENDERLE, KH; ARENDS, BG; BERNER, A; SOLLY, I; KRUISZ, C; REISCHL, G; PAHL, S; KAMINSKI, U; WINKLER, P; OGREN, JA; NOONE, KJ; HALLBERG, A; FIERLINGEROBERLINNINGER, H; PUXBAUM, H; MARZORATI, A; HANSSON, HC; WIEDENSOHLER, A; SVENNINGSSON, IB; MARTINSSON, BG; SCHELL, D; GEORGII, HW
1992 | Tellus B Chem Phys Meteorol | 44 (5) (448-468)

An outline is presented here of the Po Valley Fog Experiment 1989, carried out within the EUROTRAC-GCE project. This experiment is a joint effort by several European research groups from 5 countries. The physical and chemical behaviour of the fog multiphase system was studied experimentally following the temporal evolution of the relevant chemical species in the different phases (gas, droplet, interstitial aerosol) and the evolution of micrometeorological and microphysical conditions, from the pre-fog situation through the whole fog evolution, to the post-fog period. Some general results, useful for describing the general features of the fog system, are presented here, while specific scientific questions on the different processes taking place within the system itself will be addressed in other companion papers of this same issue.

PHASE PARTITIONING FOR DIFFERENT AEROSOL SPECIES IN FOG

HALLBERG, A; OGREN, JA; NOONE, KJ; HEINTZENBERG, J; BERNER, A; SOLLY, I; KRUISZ, C; REISCHL, G; FUZZI, S; FACCHINI, MC; HANSSON, HC; WIEDENSOHLER, A; SVENNINGSSON, IB
1992 | Tellus B Chem Phys Meteorol | 44 (5) (545-555)

Simultaneous measurements of several non-volatile species in unscavenged aerosol particles and in fog droplets have revealed differences in partitioning for different chemical species. The average scavenged fraction of sulphate was 18 % and the corresponding fraction of elemental carbon was only 6 %. This suggests that the aerosol was externally mixed, and that the chemical mixture of the aerosol as a function of size is important in the context of nucleation scavenging. The measurements obtained could not distinguish between the two primary hypotheses for explaining the observed differences, (a) that the particles had the same size distribution and their chemical composition was the controlling factor, and (b) that the elemental carbon was associated with smaller particles than the sulphate, so that the difference in scavenging efficiency was controlled by the size distribution of the particles.

HYGROSCOPIC GROWTH OF AEROSOL-PARTICLES IN THE PO VALLEY

SVENNINGSSON, IB; HANSSON, HC; WIEDENSOHLER, A; OGREN, JA; NOONE, KJ; HALLBERG, A
1992 | Tellus B Chem Phys Meteorol | 44 (5) (556-569)

A Tandem Differential Mobility Analyser (TDMA) was used to study the hygroscopic growth of individual ambient aerosol particles in the Po Valley, Italy. The measurements were made during the GCE fog experiment in November 1989. During fog, the interstitial aerosol (D(p)(at ambient relative humidity) < 5 mum) was sampled. Two modes of particles with different hygroscopic growth were found for 0.030 mum < D(p)(dry) < 0.20 mum. On average, the fraction of particles in the two modes were almost equal. The mean growth factor at 85% r.h. was 1.44 +/- 0.14 for the more-hygroscopic mode and 1. 1 +/- 0.07 for the less-hygroscopic mode. The growth factors and the proportion of the particles that were less hygroscopic varied considerably from day to day, but no significant size dependence was seen. Comparison of growth factors for pure salt particles and the measured growth factors indicates that both hygroscopic modes contain a major insoluble part. The effect of the external mixing of hygroscopic properties on the activation of particles to fog droplets is discussed and the fraction of particles that were activated as a function of particle size is predicted. Comparison with the measured scavenging fraction as a function of particle size shows that the hygroscopic properties of the individual particle are as important as the particle size in determining if it will be activated in a fog.

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