| 1. |
- Berg, Olle H., et al.
(författare)
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Comparison of observed and modeled hygroscopic behavior of atmospheric particles
- 1998
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Ingår i: Contributions to Atmospheric Physics. - 0005-8173. ; 71:1, s. 47-64
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Forskningsöversikt (refereegranskat)abstract
- The hygroscopic behavior of sub-micrometer atmospheric aerosol particles was studied with a Tandem Differential Mobility Analyzer (TDMA) at a field site in the Po Valley, Italy. The measurements were done in a continental polluted aerosol during the CHEMDROP fog and haze field experiment at San Pietro di Capofiume in November 1994. In this study, hygroscopic diameter growth factors of individual particles were measured when taken from a dry state, to a relative humidity of 90 %. The aerosol consisted of two groups of particles with different hygroscopic properties, as also seen in an earlier field experiment at the same location in 1989 and at other continental sites. The present work is a closure study on the hygroscopic behavior of sub-micrometer aerosol particles and their mass. Ammonium sulfate was used to model the hygroscopic growth with a model based on thermodynamic data for non-ideal aqueous solutions at water vapor subsaturation. The study was made in two steps: The first step is a comparison between hygroscopic active aerosol volume fractions derived from TDMA measurements on individual particles integrated over the particle size distributions, and collected volume fractions of major ions sampled by size resolved cascade impactors. The model of hygroscopic growth was also used, in the second step, to calculate ambient sizes of individual aerosol particles. These sizes were then compared to the actual ambient sizes as measured by the Droplet Aerosol Analyzer. The result shows agreement, within the estimated errors, between the integrated hygroscopic active volume fractions and the collected volume fractions of inorganic salts, for five events out of six studied. A mass balance could also be obtained between the masses collected with the impactors and the integrated volume distributions, by attributing reasonable densities to the hygroscopically active and inactive fractions. The differences between the calculated and measured ambient sizes were within measurement errors, when Raoult's law was used to model the occasions with relative humidities larger than 95 %.
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| 2. |
- Frank, Göran, et al.
(författare)
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Droplet Formation and Growth in Polluted Fogs
- 1998
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Ingår i: Contributions to Atmospheric Physics. - 0005-8173. ; 71:1, s. 65-85
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Tidskriftsartikel (refereegranskat)abstract
- Fog droplet formation and growth related to fog droplet activation were studied in a polluted region. The joint field experiments were carried out at San Pietro Capofiume in northern Italy during November 1994. It was found that the fog droplet number distribution was continuous in the size region 1-47 µm and that for most of the time the fog consisted of unactivated droplets, i.e. the droplets were smaller than the critical diameter for activation according to the Köhler equation. During a few time periods some of the droplets were possibly slightly larger than the critical diameter for activation. The solute concentration in the fog droplets was found to be strongly dependent and decreasing with increasing droplet size. The experimental results were compared with results obtaied using a fog model. Good overall agreement was found between the model and the experimental results, with respect to fog droplet size related to dry residue size, and to fog droplet number distribution. The fog model was also used to study the influence on fog droplet growth of the rate of temperature decrease, the aerosol particle mass load and fog liquid water content. In addition the effect of aging of the fog was also considered.
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| 3. |
- Fuzzi, Sandro, et al.
(författare)
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Overview of the Po valley fog experiment 1994 (CHEMDROP)
- 1998
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Ingår i: Contributions to Atmospheric Physics. - 0005-8173. ; 71:1, s. 3-19
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Forskningsöversikt (refereegranskat)abstract
- The paper presents an outline of the CHEMDROP field experiment, carried out in November 1994 at the field station of S. Pietro Capofiume in the Po Valley, Italy. The main objective of the project was to address the issue of the size-dependent chemical composition of fog droplets, by experimentally investigating the following processes, which are expected to affect (or be affected by) the chemical composition of fog droplets as a function of size: a) the connection of the size-dependent chemical composition of CCN to the size-dependent composition of fog droplets; b) the gas/liquid partitioning of the gaseous species NH3, SO2, HCHO, HNO3 in fog; c) the Fe(II)/Fe(III) redox cycle in fog water. Some general results and overall conclusions of the experiment are reported in this paper, while more specific scientific questions are discussed in other companion papers in this issue. CHEMDROP results show that several processes concur in determining the size-dependence of fog droplets chemical composition: nucleation scavenging of pre-existing CCN, fog dynamical evolution and gas/liquid exchange between interstitial air and fog droplets. Chemical transformations in the liquid phase can cause further changes in the chemical composition of the droplets. Only by taking into account the combination of all these processes, is it possible to explain the inhomogeneities in fog droplet chemical composition.
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| 4. |
- Heintzenberg, Jost, et al.
(författare)
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Characteristics of haze, mist and fog
- 1998
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Ingår i: Contributions to Atmospheric Physics. - 0005-8173. ; 71:1, s. 21-31
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Tidskriftsartikel (refereegranskat)abstract
- An aerosol and fog data set from a field experiment in November 1994 at San Pietro Capofiume, Northern Italy was analysed. With objective criteria developed from visibility measurements average aerosol characteristics in the dry and wet state were calculated for haze, mist and fog conditions which can be seen as representative for continental air masses in an industrialised region. Dry particle size distributions between three and 800 nm and ambient size distributions between and 50 μm were measured with a system consisting of the three size-segregating particle sensors differential mobility particle sizer, droplet aerosol analyser and FSSP. Systematic changes in particle properties were found for the transition from haze to fog that can be used to derive internally consistent optical aerosol properties. The analysis of the data set demonstrates that atmospheric sensors which have been developed for cloud and fog studies yield useful data for haze conditions.
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| 5. |
- Martinsson, Bengt G., et al.
(författare)
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Droplet nucleation and growth in orographic clouds in relation to the aerosol population
- 1999
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Ingår i: Atmospheric Research. - 0169-8095. ; 50:3-4, s. 289-315
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Tidskriftsartikel (refereegranskat)abstract
- The formation and development of orographic clouds was studied in a field experiment comprising several measurement sites at a mountain ridge. The influence of the aerosol population present on the cloud microstructure was studied in relation to the dynamics in the cloud formation. Droplet nucleation scavenging was investigated by the introduction of a non-dimensional particle diameter related to the process, and it was found that the scavenging rose rapidly in a relatively narrow particle size interval. The size dependency of the scavenging could partly be explained by external mixture of the aerosol. The large particles in the cloud interstitial aerosol was found to be of a chemical nature which allows for only a very weak uptake of water, implying that the chemical composition of these particles rather than entrainment of dry air prevented the droplet nucleation. The aerosol particle number concentration was found to strongly influence the cloud microstructure. Droplet number concentrations up to approximately 2000 cm-3 were observed together with a substantially reduced effective droplet diameter. The observed effect of elevated particle number concentrations in orographic clouds was generalised to the climatologically more important stratiform clouds by the use of a cloud model. It was found that the microstructure of stratiform clouds was strongly dependent on the aerosol population present as well on the dynamics in the cloud formation.
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| 6. |
- Schmale, Julia, et al.
(författare)
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Long-term cloud condensation nuclei number concentration, particle number size distribution and chemical composition measurements at regionally representative observatories
- 2018
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:4, s. 2853-2881
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Tidskriftsartikel (refereegranskat)abstract
- Aerosol-cloud interactions (ACI) constitute the single largest uncertainty in anthropogenic radiative forcing. To reduce the uncertainties and gain more confidence in the simulation of ACI, models need to be evaluated against observations, in particular against measurements of cloud condensation nuclei (CCN). Here we present a data set - ready to be used for model validation - of long-term observations of CCN number concentrations, particle number size distributions and chemical composition from 12 sites on 3 continents. Studied environments include coastal background, rural background, alpine sites, remote forests and an urban surrounding. Expectedly, CCN characteristics are highly variable across site categories. However, they also vary within them, most strongly in the coastal background group, where CCN number concentrations can vary by up to a factor of 30 within one season. In terms of particle activation behaviour, most continental stations exhibit very similar activation ratios (relative to particles 20nm) across the range of 0.1 to 1.0% supersaturation. At the coastal sites the transition from particles being CCN inactive to becoming CCN active occurs over a wider range of the supersaturation spectrum. Several stations show strong seasonal cycles of CCN number concentrations and particle number size distributions, e.g. at Barrow (Arctic haze in spring), at the alpine stations (stronger influence of polluted boundary layer air masses in summer), the rain forest (wet and dry season) or Finokalia (wildfire influence in autumn). The rural background and urban sites exhibit relatively little variability throughout the year, while short-term variability can be high especially at the urban site. The average hygroscopicity parameter, calculated from the chemical composition of submicron particles was highest at the coastal site of Mace Head (0.6) and lowest at the rain forest station ATTO (0.2-0.3). We performed closure studies based on -Köhler theory to predict CCN number concentrations. The ratio of predicted to measured CCN concentrations is between 0.87 and 1.4 for five different types of . The temporal variability is also well captured, with Pearson correlation coefficients exceeding 0.87. Information on CCN number concentrations at many locations is important to better characterise ACI and their radiative forcing. But long-term comprehensive aerosol particle characterisations are labour intensive and costly. Hence, we recommend operating migrating-CCNCs to conduct collocated CCN number concentration and particle number size distribution measurements at individual locations throughout one year at least to derive a seasonally resolved hygroscopicity parameter. This way, CCN number concentrations can only be calculated based on continued particle number size distribution information and greater spatial coverage of long-term measurements can be achieved.
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| 7. |
- Swietlicki, Erik, et al.
(författare)
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Hygroscopic properties of aerosol particles in the northeastern Atlantic during ACE-2
- 2000
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Ingår i: Tellus. Series B: Chemical and Physical Meteorology. - : Stockholm University Press. - 0280-6509 .- 1600-0889. ; 52:2, s. 201-227
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Tidskriftsartikel (refereegranskat)abstract
- Measurements of the hygroscopic properties of sub-micrometer atmospheric aerosol particles were performed with hygroscopic tandem differential mobility analysers (H-TDMA) at 5 sites in the subtropical north-eastern Atlantic during the second Aerosol Characterization Experiment (ACE-2) from 16 June to 25 July 1997. Four of the sites were in the marine boundary layer and one was, at least occasionally, in the lower free troposphere. The hygroscopic diameter growth factors of individual aerosol particles in the dry particle diameter range 10-440 nm were generally measured for changes in relative humidity (RH) from <10% to 90%. In the marine boundary layer, growth factors at 90% RH were dependent on location, air mass type and particle size. The data was dominated by a unimodal growth distribution of more-hygroscopic particles, although a bimodal growth distribution including less-hygroscopic particles was observed at times, most often in the more polluted air masses. In clean marine air masses the more-hygroscopic growth factors ranged from about 1.6 to 1.8 with a consistent increase in growth factor with increasing particle size. There was also a tendency toward higher growth factors as sodium to sulphate molar ratio increased with increasing sea-salt contribution at higher wind speeds. During outbreaks of European pollution in the ACE-2 region, the growth factors of the largest particles were reduced, but only slightly. Growth factors at all sizes in both clean and polluted air masses were markedly lower at the Sagres, Portugal site due to more proximate continental influences. The frequency of occurrence of less-hygroscopic particles with a growth factor of ca. 1.15 was greatest during polluted conditions at Sagres. The free tropospheric 50 nm particles were predominately less-hygroscopic, with an intermediate growth factor of 1.4, but more-hygroscopic particles with growth factors of about 1.6 were also frequent. While these particles probably originate from within the marine boundary layer, the less-hygroscopic particles are probably more characteristic of lower free tropospheric air masses. For those occasions when measurements were made at 90% and an intermediate 60% or 70% RH, the growth factor G(RH) of the more-hygroscopic particles could be modelled empirically by a power law expression. For the ubiquitous more-hygroscopic particles, the expressions G(RH) = (1 - RH/100)-0.210 for 50 nm Aitken mode particles and G(RH) = (1 - RH/100)-0.233 for 166 nm accumulation mode particles are recommended for clean marine air masses in the north-eastern Atlantic within the range 0 < RH < 95%, and for wind speeds for which the local sea-salt production is small (< ca. 8 m s-1).
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| 8. |
- Yuskiewicz, Brett A., et al.
(författare)
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Changes in submicrometer particle distributions and light scattering during haze and fog events in a highly polluted environment
- 1998
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Ingår i: Contributions to Atmospheric Physics. - 0005-8173. ; 71:1, s. 33-45
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Tidskriftsartikel (refereegranskat)abstract
- The changes in submicrometer atmospheric particle size distributions measured with a Differential Mobility Particle Sizer (DMPS) system during a polluted fog experiment during November, 1994 are presented in this study. Results reveal three modes commonly evident in the size distribution (3 < DN < 843 nm) measurements; the ultrafine, Aitken and accumulation with respective geometric diameters, (Dgn), of 17, 110 and 400 nm. An additional mode, appears between the ultrafine and Aitken modes (Dgn = 52 nm) in approximately one quarter of the measurements and is linked to several industrial cities upwind of the measurement site. A stabile ultrafine mode appears consistently (84% of measurements) at 16-17 nm throughout the campaign, suggestive of a source, such as a highway in the near vicinity. During fog and haze periods number concentrations for particles less than 25 nm and greater than 400 nm decrease by 78 and 95%, respectively. These changes do not affect the aerosol scattering efficiency significantly. The overall aerosol mass scattering efficiency determined for the Po Valley region is 4.3 ± 0.6 m2 g-1. Closure is achieved for light extinction predicted from droplet distributions and measured with a transmissiometer in 37 of 39 cases during fog periods. Measured and calculated light extinction, bext, covary strongly with an R2 of 0.92.
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| 9. |
- Almeida, Joao, et al.
(författare)
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Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere
- 2013
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Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 502:7471, s. 359-
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Tidskriftsartikel (refereegranskat)abstract
- Nucleation of aerosol particles from trace atmospheric vapours is thought to provide up to half of global cloud condensation nuclei(1). Aerosols can cause a net cooling of climate by scattering sunlight and by leading to smaller but more numerous cloud droplets, which makes clouds brighter and extends their lifetimes(2). Atmospheric aerosols derived from human activities are thought to have compensated for a large fraction of the warming caused by greenhouse gases(2). However, despite its importance for climate, atmospheric nucleation is poorly understood. Recently, it has been shown that sulphuric acid and ammonia cannot explain particle formation rates observed in the lower atmosphere(3). It is thought that amines may enhance nucleation(4-16), but until now there has been no direct evidence for amine ternary nucleation under atmospheric conditions. Here we use the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN and find that dimethylamine above three parts per trillion by volume can enhance particle formation rates more than 1,000-fold compared with ammonia, sufficient to account for the particle formation rates observed in the atmosphere. Molecular analysis of the clusters reveals that the faster nucleation is explained by a base-stabilization mechanism involving acid-amine pairs, which strongly decrease evaporation. The ion-induced contribution is generally small, reflecting the high stability of sulphuric acid-dimethylamine clusters and indicating that galactic cosmic rays exert only a small influence on their formation, except at low overall formation rates. Our experimental measurements are well reproduced by a dynamical model based on quantum chemical calculations of binding energies of molecular clusters, without any fitted parameters. These results show that, in regions of the atmosphere near amine sources, both amines and sulphur dioxide should be considered when assessing the impact of anthropogenic activities on particle formation.
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| 10. |
- Bower, K. N., et al.
(författare)
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The Great Dun Fell experiment 1995 : An overview
- 1999
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Ingår i: Atmospheric Research. - 0169-8095. ; 50:3-4, s. 151-184
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Tidskriftsartikel (refereegranskat)abstract
- During March and April of 1995 a major international field project was conducted at the UMIST field station site on Great Dun Fell in Cumbria, Northern England. The hill cap cloud which frequently envelopes this site was used as a natural flow through reactor to examine the sensitivity of the cloud microphysics to the aerosol entering the cloud and also to investigate the effects of the cloud in changing the aerosol size distribution, chemical composition and associated optical properties. To investigate these processes, detailed measurements of the cloud water chemistry (including the chemistry of sulphur compounds, organic and inorganic oxidised nitrogen and ammonia), cloud microphysics and properties of the aerosol and trace gas concentrations upwind and downwind of the cap cloud were undertaken. It was found that the cloud droplet number was generally strongly correlated to aerosol number concentration, with up to 2000 activated droplets cm-3 being observed in the most polluted conditions. In such conditions it was inferred that hygroscopic organic compounds were important in the activation process. Often, the size distribution of the aerosol was substantially modified by the cloud processing, largely due to the aqueous phase oxidation of S(IV) to sulphate by hydrogen peroxide, but also through the uptake and fixing of gas phase nitric acid as nitrate, increasing the calculated optical scattering of the aerosol substantially (by up to 24%). New particle formation was also observed in the ultrafine aerosol mode (at about 5 nm) downwind of the cap cloud, particularly in conditions of low total aerosol surface area and in the presence of ammonia and HCl gases. This was seen to occur at night as well as during the day via a mechanism which is not yet understood. The implications of these results for parameterising aerosol growth in Global Climate Models are explored.
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