| 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
-
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
-
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
-
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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| 11. |
- DeMott, Paul J., et al.
(författare)
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The Fifth International Workshop on Ice Nucleation phase 2 (FIN-02) : Laboratory intercomparison of ice nucleation measurements
- 2018
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Ingår i: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 11:11, s. 6231-6257
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Tidskriftsartikel (refereegranskat)abstract
- The second phase of the Fifth International Ice Nucleation Workshop (FIN-02) involved the gathering of a large number of researchers at the Karlsruhe Institute of Technology's Aerosol Interactions and Dynamics of the Atmosphere (AIDA) facility to promote characterization and understanding of ice nucleation measurements made by a variety of methods used worldwide. Compared to the previous workshop in 2007, participation was doubled, reflecting a vibrant research area. Experimental methods involved sampling of aerosol particles by direct processing ice nucleation measuring systems from the same volume of air in separate experiments using different ice nucleating particle (INP) types, and collections of aerosol particle samples onto filters or into liquid for sharing amongst measurement techniques that post-process these samples. In this manner, any errors introduced by differences in generation methods when samples are shared across laboratories were mitigated. Furthermore, as much as possible, aerosol particle size distribution was controlled so that the size limitations of different methods were minimized. The results presented here use data from the workshop to assess the comparability of immersion freezing measurement methods activating INPs in bulk suspensions, methods that activate INPs in condensation and/or immersion freezing modes as single particles on a substrate, continuous flow diffusion chambers (CFDCs) directly sampling and processing particles well above water saturation to maximize immersion and subsequent freezing of aerosol particles, and expansion cloud chamber simulations in which liquid cloud droplets were first activated on aerosol particles prior to freezing. The AIDA expansion chamber measurements are expected to be the closest representation to INP activation in atmospheric cloud parcels in these comparisons, due to exposing particles freely to adiabatic cooling. The different particle types used as INPs included the minerals illite NX and potassium feldspar (K-feldspar), two natural soil dusts representative of arable sandy loam (Argentina) and highly erodible sandy dryland (Tunisia) soils, respectively, and a bacterial INP (Snomax®). Considered together, the agreement among post-processed immersion freezing measurements of the numbers and fractions of particles active at different temperatures following bulk collection of particles into liquid was excellent, with possible temperature uncertainties inferred to be a key factor in determining INP uncertainties. Collection onto filters for rinsing versus directly into liquid in impingers made little difference. For methods that activated collected single particles on a substrate at a controlled humidity at or above water saturation, agreement with immersion freezing methods was good in most cases, but was biased low in a few others for reasons that have not been resolved, but could relate to water vapor competition effects. Amongst CFDC-style instruments, various factors requiring (variable) higher supersaturations to achieve equivalent immersion freezing activation dominate the uncertainty between these measurements, and for comparison with bulk immersion freezing methods. When operated above water saturation to include assessment of immersion freezing, CFDC measurements often measured at or above the upper bound of immersion freezing device measurements, but often underestimated INP concentration in comparison to an immersion freezing method that first activates all particles into liquid droplets prior to cooling (the PIMCA-PINC device, or Portable Immersion Mode Cooling chAmber-Portable Ice Nucleation Chamber), and typically slightly underestimated INP number concentrations in comparison to cloud parcel expansions in the AIDA chamber; this can be largely mitigated when it is possible to raise the relative humidity to sufficiently high values in the CFDCs, although this is not always possible operationally. Correspondence of measurements of INPs among direct sampling and post-processing systems varied depending on the INP type. Agreement was best for Snomax® particles in the temperature regime colder than -10°C, where their ice nucleation activity is nearly maximized and changes very little with temperature. At temperatures warmer than -10°C, Snomax® INP measurements (all via freezing of suspensions) demonstrated discrepancies consistent with previous reports of the instability of its protein aggregates that appear to make it less suitable as a calibration INP at these temperatures. For Argentinian soil dust particles, there was excellent agreement across all measurement methods; measures ranged within 1 order of magnitude for INP number concentrations, active fractions and calculated active site densities over a 25 to 30°C range and 5 to 8 orders of corresponding magnitude change in number concentrations. This was also the case for all temperatures warmer than -25°C in Tunisian dust experiments. In contrast, discrepancies in measurements of INP concentrations or active site densities that exceeded 2 orders of magnitude across a broad range of temperature measurements found at temperatures warmer than -25°C in a previous study were replicated for illite NX. Discrepancies also exceeded 2 orders of magnitude at temperatures of -20 to -25°C for potassium feldspar (K-feldspar), but these coincided with the range of temperatures at which INP concentrations increase rapidly at approximately an order of magnitude per 2°C cooling for K-feldspar. These few discrepancies did not outweigh the overall positive outcomes of the workshop activity, nor the future utility of this data set or future similar efforts for resolving remaining measurement issues. Measurements of the same materials were repeatable over the time of the workshop and demonstrated strong consistency with prior studies, as reflected by agreement of data broadly with parameterizations of different specific or general (e.g., soil dust) aerosol types. The divergent measurements of the INP activity of illite NX by direct versus post-processing methods were not repeated for other particle types, and the Snomax° data demonstrated that, at least for a biological INP type, there is no expected measurement bias between bulk collection and direct immediately processed freezing methods to as warm as -10°C. Since particle size ranges were limited for this workshop, it can be expected that for atmospheric populations of INPs, measurement discrepancies will appear due to the different capabilities of methods for sampling the full aerosol size distribution, or due to limitations on achieving sufficient water supersaturations to fully capture immersion freezing in direct processing instruments. Overall, this workshop presents an improved picture of present capabilities for measuring INPs than in past workshops, and provides direction toward addressing remaining measurement issues.
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| 12. |
- Hsu, Chia-Jui, et al.
(författare)
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Revealing the interface nature of ZDDP tribofilm by X-ray photoelectron spectroscopy and atom probe tomography
- 2020
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Ingår i: Industrial Lubrication and Tribology. - 0036-8792. ; 72:7, s. 923-930
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Tidskriftsartikel (refereegranskat)abstract
- Purpose To decrease wear and friction, zinc dialkyldithiophosphate (ZDDP) has been used in engine oil for several decades, but the mechanism of the tribofilm formation is still unclear. The purpose of this study is to characterize the chemical details of the tribofilm by using high-resolution approaching. Design/methodology/approach An ISO VG 100 mineral oil mixed with ZDDP was used in sliding tests on cylindrical roller bearings. Tribofilm formation was observed after 2 h of the sliding test. X-ray photoelectron spectroscopy (XPS) and atom probe tomography (APT) were used for chemical analysis of the tribofilm. Findings The results show that the ZDDP tribofilm consists of the common ZDDP elements along with iron oxides. A considerable amount of zinc and a small amount of sulfur were observed. In particular, an oxide interlayer with sulfur enrichment was revealed by APT between the tribofilm and the steel substrate. The depth profile of the chemical composition was obtained, and a tribofilm of approximately 40 nm thickness was identified by XPS. Originality/value A sulfur enrichment at the interface is observed by APT, which is beneath an oxygen enrichment. The clear evidence of the S interlayer confirms the hard and soft acids and bases principle.
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| 13. |
- Kirkby, Jasper, et al.
(författare)
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Atmospheric new particle formation from the CERN CLOUD experiment
- 2023
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Ingår i: Nature Geoscience. - 1752-0894 .- 1752-0908. ; 16:11, s. 948-957
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Tidskriftsartikel (refereegranskat)abstract
- Aerosol particles in the atmosphere profoundly influence public health and climate. Ultrafine particles enter the body through the lungs and can translocate to essentially all organs, and they represent a major yet poorly understood health risk. Human activities have considerably increased aerosols and cloudiness since preindustrial times, but they remain persistently uncertain and underrepresented in global climate models. Here we present a synthesis of the current understanding of atmospheric new particle formation derived from laboratory measurements at the CERN CLOUD chamber. Whereas the importance of sulfuric acid has long been recognized, condensable vapours such as highly oxygenated organics and iodine oxoacids also play key roles, together with stabilizers such as ammonia, amines and ions from galactic cosmic rays. We discuss how insights from CLOUD experiments are helping to interpret new particle formation in different atmospheric environments, and to provide a mechanistic foundation for air quality and climate models. The CLOUD experiment provides important insights into new particle formation in different atmospheric environments.
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| 14. |
- Kirkby, Jasper, et al.
(författare)
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Ion-induced nucleation of pure biogenic particles
- 2016
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Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 533:7604, s. 521-526
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Tidskriftsartikel (refereegranskat)abstract
- Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood(1). Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours(2). It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere(3,4), and that ions have a relatively minor role(5). Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded(6,7). Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of a-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.
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| 15. |
- Lacher, Larissa, et al.
(författare)
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The Puy de Dôme ICe Nucleation Intercomparison Campaign (PICNIC): comparison between online and offline methods in ambient air
- 2024
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Ingår i: ATMOSPHERIC CHEMISTRY AND PHYSICS. - 1680-7316 .- 1680-7324. ; 24:4, s. 2651-2678
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Tidskriftsartikel (refereegranskat)abstract
- Ice crystal formation in mixed-phase clouds is initiated by specific aerosol particles, termed ice-nucleating particles (INPs). Only a tiny fraction of all aerosol particles are INPs, providing a challenge for contemporary INP measurement techniques. Models have shown that the presence of INPs in clouds can impact their radiative properties and induce precipitation formation. However, for a qualified implementation of INPs in models, measurement techniques able to accurately detect the temperature-dependent INP concentration are needed. Here we present measurements of INP concentrations in ambient air under conditions relevant to mixed-phase clouds from a total of 10 INP methods over 2 weeks in October 2018 at the Puy de Dome observatory in central France. A special focus in this intercomparison campaign was placed on having overlapping sampling periods. Although a variety of different measurement principles were used, the majority of the data show INP concentrations within a factor of 5 of one another, demonstrating the suitability of the instruments to derive model-relevant INP data.Lower values of comparability are likely due to instrument-specific features such as aerosol lamina spreading in continuous-flow diffusion chambers, demonstrating the need to account for such phenomena when interpreting INP concentration data from online instruments. Moreover, consistently higher INP concentrations were observed from aerosol filters collected on the rooftop at the Puy de Dome station without the use of an aerosol inlet.
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| 16. |
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| 17. |
- Sipila, Mikko, et al.
(författare)
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The Role of Sulfuric Acid in Atmospheric Nucleation
- 2010
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Ingår i: Science. - : American Association for the Advancement of Science (AAAS). - 0036-8075 .- 1095-9203. ; 327:5970, s. 1243-1246
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Tidskriftsartikel (refereegranskat)abstract
- Nucleation is a fundamental step in atmospheric new-particle formation. However, laboratory experiments on nucleation have systematically failed to demonstrate sulfuric acid particle formation rates as high as those necessary to account for ambient atmospheric concentrations, and the role of sulfuric acid in atmospheric nucleation has remained a mystery. Here, we report measurements of new particles ( with diameters of approximately 1.5 nanometers) observed immediately after their formation at atmospherically relevant sulfuric acid concentrations. Furthermore, we show that correlations between measured nucleation rates and sulfuric acid concentrations suggest that freshly formed particles contain one to two sulfuric acid molecules, a number consistent with assumptions that are based on atmospheric observations. Incorporation of these findings into global models should improve the understanding of the impact of secondary particle formation on climate.
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| 18. |
- Snider, J. R., et al.
(författare)
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Intercomparison of cloud condensation nuclei and hygroscopic fraction measurements: Coated soot particles investigated during the LACIS Experiment in November (LExNo)
- 2010
-
Ingår i: Journal of Geophysical Research. - 2156-2202. ; 115, s. 11205-11205
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Tidskriftsartikel (refereegranskat)abstract
- Four cloud condensation nuclei (CCN) instruments were used to sample size-selected particles prepared at the Leipzig Aerosol Cloud Interaction Simulator facility. Included were two Wyoming static diffusion CCN instruments, the continuous flow instrument built by Droplet Measurement Technologies, and the continuous flow Leipzig instrument. The aerosols were composed of ammonium sulfate, levoglucosan, levoglucosan and soot, and ammonium hydrogen sulfate and soot. Comparisons are made among critical supersaturation values from the CCN instruments and derived from measurements made with a humidified tandem differential mobility system. The comparison is quite encouraging: with few exceptions the reported critical supersaturations agree within known experimental uncertainty limits. Also reported are CCN- and hygroscopicity-based estimates of the soot particles' solute fraction. Relative differences between these are as large as 40%, but an error analysis demonstrates that agreement within experimental uncertainty is achieved. We also analyze data from the Droplet Measurement Technologies and the two Wyoming static diffusion instruments for evidence of size distribution broadening and investigate levoglucosan particle growth kinetics in the Wyoming CCN instrument.
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| 19. |
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| 20. |
- Tsagkogeorgas, Georgios, et al.
(författare)
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Evaporation of sulfate aerosols at low relative humidity
- 2017
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:14, s. 8923-8938
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Tidskriftsartikel (refereegranskat)abstract
- Evaporation of sulfuric acid from particles can be important in the atmospheres of Earth and Venus. However, the equilibrium constant for the dissociation of H2SO4 to bisulfate ions, which is the one of the fundamental parameters controlling the evaporation of sulfur particles, is not well constrained. In this study we explore the volatility of sulfate particles at very low relative humidity. We measured the evaporation of sulfur particles versus temperature and relative humidity in the CLOUD chamber at CERN. We modelled the observed sulfur particle shrinkage with the ADCHAM model. Based on our model results, we conclude that the sulfur particle shrinkage is mainly governed by H2SO4 and potentially to some extent by SO3 evaporation. We found that the equilibrium constants for the dissociation of H2SO4 to HSO4-(KH2SO4) and the dehydration of H2SO4 to SO3 (KSO3) are KH2SO4 Combining double low line 2-4 × 109 kg-1 and KSO3 ≥ 1.4 × g 1010 at 288.8± 5K.
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| 21. |
- Welti, André, et al.
(författare)
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Ship-based measurements of ice nuclei concentrations over the Arctic, Atlantic, Pacific and Southern oceans
- 2020
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:23, s. 15191-15206
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Tidskriftsartikel (refereegranskat)abstract
- Ambient concentrations of ice-forming particles measured during ship expeditions are collected and summarised with the aim of determining the spatial distribution and variability in ice nuclei in oceanic regions. The presented data from literature and previously unpublished data from over 23 months of ship-based measurements stretch from the Arctic to the Southern Ocean and include a circumnavigation of Antarctica. In comparison to continental observations, ship-based measurements of ambient ice nuclei show 1 to 2 orders of magnitude lower mean concentrations. To quantify the geographical variability in oceanic areas, the concentration range of potential ice nuclei in different climate zones is analysed by meridionally dividing the expedition tracks into tropical, temperate and polar climate zones. We find that concentrations of ice nuclei in these meridional zones follow temperature spectra with similar slopes but vary in absolute concentration. Typically, the frequency with which specific concentrations of ice nuclei are observed at a certain temperature follows a log-normal distribution. A consequence of the log-normal distribution is that the mean concentration is higher than the most frequently measured concentration. Finally, the potential contribution of ship exhaust to the measured ice nuclei concentration on board research vessels is analysed as function of temperature. We find a sharp onset of the influence at approximately -36 degrees C but none at warmer temperatures that could bias ship-based measurements.
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