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  • 1
    Publication Date: 2019-01-01
    Description: This chapter reviews the history of the discovery of cloud nuclei and their impacts on cloud microphysics and the climate system. Pioneers including John Aitken, Sir John Mason, Hilding Köhler, Christian Junge, Sean Twomey, and Kenneth Whitby laid the foundations of the field. Through their contributions and those of many others, rapid progress has been made in the last 100 years in understanding the sources, evolution, and composition of the atmospheric aerosol, the interactions of particles with atmospheric water vapor, and cloud microphysical processes. Major breakthroughs in measurement capabilities and in theoretical understanding have elucidated the characteristics of cloud condensation nuclei and ice nucleating particles and the role these play in shaping cloud microphysical properties and the formation of precipitation. Despite these advances, not all their impacts on cloud formation and evolution have been resolved. The resulting radiative forcing on the climate system due to aerosol–cloud interactions remains an unacceptably large uncertainty in future climate projections. Process-level understanding of aerosol–cloud interactions remains insufficient to support technological mitigation strategies such as intentional weather modification or geoengineering to accelerating Earth-system-wide changes in temperature and weather patterns.
    Print ISSN: 0065-9401
    Electronic ISSN: 1943-3646
    Topics: Geography , Geosciences , Physics
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  • 2
    Publication Date: 2016-01-30
    Description: This work presents experimental data on the cloud condensation nuclei (CCN) activity of two-component mixtures containing surfactants. Nine binary systems were tested combining strong ionic (sodium dodecyl sulfate) and non-ionic surfactants (Zonyl FS-300 and Triton X-100) with non-surfactant compounds (glucose, ammonium sulfate, or sodium chloride). Control tests were performed for systems combining organic (glucose) and inorganic compounds (ammonium sulfate or sodium chloride). Results show that CCN activity deviates strongly relative to predictions made from measurements of bulk surface tension. Köhler theory accounting for surface tension reduction and surface partitioning underpredicts the CCN activity of particles containing Zonyl FS-300 and Triton X-100. Partitioning theory better describes data for Zonyl FS-300 and Triton X-100 when limiting surface adsorption to 1.5 monolayers of the growing drop. Deviations from predictions were observed. Likely explanations include solute-solute interactions and non-spherical particle shape. The findings presented here examine in detail the perturbation of CCN activity by surfactants and may offer insight into both the success and limitations of physical models describing CCN activity of surface active molecules.
    Print ISSN: 0148-0227
    Topics: Geosciences , Physics
    Published by Wiley on behalf of American Geophysical Union (AGU).
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  • 3
    Publication Date: 2020-12-01
    Print ISSN: 1352-2310
    Electronic ISSN: 1873-2844
    Topics: Energy, Environment Protection, Nuclear Power Engineering , Geosciences , Physics
    Published by Elsevier
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  • 4
    Publication Date: 2020-09-16
    Description: Atmospheric aerosols can assume liquid, amorphous semi-solid or glassy, and crystalline phase states. Particle phase state plays a critical role in understanding and predicting aerosol impacts on human health, visibility, cloud formation, and climate. Melting point depression increases with decreasing particle diameter and is predicted by the Gibbs–Thompson relationship. This work reviews existing data on the melting point depression to constrain a simple parameterization of the process. The parameter $$xi $$ ξ describes the degree to which particle size lowers the melting point and is found to vary between 300 and 1800 K nm for a wide range of particle compositions. The parameterization is used together with existing frameworks for modeling the temperature and RH dependence of viscosity to predict the influence of particle size on the glass transition temperature and viscosity of secondary organic aerosol formed from the oxidation of $$alpha $$ α -pinene. Literature data are broadly consistent with the predictions. The model predicts a sharp decrease in viscosity for particles less than 100 nm in diameter. It is computationally efficient and suitable for inclusion in models to evaluate the potential influence of the phase change on atmospheric processes. New experimental data of the size-dependence of particle viscosity for atmospheric aerosol mimics are needed to thoroughly validate the predictions.
    Electronic ISSN: 2045-2322
    Topics: Natural Sciences in General
    Published by Springer Nature
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  • 5
    Publication Date: 2019-03-14
    Description: Particles composed of organic and inorganic components can assume core-shell morphologies. The kinetic limitation of water uptake due to the presence of a hydrophobic viscous outer shell may increase the critical supersaturation required to activate such particles into cloud droplets. Here we test this hypothesis through laboratory experiments. Results show that the viscosity of polyethylene particles is 5×106 Pa s at 60 ∘C. Extrapolation of temperature dependent viscosity measurements suggests that the particles are glassy at room temperature. Cloud condensation nuclei (CCN) activity measurements demonstrate that pure polyethylene particles are CCN inactive at diameters less than 741 nm and 2.5 % water supersaturation. Thus, polyethylene is used as proxy for hydrophobic glassy organic material. Ammonium sulfate is used as proxy for hygroscopic CCN active inorganic material. Mixed particles were generated using coagulation of oppositely charged particles; charge-neutral polyethylene–ammonium sulfate dimer particles were then isolated for online observation. Morphology of these dimer particles was varied by heating, such that liquefied polyethylene partially or completely engulfed the ammonium sulfate. Critical supersaturation was measured as a function of dry particle volume, particle morphology, and organic volume fraction. The data show that kinetic limitations do not change the critical supersaturation of 50 nm ammonium sulfate cores coated with polyethylene and polyethylene volume fractions up to 97 %. Based on these results, and a synthesis of literature data, it is suggested that mass transfer limitations by glassy organic shells are unlikely to affect cloud droplet activation near laboratory temperatures.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 6
    Publication Date: 2019-02-04
    Description: A new cloud parcel model (CPM) including activation, condensation, collision–coalescence, and lateral entrainment processes is used to investigate aerosol–cloud interactions (ACIs) in cumulus development prior to rainfall onset. The CPM was applied with surface aerosol measurements to predict the vertical structure of cloud development at early stages, and the model results were evaluated against airborne observations of cloud microphysics and thermodynamic conditions collected during the Integrated Precipitation and Hydrology Experiment (IPHEx) in the inner region of the southern Appalachian Mountains (SAM). Sensitivity analysis was conducted to examine the model response to variations in key ACI physiochemical parameters and initial conditions. The CPM sensitivities mirror those found in parcel models without entrainment and collision–coalescence, except for the evolution of the droplet spectrum and liquid water content with height. Simulated cloud droplet number concentrations (CDNCs) exhibit high sensitivity to variations in the initial aerosol concentration at cloud base, but weak sensitivity to bulk aerosol hygroscopicity. The condensation coefficient ac plays a governing role in determining the evolution of CDNC, liquid water content (LWC), and cloud droplet spectra (CDS) in time and with height. Lower values of ac lead to higher CDNCs and broader CDS above cloud base, and higher maximum supersaturation near cloud base. Analysis of model simulations reveals that competitive interference among turbulent dispersion, activation, and droplet growth processes modulates spectral width and explains the emergence of bimodal CDS and CDNC heterogeneity in aircraft measurements from different cloud regions and at different heights. Parameterization of nonlinear interactions among entrainment, condensational growth, and collision–coalescence processes is therefore necessary to simulate the vertical structures of CDNCs and CDSs in convective clouds. Comparisons of model predictions with data suggest that the representation of lateral entrainment remains challenging due to the spatial heterogeneity of the convective boundary layer and the intricate 3-D circulations in mountainous regions.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 7
    Publication Date: 2017-01-31
    Description: During the CalWater 2015 field campaign, ground-level observations of aerosol size, concentration, chemical composition, and cloud activity were made at Bodega Bay, CA, on the remote California coast. A strong anthropogenic influence on air quality, aerosol physicochemical properties, and cloud activity was observed at Bodega Bay during periods with special weather conditions, known as Petaluma Gap flow, in which air from California's interior is transported to the coast. This study applies a diverse set of chemical, cloud microphysical, and meteorological measurements to the Petaluma Gap flow phenomenon for the first time. It is demonstrated that the sudden and often dramatic change in aerosol properties is strongly related to regional meteorology and anthropogenically influenced chemical processes in California's Central Valley. In addition, it is demonstrated that the change in air mass properties from those typical of a remote marine environment to properties of a continental regime has the potential to impact atmospheric radiative balance and cloud formation in ways that must be accounted for in regional climate simulations.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 8
    Publication Date: 2019-04-10
    Description: We present the laboratory results of immersion freezing efficiencies of cellulose particles at supercooled temperature (T) conditions. Three types of chemically homogeneous cellulose samples are used as surrogates that represent supermicron and submicron ice-nucleating plant structural polymers. These samples include microcrystalline cellulose (MCC), fibrous cellulose (FC) and nanocrystalline cellulose (NCC). Our immersion freezing dataset includes data from various ice nucleation measurement techniques available at 17 different institutions, including nine dry dispersion and 11 aqueous suspension techniques. With a total of 20 methods, we performed systematic accuracy and precision analysis of measurements from all 20 measurement techniques by evaluating T-binned (1 ∘C) data over a wide T range (−36 ∘C 
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 9
    Publication Date: 2017-09-22
    Description: A number of new measurement methods for ice nucleating particles (INPs) have been introduced in recent years, and it is important to address how these methods compare. Laboratory comparisons of instruments sampling major INP types are common, but few comparisons have occurred for ambient aerosol measurements exploring the utility, consistency and complementarity of different methods to cover the large dynamic range of INP concentrations that exists in the atmosphere. In this study, we assess the comparability of four offline immersion freezing measurement methods (Colorado State University ice spectrometer, IS; North Carolina State University cold stage, CS; National Institute for Polar Research Cryogenic Refrigerator Applied to Freezing Test, CRAFT; University of British Columbia micro-orifice uniform deposit impactor–droplet freezing technique, MOUDI-DFT) and an online method (continuous flow diffusion chamber, CFDC) used in a manner deemed to promote/maximize immersion freezing, for the detection of INPs in ambient aerosols at different locations and in different sampling scenarios. We also investigated the comparability of different aerosol collection methods used with offline immersion freezing instruments. Excellent agreement between all methods could be obtained for several cases of co-sampling with perfect temporal overlap. Even for sampling periods that were not fully equivalent, the deviations between atmospheric INP number concentrations measured with different methods were mostly less than 1 order of magnitude. In some cases, however, the deviations were larger and not explicable without sampling and measurement artifacts. Overall, the immersion freezing methods seem to effectively capture INPs that activate as single particles in the modestly supercooled temperature regime (〉 −20 °C), although more comparisons are needed in this temperature regime that is difficult to access with online methods. Relative to the CFDC method, three immersion freezing methods that disperse particles into a bulk liquid (IS, CS, CRAFT) exhibit a positive bias in measured INP number concentrations below −20 °C, increasing with decreasing temperature. This bias was present but much less pronounced for a method that condenses separate water droplets onto limited numbers of particles prior to cooling and freezing (MOUDI-DFT). Potential reasons for the observed differences are discussed, and further investigations proposed to elucidate the role of all factors involved.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 10
    Publication Date: 2018-11-19
    Description: 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.
    Print ISSN: 1867-1381
    Electronic ISSN: 1867-8548
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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