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Sökning: WFRF:(DeMott Paul J.)

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1.
  • DeMott, Paul J., et al. (författare)
  • The Fifth International Workshop on Ice Nucleation phase 2 (FIN-02) : Laboratory intercomparison of ice nucleation measurements
  • 2018
  • Ingår i: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 11:11, s. 6231-6257
  • 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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2.
  • Lacher, Larissa, et al. (författare)
  • The Puy de Dôme ICe Nucleation Intercomparison Campaign (PICNIC): comparison between online and offline methods in ambient air
  • 2024
  • Ingår i: ATMOSPHERIC CHEMISTRY AND PHYSICS. - 1680-7316 .- 1680-7324. ; 24:4, s. 2651-2678
  • 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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3.
  • Geerts, Bart, et al. (författare)
  • The COMBLE Campaign : A Study of Marine Boundary Layer Clouds in Arctic Cold-Air Outbreaks
  • 2022
  • Ingår i: Bulletin of The American Meteorological Society - (BAMS). - 0003-0007 .- 1520-0477. ; 103:5, s. E1371-E1389
  • Tidskriftsartikel (refereegranskat)abstract
    • One of the most intense air mass transformations on Earth happens when cold air flows from frozen surfaces to much warmer open water in cold-air outbreaks (CAOs), a process captured beautifully in satellite imagery. Despite the ubiquity of the CAO cloud regime over high-latitude oceans, we have a rather poor understanding of its properties, its role in energy and water cycles, and its treatment in weather and climate models. The Cold-Air Outbreaks in the Marine Boundary Layer Experiment (COMBLE) was conducted to better understand this regime and its representation in models. COMBLE aimed to examine the relations between surface fluxes, boundary layer structure, aerosol, cloud, and precipitation properties, and mesoscale circulations in marine CAOs. Processes affecting these properties largely fall in a range of scales where boundary layer processes, convection, and precipitation are tightly coupled, which makes accurate representation of the CAO cloud regime in numerical weather prediction and global climate models most challenging. COMBLE deployed an Atmospheric Radiation Measurement Mobile Facility at a coastal site in northern Scandinavia (69°N), with additional instruments on Bear Island (75°N), from December 2019 to May 2020. CAO conditions were experienced 19% (21%) of the time at the main site (on Bear Island). A comprehensive suite of continuous in situ and remote sensing observations of atmospheric conditions, clouds, precipitation, and aerosol were collected. Because of the clouds’ well-defined origin, their shallow depth, and the broad range of observed temperature and aerosol concentrations, the COMBLE dataset provides a powerful modeling testbed for improving the representation of mixed-phase cloud processes in large-eddy simulations and large-scale models.  
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4.
  • Welti, André, et al. (författare)
  • Ship-based measurements of ice nuclei concentrations over the Arctic, Atlantic, Pacific and Southern oceans
  • 2020
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:23, s. 15191-15206
  • 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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7.
  • Zhao, Xi, et al. (författare)
  • Important Ice Processes Are Missed by the Community Earth System Model in Southern Ocean Mixed-Phase Clouds : Bridging SOCRATES Observations to Model Developments
  • 2023
  • Ingår i: Journal of Geophysical Research: Atmospheres. - 2169-897X. ; 128:4
  • Tidskriftsartikel (refereegranskat)abstract
    • Global climate models (GCMs) are challenged by difficulties in simulating cloud phase and cloud radiative effect over the Southern Ocean (SO). Some of the new-generation GCMs predict too much liquid and too little ice in mixed-phase clouds. This misrepresentation of cloud phase in GCMs results in weaker negative cloud feedback over the SO and a higher climate sensitivity. Based on a model comparison with observational data obtained during the Southern Ocean Cloud Radiation and Aerosol Transport Experimental Study, this study addresses a key uncertainty in the Community Earth System Model version 2 (CESM2) related to cloud phase, namely ice formation in pristine remote SO clouds. It is found that sea spray organic aerosols (SSOAs) are the most important type of ice nucleating particles (INPs) over the SO with concentrations 1 order of magnitude higher than those of dust INPs based on measurements and CESM2 simulations. Secondary ice production (SIP) which includes riming splintering, rain droplet shattering, and ice-ice collisional fragmentation as implemented in CESM2 is the dominant ice production process in moderately cold clouds with cloud temperatures greater than −20°C. SIP enhances the in-cloud ice number concentrations (Ni) by 1–3 orders of magnitude and predicts more mixed-phase (with percentage occurrence increased from 15% to 21%), in better agreement with the observations. This study highlights the importance of accurately representing the cloud phase over the pristine remote SO by considering the ice nucleation of SSOA and SIP processes, which are currently missing in most GCM cloud microphysics parameterizations.
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8.
  • Waman, Deepak, et al. (författare)
  • Dependencies of Four Mechanisms of Secondary Ice Production on Cloud-Top Temperature in a Continental Convective Storm
  • 2022
  • Ingår i: Journal of Atmospheric Sciences. - 1520-0469. ; 79:12, s. 3375-3404
  • Tidskriftsartikel (refereegranskat)abstract
    • Various mechanisms of secondary ice production (SIP) cause multiplication of numbers of ice particle, after the onset of primary ice. A measure of SIP is the ice enhancement ratio (“IE ratio”) defined here as the ratio between number concentrations of total ice (excluding homogeneously nucleated ice) and active ice-nucleating particles (INPs). A convective line observed on 11 May 2011 over the Southern Great Plains in the Mesoscale Continental Convective Cloud Experiment (MC3E) campaign was simulated with the “Aerosol–Cloud” (AC) model. AC is validated against coincident MC3E observations by aircraft, ground-based instruments, and satellite. Four SIP mechanisms are represented in AC: the Hallett–Mossop (HM) process of rime splintering, and fragmentation during ice–ice collisions, raindrop freezing, and sublimation. The vertical profile of the IE ratio, averaged over the entire simulation, is almost uniform (102 to 103) because fragmentation in ice–ice collisions dominates at long time scales, driving the ice concentration toward a theoretical maximum. The IE ratio increases with both the updraft (HM process, fragmentation during raindrop freezing, and ice–ice collisions) and downdraft speed (fragmentation during ice–ice collisions and sublimation). As reported historically in aircraft sampling, IE ratios were predicted to peak near 103 for cloud-top temperatures close to the −12°C level, mostly due to the HM process in typically young clouds with their age less than 15 min. At higher altitudes with temperatures of −20° to −30°C, the predicted IE ratios were smaller, ranging from 10 to 102, and mainly resulted from fragmentation in ice–ice collisions.
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