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- ItemIntercomparison study and optical asphericity measurements of small ice particles in the CERN CLOUD experiment(Katlenburg-Lindau : Copernicus, 2017) Nichman, Leonid; Järvinen, Emma; Dorsey, James; Connolly, Paul; Duplissy, Jonathan; Fuchs, Claudia; Ignatius, Karoliina; Sengupta, Kamalika; Stratmann, Frank; Möhler, Ottmar; Schnaiter, Martin; Gallagher, MartinOptical probes are frequently used for the detection of microphysical cloud particle properties such as liquid and ice phase, size and morphology. These properties can eventually influence the angular light scattering properties of cirrus clouds as well as the growth and accretion mechanisms of single cloud particles. In this study we compare four commonly used optical probes to examine their response to small cloud particles of different phase and asphericity. Cloud simulation experiments were conducted at the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at European Organisation for Nuclear Research (CERN). The chamber was operated in a series of multi-step adiabatic expansions to produce growth and sublimation of ice particles at super- and subsaturated ice conditions and for initial temperatures of -30, -40 and -50°C. The experiments were performed for ice cloud formation via homogeneous ice nucleation. We report the optical observations of small ice particles in deep convection and in situ cirrus simulations. Ice crystal asphericity deduced from measurements of spatially resolved single particle light scattering patterns by the Particle Phase Discriminator mark 2 (PPD-2K, Karlsruhe edition) were compared with Cloud and Aerosol Spectrometer with Polarisation (CASPOL) measurements and image roundness captured by the 3View Cloud Particle Imager (3V-CPI). Averaged path light scattering properties of the simulated ice clouds were measured using the Scattering Intensity Measurements for the Optical detectioN of icE (SIMONE) and single particle scattering properties were measured by the CASPOL. We show the ambiguity of several optical measurements in ice fraction determination of homogeneously frozen ice in the case where sublimating quasi-spherical ice particles are present. Moreover, most of the instruments have difficulties of producing reliable ice fraction if small aspherical ice particles are present, and all of the instruments cannot separate perfectly spherical ice particles from supercooled droplets. Correlation analysis of bulk averaged path depolarisation measurements and single particle measurements of these clouds showed higher R2 values at high concentrations and small diameters, but these results require further confirmation. We find that none of these instruments were able to determine unambiguously the phase of the small particles. These results have implications for the interpretation of atmospheric measurements and parametrisations for modelling, particularly for low particle number concentration clouds.
- ItemHomogeneous and heterogeneous ice nucleation at LACIS: Operating principle and theoretical studies(München : European Geopyhsical Union, 2011) Hartmann, S.; Niedermeier, D.; Voigtländer, J.; Clauss, T.; Shaw, R.A.; Wex, H.; Kiselev, A.; Stratmann, F.At the Leipzig Aerosol Cloud Interaction Simulator (LACIS) experiments investigating homogeneous and heterogeneous nucleation of ice (particularly immersion freezing in the latter case) have been carried out. Here both the physical LACIS setup and the numerical model developed to design experiments at LACIS and interpret their results are presented in detail. Combining results from the numerical model with experimental data, it was found that for the experimental parameter space considered, classical homogeneous ice nucleation theory is able to predict the freezing behavior of highly diluted ammonium sulfate solution droplets, while classical heterogeneous ice nucleation theory, together with the assumption of a constant contact angle, fails to predict the immersion freezing behavior of surrogate mineral dust particles (Arizona Test Dust, ATD). The main reason for this failure is the compared to experimental data apparently overly strong temperature dependence of the nucleation rate coefficient. Assuming, in the numerical model, Classical Nucleation Theory (CNT) for homogeneous ice nucleation and a CNT-based parameterization for the nucleation rate coefficient in the immersion freezing mode, recently published by our group, it was found that even for a relatively effective ice nucleating agent such as pure ATD, there is a temperature range where homogeneous ice nucleation is dominant. The main explanation is the apparently different temperature dependencies of the two freezing mechanisms. Finally, reviewing the assumptions made during the derivation of the CNT-based parameterization for immersion freezing, it was found that the assumption of constant temperature during ice nucleation and the chosen ice nucleation time were justified, underlining the applicability of the method to determine the fitting coefficients in the parameterization equation.
- ItemHeterogeneous ice nucleation: Exploring the transition from stochastic to singular freezing behavior(München : European Geopyhsical Union, 2011) Niedermeier, D.; Shaw, R.A.; Hartmann, S.; Wex, H.; Clauss, T.; Voigtländer, J.; Stratmann, F.Heterogeneous ice nucleation, a primary pathway for ice formation in the atmosphere, has been described alternately as being stochastic, in direct analogy with homogeneous nucleation, or singular, with ice nuclei initiating freezing at deterministic temperatures. We present an idealized, conceptual model to explore the transition between stochastic and singular ice nucleation. This "soccer ball" model treats particles as being covered with surface sites (patches of finite area) characterized by different nucleation barriers, but with each surface site following the stochastic nature of ice embryo formation. The model provides a phenomenological explanation for seemingly contradictory experimental results obtained in our research groups. Even with ice nucleation treated fundamentally as a stochastic process this process can be masked by the heterogeneity of surface properties, as might be typical for realistic atmospheric particle populations. Full evaluation of the model findings will require experiments with well characterized ice nucleating particles and the ability to vary both temperature and waiting time for freezing.
- ItemAnnual variability of ice-nucleating particle concentrations at different Arctic locations(Göttingen : Copernicus GmbH, 2019) Wex, H.; Huang, L.; Zhang, W.; Hung, H.; Traversi, R.; Becagli, S.; Sheesley, R.J.; Moffett, C.E.; Barrett, T.E.; Bossi, R.; Skov, H.; Hünerbein, A.; Lubitz, J.; Löffler, M.; Linke, O.; Hartmann, M.; Herenz, P.; Stratmann, F.Number concentrations of ice-nucleating particles (NINP) in the Arctic were derived from ground-based filter samples. Examined samples had been collected in Alert (Nunavut, northern Canadian archipelago on Ellesmere Island), Utqiagvik, formerly known as Barrow (Alaska), Nyalesund (Svalbard), and at the Villum Research Station (VRS; northern Greenland). For the former two stations, examined filters span a full yearly cycle. For VRS, 10 weekly samples, mostly from different months of one year, were included. Samples from Ny-Alesund were collected during the months from March until September of one year. At all four stations, highest concentrations were found in the summer months from roughly June to September. For those stations with sufficient data coverage, an annual cycle can be seen. The spectra of NINP observed at the highest temperatures, i.e., those obtained for summer months, showed the presence of INPs that nucleate ice up to-5 °C. Although the nature of these highly ice-active INPs could not be determined in this study, it often has been described in the literature that ice activity observed at such high temperatures originates from the presence of ice-active material of biogenic origin. Spectra observed at the lowest temperatures, i.e., those derived for winter months, were on the lower end of the respective values from the literature on Arctic INPs or INPs from midlatitude continental sites, to which a comparison is presented herein. An analysis concerning the origin of INPs that were ice active at high temperatures was carried out using back trajectories and satellite information. Both terrestrial locations in the Arctic and the adjacent sea were found to be possible source areas for highly active INPs.
- ItemConcentration and variability of ice nuclei in the subtropical maritime boundary layer(Katlenburg-Lindau : EGU, 2018) Welti, André; Müller, Konrad; Fleming, Zoë L.; Stratmann, FrankMeasurements of the concentration and variability of ice nucleating particles in the subtropical maritime boundary layer are reported. Filter samples collected in Cabo Verde over the period 2009-2013 are analyzed with a drop freezing experiment with sensitivity to detect the few rare ice nuclei active at low supercooling. The data set is augmented with continuous flow diffusion chamber measurements at temperatures below -24 °C from a 2-month field campaign in Cabo Verde in 2016. The data set is used to address the following questions: what are typical concentrations of ice nucleating particles active at a certain temperature? What affects their concentration and where are their sources? Concentration of ice nucleating particles is found to increase exponentially by 7 orders of magnitude from -5 to -38 °C. Sample-to-sample variation in the steepness of the increase indicates that particles of different origin, with different ice nucleation properties (size, composition), contribute to the ice nuclei concentration at different temperatures. The concentration of ice nuclei active at a specific temperature varies over a range of up to 4 orders of magnitude. The frequency with which a certain ice nuclei concentration is measured within this range is found to follow a lognormal distribution, which can be explained by random dilution during transport. To investigate the geographic origin of ice nuclei, source attribution of air masses from dispersion modeling is used to classify the data into seven typical conditions. While no source could be attributed to the ice nuclei active at temperatures higher than -12 °C, concentrations at lower temperatures tend to be elevated in air masses originating from the Sahara.
- ItemClassification of Arctic, midlatitude and tropical clouds in the mixed-phase temperature regime(Katlenburg-Lindau : EGU, 2017) Costa, Anja; Meyer, Jessica; Afchine, Armin; Luebke, Anna; Günther, Gebhard; Dorsey, James R.; Gallagher, Martin W.; Ehrlich, Andre; Wendisch, Manfred; Baumgardner, Darrel; Wex, Heike; Krämer, MartinaThe degree of glaciation of mixed-phase clouds constitutes one of the largest uncertainties in climate prediction. In order to better understand cloud glaciation, cloud spectrometer observations are presented in this paper, which were made in the mixed-phase temperature regime between 0 and -38°C (273 to 235K), where cloud particles can either be frozen or liquid. The extensive data set covers four airborne field campaigns providing a total of 139000 1Hz data points (38.6h within clouds) over Arctic, midlatitude and tropical regions. We develop algorithms, combining the information on number concentration, size and asphericity of the observed cloud particles to classify four cloud types: liquid clouds, clouds in which liquid droplets and ice crystals coexist, fully glaciated clouds after the Wegener-Bergeron-Findeisen process and clouds where secondary ice formation occurred. We quantify the occurrence of these cloud groups depending on the geographical region and temperature and find that liquid clouds dominate our measurements during the Arctic spring, while clouds dominated by the Wegener-Bergeron-Findeisen process are most common in midlatitude spring. The coexistence of liquid water and ice crystals is found over the whole mixed-phase temperature range in tropical convective towers in the dry season. Secondary ice is found at midlatitudes at -5 to -10°C (268 to 263K) and at higher altitudes, i.e. lower temperatures in the tropics. The distribution of the cloud types with decreasing temperature is shown to be consistent with the theory of evolution of mixed-phase clouds. With this study, we aim to contribute to a large statistical database on cloud types in the mixed-phase temperature regime.
- ItemLeipzig Ice Nucleation chamber Comparison (LINC): Intercomparison of four online ice nucleation counters(Katlenburg-Lindau : EGU, 2017) Burkert-Kohn, Monika; Wex, Heike; Welti, André; Hartmann, Susan; Grawe, Sarah; Hellner, Lisa; Herenz, Paul; Atkinson, James D.; Stratmann, Frank; Kanji, Zamin A.Ice crystal formation in atmospheric clouds has a strong effect on precipitation, cloud lifetime, cloud radiative properties, and thus the global energy budget. Primary ice formation above 235 K is initiated by nucleation on seed aerosol particles called ice-nucleating particles (INPs). Instruments that measure the ice-nucleating potential of aerosol particles in the atmosphere need to be able to accurately quantify ambient INP concentrations. In the last decade several instruments have been developed to investigate the ice-nucleating properties of aerosol particles and to measure ambient INP concentrations. Therefore, there is a need for intercomparisons to ensure instrument differences are not interpreted as scientific findings. In this study, we intercompare the results from parallel measurements using four online ice nucleation chambers. Seven different aerosol types are tested including untreated and acid-treated mineral dusts (microcline, which is a K-feldspar, and kaolinite), as well as birch pollen washing waters. Experiments exploring heterogeneous ice nucleation above and below water saturation are performed to cover the whole range of atmospherically relevant thermodynamic conditions that can be investigated with the intercompared chambers. The Leipzig Aerosol Cloud Interaction Simulator (LACIS) and the Portable Immersion Mode Cooling chAmber coupled to the Portable Ice Nucleation Chamber (PIMCA-PINC) performed measurements in the immersion freezing mode. Additionally, two continuous-flow diffusion chambers (CFDCs) PINC and the Spectrometer for Ice Nuclei (SPIN) are used to perform measurements below and just above water saturation, nominally presenting deposition nucleation and condensation freezing. The results of LACIS and PIMCA-PINC agree well over the whole range of measured frozen fractions (FFs) and temperature. In general PINC and SPIN compare well and the observed differences are explained by the ice crystal growth and different residence times in the chamber. To study the mechanisms responsible for the ice nucleation in the four instruments, the FF (from LACIS and PIMCA-PINC) and the activated fraction, AF (from PINC and SPIN), are compared. Measured FFs are on the order of a factor of 3 higher than AFs, but are not consistent for all aerosol types and temperatures investigated. It is shown that measurements from CFDCs cannot be assumed to produce the same results as those instruments exclusively measuring immersion freezing. Instead, the need to apply a scaling factor to CFDCs operating above water saturation has to be considered to allow comparison with immersion freezing devices. Our results provide further awareness of factors such as the importance of dispersion methods and the quality of particle size selection for intercomparing online INP counters.
- ItemHeterogeneous ice nucleation on dust particles sourced from nine deserts worldwide - Part 1: Immersion freezing(Katlenburg-Lindau : EGU, 2016) Boose, Yvonne; Welti, André; Atkinson, James; Ramelli, Fabiola; Danielczok, Anja; Bingemer, Heinz G.; Plötze, Michael; Sierau, Berko; Kanji, Zamin A.; Lohmann, UlrikeDesert dust is one of the most abundant ice nucleating particle types in the atmosphere. Traditionally, clay minerals were assumed to determine the ice nucleation ability of desert dust and constituted the focus of ice nucleation studies over several decades. Recently some feldspar species were identified to be ice active at much higher temperatures than clay minerals, redirecting studies to investigate the contribution of feldspar to ice nucleation on desert dust. However, so far no study has shown the atmospheric relevance of this mineral phase. For this study four dust samples were collected after airborne transport in the troposphere from the Sahara to different locations (Crete, the Peloponnese, Canary Islands, and the Sinai Peninsula). Additionally, 11 dust samples were collected from the surface from nine of the biggest deserts worldwide. The samples were used to study the ice nucleation behavior specific to different desert dusts. Furthermore, we investigated how representative surface-collected dust is for the atmosphere by comparing to the ice nucleation activity of the airborne samples. We used the IMCA-ZINC setup to form droplets on single aerosol particles which were subsequently exposed to temperatures between 233 and 250 K. Dust particles were collected in parallel on filters for offline cold-stage ice nucleation experiments at 253–263 K. To help the interpretation of the ice nucleation experiments the mineralogical composition of the dusts was investigated. We find that a higher ice nucleation activity in a given sample at 253 K can be attributed to the K-feldspar content present in this sample, whereas at temperatures between 238 and 245 K it is attributed to the sum of feldspar and quartz content present. A high clay content, in contrast, is associated with lower ice nucleation activity. This confirms the importance of feldspar above 250 K and the role of quartz and feldspars determining the ice nucleation activities at lower temperatures as found by earlier studies for monomineral dusts. The airborne samples show on average a lower ice nucleation activity than the surface-collected ones. Furthermore, we find that under certain conditions milling can lead to a decrease in the ice nucleation ability of polymineral samples due to the different hardness and cleavage of individual mineral phases causing an increase of minerals with low ice nucleation ability in the atmospherically relevant size fraction. Comparison of our data set to an existing desert dust parameterization confirms its applicability for climate models. Our results suggest that for an improved prediction of the ice nucleation ability of desert dust in the atmosphere, the modeling of emission and atmospheric transport of the feldspar and quartz mineral phases would be key, while other minerals are only of minor importance.
- ItemIce nucleating particles over the Eastern Mediterranean measured by unmanned aircraft systems(Katlenburg-Lindau : EGU, 2017) Schrod, Jann; Weber, Daniel; Drücke, Jaqueline; Keleshis, Christos; Pikridas, Michael; Ebert, Martin; Cvetković, Bojan; Nickovic, Slobodan; Marinou, Eleni; Baars, Holger; Ansmann, Albert; Vrekoussis, Mihalis; Mihalopoulos, Nikos; Sciare, Jean; Curtius, Joachim; Bingemer, Heinz G.During an intensive field campaign on aerosol, clouds, and ice nucleation in the Eastern Mediterranean in April 2016, we measured the abundance of ice nucleating particles (INPs) in the lower troposphere from unmanned aircraft systems (UASs). Aerosol samples were collected by miniaturized electrostatic precipitators onboard the UASs at altitudes up to 2.5 km. The number of INPs in these samples, which are active in the deposition and condensation modes at temperatures from -20 to -30 °C, were analyzed immediately after collection on site using the ice nucleus counter FRIDGE (FRankfurt Ice nucleation Deposition freezinG Experiment). During the 1-month campaign, we encountered a series of Saharan dust plumes that traveled at several kilometers' altitude. Here we present INP data from 42 individual flights, together with aerosol number concentrations, observations of lidar backscattering, dust concentrations derived by the dust transport model DREAM (Dust Regional Atmospheric Model), and results from scanning electron microscopy. The effect of the dust plumes is reflected by the coincidence of INPs with the particulate matter (PM), the lidar signal, and the predicted dust mass of the model. This suggests that mineral dust or a constituent related to dust was a major contributor to the ice nucleating properties of the aerosol. Peak concentrations of above 100 INPs std L-1 were measured at -30 °C. The INP concentration in elevated plumes was on average a factor of 10 higher than at ground level. Since desert dust is transported for long distances over wide areas of the globe predominantly at several kilometers' altitude, we conclude that INP measurements at ground level may be of limited significance for the situation at the level of cloud formation.
- ItemEstimated desert-dust ice nuclei profiles from polarization lidar: Methodology and case studies(München : European Geopyhsical Union, 2015) Mamouri, R.E.; Ansmann, A.A lidar method is presented that permits the estimation of height profiles of ice nuclei concentrations (INC) in desert dust layers. The polarization lidar technique is applied to separate dust and non-dust backscatter and extinction coefficients. The desert dust extinction coefficients σd are then converted to aerosol particle number concentrations APC280 which consider particles with radius > 280 nm only. By using profiles of APC280 and ambient temperature T along the laser beam, the profile of INC can be estimated within a factor of 3 by means of APC-T-INC parameterizations from the literature. The observed close relationship between σd at 500 nm and APC280 is of key importance for a successful INC retrieval. We studied this link by means of AERONET (Aerosol Robotic Network) sun/sky photometer observations at Morocco, Cabo Verde, Barbados, and Cyprus during desert dust outbreaks. The new INC retrieval method is applied to lidar observations of dust layers with the spaceborne lidar CALIOP (Cloud Aerosol Lidar with Orthogonal Polarization) during two overpasses over the EARLINET (European Aerosol Research Lidar Network) lidar site of the Cyprus University of Technology (CUT), Limassol (34.7° N, 33° E), Cyprus. The good agreement between the CALIOP and CUT lidar retrievals of σd, APC280, and INC profiles corroborates the potential of CALIOP to provide 3-D global desert dust APC280 and INC data sets.