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    Concentration and variability of ice nuclei in the subtropical maritime boundary layer
    (Katlenburg-Lindau : EGU, 2018) Welti, André; Müller, Konrad; Fleming, Zoë L.; Stratmann, Frank
    Measurements 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.
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    Leipzig 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.
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    Heterogeneous 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, Ulrike
    Desert 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.
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    Comparing contact and immersion freezing from continuous flow diffusion chambers
    (München : European Geopyhsical Union, 2016) Nagare, Baban; Marcolli, Claudia; Welti, André; Stetzer, Olaf; Lohmann, Ulrike
    Ice nucleating particles (INPs) in the atmosphere are responsible for glaciating cloud droplets between 237 and 273 K. Different mechanisms of heterogeneous ice nucleation can compete under mixed-phase cloud conditions. Contact freezing is considered relevant because higher ice nucleation temperatures than for immersion freezing for the same INPs were observed. It has limitations because its efficiency depends on the number of collisions between cloud droplets and INPs. To date, direct comparisons of contact and immersion freezing with the same INP, for similar residence times and concentrations, are lacking. This study compares immersion and contact freezing efficiencies of three different INPs. The contact freezing data were obtained with the ETH CoLlision Ice Nucleation CHamber (CLINCH) using 80 µm diameter droplets, which can interact with INPs for residence times of 2 and 4 s in the chamber. The contact freezing efficiency was calculated by estimating the number of collisions between droplets and particles. Theoretical formulations of collision efficiencies gave too high freezing efficiencies for all investigated INPs, namely AgI particles with 200 nm electrical mobility diameter, 400 and 800 nm diameter Arizona Test Dust (ATD) and kaolinite particles. Comparison of freezing efficiencies by contact and immersion freezing is therefore limited by the accuracy of collision efficiencies. The concentration of particles was 1000 cm−3 for ATD and kaolinite and 500, 1000, 2000 and 5000 cm−3 for AgI. For concentrations  <  5000 cm−3, the droplets collect only one particle on average during their time in the chamber. For ATD and kaolinite particles, contact freezing efficiencies at 2 s residence time were smaller than at 4 s, which is in disagreement with a collisional contact freezing process but in accordance with immersion freezing or adhesion freezing. With “adhesion freezing”, we refer to a contact nucleation process that is enhanced compared to immersion freezing due to the position of the INP on the droplet, and we discriminate it from collisional contact freezing, which assumes an enhancement due to the collision of the particle with the droplet. For best comparison with contact freezing results, immersion freezing experiments of the same INPs were performed with the continuous flow diffusion chamber Immersion Mode Cooling chAmber–Zurich Ice Nucleation Chamber (IMCA–ZINC) for a 3 s residence time. In IMCA–ZINC, each INP is activated into a droplet in IMCA and provides its surface for ice nucleation in the ZINC chamber. The comparison of contact and immersion freezing results did not confirm a general enhancement of freezing efficiency for contact compared with immersion freezing experiments. For AgI particles the onset of heterogeneous freezing in CLINCH was even shifted to lower temperatures compared with IMCA–ZINC. For ATD, freezing efficiencies for contact and immersion freezing experiments were similar. For kaolinite particles, contact freezing became detectable at higher temperatures than immersion freezing. Using contact angle information between water and the INP, it is discussed how the position of the INP in or on the droplets may influence its ice nucleation activity.