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- ItemVariation of Ice Nucleating Particles in the European Arctic Over the Last Centuries(Hoboken, NJ [u.a.] : Wiley, 2019) Hartmann, M.; Blunier, T.; Brügger, S.O.; Schmale, J.; Schwikowski, M.; Vogel, A.; Wex, H.; Stratmann, F.The historical development of ice nucleating particle concentrations (NINP) is still unknown. Here, we present for the first time NINP from the past 500 years at two Arctic sites derived from ice core samples. The samples originate from the EUROCORE ice core (Summit, Central Greenland) and from the Lomo09 ice core (Lomonosovfonna, Svalbard). No long-term trend is obvious in the measured samples, and the overall range of NINP is comparable to present-day observations. We observe that the short-term variations in NINP is larger than the long-term variability, but neither anthropogenic pollution nor volcanic eruptions seem to have influenced NINP in the measured temperature range. Shape and onset temperature of several INP spectra suggest that INP of biogenic origin contributed to the Arctic INP population throughout the past. ©2019. The Authors.
- ItemWintertime Airborne Measurements of Ice Nucleating Particles in the High Arctic: A Hint to a Marine, Biogenic Source for Ice Nucleating Particles(Hoboken, NJ [u.a.] : Wiley, 2020) Hartmann, M.; Adachi, K.; Eppers, O.; Haas, C.; Herber, A.; Holzinger, R.; Hünerbein, A.; Jäkel, E.; Jentzsch, C.; van Pinxteren, M.; Wex, H.; Willmes, S.; Stratmann, F.Ice nucleating particles (INPs) affect the radiative properties of cold clouds. Knowledge concerning their concentration above ground level and their potential sources is scarce. Here we present the first highly temperature resolved ice nucleation spectra of airborne samples from an aircraft campaign during late winter in 2018. Most INP spectra featured low concentration levels (<3 · 10−4 L−1 at −15°C). However, we also found INP concentrations of up to 1.8·10−2 L−1 at −15°C and freezing onsets as high as −7.5°C for samples mainly from the marine boundary layer. Shape and onset temperature of the ice nucleation spectra of those samples as well as heat sensitivity hint at biogenic INP. Colocated measurements additionally indicate a local marine influence rather than long-range transport. Our results suggest that even in late winter above 80°N a local marine source for biogenic INP, which can efficiently nucleate ice at high temperatures, is present. ©2020. The Authors.
- 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.
- ItemKaolinite particles as ice nuclei: Learning from the use of different kaolinite samples and different coatings(Göttingen : Copernicus, 2014) Wex, H.; Demott, P.J.; Tobo, Y.; Hartmann, S.; Rösch, M.; Clauss, T.; Tomsche, L.; Niedermeier, D.; Stratmann, F.Kaolinite particles from two different sources (Fluka and Clay Minerals Society (CMS)) were examined with respect to their ability to act as ice nuclei (IN). This was done in the water-subsaturated regime where often deposition ice nucleation is assumed to occur, and for water-supersaturated conditions, i.e., in the immersion freezing mode. Measurements were done using a flow tube (the Leipzig Aerosol Cloud Interaction Simulator, LACIS) and a continuous-flow diffusion chamber (CFDC). Pure and coated particles were used, with coating thicknesses of a few nanometers or less, where the coating consisted of levoglucosan, succinic acid or sulfuric acid. In general, it was found that the coatings strongly reduced deposition ice nucleation. Remaining ice formation in the water-subsaturated regime could be attributed to immersion freezing, with particles immersed in concentrated solutions formed by the coatings. In the immersion freezing mode, ice nucleation rate coefficients het from both instruments agreed well with each other, particularly when the residence times in the instruments were accounted for. Fluka kaolinite particles coated with either levoglucosan or succinic acid showed the same IN activity as pure Fluka kaolinite particles; i.e., it can be assumed that these two types of coating did not alter the ice-active surface chemically, and that the coatings were diluted enough in the droplets that were formed prior to the ice nucleation, so that freezing point depression was negligible. However, Fluka kaolinite particles, which were either coated with pure sulfuric acid or were first coated with the acid and then exposed to additional water vapor, both showed a reduced ability to nucleate ice compared to the pure particles. For the CMS kaolinite particles, the ability to nucleate ice in the immersion freezing mode was similar for all examined particles, i.e., for the pure ones and the ones with the different types of coating. Moreover, het derived for the CMS kaolinite particles was comparable to het derived for Fluka kaolinite particles coated with sulfuric acid. This is suggestive for the Fluka kaolinite possessing a type of ice-nucleating surface feature which is not present on the CMS kaolinite, and which can be destroyed by reaction with sulfuric acid. This might be potassium feldspar.
- ItemCCN measurements at the Princess Elisabeth Antarctica research station during three austral summers(Göttingen : Copernicus GmbH, 2019) Herenz, P.; Wex, H.; Mangold, A.; Laffineur, Q.; Gorodetskaya, I.V.; Fleming, Z.L.; Panagi, M.; Stratmann, F.For three austral summer seasons (2013-2016, each from December to February) aerosol particles arriving at the Belgian Antarctic research station Princess Elisabeth (PE) in Dronning Maud Land in East Antarctica were characterized. This included number concentrations of total aerosol particles (N CN ) and cloud condensation nuclei (N CCN ), the particle number size distribution (PNSD), the aerosol particle hygroscopicity, and the influence of the air mass origin on N CN and N CCN . In general N CN was found to range from 40 to 6700cm -3 , with a median of 333cm -3 , while N CCN was found to cover a range between less than 10 and 1300cm-3 for supersaturations (SSs) between 0.1% and 0.7%. It is shown that the aerosol is dominated by the Aitken mode, being characterized by a significant amount of small, and therefore likely secondarily formed, aerosol particles, with 94% and 36% of the aerosol particles smaller than 90 and ≈35nm, respectively. Measurements of the basic meteorological parameters as well as the history of the air masses arriving at the measurement station indicate that the station is influenced by both marine air masses originating from the Southern Ocean and coastal areas around Antarctica (marine events - MEs) and continental air masses (continental events - CEs). CEs, which were defined as instances when the air masses spent at least 90% of the time over the Antarctic continent during the last 10 days prior to arrival at the measurements station, occurred during 61% of the time during which measurements were done. CEs came along with rather constant N CN and N CCN values, which we denote as Antarctic continental background concentrations. MEs, however, cause large fluctuations in N CN and N CCN , with low concentrations likely caused by scavenging due to precipitation and high concentrations likely originating from new particle formation (NPF) based on marine precursors. The application of HYSPLIT back trajectories in form of the potential source contribution function (PSCF) analysis indicate that the region of the Southern Ocean is a potential source of Aitken mode particles. On the basis of PNSDs, together with N CCN measured at an SS of 0.1%, median values for the critical diameter for cloud droplet activation and the aerosol particle hygroscopicity parameter ° were determined to be 110nm and 1, respectively. For particles larger than ĝ‰110nm the Southern Ocean together with parts of the Antarctic ice shelf regions were found to be potential source regions. While the former may contribute sea spray particles directly, the contribution of the latter may be due to the emission of sea salt aerosol particles, released from snow particles from surface snow layers, e.g., during periods of high wind speed, leading to drifting or blowing snow. The region of the Antarctic inland plateau, however, was not found to feature a significant source region for aerosol particles in general or page276 for cloud condensation nuclei measured at the PE station in the austral summer.
- ItemCharacterization of aerosol properties at Cyprus, focusing on cloud condensation nuclei and ice-nucleating particles(Göttingen : Copernicus GmbH, 2019) Gong, X.; Wex, H.; Müller, T.; Wiedensohler, A.; Höhler, K.; Kandler, K.; Ma, N.; Dietel, B.; Schiebel, T.; Möhler, O.; Stratmann, F.As part of the A-LIFE (Absorbing aerosol layers in a changing climate: aging, LIFEtime and dynamics) campaign, ground-based measurements were carried out in Paphos, Cyprus, to characterize the abundance, properties, and sources of aerosol particles in general and cloud condensation nuclei (CCN) and ice-nucleating particles (INP) in particular. New particle formation (NPF) events with subsequent growth of the particles into the CCN size range were observed. Aitken mode particles featured k values of 0.21 to 0.29, indicating the presence of organic materials. Accumulation mode particles featured a higher hygroscopicity parameter, with a median k value of 0.57, suggesting the presence of sulfate and maybe sea salt particles mixed with organic carbon. A clear downward trend of k with increasing supersaturation and decreasing dcrit was found. Super-micron particles originated mainly from sea-spray aerosol (SSA) and partly from mineral dust. INP concentrations (NINP) were measured in the temperature range from-6:5 to-26:5 °C, using two freezing array-type instruments. NINP at a particular temperature span around 1 order of magnitude below-20 °C and about 2 orders of magnitude at warmer temperatures (T >-18 °C). Few samples showed elevated concentrations at temperatures >-15 °C, which suggests a significant contribution of biological particles to the INP population, which possibly could originate from Cyprus. Both measured temperature spectra and NINP probability density functions (PDFs) indicate that the observed INP (ice active in the temperature range between-15 and-20 °C) mainly originate from long-range transport. There was no correlation between NINP and particle number concentration in the size range> 500 nm (N>500 nm). Parameterizations based on N>500 nm were found to overestimate NINP by about 1 to 2 orders of magnitude. There was also no correlation between NINP and particle surface area concentration. The ice active surface site density (ns) for the polluted aerosol encountered in the eastern Mediterranean in this study is about 1 to 3 orders of magnitude lower than the ns found for dust aerosol particles in previous studies. This suggests that observed NINP PDFs such as those derived here could be a better choice for modeling NINP if the aerosol particle composition is unknown or uncertain.