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- 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.
- ItemThe efficiency of secondary organic aerosol particles acting as ice-nucleating particles under mixed-phase cloud conditions(Katlenburg-Lindau : EGU, 2018) Frey, Wiebke; Hu, Dawei; Dorsey, James; Alfarra, M. Rami; Pajunoja, Aki; Virtanen, Annele; Connolly, Paul; McFiggans, GordonSecondary organic aerosol (SOA) particles have been found to be efficient ice-nucleating particles under the cold conditions of (tropical) upper-tropospheric cirrus clouds. Whether they also are efficient at initiating freezing under slightly warmer conditions as found in mixed-phase clouds remains undetermined. Here, we study the ice-nucleating ability of photochemically produced SOA particles with the combination of the Manchester Aerosol Chamber and Manchester Ice Cloud Chamber. Three SOA systems were tested resembling biogenic and anthropogenic particles as well as particles of different phase state. These are namely α-pinene, heptadecane, and 1,3,5-trimethylbenzene. After the aerosol particles were formed, they were transferred into the cloud chamber, where subsequent quasi-adiabatic cloud activation experiments were performed. Additionally, the ice-forming abilities of ammonium sulfate and kaolinite were investigated as a reference to test the experimental setup.
Clouds were formed in the temperature range of −20 to −28.6 °C. Only the reference experiment using dust particles showed evidence of ice nucleation. No ice particles were observed in any other experiment. Thus, we conclude that SOA particles produced under the conditions of the reported experiments are not efficient ice-nucleating particles starting at liquid saturation under mixed-phase cloud conditions. - ItemIon-particle interactions during particle formation and growth at a coniferous forest site in central Europe(München : European Geopyhsical Union, 2014) Gonser, S.G.; Klein, F.; Birmili, W.; Größ, J.; Kulmala, M.; Manninen, H.E.; Wiedensohler, A.; Held, A.In this work, we examined the interaction of ions and neutral particles during atmospheric new particle formation (NPF) events. The analysis is based on simultaneous field measurements of atmospheric ions and total particles using a neutral cluster and air ion spectrometer (NAIS) across the diameter range 2–25 nm. The Waldstein research site is located in a spruce forest in NE Bavaria, Southern Germany, known for enhanced radon concentrations, presumably leading to elevated ionization rates. Our observations show that the occurrence of the ion nucleation mode preceded that of the total particle nucleation mode during all analyzed NPF events. The time difference between the appearance of 2 nm ions and 2 nm total particles was typically about 20 to 30 min. A cross correlation analysis showed a rapid decrease of the time difference between the ion and total modes during the growth process. Eventually, this time delay vanished when both ions and total particles did grow to larger diameters. Considering the growth rates of ions and total particles separately, total particles exhibited enhanced growth rates at diameters below 15 nm. This observation cannot be explained by condensation or coagulation, because these processes would act more efficiently on charged particles compared to neutral particles. To explain our observations, we propose a mechanism including recombination and attachment of continuously present cluster ions with the ion nucleation mode and the neutral nucleation mode, respectively.
- ItemVariability of sub-micrometer particle number size distributions and concentrations in the Western Mediterranean regional background(Milton Park : Taylor & Francis, 2013) Cusack, Michael; Pérez, NoemÍ; Pey, Jorge; Wiedensohler, Alfred; Alastuey, AndrésThis study focuses on the daily and seasonal variability of particle number size distributions and concentrations, performed at the Montseny (MSY) regional background station in the western Mediterranean from October 2010 to June 2011. Particle number concentrations at MSY were shown to be within range of various other sites across Europe reported in literature, but the seasonality of the particle number size distributions revealed significant differences. The Aitken mode is the dominant particle mode at MSY, with arithmetic mean concentrations of 1698 cm3, followed by the accumulation mode (877 cm3) and the nucleation mode (246 cm3). Concentrations showed a strong seasonal variability with large increases in particle number concentrations observed from the colder to warmer months. The modality of median size distributions was typically bimodal, except under polluted conditions when the size distribution was unimodal. During the colder months, the daily variation of particle number size distributions are strongly influenced by a diurnal breeze system, whereby the Aitken and accumulation modes vary similarly to PM1 and BC mass concentrations, with nocturnal minima and sharp day-time increases owing to the development of a diurnal mountain breeze. Under clean air conditions, high levels of nucleation and lower Aitken mode concentrations were measured, highlighting the importance of new particle formation as a source of particles in the absence of a significant condensation sink. During the warmer months, nucleation mode concentrations were observed to be relatively elevated both under polluted and clean conditions due to increased photochemical reactions, with enhanced subsequent growth owing to elevated concentrations of condensable organic vapours produced from biogenic volatile organic compounds, indicating that nucleation at MSY does not exclusively occur under clean air conditions. Finally, mixing of air masses between polluted and non-polluted boundary layer air, and brief changes in the air mass being sampled gave rise to unusual particle number size distributions, with specific cases of such behaviour discussed at length.
- ItemNucleation of jet engine oil vapours is a large source of aviation-related ultrafine particles(London : Springer Nature, 2022) Ungeheuer, Florian; Caudillo, Lucía; Ditas, Florian; Simon, Mario; van Pinxteren, Dominik; Kılıç, Doğuşhan; Rose, Diana; Jacobi, Stefan; Kürten, Andreas; Curtius, Joachim; Vogel, Alexander L.Large airports are a major source of ultrafine particles, which spread across densely populated residential areas, affecting air quality and human health. Jet engine lubrication oils are detectable in aviation-related ultrafine particles, however, their role in particle formation and growth remains unclear. Here we show the volatility and new-particle-formation ability of a common synthetic jet oil, and the quantified oil fraction in ambient ultrafine particles downwind of Frankfurt International Airport, Germany. We find that the oil mass fraction is largest in the smallest particles (10-18 nm) with 21% on average. Combining ambient particle-phase concentration and volatility of the jet oil compounds, we determine a lower-limit saturation ratio larger than 1 × 105 for ultra-low volatility organic compounds. This indicates that the oil is an efficient nucleation agent. Our results demonstrate that jet oil nucleation is an important mechanism that can explain the abundant observations of high number concentrations of non-refractory ultrafine particles near airports.
- 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.
- ItemThe SPectrometer for Ice Nuclei (SPIN): An instrument to investigate ice nucleation(München : European Geopyhsical Union, 2016) Garimella, Sarvesh; Kristensen, Thomas Bjerring; Ignatius, Karolina; Welti, Andre; Voigtländer, Jens; Kulkarni, Gourihar R.; Sagan, Frank; Kok, Gregory Lee; Dorsey, James; Nichman, Leonid; Rothenberg, Daniel Alexander; Rösch, Michael; Kirchgäßner, Amélie Catharina Ruth; Ladkin, Russell; Wex, Heike; Wilson, Theodore W.; Ladino, Luis Antonio; Abbatt, Jon P.D.; Stetzer, Olaf; Lohmann, Ulrike; Stratmann, Frank; Cziczo, Daniel JamesThe SPectrometer for Ice Nuclei (SPIN) is a commercially available ice nucleating particle (INP) counter manufactured by Droplet Measurement Technologies in Boulder, CO. The SPIN is a continuous flow diffusion chamber with parallel plate geometry based on the Zurich Ice Nucleation Chamber and the Portable Ice Nucleation Chamber. This study presents a standard description for using the SPIN instrument and also highlights methods to analyze measurements in more advanced ways. It characterizes and describes the behavior of the SPIN chamber, reports data from laboratory measurements, and quantifies uncertainties associated with the measurements. Experiments with ammonium sulfate are used to investigate homogeneous freezing of deliquesced haze droplets and droplet breakthrough. Experiments with kaolinite, NX illite, and silver iodide are used to investigate heterogeneous ice nucleation. SPIN nucleation results are compared to those from the literature. A machine learning approach for analyzing depolarization data from the SPIN optical particle counter is also presented (as an advanced use). Overall, we report that the SPIN is able to reproduce previous INP counter measurements.
- ItemColumnar modelling of nucleation burst evolution in the convective boundary layer - First results from a feasibility study, Part I: Modelling approach(München : European Geopyhsical Union, 2006) Hellmuth, O.A high-order modelling approach to interpret "continental-type" particle formation bursts in the anthropogenically influenced convective boundary layer (CBL) is proposed. The model considers third-order closure for planetary boundary layer turbulence, sulphur and ammonia chemistry as well as aerosol dynamics. In Paper I of four papers, previous observations of ultrafine particle evolution are reviewed, model equations are derived, the model setup for a conceptual study on binary and ternary homogeneous nucleation is defined and shortcomings of process parameterisation are discussed. In the subsequent Papers II, III and IV simulation results, obtained within the framework of a conceptual study on the CBL evolution and new particle formation (NPF), will be presented and compared with observational findings.
- ItemIce-nucleating particle versus ice crystal number concentrationin altocumulus and cirrus layers embedded in Saharan dust: a closure study(Katlenburg-Lindau : EGU, 2019) Ansmann, Albert; Mamouri, Rodanthi-Elisavet; Bühl, Johannes; Seifert, Patric; Engelmann, Ronny; Hofer, Julian; Nisantzi, Argyro; Atkinson, James D.; Kanji, Zamin A.; Sierau, Berko; Vrekoussis, Mihalis; Sciare, JeanFor the first time, a closure study of the relationship between the ice-nucleating particle concentration (INP; INPC) and ice crystal number concentration (ICNC) in altocumulus and cirrus layers, solely based on groundbased active remote sensing, is presented. Such aerosol- cloud closure experiments are required (a) to better understand aerosol-cloud interaction in the case of mixed-phase clouds, (b) to explore to what extent heterogeneous ice nucleation can contribute to cirrus formation, which is usually controlled by homogeneous freezing, and (c) to check the usefulness of available INPC parameterization schemes, applied to lidar profiles of aerosol optical and microphysical properties up to the tropopause level. The INPC-ICNC closure studies were conducted in Cyprus (Limassol and Nicosia) during a 6-week field campaign in March-April 2015 and during the 17-month CyCARE (Cyprus Clouds Aerosol and Rain Experiment) campaign. The focus was on altocumulus and cirrus layers which developed in pronounced Saharan dust layers at heights from 5 to 11 km. As a highlight, a long-lasting cirrus event was studied which was linked to the development of a very strong dust-infused baroclinic storm (DIBS) over Algeria. The DIBS was associated with strong convective cloud development and lifted large amounts of Saharan dust into the upper troposphere, where the dust influenced the evolution of an unusually large anvil cirrus shield and the subsequent transformation into an cirrus uncinus cloud system extending from the eastern Mediterranean to central Asia, and thus over more than 3500 km. Cloud top temperatures of the three discussed closure study cases ranged from - 20 to -57 °C. The INPC was estimated from polarization/Raman lidar observations in combination with published INPC parameterization schemes, whereas the ICNC was retrieved from combined Doppler lidar, aerosol lidar, and cloud radar observations of the terminal velocity of falling ice crystals, radar reflectivity, and lidar backscatter in combination with the modeling of backscattering at the 532 and 8.5 mm wavelengths. A good-to-acceptable agreement between INPC (observed before and after the occurrence of the cloud layer under investigation) and ICNC values was found in the discussed three proof-of-concept closure experiments. In these case studies, INPC and ICNC values matched within an order of magnitude (i.e., within the uncertainty ranges of the INPC and ICNC estimates), and they ranged from 0.1 to 10 L-1 in the altocumulus layers and 1 to 50 L-1 in the cirrus layers observed between 8 and 11 km height. The successful closure experiments corroborate the important role of heterogeneous ice nucleation in atmospheric ice formation processes when mineral dust is present. The observed longlasting cirrus event could be fully explained by the presence of dust, i.e., without the need for homogeneous ice nucleation processes. © 2019 Author(s).
- ItemIntercomparing different devices for the investigation of ice nucleating particles using Snomax® as test substance(München : European Geopyhsical Union, 2015) Wex, H.; Augustin-Bauditz, S.; Boose, Y.; Budke, C.; Curtius, J.; Diehl, K.; Dreyer, A.; Frank, F.; Hartmann, S.; Hiranuma, N.; Jantsch, E.; Kanji, Z.A.; Kiselev, A.; Koop, T.; Möhler, O.; Niedermeier, D.; Nillius, B.; Rösch, M.; Rose, D.; Schmidt, C.; Steinke, I.; Stratmann, F.Seven different instruments and measurement methods were used to examine the immersion freezing of bacterial ice nuclei from Snomax® (hereafter Snomax), a product containing ice-active protein complexes from non-viable Pseudomonas syringae bacteria. The experimental conditions were kept as similar as possible for the different measurements. Of the participating instruments, some examined droplets which had been made from suspensions directly, and the others examined droplets activated on previously generated Snomax particles, with particle diameters of mostly a few hundred nanometers and up to a few micrometers in some cases. Data were obtained in the temperature range from −2 to −38 °C, and it was found that all ice-active protein complexes were already activated above −12 °C. Droplets with different Snomax mass concentrations covering 10 orders of magnitude were examined. Some instruments had very short ice nucleation times down to below 1 s, while others had comparably slow cooling rates around 1 K min−1. Displaying data from the different instruments in terms of numbers of ice-active protein complexes per dry mass of Snomax, nm, showed that within their uncertainty, the data agree well with each other as well as to previously reported literature results. Two parameterizations were taken from literature for a direct comparison to our results, and these were a time-dependent approach based on a contact angle distribution (Niedermeier et al., 2014) and a modification of the parameterization presented in Hartmann et al. (2013) representing a time-independent approach. The agreement between these and the measured data were good; i.e., they agreed within a temperature range of 0.6 K or equivalently a range in nm of a factor of 2. From the results presented herein, we propose that Snomax, at least when carefully shared and prepared, is a suitable material to test and compare different instruments for their accuracy of measuring immersion freezing.