Browsing by Author "Mertes, Stephan"

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    Aerosol partitioning between the interstitial and the condensed phase in mixed‐phase clouds
    (Wiley, 13.12.2007) Verheggen, Bart; Cozic, Julie; Weingartner, Ernest; Bower, Keith; Mertes, Stephan; Connolly, Paul; Gallagher, Martin; Flynn, Michael; Choularton, Tom; Baltensperger, Urs [in: Journal of Geophysical Research: Atmospheres]
    The partitioning of aerosol particles between the cloud and the interstitial phase (i.e., unactivated aerosol) has been investigated during several Cloud and Aerosol Characterization Experiments (CLACE‐3, CLACE‐3½ and CLACE‐4) conducted in winter and summer 2004 and winter 2005 at the high alpine research station Jungfraujoch (3580 m altitude, Switzerland). Ambient air was sampled using different inlets in order to determine the activated fraction of aerosol particles, FN, defined as the fraction of the total aerosol number concentration (with particle diameter dp > 100 nm) that has been incorporated into cloud particles. The liquid and ice water content of mixed‐phase clouds were characterized by analyzing multiple cloud probes. The dependence of the activated fraction on several environmental factors is discussed on the basis of more than 900 h of in‐cloud observations and parameterizations for key variables are given. FN is found to increase with increasing liquid water content and to decrease with increasing particle number concentration in liquid clouds. FN also decreases with increasing cloud ice mass fraction and with decreasing temperature from 0 to −25°C. The Wegener‐Bergeron‐Findeisen process probably contributed to this trend, since the presence of ice crystals causes liquid droplets to evaporate, thus releasing the formerly activated particles back into the interstitial phase. Ice nucleation could also have prevented additional cloud condensation nuclei from activating. The observed activation behavior has significant implications for our understanding of the indirect effect of aerosols on climate.
    01A - Beitrag in wissenschaftlicher Zeitschrift
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    Black carbon enrichment in atmospheric ice particle residuals observed in lower tropospheric mixed phase clouds
    (Wiley, 15.08.2008) Cozic, Julie; Mertes, Stephan; Verheggen, Bart; Cziczo, Daniel James; Gallavardin, Stephane J.; Walter, Saskia; Baltensperger, Urs; Weingartner, Ernest [in: Journal of Geophysical Research: Atmospheres]
    The enrichment of black carbon (BC) mass in residuals of small ice crystals was investigated during intensive experiments in winter 2004 and 2005 at the high alpine research station Jungfraujoch (3580 m asl, Switzerland). Two inlets were used to sample the bulk aerosol (residuals of cloud droplets and ice crystals and nonactivated aerosol particles) and the residual particles of small ice crystals (diameter 5–20 μm). An enrichment of the BC mass fraction in the ice particle residuals was observed by investigating the measured BC mass concentration as a fraction of the bulk (submicrometer) aerosol mass concentration sampled by the two inlets. On the average, the BC mass fraction was 5% for the bulk aerosol but 27% for the ice particle residuals. The observed enrichment of BC in ice particle residuals suggests that some BC‐containing particles may preferentially act as ice nuclei, with important implications for the indirect aerosol effect via glaciation of clouds if these particles represent a significant fraction of the number of ice crystals nucleated.
    01A - Beitrag in wissenschaftlicher Zeitschrift
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    Chemical composition and mixing-state of ice residuals sampled within mixed phase clouds
    (Copernicus, 25.03.2011) Ebert, Martin; Worringen, Annette; Benker, Nathalie; Mertes, Stephan; Weingartner, Ernest; Weinbruch, Stephan [in: Atmospheric Chemistry and Physics]
    Abstract. During an intensive campaign at the high alpine research station Jungfraujoch, Switzerland, in February/March 2006 ice particle residuals within mixed-phase clouds were sampled using the Ice-counterflow virtual impactor (Ice-CVI). Size, morphology, chemical composition, mineralogy and mixing state of the ice residual and the interstitial (i.e., non-activated) aerosol particles were analyzed by scanning and transmission electron microscopy. Ice nuclei (IN) were identified from the significant enrichment of particle groups in the ice residual (IR) samples relative to the interstitial aerosol. In terms of number lead-bearing particles are enriched by a factor of approximately 25, complex internal mixtures with silicates or metal oxides as major components by a factor of 11, and mixtures of secondary aerosol and carbonaceous material (C-O-S particles) by a factor of 2. Other particle groups (sulfates, sea salt, Ca-rich particles, external silicates) observed in the ice-residual samples cannot be assigned unambiguously as IN. Between 9 and 24% of all IR are Pb-bearing particles. Pb was found as major component in around 10% of these particles (PbO, PbCl2). In the other particles, Pb was found as some 100 nm sized agglomerates consisting of 3–8 nm sized primary particles (PbS, elemental Pb). C-O-S particles are present in the IR at an abundance of 17–27%. The soot component within these particles is strongly aged. Complex internal mixtures occur in the IR at an abundance of 9–15%. Most IN identified at the Jungfraujoch station are internal mixtures containing anthropogenic components (either as main or minor constituent), and it is concluded that admixture of the anthropogenic component is responsible for the increased IN efficiency within mixed phase clouds. The mixing state appears to be a key parameter for the ice nucleation behaviour that cannot be predicted from the sole knowledge of the main component of an individual particle.
    01A - Beitrag in wissenschaftlicher Zeitschrift
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    Counterflow virtual impactor based collection of small ice particles in mixed-phase clouds for the physico-chemical characterization of tropospheric ice nuclei. sampler description and first case study
    (Taylor & Francis, 07.09.2007) Mertes, Stephan; Verheggen, Bart; Walter, Saskia; Connolly, Paul; Ebert, Martin; Schneider, Johannes; Bower, Keith N.; Cozic, Julie; Weinbruch, Stephan; Baltensperger, Urs; Weingartner, Ernest [in: Aerosol Science and Technology]
    A ground-based sampling system named Ice-CVI is introduced that is able to extract small ice particles with sizes between 5 and 20 μ m out of mixed-phase clouds. The instrument is based on a counterflow virtual impactor (CVI) removing interstitial particles and is supplemented by additional modules that pre-segregate other constituents of mixed-phase clouds. Ice particles of 20 μ m and smaller are expected to grow only by water vapor diffusion and there is a negligible probability that they scavenge aerosol particles by impaction and riming. Thus, their residuals which are released by the Ice-CVI can be interpreted as the original ice nuclei (IN). In a first field test within the Cloud and Aerosol Characterization Experiment (CLACE-3) at the high alpine research station Jungfraujoch, the collection behavior of the single components and the complete system was evaluated under atmospheric sampling conditions. By comparing parameters measured by the Ice-CVI with corresponding results obtained from other inlets or with in-situ instrumentation it is verified that the small ice particles are representatively collected whereas all other mixed phase cloud constituents are effectively suppressed. In a case study it is observed that super-micrometer particles preferentially serve as IN although in absolute terms the IN concentration is dominated by sub-micrometer particles. Mineral dust (Si), non-volatile organic matter and black carbon could be identified as IN components by means of different chemical analyses. The latter suggests an anthropogenic influence on the heterogeneous ice nucleation in supercooled, tropospheric clouds.
    01A - Beitrag in wissenschaftlicher Zeitschrift
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    Ice residual properties in mixed‐phase clouds at the high‐alpine Jungfraujoch site
    (Wiley, 2016) Kupiszewski, Piotr; Zanatta, Marco; Mertes, Stephan; Vochezer, Paul; Lloyd, Gary; Schneider, Johannes; Schenk, Ludwig; Schnaiter, Martin; Baltensperger, Urs; Weingartner, Ernest; Gysel, Martin [in: Journal of Geophysical Research: Atmospheres]
    Ice residual (IR) and total aerosol properties were measured in mixed‐phase clouds (MPCs) at the high‐alpine Jungfraujoch research station. Black carbon (BC) content and coating thickness of BC‐containing particles were determined using single‐particle soot photometers. The ice activated fraction (IAF), derived from a comparison of IR and total aerosol particle size distributions, showed an enrichment of large particles in the IR, with an increase in the IAF from values on the order of 10−4to 10 for 100 nm (diameter) particles to 0.2 to 0.3 for 1 μm (diameter) particles. Nonetheless, due to the high number fraction of submicrometer particles with respect to total particle number, IR size distributions were still dominated by the submicrometer aerosol. A comparison of simultaneously measured number size distributions of BC‐free and BC‐containing IR and total aerosol particles showed depletion of BC by number in the IR, suggesting that BC does not play a significant role in ice nucleation in MPCs at the Jungfraujoch. The potential anthropogenic climate impact of BC via the glaciation effect in MPCs is therefore likely to be negligible at this site and in environments with similar meteorological conditions and a similar aerosol population. The IAF of the BC‐containing particles also increased with total particle size, in a similar manner as for the BC‐free particles, but on a level 1 order of magnitude lower. Furthermore, BC‐containing IR were found to have a thicker coating than the BC‐containing total aerosol, suggesting the importance of atmospheric aging for ice nucleation.
    01A - Beitrag in wissenschaftlicher Zeitschrift
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    Scavenging of black carbon in mixed phase clouds at the high alpine site Jungfraujoch
    (Copernicus, 11.04.2007) Cozic, Julie; Verheggen, Bart; Mertes, Stephan; Connolly, Paul; Bower, Keith N.; Petzold, Andreas; Baltensperger, Urs; Weingartner, Ernest [in: Atmospheric Chemistry and Physics]
    The scavenging of black carbon (BC) in liquid and mixed phase clouds was investigated during intensive experiments in winter 2004, summer 2004 and winter 2005 at the high alpine research station Jungfraujoch (3580 m a.s.l., Switzerland). Aerosol residuals were sampled behind two well characterized inlets; a total inlet which collected cloud particles (droplets and ice particles) as well as interstitial (unactivated) aerosol particles; an interstitial inlet which collected only interstitial aerosol particles. BC concentrations were measured behind each of these inlets along with the submicrometer aerosol number size distribution, from which a volume concentration was derived. These measurements were complemented by in-situ measurements of cloud microphysical parameters. BC was found to be scavenged into the condensed phase to the same extent as the bulk aerosol, which suggests that BC was covered with soluble material through aging processes, rendering it more hygroscopic. The scavenged fraction of BC (FScav,BC), defined as the fraction of BC that is incorporated into cloud droplets and ice crystals, decreases with increasing cloud ice mass fraction (IMF) from FScav,BC=60% in liquid phase clouds to FScav,BC~5–10% in mixed-phase clouds with IMF>0.2. This can be explained by the evaporation of liquid droplets in the presence of ice crystals (Wegener-Bergeron-Findeisen process), releasing BC containing cloud condensation nuclei back into the interstitial phase. In liquid clouds, the scavenged BC fraction is found to decrease with decreasing cloud liquid water content. The scavenged BC fraction is also found to decrease with increasing BC mass concentration since there is an increased competition for the available water vapour.
    01A - Beitrag in wissenschaftlicher Zeitschrift
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    Single-particle characterization of ice-nucleating particles and ice particle residuals sampled by three different techniques
    (Copernicus, 2015) Worringen, Annette; Kandler, Konrad; Benker, Nathlie; Dirsch, Thomas; Mertes, Stephan; Schenk, Ludwig; Kästner, Udo; Frank, Fabian; Nillius, Björn; Bundke, Ulrich; Rose, D.; Curtius, Joachim; Kupiszewski, Piotr; Weingartner, Ernest; Vochezer, Paul; Schneider, Johannes; Schmidt, S.; Weinbruch, Stephan; Ebert, Martin [in: Atmospheric Chemistry and Physics]
    In the present work, three different techniques to separate ice-nucleating particles (INPs) as well as ice particle residuals (IPRs) from non-ice-active particles are compared. The Ice Selective Inlet (ISI) and the Ice Counterflow Virtual Impactor (Ice-CVI) sample ice particles from mixed-phase clouds and allow after evaporation in the instrument for the analysis of the residuals. The Fast Ice Nucleus Chamber (FINCH) coupled with the Ice Nuclei Pumped Counterflow Virtual Impactor (IN-PCVI) provides ice-activating conditions to aerosol particles and extracts the activated particles for analysis. The instruments were run during a joint field campaign which took place in January and February 2013 at the High Alpine Research Station Jungfraujoch (Switzerland). INPs and IPRs were analyzed offline by scanning electron microscopy and energy-dispersive X-ray microanalysis to determine their size, chemical composition and mixing state. Online analysis of the size and chemical composition of INP activated in FINCH was performed by laser ablation mass spectrometry. With all three INP/IPR separation techniques high abundances (median 20–70%) of instrumental contamination artifacts were observed (ISI: Si-O spheres, probably calibration aerosol; Ice-CVI: Al-O particles; FINCH + IN-PCVI: steel particles). After removal of the instrumental contamination particles, silicates, Ca-rich particles, carbonaceous material and metal oxides were the major INP/IPR particle types obtained by all three techniques. In addition, considerable amounts (median abundance mostly a few percent) of soluble material (e.g., sea salt, sulfates) were observed. As these soluble particles are often not expected to act as INP/IPR, we consider them as potential measurement artifacts. Minor types of INP/IPR include soot and Pb-bearing particles. The Pb-bearing particles are mainly present as an internal mixture with other particle types. Most samples showed a maximum of the INP/IPR size distribution at 200–400 nm in geometric diameter. In a few cases, a second supermicron maximum was identified. Soot/carbonaceous material and metal oxides were present mainly in the sub-micrometer range. Silicates and Ca-rich particles were mainly found with diameters above 1 μm (using ISI and FINCH), in contrast to the Ice-CVI which also sampled many submicron particles of both groups. Due to changing meteorological conditions, the INP/IPR composition was highly variable if different samples were compared. Thus, the observed discrepancies between the different separation techniques may partly result from the non-parallel sampling. The differences of the particle group relative number abundance as well as the mixing state of INP/IPR clearly demonstrate the need of further studies to better understand the influence of the separation techniques on the INP/IPR chemical composition. Also, it must be concluded that the abundance of contamination artifacts in the separated INP and IPR is generally large and should be corrected for, emphasizing the need for the accompanying chemical measurements. Thus, further work is needed to allow for routine operation of the three separation techniques investigated.
    01A - Beitrag in wissenschaftlicher Zeitschrift
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    The ice selective inlet. a novel technique for exclusive extraction of pristine ice crystals in mixed-phase clouds
    (Copernicus, 2015) Kupiszewski, Piotr; Weingartner, Ernest; Vochezer, Paul; Schnaiter, Martin; Bigi, Alessandro; Gysel, Martin; Rosati, Bernadette; Toprak, Emre; Mertes, Stephan; Baltensperger, Urs [in: Atmospheric Measurement Techniques]
    Climate predictions are affected by high uncertainties partially due to an insufficient knowledge of aerosol–cloud interactions. One of the poorly understood processes is formation of mixed-phase clouds (MPCs) via heterogeneous ice nucleation. Field measurements of the atmospheric ice phase in MPCs are challenging due to the presence of much more numerous liquid droplets. The Ice Selective Inlet (ISI), presented in this paper, is a novel inlet designed to selectively sample pristine ice crystals in mixed-phase clouds and extract the ice residual particles contained within the crystals for physical and chemical characterization. Using a modular setup composed of a cyclone impactor, droplet evaporation unit and pumped counterflow virtual impactor (PCVI), the ISI segregates particles based on their inertia and phase, exclusively extracting small ice particles between 5 and 20 μm in diameter. The setup also includes optical particle spectrometers for analysis of the number size distribution and shape of the sampled hydrometeors. The novelty of the ISI is a droplet evaporation unit, which separates liquid droplets and ice crystals in the airborne state, thus avoiding physical impaction of the hydrometeors and limiting potential artefacts. The design and validation of the droplet evaporation unit is based on modelling studies of droplet evaporation rates and computational fluid dynamics simulations of gas and particle flows through the unit. Prior to deployment in the field, an inter-comparison of the optical particle size spectrometers and a characterization of the transmission efficiency of the PCVI was conducted in the laboratory. The ISI was subsequently deployed during the Cloud and Aerosol Characterization Experiment (CLACE) 2013 and 2014 – two extensive international field campaigns encompassing comprehensive measurements of cloud microphysics, as well as bulk aerosol, ice residual and ice nuclei properties. The campaigns provided an important opportunity for a proof of concept of the inlet design. In this work we present the setup of the ISI, including the modelling and laboratory characterization of its components, as well as field measurements demonstrating the ISI performance and validating the working principle of the inlet. Finally, measurements of biological aerosol during a Saharan dust event (SDE) are presented, showing a first indication of enrichment of bio-material in sub-2 μm ice residuals.
    01A - Beitrag in wissenschaftlicher Zeitschrift