Single-particle Characterization of Ice-nucleating Particles and Ice Particle Residuals Sampled by Three Different Techniques , Björn Nillius

In the present work, three different techniques to separate ice-nucleating particles (INP) as well as ice particle residuals (IPR) 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). INP and IPR were analyzed offline by scanning electron microscopy and energy-dispersive X-ray microanalysis to determine their size, chemical composition and mixing state. On-line analysis of the size and chemical composition of INP activated in FINCH was performed by laser ablation mass spectrometry. With all three INP/IPRseparation 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 + INPCVI: 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 %) of soluble material (e.g., sea salt, sulfates) occurred. 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 nm to 400 nm geometric diameter. In a few cases, a second super-micron 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 are 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. Single-particle characterization of ice-nucleating particles and ice particle residuals sampled by three different techniques Annette Worringen (1,7) , Konrad Kandler (1) , Nathalie Benker (1) , Thomas Dirsch (1) , Stephan Mertes (2) , Ludwig Schenk (2) , Udo Kästner (2) , Fabian Frank (3) , Björn Nillius (3,*) , Ulrich Bundke (3,**) , Diana Rose (3) , Joachim Curtius (3) , Piotr Kupiszewski (4) , Ernest Weingartner (4,***) , Paul Vochezer (5) , Johannes Schneider (6) , Susan Schmidt (6) , Stephan Weinbruch (1) , Martin Ebert (1) (1) Institut für Angewandte Geowissenschaften, Technische Universität Darmstadt, Schnittspahnstr. 9, 64287 Darmstadt, Germany (2) Leibniz-Institut für Troposphärenforschung, Permoserstraße 15, 04318 Leipzig, Germany (3) Institut für Atmosphäre und Umwelt, Goethe-Universität Frankfurt am Main, Altenhöferallee 1, 60438 Frankfurt am Main, Germany (4) Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, 5232 Villigen PSI, Switzerland (5) Institute for Meteorology and Climate Research, Karlsruhe Institute of Technology, P.O. Box 3640, 76021 Karlsruhe Germany (6) Max-Planck-Institut für Chemie, Hahn-Meitner-Weg 1, 55128 Mainz, Germany (7) Institut für Physik der Atmosphäre, Johannes Gutenberg Universität Mainz, 55099 Mainz, Germany (*) now at: Max-Planck-Institute für Chemie, Hahn-Meitner-Weg 1, 55128 Mainz, Germany (**) now at: Forschungszentrum Juelich GmbH, 52425 Juelich (***) now at: University of Applied Sciences and Arts Northwestern Switzerland, School of Engineering, Institute of Aerosol and Sensor Technology, Klosterzelgstrasse 2, 5210 Windisch, Switzerland Correspondence to: Stephan Weinbruch ([email protected])