Atmospheric Chemistry and Physics Discussions www.atmos-chem-phys-discuss.net 1680-7367 1680-7375 9 4 2009 10.5194/acpd-9-15375-2009 http://www.atmos-chem-phys-discuss.net/9/15375/2009/ http://www.atmos-chem-phys-discuss.net/9/15375/2009/acpd-9-15375-2009.html http://www.atmos-chem-phys-discuss.net/9/15375/2009/acpd-9-15375-2009.pdf 15375 15421 2009-07-17 Chemical composition of ambient aerosol, ice residues and cloud droplet residues in mixed-phase clouds: single particle analysis during the Cloud and Aerosol Characterization Experiment (CLACE 6) M. Kamphus M. Ettner-Mahl F. Drewnick L. Keller D. J. Cziczo S. Mertes S. Borrmann J. Curtius curtius@iau.uni-frankfurt.de Institute for Atmospheric Physics, Johannes Gutenberg University, Mainz, Germany Max Planck Institute for Chemistry, Mainz, Germany Institute for Atmospheric and Climate Science, ETH Zurich, Zurich, Switzerland Leibniz Institute for Tropospheric Research, Leipzig, Germany now at: Boehringer Ingelheim Pharma GmbH & Co KG, Ingelheim am Rhein, Germany now at: Atmospheric Science & Global Change Division, Pacific Northwest National Laboratory, Richland, WA, USA now at: Institute for Atmospheric and Environmental Sciences, J. W. Goethe-University Frankfurt, Frankfurt am Main, Germany Two different single particle mass spectrometers were operated in parallel at the Swiss High Alpine Research Station Jungfraujoch (JFJ, 3580 m a.s.l.) during the Cloud and Aerosol Characterization Experiment (CLACE 6) in February and March 2007. During mixed phase cloud events ice crystals from 5 μm up to 20 μm were separated from large ice aggregates, non-activated, interstitial aerosol particles and supercooled droplets using an Ice-Counterflow Virtual Impactor (Ice-CVI). During one cloud period supercooled droplets were additionally sampled and analyzed by changing the Ice-CVI setup. The small ice particles and droplets were evaporated by injection into dry air inside the Ice-CVI. The resulting ice and droplet residues (IR and DR) were analyzed for size and composition by two single particle mass spectrometers: a custom-built Single Particle Laser-Ablation Time-of-Flight Mass Spectrometer (SPLAT) and a commercial Aerosol Time of Flight Mass Spectrometer (ATOFMS, TSI Model 3800). During CLACE 6 the SPLAT instrument characterized 355 individual ice residues that produced a mass spectrum for at least one polarity and the ATOFMS measured 152 particles. The mass spectra were binned in classes, based on the combination of dominating substances, such as mineral dust, sulfate, potassium and elemental carbon or organic material. The derived chemical information from the ice residues is compared to the JFJ ambient aerosol that was sampled while the measurement station was out of clouds (several thousand particles analyzed by SPLAT and ATOFMS) and to the composition of the residues of supercooled cloud droplets (SPLAT: 162 cloud droplet residues analyzed, ATOFMS: 1094). The measurements showed that mineral dust particles were strongly enhanced in the ice particle residues. 57% of the SPLAT spectra from ice residues were dominated by signatures from mineral compounds, and 78% of the ATOFMS spectra. Sulfate and nitrate containing particles were strongly depleted in the ice residues. Sulfate was found to dominate the droplet residues (~90% of the particles). 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