2016, Kupiszewski, Piotr, Zanatta, Marco, Mertes, Stephan, Vochezer, Paul, Lloyd, Gary, Schneider, Johannes, Schenk, Ludwig, Schnaiter, Martin, Baltensperger, Urs, Weingartner, Ernest, Gysel, Martin

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 10−4 to 10−3 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.

2016, Kürten, Andreas, Bianchi, Federico, Almeida, Joao, Kupiainen-Määttä, Oona, Dunne, Eimear M., Duplissy, Jonathan, Williamson, Christina, Barmet, Peter, Breitenlechner, Martin, Dommen, Josef, Donahue, Neil M., Flagan, Richard C., Franchin, Alessandro, Gordon, Hamish, Hakala, Jani, Hansel, Armin, Heinritzi, Martin, Ickes, Luisa, Jokinen, Tuija, Kangasluoma, Juha, Kim, Jaeseok, Kirkby, Jasper, Kupc, Agnieszka, Lehtipalo, Katrianne, Leiminger, Markus, Makhmutov, Vladimir, Onnela, Antti, Ortega, Ismael K., Petäjä, Tuukka, Praplan, Arnaud P., Riccobono, Francesco, Rissanen, Matti P., Rondo, Linda, Schnitzhofer, Ralf, Schobesberger, Siegfried, Smith, James N., Steiner, Gerhard, Stozhkov, Yuri, Tomé, António, Tröstl, Jasmin, Tsagkogeorgas, Georgios, Wagner, Paul E., Wimmer, Daniela, Ye, Penglin, Baltensperger, Urs, Carslaw, Ken, Kulmala, Markku, Curtius, Joachim

Binary nucleation of sulfuric acid and water as well as ternary nucleation involving ammonia are thought to be the dominant processes responsible for new particle formation (NPF) in the cold temperatures of the middle and upper troposphere. Ions are also thought to be important for particle nucleation in these regions. However, global models presently lack experimentally measured NPF rates under controlled laboratory conditions and so at present must rely on theoretical or empirical parameterizations. Here with data obtained in the European Organization for Nuclear Research CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we present the first experimental survey of NPF rates spanning free tropospheric conditions. The conditions during nucleation cover a temperature range from 208 to 298 K, sulfuric acid concentrations between 5 × 105 and 1 × 109 cm−3, and ammonia mixing ratios from zero added ammonia, i.e., nominally pure binary, to a maximum of ~1400 parts per trillion by volume (pptv). We performed nucleation studies under pure neutral conditions with zero ions being present in the chamber and at ionization rates of up to 75 ion pairs cm−3 s−1 to study neutral and ion-induced nucleation. We found that the contribution from ion-induced nucleation is small at temperatures between 208 and 248 K when ammonia is present at several pptv or higher. However, the presence of charges significantly enhances the nucleation rates, especially at 248 K with zero added ammonia, and for higher temperatures independent of NH3 levels. We compare these experimental data with calculated cluster formation rates from the Atmospheric Cluster Dynamics Code with cluster evaporation rates obtained from quantum chemistry.