2011, Niedermeier, D., Hartmann, S., Clauss, T., Wex, H., Kiselev, A., Sullivan, R.C., DeMott, P.J., Petters, M.D., Reitz, P., Schneider, J., Mikhailov, E., Sierau, B., Stetzer, O., Reimann, B., Bundke, U., Shaw, R.A., Buchholz, A., Mentel, T.F., Stratmann, F.

During the measurement campaign FROST 2 (FReezing Of duST 2), the Leipzig Aerosol Cloud Interaction Simulator (LACIS) was used to investigate the influence of various surface modifications on the ice nucleating ability of Arizona Test Dust (ATD) particles in the immersion freezing mode. The dust particles were exposed to sulfuric acid vapor, to water vapor with and without the addition of ammonia gas, and heat using a thermodenuder operating at 250 °C. Size selected, quasi monodisperse particles with a mobility diameter of 300 nm were fed into LACIS and droplets grew on these particles such that each droplet contained a single particle. Temperature dependent frozen fractions of these droplets were determined in a temperature range between −40 °C ≤T≤−28 °C. The pure ATD particles nucleated ice over a broad temperature range with their freezing behavior being separated into two freezing branches characterized through different slopes in the frozen fraction vs. temperature curves. Coating the ATD particles with sulfuric acid resulted in the particles' IN potential significantly decreasing in the first freezing branch (T>−35 °C) and a slight increase in the second branch (T≤−35 °C). The addition of water vapor after the sulfuric acid coating caused the disappearance of the first freezing branch and a strong reduction of the IN ability in the second freezing branch. The presence of ammonia gas during water vapor exposure had a negligible effect on the particles' IN ability compared to the effect of water vapor. Heating in the thermodenuder led to a decreased IN ability of the sulfuric acid coated particles for both branches but the additional heat did not or only slightly change the IN ability of the pure ATD and the water vapor exposed sulfuric acid coated particles. In other words, the combination of both sulfuric acid and water vapor being present is a main cause for the ice active surface features of the ATD particles being destroyed. A possible explanation could be the chemical transformation of ice active metal silicates to metal sulfates. The strongly enhanced reaction between sulfuric acid and dust in the presence of water vapor and the resulting significant reductions in IN potential are of importance for atmospheric ice cloud formation. Our findings suggest that the IN concentration can decrease by up to one order of magnitude for the conditions investigated.

2010, Stratmann, F., Herrmann, E., Petäjä, T., Kulmala, M.

In this work, we modelled activation and growth of silver particles in the water-operated TSI model 3785 water condensation particle counter (WCPC). Our objective was to investigate theoretically how various effects influence the counting efficiency of this CPC. Coupled fluid and particle dynamic processes were modelled with the computational fluid dynamics (CFD) code FLUENT in combination with the Fine Particle Model (FPM) to obtain profiles of temperature, vapour concentration, nucleation rate, and particle size. We found that the counting efficiency of the TSI 3785 for small particles might be affected by the presence of larger particles. Moreover, homogeneous nucleation processes can significantly influence counting efficiency.

2011, Deng, Z.Z., Zhao, C.S., Ma, N., Liu, P.F., Ran, L., Xu, W.Y., Chen, J., Liang, Z., Liang, S., Huang, M.Y., Ma, X.C., Zhang, Q., Quan, J.N., Yan, P., Henning, S., Mildenberger, K., Sommerhage, E., Schäfer, M., Stratmann, F., Wiedensohler, A.

Size-resolved and bulk activation properties of aerosols were measured at a regional/suburban site in the North China Plain (NCP), which is occasionally heavily polluted by anthropogenic aerosol particles and gases. A Cloud Condensation Nuclei (CCN) closure study is conducted with bulk CCN number concentration (NCCN) and calculated CCN number concentration based on the aerosol number size distribution and size-resolved activation properties. The observed CCN number concentration (NCCN-obs) are higher than those observed in other locations than China, with average NCCN-obs of roughly 2000, 3000, 6000, 10 000 and 13 000 cm−3 at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.70%, respectively. An inferred critical dry diameter (Dm) is calculated based on the NCCN-obs and aerosol number size distribution assuming homogeneous chemical composition. The inferred cut-off diameters are in the ranges of 190–280, 160–260, 95–180, 65–120 and 50–100 nm at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.7%, with their mean values 230.1, 198.4, 128.4, 86.4 and 69.2 nm, respectively. Size-resolved activation measurements show that most of the 300 nm particles are activated at the investigated supersaturations, while almost no particles of 30 nm are activated even at the highest supersaturation of 0.72%. The activation ratio increases with increasing supersaturation and particle size. The slopes of the activation curves for ambient aerosols are not as steep as those observed in calibrations with ammonium sulfate suggesting that the observed aerosols is an external mixture of more hygroscopic and hydrophobic particles. The calculated CCN number concentrations (NCCN-calc) based on the size-resolved activation ratio and aerosol number size distribution correlate well with the NCCN-obs, and show an average overestimation of 19%. Sensitivity studies of the CCN closure show that the NCCN at each supersaturation is well predicted with the campaign average of size-resolved activation curves. These results indicate that the aerosol number size distribution is critical in the prediction of possible CCN. The CCN number concentration can be reliably estimated using time-averaged, size-resolved activation efficiencies without accounting for the temporal variations.

2010, Duplissy, J., Enghoff, M.B., Aplin, K.L., Arnold, F., Aufmhoff, H., Avngaard, M., Baltensperger, U., Bondo, T., Bingham, R., Carslaw, K., Curtius, J., David, A., Fastrup, B., Gagné, S., Hahn, F., Harrison, R.G., Kellett, B., Kirkby, J., Kulmala, M., Laakso, L., Laaksonen, A., Lillestol, E., Lockwood, M., Mäkelä, J., Makhmutov, V., Marsh, N.D., Nieminen, T., Onnela, A., Pedersen, E., Pedersen, J.O.P., Polny, J., Reichl, U., Seinfeld, J.H., Sipilä, M., Stozhkov, Y., Stratmann, F., Svensmark, H., Svensmark, J., Veenhof, R., Verheggen, B., Viisanen, Y., Wagner, P.E., Wehrle, G., Weingartner, E., Wex, H., Wilhelmsson, M., Winkler, P.M.

During a 4-week run in October–November 2006, a pilot experiment was performed at the CERN Proton Synchrotron in preparation for the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment, whose aim is to study the possible influence of cosmic rays on clouds. The purpose of the pilot experiment was firstly to carry out exploratory measurements of the effect of ionising particle radiation on aerosol formation from trace H2SO4 vapour and secondly to provide technical input for the CLOUD design. A total of 44 nucleation bursts were produced and recorded, with formation rates of particles above the 3 nm detection threshold of between 0.1 and 100 cm−3s−1, and growth rates between 2 and 37 nm h−1. The corresponding H2O concentrations were typically around 106 cm−3 or less. The experimentally-measured formation rates and \htwosofour concentrations are comparable to those found in the atmosphere, supporting the idea that sulphuric acid is involved in the nucleation of atmospheric aerosols. However, sulphuric acid alone is not able to explain the observed rapid growth rates, which suggests the presence of additional trace vapours in the aerosol chamber, whose identity is unknown. By analysing the charged fraction, a few of the aerosol bursts appear to have a contribution from ion-induced nucleation and ion-ion recombination to form neutral clusters. Some indications were also found for the accelerator beam timing and intensity to influence the aerosol particle formation rate at the highest experimental SO2 concentrations of 6 ppb, although none was found at lower concentrations. Overall, the exploratory measurements provide suggestive evidence for ion-induced nucleation or ion-ion recombination as sources of aerosol particles. However in order to quantify the conditions under which ion processes become significant, improvements are needed in controlling the experimental variables and in the reproducibility of the experiments. Finally, concerning technical aspects, the most important lessons for the CLOUD design include the stringent requirement of internal cleanliness of the aerosol chamber, as well as maintenance of extremely stable temperatures (variations below 0.1 °C