Auflistung nach Autor:in "Cziczo, Daniel J."
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Publikation In situ determination of atmospheric aerosol composition as a function of hygroscopic growth(Wiley, 30.08.2008) Herich, Hanna; Kammermann, Lukas; Gysel, Martin; Weingartner, Ernest; Baltensperger, Urs; Lohmann, Ulrike; Cziczo, Daniel J.An in situ measurement setup to determine the chemical composition of aerosols as a function of hygroscopicity is presented. This has been done by connecting a custom‐built Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) and an Aerosol Time‐of‐Flight Mass Spectrometer (ATOFMS), commercially available from TSI (Model 3800). Single particle bipolar mass spectra from aerosols leaving the HTDMA could thus be obtained as a function of the hygroscopic growth factor. For these studies the HTDMA was set at a relative humidity of 82% and particles with a dry diameter of 260 nm were selected. The setup was first laboratory tested, after which field experiments were performed. Two data sets were obtained during wintertime 2007 in Switzerland: the first in the urban Zurich environment and the other at the remote high alpine research station Jungfraujoch (JFJ). In Zurich, several thousand mass spectra were obtained in less than 2 days of sampling due to a high aerosol loading. At the JFJ, due to low particle concentrations in free tropospheric air masses, a longer sampling period was required. Both in Zurich and at the JFJ, two different growth factor modes were observed. Results from these two locations show that most aerosol particles were a mixture of several compounds. A large contribution of organics and combustion species was found in the less hygroscopic growth mode for both locations. Noncombustion refractory material (e.g., metals, mineral dust, and fly ash) was also highly enhanced in the nonhygroscopic particles. Sulfate, normally considered highly soluble, was found to be a constituent in almost all particles independent of their hygroscopic growth factor.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Subarctic atmospheric aerosol composition. 3. Measured and modeled properties of cloud condensation nuclei(Wiley, 19.02.2010) Kammermann, Lukas; Gysel, Martin; Weingartner, Ernest; Herich, Hanna; Cziczo, Daniel J.; Holst, Thomas; Svenningsson, Birgitta; Arneth, Almut; Baltensperger, UrsAerosol particles can modify cloud properties by acting as cloud condensation nuclei (CCN). Predicting CCN properties is still a challenge and not properly incorporated in current climate models. Atmospheric particle number size distributions, hygroscopic growth factors, and polydisperse CCN number concentrations were measured at the remote subarctic Stordalen mire, 200 km north of the Arctic Circle in northern Sweden. The CCN number concentration was highly variable, largely driven by variations in the total number of sufficiently large particles, though the variability of chemical composition was increasingly important for decreasing supersaturation. The hygroscopicity of particles measured by a hygroscopicity tandem differential mobility analyzer (HTDMA) was in agreement with large critical diameters observed for CCN activation (κ ≈ 0.07–0.21 for D = 50–200 nm). Size distribution and time‐ and size‐resolved HTDMA data were used to predict CCN number concentrations. Agreement of predictions with measured CCN within ±11% was achieved using parameterized Köhler theory and assuming a surface tension of pure water. The sensitivity of CCN predictions to various simplifying assumptions was further explored: We found that (1) ignoring particle mixing state did not affect CCN predictions, (2) averaging the HTDMA data in time with retaining the size dependence did not introduce a substantial bias, while individual predictions became more uncertain, and (3) predictions involving the hygroscopicity parameter recommended in literature for continental sites (κ ≈ 0.3 ± 0.1) resulted in a significant prediction bias. Future modeling studies should therefore at least aim at using averaged, size‐resolved, site‐specific hygroscopicity or chemical composition data for predictions of CCN number concentrations.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Subarctic atmospheric aerosol composition: 2. Hygroscopic growth properties(Wiley, 10.07.2009) Herich, Hanna; Kammermann, Lukas; Friedman, Beth; Gross, Deborah S.; Weingartner, Ernest; Lohmann, Ulrike; Spichtinger, Peter; Gysel, Martin; Baltensperger, Urs; Cziczo, Daniel J.Subarctic aerosols were sampled during July 2007 at the Abisko Scientific Research Station Stordalen site in northern Sweden with an instrument setup consisting of a custom‐built Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) connected in series to a single particle mass spectrometer. Aerosol chemical composition in the form of bipolar single particle mass spectra was determined as a function of hygroscopic growth both in situ and in real time. The HTDMA was deployed at a relative humidity of 82%, and particles with a dry mobility diameter of 260 nm were selected. Aerosols from two distinct air masses were analyzed during the sampling period. Sea salt aerosols were found to be the dominant particle group with the highest hygroscopicity. High intensities of sodium and related peaks in the mass spectra were identified as exclusive markers for large hygroscopic growth. Particles from biomass combustion were found to be the least hygroscopic aerosol category. Species normally considered soluble (e.g., sulfates and nitrates) were found in particles ranging from high to low hygroscopicity. Furthermore, the signal intensities of the peaks related to these species did not correlate with hygroscopicity.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Water uptake of clay and desert dust aerosol particles at sub- and supersaturated water vapor conditions(Royal Society of Chemistry, 01.04.2009) Herich, Hanna; Tritscher, Torsten; Wiacek, Aldona; Gysel, Martin; Weingartner, Ernest; Lohmann, Ulrike; Baltensperger, Urs; Cziczo, Daniel J.Airborne mineral dust particles serve as cloud condensation nuclei (CCN), thereby influencing the formation and properties of warm clouds. It is therefore of atmospheric interest how dust aerosols with different mineralogy behave when exposed to high relative humidity (RH) or supersaturation (SS) with respect to liquid water. In this study the subsaturated hygroscopic growth and the supersaturated cloud condensation nucleus activity of pure clays and real desert dust aerosols were determined using a hygroscopicity tandem differential mobility analyzer (HTDMA) and a cloud condensation nuclei counter (CCNC), respectively. Five different illite, montmorillonite and kaolinite clay samples as well as three desert dust samples (Saharan dust (SD), Chinese dust (CD) and Arizona test dust (ATD)) were investigated. Aerosols were generated both with a wet and a dry disperser. The water uptake was parameterized via the hygroscopicity parameter k. The hygroscopicity of dry generated dust aerosols was found to be negligible when compared to processed atmospheric aerosols, with CCNC derived k values between 0.00 and 0.02 (the latter corresponds to a particle consisting of 96.7% by volume insoluble material and B3.3% ammonium sulfate). Pure clay aerosols were generally found to be less hygroscopic than natural desert dust particles. The illite and montmorillonite samples had k B 0.003. The kaolinite samples were less hygroscopic and had k = 0.001. SD (k = 0.023) was found to be the most hygroscopic dry-generated desert dust followed by CD (k = 0.007) and ATD (k = 0.003). Wet-generated dust showed an increased water uptake when compared to dry-generated samples. This is considered to be an artifact introduced by redistribution of soluble material between the particles. Thus, the generation method is critically important when presenting such data. These results indicate any atmospheric processing of a fresh mineral dust particle which leads to the addition of more than B3% soluble material will significantly enhance its hygroscopicity and CCN activity.01A - Beitrag in wissenschaftlicher Zeitschrift