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- ItemCoal fly ash: Linking immersion freezing behavior and physicochemical particle properties(Göttingen : Copernicus GmbH, 2018) Grawe, S.; Augustin-Bauditz, S.; Clemen, H.-C.; Ebert, M.; Eriksen Hammer, S.; Lubitz, J.; Reicher, N.; Rudich, Y.; Schneider, J.; Staacke, R.; Stratmann, F.; Welti, A.; Wex, H.To date, only a few studies have investigated the potential of coal fly ash particles to trigger heterogeneous ice nucleation in cloud droplets. The presented measurements aim at expanding the sparse dataset and improving process understanding of how physicochemical particle properties can influence the freezing behavior of coal fly ash particles immersed in water. Firstly, immersion freezing measurements were performed with two single particle techniques, i.e., the Leipzig Aerosol Cloud Interaction Simulator (LACIS) and the SPectrometer for Ice Nuclei (SPIN). The effect of suspension time on the efficiency of the coal fly ash particles when immersed in a cloud droplet is analyzed based on the different residence times of the two instruments and employing both dry and wet particle generation. Secondly, two cold-stage setups, one using microliter sized droplets (Leipzig Ice Nucleation Array) and one using nanoliter sized droplets (WeIzmann Supercooled Droplets Observation on Microarray setup) were applied. We found that coal fly ash particles are comparable to mineral dust in their immersion freezing behavior when being dry generated. However, a significant decrease in immersion freezing efficiency was observed during experiments with wet-generated particles in LACIS and SPIN. The efficiency of wet-generated particles is in agreement with the cold-stage measurements. In order to understand the reason behind the deactivation, a series of chemical composition, morphology, and crystallography analyses (single particle mass spectrometry, scanning electron microscopy coupled with energy dispersive X-ray microanalysis, X-ray diffraction analysis) were performed with dry- and wet-generated particles. From these investigations, we conclude that anhydrous CaSO4 and CaO - which, if investigated in pure form, show the same qualitative immersion freezing behavior as observed for dry-generated coal fly ash particles - contribute to triggering heterogeneous ice nucleation at the particle-water interface. The observed deactivation in contact with water is related to changes in the particle surface properties which are potentially caused by hydration of CaSO4 and CaO. The contribution of coal fly ash to the ambient population of ice-nucleating particles therefore depends on whether and for how long particles are immersed in cloud droplets.
- ItemThree years of routine Raman lidar measurements of tropospheric aerosols: Backscattering, extinction, and residual layer height(Göttingen : Copernicus GmbH, 2002) Schneider, J.; Eixmann, R.We have performed a three-year series of routine lidar measurements at preselected times. The measurements were performed between 1 December 1997, and 30 November 2000, at Kühlungsborn, Germany (54°07′N, 11°46′E). Using a Rayleigh/Mie/Raman lidar system, we measured the aerosol backscatter coefficients at three wavelengths and the extinction coefficient at one wavelength. The present data analysis focuses on after-sunset Raman measurements obtained on cloud-free days. Aerosol backscatter profiles are available for altitudes above 100 m, while the majority of the extinction measurements has been restricted to heights above the residual layer. The residual layer shows an annual cycle with its maximum height in summer (2000 m) and minimum height in winter (850 m). The backscatter coefficients in the residual layer were found to be about 10 times higher than above. The mean aerosol optical depth above the residual layer and below 5 km is 0.3(±1.0) × 10-2 in summer, and 1.5(±1.0) × 10-2 in winter, which almost is negligible compared to values measured in during daytime in the planetary boundary layer. A cluster analysis of the backward trajectories yielded two major directions of air mass origin above the residual layer and 4 major directions inside. A marked difference between the aerosol properties dependent on the air mass origin could be found for air masses originating from the west and travelling at high wind speeds. Comparing the measured spectral dependence of the backscatter coefficients with data from the Global Aerosol Data Set, we found a general agreement, but only a few conclusions with respect to the aerosol type could be drawn due to the high variability of the measured backscatter coefficients.
- ItemThe impact of mineral dust on cloud formation during the Saharan dust event in April 2014 over Europe(Göttingen : Copernicus GmbH, 2018) Weger, M.; Heinold, B.; Engler, C.; Schumann, U.; Seifert, A.; Fößig, R.; Voigt, C.; Baars, H.; Blahak, U.; Borrmann, S.; Hoose, C.; Kaufmann, S.; Krämer, M.; Seifert, P.; Senf, F.; Schneider, J.; Tegen, I.A regional modeling study on the impact of desert dust on cloud formation is presented for a major Saharan dust outbreak over Europe from 2 to 5 April 2014. The dust event coincided with an extensive and dense cirrus cloud layer, suggesting an influence of dust on atmospheric ice nucleation. Using interactive simulation with the regional dust model COSMO-MUSCAT, we investigate cloud and precipitation representation in the model and test the sensitivity of cloud parameters to dust-cloud and dust-radiation interactions of the simulated dust plume. We evaluate model results with ground-based and spaceborne remote sensing measurements of aerosol and cloud properties, as well as the in situ measurements obtained during the ML-CIRRUS aircraft campaign. A run of the model with single-moment bulk microphysics without online dust feedback considerably underestimated cirrus cloud cover over Germany in the comparison with infrared satellite imagery. This was also reflected in simulated upper-Tropospheric ice water content (IWC), which accounted for only 20 % of the observed values. The interactive dust simulation with COSMO-MUSCAT, including a two-moment bulk microphysics scheme and dust-cloud as well as dust-radiation feedback, in contrast, led to significant improvements. The modeled cirrus cloud cover and IWC were by at least a factor of 2 higher in the relevant altitudes compared to the noninteractive model run. We attributed these improvements mainly to enhanced deposition freezing in response to the high mineral dust concentrations. This was corroborated further in a significant decrease in ice particle radii towards more realistic values, compared to in situ measurements from the ML-CIRRUS aircraft campaign. By testing different empirical ice nucleation parameterizations, we further demonstrate that remaining uncertainties in the ice-nucleating properties of mineral dust affect the model performance at least as significantly as including the online representation of the mineral dust distribution. Dust-radiation interactions played a secondary role for cirrus cloud formation, but contributed to a more realistic representation of precipitation by suppressing moist convection in southern Germany. In addition, a too-low specific humidity in the 7 to 10 km altitude range in the boundary conditions was identified as one of the main reasons for misrepresentation of cirrus clouds in this model study.