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- ItemHomogeneous and heterogeneous ice nucleation at LACIS: Operating principle and theoretical studies(München : European Geopyhsical Union, 2011) Hartmann, S.; Niedermeier, D.; Voigtländer, J.; Clauss, T.; Shaw, R.A.; Wex, H.; Kiselev, A.; Stratmann, F.At the Leipzig Aerosol Cloud Interaction Simulator (LACIS) experiments investigating homogeneous and heterogeneous nucleation of ice (particularly immersion freezing in the latter case) have been carried out. Here both the physical LACIS setup and the numerical model developed to design experiments at LACIS and interpret their results are presented in detail. Combining results from the numerical model with experimental data, it was found that for the experimental parameter space considered, classical homogeneous ice nucleation theory is able to predict the freezing behavior of highly diluted ammonium sulfate solution droplets, while classical heterogeneous ice nucleation theory, together with the assumption of a constant contact angle, fails to predict the immersion freezing behavior of surrogate mineral dust particles (Arizona Test Dust, ATD). The main reason for this failure is the compared to experimental data apparently overly strong temperature dependence of the nucleation rate coefficient. Assuming, in the numerical model, Classical Nucleation Theory (CNT) for homogeneous ice nucleation and a CNT-based parameterization for the nucleation rate coefficient in the immersion freezing mode, recently published by our group, it was found that even for a relatively effective ice nucleating agent such as pure ATD, there is a temperature range where homogeneous ice nucleation is dominant. The main explanation is the apparently different temperature dependencies of the two freezing mechanisms. Finally, reviewing the assumptions made during the derivation of the CNT-based parameterization for immersion freezing, it was found that the assumption of constant temperature during ice nucleation and the chosen ice nucleation time were justified, underlining the applicability of the method to determine the fitting coefficients in the parameterization equation.
- ItemHeterogeneous ice nucleation: Exploring the transition from stochastic to singular freezing behavior(München : European Geopyhsical Union, 2011) Niedermeier, D.; Shaw, R.A.; Hartmann, S.; Wex, H.; Clauss, T.; Voigtländer, J.; Stratmann, F.Heterogeneous ice nucleation, a primary pathway for ice formation in the atmosphere, has been described alternately as being stochastic, in direct analogy with homogeneous nucleation, or singular, with ice nuclei initiating freezing at deterministic temperatures. We present an idealized, conceptual model to explore the transition between stochastic and singular ice nucleation. This "soccer ball" model treats particles as being covered with surface sites (patches of finite area) characterized by different nucleation barriers, but with each surface site following the stochastic nature of ice embryo formation. The model provides a phenomenological explanation for seemingly contradictory experimental results obtained in our research groups. Even with ice nucleation treated fundamentally as a stochastic process this process can be masked by the heterogeneity of surface properties, as might be typical for realistic atmospheric particle populations. Full evaluation of the model findings will require experiments with well characterized ice nucleating particles and the ability to vary both temperature and waiting time for freezing.
- ItemExperimental study of the role of physicochemical surface processing on the IN ability of mineral dust particles(München : European Geopyhsical Union, 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.
- ItemHeterogeneous freezing of droplets with immersed mineral dust particles – measurements and parameterization(München : European Geopyhsical Union, 2010) Niedermeier, D.; Hartmann, S.; Shaw, R.A.; Covert, D.; Mentel, T.F.; Schneider, J.; Mentel, T.F.; Poulain, L.; Reitz, P.; Spindler, C.; Clauss, T.; Kiselev, A.; Hallbauer, E.; Wex, H.; Mildenberger, K.; Stratmann, F.During the measurement campaign FROST (FReezing Of duST), LACIS (Leipzig Aerosol Cloud Interaction Simulator) was used to investigate the immersion freezing behavior of size selected, coated and uncoated Arizona Test Dust (ATD) particles with a mobility diameter of 300 nm. Particles were coated with succinic acid (C4H6O4), sulfuric acid (H2SO4) and ammonium sulfate ((NH4)2SO4). Ice fractions at mixed-phase cloud temperatures ranging from 233.15 K to 239.15 K (±0.60 K) were determined for all types of particles. In this temperature range, pure ATD particles and those coated with C4H6O4 or small amounts of H2SO4 were found to be the most efficient ice nuclei (IN). ATD particles coated with (NH4)2SO4 were the most inefficient IN. Since the supercooled droplets were highly diluted before freezing occurred, a freezing point suppression due to the soluble material on the particles (and therefore in the droplets) cannot explain this observation. Therefore, it is reasonable to assume that the coatings lead to particle surface alterations which cause the differences in the IN abilities. Two different theoretical approaches based on the stochastic and the singular hypotheses were applied to clarify and parameterize the freezing behavior of the particles investigated. Both approaches describe the experimentally determined results, yielding parameters that can subsequently be used to compare our results to those from other studies. However, we cannot clarify at the current state which of the two approaches correctly describes the investigated immersion freezing process. But both approaches confirm the assumption that the coatings lead to particle surface modifications lowering the nucleation efficiency. The stochastic approach interprets the reduction in nucleation rate from coating as primarily due to an increase in the thermodynamic barrier for ice formation (i.e., changes in interfacial free energies). The singular approach interprets the reduction as resulting from a reduced surface density of active sites.
- ItemThe fine-scale structure of the trade wind cumuli over Barbados – An introduction to the CARRIBA project(München : European Geopyhsical Union, 2013) Siebert, H.; Beals, M.; Bethke, J.; Bierwirth, E.; Conrath, T.; Dieckmann, K.; Ditas, F.; Ehrlich, A.; Farrell, D.; Hartmann, S.; Izaguirre, M.A.; Katzwinkel, J.; Nuijens, L.; Roberts, G.; Schäfer, M.; Shaw, R.A.; Schmeissner, T.; Serikov, I.; Stevens, B.; Stratmann, F.; Wehner, B.; Wendisch, M.; Werner, F.; Wex, H.The CARRIBA (Cloud, Aerosol, Radiation and tuRbulence in the trade wInd regime over BArbados) project, focused on high resolution and collocated measurements of thermodynamic, turbulent, microphysical, and radiative properties of trade wind cumuli over Barbados, is introduced. The project is based on two one-month field campaigns in November 2010 (climatic wet season) and April 2011 (climatic dry season). Observations are based on helicopter-borne and ground-based measurements in an area of 100 km2 off the coast of Barbados. CARRIBA is accompanied by long-term observations at the Barbados Cloud Observatory located at the East coast of Barbados since early in 2010 and which provides a longer-term context for the CARRIBA measurements. The deployed instrumentation and sampling strategy are presented together with a classification of the meteorological conditions. The two campaigns were influenced by different air masses advected from the Caribbean area, the Atlantic Ocean, and the African continent which led to distinct aerosol conditions. Pristine conditions with low aerosol particle number concentrations of ~100 cm3 were alternating with periods influenced by Saharan dust or aerosol from biomass burning resulting in comparably high number concentrations of ~ 500 cm3. The biomass burning aerosol was originating from both the Caribbean area and Africa. The shallow cumulus clouds responded to the different aerosol conditions with a wide range of mean droplet sizes and number concentrations. Two days with different aerosol and cloud microphysical properties but almost identical meteorological conditions have been analyzed in detail. The differences in the droplet number concentration and droplet sizes appear not to show any significant change for turbulent cloud mixing, but the relative roles of droplet inertia and sedimentation in initiating coalescence, as well as the cloud reflectivity, do change substantially.