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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.
- 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.
- ItemHygroscopic growth and droplet activation of soot particles: Uncoated, succinic or sulfuric acid coated(München : European Geopyhsical Union, 2012) Henning, S.; Ziese, M.; Kiselev, A.; Saathoff, H.; Möhler, O.; Mentel, T.F.; Buchholz, A.; Spindler, C.; Michaud, V.; Monier, M.; Sellegri, K.; Stratmann, F.The hygroscopic growth and droplet activation of uncoated soot particles and such coated with succinic acid and sulfuric acid were investigated during the IN-11 campaign at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) facility. A GFG-1000 soot generator applying either nitrogen or argon as carrier gas and a miniCAST soot generator were utilized to generate soot particles. Different organic carbon (OC) to black carbon (BC) ratios were adjusted for the CAST-soot by varying the fuel to air ratio. The hygroscopic growth was investigated by means of the mobile Leipzig Aerosol Cloud Interaction Simulator (LACIS-mobile) and two different Hygroscopicity Tandem Differential Mobility Analyzers (HTDMA, VHTDMA). Two Cloud Condensation Nucleus Counter (CCNC) were applied to measure the activation of the particles. For the untreated soot particles neither hygroscopic growth nor activation was observed at a supersaturation of 1%, with exception of a partial activation of GFG-soot generated with argon as carrier gas. Coatings of succinic acid lead to a detectable hygroscopic growth of GFG-soot and enhanced the activated fraction of GFG- (carrier gas: argon) and CAST-soot, whereas no hygroscopic growth of the coated CAST-soot was found. Sulfuric acid coatings led to an OC-content dependent hygroscopic growth of CAST-soot. Such a dependence was not observed for activation measurements. Coating with sulfuric acid decreased the amount of Polycyclic Aromatic Hydrocarbons (PAH), which were detected by AMS-measurements in the CAST-soot, and increased the amount of substances with lower molecular weight than the initial PAHs. We assume that these reaction products increased the hygroscopicity of the coated particles in addition to the coating substance itself.
- ItemApplication of linear polarized light for the discrimination of frozen and liquid droplets in ice nucleation experiments(München : European Geopyhsical Union, 2013) Clauss, T.; Kiselev, A.; Hartmann, S.; Augustin, S.; Pfeifer, S.; Niedermeier, D.; Wex, H.; Stratmann, F.We report on the development and test results of the new optical particle counter TOPS-Ice (Thermo-stabilized Optical Particle Spectrometer for the detection of Ice). The instrument uses measurements of the cross-polarized scattered light by single particles into the near-forward direction (42.5° ± 12.7°) to distinguish between spherical and non-spherical particles. This approach allows the differentiation between liquid water droplets (spherical) and ice particles (non-spherical) having similar volume-equivalent sizes and therefore can be used to determine the fraction of frozen droplets in a typical immersion freezing experiment. We show that the numerical simulation of the light scattered on non-spherical particles (spheroids in random orientation) considering the actual scattering geometry used in the instrument supports the validity of the approach, even though the cross-polarized component of the light scattered by spherical droplets does not vanish in this scattering angle. For the separation of the ice particle mode from the liquid droplet mode, we use the width of the pulse detected in the depolarization channel instead of the pulse height. Exploiting the intrinsic relationship between pulse height and pulse width for Gaussian pulses allows us to calculate the fraction of frozen droplets even if the liquid droplet mode dominates the particle ensemble. We present test results obtained with TOPS-Ice in the immersion freezing experiments at the laminar diffusion chamber LACIS (Leipzig Aerosol Cloud Interaction Simulator) and demonstrate the excellent agreement with the data obtained in similar experiments with a different optical instrument. Finally, the advantages of using the cross-polarized light measurements for the differentiation of liquid and frozen droplets in the realistic immersion freezing experiments are discussed.
- ItemIntercomparing different devices for the investigation of ice nucleating particles using Snomax® as test substance(München : European Geopyhsical Union, 2015) Wex, H.; Augustin-Bauditz, S.; Boose, Y.; Budke, C.; Curtius, J.; Diehl, K.; Dreyer, A.; Frank, F.; Hartmann, S.; Hiranuma, N.; Jantsch, E.; Kanji, Z.A.; Kiselev, A.; Koop, T.; Möhler, O.; Niedermeier, D.; Nillius, B.; Rösch, M.; Rose, D.; Schmidt, C.; Steinke, I.; Stratmann, F.Seven different instruments and measurement methods were used to examine the immersion freezing of bacterial ice nuclei from Snomax® (hereafter Snomax), a product containing ice-active protein complexes from non-viable Pseudomonas syringae bacteria. The experimental conditions were kept as similar as possible for the different measurements. Of the participating instruments, some examined droplets which had been made from suspensions directly, and the others examined droplets activated on previously generated Snomax particles, with particle diameters of mostly a few hundred nanometers and up to a few micrometers in some cases. Data were obtained in the temperature range from −2 to −38 °C, and it was found that all ice-active protein complexes were already activated above −12 °C. Droplets with different Snomax mass concentrations covering 10 orders of magnitude were examined. Some instruments had very short ice nucleation times down to below 1 s, while others had comparably slow cooling rates around 1 K min−1. Displaying data from the different instruments in terms of numbers of ice-active protein complexes per dry mass of Snomax, nm, showed that within their uncertainty, the data agree well with each other as well as to previously reported literature results. Two parameterizations were taken from literature for a direct comparison to our results, and these were a time-dependent approach based on a contact angle distribution (Niedermeier et al., 2014) and a modification of the parameterization presented in Hartmann et al. (2013) representing a time-independent approach. The agreement between these and the measured data were good; i.e., they agreed within a temperature range of 0.6 K or equivalently a range in nm of a factor of 2. From the results presented herein, we propose that Snomax, at least when carefully shared and prepared, is a suitable material to test and compare different instruments for their accuracy of measuring immersion freezing.
- ItemCalibration of LACIS as a CCN detector and its use in measuring activation and hygroscopic growth of atmospheric aerosol particles(München : European Geopyhsical Union, 2006) Wex, H.; Kiselev, A.; Ziese, M.; Stratmann, F.A calibration for LACIS (Leipzig Aerosol Cloud Interaction Simulator) for its use as a CCN (cloud condensation nuclei) detector has been developed. For this purpose, sodium chloride and ammonium sulfate particles of known sizes were generated and their grown sizes were detected at the LACIS outlet. From these signals, the effective critical super-saturation was derived as a function of the LACIS wall temperature. With this, LACIS is calibrated for its use as a CCN detector. The applicability of LACIS for measurements of the droplet activation, and also of the hygroscopic growth of atmospheric aerosol particles was tested. The activation of the urban aerosol particles used in the measurements was found to occur at a critical super-saturation of 0.46% for particles with a dry diameter of 75 nm, and at 0.42% for 85 nm, respectively. Hygroscopic growth was measured for atmospheric aerosol particles with dry diameters of 150, 300 and 350 nm at relative humidities of 98 and 99%, and it was found that the larger dry particles contained a larger soluble volume fraction of about 0.85, compared to about 0.6 for the 150 nm particles.
- ItemLACIS-measurements and parameterization of sea-salt particle hygroscopic growth and activation(München : European Geopyhsical Union, 2008) Niedermeier, D.; Wex, H.; Voigtländer, J.; Stratmann, F.; Brüggemann, E.; Kiselev, A.; Henk, H.; Heintzenberg, J.The Leipzig Aerosol Cloud Interaction Simulator (LACIS) was used to investigate the hygroscopic growth and activation of sea-salt particles which were generated from three different sea-water samples. The measurements showed that the sea-salt particles exhibit a slightly reduced hygroscopic growth compared to pure NaCl particles. Köhler theory was utilized to model the hygroscopic growth of these particles. Some parameters used in this model are unknown for sea-salt. These parameters are combined in an "ionic density" ρion. For each sea-salt sample an average ρion was determined by fitting the Köhler equation to the data from the hygroscopic growth measurements. LACIS was also used to measure the activation of the sea-salt particles at three different supersaturations: 0.11%, 0.17% and 0.32%. A CCN-closure was tested by calculating the critical diameters Dcrit for the sea-salt particles at these supersaturations, using the Köhler model and the corresponding ρion as derived from the hygroscopic growth data. These calculated critical diameters were compared to the measured ones. Measured and calculated values of Dcrit agree within the level of uncertainty. Based on this successful closure, a new parameterization to describe sea-salt-particle hygroscopic growth (at RH>95%) and activation has been developed.