scholarly journals The Leipzig Cloud Interaction Simulator (LACIS): operating principle and theoretical studies concerning homogeneous and heterogeneous ice nucleation

2010 ◽  
Vol 10 (11) ◽  
pp. 25577-25617
Author(s):  
S. Hartmann ◽  
D. Niedermeier ◽  
J. Voigtländer ◽  
T. Clauss ◽  
R. A. Shaw ◽  
...  
Keyword(s):  
Experimental Data ◽  
Numerical Model ◽  
Nucleation Rate ◽  
Rate Coefficient ◽  
Ice Nucleation ◽  
Freezing Behavior ◽  
Nucleation Theory ◽  
Dust Particles ◽  
Immersion Freezing ◽  
Heterogeneous Ice Nucleation

Abstract. At the Leipzig 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 parameterization, it was found that the assumption of constant temperature during ice nucleation and the chosen nucleation time were highly justified, underlining the applicability of both the method to determine the fitting coefficients in the parameterization equation, and the validity of the parameterization concept itself.

scholarly journals Homogeneous and heterogeneous ice nucleation at LACIS: operating principle and theoretical studies

2011 ◽  
Vol 11 (4) ◽  
pp. 1753-1767 ◽  
Author(s):  
S. Hartmann ◽  
D. Niedermeier ◽  
J. Voigtländer ◽  
T. Clauss ◽  
R. A. Shaw ◽  
...  
Keyword(s):  
Experimental Data ◽  
Numerical Model ◽  
Nucleation Rate ◽  
Rate Coefficient ◽  
Ice Nucleation ◽  
Freezing Behavior ◽  
Nucleation Theory ◽  
Dust Particles ◽  
Immersion Freezing ◽  
Heterogeneous Ice Nucleation

Abstract. 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.

scholarly journals A new multi-component heterogeneous ice nucleation model and its application to Snomax bacterial particles and a Snomax-illte mineral particle mixture

2017 ◽  
Author(s):  
Hassan Beydoun ◽  
Michael Polen ◽  
Ryan C. Sullivan
Keyword(s):  
Cloud Microphysics ◽  
Ice Nucleation ◽  
Freezing Behavior ◽  
Dust Particles ◽  
Mineral Particle ◽  
Critical Surface ◽  
Wide Range ◽  
Nucleation Model ◽  
Immersion Freezing ◽  
Heterogeneous Ice Nucleation

Abstract. Some biological particles, such as Snomax, are very active ice nucleating particles, inducing heterogeneous freezing in supercooled water at temperatures above −15° C and up to −2° C. Despite their exceptional freezing abilities, large uncertainties remain regarding the atmospheric abundance of biological ice nucleating particles, and their contribution to atmospheric ice nucleation. It has been suggested that small biological ice nucleating macromolecules or fragments can be carried on the surfaces of dust and other atmospheric particles. This could combine the atmospheric abundance of dust particles with the ice nucleating strength of biological material to create strongly enhanced and abundant ice nucleating surfaces in the atmosphere, with significant implications for the budget and distribution of atmospheric ice nucleating particles, and their consequent effects on cloud microphysics and mixed-phase clouds. The new critical surface area “g” framework that was developed by Beydoun et al. (2016), is extended to produce a heterogeneous ice nucleation mixing model that can predict the freezing behavior of multi-component particle surfaces immersed in droplets. The model successfully predicts the immersion freezing properties of droplets containing Snomax bacterial particles across a mass concentration range of seven orders of magnitude, by treating Snomax as comprised of two distinct distributions of heterogeneous ice nucleating activity. Furthermore, the model successfully predicts the immersion freezing behavior of a low concentration mixture of Snomax and illite mineral particles, a proxy for the biological-dust mixtures observed in atmospheric aerosols. It is shown that even at very low Snomax concentrations in the mixture, droplet freezing at higher temperatures is still determined solely by the second less active and more abundant distribution of heterogeneous ice nucleating activity of Snomax, while freezing at lower temperatures is determined solely by the heterogeneous ice nucleating activity of pure illite. This demonstrates that in this proxy system, biological ice nucleating particles do not compromise their ice nucleating activity upon mixing with dust and no new range of intermediary freezing temperatures associated with the mixture of ice nucleating particles of differing activities is produced. The study is the first to directly examine the freezing behavior of a mixture of Snomax and illite and presents the first multi-component ice nucleation model experimentally evaluated using a wide range of ice nucleating particle concentration mixtures in droplets.

scholarly journals A new multicomponent heterogeneous ice nucleation model and its application to Snomax bacterial particles and a Snomax–illite mineral particle mixture

2017 ◽  
Vol 17 (22) ◽  
pp. 13545-13557 ◽  
Author(s):  
Hassan Beydoun ◽  
Michael Polen ◽  
Ryan C. Sullivan
Keyword(s):  
Biological Material ◽  
Cloud Microphysics ◽  
Ice Nucleation ◽  
Freezing Behavior ◽  
Dust Particles ◽  
Critical Surface ◽  
Wide Range ◽  
Nucleation Model ◽  
Immersion Freezing ◽  
Heterogeneous Ice Nucleation

Abstract. Some biological particles, such as Snomax, are very active ice nucleating particles, inducing heterogeneous freezing in supercooled water at temperatures above −15 and up to −2 °C. Despite their exceptional freezing abilities, large uncertainties remain regarding the atmospheric abundance of biological ice nucleating particles, and their contribution to atmospheric ice nucleation. It has been suggested that small biological ice nucleating macromolecules or fragments can be carried on the surfaces of dust and other atmospheric particles. This could combine the atmospheric abundance of dust particles with the ice nucleating strength of biological material to create strongly enhanced and abundant ice nucleating surfaces in the atmosphere, with significant implications for the budget and distribution of atmospheric ice nucleating particles, and their consequent effects on cloud microphysics and mixed-phase clouds. The new critical surface area g framework that was developed by Beydoun et al. (2016) is extended to produce a heterogeneous ice nucleation mixing model that can predict the freezing behavior of multicomponent particle surfaces immersed in droplets. The model successfully predicts the immersion freezing properties of droplets containing Snomax bacterial particles across a mass concentration range of 7 orders of magnitude, by treating Snomax as comprised of two distinct distributions of heterogeneous ice nucleating activity. Furthermore, the model successfully predicts the immersion freezing behavior of a low-concentration mixture of Snomax and illite mineral particles, a proxy for the biological material–dust (bio-dust) mixtures observed in atmospheric aerosols. It is shown that even at very low Snomax concentrations in the mixture, droplet freezing at higher temperatures is still determined solely by the second less active and more abundant distribution of heterogeneous ice nucleating activity of Snomax, while freezing at lower temperatures is determined solely by the heterogeneous ice nucleating activity of pure illite. This demonstrates that in this proxy system, biological ice nucleating particles do not compromise their ice nucleating activity upon mixing with dust and no new range of intermediary freezing temperatures associated with the mixture of ice nucleating particles of differing activities is produced. The study is the first to directly examine the freezing behavior of a mixture of Snomax and illite and presents the first multicomponent ice nucleation model experimentally evaluated using a wide range of ice nucleating particle concentration mixtures in droplets.

scholarly journals A New Ice Nucleation Active Site Parameterization for Desert Dust and Soot

2017 ◽  
Vol 74 (3) ◽  
pp. 699-717 ◽  
Author(s):  
Romy Ullrich ◽  
Corinna Hoose ◽  
Ottmar Möhler ◽  
Monika Niemand ◽  
Robert Wagner ◽  
...  
Keyword(s):  
Active Surface ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Negative Slope ◽  
Organic Carbon Content ◽  
Desert Dust ◽  
Soot Aerosol ◽  
Immersion Freezing ◽  
Heterogeneous Ice Nucleation

Abstract Based on results of 11 yr of heterogeneous ice nucleation experiments at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) chamber in Karlsruhe, Germany, a new empirical parameterization framework for heterogeneous ice nucleation was developed. The framework currently includes desert dust and soot aerosol and quantifies the ice nucleation efficiency in terms of the ice nucleation active surface site (INAS) approach. The immersion freezing INAS densities nS of all desert dust experiments follow an exponential fit as a function of temperature, well in agreement with an earlier analysis of AIDA experiments. The deposition nucleation nS isolines for desert dust follow u-shaped curves in the ice saturation ratio–temperature (Si–T) diagram at temperatures below about 240 K. The negative slope of these isolines toward lower temperatures may be explained by classical nucleation theory (CNT), whereas the behavior toward higher temperatures may be caused by a pore condensation and freezing mechanism. The deposition nucleation measured for soot at temperatures below about 240 K also follows u-shaped isolines with a shift toward higher Si for soot with higher organic carbon content. For immersion freezing of soot aerosol, only upper limits for nS were determined and used to rescale an existing parameterization line. The new parameterization framework is compared to a CNT-based parameterization and an empirical framework as used in models. The comparison shows large differences in shape and magnitude of the nS isolines especially for deposition nucleation. For the application in models, implementation of this new framework is simple compared to that of other expressions.

scholarly journals Laboratory-generated mixtures of mineral dust particles with biological substances: characterization of the particle mixing state and immersion freezing behavior

2016 ◽  
Vol 16 (9) ◽  
pp. 5531-5543 ◽  
Author(s):  
Stefanie Augustin-Bauditz ◽  
Heike Wex ◽  
Cyrielle Denjean ◽  
Susan Hartmann ◽  
Johannes Schneider ◽  
...  
Keyword(s):  
Biological Material ◽  
Mineral Dust ◽  
Research Unit ◽  
Ice Nucleation ◽  
Freezing Behavior ◽  
Dust Particles ◽  
Mixing State ◽  
Nucleation Behavior ◽  
Immersion Freezing

Abstract. Biological particles such as bacteria, fungal spores or pollen are known to be efficient ice nucleating particles. Their ability to nucleate ice is due to ice nucleation active macromolecules (INMs). It has been suggested that these INMs maintain their nucleating ability even when they are separated from their original carriers. This opens the possibility of an accumulation of such INMs in soils, resulting in an internal mixture of mineral dust and INMs. If particles from such soils which contain biological INMs are then dispersed into the atmosphere due to wind erosion or agricultural processes, they could induce ice nucleation at temperatures typical for biological substances, i.e., above −20 up to almost 0 °C, while they might be characterized as mineral dust particles due to a possibly low content of biological material. We conducted a study within the research unit INUIT (Ice Nucleation research UnIT), where we investigated the ice nucleation behavior of mineral dust particles internally mixed with INM. Specifically, we mixed a pure mineral dust sample (illite-NX) with ice active biological material (birch pollen washing water) and quantified the immersion freezing behavior of the resulting particles utilizing the Leipzig Aerosol Cloud Interaction Simulator (LACIS). A very important topic concerning the investigations presented here as well as for atmospheric application is the characterization of the mixing state of aerosol particles. In the present study we used different methods like single-particle aerosol mass spectrometry, Scanning Electron Microscopy (SEM), Energy Dispersive X-ray analysis (EDX), and a Volatility–Hygroscopicity Tandem Differential Mobility Analyser (VH-TDMA) to investigate the mixing state of our generated aerosol. Not all applied methods performed similarly well in detecting small amounts of biological material on the mineral dust particles. Measuring the hygroscopicity/volatility of the mixed particles with the VH-TDMA was the most sensitive method. We found that internally mixed particles, containing ice active biological material, follow the ice nucleation behavior observed for the pure biological particles. We verified this by modeling the freezing behavior of the mixed particles with the Soccerball model (SBM). It can be concluded that a single INM located on a mineral dust particle determines the freezing behavior of that particle with the result that freezing occurs at temperatures at which pure mineral dust particles are not yet ice active.

scholarly journals Immersion freezing of ice nucleating active protein complexes

2012 ◽  
Vol 12 (8) ◽  
pp. 21321-21353 ◽  
Author(s):  
S. Hartmann ◽  
S. Augustin ◽  
T. Clauss ◽  
J. Voigtländer ◽  
D. Niedermeier ◽  
...  
Keyword(s):  
Pseudomonas Syringae ◽  
Nucleation Rate ◽  
Protein Complex ◽  
Protein Complexes ◽  
Ice Nucleation ◽  
Temperature Range ◽  
Immersion Freezing ◽  
New Perspective ◽  
Lower Temperature ◽  
Heterogeneous Ice Nucleation

Abstract. Biological particles, e.g. bacteria and their Ice Nucleating Active (INA) protein complexes, might play an important role for the ice formation in atmospheric mixed-phase clouds. Therefore, the immersion freezing behavior of INA protein complexes generated from a SnomaxTM solution/suspension was investigated as function of temperature in a range of −5 °C to −38 °C at the Leipzig Aerosol Cloud Interaction Simulator (LACIS). The immersion freezing of droplets containing small numbers of INA protein complexes occurs in a temperature range of −7 °C and −10 °C. The experiments performed in the lower temperature range, where all droplets freeze which contain at least one INA protein complex, are used to determine the average number of INA protein complexes present, assuming that the INA protein complexes are Poisson distributed over the droplet ensemble. Knowing the average number of INA protein complexes, the heterogeneous ice nucleation rate and rate coefficient of a single INA protein complex is determined by using the newly-developed CHESS model (stoCHastic model of idEntical poiSSon distributed ice nuclei). Therefore, we assume the ice nucleation process to be of stochastic nature, and a parameterization of the INA protein complex's nucleation rate. Analyzing the results of immersion freezing experiments from literature (SnomaxTM and Pseudomonas syringae bacteria), to results gained in this study, demonstrates that first, a similar temperature dependence of the heterogeneous ice nucleation rate for a single INA protein complex was found in all experiments, second, the shift of the ice fraction curves to higher temperatures can be explained consistently by a higher average number of INA protein complexes being present in the droplet ensemble, and finally the heterogeneous ice nucleation rate of one single INA protein complex might be also applicable for intact Pseudomonas syringae bacteria cells. The results obtained in this study allow a new perspective on the interpretation of immersion freezing experiments considering INA protein complexes and the derived simple parameterization of the heterogeneous ice nucleation rate can be used in cloud resolving models for studying the effect of bacteria induced ice nucleation.

scholarly journals The immersion freezing behavior of mineral dust particles mixed with biological substances

2015 ◽  
Vol 15 (20) ◽  
pp. 29639-29671 ◽  
Author(s):  
S. Augustin-Bauditz ◽  
H. Wex ◽  
C. Denjean ◽  
S. Hartmann ◽  
J. Schneider ◽  
...  
Keyword(s):  
Biological Material ◽  
Mineral Dust ◽  
Fungal Spores ◽  
Birch Pollen ◽  
Ice Nucleation ◽  
Freezing Behavior ◽  
Dust Particles ◽  
Nucleation Behavior ◽  
Biological Particles ◽  
Immersion Freezing

Abstract. Biological particles such as bacteria, fungal spores or pollen are known to be efficient ice nucleating particles. Their ability to nucleate ice is due to ice nucleation active macromolecules (INM). It has been suggested that these INM maintain their nucleating ability even when they are separated from their original carriers. This opens the possibility of an accumulation of such INM in e.g., soils, resulting in an internal mixture of mineral dust and INM. If particles from such soils which contain biological INM are then dispersed into the atmosphere due to wind erosion or agricultural processes, they could induce ice nucleation at temperatures typical for biological substances, i.e., above −20 up to almost 0 °C. To explore this hypothesis, we performed a measurement campaign within the research unit INUIT, where we investigated the ice nucleation behavior of mineral dust particles internally mixed with INM. Specifically, we mixed a pure mineral dust sample (illite-NX) with ice active biological material (birch pollen washing water) and quantified the immersion freezing behavior of the resulting particles utilizing the Leipzig Aerosol Cloud Interaction Simulator (LACIS). To characterize the mixing state of the generated aerosol we used different methods which will also be discussed. We found that internally mixed particles, containing ice active biological material, follow the ice nucleation behavior observed for the purely biological particles, i.e. freezing occurs at temperatures at which mineral dusts themselves are not yet ice active. It can be concluded that INM located on a mineral dust particle determine the freezing behavior of that particle.

scholarly journals Ice nucleation from aqueous NaCl droplets with and without marine diatoms

2011 ◽  
Vol 11 (3) ◽  
pp. 8291-8336 ◽  
Author(s):  
P. A. Alpert ◽  
J. Y. Aller ◽  
D. A. Knopf
Keyword(s):  
Surface Area ◽  
Water Activity ◽  
Nucleation Rate ◽  
Particle Production ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Rate Coefficients ◽  
Freezing Temperatures ◽  
Aqueous Volume ◽  
Heterogeneous Ice Nucleation

Abstract. Ice formation in the atmosphere by homogeneous and heterogeneous nucleation is one of the least understood processes in cloud microphysics and climate. Here we describe our investigation of the marine environment as a potential source of atmospheric IN by experimentally observing homogeneous ice nucleation from aqueous NaCl droplets and comparing against heterogeneous ice nucleation from aqueous NaCl droplets containing intact and fragmented diatoms. Homogeneous and heterogeneous ice nucleation are studied as a function of temperature and water activity, aw. Additional analyses are presented on the dependence of diatom surface area and aqueous volume on heterogeneous freezing temperatures, ice nucleation rates, ωhet, ice nucleation rate coefficients, Jhet, and differential and cumulative ice nuclei spectra, k(T) and K(T), respectively. Homogeneous freezing temperatures and corresponding nucleation rate coefficients are in agreement with the water activity based homogeneous ice nucleation theory within experimental and predictive uncertainties. Our results confirm, as predicted by classical nucleation theory, that a stochastic interpretation can be used to describe this nucleation process. Heterogeneous ice nucleation initiated by intact and fragmented diatoms can be adequately represented by a modified water activity based ice nucleation theory. A horizontal shift in water activity, Δaw, het = 0.2303, of the ice melting curve can describe median heterogeneous freezing temperatures. Individual freezing temperatures showed no dependence on available diatom surface area and aqueous volume. Determined at median diatom freezing temperatures for aw from 0.8 to 0.99, ωhet ~ 0.11+0.06−0.05 s−1, Jhet ~ 1.0+1.16−0.61 × 104 cm−2 s−1, and K ~ 6.2+3.5−4.1 × 104 cm−2. The experimentally derived ice nucleation rates and nuclei spectra allow us to estimate ice particle production which we subsequently use for a comparison with observed ice crystal concentrations typically found in cirrus and polar marine mixed-phase clouds. Differences in application of time-dependent and time-independent analyses to predict ice particle production are discussed.

scholarly journals Ice nucleation from aqueous NaCl droplets with and without marine diatoms

2011 ◽  
Vol 11 (12) ◽  
pp. 5539-5555 ◽  
Author(s):  
P. A. Alpert ◽  
J. Y. Aller ◽  
D. A. Knopf
Keyword(s):  
Surface Area ◽  
Water Activity ◽  
Nucleation Rate ◽  
Particle Production ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Rate Coefficients ◽  
Freezing Temperatures ◽  
Aqueous Volume ◽  
Heterogeneous Ice Nucleation

Abstract. Ice formation in the atmosphere by homogeneous and heterogeneous nucleation is one of the least understood processes in cloud microphysics and climate. Here we describe our investigation of the marine environment as a potential source of atmospheric IN by experimentally observing homogeneous ice nucleation from aqueous NaCl droplets and comparing against heterogeneous ice nucleation from aqueous NaCl droplets containing intact and fragmented diatoms. Homogeneous and heterogeneous ice nucleation are studied as a function of temperature and water activity, aw. Additional analyses are presented on the dependence of diatom surface area and aqueous volume on heterogeneous freezing temperatures, ice nucleation rates, ωhet, ice nucleation rate coefficients, Jhet, and differential and cumulative ice nuclei spectra, k(T) and K(T), respectively. Homogeneous freezing temperatures and corresponding nucleation rate coefficients are in agreement with the water activity based homogeneous ice nucleation theory within experimental and predictive uncertainties. Our results confirm, as predicted by classical nucleation theory, that a stochastic interpretation can be used to describe the homogeneous ice nucleation process. Heterogeneous ice nucleation initiated by intact and fragmented diatoms can be adequately represented by a modified water activity based ice nucleation theory. A horizontal shift in water activity, Δaw, het = 0.2303, of the ice melting curve can describe median heterogeneous freezing temperatures. Individual freezing temperatures showed no dependence on available diatom surface area and aqueous volume. Determined at median diatom freezing temperatures for aw from 0.8 to 0.99, ωhet~0.11+0.06−0.05 s−1, Jhet~1.0+1.16−0.61×104 cm−2 s−1, and K~6.2+3.5−4.1 ×104 cm−2. The experimentally derived ice nucleation rates and nuclei spectra allow us to estimate ice particle production which we subsequently use for a comparison with observed ice crystal concentrations typically found in cirrus and polar marine mixed-phase clouds. Differences in application of time-dependent and time-independent analyses to predict ice particle production are discussed.

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