scholarly journals Development, Characterization, and Validation of a Cold Stage-Based Ice Nucleation Array (PKU-INA)

Atmosphere ◽  
2018 ◽  
Vol 9 (9) ◽  
pp. 357 ◽  
Author(s):  
Jie Chen ◽  
Xiangyu Pei ◽  
Hong Wang ◽  
Jingchuan Chen ◽  
Yishu Zhu ◽  
...  
Keyword(s):  
Ice Nucleation ◽  
Temperature Calibration ◽  
Cold Stage ◽  
Reliable Instrument ◽  
Peking University ◽  
Calibration Protocol ◽  
Immersion Freezing ◽  
And Performance ◽  
Good Agreement ◽  
Heterogeneous Ice Nucleation

A drop-freeze array (PeKing University Ice Nucleation Array, PKU-INA) was developed based on the cold-stage method to investigate heterogeneous ice nucleation properties of atmospheric particles in the immersion freezing mode from −30 to 0 °C. The instrumental details as well as characterization and performance evaluation are described in this paper. A careful temperature calibration protocol was developed in our work. The uncertainties in the reported temperatures were found to be less than 0.4 °C at various cooling rates after calibration. We also measured the ice nucleation activities of droplets containing different mass concentrations of illite NX, and the results obtained in our work show good agreement with those reported previously using other instruments with similar principles. Overall, we show that our newly developed PKU-INA is a robust and reliable instrument for investigation of heterogeneous ice nucleation in the immersion freezing mode.

scholarly journals Efficiency of immersion mode ice nucleation on surrogates of mineral dust

2007 ◽  
Vol 7 (19) ◽  
pp. 5081-5091 ◽  
Author(s):  
C. Marcolli ◽  
S. Gedamke ◽  
T. Peter ◽  
B. Zobrist
Keyword(s):  
Contact Angle ◽  
Active Sites ◽  
Quantitative Agreement ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Aqueous Suspensions ◽  
Freezing Temperatures ◽  
Good Agreement ◽  
Heterogeneous Ice Nucleation

Abstract. A differential scanning calorimeter (DSC) was used to explore heterogeneous ice nucleation of emulsified aqueous suspensions of two Arizona test dust (ATD) samples with particle diameters of nominally 0–3 and 0–7 μm, respectively. Aqueous suspensions with ATD concentrations of 0.01–20 wt% have been investigated. The DSC thermograms exhibit a homogeneous and a heterogeneous freezing peak whose intensity ratios vary with the ATD concentration in the aqueous suspensions. Homogeneous freezing temperatures are in good agreement with recent measurements by other techniques. Depending on ATD concentration, heterogeneous ice nucleation occurred at temperatures as high as 256 K or down to the onset of homogeneous ice nucleation (237 K). For ATD-induced ice formation Classical Nucleation Theory (CNT) offers a suitable framework to parameterize nucleation rates as a function of temperature, experimentally determined ATD size, and emulsion droplet volume distributions. The latter two quantities serve to estimate the total heterogeneous surface area present in a droplet, whereas the suitability of an individual heterogeneous site to trigger nucleation is described by the compatibility function (or contact angle) in CNT. The intensity ratio of homogeneous to heterogeneous freezing peaks is in good agreement with the assumption that the ATD particles are randomly distributed amongst the emulsion droplets. The observed dependence of the heterogeneous freezing temperatures on ATD concentrations cannot be described by assuming a constant contact angle for all ATD particles, but requires the ice nucleation efficiency of ATD particles to be (log)normally distributed amongst the particles. Best quantitative agreement is reached when explicitly assuming that high-compatibility sites are rare and that therefore larger particles have on average more and better active sites than smaller ones. This analysis suggests that a particle has to have a diameter of at least 0.1 μm to exhibit on average one active site.

scholarly journals An instrument for quantifying heterogeneous ice nucleation in multiwell plates using infrared emissions to detect freezing

2018 ◽  
Vol 11 (10) ◽  
pp. 5629-5641 ◽  
Author(s):  
Alexander D. Harrison ◽  
Thomas F. Whale ◽  
Rupert Rutledge ◽  
Stephen Lamb ◽  
Mark D. Tarn ◽  
...  
Keyword(s):  
Active Sites ◽  
Freezing Temperature ◽  
Equilibrium Temperature ◽  
Ice Nucleation ◽  
Ir Camera ◽  
Low Concentrations ◽  
Immersion Freezing ◽  
Mixed Phase Clouds ◽  
The City ◽  
Good Agreement

Abstract. Low concentrations of ice-nucleating particles (INPs) are thought to be important for the properties of mixed-phase clouds, but their detection is challenging. Hence, there is a need for instruments where INP concentrations of less than 0.01 L−1 can be routinely and efficiently determined. The use of larger volumes of suspension in drop assays increases the sensitivity of an experiment to rarer INPs or rarer active sites due to the increase in aerosol or surface area of particulates per droplet. Here we describe and characterise the InfraRed-Nucleation by Immersed Particles Instrument (IR-NIPI), a new immersion freezing assay that makes use of IR emissions to determine the freezing temperature of individual 50 µL droplets each contained in a well of a 96-well plate. Using an IR camera allows the temperature of individual aliquots to be monitored. Freezing temperatures are determined by detecting the sharp rise in well temperature associated with the release of heat caused by freezing. In this paper we first present the calibration of the IR temperature measurement, which makes use of the fact that following ice nucleation aliquots of water warm to the ice–liquid equilibrium temperature (i.e. 0 ∘C when water activity is ∼1), which provides a point of calibration for each individual well in each experiment. We then tested the temperature calibration using ∼100 µm chips of K-feldspar, by immersing these chips in 1 µL droplets on an established cold stage (µL-NIPI) as well as in 50 µL droplets on IR-NIPI; the results were consistent with one another, indicating no bias in the reported freezing temperature. In addition we present measurements of the efficiency of the mineral dust NX-illite and a sample of atmospheric aerosol collected on a filter in the city of Leeds. NX-illite results are consistent with literature data, and the atmospheric INP concentrations were in good agreement with the results from the µL-NIPI instrument. This demonstrates the utility of this approach, which offers a relatively high throughput of sample analysis and access to low INP concentrations.

scholarly journals Coal fly ash: linking immersion freezing behavior and physicochemical particle properties

2018 ◽  
Vol 18 (19) ◽  
pp. 13903-13923 ◽  
Author(s):  
Sarah Grawe ◽  
Stefanie Augustin-Bauditz ◽  
Hans-Christian Clemen ◽  
Martin Ebert ◽  
Stine Eriksen Hammer ◽  
...  
Keyword(s):  
Fly Ash ◽  
Single Particle ◽  
Coal Fly Ash ◽  
Ice Nucleation ◽  
Freezing Behavior ◽  
Cloud Droplets ◽  
X Ray ◽  
Particle Properties ◽  
Cold Stage ◽  
Immersion Freezing

Abstract. 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.

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 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 BINARY: an optical freezing array for assessing temperature and time dependence of heterogeneous ice nucleation

2015 ◽  
Vol 8 (2) ◽  
pp. 689-703 ◽  
Author(s):  
C. Budke ◽  
T. Koop
Keyword(s):  
Time Dependence ◽  
Ice Nucleation ◽  
Small Time ◽  
Cooling Rates ◽  
Vapor Transfer ◽  
Ice Nucleators ◽  
Immersion Freezing ◽  
Type Water ◽  
Optical Brightness ◽  
Heterogeneous Ice Nucleation

Abstract. A new optical freezing array for the study of heterogeneous ice nucleation in microliter-sized droplets is introduced, tested and applied to the study of immersion freezing in aqueous Snomax® suspensions. In the Bielefeld Ice Nucleation ARraY (BINARY) ice nucleation can be studied simultaneously in 36 droplets at temperatures down to −40 °C (233 K) and at cooling rates between 0.1 and 10 K min−1. The droplets are separated from each other in individual compartments, thus preventing a Wegener–Bergeron–Findeisen type water vapor transfer between droplets as well as avoiding the seeding of neighboring droplets by formation and surface growth of frost halos. Analysis of freezing and melting occurs via an automated real-time image analysis of the optical brightness of each individual droplet. As an application ice nucleation in water droplets containing Snomax® at concentrations from 1 ng mL−1 to 1 mg mL−1 was investigated. Using different cooling rates, a small time dependence of ice nucleation induced by two different classes of ice nucleators (INs) contained in Snomax® was detected and the corresponding heterogeneous ice nucleation rate coefficient was quantified. The observed time dependence is smaller than those of other types of INs reported in the literature, suggesting that the BINARY setup is suitable for quantifying time dependence for most other INs of atmospheric interest, making it a useful tool for future investigations.

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 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 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.

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