Supplementary material to "Heterogeneous ice nucleation on dust particles sourced from 9 deserts worldwide – Part 1: Immersion freezing"

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.

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

Atmospheric Chemistry and Physics ◽

10.5194/acp-17-13545-2017 ◽

2017 ◽

Vol 17 (22) ◽

pp. 13545-13557 ◽

Cited By ~ 11

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.

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

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-10-25577-2010 ◽

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.

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

Atmospheric Chemistry and Physics ◽

10.5194/acp-11-1753-2011 ◽

2011 ◽

Vol 11 (4) ◽

pp. 1753-1767 ◽

Cited By ~ 54

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.

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Integrating laboratory and field data to quantify the immersion freezing ice nucleation activity of mineral dust particles

Atmospheric Chemistry and Physics ◽

10.5194/acp-15-393-2015 ◽

2015 ◽

Vol 15 (1) ◽

pp. 393-409 ◽

Cited By ~ 157

Author(s):

P. J. DeMott ◽

A. J. Prenni ◽

G. R. McMeeking ◽

R. C. Sullivan ◽

M. D. Petters ◽

...

Keyword(s):

Mineral Dust ◽

Order Approximation ◽

Ice Nucleation ◽

Calibration Factor ◽

Dust Particles ◽

Single Type ◽

Aerosol Layer ◽

Atmospheric Measurements ◽

Immersion Freezing ◽

Nucleation Activity

Abstract. Data from both laboratory studies and atmospheric measurements are used to develop an empirical parameterization for the immersion freezing activity of natural mineral dust particles. Measurements made with the Colorado State University (CSU) continuous flow diffusion chamber (CFDC) when processing mineral dust aerosols at a nominal 105% relative humidity with respect to water (RHw) are taken as a measure of the immersion freezing nucleation activity of particles. Ice active frozen fractions vs. temperature for dusts representative of Saharan and Asian desert sources were consistent with similar measurements in atmospheric dust plumes for a limited set of comparisons available. The parameterization developed follows the form of one suggested previously for atmospheric particles of non-specific composition in quantifying ice nucleating particle concentrations as functions of temperature and the total number concentration of particles larger than 0.5 μm diameter. Such an approach does not explicitly account for surface area and time dependencies for ice nucleation, but sufficiently encapsulates the activation properties for potential use in regional and global modeling simulations, and possible application in developing remote sensing retrievals for ice nucleating particles. A calibration factor is introduced to account for the apparent underestimate (by approximately 3, on average) of the immersion freezing fraction of mineral dust particles for CSU CFDC data processed at an RHw of 105% vs. maximum fractions active at higher RHw. Instrumental factors that affect activation behavior vs. RHw in CFDC instruments remain to be fully explored in future studies. Nevertheless, the use of this calibration factor is supported by comparison to ice activation data obtained for the same aerosols from Aerosol Interactions and Dynamics of the Atmosphere (AIDA) expansion chamber cloud parcel experiments. Further comparison of the new parameterization, including calibration correction, to predictions of the immersion freezing surface active site density parameterization for mineral dust particles, developed separately from AIDA experimental data alone, shows excellent agreement for data collected in a descent through a Saharan aerosol layer. These studies support the utility of laboratory measurements to obtain atmospherically relevant data on the ice nucleation properties of dust and other particle types, and suggest the suitability of considering all mineral dust as a single type of ice nucleating particle as a useful first-order approximation in numerical modeling investigations.

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Heterogeneous Ice Nucleation of Aqueous Solutions with Immersed Mineral Dust Particles

Nucleation and Atmospheric Aerosols ◽

10.1007/978-1-4020-6475-3_92 ◽

2007 ◽

pp. 461-465

Author(s):

C. Marcolli ◽

T. Peter ◽

B. Zobrist ◽

Thomas Koop

Keyword(s):

Aqueous Solutions ◽

Mineral Dust ◽

Ice Nucleation ◽

Dust Particles ◽

Heterogeneous Ice Nucleation

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Influence of organic and biogenic substances on the ice nucleation properties of mineral dust particles

10.5194/egusphere-egu2020-19183 ◽

2020 ◽

Author(s):

Kristian Klumpp ◽

Claudia Marcolli ◽

Thomas Peter

Keyword(s):

Amino Acids ◽

Organic Acids ◽

Mineral Dust ◽

Particle Surface ◽

Ice Nucleation ◽

Dust Particles ◽

Biogenic Substances ◽

Immersion Freezing ◽

Mixed Phase Clouds ◽

Ice Nucleation Activity

The formation of ice in mixed phase clouds occurs in the presence of aerosol particles with the ability to nucleate ice on their surface. These ice-nucleating particles (INPs) represent usually a small fraction of particles in an atmospheric aerosol. One of the main particle types which act as INPs are mineral dust particles. Among other factors, the accumulation of semivolatile substances on the particle surface can alter the ice nucleation properties of such particles.In recent immersion freezing experiments, we investigated the influence of organic acids, amino acids and polyols on the highly ice nucleation active K-feldspar microcline. Microcline dust was suspended in solutions of the above-mentioned substances and frozen in a differential scanning calorimeter (DSC). These experiments give us insight into the ice nucleation characteristics of the particles in the presence of the tested organic and biogenic substances. Our measurements show an overall decrease in ice nucleation activity of microcline in the presence of organic acids and amino acids.

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Chemical processing does not always impair heterogeneous ice nucleation of mineral dust particles

Geophysical Research Letters ◽

10.1029/2010gl045540 ◽

2010 ◽

Vol 37 (24) ◽

pp. n/a-n/a ◽

Cited By ~ 87

Author(s):

Ryan C. Sullivan ◽

Lorena Miñambres ◽

Paul J. DeMott ◽

Anthony J. Prenni ◽

Christian M. Carrico ◽

...

Keyword(s):

Mineral Dust ◽

Ice Nucleation ◽

Dust Particles ◽

Chemical Processing ◽

Heterogeneous Ice Nucleation

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The WeIzmann Supercooled Droplets Observation on a Microarray (WISDOM) and application for ambient dust

Atmospheric Measurement Techniques ◽

10.5194/amt-11-233-2018 ◽

2018 ◽

Vol 11 (1) ◽

pp. 233-248 ◽

Cited By ~ 21

Author(s):

Naama Reicher ◽

Lior Segev ◽

Yinon Rudich

Keyword(s):

Active Surface ◽

Ice Nucleation ◽

Saharan Dust ◽

Dust Particles ◽

Active Surface Site ◽

Immersion Freezing ◽

Measurement Uncertainties ◽

Homogeneous Freezing ◽

Validation Experiments

Abstract. The WeIzmann Supercooled Droplets Observation on Microarray (WISDOM) is a new setup for studying ice nucleation in an array of monodisperse droplets for atmospheric implications. WISDOM combines microfluidics techniques for droplets production and a cryo-optic stage for observation and characterization of freezing events of individual droplets. This setup is designed to explore heterogeneous ice nucleation in the immersion freezing mode, down to the homogeneous freezing of water (235 K) in various cooling rates (typically 0.1–10 K min−1). It can also be used for studying homogeneous freezing of aqueous solutions in colder temperatures. Frozen fraction, ice nucleation active surface site densities and freezing kinetics can be obtained from WISDOM measurements for hundreds of individual droplets in a single freezing experiment. Calibration experiments using eutectic solutions and previously studied materials are described. WISDOM also allows repeatable cycles of cooling and heating for the same array of droplets. This paper describes the WISDOM setup, its temperature calibration, validation experiments and measurement uncertainties. Finally, application of WISDOM to study the ice nucleating particle (INP) properties of size-selected ambient Saharan dust particles is presented.

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

Journal of the Atmospheric Sciences ◽

10.1175/jas-d-16-0074.1 ◽

2017 ◽

Vol 74 (3) ◽

pp. 699-717 ◽

Cited By ~ 64

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.

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