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 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 A new temperature- and humidity-dependent surface site density approach for deposition ice nucleation

2015 ◽  
Vol 15 (7) ◽  
pp. 3703-3717 ◽  
Author(s):  
I. Steinke ◽  
C. Hoose ◽  
O. Möhler ◽  
P. Connolly ◽  
T. Leisner
Keyword(s):  
Contact Angle ◽  
Relative Humidity ◽  
Active Surface ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Aerosol Size Distribution ◽  
Surface Site ◽  
Linear Behavior ◽  
Temperature And Humidity

Abstract. Deposition nucleation experiments with Arizona Test Dust (ATD) as a surrogate for mineral dusts were conducted at the AIDA cloud chamber at temperatures between 220 and 250 K. The influence of the aerosol size distribution and the cooling rate on the ice nucleation efficiencies was investigated. Ice nucleation active surface site (INAS) densities were calculated to quantify the ice nucleation efficiency as a function of temperature, humidity and the aerosol surface area concentration. Additionally, a contact angle parameterization according to classical nucleation theory was fitted to the experimental data in order to relate the ice nucleation efficiencies to contact angle distributions. From this study it can be concluded that the INAS density formulation is a very useful tool to describe the temperature- and humidity-dependent ice nucleation efficiency of ATD particles. Deposition nucleation on ATD particles can be described by a temperature- and relative-humidity-dependent INAS density function ns(T, Sice) with ns(xtherm) = 1.88 ×105 · exp(0.2659 · xtherm) [m−2] , (1) where the temperature- and saturation-dependent function xtherm is defined as xtherm = −(T−273.2)+(Sice−1) ×100, (2) with the saturation ratio with respect to ice Sice >1 and within a temperature range between 226 and 250 K. For lower temperatures, xtherm deviates from a linear behavior with temperature and relative humidity over ice. Also, two different approaches for describing the time dependence of deposition nucleation initiated by ATD particles are proposed. Box model estimates suggest that the time-dependent contribution is only relevant for small cooling rates and low number fractions of ice-active particles.

scholarly journals Immersion freezing of water and aqueous ammonium sulfate droplets initiated by humic-like substances as a function of water activity

2013 ◽  
Vol 13 (13) ◽  
pp. 6603-6622 ◽  
Author(s):  
Y. J. Rigg ◽  
P. A. Alpert ◽  
D. A. Knopf
Keyword(s):  
Water Activity ◽  
Active Sites ◽  
Melting Curve ◽  
Contact Angles ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Surface Areas ◽  
Immersion Freezing ◽  
Freezing Temperatures

Abstract. Immersion freezing of water and aqueous (NH4)2SO4 droplets containing leonardite (LEO) and Pahokee peat (PP) serving as surrogates for humic-like substances (HULIS) has been investigated. Organic aerosol containing HULIS are ubiquitous in the atmosphere; however, their potential for ice cloud formation is uncertain. Immersion freezing has been studied for temperatures as low as 215 K and solution water activity, aw, from 0.85 to 1.0. The freezing temperatures of water and aqueous solution droplets containing LEO and PP are 5–15 K warmer than homogeneous ice nucleation temperatures. Heterogeneous freezing temperatures can be represented by a horizontal shift of the ice melting curve as a function of solution aw by Δaw = 0.2703 and 0.2466, respectively. Corresponding hetrogeneous ice nucleation rate coefficients, Jhet, are (9.6 ± 2.5)×104 and (5.4 ± 1.4)×104 cm−2 s−1 for LEO and PP containing droplets, respectively, and remain constant along freezing curves characterized by Δaw. Consequently predictions of freezing temperatures and kinetics can be made without knowledge of the solute type when relative humidity and ice nuclei (IN) surface areas are known. The acquired ice nucleation data are applied to evaluate different approaches to fit and reproduce experimentally derived frozen fractions. In addition, we apply a basic formulation of classical nucleation theory (α(T)-model) to calculate contact angles and frozen fractions. Contact angles calculated for each ice nucleus as a function of temperature, α(T)-model, reproduce exactly experimentally derived frozen fractions without involving free-fit parameters. However, assigning the IN a single contact angle for the entire population (single-α model) is not suited to represent the frozen fractions. Application of α-PDF, active sites, and deterministic model approaches to measured frozen fractions yield similar good representations. Furthermore, when using a single parameterization of α-PDF or active sites distribution to fit all individual aw immersion freezing data simultaneously, frozen fraction curves are not reproduced. This implies that these fitting formulations cannot be applied to immersion freezing of aqueous solutions, and suggests that derived fit parameters do not represent independent particle properties. Thus, from fitting frozen fractions only, the underlying ice nucleation mechanism and nature of the ice nucleating sites cannot be inferred. In contrast to using fitted functions obtained to represent experimental conditions only, we suggest to use experimentally derived Jhet as a function of temperature and aw that can be applied to conditions outside of those probed in laboratory. This is because Jhet(T) is independent of time and IN surface areas in contrast to the fit parameters obtained by representation of experimentally derived frozen fractions.

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 A new temperature and humidity dependent surface site density approach for deposition ice nucleation

2014 ◽  
Vol 14 (12) ◽  
pp. 18499-18539 ◽  
Author(s):  
I. Steinke ◽  
C. Hoose ◽  
O. Möhler ◽  
P. Connolly ◽  
T. Leisner
Keyword(s):  
Contact Angle ◽  
Relative Humidity ◽  
Active Surface ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Aerosol Size Distribution ◽  
Surface Site ◽  
Linear Behavior ◽  
Temperature And Humidity

Abstract. Deposition nucleation experiments with Arizona Test Dust (ATD) as a surrogate for mineral dusts were conducted at the AIDA cloud chamber at temperatures between 220 and 250 K. The influence of the aerosol size distribution and the cooling rate on the ice nucleation efficiencies was investigated. Ice nucleation active surface site (INAS) densities were calculated to quantify the ice nucleation efficiency as a function of temperature, humidity and the aerosol surface area concentration. Additionally, a contact angle parameterization according to classical nucleation theory was fitted to the experimental data in order to relate the ice nucleation efficiencies to contact angle distributions. From this study it can be concluded that the INAS density formulation is a very useful tool to decribe the temperature and humidity dependent ice nucleation efficiency of ATD particles. Deposition nucleation on ATD particles can be described by a temperature and relative humidity dependent INAS density function ns(T, Sice) with ns(xtherm) = 1.88 × 105 · exp(0.2659 · xtherm) [m−2]                (1) where the thermodynamic variable xtherm is defined as xtherm = −(T − 273.2) + (Sice−1) × 100                                      (2) with Sice>1 and within a temperature range between 226 and 250 K. For lower temperatures, xtherm deviates from a linear behavior with temperature and relative humidity over ice. Two different approaches for describing the time dependence of deposition nucleation initiated by ATD particles are proposed. Box model estimates suggest that the time dependent contribution is only relevant for small cooling rates and low number fractions of ice-active particles.

scholarly journals Heterogeneous ice nucleation on atmospheric aerosols: a review of results from laboratory experiments

2012 ◽  
Vol 12 (5) ◽  
pp. 12531-12621 ◽  
Author(s):  
C. Hoose ◽  
O. Möhler
Keyword(s):  
Laboratory Experiments ◽  
Mineral Dust ◽  
Fungal Spores ◽  
Pollen Grains ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Small Subset ◽  
Ice Nuclei ◽  
Heterogeneous Ice Nucleation

Abstract. A small subset of the atmospheric aerosol population has the ability to induce ice formation at conditions under which ice would not form without them (heterogeneous ice nucleation). While no closed theoretical description of this process and the requirements for good ice nuclei is available, numerous studies have attempted to quantify the ice nucleation ability of different particles empirically in laboratory experiments. In this article, an overview of these results is provided. Ice nucleation onset conditions for various mineral dust, soot, biological, organic and ammonium sulphate particles are summarized. Typical temperature-supersaturation regions can be identified for the onset of ice nucleation of these different particle types, but the various particle sizes and activated fractions reported in different studies have to be taken into account when comparing results obtained with different methodologies. When intercomparing only data obtained under the same conditions, it is found that dust mineralogy is not a consistent predictor of higher or lower ice nucleation ability. However, the broad majority of studies agrees on a reduction of deposition nucleation by various coatings on mineral dust. The ice nucleation active surface site (INAS) density is discussed as a normalized measure for ice nucleation activity. For most immersion and condensation freezing measurements on mineral dust, estimates of the temperature-dependent INAS density agree within about two orders of magnitude. For deposition nucleation on dust, the spread is significantly larger, but a general trend of increasing INAS densities with increasing supersaturation is found. For soot, the presently available results are divergent. Estimated average INAS densities are high for ice-nucleation active bacteria at high subzero temperatures. At the same time, it is shown that some other biological aerosols, like certain pollen grains and fungal spores, are not intrinsically better ice nuclei than dust, but owe their high ice nucleation onsets to their large sizes. Surface-area-dependent parameterizations of heterogeneous ice nucleation are discussed. For immersion freezing on mineral dust, fitted INAS densities are available, but should not be used outside the temperature interval of the data they were based on. Classical nucleation theory, if employed with one fitted contact angle, does not reproduce the observed temperature dependence for immersion nucleation, temperature and supersaturation dependence for deposition nucleation, and time dependence.

scholarly journals Heterogeneous ice nucleation on atmospheric aerosols: a review of results from laboratory experiments

2012 ◽  
Vol 12 (20) ◽  
pp. 9817-9854 ◽  
Author(s):  
C. Hoose ◽  
O. Möhler
Keyword(s):  
Laboratory Experiments ◽  
Mineral Dust ◽  
Fungal Spores ◽  
Pollen Grains ◽  
Contact Angles ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Small Subset ◽  
Heterogeneous Ice Nucleation

Abstract. A small subset of the atmospheric aerosol population has the ability to induce ice formation at conditions under which ice would not form without them (heterogeneous ice nucleation). While no closed theoretical description of this process and the requirements for good ice nuclei is available, numerous studies have attempted to quantify the ice nucleation ability of different particles empirically in laboratory experiments. In this article, an overview of these results is provided. Ice nucleation "onset" conditions for various mineral dust, soot, biological, organic and ammonium sulfate particles are summarized. Typical temperature-supersaturation regions can be identified for the "onset" of ice nucleation of these different particle types, but the various particle sizes and activated fractions reported in different studies have to be taken into account when comparing results obtained with different methodologies. When intercomparing only data obtained under the same conditions, it is found that dust mineralogy is not a consistent predictor of higher or lower ice nucleation ability. However, the broad majority of studies agrees on a reduction of deposition nucleation by various coatings on mineral dust. The ice nucleation active surface site (INAS) density is discussed as a simple and empirical normalized measure for ice nucleation activity. For most immersion and condensation freezing measurements on mineral dust, estimates of the temperature-dependent INAS density agree within about two orders of magnitude. For deposition nucleation on dust, the spread is significantly larger, but a general trend of increasing INAS densities with increasing supersaturation is found. For soot, the presently available results are divergent. Estimated average INAS densities are high for ice-nucleation active bacteria at high subzero temperatures. At the same time, it is shown that INAS densities of some other biological aerosols, like certain pollen grains, fungal spores and diatoms, tend to be similar to those of dust. These particles may owe their high ice nucleation onsets to their large sizes. Surface-area-dependent parameterizations of heterogeneous ice nucleation are discussed. For immersion freezing on mineral dust, fitted INAS densities are available, but should not be used outside the temperature interval of the data they were based on. Classical nucleation theory, if employed with only one fitted contact angle, does not reproduce the observed temperature dependence for immersion nucleation, the temperature and supersaturation dependence for deposition nucleation, and the time dependence of ice nucleation. Formulations of classical nucleation theory with distributions of contact angles offer possibilities to overcome these weaknesses.

scholarly journals Immersion freezing of water and aqueous ammonium sulphate droplets initiated by Humic Like Substances as a function of water activity

2013 ◽  
Vol 13 (2) ◽  
pp. 4917-4961
Author(s):  
Y. J. Rigg ◽  
P. A. Alpert ◽  
D. A. Knopf
Keyword(s):  
Water Activity ◽  
Active Sites ◽  
Melting Curve ◽  
Contact Angles ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Surface Areas ◽  
Immersion Freezing ◽  
Freezing Temperatures

Abstract. Immersion freezing of water and aqueous (NH4)2SO4 droplets containing Leonardite (LEO) and Pahokee peat (PP) serving as surrogates for Humic Like Substances (HULIS) has been investigated. Organic aerosol containing HULIS are ubiquitous in the atmosphere, however, their potential for ice cloud formation is uncertain. Immersion freezing has been studied for temperatures as low as 215 K and solution water activity, aw, from 0.85–1.0. The freezing temperatures of water and aqueous solution droplets containing LEO and PP are 5–15 K warmer than homogeneous ice nucleation temperatures. Heterogeneous freezing temperatures can be represented by a horizontal shift of the ice melting curve as a function of solution aw, Δaw, by 0.2703 and 0.2466, respectively. Corresponding heterogeneous ice nucleation rate coefficients, Jhet, are (9.6 ± 2.5)×104 and (5.4 ± 1.4)×104 cm−2 s−1 for LEO and PP containing droplets, respectively, and remain constant along freezing curves characterized by Δaw. Consequently predictions of freezing temperatures and kinetics can be made without knowledge of the solute type when relative humidity and IN surface areas are known. The acquired ice nucleation data are applied to evaluate different approaches to fit and reproduce experimentally derived frozen fractions. In addition, we apply a basic formulation of classical nucleation theory (α(T)-model) to calculate contact angles and frozen fractions. Contact angles calculated for each ice nucleus as a function of temperature, α(T)-model, reproduce exactly experimentally derived frozen fractions without involving free fit parameters. However, assigning the IN a single contact angle for entire population (single-α model) is not suited to represent the frozen fractions. Application of α-PDF, active sites, and deterministic model approaches to measured frozen fractions yield similar good representations. Thus, from fitting frozen fractions only, the underlying ice nucleation mechanism and nature of the ice nucleating sites cannot be inferred. In contrast to using fitted functions obtained to represent experimental conditions only, we suggest to use experimentally derived Jhet as a function of temperature and aw that can be applied to conditions outside of those probed in laboratory. This is because Jhet(T) is independent of time and IN surface areas in contrast to the fit parameters obtained by representation of experimentally derived frozen fractions.

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

2007 ◽  
Vol 7 (4) ◽  
pp. 9687-9716
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 heterogeneous 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 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.

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