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 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 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 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 Impact of heterogeneous ice nucleation by natural dust and soot based on a probability density function of contact angle model with the Community Atmospheric Model version 5

2014 ◽  
Vol 14 (6) ◽  
pp. 7141-7186 ◽  
Author(s):  
Y. Wang ◽  
X. Liu ◽  
C. Hoose ◽  
B. Wang
Keyword(s):  
Contact Angle ◽  
Standard Deviation ◽  
Probability Density Function ◽  
Atmospheric Model ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Pdf Model ◽  
Mixed Phase Clouds ◽  
The Impact

Abstract. In order to investigate the impact of different treatments for the contact angle (α) in heterogeneous ice nucleating properties of natural dust and black carbon (BC) particles, we implement the classical-nucleation-theory-based parameterization of heterogeneous ice nucleation (Hoose et al., 2010) in the Community Atmospheric Model version 5 (CAM5), and then improve it by replacing the original single contact angle model with the probability density function of α (α-PDF) model to better represent the ice nucleation behavior of natural dust found in observations. We re-fit the classical nucleation theory (CNT) to constrain the uncertain parameters (i.e., onset α and activation energy in the single α model; mean contact angle and standard deviation in the α-PDF model) using recent observation datasets for Saharan natural dust and BC (soot). We investigate the impact of time-dependence of droplet freezing on mixed-phase clouds and climate in CAM5, and the roles of natural dust and soot by different nucleation mechanisms. Our results show that when comparing with observations, the potential ice nuclei (IN) calculated by the α-PDF model has a better agreement than that calculated by the single-α model at warm temperatures (T > −20 °C). Ice crystals can form at lower altitudes (with warmer temperatures) simulated by the α-PDF model compared with the single-α model in CAM5. All of these can be attributed to different ice nucleation efficiencies among aerosol particles with some particles having smaller contact angles (higher efficiencies) in the α-PDF model. In the sensitivity tests with the α-PDF model, we find that the change of mean contact angle has larger impact on the active fraction than that of standard deviation, even though the change of standard deviation can lead to the transition of freezing behavior. Both the single α and the α-PDF model indicates that the immersion freezing of natural dust plays a more important role in the heterogeneous nucleation than that of soot in mixed-phase clouds.

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 Different contact angle distributions for heterogeneous ice nucleation in the Community Atmospheric Model version 5

2014 ◽  
Vol 14 (19) ◽  
pp. 10411-10430 ◽  
Author(s):  
Y. Wang ◽  
X. Liu ◽  
C. Hoose ◽  
B. Wang
Keyword(s):  
Contact Angle ◽  
Standard Deviation ◽  
Atmospheric Model ◽  
Ice Nucleation ◽  
Mixed Phase ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Pdf Model ◽  
Mixed Phase Clouds ◽  
The Impact

Abstract. In order to investigate the impact of different treatments for the contact angle (α) in heterogeneous ice nucleating properties of natural dust and black carbon (BC) particles, we implement the classical-nucleation-theory-based parameterization of heterogeneous ice nucleation (Hoose et al., 2010) in the Community Atmospheric Model version 5 (CAM5) and then improve it by replacing the original single-contact-angle model with the probability-density-function-of-α (α-PDF) model to better represent the ice nucleation behavior of natural dust found in observations. We refit the classical nucleation theory (CNT) to constrain the uncertain parameters (i.e., onset α and activation energy in the single-α model; mean contact angle and standard deviation in the α-PDF model) using recent observation data sets for Saharan natural dust and BC (soot). We investigate the impact of the time dependence of droplet freezing on mixed-phase clouds and climate in CAM5 as well as the roles of natural dust and soot in different nucleation mechanisms. Our results show that, when compared with observations, the potential ice nuclei (IN) calculated by the α-PDF model show better agreement than those calculated by the single-α model at warm temperatures (T; T > −20 °C). More ice crystals can form at low altitudes (with warm temperatures) simulated by the α-PDF model than compared to the single-α model in CAM5. All of these can be attributed to different ice nucleation efficiencies among aerosol particles, with some particles having smaller contact angles (higher efficiencies) in the α-PDF model. In the sensitivity tests with the α-PDF model, we find that the change in mean contact angle has a larger impact on the active fraction at a given temperature than a change in standard deviation, even though the change in standard deviation can lead to a change in freezing behavior. Both the single-α and the α-PDF model indicate that the immersion freezing of natural dust plays a more important role in the heterogeneous nucleation than that of soot in mixed-phase clouds. The new parameterizations implemented in CAM5 induce more significant aerosol indirect effects than the default parameterization.

scholarly journals Parameterizing ice nucleation rates using contact angle and activation energy derived from laboratory data

2008 ◽  
Vol 8 (24) ◽  
pp. 7431-7449 ◽  
Author(s):  
J.-P. Chen ◽  
A. Hazra ◽  
Z. Levin
Keyword(s):  
Activation Energy ◽  
Contact Angle ◽  
Thermodynamic Parameters ◽  
Laboratory Data ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Curvature Effects ◽  
Ice Nuclei ◽  
Cloud Models

Abstract. The rate of ice nucleation in clouds is not easily determined and large discrepancies exist between model predictions and actual ice crystal concentration measured in clouds. In an effort to improve the parameterization of ice nucleating in cloud models, we investigate the rate of heterogeneous ice nucleation under specific ambient conditions by knowing the sizes as well as two thermodynamic parameters of the ice nuclei – contact angle and activation energy. Laboratory data of freezing and deposition nucleation modes were analyzed to derive inversely the two thermodynamic parameters for a variety of ice nuclei, including mineral dusts, bacteria, pollens, and soot particles. The analysis considered the Zeldovich factor for the adjustment of ice germ formation, as well as the solute and curvature effects on surface tension; the latter effects have strong influence on the contact angle. Contact angle turns out to be a more important factor than the activation energy in discriminating the nucleation capabilities of various ice nuclei species. By extracting these thermodynamic parameters, laboratory results can be converted into a formulation that follows classical nucleation theory, which then has the flexibility of incorporating factors such as the solute effect and curvature effect that were not considered in the experiments. Due to various uncertainties, contact angle and activation energy derived in this study should be regarded as "apparent" thermodynamics parameters.

scholarly journals Parameterizing ice nucleation rates for cloud modeling using contact angle and activation energy derived from laboratory data

2008 ◽  
Vol 8 (4) ◽  
pp. 14419-14465 ◽  
Author(s):  
J.-P. Chen ◽  
A. Hazra ◽  
Z. Levin
Keyword(s):  
Activation Energy ◽  
Contact Angle ◽  
Thermodynamic Parameters ◽  
Laboratory Data ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Curvature Effects ◽  
Ice Nuclei ◽  
Cloud Models

Abstract. The rate of ice nucleation in clouds is not easily determined and large discrepancies exist between model predictions and actual ice crystal concentration measured in clouds. In an effort to improve the parameterization of ice nucleating in cloud models, we investigate the rate of heterogeneous ice nucleation under specific ambient conditions by knowing the sizes as well as two thermodynamic parameters of the ice nuclei – contact angle and activation energy. Laboratory data of freezing and deposition nucleation modes were analyzed to derive inversely the two thermodynamic parameters for a variety of ice nuclei, including mineral dusts, bacteria, pollens, and soot particles. The analysis considered the Zeldovich factor for the adjustment of ice germ formation, as well as the solute and curvature effects on surface tension, the latter effects have strong influence on the contact angle. Contact angle turns out to be a more important factor than the activation energy in discriminating the nucleation capabilities of various ice nuclei species. By extracting these thermodynamic parameters, laboratory results can be converted into a formulation that follows classical nucleation theory, which then has the flexibility of incorporating factors such as the solute effect and curvature effect that were not considered in the experiments.

scholarly journals Brief Overview of Ice Nucleation

Molecules ◽  
2021 ◽  
Vol 26 (2) ◽  
pp. 392
Author(s):  
Nobuo Maeda
Keyword(s):  
Molecular Level ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Radiation Balance ◽  
Feature Article ◽  
Aircraft Wings ◽  
Food Engineering ◽  
Research Activities ◽  
Important Field

The nucleation of ice is vital in cloud physics and impacts on a broad range of matters from the cryopreservation of food, tissues, organs, and stem cells to the prevention of icing on aircraft wings, bridge cables, wind turbines, and other structures. Ice nucleation thus has broad implications in medicine, food engineering, mineralogy, biology, and other fields. Nowadays, the growing threat of global warming has led to intense research activities on the feasibility of artificially modifying clouds to shift the Earth’s radiation balance. For these reasons, nucleation of ice has been extensively studied over many decades and rightfully so. It is thus not quite possible to cover the whole subject of ice nucleation in a single review. Rather, this feature article provides a brief overview of ice nucleation that focuses on several major outstanding fundamental issues. The author’s wish is to aid early researchers in ice nucleation and those who wish to get into the field of ice nucleation from other disciplines by concisely summarizing the outstanding issues in this important field. Two unresolved challenges stood out from the review, namely the lack of a molecular-level picture of ice nucleation at an interface and the limitations of classical nucleation theory.

scholarly journals Analysis of the effect of water activity on ice formation using a new thermodynamic framework

2014 ◽  
Vol 14 (14) ◽  
pp. 7665-7680 ◽  
Author(s):  
D. Barahona
Keyword(s):  
Water Activity ◽  
Nucleation Rate ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Cloud Formation ◽  
Classical Nucleation Theory ◽  
Solid Matrix ◽  
Effect Of Water ◽  
Thermodynamic Framework ◽  
New Framework

Abstract. In this work a new thermodynamic framework is developed and used to investigate the effect of water activity on the formation of ice within supercooled droplets. The new framework is based on a novel concept where the interface is assumed to be made of liquid molecules "trapped" by the solid matrix. It also accounts for the change in the composition of the liquid phase upon nucleation. Using this framework, new expressions are developed for the critical ice germ size and the nucleation work with explicit dependencies on temperature and water activity. However unlike previous approaches, the new model does not depend on the interfacial tension between liquid and ice. The thermodynamic framework is introduced within classical nucleation theory to study the effect of water activity on the ice nucleation rate. Comparison against experimental results shows that the new approach is able to reproduce the observed effect of water activity on the nucleation rate and the freezing temperature. It allows for the first time a phenomenological derivation of the constant shift in water activity between melting and nucleation. The new framework offers a consistent thermodynamic view of ice nucleation, simple enough to be applied in atmospheric models of cloud formation.

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