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

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.

2012 ◽  
Vol 12 (20) ◽  
pp. 9817-9854 ◽  
Author(s):  
C. Hoose ◽  
O. Möhler

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.


2007 ◽  
Vol 7 (19) ◽  
pp. 5081-5091 ◽  
Author(s):  
C. Marcolli ◽  
S. Gedamke ◽  
T. Peter ◽  
B. Zobrist

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.


2017 ◽  
Vol 74 (3) ◽  
pp. 699-717 ◽  
Author(s):  
Romy Ullrich ◽  
Corinna Hoose ◽  
Ottmar Möhler ◽  
Monika Niemand ◽  
Robert Wagner ◽  
...  

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.


2010 ◽  
Vol 67 (8) ◽  
pp. 2483-2503 ◽  
Author(s):  
Corinna Hoose ◽  
Jón Egill Kristjánsson ◽  
Jen-Ping Chen ◽  
Anupam Hazra

Abstract An ice nucleation parameterization based on classical nucleation theory, with aerosol-specific parameters derived from experiments, has been implemented into a global climate model—the Community Atmosphere Model (CAM)-Oslo. The parameterization treats immersion, contact, and deposition nucleation by mineral dust, soot, bacteria, fungal spores, and pollen in mixed-phase clouds at temperatures between 0° and −38°C. Immersion freezing is considered for insoluble particles that are activated to cloud droplets, and deposition and contact nucleation are only allowed for uncoated, unactivated aerosols. Immersion freezing by mineral dust is found to be the dominant ice formation process, followed by immersion and contact freezing by soot. The simulated biological aerosol contribution to global atmospheric ice formation is marginal, even with high estimates of their ice nucleation activity, because the number concentration of ice nucleation active biological particles in the atmosphere is low compared to other ice nucleating aerosols. Because of the dominance of mineral dust, the simulated ice nuclei concentrations at temperatures below −20°C are found to correlate with coarse-mode aerosol particle concentrations. The ice nuclei (IN) concentrations in the model agree well overall with in situ continuous flow diffusion chamber measurements. At individual locations, the model exhibits a stronger temperature dependence on IN concentrations than what is observed. The simulated IN composition (77% mineral dust, 23% soot, and 10−5% biological particles) lies in the range of observed ice nuclei and ice crystal residue compositions.


2007 ◽  
Vol 7 (4) ◽  
pp. 9687-9716
Author(s):  
C. Marcolli ◽  
S. Gedamke ◽  
T. Peter ◽  
B. Zobrist

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.


2008 ◽  
Vol 8 (24) ◽  
pp. 7431-7449 ◽  
Author(s):  
J.-P. Chen ◽  
A. Hazra ◽  
Z. Levin

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.


2008 ◽  
Vol 8 (4) ◽  
pp. 14419-14465 ◽  
Author(s):  
J.-P. Chen ◽  
A. Hazra ◽  
Z. Levin

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.


2021 ◽  
Vol 11 (1) ◽  
Author(s):  
Slobodan Nickovic ◽  
Bojan Cvetkovic ◽  
Slavko Petković ◽  
Vassilis Amiridis ◽  
Goran Pejanović ◽  
...  

AbstractIce particles in high-altitude cold clouds can obstruct aircraft functioning. Over the last 20 years, there have been more than 150 recorded cases with engine power-loss and damage caused by tiny cloud ice crystals, which are difficult to detect with aircraft radars. Herein, we examine two aircraft accidents for which icing linked to convective weather conditions has been officially reported as the most likely reason for catastrophic consequences. We analyze whether desert mineral dust, known to be very efficient ice nuclei and present along both aircraft routes, could further augment the icing process. Using numerical simulations performed by a coupled atmosphere-dust model with an included parameterization for ice nucleation triggered by dust aerosols, we show that the predicted ice particle number sharply increases at approximate locations and times of accidents where desert dust was brought by convective circulation to the upper troposphere. We propose a new icing parameter which, unlike existing icing indices, for the first time includes in its calculation the predicted dust concentration. This study opens up the opportunity to use integrated atmospheric-dust forecasts as warnings for ice formation enhanced by mineral dust presence.


Molecules ◽  
2021 ◽  
Vol 26 (2) ◽  
pp. 392
Author(s):  
Nobuo Maeda

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.


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