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- Author or Editor: Thomas Leisner x
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Abstract
Ice multiplication processes are known to be responsible for the higher concentration of ice particles versus ice nucleating particles in clouds, but the exact secondary ice formation mechanisms remain to be quantified. Recent in-cloud observations and modeling studies have suggested the importance of secondary ice production upon shattering of freezing drizzle droplets. In one of our previous studies, four categories of secondary ice formation during freezing of supercooled droplets have been identified: breakup, cracking, jetting, and bubble bursts. In this work, we extend the study to include pure water and an aqueous solution of analog sea salt drizzle droplets moving at terminal velocity with respect to the surrounding cold humid air. We observe an enhancement in the droplet shattering probability as compared to the stagnant air conditions used in the previous study. Under free-fall conditions, bubble bursts are the most common secondary ice production mode in sea salt drizzle droplets, while droplet fragmentation controls the secondary ice production in pure water droplets.
Abstract
Ice multiplication processes are known to be responsible for the higher concentration of ice particles versus ice nucleating particles in clouds, but the exact secondary ice formation mechanisms remain to be quantified. Recent in-cloud observations and modeling studies have suggested the importance of secondary ice production upon shattering of freezing drizzle droplets. In one of our previous studies, four categories of secondary ice formation during freezing of supercooled droplets have been identified: breakup, cracking, jetting, and bubble bursts. In this work, we extend the study to include pure water and an aqueous solution of analog sea salt drizzle droplets moving at terminal velocity with respect to the surrounding cold humid air. We observe an enhancement in the droplet shattering probability as compared to the stagnant air conditions used in the previous study. Under free-fall conditions, bubble bursts are the most common secondary ice production mode in sea salt drizzle droplets, while droplet fragmentation controls the secondary ice production in pure water droplets.
Abstract
The formation of secondary ice in clouds, that is, ice particles that are created at temperatures above the limit for homogeneous freezing without the direct involvement of a heterogeneous ice nucleus, is one of the longest-standing puzzles in cloud physics. Here, we present comprehensive laboratory investigations on the formation of small ice particles upon the freezing of drizzle-sized cloud droplets levitated in an electrodynamic balance. Four different categories of secondary ice formation (bubble bursting, jetting, cracking, and breakup) could be detected, and their respective frequencies of occurrence as a function of temperature and droplet size are given. We find that bubble bursting occurs more often than droplet splitting. While we do not observe the shattering of droplets into many large fragments, we find that the average number of small secondary ice particles released during freezing is strongly dependent on droplet size and may well exceed unity for droplets larger than 300 μm in diameter. This leaves droplet fragmentation as an important secondary ice process effective at temperatures around −10°C in clouds where large drizzle droplets are present.
Abstract
The formation of secondary ice in clouds, that is, ice particles that are created at temperatures above the limit for homogeneous freezing without the direct involvement of a heterogeneous ice nucleus, is one of the longest-standing puzzles in cloud physics. Here, we present comprehensive laboratory investigations on the formation of small ice particles upon the freezing of drizzle-sized cloud droplets levitated in an electrodynamic balance. Four different categories of secondary ice formation (bubble bursting, jetting, cracking, and breakup) could be detected, and their respective frequencies of occurrence as a function of temperature and droplet size are given. We find that bubble bursting occurs more often than droplet splitting. While we do not observe the shattering of droplets into many large fragments, we find that the average number of small secondary ice particles released during freezing is strongly dependent on droplet size and may well exceed unity for droplets larger than 300 μm in diameter. This leaves droplet fragmentation as an important secondary ice process effective at temperatures around −10°C in clouds where large drizzle droplets are present.
Abstract
The freezing process of a supercooled water droplet freely falling through air is a remarkably dynamic and eventful process. During freezing from the outside in, the volume increase of liquid water upon solidification leads to a pressure rise inside the droplet. The pressure is released in various ways, e.g., by cracking or by complete fragmentation of the ice shell. These processes may be the source of secondary ice particles that are emitted during droplet freezing. In this study, the surface temperature of freezing drizzle-sized water droplets was measured with a high-resolution infrared thermography system, while recording the changes in shape and structure of the droplet by a high-speed video camera. The droplets were levitated in an electrodynamic trap under controlled conditions with respect to temperature, humidity, and airflow velocity. Measurement of the surface temperature during freezing allowed for determination of the absolute pressure inside the liquid core. During the freezing of a droplet the pressure rise is interrupted many times by rapid pressure release events, each being a possible source of secondary ice. Pressure release events were 3 times more frequent for droplets freezing under free-fall conditions compared to droplets freezing in stagnant air. Naturally occurring sea salt content (<100 mg L−1) does not inhibit the pressure buildup inside freezing drizzle droplets.
Abstract
The freezing process of a supercooled water droplet freely falling through air is a remarkably dynamic and eventful process. During freezing from the outside in, the volume increase of liquid water upon solidification leads to a pressure rise inside the droplet. The pressure is released in various ways, e.g., by cracking or by complete fragmentation of the ice shell. These processes may be the source of secondary ice particles that are emitted during droplet freezing. In this study, the surface temperature of freezing drizzle-sized water droplets was measured with a high-resolution infrared thermography system, while recording the changes in shape and structure of the droplet by a high-speed video camera. The droplets were levitated in an electrodynamic trap under controlled conditions with respect to temperature, humidity, and airflow velocity. Measurement of the surface temperature during freezing allowed for determination of the absolute pressure inside the liquid core. During the freezing of a droplet the pressure rise is interrupted many times by rapid pressure release events, each being a possible source of secondary ice. Pressure release events were 3 times more frequent for droplets freezing under free-fall conditions compared to droplets freezing in stagnant air. Naturally occurring sea salt content (<100 mg L−1) does not inhibit the pressure buildup inside freezing drizzle droplets.
Abstract
In climate and weather models, the quantitative description of aerosol and cloud processes relies on simplified assumptions. This contributes major uncertainties to the prediction of global and regional climate change. Therefore, models need good parameterizations for heterogeneous ice nucleation by atmospheric aerosols. Here the authors present a new parameterization of immersion freezing on desert dust particles derived from a large number of experiments carried out at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud chamber facility. The parameterization is valid in the temperature range between −12° and −36°C at or above water saturation and can be used in atmospheric models that include information about the dust surface area. The new parameterization was applied to calculate distribution maps of ice nuclei during a Saharan dust event based on model results from the regional-scale model Consortium for Small-Scale Modelling–Aerosols and Reactive Trace Gases (COSMO-ART). The results were then compared to measurements at the Taunus Observatory on Mount Kleiner Feldberg, Germany, and to three other parameterizations applied to the dust outbreak. The aerosol number concentration and surface area from the COSMO-ART model simulation were taken as input to different parameterizations. Although the surface area from the model agreed well with aerosol measurements during the dust event at Kleiner Feldberg, the ice nuclei (IN) number concentration calculated from the new surface-area-based parameterization was about a factor of 13 less than IN measurements during the same event. Systematic differences of more than a factor of 10 in the IN number concentration were also found among the different parameterizations. Uncertainties in the modeled and measured parameters probably both contribute to this discrepancy and should be addressed in future studies.
Abstract
In climate and weather models, the quantitative description of aerosol and cloud processes relies on simplified assumptions. This contributes major uncertainties to the prediction of global and regional climate change. Therefore, models need good parameterizations for heterogeneous ice nucleation by atmospheric aerosols. Here the authors present a new parameterization of immersion freezing on desert dust particles derived from a large number of experiments carried out at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud chamber facility. The parameterization is valid in the temperature range between −12° and −36°C at or above water saturation and can be used in atmospheric models that include information about the dust surface area. The new parameterization was applied to calculate distribution maps of ice nuclei during a Saharan dust event based on model results from the regional-scale model Consortium for Small-Scale Modelling–Aerosols and Reactive Trace Gases (COSMO-ART). The results were then compared to measurements at the Taunus Observatory on Mount Kleiner Feldberg, Germany, and to three other parameterizations applied to the dust outbreak. The aerosol number concentration and surface area from the COSMO-ART model simulation were taken as input to different parameterizations. Although the surface area from the model agreed well with aerosol measurements during the dust event at Kleiner Feldberg, the ice nuclei (IN) number concentration calculated from the new surface-area-based parameterization was about a factor of 13 less than IN measurements during the same event. Systematic differences of more than a factor of 10 in the IN number concentration were also found among the different parameterizations. Uncertainties in the modeled and measured parameters probably both contribute to this discrepancy and should be addressed in future studies.
A New Ice Nucleation Active Site Parameterization for Desert Dust and SootAbstract
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 n S 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 n S isolines for desert dust follow u-shaped curves in the ice saturation ratio–temperature (S i –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 S i for soot with higher organic carbon content. For immersion freezing of soot aerosol, only upper limits for n S 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 n S isolines especially for deposition nucleation. For the application in models, implementation of this new framework is simple compared to that of other expressions.
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 n S 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 n S isolines for desert dust follow u-shaped curves in the ice saturation ratio–temperature (S i –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 S i for soot with higher organic carbon content. For immersion freezing of soot aerosol, only upper limits for n S 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 n S isolines especially for deposition nucleation. For the application in models, implementation of this new framework is simple compared to that of other expressions.
Abstract
The contribution of heterogeneous ice nucleation to the formation of cirrus cloud ice crystals is still not well quantified. This results in large uncertainties when predicting cirrus radiative effects and their role in Earth’s climate system. The goal of this case study is to simulate the composition, and thus activation conditions, of ice nucleating particles (INPs) to evaluate their contribution to heterogeneous cirrus ice formation in relation to homogeneous ice nucleation. For this, the regional model COSMO—Aerosols and Reactive Trace Gases (COSMO-ART) was used to simulate a synoptic cirrus cloud over Texas on 13 April 2011. The simulated INP composition was then compared to measured ice residual particle (IRP) composition from the actual event obtained during the NASA Midlatitude Airborne Cirrus Properties Experiment (MACPEX) aircraft campaign. These IRP measurements indicated that the dominance of heterogeneous ice nucleation was mainly driven by mineral dust with contributions from a variety of other particle types. Applying realistic activation thresholds and concentrations of airborne transported mineral dust and biomass-burning particles, the model implementing the heterogeneous ice nucleation parameterization scheme of Ullrich et al. is able to reproduce the overall dominating ice formation mechanism in contrast to the model simulation with the scheme of Phillips et al. However, the model showed flaws in reproducing the IRP composition.
Abstract
The contribution of heterogeneous ice nucleation to the formation of cirrus cloud ice crystals is still not well quantified. This results in large uncertainties when predicting cirrus radiative effects and their role in Earth’s climate system. The goal of this case study is to simulate the composition, and thus activation conditions, of ice nucleating particles (INPs) to evaluate their contribution to heterogeneous cirrus ice formation in relation to homogeneous ice nucleation. For this, the regional model COSMO—Aerosols and Reactive Trace Gases (COSMO-ART) was used to simulate a synoptic cirrus cloud over Texas on 13 April 2011. The simulated INP composition was then compared to measured ice residual particle (IRP) composition from the actual event obtained during the NASA Midlatitude Airborne Cirrus Properties Experiment (MACPEX) aircraft campaign. These IRP measurements indicated that the dominance of heterogeneous ice nucleation was mainly driven by mineral dust with contributions from a variety of other particle types. Applying realistic activation thresholds and concentrations of airborne transported mineral dust and biomass-burning particles, the model implementing the heterogeneous ice nucleation parameterization scheme of Ullrich et al. is able to reproduce the overall dominating ice formation mechanism in contrast to the model simulation with the scheme of Phillips et al. However, the model showed flaws in reproducing the IRP composition.
Abstract
Homogeneous freezing of supercooled droplets occurs in convective systems in low and midlatitudes. This droplet-freezing process leads to the formation of a large amount of small ice particles, so-called frozen droplets, that are transported to the upper parts of anvil outflows, where they can influence the cloud radiative properties. However, the detailed microphysics and, thus, the scattering properties of these small ice particles are highly uncertain. Here, the link between the microphysical and optical properties of frozen droplets is investigated in cloud chamber experiments, where the frozen droplets were formed, grown, and sublimated under controlled conditions. It was found that frozen droplets developed a high degree of small-scale complexity after their initial formation and subsequent growth. During sublimation, the small-scale complexity disappeared, releasing a smooth and near-spherical ice particle. Angular light scattering and depolarization measurements confirmed that these sublimating frozen droplets scattered light similar to spherical particles: that is, they had angular light-scattering properties similar to water droplets. The knowledge gained from this laboratory study was applied to two case studies of aircraft measurements in midlatitude and tropical convective systems. The in situ aircraft measurements confirmed that the microphysics of frozen droplets is dependent on the humidity conditions they are exposed to (growth or sublimation). The existence of optically spherical frozen droplets can be important for the radiative properties of detraining convective outflows.
Abstract
Homogeneous freezing of supercooled droplets occurs in convective systems in low and midlatitudes. This droplet-freezing process leads to the formation of a large amount of small ice particles, so-called frozen droplets, that are transported to the upper parts of anvil outflows, where they can influence the cloud radiative properties. However, the detailed microphysics and, thus, the scattering properties of these small ice particles are highly uncertain. Here, the link between the microphysical and optical properties of frozen droplets is investigated in cloud chamber experiments, where the frozen droplets were formed, grown, and sublimated under controlled conditions. It was found that frozen droplets developed a high degree of small-scale complexity after their initial formation and subsequent growth. During sublimation, the small-scale complexity disappeared, releasing a smooth and near-spherical ice particle. Angular light scattering and depolarization measurements confirmed that these sublimating frozen droplets scattered light similar to spherical particles: that is, they had angular light-scattering properties similar to water droplets. The knowledge gained from this laboratory study was applied to two case studies of aircraft measurements in midlatitude and tropical convective systems. The in situ aircraft measurements confirmed that the microphysics of frozen droplets is dependent on the humidity conditions they are exposed to (growth or sublimation). The existence of optically spherical frozen droplets can be important for the radiative properties of detraining convective outflows.
Understanding cloud and precipitation responses to variations in atmospheric aerosols remains an important research topic for improving the prediction of climate. Knowledge is most uncertain, and the potential impact on climate is largest with regard to how aerosols impact ice formation in clouds. In this paper, we show that research on atmospheric ice nucleation, including the development of new measurement systems, is occurring at a renewed and historically unparalleled level. A historical perspective is provided on the methods and challenges of measuring ice nuclei, and the various factors that led to a lull in research efforts during a nearly 20-yr period centered about 30 yr ago. Workshops played a major role in defining critical needs for improving measurements at that time and helped to guide renewed efforts. Workshops were recently revived for evaluating present research progress. We argue that encouraging progress has been made in the consistency of measurements using the present generation of ice nucleation instruments. Through comparison to laboratory cloud simulations, these ice nuclei measurements have provided increased confidence in our ability to quantify primary ice formation by atmospheric aerosols.
Understanding cloud and precipitation responses to variations in atmospheric aerosols remains an important research topic for improving the prediction of climate. Knowledge is most uncertain, and the potential impact on climate is largest with regard to how aerosols impact ice formation in clouds. In this paper, we show that research on atmospheric ice nucleation, including the development of new measurement systems, is occurring at a renewed and historically unparalleled level. A historical perspective is provided on the methods and challenges of measuring ice nuclei, and the various factors that led to a lull in research efforts during a nearly 20-yr period centered about 30 yr ago. Workshops played a major role in defining critical needs for improving measurements at that time and helped to guide renewed efforts. Workshops were recently revived for evaluating present research progress. We argue that encouraging progress has been made in the consistency of measurements using the present generation of ice nucleation instruments. Through comparison to laboratory cloud simulations, these ice nuclei measurements have provided increased confidence in our ability to quantify primary ice formation by atmospheric aerosols.
