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1
Hoffmann, N., A. Kiselev, D. Rzesanke, D. Duft, and T. Leisner. "Experimental quantification of contact freezing in an electrodynamic balance." Atmospheric Measurement Techniques 6, no. 9 (September 12, 2013): 2373–82. http://dx.doi.org/10.5194/amt-6-2373-2013.
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Abstract. Heterogeneous nucleation of ice in a supercooled water droplet induced by external contact with a dry aerosol particle has long been known to be more effective than freezing induced by the same nucleus immersed in the droplet. However, the experimental quantification of contact freezing is challenging. Here we report an experimental method to determine the temperature-dependent ice nucleation probability of size-selected aerosol particles. The method is based on the suspension of supercooled charged water droplets in a laminar flow of air containing aerosol particles as contact freezing nuclei. The rate of droplet–particle collisions is calculated numerically with account for Coulomb attraction, drag force and induced dipole interaction between charged droplet and aerosol particles. The calculation is verified by direct counting of aerosol particles collected by a levitated droplet. By repeating the experiment on individual droplets for a sufficient number of times, we are able to reproduce the statistical freezing behavior of a large ensemble of supercooled droplets and measure the average rate of freezing events. The freezing rate is equal to the product of the droplet–particle collision rate and the probability of freezing on a single contact, the latter being a function of temperature, size and composition of the contact ice nuclei. Based on these observations, we show that for the types of particles investigated so far, contact freezing is the dominating freezing mechanism on the timescale of our experiment.
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Hoffmann, N., A. Kiselev, D. Rzesanke, D. Duft, and T. Leisner. "Experimental quantification of contact freezing in an electrodynamic balance." Atmospheric Measurement Techniques Discussions 6, no. 2 (April 10, 2013): 3407–37. http://dx.doi.org/10.5194/amtd-6-3407-2013.
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Abstract. Heterogeneous nucleation of ice in a supercooled water droplet induced by an external contact with a dry aerosol particle has long been known to be more effective than freezing induced by the same nucleus immersed in the droplet. However, the experimental quantification of contact freezing is challenging. Here we report an experimental method allowing to determine the temperature dependent ice nucleation probability of size selected aerosol particles. The method uses supercooled charged water droplets suspended in a laminar flow of air containing aerosol particles as contact freezing nuclei. The rate of droplet–particle collisions is calculated numerically with account for Coulomb attraction, drag force and induced dipole interaction between charged droplet and aerosol particles. The calculation is verified by direct counting of aerosol particles collected by a levitated droplet. By repeating the experiment on individual droplets for a sufficient number of times, we are able to reproduce the statistical freezing behavior of a large ensemble of supercooled droplets and measure the average rate of freezing events. The freezing rate is equal to the product of the droplet–particle collision rate and the probability of freezing on a single contact, the latter being a function of temperature, size and composition of the contact ice nuclei. Based on these observations, we show that for the types of particles investigated so far, contact freezing is the dominating freezing mechanism on the time scale of our experiment.
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Lauber, Annika, Alexei Kiselev, Thomas Pander, Patricia Handmann, and Thomas Leisner. "Secondary Ice Formation during Freezing of Levitated Droplets." Journal of the Atmospheric Sciences 75, no. 8 (July 31, 2018): 2815–26. http://dx.doi.org/10.1175/jas-d-18-0052.1.
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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.
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Svensson, E. A., C. Delval, P. von Hessberg, M. S. Johnson, and J. B. C. Pettersson. "Freezing of water droplets colliding with kaolinite particles." Atmospheric Chemistry and Physics 9, no. 13 (July 3, 2009): 4295–300. http://dx.doi.org/10.5194/acp-9-4295-2009.
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Abstract. Contact freezing of single supercooled water droplets colliding with kaolinite dust particles has been investigated. The experiments were performed with droplets levitated in an electrodynamic balance at temperatures from 240 to 268 K. Under relatively dry conditions (when no water vapor was added) freezing was observed to occur below 249 K, while a freezing threshold of 267 K was observed when water vapor was added to the air in the chamber. The effect of relative humidity is attributed to an influence on the contact freezing process for the kaolinite-water droplet system, and it is not related to the lifetime of the droplets in the electrodynamic balance. Freezing probabilities per collision were derived assuming that collisions at the lowest temperature employed had a probability of unity. Mechanisms for contact freezing are briefly discussed.
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Chuah, Y. K., J. T. Lin, and K. H. Yu. "An Experimental Study on the Heat Transfer of Traveling Airborne Water Droplets in Cold Environment." Journal of Mechanics 32, no. 2 (January 2015): 219–25. http://dx.doi.org/10.1017/jmech.2015.84.
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AbstractThis paper presents experimental results on rapid freezing of water droplets injected into a low temperature environment. A heat balance method was applied to determine the ratio of the water droplets frozen at the collection after the airborne time. The experimental results show that rapid freezing of water droplets could be achieved within three seconds of airborne time. Droplet size distribution of the frozen water droplets after collection was estimated. Heat transfer during the airborne time was calculated with consideration of the droplet size distribution. At attempt was taken to compare the heat transfer obtained with some previous studies on heat transfer of spherical objects in air. The research results show that droplet size distribution is important for the prediction of heat transfer of water droplets traveling in air. The results presented in this study contribute to the understanding of heat transfer of water droplets injected into a low temperature air.
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Alpert, P. A., and D. A. Knopf. "Analysis of isothermal and cooling rate dependent immersion freezing by a unifying stochastic ice nucleation model." Atmospheric Chemistry and Physics Discussions 15, no. 9 (May 5, 2015): 13109–66. http://dx.doi.org/10.5194/acpd-15-13109-2015.
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Abstract. Immersion freezing is an important ice nucleation pathway involved in the formation of cirrus and mixed-phase clouds. Laboratory immersion freezing experiments are necessary to determine the range in temperature (T) and relative humidity (RH) at which ice nucleation occurs and to quantify the associated nucleation kinetics. Typically, isothermal (applying a constant temperature) and cooling rate dependent immersion freezing experiments are conducted. In these experiments it is usually assumed that the droplets containing ice nuclei (IN) all have the same IN surface area (ISA), however the validity of this assumption or the impact it may have on analysis and interpretation of the experimental data is rarely questioned. A stochastic immersion freezing model based on first principles of statistics is presented, which accounts for variable ISA per droplet and uses physically observable parameters including the total number of droplets (Ntot) and the heterogeneous ice nucleation rate coefficient, Jhet(T). This model is applied to address if (i) a time and ISA dependent stochastic immersion freezing process can explain laboratory immersion freezing data for different experimental methods and (ii) the assumption that all droplets contain identical ISA is a valid conjecture with subsequent consequences for analysis and interpretation of immersion freezing. The simple stochastic model can reproduce the observed time and surface area dependence in immersion freezing experiments for a variety of methods such as: droplets on a cold-stage exposed to air or surrounded by an oil matrix, wind and acoustically levitated droplets, droplets in a continuous flow diffusion chamber (CFDC), the Leipzig aerosol cloud interaction simulator (LACIS), and the aerosol interaction and dynamics in the atmosphere (AIDA) cloud chamber. Observed time dependent isothermal frozen fractions exhibiting non-exponential behavior with time can be readily explained by this model considering varying ISA. An apparent cooling rate dependence ofJhet is explained by assuming identical ISA in each droplet. When accounting for ISA variability, the cooling rate dependence of ice nucleation kinetics vanishes as expected from classical nucleation theory. The model simulations allow for a quantitative experimental uncertainty analysis for parameters Ntot, T, RH, and the ISA variability. In an idealized cloud parcel model applying variability in ISAs for each droplet, the model predicts enhanced immersion freezing temperatures and greater ice crystal production compared to a case when ISAs are uniform in each droplet. The implications of our results for experimental analysis and interpretation of the immersion freezing process are discussed.
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Svensson, E. A., C. Delval, P. von Hessberg, M. S. Johnson, and J. B. C. Pettersson. "Freezing of water droplets colliding with kaolinite particles." Atmospheric Chemistry and Physics Discussions 9, no. 1 (January 27, 2009): 2417–33. http://dx.doi.org/10.5194/acpd-9-2417-2009.
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Abstract. Contact freezing of single supercooled water droplets colliding with kaolinite dust particles has been investigated. The experiments were performed with droplets levitated in an electrodynamic balance at temperatures from 240 to 268 K. Under dry conditions freezing was observed to occur below 249 K, while a freezing threshold of 267 K was observed at high relative humidity. The effect of relative humidity is attributed to an influence on the contact freezing process for the kaolinite-water droplet system, and it is not related to the lifetime of the droplets in the electrodynamic balance. Freezing probabilities per collision were derived assuming that collisions at the lowest temperature employed had a probability of unity. The data recorded at high humidity should be most relevant to atmospheric conditions, and the results indicate that parameterizations currently used in modelling studies to describe freezing rates are appropriate for kaolinite aerosol particles. Mechanisms for contact freezing are briefly discussed.
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Nagare, Baban, Claudia Marcolli, André Welti, Olaf Stetzer, and Ulrike Lohmann. "Comparing contact and immersion freezing from continuous flow diffusion chambers." Atmospheric Chemistry and Physics 16, no. 14 (July 19, 2016): 8899–914. http://dx.doi.org/10.5194/acp-16-8899-2016.
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Abstract. Ice nucleating particles (INPs) in the atmosphere are responsible for glaciating cloud droplets between 237 and 273 K. Different mechanisms of heterogeneous ice nucleation can compete under mixed-phase cloud conditions. Contact freezing is considered relevant because higher ice nucleation temperatures than for immersion freezing for the same INPs were observed. It has limitations because its efficiency depends on the number of collisions between cloud droplets and INPs. To date, direct comparisons of contact and immersion freezing with the same INP, for similar residence times and concentrations, are lacking. This study compares immersion and contact freezing efficiencies of three different INPs. The contact freezing data were obtained with the ETH CoLlision Ice Nucleation CHamber (CLINCH) using 80 µm diameter droplets, which can interact with INPs for residence times of 2 and 4 s in the chamber. The contact freezing efficiency was calculated by estimating the number of collisions between droplets and particles. Theoretical formulations of collision efficiencies gave too high freezing efficiencies for all investigated INPs, namely AgI particles with 200 nm electrical mobility diameter, 400 and 800 nm diameter Arizona Test Dust (ATD) and kaolinite particles. Comparison of freezing efficiencies by contact and immersion freezing is therefore limited by the accuracy of collision efficiencies. The concentration of particles was 1000 cm−3 for ATD and kaolinite and 500, 1000, 2000 and 5000 cm−3 for AgI. For concentrations < 5000 cm−3, the droplets collect only one particle on average during their time in the chamber. For ATD and kaolinite particles, contact freezing efficiencies at 2 s residence time were smaller than at 4 s, which is in disagreement with a collisional contact freezing process but in accordance with immersion freezing or adhesion freezing. With “adhesion freezing”, we refer to a contact nucleation process that is enhanced compared to immersion freezing due to the position of the INP on the droplet, and we discriminate it from collisional contact freezing, which assumes an enhancement due to the collision of the particle with the droplet. For best comparison with contact freezing results, immersion freezing experiments of the same INPs were performed with the continuous flow diffusion chamber Immersion Mode Cooling chAmber–Zurich Ice Nucleation Chamber (IMCA–ZINC) for a 3 s residence time. In IMCA–ZINC, each INP is activated into a droplet in IMCA and provides its surface for ice nucleation in the ZINC chamber. The comparison of contact and immersion freezing results did not confirm a general enhancement of freezing efficiency for contact compared with immersion freezing experiments. For AgI particles the onset of heterogeneous freezing in CLINCH was even shifted to lower temperatures compared with IMCA–ZINC. For ATD, freezing efficiencies for contact and immersion freezing experiments were similar. For kaolinite particles, contact freezing became detectable at higher temperatures than immersion freezing. Using contact angle information between water and the INP, it is discussed how the position of the INP in or on the droplets may influence its ice nucleation activity.
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Ettner, M., S. K. Mitra, and S. Borrmann. "Heterogeneous freezing of single sulfuric acid solution droplets: laboratory experiments utilizing an acoustic levitator." Atmospheric Chemistry and Physics 4, no. 7 (September 29, 2004): 1925–32. http://dx.doi.org/10.5194/acp-4-1925-2004.
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Abstract. The heterogeneous freezing temperatures of single binary sulfuric acid solution droplets were measured in dependency of acid concentration down to temperatures as low as -50°C. In order to avoid influence of supporting substrates on the freezing characteristics, a new technique has been developed to suspend the droplet by means of an acoustic levitator. The droplets contained immersed particles of graphite, kaolin or montmorillonite in order to study the influence of the presence of such contamination on the freezing temperature. The radii of the suspended droplets spanned the range between 0.4 and 1.1mm and the concentration of the sulfuric acid solution varied between 5 and 14 weight percent. The presence of the particles in the solution raises the freezing temperature with respect to homogeneous freezing of these solution droplets. The pure solution droplets can be supercooled up to 40 degrees below the ice-acid solution thermodynamic equilibrium curve. Depending on the concentration of sulfuric acid and the nature of the impurity the polluted droplets froze between -11°C and -35°C. The new experimental set-up, combining a deep freezer with a movable ultrasonic levitator and suitable optics, proved to be a useful approach for such investigations on individual droplets.
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Phillips, Vaughan T. J., Leo J. Donner, and Stephen T. Garner. "Nucleation Processes in Deep Convection Simulated by a Cloud-System-Resolving Model with Double-Moment Bulk Microphysics." Journal of the Atmospheric Sciences 64, no. 3 (March 1, 2007): 738–61. http://dx.doi.org/10.1175/jas3869.1.
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Abstract A novel type of limited double-moment scheme for bulk microphysics is presented here for cloud-system-resolving models (CSRMs). It predicts the average size of cloud droplets and crystals, which is important for representing the radiative impact of clouds on the climate system. In this new scheme, there are interactive components for ice nuclei (IN) and cloud condensation nuclei (CCN). For cloud ice, the processes of primary ice nucleation, Hallett–Mossop (HM) multiplication of ice particles (secondary ice production), and homogeneous freezing of aerosols and droplets provide the source of ice number. The preferential evaporation of smaller droplets during homogeneous freezing of cloud liquid is represented for the first time. Primary and secondary (i.e., in cloud) droplet nucleation are also represented, by predicting the supersaturation as a function of the vertical velocity and local properties of cloud liquid. A linearized scheme predicts the supersaturation, explicitly predicting rates of condensation and vapor deposition onto liquid (cloud liquid, rain) and ice (cloud ice, snow, graupel) species. The predicted supersaturation becomes the input for most nucleation processes, including homogeneous aerosol freezing and secondary droplet activation. Comparison of the scheme with available aircraft and satellite data is performed for two cases of deep convection over the tropical western Pacific Ocean. Sensitivity tests are performed with respect to a range of nucleation processes. The HM process of ice particle multiplication has an important impact on the domain-wide ice concentration in the lower half of the mixed-phase region, especially when a lack of upper-level cirrus suppresses homogeneous freezing. Homogeneous freezing of droplets and, especially, aerosols is found to be the key control on number and sizes of cloud particles in the simulated cloud ensemble. Preferential evaporation of smaller droplets during homogeneous freezing produces a major impact on ice concentrations aloft. Aerosols originating from the remote free troposphere become activated in deep convective updrafts and produce most of the supercooled cloud droplets that freeze homogeneously aloft. Homogeneous aerosol freezing is found to occur only in widespread regions of weak ascent while homogeneous droplet freezing is restricted to deep convective updrafts. This means that homogeneous aerosol freezing can produce many more crystals than homogeneous droplet freezing, if conditions in the upper troposphere are favorable. These competing mechanisms of homogeneous freezing determine the overall response of the ice concentration to environmental CCN concentrations in the simulated cloud ensemble. The corresponding sensitivity with respect to environmental IN concentrations is much lower. Nevertheless, when extremely high concentrations of IN are applied, that are typical for plumes of desert dust, the supercooled cloud liquid is completely eliminated in the upper half of the mixed phase region. This shuts down the process of homogeneous droplet freezing.
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Tong, H. J., B. Ouyang, F. D. Pope, and M. Kalberer. "A new electrodynamic balance design for low temperature studies." Atmospheric Measurement Techniques Discussions 7, no. 7 (July 28, 2014): 7671–700. http://dx.doi.org/10.5194/amtd-7-7671-2014.
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Abstract. In this paper we describe a newly designed cold electrodynamic balance (CEDB) system, which was built to study the evaporation kinetics and freezing properties of supercooled water droplets. The temperature of the CEDB chamber at the location of the levitated water droplet can be controlled in the range: −40 to +40 °C, which is achieved using a combination of liquid nitrogen cooling and heating by positive temperature coefficient heaters. The measurement of liquid droplet radius is obtained by analyzing the Mie elastic light scattering from a 532 nm laser. The Mie scattering signal was also used to characterize and distinguish droplet freezing events; liquid droplets produce a regular fringe pattern whilst the pattern from frozen particles is irregular. The evaporation rate of singly levitated water droplets was calculated from time resolved measurements of the radii of evaporating droplets and a clear trend of the evaporation rate on temperature was measured. The statistical freezing probabilities of aqueous pollen extracts (pollen washing water) are obtained in the temperature range: −4.5 to −40 °C. It was found that that pollen washing water from water birch (Betula fontinalis occidentalis) pollen can act as ice nuclei in the immersion freezing mode at temperatures as warm as −22.45 (±0.65) °C.
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O, Kuan-Ting, and Robert Wood. "Exploring an approximation for the homogeneous freezing temperature of water droplets." Atmospheric Chemistry and Physics 16, no. 11 (June 10, 2016): 7239–49. http://dx.doi.org/10.5194/acp-16-7239-2016.
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Abstract. In this work, based on the well-known formulae of classical nucleation theory (CNT), the temperature TNc = 1 at which the mean number of critical embryos inside a droplet is unity is derived from the Boltzmann distribution function and explored as an approximation for homogeneous freezing temperature of water droplets. Without including the information of the applied cooling rate γcooling and the number of observed droplets Ntotal_droplets in the calculation, the approximation TNc = 1 is able to reproduce the dependence of homogeneous freezing temperature on drop size V and water activity aw of aqueous drops observed in a wide range of experimental studies for droplet diameter > 10 µm and aw > 0.85, suggesting the effect of γcooling and Ntotal_droplets may be secondary compared to the effect of V and aw on homogeneous freezing temperatures in these size and water activity ranges under realistic atmospheric conditions. We use the TNc = 1 approximation to argue that the distribution of homogeneous freezing temperatures observed in the experiments may be partly explained by the spread in the size distribution of droplets used in the particular experiment. It thus appears that the simplicity of this approximation makes it potentially useful for predicting homogeneous freezing temperatures of water droplets in the atmosphere.
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Keinert, Alice, Dominik Spannagel, Thomas Leisner, and Alexei Kiselev. "Secondary Ice Production upon Freezing of Freely Falling Drizzle Droplets." Journal of the Atmospheric Sciences 77, no. 8 (August 1, 2020): 2959–67. http://dx.doi.org/10.1175/jas-d-20-0081.1.
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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.
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Tarn, Mark D., Sebastien N. F. Sikora, Grace C. E. Porter, Jung-uk Shim, and Benjamin J. Murray. "Homogeneous Freezing of Water Using Microfluidics." Micromachines 12, no. 2 (February 23, 2021): 223. http://dx.doi.org/10.3390/mi12020223.
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The homogeneous freezing of water is important in the formation of ice in clouds, but there remains a great deal of variability in the representation of the homogeneous freezing of water in the literature. The development of new instrumentation, such as droplet microfluidic platforms, may help to constrain our understanding of the kinetics of homogeneous freezing via the analysis of monodisperse, size-selected water droplets in temporally and spatially controlled environments. Here, we evaluate droplet freezing data obtained using the Lab-on-a-Chip Nucleation by Immersed Particle Instrument (LOC-NIPI), in which droplets are generated and frozen in continuous flow. This high-throughput method was used to analyse over 16,000 water droplets (86 μm diameter) across three experimental runs, generating data with high precision and reproducibility that has largely been unrepresented in the microfluidic literature. Using this data, a new LOC-NIPI parameterisation of the volume nucleation rate coefficient (JV(T)) was determined in the temperature region of −35.1 to −36.9 °C, covering a greater JV(T) compared to most other microfluidic techniques thanks to the number of droplets analysed. Comparison to recent theory suggests inconsistencies in the theoretical representation, further implying that microfluidics could be used to inform on changes to parameterisations. By applying classical nucleation theory (CNT) to our JV(T) data, we have gone a step further than other microfluidic homogeneous freezing examples by calculating the stacking-disordered ice–supercooled water interfacial energy, estimated to be 22.5 ± 0.7 mJ m−2, again finding inconsistencies when compared to theoretical predictions. Further, we briefly review and compile all available microfluidic homogeneous freezing data in the literature, finding that the LOC-NIPI and other microfluidically generated data compare well with commonly used non-microfluidic datasets, but have generally been obtained with greater ease and with higher numbers of monodisperse droplets.
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Tong, H. J., B. Ouyang, N. Nikolovski, D. M. Lienhard, F. D. Pope, and M. Kalberer. "A new electrodynamic balance (EDB) design for low-temperature studies: application to immersion freezing of pollen extract bioaerosols." Atmospheric Measurement Techniques 8, no. 3 (March 10, 2015): 1183–95. http://dx.doi.org/10.5194/amt-8-1183-2015.
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Abstract. In this paper we describe a newly designed cold electrodynamic balance(CEDB) system, built to study the evaporation kinetics and freezing properties of supercooled water droplets. The temperature of the CEDB chamber at the location of the levitated water droplet can be controlled in the range −40 to &plus;40 °C, which is achieved using a combination of liquid nitrogen cooling and heating by positive temperature coefficient heaters. The measurement of liquid droplet radius is obtained by analysing the Mie elastic light scattering from a 532 nm laser. The Mie scattering signal was also used to characterise and distinguish droplet freezing events; liquid droplets produce a regular fringe pattern, whilst the pattern from frozen particles is irregular. The evaporation rate of singly levitated water droplets was calculated from time-resolved measurements of the radii of evaporating droplets and a clear trend of the evaporation rate on temperature was measured. The statistical freezing probabilities of aqueous pollen extracts (pollen washing water) are obtained in the temperature range −4.5 to −40 °C. It was found that that pollen washing water from water birch (Betula fontinalis occidentalis) pollen can act as ice nuclei in the immersion freezing mode at temperatures as warm as −22.45 (±0.65) °C. Furthermore it was found that the protein-rich component of the washing water was significantly more ice-active than the non-proteinaceous component.
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O, K. T., and R. Wood. "An approximation for homogeneous freezing temperature of water droplets." Atmospheric Chemistry and Physics Discussions 15, no. 21 (November 12, 2015): 31867–89. http://dx.doi.org/10.5194/acpd-15-31867-2015.
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Abstract. In this work, based on the well-known formulae of classical nucleation theory (CNT), the temperature TNc = 1 at which the mean number of critical embryos inside a droplet is unity is derived and proposed as a new approximation for homogeneous freezing temperature of water droplets. Without consideration of time dependence and stochastic nature of the ice nucleation process, the approximation TNc = 1 is able to reproduce the dependence of homogeneous freezing temperature on drop size and water activity of aqueous drops observed in a wide range of experimental studies. We use the TNc = 1 approximation to argue that the distribution of homogeneous freezing temperatures observed in the experiments may largely be explained by the spread in the size distribution of droplets used in the particular experiment. It thus appears that this approximation is useful for predicting homogeneous freezing temperatures of water droplets in the atmosphere.
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Shayunusov, Doston, Dmitry Eskin, Boris V. Balakin, Svyatoslav Chugunov, Stein Tore Johansen, and Iskander Akhatov. "Modeling Water Droplet Freezing and Collision with a Solid Surface." Energies 14, no. 4 (February 16, 2021): 1020. http://dx.doi.org/10.3390/en14041020.
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Water droplets released from the sea surface represent one of the major causes of ice accretion on marine vessels. A one-dimensional model of the freezing of a spherical water droplet moving in cold air was developed. The crystallization model allows one to obtain an analytical solution if a uniform temperature distribution over the liquid’s core is assumed. The model was validated using STAR CCM+ Computational fluid dynamics (CFD) code. A collision of a partially frozen droplet with a solid wall assuming the plastic deformation of an ice crust was also considered. The ratio of the crust deformation to the crust thickness was evaluated. It was assumed that if this ratio were to exceed unity, the droplet would stick to the wall’s surface due to ice bridge formation caused by the water released from the droplet’s core.
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Vu, Truong V., Binh Duy Pham, Lien V. T. Nguyen, Cuong Nguyen, Hoe Nguyen, Vinh Nguyen, and Hung Vu. "DIRECT NUMERICAL SIMULATION STUDY OF WATER DROPLETS FREEZING ON A HORIZONTAL PLATE." Vietnam Journal of Science and Technology 59, no. 3 (May 17, 2021): 380. http://dx.doi.org/10.15625/2525-2518/59/3/15434.
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We present the numerical results of the solidification process of water droplets on a cold plate with different wetting angles. The numerical method used is an axisymmetric front-tracking technique. The water droplets are assumed as a spherical cap and placed on the cold plate which is kept at a subfreezing temperature. At the end of solidification, we obtain a small protrusion shape at the top of the frozen water droplet and its height is also higher than that of the initial water droplet. The frozen water droplets are also compared with the corresponding experimental ones reported in the literature.
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Polen, Michael, Thomas Brubaker, Joshua Somers, and Ryan C. Sullivan. "Cleaning up our water: reducing interferences from nonhomogeneous freezing of “pure” water in droplet freezing assays of ice-nucleating particles." Atmospheric Measurement Techniques 11, no. 9 (September 24, 2018): 5315–34. http://dx.doi.org/10.5194/amt-11-5315-2018.
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Abstract. Droplet freezing techniques (DFTs) have been used for half a century to measure the concentration of ice-nucleating particles (INPs) in the atmosphere and determine their freezing properties to understand the effects of INPs on mixed-phase clouds. The ice nucleation community has recently adopted droplet freezing assays as a commonplace experimental approach. These droplet freezing experiments are often limited by contamination that causes nonhomogeneous freezing of the “pure” water used to generate the droplets in the heterogeneous freezing temperature regime that is being measured. Interference from the early freezing of water is often overlooked and not fully reported, or measurements are restricted to analyzing the more ice-active INPs that freeze well above the temperature of the background water. However, this avoidance is not viable for analyzing the freezing behavior of less active INPs in the atmosphere that still have potentially important effects on cold-cloud microphysics. In this work we review a number of recent droplet freezing techniques that show great promise in reducing these interferences, and we report our own extensive series of measurements using similar methodologies. By characterizing the performance of different substrates on which the droplets are placed and of different pure water generation techniques, we recommend best practices to reduce these interferences. We tested different substrates, water sources, droplet matrixes, and droplet sizes to provide deeper insight into what methodologies are best suited for DFTs. Approaches for analyzing droplet freezing temperature spectra and accounting and correcting for the background “pure” water control spectrum are also presented. Finally, we propose experimental and data analysis procedures for future homogeneous and heterogeneous ice nucleation studies to promote a more uniform and reliable methodology that facilitates the ready intercomparison of ice-nucleating particles measured by DFTs.
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Beydoun, Hassan, Michael Polen, and Ryan C. Sullivan. "Effect of particle surface area on ice active site densities retrieved from droplet freezing spectra." Atmospheric Chemistry and Physics 16, no. 20 (October 28, 2016): 13359–78. http://dx.doi.org/10.5194/acp-16-13359-2016.
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Abstract. Heterogeneous ice nucleation remains one of the outstanding problems in cloud physics and atmospheric science. Experimental challenges in properly simulating particle-induced freezing processes under atmospherically relevant conditions have largely contributed to the absence of a well-established parameterization of immersion freezing properties. Here, we formulate an ice active, surface-site-based stochastic model of heterogeneous freezing with the unique feature of invoking a continuum assumption on the ice nucleating activity (contact angle) of an aerosol particle's surface that requires no assumptions about the size or number of active sites. The result is a particle-specific property g that defines a distribution of local ice nucleation rates. Upon integration, this yields a full freezing probability function for an ice nucleating particle. Current cold plate droplet freezing measurements provide a valuable and inexpensive resource for studying the freezing properties of many atmospheric aerosol systems. We apply our g framework to explain the observed dependence of the freezing temperature of droplets in a cold plate on the concentration of the particle species investigated. Normalizing to the total particle mass or surface area present to derive the commonly used ice nuclei active surface (INAS) density (ns) often cannot account for the effects of particle concentration, yet concentration is typically varied to span a wider measurable freezing temperature range. A method based on determining what is denoted an ice nucleating species' specific critical surface area is presented and explains the concentration dependence as a result of increasing the variability in ice nucleating active sites between droplets. By applying this method to experimental droplet freezing data from four different systems, we demonstrate its ability to interpret immersion freezing temperature spectra of droplets containing variable particle concentrations. It is shown that general active site density functions, such as the popular ns parameterization, cannot be reliably extrapolated below this critical surface area threshold to describe freezing curves for lower particle surface area concentrations. Freezing curves obtained below this threshold translate to higher ns values, while the ns values are essentially the same from curves obtained above the critical area threshold; ns should remain the same for a system as concentration is varied. However, we can successfully predict the lower concentration freezing curves, which are more atmospherically relevant, through a process of random sampling from g distributions obtained from high particle concentration data. Our analysis is applied to cold plate freezing measurements of droplets containing variable concentrations of particles from NX illite minerals, MCC cellulose, and commercial Snomax bacterial particles. Parameterizations that can predict the temporal evolution of the frozen fraction of cloud droplets in larger atmospheric models are also derived from this new framework.
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Alpert, Peter A., and Daniel A. Knopf. "Analysis of isothermal and cooling-rate-dependent immersion freezing by a unifying stochastic ice nucleation model." Atmospheric Chemistry and Physics 16, no. 4 (February 24, 2016): 2083–107. http://dx.doi.org/10.5194/acp-16-2083-2016.
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Abstract. Immersion freezing is an important ice nucleation pathway involved in the formation of cirrus and mixed-phase clouds. Laboratory immersion freezing experiments are necessary to determine the range in temperature, T, and relative humidity, RH, at which ice nucleation occurs and to quantify the associated nucleation kinetics. Typically, isothermal (applying a constant temperature) and cooling-rate-dependent immersion freezing experiments are conducted. In these experiments it is usually assumed that the droplets containing ice nucleating particles (INPs) all have the same INP surface area (ISA); however, the validity of this assumption or the impact it may have on analysis and interpretation of the experimental data is rarely questioned. Descriptions of ice active sites and variability of contact angles have been successfully formulated to describe ice nucleation experimental data in previous research; however, we consider the ability of a stochastic freezing model founded on classical nucleation theory to reproduce previous results and to explain experimental uncertainties and data scatter. A stochastic immersion freezing model based on first principles of statistics is presented, which accounts for variable ISA per droplet and uses parameters including the total number of droplets, Ntot, and the heterogeneous ice nucleation rate coefficient, Jhet(T). This model is applied to address if (i) a time and ISA-dependent stochastic immersion freezing process can explain laboratory immersion freezing data for different experimental methods and (ii) the assumption that all droplets contain identical ISA is a valid conjecture with subsequent consequences for analysis and interpretation of immersion freezing. The simple stochastic model can reproduce the observed time and surface area dependence in immersion freezing experiments for a variety of methods such as: droplets on a cold-stage exposed to air or surrounded by an oil matrix, wind and acoustically levitated droplets, droplets in a continuous-flow diffusion chamber (CFDC), the Leipzig aerosol cloud interaction simulator (LACIS), and the aerosol interaction and dynamics in the atmosphere (AIDA) cloud chamber. Observed time-dependent isothermal frozen fractions exhibiting non-exponential behavior can be readily explained by this model considering varying ISA. An apparent cooling-rate dependence of Jhet is explained by assuming identical ISA in each droplet. When accounting for ISA variability, the cooling-rate dependence of ice nucleation kinetics vanishes as expected from classical nucleation theory. The model simulations allow for a quantitative experimental uncertainty analysis for parameters Ntot, T, RH, and the ISA variability. The implications of our results for experimental analysis and interpretation of the immersion freezing process are discussed.
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Nagare, B., C. Marcolli, O. Stetzer, and U. Lohmann. "Estimating collision efficiencies from contact freezing experiments." Atmospheric Chemistry and Physics Discussions 15, no. 8 (April 23, 2015): 12167–212. http://dx.doi.org/10.5194/acpd-15-12167-2015.
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Abstract. Interactions of atmospheric aerosols with clouds influence cloud properties and modify the aerosol life cycle. Aerosol particles act as cloud condensation nuclei and ice nucleating particles or become incorporated into cloud droplets by scavenging. For an accurate description of aerosol scavenging and ice nucleation in contact mode, collision efficiency between droplets and aerosol particles needs to be known. This study derives the collision rate from experimental contact freezing data obtained with the ETH Collision Ice Nucleation Chamber CLINCH. Freely falling 80 μm water droplets are exposed to an aerosol consisting of 200 nm diameter silver iodide particles of concentrations from 500–5000 cm−3, which act as ice nucleating particles in contact mode. The chamber is kept at ice saturation in the temperature range from 236–261 K leading to slow evaporation of water droplets giving rise to thermophoresis and diffusiophoresis. Droplets and particles bear charges inducing electrophoresis. The experimentally derived collision efficiency of 0.13 is around one order of magnitude higher than theoretical formulations which include Brownian diffusion, impaction, interception, thermophoretic, diffusiophoretic and electric forces. This discrepancy is most probably due to uncertainties and inaccuracies in the description of thermophoretic and diffusiophoretic processes acting together. This is to the authors knowledge the first dataset of collision efficiencies acquired below 273 K. More such experiments with different droplet and particle diameters are needed to improve our understanding of collision processes acting together.
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Karlsson, Linn, Anna-Lena Ljung, and T. Staffan Lundström. "Comparing Internal Flow in Freezing and Evaporating Water Droplets Using PIV." Water 12, no. 5 (May 23, 2020): 1489. http://dx.doi.org/10.3390/w12051489.
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The study of evaporation and freezing of droplets is important in, e.g., spray cooling, surface coating, ink-jet printing, and when dealing with icing on wind turbines, airplane wings, and roads. Due to the complex nature of the flow within droplets, a wide range of temperatures, from freezing temperatures to heating temperatures, have to be taken into account in order to increase the understanding of the flow behavior. This study aimed to reveal if natural convection and/or Marangoni convection influence the flow in freezing and evaporating droplets. Droplets were released on cold and warm surfaces using similar experimental techniques and setups, and the internal flow within freezing and evaporating water droplets were then investigated and compared to one another using Particle Image Velocimetry. It was shown that, for both freezing and evaporating droplets, a shift in flow direction occurs early in the processes. For the freezing droplets, this effect could be traced to the Marangoni convection, but this could not be concluded for the evaporating droplets. For both evaporating and freezing droplets, after the shift in flow direction, natural convection dominates the flow. In the end of the freezing process, conduction seems to be the only contributing factor for the flow.
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Sear, R. P. "Generalisation of Levine's prediction for the distribution of freezing temperatures of droplets: a general singular model for ice nucleation." Atmospheric Chemistry and Physics Discussions 13, no. 4 (April 19, 2013): 10499–520. http://dx.doi.org/10.5194/acpd-13-10499-2013.
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Abstract. Models without an explicit time dependence, called singular models, are widely used for fitting the distribution of temperatures at which water droplets freeze. In 1950 Levine developed the original singular model. His key assumption was that each droplet contained many nucleation sites, and that freezing occurred due to the nucleation site with the highest freezing temperature. The fact that freezing occurs due to the maximum value out of large number of nucleation temperatures, means that we can apply the results of what is called extreme-value statistics. This is the statistics of the extreme, i.e., maximum or minimum, value of a large number of random variables. Here we use the results of extreme-value statistics to show that we can generalise Levine's model to produce the most general singular model possible. We show that when a singular model is a good approximation, the distribution of freezing temperatures should always be given by what is called the generalised extreme-value distribution. In addition, we also show that the distribution of freezing temperatures for droplets of one size, can be used to make predictions for the scaling of the median nucleation temperature with droplet size, and vice versa.
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Sear, R. P. "Generalisation of Levine's prediction for the distribution of freezing temperatures of droplets: a general singular model for ice nucleation." Atmospheric Chemistry and Physics 13, no. 14 (July 30, 2013): 7215–23. http://dx.doi.org/10.5194/acp-13-7215-2013.
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Abstract. Models without an explicit time dependence, called singular models, are widely used for fitting the distribution of temperatures at which water droplets freeze. In 1950 Levine developed the original singular model. His key assumption was that each droplet contained many nucleation sites, and that freezing occurred due to the nucleation site with the highest freezing temperature. The fact that freezing occurs due to the maximum value out of a large number of nucleation temperatures, means that we can apply the results of what is called extreme-value statistics. This is the statistics of the extreme, i.e. maximum or minimum, value of a large number of random variables. Here we use the results of extreme-value statistics to show that we can generalise Levine's model to produce the most general singular model possible. We show that when a singular model is a good approximation, the distribution of freezing temperatures should always be given by what is called the generalised extreme-value distribution. In addition, we also show that the distribution of freezing temperatures for droplets of one size, can be used to make predictions for the scaling of the median nucleation temperature with droplet size, and vice versa.
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Dutra, Lara, Ole Franz, Veli-Mikko Puupponen, and Marja Tiirola. "DNA recovery from Droplet Digital™ PCR emulsions using liquid nitrogen." BioTechniques 69, no. 6 (December 2020): 450–54. http://dx.doi.org/10.2144/btn-2020-0076.
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Droplet microfluidics is a technology that enables the production and manipulation of small volumes. In biosciences, the most popular application of this technology is Droplet Digital™ PCR (ddPCR™), where parallel nanoliter-scale PCR assays are used to provide a high sensitivity and specificity for DNA detection. However, the recovery of PCR products for downstream applications such as sequencing can be challenging due to the droplets' stability. Here we compared five methods for disrupting the droplets to recover DNA. We found that rapid freezing in liquid nitrogen results in a clear phase separation and recovery of up to 70% of the DNA content. Liquid nitrogen freezing can thus offer a simple and environmentally friendly protocol for recovering DNA from ddPCR.
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Luo, Beiping, Thomas Peter, and Paul Crutzen. "Freezing of stratospheric aerosol droplets." Geophysical Research Letters 21, no. 13 (June 22, 1994): 1447–50. http://dx.doi.org/10.1029/93gl03076.
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Guttman, Shani, Zvi Sapir, Moty Schultz, Alexander V. Butenko, Benjamin M. Ocko, Moshe Deutsch, and Eli Sloutskin. "How faceted liquid droplets grow tails." Proceedings of the National Academy of Sciences 113, no. 3 (January 5, 2016): 493–96. http://dx.doi.org/10.1073/pnas.1515614113.
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Liquid droplets, widely encountered in everyday life, have no flat facets. Here we show that water-dispersed oil droplets can be reversibly temperature-tuned to icosahedral and other faceted shapes, hitherto unreported for liquid droplets. These shape changes are shown to originate in the interplay between interfacial tension and the elasticity of the droplet’s 2-nm-thick interfacial monolayer, which crystallizes at some T = Ts above the oil’s melting point, with the droplet’s bulk remaining liquid. Strikingly, at still-lower temperatures, this interfacial freezing (IF) effect also causes droplets to deform, split, and grow tails. Our findings provide deep insights into molecular-scale elasticity and allow formation of emulsions of tunable stability for directed self-assembly of complex-shaped particles and other future technologies.
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Ettner, M., S. K. Mitra, and S. Borrmann. "Heterogeneous freezing of single sulphuric acid solution droplets: laboratory experiments utilising an acoustic levitator." Atmospheric Chemistry and Physics Discussions 4, no. 2 (March 25, 2004): 1887–909. http://dx.doi.org/10.5194/acpd-4-1887-2004.
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Abstract. The heterogeneous freezing temperatures of single binary sulphuric acid solution droplets were measured in dependency of acid concentration down to temperatures as low as −70°C. In order to avoid influence of supporting substrates on the freezing characteristics, the droplets were suspended by means of an acoustic levitator. The droplets contained immersed particles of graphite, kaolin or montmorillonite in order to study the influence of the presence of such contamination on the freezing temperature. The radii of the suspended droplets spanned the range between 0,4 and 1,1 mm and the concentration of the sulphuric acid solution varied between 5 and 25 weight percent. The presence of the particles in the solution raises the freezing temperature with respect to homogeneous freezing of these solution droplets. The pure solution droplets can be supercooled up to 40° below the ice-acid solution thermodynamic equilibrium curve. Depending on the concentration of sulphuric acid and the nature of the impurity the polluted droplets froze between −11°C and −35°C. The experimental set-up, combining a deep freezer with a movable ultrasonic levitator and suitable optics, proved to be a useful approach for such investigations on individual droplets.
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Budke, C., and T. Koop. "BINARY: an optical freezing array for assessing temperature and time dependence of heterogeneous ice nucleation." Atmospheric Measurement Techniques 8, no. 2 (February 10, 2015): 689–703. http://dx.doi.org/10.5194/amt-8-689-2015.
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Abstract. A new optical freezing array for the study of heterogeneous ice nucleation in microliter-sized droplets is introduced, tested and applied to the study of immersion freezing in aqueous Snomax® suspensions. In the Bielefeld Ice Nucleation ARraY (BINARY) ice nucleation can be studied simultaneously in 36 droplets at temperatures down to −40 °C (233 K) and at cooling rates between 0.1 and 10 K min−1. The droplets are separated from each other in individual compartments, thus preventing a Wegener–Bergeron–Findeisen type water vapor transfer between droplets as well as avoiding the seeding of neighboring droplets by formation and surface growth of frost halos. Analysis of freezing and melting occurs via an automated real-time image analysis of the optical brightness of each individual droplet. As an application ice nucleation in water droplets containing Snomax® at concentrations from 1 ng mL−1 to 1 mg mL−1 was investigated. Using different cooling rates, a small time dependence of ice nucleation induced by two different classes of ice nucleators (INs) contained in Snomax® was detected and the corresponding heterogeneous ice nucleation rate coefficient was quantified. The observed time dependence is smaller than those of other types of INs reported in the literature, suggesting that the BINARY setup is suitable for quantifying time dependence for most other INs of atmospheric interest, making it a useful tool for future investigations.
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Reicher, Naama, Lior Segev, and Yinon Rudich. "The WeIzmann Supercooled Droplets Observation on a Microarray (WISDOM) and application for ambient dust." Atmospheric Measurement Techniques 11, no. 1 (January 12, 2018): 233–48. http://dx.doi.org/10.5194/amt-11-233-2018.
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Abstract. The WeIzmann Supercooled Droplets Observation on Microarray (WISDOM) is a new setup for studying ice nucleation in an array of monodisperse droplets for atmospheric implications. WISDOM combines microfluidics techniques for droplets production and a cryo-optic stage for observation and characterization of freezing events of individual droplets. This setup is designed to explore heterogeneous ice nucleation in the immersion freezing mode, down to the homogeneous freezing of water (235 K) in various cooling rates (typically 0.1–10 K min−1). It can also be used for studying homogeneous freezing of aqueous solutions in colder temperatures. Frozen fraction, ice nucleation active surface site densities and freezing kinetics can be obtained from WISDOM measurements for hundreds of individual droplets in a single freezing experiment. Calibration experiments using eutectic solutions and previously studied materials are described. WISDOM also allows repeatable cycles of cooling and heating for the same array of droplets. This paper describes the WISDOM setup, its temperature calibration, validation experiments and measurement uncertainties. Finally, application of WISDOM to study the ice nucleating particle (INP) properties of size-selected ambient Saharan dust particles is presented.
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Clauss, T., A. Kiselev, S. Hartmann, S. Augustin, S. Pfeifer, D. Niedermeier, H. Wex, and F. Stratmann. "Application of linear polarized light for the discrimination of frozen and liquid droplets in ice nucleation experiments." Atmospheric Measurement Techniques 6, no. 4 (April 19, 2013): 1041–52. http://dx.doi.org/10.5194/amt-6-1041-2013.
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Abstract. We report on the development and test results of the new optical particle counter TOPS-Ice (Thermo-stabilized Optical Particle Spectrometer for the detection of Ice). The instrument uses measurements of the cross-polarized scattered light by single particles into the near-forward direction (42.5° ± 12.7°) to distinguish between spherical and non-spherical particles. This approach allows the differentiation between liquid water droplets (spherical) and ice particles (non-spherical) having similar volume-equivalent sizes and therefore can be used to determine the fraction of frozen droplets in a typical immersion freezing experiment. We show that the numerical simulation of the light scattered on non-spherical particles (spheroids in random orientation) considering the actual scattering geometry used in the instrument supports the validity of the approach, even though the cross-polarized component of the light scattered by spherical droplets does not vanish in this scattering angle. For the separation of the ice particle mode from the liquid droplet mode, we use the width of the pulse detected in the depolarization channel instead of the pulse height. Exploiting the intrinsic relationship between pulse height and pulse width for Gaussian pulses allows us to calculate the fraction of frozen droplets even if the liquid droplet mode dominates the particle ensemble. We present test results obtained with TOPS-Ice in the immersion freezing experiments at the laminar diffusion chamber LACIS (Leipzig Aerosol Cloud Interaction Simulator) and demonstrate the excellent agreement with the data obtained in similar experiments with a different optical instrument. Finally, the advantages of using the cross-polarized light measurements for the differentiation of liquid and frozen droplets in the realistic immersion freezing experiments are discussed.
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Clauss, T., A. Kiselev, S. Hartmann, S. Augustin, S. Pfeifer, D. Niedermeier, H. Wex, and F. Stratmann. "Application of linear polarized light for the discrimination of frozen and liquid droplets in ice nucleation experiments." Atmospheric Measurement Techniques Discussions 5, no. 4 (August 20, 2012): 5753–85. http://dx.doi.org/10.5194/amtd-5-5753-2012.
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Abstract. We report on the development and test results of the new optical particle counter TOPS-Ice (Thermostabilized Optical Particle Spectrometer for the detection of Ice particles). The instrument uses measurements of the depolarized component of light scattered by single particles into the near-forward direction (42.5° ± 12.7°) to distinguish between spherical and non-spherical particles. This approach allows the differentiation between liquid water droplets (spherical) and ice particles (non-spherical) having similar volume equivalent sizes and therefore can be used to determine the fraction of frozen droplets in a typical immersion freezing experiment. We show that the numerical simulation of the light scattering on non-spherical particles (ellipsoids in random orientation) with account for the actual scattering geometry used in the instrument supports the validity of the approach, even though the cross polarized component of the light scattered by spherical droplets is not vanishing in this scattering angle. For the separation of the ice particle mode from the liquid droplet mode, we use the width of the pulse detected in the depolarization channel instead of the pulse height. Exploiting the intrinsic relationship between pulse height and pulse width for Gaussian pulses allows us to calculate the fraction of frozen droplets even if the liquid droplet mode dominates the particle ensemble. We present test results obtained with TOPS-Ice in the immersion freezing experiments at the laminar diffusion chamber LACIS (Leipzig Aerosol Cloud Interaction Simulator) and demonstrate the excellent agreement with the data obtained in the same experiment with a different optical instrument. Finally, the advantages of using the cross-polarized light measurements for the differentiation of liquid and frozen droplets in the realistic immersion freezing experiments are discussed.
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Graeber, Gustav, Thomas M. Schutzius, Hadi Eghlidi, and Dimos Poulikakos. "Spontaneous self-dislodging of freezing water droplets and the role of wettability." Proceedings of the National Academy of Sciences 114, no. 42 (September 25, 2017): 11040–45. http://dx.doi.org/10.1073/pnas.1705952114.
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Spontaneous removal of liquid, solidifying liquid and solid forms of matter from surfaces, is of significant importance in nature and technology, where it finds applications ranging from self-cleaning to icephobicity and to condensation systems. However, it is a great challenge to understand fundamentally the complex interaction of rapidly solidifying, typically supercooled, droplets with surfaces, and to harvest benefit from it for the design of intrinsically icephobic materials. Here we report and explain an ice removal mechanism that manifests itself simultaneously with freezing, driving gradual self-dislodging of droplets cooled via evaporation and sublimation (low environmental pressure) or convection (atmospheric pressure) from substrates. The key to successful self-dislodging is that the freezing at the droplet free surface and the droplet contact area with the substrate do not occur simultaneously: The frozen phase boundary moves inward from the droplet free surface toward the droplet–substrate interface, which remains liquid throughout most of the process and freezes last. We observe experimentally, and validate theoretically, that the inward motion of the phase boundary near the substrate drives a gradual reduction in droplet–substrate contact. Concurrently, the droplet lifts from the substrate due to its incompressibility, density differences, and the asymmetric freezing dynamics with inward solidification causing not fully frozen mass to be displaced toward the unsolidified droplet–substrate interface. Depending on surface topography and wetting conditions, we find that this can lead to full dislodging of the ice droplet from a variety of engineered substrates, rendering the latter ice-free.
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Järvinen, Emma, Martin Schnaiter, Guillaume Mioche, Olivier Jourdan, Valery N. Shcherbakov, Anja Costa, Armin Afchine, et al. "Quasi-Spherical Ice in Convective Clouds." Journal of the Atmospheric Sciences 73, no. 10 (September 21, 2016): 3885–910. http://dx.doi.org/10.1175/jas-d-15-0365.1.
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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.
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Murray, B. J., T. W. Wilson, S. L. Broadley, and R. H. Wills. "Heterogeneous freezing of water droplets containing kaolinite and montmorillonite particles." Atmospheric Chemistry and Physics Discussions 10, no. 4 (April 16, 2010): 9695–729. http://dx.doi.org/10.5194/acpd-10-9695-2010.
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Abstract. Clouds composed of both ice particles and supercooled liquid water droplets exist at temperatures above ~236 K. These mixed phase clouds, which strongly impact climate, are very sensitive to the presence of solid particles that can catalyse freezing. In this paper we describe experiments to determine the rate at which kaolinite and montmorillonite nucleate ice when immersed within water droplets. These are the first immersion mode experiments in which the ice nucleating ability of individual minerals has been determined quantitatively. Water droplets containing a known amount of clay mineral were supported on a hydrophobic surface and cooled at a rate of 10 K min−1. The temperatures at which individual 10–40 μm diameter droplets froze were determined by optical microscopy. As the concentration of kaolinite in the droplets was increased from 0.005 wt% to 1 wt% the median nucleation temperature increased from close to the homogeneous nucleation limit (236 K) to 240.8±0.6 K. We go onto show that the probability of freezing scales with surface area of the kaolinite inclusions rather than, as is often assumed, the volume of the droplet. When droplets contained montmorillonite ice always nucleated at 245.8±0.6 K, independent of the mineral concentration. We report temperature dependent nucleation rates and present parameterisations for nucleation by these minerals which capture the surface area and cooling rate dependence of the nucleation rate. We show that our parameterisations produce significantly different results to parameterisations employed in global models. These results also highlight the importance of understanding the ice nucleating properties of individual minerals rather than complex mixtures of minerals found in natural dusts and so-called test dusts.
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Fagerström, Erik, Anna-Lena Ljung, Linn Karlsson, and Henrik Lycksam. "Influence of Substrate Material on Flow in Freezing Water Droplets—An Experimental Study." Water 13, no. 12 (June 9, 2021): 1628. http://dx.doi.org/10.3390/w13121628.
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Freezing water droplets are a natural phenomenon that occurs regularly in the Arctic climate. It affects areas such as aircrafts, wind turbine blades and roads, where it can be a safety issue. To further scrutinize the freezing process, the main objective of this paper is to experimentally examine the influence of substrate material on the internal flow of a water droplet. The secondary goal is to reduce uncertainties in the freezing process by decreasing the randomness of the droplet size and form by introducing a groove in the substrate material. Copper, aluminium and steel was chosen due to their differences in thermal conductivities. Measurements were performed with Particle Image Velociometry (PIV) to be able to analyse the velocity field inside the droplet during the freezing process. During the investigation for the secondary goal, it could be seen that by introducing a groove in the substrate material, the contact radius could be controlled with a standard deviation of 0.85%. For the main objective, the velocity profile was investigated during different stages of the freezing process. Five points along the symmetry line of the droplet were compared and copper, which also has the highest thermal conductivity, showed the highest internal velocity. The difference between aluminium and steel was in their turn more difficult to distinguish, since the maximum velocity switched between the two materials along the symmetry line.
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Budke, C., and T. Koop. "BINARY: an optical freezing array for assessing temperature and time dependence of heterogeneous ice nucleation." Atmospheric Measurement Techniques Discussions 7, no. 9 (September 10, 2014): 9137–72. http://dx.doi.org/10.5194/amtd-7-9137-2014.
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Abstract. A new optical freezing array for the study of heterogeneous ice nucleation in microliter-sized droplets is introduced, tested and applied to the study of immersion freezing in aqueous Snomax® suspensions. In the Bielefeld Ice Nucleation ARraY (BINARY) ice nucleation can be studied simultaneously in 36 droplets at temperatures down to −40 °C (233 K) and at cooling rates between 0.1 K min−1 and 10 K min−1. The droplets are separated from each other in individual compartments, thus preventing a Wegener–Bergeron–Findeisen type water vapor transfer between droplets as well as avoiding the seeding of neighboring droplets by formation and surface growth of frost halos. Analysis of freezing and melting occurs via an automated real time image analysis of the optical brightness of each individual droplet. As an application ice nucleation in water droplets containing Snomax® at concentrations from 1 ng mL−1 to 1 mg mL−1 was investigated. Using different cooling rates a minute time dependence of ice nucleation induced by Class A and Class C ice nucleators contained in Snomax® was detected. For the Class A IN a very strong increase of the heterogeneous ice nucleation rate coefficient with decreasing temperature of λ ≡ −dln(jhet)/dT = 8.7 K−1 was observed emphasizing the capability of the BINARY device. This value is larger than those of other types of IN reported in the literature, suggesting that the BINARY setup is suitable for quantifying time dependence for most other IN of atmospheric interest, making it a useful tool for future investigations.
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Nespoulous, Mathieu, Renaud Denoyel, and Mickaël Antoni. "Microstructure Formation in Freezing Nanosuspension Droplets." Journal of Physical Chemistry Letters 9, no. 10 (May 7, 2018): 2714–19. http://dx.doi.org/10.1021/acs.jpclett.8b00984.
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Shaw, Raymond A., and Dennis Lamb. "Homogeneous freezing of evaporating cloud droplets." Geophysical Research Letters 26, no. 8 (April 15, 1999): 1181–84. http://dx.doi.org/10.1029/1999gl900170.
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Wardhono, Endarto Yudo, Mekro Permana Pinem, Hadi Wahyudi, and Sri Agustina. "Calorimetry Technique for Observing the Evolution of Dispersed Droplets of Concentrated Water-in-Oil (W/O) Emulsion during Preparation, Storage and Destabilization." Applied Sciences 9, no. 24 (December 4, 2019): 5271. http://dx.doi.org/10.3390/app9245271.
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In this work, the evolution of dispersed droplets in a water-in-oil (W/O) emulsion during formation, storage, and destabilization was observed using a calorimetry technique. The emulsion was prepared by dispersing drop by drop an aqueous phase into an oil continuous phase at room temperature using a rotor-stator homogenizer. The evolution of droplets during (1) preparation; (2) storage; and (3) destabilization was observed using differential scanning calorimetry (DSC). The samples were gently cooled-down below its solid-liquid equilibrium temperature then heated back above the melting point to determine its freezing temperature. The energy released during the process was recorded in order to get information about the water droplet dispersion state. The mean droplet size distribution of the sample emulsion was correlated to its freezing temperature and the morphology was followed by optical microscopy. The results indicated that the calorimetry technique is so far a very good technique of characterization concentrated W/O emulsions.
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Kulkarni, Gourihar, Naruki Hiranuma, Ottmar Möhler, Kristina Höhler, Swarup China, Daniel J. Cziczo, and Paul J. DeMott. "A new method for operating a continuous-flow diffusion chamber to investigate immersion freezing: assessment and performance study." Atmospheric Measurement Techniques 13, no. 12 (December 9, 2020): 6631–43. http://dx.doi.org/10.5194/amt-13-6631-2020.
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Abstract. Glaciation in mixed-phase clouds predominantly occurs through the immersion-freezing mode where ice-nucleating particles (INPs) immersed within supercooled droplets induce the nucleation of ice. Model representations of this process currently are a large source of uncertainty in simulating cloud radiative properties, so to constrain these estimates, continuous-flow diffusion chamber (CFDC)-style INP devices are commonly used to assess the immersion-freezing efficiencies of INPs. This study explored a new approach to operating such an ice chamber that provides maximum activation of particles without droplet breakthrough and correction factor ambiguity to obtain high-quality INP measurements in a manner that previously had not been demonstrated to be possible. The conditioning section of the chamber was maintained at −20 ∘C and water relative humidity (RHw) conditions of 113 % to maximize the droplet activation, and the droplets were supercooled with an independently temperature-controlled nucleation section at a steady cooling rate (0.5 ∘C min−1) to induce the freezing of droplets and evaporation of unfrozen droplets. The performance of the modified compact ice chamber (MCIC) was evaluated using four INP species: K-feldspar, illite-NX, Argentinian soil dust, and airborne soil dusts from an arable region that had shown ice nucleation over a wide span of supercooled temperatures. Dry-dispersed and size-selected K-feldspar particles were generated in the laboratory. Illite-NX and soil dust particles were sampled during the second phase of the Fifth International Ice Nucleation Workshop (FIN-02) campaign, and airborne soil dust particles were sampled from an ambient aerosol inlet. The measured ice nucleation efficiencies of model aerosols that had a surface active site density (ns) metric were higher but mostly agreed within 1 order of magnitude compared to results reported in the literature.
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Welti, A., F. Lüönd, Z. A. Kanji, O. Stetzer, and U. Lohmann. "Time dependence of immersion freezing." Atmospheric Chemistry and Physics Discussions 12, no. 5 (May 16, 2012): 12623–62. http://dx.doi.org/10.5194/acpd-12-12623-2012.
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Abstract. The time dependence of immersion freezing was studied for temperatures between 236 K and 243 K. Droplets with single immersed, size-selected 400 nm and 800 nm kaolinite particles were produced at 300 K, cooled down to supercooled temperatures typical for mixed-phase cloud conditions, and the fraction of frozen droplets with increasing residence time was detected. To simulate the conditions of immersion freezing in mixed-phase clouds we used the Zurich Ice Nucleation Chamber (ZINC) and its vertical extension, the Immersion Mode Cooling chAmber (IMCA). We observed that the frozen fraction of droplets increased with increasing residence time in the chamber. This suggests that there is a time dependence of immersion freezing and supports the importance of a stochastic component in the ice nucleation process. The rate at which droplets freeze was observed to decrease towards higher temperatures and smaller particle sizes. Comparison of the laboratory data with four different ice nucleation models, three based on classical nucleation theory with different representations of the particle surface properties and one singular, suggest that the classical, stochastic approach combined with a distribution of contact angles is able to reproduce the ice nucleation observed in these experiments most accurately. Using the models to calculate the increase in frozen fraction at typical mixed-phase cloud temperatures over an extended period of time, yields an equivalent effect of −1 K temperature shift and an increase in time scale by a factor of ~10.
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Grawe, Sarah, Stefanie Augustin-Bauditz, Hans-Christian Clemen, Martin Ebert, Stine Eriksen Hammer, Jasmin Lubitz, Naama Reicher, et al. "Coal fly ash: linking immersion freezing behavior and physicochemical particle properties." Atmospheric Chemistry and Physics 18, no. 19 (October 2, 2018): 13903–23. http://dx.doi.org/10.5194/acp-18-13903-2018.
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Abstract. To date, only a few studies have investigated the potential of coal fly ash particles to trigger heterogeneous ice nucleation in cloud droplets. The presented measurements aim at expanding the sparse dataset and improving process understanding of how physicochemical particle properties can influence the freezing behavior of coal fly ash particles immersed in water. Firstly, immersion freezing measurements were performed with two single particle techniques, i.e., the Leipzig Aerosol Cloud Interaction Simulator (LACIS) and the SPectrometer for Ice Nuclei (SPIN). The effect of suspension time on the efficiency of the coal fly ash particles when immersed in a cloud droplet is analyzed based on the different residence times of the two instruments and employing both dry and wet particle generation. Secondly, two cold-stage setups, one using microliter sized droplets (Leipzig Ice Nucleation Array) and one using nanoliter sized droplets (WeIzmann Supercooled Droplets Observation on Microarray setup) were applied. We found that coal fly ash particles are comparable to mineral dust in their immersion freezing behavior when being dry generated. However, a significant decrease in immersion freezing efficiency was observed during experiments with wet-generated particles in LACIS and SPIN. The efficiency of wet-generated particles is in agreement with the cold-stage measurements. In order to understand the reason behind the deactivation, a series of chemical composition, morphology, and crystallography analyses (single particle mass spectrometry, scanning electron microscopy coupled with energy dispersive X-ray microanalysis, X-ray diffraction analysis) were performed with dry- and wet-generated particles. From these investigations, we conclude that anhydrous CaSO4 and CaO – which, if investigated in pure form, show the same qualitative immersion freezing behavior as observed for dry-generated coal fly ash particles – contribute to triggering heterogeneous ice nucleation at the particle–water interface. The observed deactivation in contact with water is related to changes in the particle surface properties which are potentially caused by hydration of CaSO4 and CaO. The contribution of coal fly ash to the ambient population of ice-nucleating particles therefore depends on whether and for how long particles are immersed in cloud droplets.
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Bromley, Keith M., and Cait E. MacPhee. "BslA-stabilized emulsion droplets with designed microstructure." Interface Focus 7, no. 4 (June 16, 2017): 20160124. http://dx.doi.org/10.1098/rsfs.2016.0124.
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Emulsions are a central component of many modern formulations in food, pharmaceuticals, agrichemicals and personal care products. The droplets in these formulations are limited to being spherical as a consequence of the interfacial tension between the dispersed phase and continuous phase. The ability to control emulsion droplet morphology and stabilize non-spherical droplets would enable the modification of emulsion properties such as stability, substrate binding, delivery rate and rheology. One way of controlling droplet microstructure is to apply an elastic film around the droplet to prevent it from relaxing into a sphere. We have previously shown that BslA, an interfacial protein produced by the bacterial genus Bacillus , forms an elastic film when exposed to an oil- or air–water interface. Here, we highlight BslA's ability to stabilize anisotropic emulsion droplets. First, we show that BslA is capable of arresting dynamic emulsification processes leading to emulsions with variable morphologies depending on the conditions and emulsification technique applied. We then show that frozen emulsion droplets can be manipulated to induce partial coalescence. The structure of the partially coalesced droplets is retained after melting, but only when there is sufficient free BslA in the continuous phase. That the fidelity of replication can be tuned by adjusting the amount of free BslA in solution suggests that freezing BslA-stabilized droplets disrupts the BslA film. Finally, we use BslA's ability to preserve emulsion droplet structural integrity throughout the melting process to design emulsion droplets with a chosen shape and size.
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Swanson, Brian D. "How Well Does Water Activity Determine Homogeneous Ice Nucleation Temperature in Aqueous Sulfuric Acid and Ammonium Sulfate Droplets?" Journal of the Atmospheric Sciences 66, no. 3 (March 1, 2009): 741–54. http://dx.doi.org/10.1175/2008jas2542.1.
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Abstract Frozen fraction measurements made using a droplet free-fall freezing tube apparatus are presented and used, along with other recent laboratory measurements, to evaluate how well both the water activity idea and the translated melting-point curve idea of Koop et al. predict homogeneous freezing-point temperatures for aqueous ammonium sulfate and sulfuric acid solution droplets. The new freezing-point temperature datasets agree with the previous lowest-temperature results for both solutes. The lowest measured freezing-point temperatures for aqueous ammonium sulfate solutions agree with a curve shaped like the translated melting-point curve. However, those for aqueous sulfuric acid solutions are significantly lower than predicted by the translated melting-point curve idea, and a single water activity freezing-point temperature curve does not represent the lowest-temperature freezing-point temperature data for both solutes. A linear extrapolation of the new aqueous sulfuric acid solution freezing data to low temperatures predicts that high critical supersaturations in cloud-free regions of the upper troposphere will occur when homogeneous ice nucleation in an aqueous sulfuric acid aerosol is the primary ice formation mechanism.
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Nagare, B., C. Marcolli, O. Stetzer, and U. Lohmann. "Comparison of measured and calculated collision efficiencies at low temperatures." Atmospheric Chemistry and Physics 15, no. 23 (December 15, 2015): 13759–76. http://dx.doi.org/10.5194/acp-15-13759-2015.
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Abstract. Interactions of atmospheric aerosols with clouds influence cloud properties and modify the aerosol life cycle. Aerosol particles act as cloud condensation nuclei and ice nucleating particles or become incorporated into cloud droplets by scavenging. For an accurate description of aerosol scavenging and ice nucleation in contact mode, collision efficiency between droplets and aerosol particles needs to be known. This study derives the collision rate from experimental contact freezing data obtained with the ETH CoLlision Ice Nucleation CHamber (CLINCH). Freely falling 80 μm diameter water droplets are exposed to an aerosol consisting of 200 and 400 nm diameter silver iodide particles of concentrations from 500 to 5000 and 500 to 2000 cm−3, respectively, which act as ice nucleating particles in contact mode. The experimental data used to derive collision efficiency are in a temperature range of 238–245 K, where each collision of silver iodide particles with droplets can be assumed to result in the freezing of the droplet. An upper and lower limit of collision efficiency is also estimated for 800 nm diameter kaolinite particles. The chamber is kept at ice saturation at a temperature range of 236 to 261 K, leading to the slow evaporation of water droplets giving rise to thermophoresis and diffusiophoresis. Droplets and particles bear charges inducing electrophoresis. The experimentally derived collision efficiency values of 0.13, 0.07 and 0.047–0.11 for 200, 400 and 800 nm particles are around 1 order of magnitude higher than theoretical formulations which include Brownian diffusion, impaction, interception, thermophoretic, diffusiophoretic and electric forces. This discrepancy is most probably due to uncertainties and inaccuracies in the description of thermophoretic and diffusiophoretic processes acting together. This is, to the authors' knowledge, the first data set of collision efficiencies acquired below 273 K. More such experiments with different droplet and particle diameters are needed to improve our understanding of collision processes acting together.
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Kuhn, T., M. E. Earle, A. F. Khalizov, and J. J. Sloan. "Size dependence of volume and surface nucleation rates for homogeneous freezing of supercooled water droplets." Atmospheric Chemistry and Physics Discussions 9, no. 5 (October 28, 2009): 22929–53. http://dx.doi.org/10.5194/acpd-9-22929-2009.
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Abstract. We investigated the relative roles of volume and surface nucleation in the freezing of water droplets. Nucleation experiments were carried out in a cryogenic laminar aerosol flow tube using supercooled liquid water aerosols with radii between about 1 and 3 μ m. Temperature- and size-dependent values of volume- and surface-based homogeneous nucleation rate between 234.8 and 236.2 K are derived with help of a microphysical model from aerosol compositions and size distributions based on infrared extinction measurements in the aerosol flow tube. The results show that the contribution from nucleation at the droplet surface increases with decreasing droplet radius and dominates over nucleation in the bulk droplet volume for droplets with radii smaller than approximately 5 μm. This is interpreted in terms of a lowered free energy of ice germ formation in the surface-based process and has implications for the parameterization of homogeneous ice nucleation in numerical models.
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Kuhn, T., M. E. Earle, A. F. Khalizov, and J. J. Sloan. "Size dependence of volume and surface nucleation rates for homogeneous freezing of supercooled water droplets." Atmospheric Chemistry and Physics 11, no. 6 (March 28, 2011): 2853–61. http://dx.doi.org/10.5194/acp-11-2853-2011.
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Abstract. The relative roles of volume and surface nucleation were investigated for the homogeneous freezing of pure water droplets. Experiments were carried out in a cryogenic laminar aerosol flow tube using supercooled water aerosols with maximum volume densities at radii between 1 and 3 μm. Temperature- and size-dependent values of volume- and surface-based homogeneous nucleation rates between 234.8 and 236.2 K were derived using a microphysical model and aerosol phase compositions and size distributions determined from infrared extinction measurements in the flow tube. The results show that the contribution from nucleation at the droplet surface increases with decreasing droplet radius and dominates over nucleation in the bulk droplet volume for droplets with radii smaller than approximately 5 μm. This is interpreted in terms of a lowered free energy of ice germ formation in the surface-based process. The implications of surface nucleation for the parameterization of homogeneous ice nucleation in numerical models are considered.
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Peckhaus, Andreas, Alexei Kiselev, Thibault Hiron, Martin Ebert, and Thomas Leisner. "A comparative study of K-rich and Na/Ca-rich feldspar ice-nucleating particles in a nanoliter droplet freezing assay." Atmospheric Chemistry and Physics 16, no. 18 (September 15, 2016): 11477–96. http://dx.doi.org/10.5194/acp-16-11477-2016.
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Abstract. A recently designed droplet freezing assay was used to study the freezing of up to 1500 identical 0.2 nL water droplets containing suspensions of one Na/Ca-rich feldspar and three K-rich and one Na/Ca-rich feldspar particles. Three types of experiments have been conducted: cooling ramp, isothermal freezing at a constant temperature, and freeze–thaw cycles. The observed freezing behavior has been interpreted with the help of a model based on the classical nucleation theory (soccer ball model (SBM); Niedermeier et al., 2015). By applying the model to the different freezing experiments conducted with the same ice-nucleating material, the unique sets of model parameters for specific feldspar suspensions could be derived. The SBM was shown to adequately describe the observed cooling rate dependence, the ice-nucleating active sites (INAS) surface density ns(T) in a wide temperature range, and the shift of the freezing curves towards lower temperature with dilution. Moreover, the SBM was capable of reproducing the variation of INAS surface density ns(T) with concentration of ice-nucleating particles in the suspension droplets and correctly predicting the leveling-off of ns(T) at low temperature. The freeze–thaw experiments have clearly shown that the heterogeneous freezing induced even by very active ice-nucleating species still possesses a stochastic nature, with the degree of randomness increasing towards homogeneous nucleation. A population of the high-temperature INAS has been identified in one of the K-rich feldspar samples. The freezing of 0.8 wt % suspension droplets of this particular feldspar was observed already at −5 °C. These high-temperature active sites could be deactivated by treating the sample with hydrogen peroxide but survived heating up to 90 °C. Given a high mass concentration of these high-temperature active sites (2.9 × 108 g−1) and a very low value of contact angle (0.56 rad) the possibility of biological contamination of the sample was concluded to be unlikely but could not be completely ruled out. The freezing efficacy of all feldspar samples has been shown to reduce only slightly after suspension in water for over 5 months.