scholarly journals Comparative study on immersion freezing utilizing single-droplet levitation methods

2021 ◽  
Vol 21 (5) ◽  
pp. 3289-3316
Author(s):  
Miklós Szakáll ◽  
Michael Debertshäuser ◽  
Christian Philipp Lackner ◽  
Amelie Mayer ◽  
Oliver Eppers ◽  
...  
Keyword(s):  
Active Sites ◽  
Temperature Shift ◽  
Freezing Temperature ◽  
Stochastic Approach ◽  
Ice Nucleation ◽  
Biological Species ◽  
Single Droplet ◽  
Cooling Rates ◽  
Immersion Freezing ◽  
Comparison Of The Results

Abstract. Immersion freezing experiments were performed utilizing two distinct single-droplet levitation methods. In the Mainz vertical wind tunnel, supercooled droplets of 700 µm diameter were freely floated in a vertical airstream at constant temperatures ranging from −5 to −30 ∘C, where heterogeneous freezing takes place. These investigations under isothermal conditions allow the application of the stochastic approach to analyze and interpret the results in terms of the freezing or nucleation rate. In the Mainz acoustic levitator, 2 mm diameter drops were levitated while their temperature was continuously cooling from +20 to −28 ∘C by adapting to the ambient temperature. Therefore, in this case the singular approach was used for analysis. From the experiments, the densities of ice nucleation active sites were obtained as a function of temperature. The direct comparison of the results from two different instruments indicates a shift in the mean freezing temperatures of the investigated drops towards lower values that was material-dependent. As ice-nucleating particles, seven materials were investigated; two representatives of biological species (fibrous and microcrystalline cellulose), four mineral dusts (feldspar, illite NX, montmorillonite, and kaolinite), and natural Sahara dust. Based on detailed analysis of our results we determined a material-dependent parameter for calculating the freezing-temperature shift due to a change in cooling rate for each investigated particle type. The analysis allowed further classification of the investigated materials to be described by a single- or a multiple-component approach. From our experiences during the present synergetic studies, we listed a number of suggestions for future experiments regarding cooling rates, determination of the drop temperature, purity of the water used to produce the drops, and characterization of the ice-nucleating material. The observed freezing-temperature shift is significantly important for the intercomparison of ice nucleation instruments with different cooling rates.

scholarly journals Comparative Study On Immersion Freezing Utilizing Single Droplet Levitation Methods

2020 ◽  
Author(s):  
Miklós Szakáll ◽  
Michael Debertshäuser ◽  
Christian Philipp Lackner ◽  
Amelie Mayer ◽  
Oliver Eppers ◽  
...  
Keyword(s):  
High Speed ◽  
Active Sites ◽  
Cloud Model ◽  
Temperature Shift ◽  
Freezing Temperature ◽  
Biological Species ◽  
Temperature Correction ◽  
Single Droplet ◽  
Cooling Rates ◽  
Immersion Freezing

Abstract. Immersion freezing experiments were performed utilizing two distinct single-droplet levitation methods. In the Mainz vertical wind tunnel (M-WT) supercooled droplets of 700 μm diameter were freely floated in a vertical air stream at constant temperatures ranging from −5 °C to −30 °C where heterogeneous freezing takes place. These investigations under isothermal conditions allow applying the stochastic approach to analyze and interpret the results in terms of the freezing or nucleation rate. In the Mainz acoustic levitator (M-AL) 2 mm diameter drops were levitated while their temperature was continuously cooling from +20 °C to −28 °C by adapting to the ambient temperature. Therefore, in this case the singular approach was used for analysis. From the experiments, the densities of ice nucleating active sites (INAS) were obtained as function of temperature. The direct comparison of the results from two different instruments indicates a shift of the freezing temperatures towards lower values that was material dependent. As ice nucleating particles, seven materials were investigated, two representatives of biological species (fibrous and microcrystalline cellulose), four mineral dusts (feldspar, illite NX, montmorillonite, and kaolinite), and natural Sahara dust. Based on detailed analysis of our results we determined a material dependent temperature correction factor for each investigated particle type. The analysis allowed further classifying the investigated materials as single- or multiple-component. From our experiences during the present synergetic studies, we listed a number of suggestions for future experiments regarding cooling rates, determination of the drop temperature, purity of the water used to produce the drops, and characterization of the ice nucleating material. The observed freezing temperature shift is significantly important not only for the intercomparison of ice nucleation instruments with different cooling rates but also for cloud model simulations with high speed ascents of air masses.

scholarly journals An instrument for quantifying heterogeneous ice nucleation in multiwell plates using infrared emissions to detect freezing

2018 ◽  
Vol 11 (10) ◽  
pp. 5629-5641 ◽  
Author(s):  
Alexander D. Harrison ◽  
Thomas F. Whale ◽  
Rupert Rutledge ◽  
Stephen Lamb ◽  
Mark D. Tarn ◽  
...  
Keyword(s):  
Active Sites ◽  
Freezing Temperature ◽  
Equilibrium Temperature ◽  
Ice Nucleation ◽  
Ir Camera ◽  
Low Concentrations ◽  
Immersion Freezing ◽  
Mixed Phase Clouds ◽  
The City ◽  
Good Agreement

Abstract. Low concentrations of ice-nucleating particles (INPs) are thought to be important for the properties of mixed-phase clouds, but their detection is challenging. Hence, there is a need for instruments where INP concentrations of less than 0.01 L−1 can be routinely and efficiently determined. The use of larger volumes of suspension in drop assays increases the sensitivity of an experiment to rarer INPs or rarer active sites due to the increase in aerosol or surface area of particulates per droplet. Here we describe and characterise the InfraRed-Nucleation by Immersed Particles Instrument (IR-NIPI), a new immersion freezing assay that makes use of IR emissions to determine the freezing temperature of individual 50 µL droplets each contained in a well of a 96-well plate. Using an IR camera allows the temperature of individual aliquots to be monitored. Freezing temperatures are determined by detecting the sharp rise in well temperature associated with the release of heat caused by freezing. In this paper we first present the calibration of the IR temperature measurement, which makes use of the fact that following ice nucleation aliquots of water warm to the ice–liquid equilibrium temperature (i.e. 0 ∘C when water activity is ∼1), which provides a point of calibration for each individual well in each experiment. We then tested the temperature calibration using ∼100 µm chips of K-feldspar, by immersing these chips in 1 µL droplets on an established cold stage (µL-NIPI) as well as in 50 µL droplets on IR-NIPI; the results were consistent with one another, indicating no bias in the reported freezing temperature. In addition we present measurements of the efficiency of the mineral dust NX-illite and a sample of atmospheric aerosol collected on a filter in the city of Leeds. NX-illite results are consistent with literature data, and the atmospheric INP concentrations were in good agreement with the results from the µL-NIPI instrument. This demonstrates the utility of this approach, which offers a relatively high throughput of sample analysis and access to low INP concentrations.

scholarly journals Effect of particle surface area on ice active site densities retrieved from droplet freezing spectra

2016 ◽  
Vol 16 (20) ◽  
pp. 13359-13378 ◽  
Author(s):  
Hassan Beydoun ◽  
Michael Polen ◽  
Ryan C. Sullivan
Keyword(s):  
Surface Area ◽  
Active Sites ◽  
Particle Surface ◽  
Active Surface ◽  
Freezing Temperature ◽  
Ice Nucleation ◽  
Critical Surface ◽  
Cold Plate ◽  
Particle Surface Area ◽  
Immersion Freezing

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.

scholarly journals Ice nucleation efficiency of AgI: review and new insights

2016 ◽  
Author(s):  
Claudia Marcolli ◽  
Baban Nagare ◽  
André Welti ◽  
Ulrike Lohmann
Keyword(s):  
Water Saturation ◽  
Experimental Studies ◽  
Freezing Temperature ◽  
Nucleating Agent ◽  
Companion Paper ◽  
Chem Phys ◽  
Ice Nucleation ◽  
Lattice Match ◽  
Ice Nuclei ◽  
Immersion Freezing

Abstract. AgI is one of the best investigated ice nuclei. It has relevance for the atmosphere since it is used for glaciogenic cloud seeding. Theoretical and experimental studies over the last sixty years provide a complex picture of silver iodide as ice nucleating agent with conflicting and inconsistent results. This review compares experimental ice nucleation studies in order to analyse the factors that influence the ice nucleation ability of AgI. We have performed experiments to compare contact and immersion freezing by AgI. This is one of three papers that describe and analyse contact and immersion freezing experiments with AgI. In Nagare et al. (Nagare, B., Marcolli, C., Stetzer, O., and Lohmann, U.: Comparison of measured and calculated collision efficiencies at low temperatures, Atmos. Chem. Phys., 15, 13759–13776, doi:10.5194/acp-15-13759-2015, 2015) collision efficiencies based on contact freezing experiments with AgI are determined and compared with theoretical formulations. In a companion paper, contact freezing experiments are compared with immersion freezing experiments conducted with AgI, kaolinite, and ATD as ice nuclei. The following picture emerges from this analysis: The ice nucleation ability of AgI seems to be enhanced when the AgI particle is on the surface of a droplet, which is indeed the position that a particle takes when it can freely move in a droplet. Ice nucleation by particles with surfaces exposed to air, depends on water adsorption. AgI surfaces seem to be most efficient as ice nuclei when they are exposed to relative humidity at or even above water saturation. For AgI particles that are totally immersed in water, the freezing temperature increases with increasing AgI surface area. Higher threshold freezing temperature seem to correlate with improved lattice matches as can be seen for AgI-AgCl solid solutions and 3AgI•NH4I•6H2O, which have slightly better lattice matches with ice than AgI and also higher threshold freezing temperatures. However, the effect of a good lattice match is annihilated when the surfaces have charges. Also, the ice nucleation ability seems to decrease during dissolution of AgI particles. This introduces an additional history and time dependence of ice nucleation in cloud chambers with short residence times.

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

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

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

scholarly journals Development of the drop Freezing Ice Nuclei Counter (FINC), intercomparison of droplet freezing techniques, and use of soluble lignin as an atmospheric ice nucleation standard

2020 ◽  
Author(s):  
Anna J. Miller ◽  
Killian P. Brennan ◽  
Claudia Mignani ◽  
Jörg Wieder ◽  
Assaf Zipori ◽  
...  
Keyword(s):  
Limit Of Detection ◽  
Supercooled Liquid ◽  
Freezing Temperature ◽  
Ice Nucleation ◽  
Water Soluble ◽  
Aerosol Sample ◽  
Solution Stability ◽  
Ice Nuclei ◽  
Immersion Freezing ◽  
Aerosol Cloud Interactions

Abstract. Aerosol-cloud interactions, including the ice nucleation of supercooled liquid water droplets caused by ice nucleating particles (INPs) and macromolecules (INMs), are a source of uncertainty in predicting future climate. Because of INPs' and INMs' spatial and temporal heterogeneity in source, number, and composition, predicting their concentration and distribution is a challenge, requiring apt analytical instrumentation. Here, we present the development of our drop Freezing Ice Nucleation Counter (FINC), a droplet freezing technique (DFT), for the quantification of INP and INM concentrations in the immersion freezing mode. FINC's design builds upon previous DFTs and uses an ethanol bath to cool sample aliquots while detecting freezing using a camera. Specifically, FINC uses 288 sample wells of 5–60 µL volume, has a limit of detection of −25.37 ± 0.15 ˚C with 5 µL, and has an instrument temperature uncertainty of ± 0.5 ˚C. We further conducted freezing control experiments to quantify the non-homogeneous behavior of our developed DFT, including the consideration of eight different sources of contamination. As part of the validation of FINC, an intercomparison campaign was conducted using an NX-illite suspension and an ambient aerosol sample with two other drop-freezing instruments: ETH's DRoplet Ice Nuclei Counter Zurich (DRINCZ) and University of Basel’s LED-based ice nucleation detection apparatus (LINDA). We also tabulated an exhaustive list of peer-reviewed DFTs, to which we added our characterized and validated FINC. In addition, we propose herein the use of a water-soluble biopolymer, lignin, as a suitable ice nucleating standard. An ideal INM standard should be inexpensive, accessible, reproducible, unaffected by sample preparation, and consistent across techniques. First, we show that commercial lignin has a consistent ice nucleating activity across product batches. Second, we demonstrate that aqueous lignin solutions exhibit good solution stability over time. Third, we compare its freezing temperature across different drop-freezing instruments, including on DRINCZ, LINDA, and on the Weizmann Institute's Supercooled Droplets Observation on a Microarray (WISDOM) and determine an empirical fit parameter for future drop freezing validations. With these findings, we aim to show that lignin can be used as a good immersion freezing standard in future technique intercomparisons in the field of atmospheric ice nucleation.

scholarly journals BINARY: an optical freezing array for assessing temperature and time dependence of heterogeneous ice nucleation

2015 ◽  
Vol 8 (2) ◽  
pp. 689-703 ◽  
Author(s):  
C. Budke ◽  
T. Koop
Keyword(s):  
Time Dependence ◽  
Ice Nucleation ◽  
Small Time ◽  
Cooling Rates ◽  
Vapor Transfer ◽  
Ice Nucleators ◽  
Immersion Freezing ◽  
Type Water ◽  
Optical Brightness ◽  
Heterogeneous Ice Nucleation

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.

scholarly journals Enhanced ice nucleation efficiency of microcline immersed in dilute NH<sub>3</sub> and NH<sub>4</sub><sup>+</sup>-containing solutions

2018 ◽  
Author(s):  
Anand Kumar ◽  
Claudia Marcolli ◽  
Beiping Luo ◽  
Thomas Peter
Keyword(s):  
Volume Fraction ◽  
Pure Water ◽  
Freezing Temperature ◽  
Ice Nucleation ◽  
Ice Melting ◽  
Salt Solutions ◽  
Point Curve ◽  
Mineral Dusts ◽  
Immersion Freezing ◽  
Mixed Phase Clouds

Abstract. Potassium containing feldspars (K-feldspars) have been considered key mineral dusts for ice nucleation (IN) in mixed-phase clouds. To investigate the effect of solutes on their IN efficiency, we performed immersion freezing experiments with the K-feldspar microcline, which is highly IN active. Freezing of emulsified droplets with microcline suspended in aqueous solutions of NH3, (NH4)2SO4, NH4HSO4, NH4NO3, NH4Cl, Na2SO4, H2SO4, K2SO4 and KCl, with solute concentrations corresponding to water activities aw = 0.9–1.0, were investigated by means of a differential scanning calorimeter (DSC). The measured heterogeneous ice nucleation onset temperatures, Thet (aw) deviate strongly from Thet∆awhet (aw), the values calculated from the water-activity-based approach (where Thet∆awhet (aw) = Tmelt (aw + ∆awhet) with a constant offset ∆awhet with respect to the ice melting point curve). Surprisingly, for very dilute solutions of NH3 and NH4+-salts (molalities  ~ 0.96), we find IN temperatures raised by up to 4.5 K above the onset freezing temperature of microcline in pure water (Thet (aw = 1)) and 5.5 K above Thet∆awhet (aw), revealing NH3 and NH4+ to significantly enhance the IN of the microcline surface. Conversely, more concentrated NH3 and NH4+ solutions show a depression of the onset temperature below Thet∆awhet (aw) by as much as 13.5 K caused by a decline in IN ability accompanied with a reduction in the volume fraction of water frozen heterogeneously. All salt solutions not containing NH4+ as cation exhibit nucleation temperatures Thet (aw)  ~ 0.96) at warm (252–257 K) and NH3/NH4+-rich conditions.

scholarly journals Online Ice-Nucleating Particle Measurements in the Southern Great Plains (SGP) Using the Portable Ice Nucleation Experiment (PINE) Chamber

2020 ◽  
Vol 4 (1) ◽  
pp. 25
Author(s):  
Hemanth S. K. Vepuri ◽  
Larissa Lacher ◽  
Jens Nadolny ◽  
Ottmar Möhler ◽  
Naruki Hiranuma
Keyword(s):  
Great Plains ◽  
Cloud Condensation Nuclei ◽  
Active Surface ◽  
Freezing Temperature ◽  
Statistical Correlation ◽  
Ice Nucleation ◽  
High Time Resolution ◽  
Field Campaign ◽  
Southern Great Plains ◽  
Immersion Freezing

We present our field results of ice-nucleating particle (INP) measurements from the commercialized version of the Portable Ice Nucleation Experiment (PINE) chamber from two different campaigns. Our first field campaign, TxTEST, was conducted at West Texas A&M University (July–August 2019), and the other campaign, ExINP-SGP, was held at the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site (October–November 2019). In both campaigns, the PINE made semi-autonomous INP measurements at a high-time-resolution of 8 min for individual expansions with continuous temperature scans from −5 to −35 °C in 90 min. The PINE instrument was set to have a minimum detection capability of ~0.3 INPs per liter of air. To complement our online PINE measurements, polycarbonate filter impactor and liquid impinger samples were also collected next to the PINE. Offline droplet-freezing assays were later conducted from the filter and impinger samples for the immersion freezing mode. Our preliminary results suggested that the immersion freezing mode was the dominant ice-nucleation mechanism at the SGP site compared to the deposition mode. We did not find any statistical correlation between cloud condensation nuclei (CCN) and INP concentration during our ExINP-SGP period, suggesting that CCN activation is not a significant prerequisite for ice nucleation at the SGP site. In addition, we analyzed the relationship between various aerosol particle size ranges and INP abundance. At SGP, we found an increase in INPs with the super-micron particles, especially for diameters >2 μm across the entire heterogeneous freezing temperature range examined by PINE. Lastly, we computed a variety of INP parameters, such as, ice nucleation active surface site density, water activity-based freezing, and cumulative INP per liter of air, representing the ambient INPs in the SGP. Our field campaign results demonstrated the PINE’s ability to make remote INP measurements, promising future long-term operations including at isolated locations.

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

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

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

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