scholarly journals A comprehensive characterization of ice nucleation by three different types of cellulose particles immersed in water

2019 ◽  
Vol 19 (7) ◽  
pp. 4823-4849 ◽  
Author(s):  
Naruki Hiranuma ◽  
Kouji Adachi ◽  
David M. Bell ◽  
Franco Belosi ◽  
Hassan Beydoun ◽  
...  
Keyword(s):  
Aqueous Suspension ◽  
Measurement Techniques ◽  
Active Surface ◽  
Ice Nucleation ◽  
Accuracy And Precision ◽  
Active Surface Site ◽  
Two Samples ◽  
Order Of Magnitude ◽  
Immersion Freezing ◽  
T Values

Abstract. We present the laboratory results of immersion freezing efficiencies of cellulose particles at supercooled temperature (T) conditions. Three types of chemically homogeneous cellulose samples are used as surrogates that represent supermicron and submicron ice-nucleating plant structural polymers. These samples include microcrystalline cellulose (MCC), fibrous cellulose (FC) and nanocrystalline cellulose (NCC). Our immersion freezing dataset includes data from various ice nucleation measurement techniques available at 17 different institutions, including nine dry dispersion and 11 aqueous suspension techniques. With a total of 20 methods, we performed systematic accuracy and precision analysis of measurements from all 20 measurement techniques by evaluating T-binned (1 ∘C) data over a wide T range (−36 ∘C <T<-4 ∘C). Specifically, we intercompared the geometric surface area-based ice nucleation active surface site (INAS) density data derived from our measurements as a function of T, ns,geo(T). Additionally, we also compared the ns,geo(T) values and the freezing spectral slope parameter (Δlog(ns,geo)/ΔT) from our measurements to previous literature results. Results show all three cellulose materials are reasonably ice active. The freezing efficiencies of NCC samples agree reasonably well, whereas the diversity for the other two samples spans ≈ 10 ∘C. Despite given uncertainties within each instrument technique, the overall trend of the ns,geo(T) spectrum traced by the T-binned average of measurements suggests that predominantly supermicron-sized cellulose particles (MCC and FC) generally act as more efficient ice-nucleating particles (INPs) than NCC with about 1 order of magnitude higher ns,geo(T).

scholarly journals A comprehensive characterization of ice nucleation by three different types of cellulose particles immersed in water: lessons learned and future research directions

2018 ◽  
Author(s):  
Naruki Hiranuma ◽  
Kouji Adachi ◽  
David Bell ◽  
Franco Belosi ◽  
Hassan Beydoun ◽  
...  
Keyword(s):  
Aqueous Suspension ◽  
Measurement Techniques ◽  
Ice Nucleation ◽  
Lessons Learned ◽  
Future Research ◽  
Crystalline Cellulose ◽  
Nano Crystalline ◽  
Accuracy And Precision ◽  
Immersion Freezing ◽  
Future Research Directions

Abstract. We present the laboratory results of immersion freezing efficiencies of cellulose particles at supercooled temperature (T) conditions. Three types of chemically homogeneous cellulose samples are used as surrogates that represent supermicron and submicron ice nucleating plant structural polymers. These samples include micro-crystalline cellulose (MCC), fibrous cellulose (FC) and nano-crystalline cellulose (NCC). Our experimental data show that particles resembling the MCC lab particle occur also in the atmosphere. Our immersion freezing dataset includes data from various ice nucleation measurement techniques available at seventeen different institutions, including nine dry dispersion and eleven aqueous suspension techniques. With a total of twenty methods, we performed systematic accuracy and precision analysis of measurements from all twenty measurement techniques by evaluating T-binned (1 °C) data over a wide T range (−36 °C 

scholarly journals The WeIzmann Supercooled Droplets Observation on a Microarray (WISDOM) and application for ambient dust

2018 ◽  
Vol 11 (1) ◽  
pp. 233-248 ◽  
Author(s):  
Naama Reicher ◽  
Lior Segev ◽  
Yinon Rudich
Keyword(s):  
Active Surface ◽  
Ice Nucleation ◽  
Saharan Dust ◽  
Dust Particles ◽  
Active Surface Site ◽  
Immersion Freezing ◽  
Measurement Uncertainties ◽  
Homogeneous Freezing ◽  
Validation Experiments

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.

scholarly journals Ice nucleation properties of fine ash particles from the Eyjafjallajökull eruption in April 2010

2011 ◽  
Vol 11 (6) ◽  
pp. 17665-17698 ◽  
Author(s):  
I. Steinke ◽  
O. Möhler ◽  
A. Kiselev ◽  
M. Niemand ◽  
H. Saathoff ◽  
...  
Keyword(s):  
Volcanic Ash ◽  
Active Surface ◽  
Ice Nucleation ◽  
Saharan Dust ◽  
Surface Site ◽  
Ice Nuclei ◽  
Active Surface Site ◽  
Mineral Dusts ◽  
Immersion Freezing ◽  
Ice Fraction

Abstract. During the eruption of the Eyjafjallajökull volcano in the south of Iceland in April/May 2010, about 40 Tg of ash mass were emitted into the atmosphere. However, it was unclear whether volcanic ash particles with d < 10 μm facilitate the glaciation of clouds. Thus, ice nucleation properties of volcanic ash particles were investigated in AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber experiments simulating atmospherically relevant conditions. The ash sample that was used for our experiments had been collected at a distance of 58 km from the Eyjafjallajökull during the eruption period in April 2010. The temperature range covered by our ice nucleation experiments extended from 219 to 264 K, and both ice nucleation via immersion freezing and deposition nucleation could be observed. Immersion freezing was first observed at 252 K, whereas the deposition nucleation onset lay at 242 K and RHice = 126 %. About 0.1 % of the volcanic ash particles were active as immersion freezing nuclei at a temperature of 249 K. For deposition nucleation, an ice fraction of 0.1 % was observed at around 233 K and RHice = 116 %. Taking ice-active surface site densities as a measure for the ice nucleation efficiency, volcanic ash particles are similarly efficient ice nuclei in immersion freezing mode (ns, imm ~ 109 m−2 at 247 K) compared to certain mineral dusts. For deposition nucleation, the observed ice-active surface site densities ns, dep were found to be 1011 m−2 at 224 K and RHice = 116 %. Thus, volcanic ash particles initiate deposition nucleation more efficiently than Asian and Saharan dust but appear to be poorer ice nuclei than ATD particles. Based on the experimental data, we have derived ice-active surface site densities as a function of temperature for immersion freezing and of relative humidity over ice and temperature for deposition nucleation.

scholarly journals The WeIzmann Supercooled Droplets Observation (WISDOM) on a Microarray and application for ambient dust

2017 ◽  
Author(s):  
Naama Reicher ◽  
Lior Segev ◽  
Yinon Rudich
Keyword(s):  
Active Surface ◽  
Mineral Oil ◽  
Ice Nucleation ◽  
Saharan Dust ◽  
Dust Particles ◽  
Active Surface Site ◽  
Immersion Freezing ◽  
Measurement Uncertainties ◽  
Validation Experiments

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 homogenous freezing of water (235 K) in various cooling rates (typically 0.1-10 K min−1). It can also be used for studying homogenous freezing of aqueous solutions in colder temperatures. Frozen fraction, ice nucleation active surface site (INAS) densities and freezing kinetics can be obtained from WISDOM measurements with excellent statistics of hundreds of individual droplets in a single freezing experiment. Droplets are surrounded by a mineral oil phase which assures the isolation of the droplets and prevents mutual seeding, mass transfer or evaporation, and hence increases the reliability and reproducibility of the measurement. 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 INP properties of size-selected ambient Saharan dust particles is presented.

scholarly journals Ice nucleation properties of fine ash particles from the Eyjafjallajökull eruption in April 2010

2011 ◽  
Vol 11 (24) ◽  
pp. 12945-12958 ◽  
Author(s):  
I. Steinke ◽  
O. Möhler ◽  
A. Kiselev ◽  
M. Niemand ◽  
H. Saathoff ◽  
...  
Keyword(s):  
Volcanic Ash ◽  
Active Surface ◽  
Ice Nucleation ◽  
Saharan Dust ◽  
Surface Site ◽  
Ice Nuclei ◽  
Active Surface Site ◽  
Mineral Dusts ◽  
Immersion Freezing ◽  
Ice Fraction

Abstract. During the eruption of the Eyjafjallajökull volcano in the south of Iceland in April/May 2010, about 40 Tg of ash mass were emitted into the atmosphere. It was unclear whether volcanic ash particles with d < 10 μm facilitate the glaciation of clouds. Thus, ice nucleation properties of volcanic ash particles were investigated in AIDA (Aerosol Interaction and Dynamics in the Atmosphere) cloud chamber experiments simulating atmospherically relevant conditions. The ash sample that was used for our experiments had been collected at a distance of 58 km from the Eyjafjallajökull during the eruption period in April 2010. The temperature range covered by our ice nucleation experiments extended from 219 to 264 K, and both ice nucleation via immersion freezing and deposition nucleation could be observed. Immersion freezing was first observed at 252 K, whereas the deposition nucleation onset lay at 242 K and RHice =126%. About 0.1% of the volcanic ash particles were active as immersion freezing nuclei at a temperature of 249 K. For deposition nucleation, an ice fraction of 0.1% was observed at around 233 K and RHice =116%. Taking ice-active surface site densities as a measure for the ice nucleation efficiency, volcanic ash particles are similarly efficient ice nuclei in immersion freezing mode (ns,imm ~ 109 m−2 at 247 K) compared to certain mineral dusts. For deposition nucleation, the observed ice-active surface site densities ns,dep were found to be 1011 m−2 at 224 K and RHice =116%. Thus, volcanic ash particles initiate deposition nucleation more efficiently than Asian and Saharan dust but appear to be poorer ice nuclei than ATD particles. Based on the experimental data, we have derived ice-active surface site densities as a function of temperature for immersion freezing and of relative humidity over ice and temperature for deposition nucleation.

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 A New Ice Nucleation Active Site Parameterization for Desert Dust and Soot

2017 ◽  
Vol 74 (3) ◽  
pp. 699-717 ◽  
Author(s):  
Romy Ullrich ◽  
Corinna Hoose ◽  
Ottmar Möhler ◽  
Monika Niemand ◽  
Robert Wagner ◽  
...  
Keyword(s):  
Active Surface ◽  
Ice Nucleation ◽  
Nucleation Theory ◽  
Classical Nucleation Theory ◽  
Negative Slope ◽  
Organic Carbon Content ◽  
Desert Dust ◽  
Soot Aerosol ◽  
Immersion Freezing ◽  
Heterogeneous Ice Nucleation

Abstract Based on results of 11 yr of heterogeneous ice nucleation experiments at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) chamber in Karlsruhe, Germany, a new empirical parameterization framework for heterogeneous ice nucleation was developed. The framework currently includes desert dust and soot aerosol and quantifies the ice nucleation efficiency in terms of the ice nucleation active surface site (INAS) approach. The immersion freezing INAS densities nS of all desert dust experiments follow an exponential fit as a function of temperature, well in agreement with an earlier analysis of AIDA experiments. The deposition nucleation nS isolines for desert dust follow u-shaped curves in the ice saturation ratio–temperature (Si–T) diagram at temperatures below about 240 K. The negative slope of these isolines toward lower temperatures may be explained by classical nucleation theory (CNT), whereas the behavior toward higher temperatures may be caused by a pore condensation and freezing mechanism. The deposition nucleation measured for soot at temperatures below about 240 K also follows u-shaped isolines with a shift toward higher Si for soot with higher organic carbon content. For immersion freezing of soot aerosol, only upper limits for nS were determined and used to rescale an existing parameterization line. The new parameterization framework is compared to a CNT-based parameterization and an empirical framework as used in models. The comparison shows large differences in shape and magnitude of the nS isolines especially for deposition nucleation. For the application in models, implementation of this new framework is simple compared to that of other expressions.

scholarly journals A comprehensive laboratory study on the immersion freezing behavior of illite NX particles: a comparison of 17 ice nucleation measurement techniques

2015 ◽  
Vol 15 (5) ◽  
pp. 2489-2518 ◽  
Author(s):  
N. Hiranuma ◽  
S. Augustin-Bauditz ◽  
H. Bingemer ◽  
C. Budke ◽  
J. Curtius ◽  
...  
Keyword(s):  
Cooling Rate ◽  
Surface Area ◽  
Mineral Dust ◽  
Measurement Techniques ◽  
Ice Nucleation ◽  
Measurement Methods ◽  
Dust Particles ◽  
Immersion Freezing ◽  
Nucleation Activity ◽  
Ice Nucleation Activity

Abstract. Immersion freezing is the most relevant heterogeneous ice nucleation mechanism through which ice crystals are formed in mixed-phase clouds. In recent years, an increasing number of laboratory experiments utilizing a variety of instruments have examined immersion freezing activity of atmospherically relevant ice-nucleating particles. However, an intercomparison of these laboratory results is a difficult task because investigators have used different ice nucleation (IN) measurement methods to produce these results. A remaining challenge is to explore the sensitivity and accuracy of these techniques and to understand how the IN results are potentially influenced or biased by experimental parameters associated with these techniques. Within the framework of INUIT (Ice Nuclei Research Unit), we distributed an illite-rich sample (illite NX) as a representative surrogate for atmospheric mineral dust particles to investigators to perform immersion freezing experiments using different IN measurement methods and to obtain IN data as a function of particle concentration, temperature (T), cooling rate and nucleation time. A total of 17 measurement methods were involved in the data intercomparison. Experiments with seven instruments started with the test sample pre-suspended in water before cooling, while 10 other instruments employed water vapor condensation onto dry-dispersed particles followed by immersion freezing. The resulting comprehensive immersion freezing data set was evaluated using the ice nucleation active surface-site density, ns, to develop a representative ns(T) spectrum that spans a wide temperature range (−37 °C < T < −11 °C) and covers 9 orders of magnitude in ns. In general, the 17 immersion freezing measurement techniques deviate, within a range of about 8 °C in terms of temperature, by 3 orders of magnitude with respect to ns. In addition, we show evidence that the immersion freezing efficiency expressed in ns of illite NX particles is relatively independent of droplet size, particle mass in suspension, particle size and cooling rate during freezing. A strong temperature dependence and weak time and size dependence of the immersion freezing efficiency of illite-rich clay mineral particles enabled the ns parameterization solely as a function of temperature. We also characterized the ns(T) spectra and identified a section with a steep slope between −20 and −27 °C, where a large fraction of active sites of our test dust may trigger immersion freezing. This slope was followed by a region with a gentler slope at temperatures below −27 °C. While the agreement between different instruments was reasonable below ~ −27 °C, there seemed to be a different trend in the temperature-dependent ice nucleation activity from the suspension and dry-dispersed particle measurements for this mineral dust, in particular at higher temperatures. For instance, the ice nucleation activity expressed in ns was smaller for the average of the wet suspended samples and higher for the average of the dry-dispersed aerosol samples between about −27 and −18 °C. Only instruments making measurements with wet suspended samples were able to measure ice nucleation above −18 °C. A possible explanation for the deviation between −27 and −18 °C is discussed. Multiple exponential distribution fits in both linear and log space for both specific surface area-based ns(T) and geometric surface area-based ns(T) are provided. These new fits, constrained by using identical reference samples, will help to compare IN measurement methods that are not included in the present study and IN data from future IN instruments.

scholarly journals Kaolinite particles as ice nuclei: learning from the use of different kaolinite samples and different coatings

2014 ◽  
Vol 14 (11) ◽  
pp. 5529-5546 ◽  
Author(s):  
H. Wex ◽  
P. J. DeMott ◽  
Y. Tobo ◽  
S. Hartmann ◽  
M. Rösch ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Succinic Acid ◽  
Freezing Point ◽  
Active Surface ◽  
Diffusion Chamber ◽  
Ice Nucleation ◽  
Rate Coefficients ◽  
Ice Nuclei ◽  
Ability To Act ◽  
Immersion Freezing

Abstract. Kaolinite particles from two different sources (Fluka and Clay Minerals Society (CMS)) were examined with respect to their ability to act as ice nuclei (IN). This was done in the water-subsaturated regime where often deposition ice nucleation is assumed to occur, and for water-supersaturated conditions, i.e., in the immersion freezing mode. Measurements were done using a flow tube (the Leipzig Aerosol Cloud Interaction Simulator, LACIS) and a continuous-flow diffusion chamber (CFDC). Pure and coated particles were used, with coating thicknesses of a few nanometers or less, where the coating consisted of levoglucosan, succinic acid or sulfuric acid. In general, it was found that the coatings strongly reduced deposition ice nucleation. Remaining ice formation in the water-subsaturated regime could be attributed to immersion freezing, with particles immersed in concentrated solutions formed by the coatings. In the immersion freezing mode, ice nucleation rate coefficients jhet from both instruments agreed well with each other, particularly when the residence times in the instruments were accounted for. Fluka kaolinite particles coated with either levoglucosan or succinic acid showed the same IN activity as pure Fluka kaolinite particles; i.e., it can be assumed that these two types of coating did not alter the ice-active surface chemically, and that the coatings were diluted enough in the droplets that were formed prior to the ice nucleation, so that freezing point depression was negligible. However, Fluka kaolinite particles, which were either coated with pure sulfuric acid or were first coated with the acid and then exposed to additional water vapor, both showed a reduced ability to nucleate ice compared to the pure particles. For the CMS kaolinite particles, the ability to nucleate ice in the immersion freezing mode was similar for all examined particles, i.e., for the pure ones and the ones with the different types of coating. Moreover, jhet derived for the CMS kaolinite particles was comparable to jhet derived for Fluka kaolinite particles coated with sulfuric acid. This is suggestive for the Fluka kaolinite possessing a type of ice-nucleating surface feature which is not present on the CMS kaolinite, and which can be destroyed by reaction with sulfuric acid. This might be potassium feldspar.

scholarly journals Seasonal variability of Saharan desert dust and ice nucleating particles over Europe

2015 ◽  
Vol 15 (8) ◽  
pp. 4389-4397 ◽  
Author(s):  
L. B. Hande ◽  
C. Engler ◽  
C. Hoose ◽  
I. Tegen
Keyword(s):  
Seasonal Variability ◽  
Mesoscale Model ◽  
Ice Nucleation ◽  
Saharan Dust ◽  
Dust Particles ◽  
Limited Area ◽  
Order Of Magnitude ◽  
Immersion Freezing ◽  
Best Fit ◽  
Normal Background

Abstract. Dust aerosols are thought to be the main contributor to atmospheric ice nucleation. While there are case studies supporting this, a climatological sense of the importance of dust to atmospheric ice nucleating particle (INP) concentrations and its seasonal variability over Europe is lacking. Here, we use a mesoscale model to estimate Saharan dust concentrations over Europe in 2008. There are large differences in median dust concentrations between seasons, with the highest concentrations and highest variability in the lower to mid-troposphere. Laboratory-based ice nucleation parameterisations are applied to these simulated dust number concentrations to calculate the potential INP resulting from immersion freezing and deposition nucleation on these dust particles. The potential INP concentrations increase exponentially with height due to decreasing temperatures in the lower and mid-troposphere. When the ice-activated fraction increases sufficiently, INP concentrations follow the dust particle concentrations. The potential INP profiles exhibit similarly large differences between seasons, with the highest concentrations in spring (median potential immersion INP concentrations nearly 105 m−3, median potential deposition INP concentrations at 120% relative humidity with respect to ice over 105 m−3), about an order of magnitude larger than those in summer. Using these results, a best-fit function is provided to estimate the potential INPs for use in limited-area models, which is representative of the normal background INP concentrations over Europe. A statistical evaluation of the results against field and laboratory measurements indicates that the INP concentrations are in close agreement with observations.

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