Sample records for homogeneous ice nucleation
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Knopf, Daniel A; Rigg, Yannick J
2011-02-10
Homogeneous ice nucleation plays an important role in the formation of cirrus clouds with subsequent effects on the global radiative budget. Here we report on homogeneous ice nucleation temperatures and corresponding nucleation rate coefficients of aqueous droplets serving as surrogates of biomass burning aerosol. Micrometer-sized (NH(4))(2)SO(4)/levoglucosan droplets with mass ratios of 10:1, 1:1, 1:5, and 1:10 and aqueous multicomponent organic droplets with and without (NH(4))(2)SO(4) under typical tropospheric temperatures and relative humidities are investigated experimentally using a droplet conditioning and ice nucleation apparatus coupled to an optical microscope with image analysis. Homogeneous freezing was determined as a function of temperature and water activity, a(w), which was set at droplet preparation conditions. The ice nucleation data indicate that minor addition of (NH(4))(2)SO(4) to the aqueous organic droplets renders the temperature dependency of water activity negligible in contrast to the case of aqueous organic solution droplets. The mean homogeneous ice nucleation rate coefficient derived from 8 different aqueous droplet compositions with average diameters of ∼60 μm for temperatures as low as 195 K and a(w) of 0.82-1 is 2.18 × 10(6) cm(-3) s(-1). The experimentally derived freezing temperatures and homogeneous ice nucleation rate coefficients are in agreement with predictions of the water activity-based homogeneous ice nucleation theory when taking predictive uncertainties into account. However, the presented ice nucleation data indicate that the water activity-based homogeneous ice nucleation theory overpredicts the freezing temperatures by up to 3 K and corresponding ice nucleation rate coefficients by up to ∼2 orders of magnitude. A shift of 0.01 in a(w), which is well within the uncertainty of typical field and laboratory relative humidity measurements, brings experimental and predicted freezing temperatures and homogeneous ice
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Ice nucleation triggered by negative pressure.
Marcolli, Claudia
2017-11-30
Homogeneous ice nucleation needs supercooling of more than 35 K to become effective. When pressure is applied to water, the melting and the freezing points both decrease. Conversely, melting and freezing temperatures increase under negative pressure, i.e. when water is stretched. This study presents an extrapolation of homogeneous ice nucleation temperatures from positive to negative pressures as a basis for further exploration of ice nucleation under negative pressure. It predicts that increasing negative pressure at temperatures below about 262 K eventually results in homogeneous ice nucleation while at warmer temperature homogeneous cavitation, i. e. bubble nucleation, dominates. Negative pressure occurs locally and briefly when water is stretched due to mechanical shock, sonic waves, or fragmentation. The occurrence of such transient negative pressure should suffice to trigger homogeneous ice nucleation at large supercooling in the absence of ice-nucleating surfaces. In addition, negative pressure can act together with ice-inducing surfaces to enhance their intrinsic ice nucleation efficiency. Dynamic ice nucleation can be used to improve properties and uniformity of frozen products by applying ultrasonic fields and might also be relevant for the freezing of large drops in rainclouds.
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A simulation study of homogeneous ice nucleation in supercooled salty water
Soria, Guiomar D.; Espinosa, Jorge R.; Ramirez, Jorge; Valeriani, Chantal; Vega, Carlos; Sanz, Eduardo
2018-06-01
We use computer simulations to investigate the effect of salt on homogeneous ice nucleation. The melting point of the employed solution model was obtained both by direct coexistence simulations and by thermodynamic integration from previous calculations of the water chemical potential. Using a seeding approach, in which we simulate ice seeds embedded in a supercooled aqueous solution, we compute the nucleation rate as a function of temperature for a 1.85 NaCl mol per water kilogram solution at 1 bar. To improve the accuracy and reliability of our calculations, we combine seeding with the direct computation of the ice-solution interfacial free energy at coexistence using the Mold Integration method. We compare the results with previous simulation work on pure water to understand the effect caused by the solute. The model captures the experimental trend that the nucleation rate at a given supercooling decreases when adding salt. Despite the fact that the thermodynamic driving force for ice nucleation is higher for salty water for a given supercooling, the nucleation rate slows down with salt due to a significant increase of the ice-fluid interfacial free energy. The salty water model predicts an ice nucleation rate that is in good agreement with experimental measurements, bringing confidence in the predictive ability of the model. We expect that the combination of state-of-the-art simulation methods here employed to study ice nucleation from solution will be of much use in forthcoming numerical investigations of crystallization in mixtures.
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Climate Impacts of Ice Nucleation
Gettelman, Andrew; Liu, Xiaohong; Barahona, Donifan; Lohmann, Ulrike; Chen, Celia
2012-01-01
Several different ice nucleation parameterizations in two different General Circulation Models (GCMs) are used to understand the effects of ice nucleation on the mean climate state, and the Aerosol Indirect Effects (AIE) of cirrus clouds on climate. Simulations have a range of ice microphysical states that are consistent with the spread of observations, but many simulations have higher present-day ice crystal number concentrations than in-situ observations. These different states result from different parameterizations of ice cloud nucleation processes, and feature different balances of homogeneous and heterogeneous nucleation. Black carbon aerosols have a small (0.06 Wm(exp-2) and not statistically significant AIE when included as ice nuclei, for nucleation efficiencies within the range of laboratory measurements. Indirect effects of anthropogenic aerosols on cirrus clouds occur as a consequence of increasing anthropogenic sulfur emissions with different mechanisms important in different models. In one model this is due to increases in homogeneous nucleation fraction, and in the other due to increases in heterogeneous nucleation with coated dust. The magnitude of the effect is the same however. The resulting ice AIE does not seem strongly dependent on the balance between homogeneous and heterogeneous ice nucleation. Regional effects can reach several Wm2. Indirect effects are slightly larger for those states with less homogeneous nucleation and lower ice number concentration in the base state. The total ice AIE is estimated at 0.27 +/- 0.10 Wm(exp-2) (1 sigma uncertainty). This represents a 20% offset of the simulated total shortwave AIE for ice and liquid clouds of 1.6 Wm(sup-2).
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On the Ice Nucleation Spectrum
Barahona, D.
2012-01-01
This work presents a novel formulation of the ice nucleation spectrum, i.e. the function relating the ice crystal concentration to cloud formation conditions and aerosol properties. The new formulation is physically-based and explicitly accounts for the dependency of the ice crystal concentration on temperature, supersaturation, cooling rate, and particle size, surface area and composition. This is achieved by introducing the concepts of ice nucleation coefficient (the number of ice germs present in a particle) and nucleation probability dispersion function (the distribution of ice nucleation coefficients within the aerosol population). The new formulation is used to generate ice nucleation parameterizations for the homogeneous freezing of cloud droplets and the heterogeneous deposition ice nucleation on dust and soot ice nuclei. For homogeneous freezing, it was found that by increasing the dispersion in the droplet volume distribution the fraction of supercooled droplets in the population increases. For heterogeneous ice nucleation the new formulation consistently describes singular and stochastic behavior within a single framework. Using a fundamentally stochastic approach, both cooling rate independence and constancy of the ice nucleation fraction over time, features typically associated with singular behavior, were reproduced. Analysis of the temporal dependency of the ice nucleation spectrum suggested that experimental methods that measure the ice nucleation fraction over few seconds would tend to underestimate the ice nuclei concentration. It is shown that inferring the aerosol heterogeneous ice nucleation properties from measurements of the onset supersaturation and temperature may carry significant error as the variability in ice nucleation properties within the aerosol population is not accounted for. This work provides a simple and rigorous ice nucleation framework where theoretical predictions, laboratory measurements and field campaign data can be
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Direct calculation of ice homogeneous nucleation rate for a molecular model of water
Haji-Akbari, Amir; Debenedetti, Pablo G.
2015-01-01
Ice formation is ubiquitous in nature, with important consequences in a variety of environments, including biological cells, soil, aircraft, transportation infrastructure, and atmospheric clouds. However, its intrinsic kinetics and microscopic mechanism are difficult to discern with current experiments. Molecular simulations of ice nucleation are also challenging, and direct rate calculations have only been performed for coarse-grained models of water. For molecular models, only indirect estimates have been obtained, e.g., by assuming the validity of classical nucleation theory. We use a path sampling approach to perform, to our knowledge, the first direct rate calculation of homogeneous nucleation of ice in a molecular model of water. We use TIP4P/Ice, the most accurate among existing molecular models for studying ice polymorphs. By using a novel topological approach to distinguish different polymorphs, we are able to identify a freezing mechanism that involves a competition between cubic and hexagonal ice in the early stages of nucleation. In this competition, the cubic polymorph takes over because the addition of new topological structural motifs consistent with cubic ice leads to the formation of more compact crystallites. This is not true for topological hexagonal motifs, which give rise to elongated crystallites that are not able to grow. This leads to transition states that are rich in cubic ice, and not the thermodynamically stable hexagonal polymorph. This mechanism provides a molecular explanation for the earlier experimental and computational observations of the preference for cubic ice in the literature. PMID:26240318
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Dynamics of ice nucleation on water repellent surfaces.
Alizadeh, Azar; Yamada, Masako; Li, Ri; Shang, Wen; Otta, Shourya; Zhong, Sheng; Ge, Liehui; Dhinojwala, Ali; Conway, Ken R; Bahadur, Vaibhav; Vinciquerra, A Joseph; Stephens, Brian; Blohm, Margaret L
2012-02-14
Prevention of ice accretion and adhesion on surfaces is relevant to many applications, leading to improved operation safety, increased energy efficiency, and cost reduction. Development of passive nonicing coatings is highly desirable, since current antiicing strategies are energy and cost intensive. Superhydrophobicity has been proposed as a lead passive nonicing strategy, yet the exact mechanism of delayed icing on these surfaces is not clearly understood. In this work, we present an in-depth analysis of ice formation dynamics upon water droplet impact on surfaces with different wettabilities. We experimentally demonstrate that ice nucleation under low-humidity conditions can be delayed through control of surface chemistry and texture. Combining infrared (IR) thermometry and high-speed photography, we observe that the reduction of water-surface contact area on superhydrophobic surfaces plays a dual role in delaying nucleation: first by reducing heat transfer and second by reducing the probability of heterogeneous nucleation at the water-substrate interface. This work also includes an analysis (based on classical nucleation theory) to estimate various homogeneous and heterogeneous nucleation rates in icing situations. The key finding is that ice nucleation delay on superhydrophobic surfaces is more prominent at moderate degrees of supercooling, while closer to the homogeneous nucleation temperature, bulk and air-water interface nucleation effects become equally important. The study presented here offers a comprehensive perspective on the efficacy of textured surfaces for nonicing applications.
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Anomalous Behavior of the Homogeneous Ice Nucleation Rate in “No-Man’s Land”
2015-01-01
We present an analysis of ice nucleation kinetics from near-ambient pressure water as temperature decreases below the homogeneous limit TH by cooling micrometer-sized droplets (microdroplets) evaporatively at 103–104 K/s and probing the structure ultrafast using femtosecond pulses from the Linac Coherent Light Source (LCLS) free-electron X-ray laser. Below 232 K, we observed a slower nucleation rate increase with decreasing temperature than anticipated from previous measurements, which we suggest is due to the rapid decrease in water’s diffusivity. This is consistent with earlier findings that microdroplets do not crystallize at nucleation rate is connected with the proposed “fragile-to-strong” transition anomaly in water. PMID:26207172
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Rate of Homogenous Nucleation of Ice in Supercooled Water.
Atkinson, James D; Murray, Benjamin J; O'Sullivan, Daniel
2016-08-25
The homogeneous freezing of water is of fundamental importance to a number of fields, including that of cloud formation. However, there is considerable scatter in homogeneous nucleation rate coefficients reported in the literature. Using a cold stage droplet system designed to minimize uncertainties in temperature measurements, we examined the freezing of over 1500 pure water droplets with diameters between 4 and 24 μm. Under the assumption that nucleation occurs within the bulk of the droplet, nucleation rate coefficients fall within the spread of literature data and are in good agreement with a subset of more recent measurements. To quantify the relative importance of surface and volume nucleation in our experiments, where droplets are supported by a hydrophobic surface and surrounded by oil, comparison of droplets with different surface area to volume ratios was performed. From our experiments it is shown that in droplets larger than 6 μm diameter (between 234.6 and 236.5 K), nucleation in the interior is more important than nucleation at the surface. At smaller sizes we cannot rule out a significant contribution of surface nucleation, and in order to further constrain surface nucleation, experiments with smaller droplets are necessary. Nevertheless, in our experiments, it is dominantly volume nucleation controlling the observed nucleation rate.
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The effects of ice on methane hydrate nucleation: a microcanonical molecular dynamics study.
Zhang, Zhengcai; Guo, Guang-Jun
2017-07-26
Although ice powders are widely used in gas hydrate formation experiments, the effects of ice on hydrate nucleation and what happens in the quasi-liquid layer of ice are still not well understood. Here, we used high-precision constant energy molecular dynamics simulations to study methane hydrate nucleation from vapor-liquid mixtures exposed to the basal, prismatic, and secondary prismatic planes of hexagonal ice (ice Ih). Although no significant difference is observed in hydrate nucleation processes for these different crystal planes, it is found, more interestingly, that methane hydrate can nucleate either on the ice surface heterogeneously or in the bulk solution phase homogeneously. Several factors are mentioned to be able to promote the heterogeneous nucleation of hydrates, including the adsorption of methane molecules at the solid-liquid interface, hydrogen bonding between hydrate cages and the ice structure, the stronger ability of ice to transfer heat than that of the aqueous solution, and the higher occurrence probability of hydrate cages in the vicinity of the ice surface than in the bulk solution. Meanwhile, however, the other factors including the hydrophilicity of ice and the ice lattice mismatch with clathrate hydrates can inhibit heterogeneous nucleation on the ice surface and virtually promote homogeneous nucleation in the bulk solution. Certainly, the efficiency of ice as a promoter and as an inhibitor for heterogeneous nucleation is different. We estimate that the former is larger than the latter under the working conditions. Additionally, utilizing the benefit of ice to absorb heat, the NVE simulation of hydrate formation with ice can mimic the phenomenon of ice shrinking during the heterogeneous nucleation of hydrates and lower the overly large temperature increase during homogeneous nucleation. These results are helpful in understanding the nucleation mechanism of methane hydrate in the presence of ice.
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Directory of Open Access Journals (Sweden)
R. Wagner
2012-09-01
Full Text Available The ice nucleation potential of airborne glassy aqueous aerosol particles has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 247 and 216 K. Four different solutes were used as proxies for oxygenated organic matter found in the atmosphere: raffinose, 4-hydroxy-3-methoxy-DL-mandelic acid (HMMA, levoglucosan, and a multi-component mixture of raffinose with five dicarboxylic acids and ammonium sulphate. Similar to previous experiments with citric acid aerosols, all particles were found to nucleate ice heterogeneously before reaching the homogeneous freezing threshold provided that the freezing cycles were started well below the respective glass transition temperatures of the compounds; this is discussed in detail in a separate article. In this contribution, we identify a further mechanism by which glassy aerosols can promote ice nucleation below the homogeneous freezing limit. If the glassy aerosol particles are probed in freezing cycles started only a few degrees below their respective glass transition temperatures, they enter the liquid regime of the state diagram upon increasing relative humidity (moisture-induced glass-to-liquid transition before being able to act as heterogeneous ice nuclei. Ice formation then only occurs by homogeneous freezing at elevated supersaturation levels. When ice forms the remaining solution freeze concentrates and re-vitrifies. If these ice cloud processed glassy aerosol particles are then probed in a second freezing cycle at the same temperature, they catalyse ice formation at a supersaturation threshold between 5 and 30% with respect to ice. By analogy with the enhanced ice nucleation ability of insoluble ice nuclei like mineral dusts after they nucleate ice once, we refer to this phenomenon as pre-activation. We propose a number of possible explanations for why glassy aerosol particles that have re
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Homogeneous crystal nucleation in polymers.
Schick, C; Androsch, R; Schmelzer, J W P
2017-11-15
The pathway of crystal nucleation significantly influences the structure and properties of semi-crystalline polymers. Crystal nucleation is normally heterogeneous at low supercooling, and homogeneous at high supercooling, of the polymer melt. Homogeneous nucleation in bulk polymers has been, so far, hardly accessible experimentally, and was even doubted to occur at all. This topical review summarizes experimental findings on homogeneous crystal nucleation in polymers. Recently developed fast scanning calorimetry, with cooling and heating rates up to 10 6 K s -1 , allows for detailed investigations of nucleation near and even below the glass transition temperature, including analysis of nuclei stability. As for other materials, the maximum homogeneous nucleation rate for polymers is located close to the glass transition temperature. In the experiments discussed here, it is shown that polymer nucleation is homogeneous at such temperatures. Homogeneous nucleation in polymers is discussed in the framework of the classical nucleation theory. The majority of our observations are consistent with the theory. The discrepancies may guide further research, particularly experiments to progress theoretical development. Progress in the understanding of homogeneous nucleation is much needed, since most of the modelling approaches dealing with polymer crystallization exclusively consider homogeneous nucleation. This is also the basis for advancing theoretical approaches to the much more complex phenomena governing heterogeneous nucleation.
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Pirim, Claire; Ikhenazene, Raouf; Ortega, Isamel Kenneth; Carpentier, Yvain; Focsa, Cristian; Chazallon, Bertrand; Ouf, François-Xavier
2016-04-01
Emissions of solid-state particles (soot) from engine exhausts due to incomplete fuel combustion is considered to influence ice and liquid water cloud droplet activation [1]. The activity of these aerosols would originate from their ability to be important centers of ice-particle nucleation, as they would promote ice formation above water homogeneous freezing point. Soot particles are reported to be generally worse ice nuclei than mineral dust because they activate nucleation at higher ice-supersaturations for deposition nucleation and at lower temperatures for immersion freezing than ratios usually expected for homogeneous nucleation [2]. In fact, there are still numerous opened questions as to whether and how soot's physico-chemical properties (structure, morphology and chemical composition) can influence their nucleation ability. Therefore, systematic investigations of soot aerosol nucleation activity via one specific nucleation mode, here deposition nucleation, combined with thorough structural and compositional analyzes are needed in order to establish any association between the particles' activity and their physico-chemical properties. In addition, since the morphology of the ice crystals can influence their radiative properties [3], we investigated their morphology as they grow over both soot and pristine substrates at different temperatures and humidity ratios. In the present work, Combustion Aerosol STandart soot samples were produced from propane using various experimental conditions. Their nucleation activity was studied in deposition mode (from water vapor), and monitored using a temperature-controlled reactor in which the sample's relative humidity is precisely measured with a cryo-hygrometer. Formation of water/ice onto the particles is followed both optically and spectroscopically, using a microscope coupled to a Raman spectrometer. Vibrational signatures of hydroxyls (O-H) emerge when the particle becomes hydrated and are used to characterize ice
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Thermodynamic Derivation of the Activation Energy for Ice Nucleation
Barahona, D.
2015-01-01
Cirrus clouds play a key role in the radiative and hydrological balance of the upper troposphere. Their correct representation in atmospheric models requires an understanding of the microscopic processes leading to ice nucleation. A key parameter in the theoretical description of ice nucleation is the activation energy, which controls the flux of water molecules from the bulk of the liquid to the solid during the early stages of ice formation. In most studies it is estimated by direct association with the bulk properties of water, typically viscosity and self-diffusivity. As the environment in the ice-liquid interface may differ from that of the bulk, this approach may introduce bias in calculated nucleation rates. In this work a theoretical model is proposed to describe the transfer of water molecules across the ice-liquid interface. Within this framework the activation energy naturally emerges from the combination of the energy required to break hydrogen bonds in the liquid, i.e., the bulk diffusion process, and the work dissipated from the molecular rearrangement of water molecules within the ice-liquid interface. The new expression is introduced into a generalized form of classical nucleation theory. Even though no nucleation rate measurements are used to fit any of the parameters of the theory the predicted nucleation rate is in good agreement with experimental results, even at temperature as low as 190 K, where it tends to be underestimated by most models. It is shown that the activation energy has a strong dependency on temperature and a weak dependency on water activity. Such dependencies are masked by thermodynamic effects at temperatures typical of homogeneous freezing of cloud droplets; however, they may affect the formation of ice in haze aerosol particles. The new model provides an independent estimation of the activation energy and the homogeneous ice nucleation rate, and it may help to improve the interpretation of experimental results and the
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Ice nucleation and cloud microphysical properties in tropical tropopause layer cirrus
Directory of Open Access Journals (Sweden)
E. J. Jensen
2010-02-01
Full Text Available In past modeling studies, it has generally been assumed that the predominant mechanism for nucleation of ice in the uppermost troposphere is homogeneous freezing of aqueous aerosols. However, recent in situ and remote-sensing measurements of the properties of cirrus clouds at very low temperatures in the tropical tropopause layer (TTL are broadly inconsistent with theoretial predictions based on the homogeneous freezing assumption. The nearly ubiquitous occurence of gravity waves in the TTL makes the predictions from homogeneous nucleation theory particularly difficult to reconcile with measurements. These measured properties include ice number concentrations, which are much lower than theory predicts; ice crystal size distributions, which are much broader than theory predicts; and cloud extinctions, which are much lower than theory predicts. Although other explanations are possible, one way to limit ice concentrations is to have on the order of 50 L−1 effective ice nuclei (IN that could nucleate ice at relatively low supersaturations. We suggest that ammonium sulfate particles, which would be dry much of the time in the cold TTL, are a potential IN candidate for TTL cirrus. However, this mechanism remains to be fully quantified for the size distribution of ammonium sulfate (possibly internally mixed with organics actually present in the upper troposphere. Possible implications of the observed cloud microphysical properties for ice sedimentation, dehydration, and cloud persistence are also discussed.
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Heterogeneous Ice Nucleation Ability of NaCl and Sea Salt Aerosol Particles at Cirrus Temperatures
Wagner, Robert; Kaufmann, Julia; Möhler, Ottmar; Saathoff, Harald; Schnaiter, Martin; Ullrich, Romy; Leisner, Thomas
2018-03-01
In situ measurements of the composition of heterogeneous cirrus ice cloud residuals have indicated a substantial contribution of sea salt in sampling regions above the ocean. We have investigated the heterogeneous ice nucleation ability of sodium chloride (NaCl) and sea salt aerosol (SSA) particles at cirrus cloud temperatures between 235 and 200 K in the Aerosol Interaction and Dynamics in the Atmosphere aerosol and cloud chamber. Effloresced NaCl particles were found to act as ice nucleating particles in the deposition nucleation mode at temperatures below about 225 K, with freezing onsets in terms of the ice saturation ratio, Sice, between 1.28 and 1.40. Above 225 K, the crystalline NaCl particles deliquesced and nucleated ice homogeneously. The heterogeneous ice nucleation efficiency was rather similar for the two crystalline forms of NaCl (anhydrous NaCl and NaCl dihydrate). Mixed-phase (solid/liquid) SSA particles were found to act as ice nucleating particles in the immersion freezing mode at temperatures below about 220 K, with freezing onsets in terms of Sice between 1.24 and 1.42. Above 220 K, the SSA particles fully deliquesced and nucleated ice homogeneously. Ice nucleation active surface site densities of the SSA particles were found to be in the range between 1.0 · 1010 and 1.0 · 1011 m-2 at T < 220 K. These values are of the same order of magnitude as ice nucleation active surface site densities recently determined for desert dust, suggesting a potential contribution of SSA particles to low-temperature heterogeneous ice nucleation in the atmosphere.
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Effect of Controlled Ice Nucleation on Stability of Lactate Dehydrogenase During Freeze-Drying.
Fang, Rui; Tanaka, Kazunari; Mudhivarthi, Vamsi; Bogner, Robin H; Pikal, Michael J
2018-03-01
Several controlled ice nucleation techniques have been developed to increase the efficiency of the freeze-drying process as well as to improve the quality of pharmaceutical products. Owing to the reduction in ice surface area, these techniques have the potential to reduce the degradation of proteins labile during freezing. The objective of this study was to evaluate the effect of ice nucleation temperature on the in-process stability of lactate dehydrogenase (LDH). LDH in potassium phosphate buffer was nucleated at -4°C, -8°C, and -12°C using ControLyo™ or allowed to nucleate spontaneously. Both the enzymatic activity and tetramer recovery after freeze-thawing linearly correlated with product ice nucleation temperature (n = 24). Controlled nucleation also significantly improved batch homogeneity as reflected by reduced inter-vial variation in activity and tetramer recovery. With the correlation established in the laboratory, the degradation of protein in manufacturing arising from ice nucleation temperature differences can be quantitatively predicted. The results show that controlled nucleation reduced the degradation of LDH during the freezing process, but this does not necessarily translate to vastly superior stability during the entire freeze-drying process. The capability of improving batch homogeneity provides potential advantages in scaling-up from lab to manufacturing scale. Copyright © 2018 American Pharmacists Association®. Published by Elsevier Inc. All rights reserved.
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Directory of Open Access Journals (Sweden)
D. Barahona
2009-08-01
Full Text Available This study presents a comprehensive ice cloud formation parameterization that computes the ice crystal number, size distribution, and maximum supersaturation from precursor aerosol and ice nuclei. The parameterization provides an analytical solution of the cloud parcel model equations and accounts for the competition effects between homogeneous and heterogeneous freezing, and, between heterogeneous freezing in different modes. The diversity of heterogeneous nuclei is described through a nucleation spectrum function which is allowed to follow any form (i.e., derived from classical nucleation theory or from observations. The parameterization reproduces the predictions of a detailed numerical parcel model over a wide range of conditions, and several expressions for the nucleation spectrum. The average error in ice crystal number concentration was −2.0±8.5% for conditions of pure heterogeneous freezing, and, 4.7±21% when both homogeneous and heterogeneous freezing were active. The formulation presented is fast and free from requirements of numerical integration.
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Cloud condensation nuclei and ice nucleation activity of hydrophobic and hydrophilic soot particles.
Koehler, Kirsten A; DeMott, Paul J; Kreidenweis, Sonia M; Popovicheva, Olga B; Petters, Markus D; Carrico, Christian M; Kireeva, Elena D; Khokhlova, Tatiana D; Shonija, Natalia K
2009-09-28
Cloud condensation nuclei (CCN) activity and ice nucleation behavior (for temperaturesnucleation experiments below -40 degrees C, AEC particles nucleated ice near the expected condition for homogeneous freezing of water from aqueous solutions. In contrast, GTS, TS, and TC1 required relative humidity well in excess of water saturation at -40 degrees C for ice formation. GTS particles required water supersaturation conditions for ice activation even at -51 degrees C. At -51 to -57 degrees C, ice formation in particles with electrical mobility diameter of 200 nm occurred in up to 1 in 1000 TS and TC1 particles, and 1 in 100 TOS particles, at relative humidities below those required for homogeneous freezing in aqueous solutions. Our results suggest that heterogeneous ice nucleation is favored in cirrus conditions on oxidized hydrophilic soot of intermediate polarity. Simple considerations suggest that the impact of hydrophilic soot particles on cirrus cloud formation would be most likely in regions of elevated atmospheric soot number concentrations. The ice formation properties of AEC soot are reasonably consistent with present understanding of the conditions required for aircraft contrail formation and the proportion of soot expected to nucleate under such conditions.
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Czech Academy of Sciences Publication Activity Database
Němec, Tomáš; Eisenschmidt, K.; Rauschenberger, P.; Weigand, B.
2012-01-01
Roč. 12, č. 1 (2012), s. 533-534 ISSN 1617-7061 R&D Projects: GA ČR GAP101/10/1819 Institutional research plan: CEZ:AV0Z20760514 Keywords : ice nucleation * ice-water surface energy * classical nucleation theory Subject RIV: BJ - Thermodynamics http://onlinelibrary.wiley.com/doi/10.1002/pamm.201210255/abstract
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Dynamics of homogeneous nucleation
DEFF Research Database (Denmark)
Toxværd, Søren
2015-01-01
The classical nucleation theory for homogeneous nucleation is formulated as a theory for a density fluctuation in a supersaturated gas at a given temperature. But molecular dynamics simulations reveal that it is small cold clusters which initiates the nucleation. The temperature in the nucleating...
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Understanding ice nucleation characteristics of selective mineral dusts suspended in solution
Kumar, Anand; Marcolli, Claudia; Kaufmann, Lukas; Krieger, Ulrich; Peter, Thomas
2016-04-01
Introduction & Objectives Freezing of liquid droplets and subsequent ice crystal growth affects optical properties of clouds and precipitation. Field measurements show that ice formation in cumulus and stratiform clouds begins at temperatures much warmer than those associated with homogeneous ice nucleation in pure water, which is ascribed to heterogeneous ice nucleation occurring on the foreign surfaces of ice nuclei (IN). Various insoluble particles such as mineral dust, soot, metallic particles, volcanic ash, or primary biological particles have been suggested as IN. Among these the suitability of mineral dusts is best established. The ice nucleation ability of mineral dust particles may be modified when secondary organic or inorganic substances are accumulating on the dust during atmospheric transport. If the coating is completely wetting the mineral dust particles, heterogeneous ice nucleation occurs in immersion mode also below 100 % RH. A previous study by Kaufmann (PhD Thesis 2015, ETHZ) with Hoggar Mountain dust suspensions in various solutes (ammonium sulfate, PEG, malonic acid and glucose) showed reduced ice nucleation efficiency (in immersion mode) of the particles. Though it is still quite unclear of how surface modifications and coatings influence the ice nucleation activity of the components present in natural dust samples. In view of these results we run freezing experiments using a differential scanning calorimeter (DSC) with the following mineral dust particles suspended in pure water and ammonium sulfate solutions: Arizona Test Dust (ATD), microcline, and kaolinite (KGa-2, Clay Mineral Society). Methodology Suspensions of mineral dust samples (ATD: 2 weight%, microcline: 5% weight, KGa-2: 5% weight) are prepared in pure water with varying solute concentrations (ammonium sulfate: 0 - 10% weight). 20 vol% of this suspension plus 80 vol% of a mixture of 95 wt% mineral oil (Aldrich Chemical) and 5 wt% lanolin (Fluka Chemical) is emulsified with a
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Thermodynamic and Dynamic Aspects of Ice Nucleation
Barahona, Donifan
2018-01-01
It is known that ice nucleating particles (INP) immersed within supercooled droplets promote the formation of ice. Common theoretical models used to represent this process assume that the immersed particle lowers the work of ice nucleation without significantly affecting the dynamics of water in the vicinity of the particle. This is contrary to evidence showing that immersed surfaces significantly affect the viscosity and diffusivity of vicinal water. To study how this may affect ice formation this work introduces a model linking the ice nucleation rate to the modification of the dynamics and thermodynamics of vicinal water by immersed particles. It is shown that INP that significantly reduce the work of ice nucleation also pose strong limitations to the growth of the nascent ice germs. This leads to the onset of a new ice nucleation regime, called spinodal ice nucleation, where the dynamics of ice germ growth instead of the ice germ size determines the nucleation rate. Nucleation in this regime is characterized by an enhanced sensitivity to particle area and cooling rate. Comparison of the predicted ice nucleation rate against experimental measurements for a diverse set of species relevant to cloud formation suggests that spinodal ice nucleation may be common in nature.
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Heterogeneous ice nucleation in aqueous solutions: the role of water activity.
Zobrist, B; Marcolli, C; Peter, T; Koop, T
2008-05-01
Heterogeneous ice nucleation experiments have been performed with four different ice nuclei (IN), namely nonadecanol, silica, silver iodide and Arizona test dust. All IN are either immersed in the droplets or located at the droplets surface. The IN were exposed to various aqueous solutions, which consist of (NH4)2SO4, H2SO4, MgCl2, NaCl, LiCl, Ca(NO3)2, K2CO3, CH3COONa, ethylene glycol, glycerol, malonic acid, PEG300 or a NaCl/malonic acid mixture. Freezing was studied using a differential scanning calorimeter and a cold finger cell. The results show that the heterogeneous ice freezing temperatures decrease with increasing solute concentration; however, the magnitude of this effect is solute dependent. In contrast, when the results are analyzed in terms of the solution water activity a very consistent behavior emerges: heterogeneous ice nucleation temperatures for all four IN converge each onto a single line, irrespective of the nature of the solute. We find that a constant offset with respect to the ice melting point curve, Deltaaw,het, can describe the observed freezing temperatures for each IN. Such a behavior is well-known for homogeneous ice nucleation from supercooled liquid droplets and has led to the development of water-activity-based ice nucleation theory. The large variety of investigated solutes together with different general types of ice nuclei studied (monolayers, ionic crystals, covalently bound network-forming compounds, and a mixture of chemically different crystallites) underlines the general applicability of water-activity-based ice nucleation theory also for heterogeneous ice nucleation in the immersion mode. Finally, the ice nucleation efficiencies of the various IN, as well as the atmospheric implication of the developed parametrization are discussed.
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Hoose, C.; Hande, L. B.; Mohler, O.; Niemand, M.; Paukert, M.; Reichardt, I.; Ullrich, R.
2016-12-01
Between 0 and -37°C, ice formation in clouds is triggered by aerosol particles acting as heterogeneous ice nuclei. At lower temperatures, heterogeneous ice nucleation on aerosols can occur at lower supersaturations than homogeneous freezing of solutes. In laboratory experiments, the ability of different aerosol species (e.g. desert dusts, soot, biological particles) has been studied in detail and quantified via various theoretical or empirical parameterization approaches. For experiments in the AIDA cloud chamber, we have quantified the ice nucleation efficiency via a temperature- and supersaturation dependent ice nucleation active site density. Here we present a new empirical parameterization scheme for immersion and deposition ice nucleation on desert dust and soot based on these experimental data. The application of this parameterization to the simulation of cirrus clouds, deep convective clouds and orographic clouds will be shown, including the extension of the scheme to the treatment of freezing of rain drops. The results are compared to other heterogeneous ice nucleation schemes. Furthermore, an aerosol-dependent parameterization of contact ice nucleation is presented.
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Homogeneous versus heterogeneous zeolite nucleation
Dokter, W.H.; Garderen, van H.F.; Beelen, T.P.M.; Santen, van R.A.; Bras, W.
1995-01-01
Aggregates of fractal dimension were found in the intermediate gel phases that organize prior to nucleation and crystallization (shown right) of silicalite from a homogeneous reaction mixture. Small- and wide-angle X-ray scattering studies prove that for zeolites nucleation may be homogeneous or
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Jensen, Eric J.
2016-01-01
Recent investigations of the influence of atmospheric waves on ice nucleation in cirrus have identified a number of key processes and sensitivities: (1) ice concentrations produced by homogeneous freezing are strongly dependent on cooling rates, with gravity waves dominating upper tropospheric cooling rates; (2) rapid cooling driven by high-frequency waves are likely responsible for the rare occurrences of very high ice concentrations in cirrus; (3) sedimentation and entrainment tend to decrease ice concentrations as cirrus age; and (4) in some situations, changes in temperature tendency driven by high-frequency waves can quench ice nucleation events and limit ice concentrations. Here we use parcel-model simulations of ice nucleation driven by long-duration, constant-pressure balloon temperature time series, along with an extensive dataset of cold cirrus microphysical properties from the recent ATTREX high-altitude aircraft campaign, to statistically examine the importance of high-frequency waves as well as the consistency between our theoretical understanding of ice nucleation and observed ice concentrations. The parcel-model simulations indicate common occurrence of peak ice concentrations exceeding several hundred per liter. Sedimentation and entrainment would reduce ice concentrations as clouds age, but 1-D simulations using a wave parameterization (which underestimates rapid cooling events) still produce ice concentrations higher than indicated by observations. We find that quenching of nucleation events by high-frequency waves occurs infrequently and does not prevent occurrences of large ice concentrations in parcel simulations of homogeneous freezing. In fact, the high-frequency variability in the balloon temperature data is entirely responsible for production of these high ice concentrations in the simulations.
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Ignatius, Karoliina; Järvinen, Emma; Nichman, Leonid; Fuchs, Claudia; Gordon, Hamish; Herenz, Paul; Hoyle, Christopher R; Duplissy, Jonathan; Garimella, Sarvesh; Dias, Antonio; Frege, Carla; Höppel, Niko; Tröstl, Jasmin; Wagner, Robert; Yan, Chao; Amorim, Antonio; Baltensperger, Urs; Curtius, Joachim; Donahue, Neil M; Gallagher, Martin W; Kirkby, Jasper; Kulmala, Markku; Möhler, Ottmar; Saathoff, Harald; Schnaiter, Martin; Tomé, Antonio; Virtanen, Annele; Worsnop, Douglas; Stratmann, Frank
2016-01-01
There are strong indications that particles containing secondary organic aerosol (SOA) exhibit amorphous solid or semi-solid phase states in the atmosphere. This may facilitate heterogeneous ice nucleation and thus influence cloud properties. However, experimental ice nucleation studies of biogenic SOA are scarce. Here, we investigated the ice nucleation ability of viscous SOA particles. The SOA particles were produced from the ozone initiated oxidation of α-pinene in an aerosol chamber at temperatures in the range from −38 to −10 ◦C at 5–15 % relative humidity with respect to water to ensure their formation in a highly viscous phase state, i.e. semi-solid or glassy. The ice nucleation ability of SOA particles with different sizes was investigated with a new continuous flow diffusion chamber. For the first time, we observed heterogeneous ice nucleation of viscous α-pinene SOA for ice saturation ratios between 1.3 and 1.4 significantly below the homogeneous freezing limit. The maximum frozen fraction...
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Ice nucleation rates near ˜225 K
Amaya, Andrew J.; Wyslouzil, Barbara E.
2018-02-01
We have measured the ice nucleation rates, Jice, in supercooled nano-droplets with radii ranging from 6.6 nm to 10 nm and droplet temperatures, Td, ranging from 225 K to 204 K. The initial temperature of the 10 nm water droplets is ˜250 K, i.e., well above the homogeneous nucleation temperature for micron sized water droplets, TH ˜235 K. The nucleation rates increase systematically from ˜1021 cm-3 s-1 to ˜1022 cm-3 s-1 in this temperature range, overlap with the nucleation rates of Manka et al. [Phys. Chem. Chem. Phys. 14, 4505 (2012)], and suggest that experiments with larger droplets would extrapolate smoothly the rates of Hagen et al. [J. Atmos. Sci. 38, 1236 (1981)]. The sharp corner in the rate data as temperature drops is, however, difficult to match with available theory even if we correct classical nucleation theory and the physical properties of water for the high internal pressure of the nanodroplets.
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The barrier to ice nucleation in monatomic water
Prestipino, Santi
2018-03-01
Crystallization from a supercooled liquid initially proceeds via the formation of a small solid embryo (nucleus), which requires surmounting an activation barrier. This phenomenon is most easily studied by numerical simulation, using specialized biased-sampling techniques to overcome the limitations imposed by the rarity of nucleation events. Here, I focus on the barrier to homogeneous ice nucleation in supercooled water, as represented by the monatomic-water model, which in the bulk exhibits a complex interplay between different ice structures. I consider various protocols to identify solidlike particles on a computer, which perform well enough for the Lennard-Jones model, and compare their respective impact on the shape and height of the nucleation barrier. It turns out that the effect is stronger on the nucleus size than on the barrier height. As a by-product of the analysis, I determine the structure of the nucleation cluster, finding that the relative amount of ice phases in the cluster heavily depends on the method used for classifying solidlike particles. Moreover, the phase which is most favored during the earlier stages of crystallization may happen, depending on the nucleation coordinate adopted, to be different from the stable polymorph. Therefore, the quality of a reaction coordinate cannot be assessed simply on the basis of the barrier height obtained. I explain how this outcome is possible and why it just points out the shortcoming of collective variables appropriate to simple fluids in providing a robust method of particle classification for monatomic water.
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Role of stacking disorder in ice nucleation.
Lupi, Laura; Hudait, Arpa; Peters, Baron; Grünwald, Michael; Gotchy Mullen, Ryan; Nguyen, Andrew H; Molinero, Valeria
2017-11-08
The freezing of water affects the processes that determine Earth's climate. Therefore, accurate weather and climate forecasts hinge on good predictions of ice nucleation rates. Such rate predictions are based on extrapolations using classical nucleation theory, which assumes that the structure of nanometre-sized ice crystallites corresponds to that of hexagonal ice, the thermodynamically stable form of bulk ice. However, simulations with various water models find that ice nucleated and grown under atmospheric temperatures is at all sizes stacking-disordered, consisting of random sequences of cubic and hexagonal ice layers. This implies that stacking-disordered ice crystallites either are more stable than hexagonal ice crystallites or form because of non-equilibrium dynamical effects. Both scenarios challenge central tenets of classical nucleation theory. Here we use rare-event sampling and free energy calculations with the mW water model to show that the entropy of mixing cubic and hexagonal layers makes stacking-disordered ice the stable phase for crystallites up to a size of at least 100,000 molecules. We find that stacking-disordered critical crystallites at 230 kelvin are about 14 kilojoules per mole of crystallite more stable than hexagonal crystallites, making their ice nucleation rates more than three orders of magnitude higher than predicted by classical nucleation theory. This effect on nucleation rates is temperature dependent, being the most pronounced at the warmest conditions, and should affect the modelling of cloud formation and ice particle numbers, which are very sensitive to the temperature dependence of ice nucleation rates. We conclude that classical nucleation theory needs to be corrected to include the dependence of the crystallization driving force on the size of the ice crystallite when interpreting and extrapolating ice nucleation rates from experimental laboratory conditions to the temperatures that occur in clouds.
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Ice nucleation properties of mineral dusts
Steinke, Isabelle
2013-01-01
Ice nucleation in clouds has a significant impact on the global hydrological cycle as well as on the radiative budget of the Earth. The AIDA cloud chamber was used to investigate the ice nucleation efficiency of various atmospherically relevant mineral dusts. From experiments with Arizona Test Dust (ATD) a humidity and temperature dependent ice nucleation active surface site density parameterization was developed to describe deposition nucleation at temperatures above 220 K. Based...
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Directory of Open Access Journals (Sweden)
D. M. Lienhard
2015-12-01
secondary organic aerosol (SOA material produced by oxidation of α-pinene and in a number of organic/inorganic model mixtures (3-methylbutane-1,2,3-tricarboxylic acid (3-MBTCA, levoglucosan, levoglucosan/NH4HSO4, raffinose are presented. These indicate that water diffusion coefficients are determined by several properties of the aerosol substance and cannot be inferred from the glass transition temperature or bouncing properties. Our results suggest that water diffusion in SOA particles is faster than often assumed and imposes no significant kinetic limitation on water uptake and release at temperatures above 220 K. The fast diffusion of water suggests that heterogeneous ice nucleation on a glassy core is very unlikely in these systems. At temperatures below 220 K, model simulations of SOA particles suggest that heterogeneous ice nucleation may occur in the immersion mode on glassy cores which remain embedded in a liquid shell when experiencing fast updraft velocities. The particles absorb significant quantities of water during these updrafts which plasticize their outer layers such that these layers equilibrate readily with the gas phase humidity before the homogeneous ice nucleation threshold is reached. Glass formation is thus unlikely to restrict homogeneous ice nucleation. Only under most extreme conditions near the very high tropical tropopause may the homogeneous ice nucleation rate coefficient be reduced as a consequence of slow condensed-phase water diffusion. Since the differences between the behavior limited or non limited by diffusion are small even at the very high tropical tropopause, condensed-phase water diffusivity is unlikely to have significant consequences on the direct climatic effects of SOA particles under tropospheric conditions.
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Efficiency of the deposition mode ice nucleation on mineral dust particles
Directory of Open Access Journals (Sweden)
O. Möhler
2006-01-01
Full Text Available The deposition mode ice nucleation efficiency of various dust aerosols was investigated at cirrus cloud temperatures between 196 and 223 K using the aerosol and cloud chamber facility AIDA (Aerosol Interaction and Dynamics in the Atmosphere. Arizona test dust (ATD as a reference material and two dust samples from the Takla Makan desert in Asia (AD1 and the Sahara (SD2 were used for the experiments at simulated cloud conditions. The dust particle sizes were almost lognormally distributed with mode diameters between 0.3 and 0.5 μm and geometric standard deviations between 1.6 and 1.9. Deposition ice nucleation was most efficient on ATD particles with ice-active particle fractions of about 0.6 and 0.8 at an ice saturation ratio SiSiSi. This indicates that deposition ice nucleation on mineral particles may not be treated in the same stochastic sense as homogeneous freezing. The suggested formulation of ice activation spectra may be used to calculate the formation rate of ice crystals in models, if the number concentration of dust particles is known. More experimental work is needed to quantify the variability of the ice activation spectra as function of the temperature and dust particle properties.
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Metya, Atanu K; Singh, Jayant K; Müller-Plathe, Florian
2016-09-29
In this work, we address the nucleation behavior of a supercooled monatomic cylindrical water droplet on nanoscale textured surfaces using molecular dynamics simulations. The ice nucleation rate at 203 K on graphite based textured surfaces with nanoscale roughness is evaluated using the mean fast-passage time method. The simulation results show that the nucleation rate depends on the surface fraction as well as the wetting states. The nucleation rate enhances with increasing surface fraction for water in the Cassie-Baxter state, while contrary behavior is observed for the case of Wenzel state. Based on the spatial histogram distribution of ice formation, we observed two pathways for ice nucleation. Heterogeneous nucleation is observed at a high surface fraction. However, the probability of homogeneous ice nucleation events increases with decreasing surface fraction. We further investigate the role of the nanopillar height in ice nucleation. The nucleation rate is enhanced with increasing nanopillar height. This is attributed to the enhanced contact area with increasing nanopillar height and the shift in nucleation events towards the three-phase contact line associated with the nanotextured surface. The ice-surface work of adhesion for the Wenzel state is found to be 1-2 times higher than that in the Cassie-Baxter state. Furthermore, the work of adhesion of ice in the Wenzel state is found to be linearly dependent on the contour length of the droplet, which is in line with that reported for liquid droplets.
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Kohn, Monika; Wex, Heike; Grawe, Sarah; Hartmann, Susan; Hellner, Lisa; Herenz, Paul; Welti, André; Stratmann, Frank; Lohmann, Ulrike; Kanji, Zamin A.
2016-04-01
Mixed-phase clouds (MPCs) are found to be the most relevant cloud type leading to precipitation in mid-latitudes. The formation of ice crystals in MPCs is not completely understood. To estimate the effect of aerosol particles on the radiative properties of clouds and to describe ice nucleation in models, the specific properties of aerosol particles acting as ice nucleating particles (INPs) still need to be identified. A number of devices are able to measure INPs in the lab and in the field. However, methods can be very different and need to be tested under controlled conditions with respect to aerosol generation and properties in order to standardize measurement and data analysis approaches for subsequent ambient measurements. Here, we present an overview of the LINC campaign hosted at TROPOS in September 2015. We compare four ice nucleation devices: PINC (Portable Ice Nucleation Chamber, Chou et al., 2011) and SPIN (SPectrometer for Ice Nuclei) are operated in deposition nucleation and condensation freezing mode. LACIS (Leipzig Aerosol Cloud Interaction Simulator, Hartmann et al., 2011) and PIMCA (Portable Immersion Mode Cooling chamber) measure in the immersion freezing mode. PIMCA is used as a vertical extension to PINC and allows activation and droplet growth prior to exposure to the investigated ice nucleation temperature. Size-resolved measurements of multiple aerosol types were performed including pure mineral dust (K-feldspar, kaolinite) and biological particles (Birch pollen washing waters) as well as some of them after treatment with sulfuric or nitric acid prior to experiments. LACIS and PIMCA-PINC operated in the immersion freezing mode showed very good agreement in the measured frozen fraction (FF). For the comparison between PINC and SPIN, which were scanning relative humidity from below to above water vapor saturation, an agreement was found for the obtained INP concentration. However, some differences were observed, which may result from ice
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Energy Technology Data Exchange (ETDEWEB)
Bogdan, A. [Helsinki Univ. (Finland). Dept. of Physics
1994-12-31
The classical theory of heterogenous ice nucleation is reviewed in detail. The modelling of ice nucleation in the adsorbed water films on natural particles by analogous ice nucleation in adsorbed water films on the walls of porous media is discussed. Ice nucleation in adsorbed films of purewater and the HNO{sub 3}/H{sub 2}0 binary system on the surface of porous aerosol (SiO{sub 2}) was investigated using the method of NMR spectroscopy. The median freezing temperature and freezing temperature region were shown to be highly sensitive both to the average thickness of the adsorbed films and to the amount of adsorbed nitric acid. The character of the ice phase formation tends to approach that of bulk liquid with increasing adsorbed film thickness. Under the given conditions the thickness of the adsorbed films decreases with an increasing amount of adsorbed nitric acid molecules The molar concentration of nitric acid in the adsorbed films is very small (of the order of 10{sup -}3 10{sup -}2 (M/l)). Nitric acid molecules tend to adsorb on the surface of aerosol to a greater extent than in subsequent layers. The concentration is greatest in layers situated close to the surface and sharply decreases with the distance from the surface. The difference between the median freezing temperatures for adsorbed pure water and for the binary system was found to be about 9 K for films of equal thickness. This is about 150 times greater than the difference between the median freezing temperatures of bulk pure water and a solution with the same concentration of nitric acid. (orig.)
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Ignatius, Karoliina; Kristensen, Thomas B.; Järvinen, Emma; Nichman, Leonid; Fuchs, Claudia; Gordon, Hamish; Herenz, Paul; Hoyle, Christopher R.; Duplissy, Jonathan; Garimella, Sarvesh; Dias, Antonio; Frege, Carla; Höppel, Niko; Tröstl, Jasmin; Wagner, Robert; Yan, Chao; Amorim, Antonio; Baltensperger, Urs; Curtius, Joachim; Donahue, Neil M.; Gallagher, Martin W.; Kirkby, Jasper; Kulmala, Markku; Möhler, Ottmar; Saathoff, Harald; Schnaiter, Martin; Tomé, Antonio; Virtanen, Annele; Worsnop, Douglas; Stratmann, Frank
2016-05-01
There are strong indications that particles containing secondary organic aerosol (SOA) exhibit amorphous solid or semi-solid phase states in the atmosphere. This may facilitate heterogeneous ice nucleation and thus influence cloud properties. However, experimental ice nucleation studies of biogenic SOA are scarce. Here, we investigated the ice nucleation ability of viscous SOA particles. The SOA particles were produced from the ozone initiated oxidation of α-pinene in an aerosol chamber at temperatures in the range from -38 to -10 °C at 5-15 % relative humidity with respect to water to ensure their formation in a highly viscous phase state, i.e. semi-solid or glassy. The ice nucleation ability of SOA particles with different sizes was investigated with a new continuous flow diffusion chamber. For the first time, we observed heterogeneous ice nucleation of viscous α-pinene SOA for ice saturation ratios between 1.3 and 1.4 significantly below the homogeneous freezing limit. The maximum frozen fractions found at temperatures between -39.0 and -37.2 °C ranged from 6 to 20 % and did not depend on the particle surface area. Global modelling of monoterpene SOA particles suggests that viscous biogenic SOA particles are indeed present in regions where cirrus cloud formation takes place. Hence, they could make up an important contribution to the global ice nucleating particle budget.
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International Nuclear Information System (INIS)
Gallavardin, S. J.; Froyd, Karl D.; Lohmann, U.; Moehler, Ottmar; Murphy, Daniel M.; Cziczo, Dan
2008-01-01
Experiments conducted at the Aerosol Interactions and Dynamics in the Atmosphere (AIDA) chamber located in Karlsruhe, Germany permit investigation of particle properties that affect the nucleation of ice at temperature and water vapor conditions relevant to cloud microphysics and climate issues. Ice clouds were generated by heterogeneous nucleation of Arizona test dust (ATD), illite, and hematite and homogeneous nucleation of sulfuric acid. Ice crystals formed in the chamber were inertially separated from unactivated, or 'interstitial' aerosol particles with a pumped counterflow virtual impactor (PCVI), then evaporated. The ice residue (i.e., the aerosol which initiated ice nucleation plus any material which was scavenged from the gas- and/or particle-phase), was chemically characterized at the single particle level using a laser ionization mass spectrometer. In this manner the species that first nucleated ice could be identified out of a mixed aerosol population in the chamber. Bare mineral dust particles were more effective ice nuclei (IN) than similar particles with a coating. Metallic particles from contamination in the chamber initiated ice nucleation before other species but there were few enough that they did not compromise the experiments. Nitrate, sulfate, and organics were often detected on particles and ice residue, evidently from scavenging of trace gas-phase species in the chamber. Hematite was a more effective ice nucleus than illite. Ice residue was frequently larger than unactivated test aerosol due to the formation of aggregates due to scavenging, condensation of contaminant gases, and the predominance of larger aerosol in nucleation
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Understanding the ice nucleation characteristics of feldspars suspended in solution
Kumar, Anand; Marcolli, Claudia; Kaufmann, Lukas; Krieger, Ulrich; Peter, Thomas
2017-04-01
Freezing of liquid droplets and subsequent ice crystal growth affects optical properties of clouds and precipitation. Field measurements show that ice formation in cumulus and stratiform clouds begins at temperatures much warmer than those associated with homogeneous ice nucleation in pure water, which is ascribed to heterogeneous ice nucleation occurring on the foreign surfaces of ice nuclei (IN). Various insoluble particles such as mineral dust, soot, metallic particles, volcanic ash, or primary biological particles have been suggested as IN. Among these the suitability of mineral dusts is best established. The ice nucleation ability of mineral dust particles may be modified when secondary organic or inorganic substances are accumulating on the dust during atmospheric transport. If the coating is completely wetting the mineral dust particles, heterogeneous ice nucleation occurs in immersion mode also below 100 % RH. A previous study by Zobrist et al. (2008) Arizona test dust, silver iodide, nonadecanol and silicon dioxide suspensions in various solutes showed reduced ice nucleation efficiency (in immersion mode) of the particles. Though it is still quite unclear how surface modifications and coatings influence the ice nucleation activity of the components present in natural dust particles at a microphysical scale. To improve our understanding how solute and mineral dust particle surface interaction, we run freezing experiments using a differential scanning calorimeter (DSC) with microcline, sanidine, plagioclase, kaolinite and quartz particles suspended in pure water and solutions containing ammonia, ammonium bisulfate, ammonium sulfate, ammonium chloride, ammonium nitrate, potassium chloride, potassium sulfate, sodium sulfate and sulfuric acid. Methodology Suspensions of mineral dust samples (2 - 5 wt%) are prepared in water with varying solute concentrations (0 - 15 wt%). 20 vol% of this suspension plus 80 vol% of a mixture of 95 wt% mineral oil (Aldrich
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Janus effect of antifreeze proteins on ice nucleation.
Liu, Kai; Wang, Chunlei; Ma, Ji; Shi, Guosheng; Yao, Xi; Fang, Haiping; Song, Yanlin; Wang, Jianjun
2016-12-20
The mechanism of ice nucleation at the molecular level remains largely unknown. Nature endows antifreeze proteins (AFPs) with the unique capability of controlling ice formation. However, the effect of AFPs on ice nucleation has been under debate. Here we report the observation of both depression and promotion effects of AFPs on ice nucleation via selectively binding the ice-binding face (IBF) and the non-ice-binding face (NIBF) of AFPs to solid substrates. Freezing temperature and delay time assays show that ice nucleation is depressed with the NIBF exposed to liquid water, whereas ice nucleation is facilitated with the IBF exposed to liquid water. The generality of this Janus effect is verified by investigating three representative AFPs. Molecular dynamics simulation analysis shows that the Janus effect can be established by the distinct structures of the hydration layer around IBF and NIBF. Our work greatly enhances the understanding of the mechanism of AFPs at the molecular level and brings insights to the fundamentals of heterogeneous ice nucleation.
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Sensitivity of ice-nucleating bacteria to ultraviolet irradiation
Energy Technology Data Exchange (ETDEWEB)
Obata, Hitoshi; Tanahashi, Shinji; Kawahara, Hidehisa (Kansai Univ., Suita, Osaka (Japan). Faculty of Engineering)
1992-01-01
The effect of ultraviolet (UV) irradiation on the ice-nucleating activity of the ice-nucleating bacteria was examined. Bacterial suspension was irradiated with UV (254 nm, 6Wx2) for 5 min at a distance of 20 cm from UV source. Although no viable cells were detected, the ice-nucreating activity of the cells was not affected. Furthermore, after UV irradiation for 3 hr, the ice-nucleating activity of Pseudomonas fluorescens and P. syringae was only slightly decreased, although that of P. viridiflava and Erwinia herbicola was significantly lowered. We succeeded in killing the ice-nucleating bacteria, while retaining their ice-nucleating activity with UV irradiation. (author).
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Directory of Open Access Journals (Sweden)
C. M. Archuleta
2005-01-01
Full Text Available This study examines the potential role of some types of mineral dust and mineral dust with sulfuric acid coatings as heterogeneous ice nuclei at cirrus temperatures. Commercially-available nanoscale powder samples of aluminum oxide, alumina-silicate and iron oxide were used as surrogates for atmospheric mineral dust particles, with and without multilayer coverage of sulfuric acid. A sample of Asian dust aerosol particles was also studied. Measurements of ice nucleation were made using a continuous-flow ice-thermal diffusion chamber (CFDC operated to expose size-selected aerosol particles to temperatures between -45 and -60°C and a range of relative humidity above ice-saturated conditions. Pure metal oxide particles supported heterogeneous ice nucleation at lower relative humidities than those required to homogeneously freeze sulfuric acid solution particles at sizes larger than about 50 nm. The ice nucleation behavior of the same metal oxides coated with sulfuric acid indicate heterogeneous freezing at lower relative humidities than those calculated for homogeneous freezing of the diluted particle coatings. The effect of soluble coatings on the ice activation relative humidity varied with the respective uncoated core particle types, but for all types the heterogeneous freezing rates increased with particle size for the same thermodynamic conditions. For a selected size of 200 nm, the natural mineral dust particles were the most effective ice nuclei tested, supporting heterogeneous ice formation at an ice relative humidity of approximately 135%, irrespective of temperature. Modified homogeneous freezing parameterizations and theoretical formulations are shown to have application to the description of heterogeneous freezing of mineral dust-like particles with soluble coatings.
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Immersion freezing of ice nucleation active protein complexes
Directory of Open Access Journals (Sweden)
S. Hartmann
2013-06-01
Full Text Available Utilising the Leipzig Aerosol Cloud Interaction Simulator (LACIS, the immersion freezing behaviour of droplet ensembles containing monodisperse particles, generated from a Snomax™ solution/suspension, was investigated. Thereto ice fractions were measured in the temperature range between −5 °C to −38 °C. Snomax™ is an industrial product applied for artificial snow production and contains Pseudomonas syringae} bacteria which have long been used as model organism for atmospheric relevant ice nucleation active (INA bacteria. The ice nucleation activity of such bacteria is controlled by INA protein complexes in their outer membrane. In our experiments, ice fractions increased steeply in the temperature range from about −6 °C to about −10 °C and then levelled off at ice fractions smaller than one. The plateau implies that not all examined droplets contained an INA protein complex. Assuming the INA protein complexes to be Poisson distributed over the investigated droplet populations, we developed the CHESS model (stoCHastic modEl of similar and poiSSon distributed ice nuclei which allows for the calculation of ice fractions as function of temperature and time for a given nucleation rate. Matching calculated and measured ice fractions, we determined and parameterised the nucleation rate of INA protein complexes exhibiting class III ice nucleation behaviour. Utilising the CHESS model, together with the determined nucleation rate, we compared predictions from the model to experimental data from the literature and found good agreement. We found that (a the heterogeneous ice nucleation rate expression quantifying the ice nucleation behaviour of the INA protein complex is capable of describing the ice nucleation behaviour observed in various experiments for both, Snomax™ and P. syringae bacteria, (b the ice nucleation rate, and its temperature dependence, seem to be very similar regardless of whether the INA protein complexes inducing ice
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Pre-activation of ice-nucleating particles by the pore condensation and freezing mechanism
Directory of Open Access Journals (Sweden)
R. Wagner
2016-02-01
Full Text Available In spite of the resurgence in ice nucleation research a comparatively small number of studies deal with the phenomenon of pre-activation in heterogeneous ice nucleation. Fifty years ago, it was shown that various mineral dust and volcanic ash particles can be pre-activated to become nuclei for ice crystal formation even at temperatures as high as 270–271 K. Pre-activation was achieved under ice-subsaturated conditions without any preceding macroscopic ice growth by just temporarily cooling the particles to temperatures below 228 K. A two-step mechanism involving capillary condensation of supercooled water and subsequent homogeneous freezing was proposed to account for the particles' enhanced ice nucleation ability at high temperatures. This work reinvestigates the efficiency of the proposed pre-activation mechanism in temperature-cycling experiments performed in a large cloud chamber with suspended particles. We find the efficiency to be highest for the clay mineral illite as well as for highly porous materials like zeolite and diatomaceous earth, whereas most aerosols generated from desert dust surface samples did not reveal a measurable pre-activation ability. The pre-activation efficiency is linked to particle pores in a certain size range. As estimated by model calculations, only pores with diameters between about 5 and 8 nm contribute to pre-activation under ice-subsaturated conditions. This range is set by a combination of requirements from the negative Kelvin effect for condensation and a critical size of ice embryos for ice nucleation and melting. In contrast to the early study, pre-activation is only observed for temperatures below 260 K. Above that threshold, the particles' improved ice nucleation ability disappears due to the melting of ice in the pores.
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Tuning Ice Nucleation with Supercharged Polypeptides
Yang, Huige; Ma, Chao; Li, Kaiyong; Liu, Kai; Loznik, Mark; Teeuwen, Rosalie; van Hest, Jan C. M.; Zhou, Xin; Herrmann, Andreas; Wang, Jianjun
2016-01-01
Supercharged unfolded polypeptides (SUPs) are exploited for controlling ice nucleation via tuning the nature of charge and charge density of SUPs. The results show that positively charged SUPs facilitate ice nucleation, while negatively charged ones suppress it. Moreover, the charge density of the
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Jensen, Eric; Kaercher, Bernd; Ueyama, Rei; Pfister, Leonhard
2017-01-01
Recent laboratory experiments have advanced our understanding of the physical properties and ice nucleating abilities of aerosol particles atlow temperatures. In particular, aerosols containing organics will transition to a glassy state at low temperatures, and these glassy aerosols are moderately effective as ice nuclei. These results have implications for ice nucleation in the cold Tropical Tropopause Layer (TTL; 13-19 km). We have developed a detailed cloud microphysical model that includes heterogeneous nucleation on a variety of aerosol types and homogeneous freezing of aqueous aerosols. This model has been incorporated into one-dimensional simulations of cirrus and water vapor driven by meteorological analysis temperature and wind fields. The model includes scavenging of ice nuclei by sedimenting ice crystals. The model is evaluated by comparing the simulated cloud properties and water vapor concentrations with aircraft and satellite measurements. In this presentation, I will discuss the relative importance of homogeneous and heterogeneous ice nucleation, the impact of ice nuclei scavenging as air slowly ascends through the TTL, and the implications for the final dehydration of air parcels crossing the tropical cold-point tropopause and entering the tropical stratosphere.
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Kulkarni, Gourihar; China, Swarup; Liu, Shang; Nandasiri, Manjula; Sharma, Noopur; Wilson, Jacqueline; Aiken, Allison C.; Chand, Duli; Laskin, Alexander; Mazzoleni, Claudio; Pekour, Mikhail; Shilling, John; Shutthanandan, Vaithiyalingam; Zelenyuk, Alla; Zaveri, Rahul A.
2016-04-01
Ice formation by diesel soot particles was investigated at temperatures ranging from -40 to -50°C. Size-selected soot particles were physically and chemically aged in an environmental chamber, and their ice nucleating properties were determined using a continuous flow diffusion type ice nucleation chamber. Bare (freshly formed), hydrated, and compacted soot particles, as well as α-pinene secondary organic aerosol (SOA)-coated soot particles at high relative humidity conditions, showed ice formation activity at subsaturation conditions with respect to water but below the homogeneous freezing threshold conditions. However, SOA-coated soot particles at dry conditions were observed to freeze at homogeneous freezing threshold conditions. Overall, our results suggest that heterogeneous ice nucleation activity of freshly emitted diesel soot particles are sensitive to some of the aging processes that soot can undergo in the atmosphere.
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Viscosity of interfacial water regulates ice nucleation
International Nuclear Information System (INIS)
Li, Kaiyong; Chen, Jing; Zhang, Qiaolan; Zhang, Yifan; Xu, Shun; Zhou, Xin; Cui, Dapeng; Wang, Jianjun; Song, Yanlin
2014-01-01
Ice formation on solid surfaces is an important phenomenon in many fields, such as cloud formation and atmospheric icing, and a key factor for applications in preventing freezing. Here, we report temperature-dependent nucleation rates of ice for hydrophilic and hydrophobic surfaces. The results show that hydrophilic surface presents a lower ice nucleation rate. We develop a strategy to extract the thermodynamic parameters, J 0 and Γ, in the context of classical nucleation theory. From the extracted J 0 and Γ, we reveal the dominant role played by interfacial water. The results provide an insight into freezing mechanism on solid surfaces
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Morris, C. E.; Sands, D. C.; Glaux, C.; Samsatly, J.; Asaad, S.; Moukahel, A. R.; Gonçalves, F. L. T.; Bigg, E. K.
2013-04-01
Various features of the biology of the rust fungi and of the epidemiology of the plant diseases they cause illustrate the important role of rainfall in their life history. Based on this insight we have characterized the ice nucleation activity (INA) of the aerially disseminated spores (urediospores) of this group of fungi. Urediospores of this obligate plant parasite were collected from natural infections of 7 species of weeds in France, from coffee in Brazil and from field and greenhouse-grown wheat in France, the USA, Turkey and Syria. Immersion freezing was used to determine freezing onset temperatures and the abundance of ice nuclei in suspensions of washed spores. Microbiological analyses of spores from France, the USA and Brazil, and subsequent tests of the ice nucleation activity of the bacteria associated with spores were deployed to quantify the contribution of bacteria to the ice nucleation activity of the spores. All samples of spores were ice nucleation active, having freezing onset temperatures as high as -4 °C. Spores in most of the samples carried cells of ice nucleation-active strains of the bacterium Pseudomonas syringae (at rates of less than 1 bacterial cell per 100 urediospores), but bacterial INA accounted for only a small fraction of the INA observed in spore suspensions. Changes in the INA of spore suspensions after treatment with lysozyme suggest that the INA of urediospores involves a polysaccharide. Based on data from the literature, we have estimated the concentrations of urediospores in air at cloud height and in rainfall. These quantities are very similar to those reported for other biological ice nucleators in these same substrates. However, at cloud level convective activity leads to widely varying concentrations of particles of surface origin, so that mean concentrations can underestimate their possible effects on clouds. We propose that spatial and temporal concentrations of biological ice nucleators active at temperatures > -10
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Morris, C. E.; Sands, D. C.; Glaux, C.; Samsatly, J.; Asaad, S.; Moukahel, A. R.; Gonçalves, F. L. T.; Bigg, E. K.
2012-10-01
In light of various features of the biology of the rust fungi and of the epidemiology of the plant diseases they cause that illustrate the important role of rainfall in their life history, we have characterized the ice nucleation activity (INA) of the aerially disseminated spores (urediospores) of this group of fungi. Urediospores of this obligate plant parasite were collected from natural infections from 7 species of weeds in France, from coffee in Brazil and from field and greenhouse-grown wheat in France, the USA, Turkey and Syria. Immersion freezing was used to determine freezing onset temperatures and the abundance of ice nuclei in suspensions of washed spores. Microbiological analyses of spores and subsequent tests of the ice nucleation activity of the bacteria associated with spores were deployed to quantify the contribution of bacteria to the ice nucleation activity of the spores. All samples of spores were ice nucleation active having freezing onset temperatures as warm as -4 °C. Spores in most of the samples carried cells of ice nucleation-active strains of the bacterium Pseudomonas syringae (at rates of less than 1 bacterial cell per 100 urediospores), but bacterial INA accounted for only a small fraction of the INA observed in spore suspensions. Changes in the INA of spore suspensions after treatment with lysozyme suggest that the INA of urediospores involves a polysaccharide. Based on data from the literature, we have estimated the concentrations of urediospores in air at cloud height and in rainfall. These quantities are very similar to those reported for other biological ice nucleators in these same substrates. We suggest that air sampling techniques have ignored the spatial and temporal variability of atmospheric concentrations that occur under conditions propitious for precipitation that could increase their local abundance intermittently. Nevertheless, we propose that the relative low abundance of warm-temperature biological ice nucleators in the
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Impact of surface nanostructure on ice nucleation.
Zhang, Xiang-Xiong; Chen, Min; Fu, Ming
2014-09-28
Nucleation of water on solid surface can be promoted noticeably when the lattice parameter of a surface matches well with the ice structure. However, the characteristic length of the surface lattice reported is generally less than 0.5 nm and is hardly tunable. In this paper, we show that a surface with nanoscale roughness can also remarkably promote ice nucleation if the characteristic length of the surface structure matches well with the ice crystal. A series of surfaces composed of periodic grooves with same depth but different widths are constructed in molecular dynamics simulations. Water cylinders are placed on the constructed surfaces and frozen at constant undercooling. The nucleation rates of the water cylinders are calculated in the simulation using the mean first-passage time method and then used to measure the nucleation promotion ability of the surfaces. Results suggest that the nucleation behavior of the supercooled water is significantly sensitive to the width of the groove. When the width of the groove matches well with the specific lengths of the ice crystal structure, the nucleation can be promoted remarkably. If the width does not match with the ice crystal, this kind of promotion disappears and the nucleation rate is even smaller than that on the smooth surface. Simulations also indicate that even when water molecules are adsorbed onto the surface structure in high-humidity environment, the solid surface can provide promising anti-icing ability as long as the characteristic length of the surface structure is carefully designed to avoid geometric match.
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A marine biogenic source of atmospheric ice-nucleating particles
Energy Technology Data Exchange (ETDEWEB)
Wilson, T. W.; Ladino, L. A.; Alpert, Peter A.; Breckels, M. N.; Brooks, I. M.; Browse, J.; Burrows, Susannah M.; Carslaw, K. S.; Huffman, J. A.; Judd, C.; Kilthau, W. P.; Mason, R. H.; McFiggans, Gordon; Miller, L. A.; Najera, J.; Polishchuk, E. A.; Rae, S.; Schiller, C. L.; Si, M.; Vergara Temprado, J.; Whale, Thomas; Wong, J P S; Wurl, O.; Yakobi-Hancock, J. D.; Abbatt, JPD; Aller, Josephine Y.; Bertram, Allan K.; Knopf, Daniel A.; Murray, Benjamin J.
2015-09-09
The formation of ice in clouds is facilitated by the presence of airborne ice nucleating particles1,2. Sea spray is one of the major global sources of atmospheric particles, but it is unclear to what extent these particles are capable of nucleating ice3–11. Here we show that material in the sea surface microlayer, which is enriched in surface active organic material representative of that found in sub-micron sea- spray aerosol12–21, nucleates ice under conditions that occur in mixed-phase clouds and high-altitude ice clouds. The ice active material is likely biogenic and is less than ~0.2 ?m in size. We also show that organic material (exudate) released by a common marine diatom nucleates ice when separated from cells and propose that organic material associated with phytoplankton cell exudates are a candidate for the observed ice nucleating ability of the microlayer samples. By combining our measurements with global model simulations of marine organic aerosol, we show that ice nucleating particles of marine origin are dominant in remote marine environments, such as the Southern Ocean, the North Pacific and the North Atlantic.
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Ice nucleation activity of polysaccharides
Bichler, Magdalena; Felgitsch, Laura; Haeusler, Thomas; Seidl-Seiboth, Verena; Grothe, Hinrich
2015-04-01
Heterogeneous ice nucleation is an important process in the atmosphere. It shows direct impact on our climate by triggering ice cloud formation and therefore it has much influence on the radiation balance of our planet (Lohmann et al. 2002; Mishchenko et al. 1996). The process itself is not completely understood so far and many questions remain open. Different substances have been found to exhibit ice nucleation activity (INA). Due to their vast differences in chemistry and morphology it is difficult to predict what substance will make good ice nuclei and which will not. Hence simple model substances must be found and be tested regarding INA. Our work aims at gaining to a deeper understanding of heterogeneous ice nucleation. We intend to find some reference standards with defined chemistry, which may explain the mechanisms of heterogeneous ice nucleation. A particular focus lies on biological carbohydrates in regards to their INA. Biological carbohydrates are widely distributed in all kingdoms of life. Mostly they are specific for certain organisms and have well defined purposes, e.g. structural polysaccharides like chitin (in fungi and insects) and pectin (in plants), which has also water-binding properties. Since they are widely distributed throughout our biosphere and mostly safe to use for nutrition purposes, they are well studied and easily accessible, rendering them ideal candidates as proxies. In our experiments we examined various carbohydrates, like the already mentioned chitin and pectin, as well as their chemical modifications. Lohmann U.; A Glaciation Indirect Aerosol Effect Caused by Soot Aerosols; J. Geoph. Res.; Vol. 24 No.4; pp 11-1 - 11-4; 2002 Mishchenko M.I., Rossow W.B., Macke A., Lacis A. A.; Sensitivity of Cirrus Cloud Albedo, Bidirectional Reflectance and Optical Thickness Retrieval Accuracy to Ice Particle Shape, J. Geoph. Res.; Vol. 101, No D12; pp. 16,973 - 16,985; 1996
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Probing Individual Ice Nucleation Events with Environmental Scanning Electron Microscopy
Wang, Bingbing; China, Swarup; Knopf, Daniel; Gilles, Mary; Laskin, Alexander
2016-04-01
Heterogeneous ice nucleation is one of the processes of critical relevance to a range of topics in the fundamental and the applied science and technologies. Heterogeneous ice nucleation initiated by particles proceeds where microscopic properties of particle surfaces essentially control nucleation mechanisms. Ice nucleation in the atmosphere on particles governs the formation of ice and mixed phase clouds, which in turn influence the Earth's radiative budget and climate. Heterogeneous ice nucleation is still insufficiently understood and poses significant challenges in predictive understanding of climate change. We present a novel microscopy platform allowing observation of individual ice nucleation events at temperature range of 193-273 K and relative humidity relevant for ice formation in the atmospheric clouds. The approach utilizes a home built novel ice nucleation cell interfaced with Environmental Scanning Electron Microscope (IN-ESEM system). The IN-ESEM system is applied for direct observation of individual ice formation events, determining ice nucleation mechanisms, freezing temperatures, and relative humidity onsets. Reported microanalysis of the ice nucleating particles (INP) include elemental composition detected by the energy dispersed analysis of X-rays (EDX), and advanced speciation of the organic content in particles using scanning transmission x-ray microscopy with near edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). The performance of the IN-ESEM system is validated through a set of experiments with kaolinite particles with known ice nucleation propensity. We demonstrate an application of the IN-ESEM system to identify and characterize individual INP within a complex mixture of ambient particles.
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Kanji, Z. A.; Mahrt, F.; David, R.; Marcolli, C.; Lohmann, U.; Fahrni, J.; Brühwiler, D.
2017-12-01
Heterogeneous ice nucleation (HIN) onto soot particles from previous studies have produced inconsistent results of temperature and relative humidity conditions required for freezing depending on the source of soot particle investigated. The ability of soot to act as HIN depended on the type of soot and size of particle. Often homogenous freezing conditions or water saturation conditions were required to freeze soot particles, rendering HIN irrelevant. Using synthesised mesoporous silica particles, we show pore condensation and freezing works with experiments performed in the Zurich Ice Nucleation Chamber (ZINC). By testing a variety of soot particles in parallel in the Horizontal Ice Nucleation Chamber (HINC), we suggest that previously observed HIN on soot particles is not the responsible mechanism for ice formation. Laboratory generated CAST brown and black soot, commercially available soot and acid treated soot were investigated for their ice nucleation abilities in the mixed-phase and cirrus cloud temperature regimes. No heterogeneous ice nucleation activity is inferred at T > -38 °C (mixed-phase cloud regime), however depending on particle size and soot type, HIN was observed for T nucleation of ice in the pores or cavities that are ubiquitous in soot particles between the primary spherules. The ability of some particles to freeze at lower relative humidity compared to others demonstrates why hydrophobicity plays a role in ice nucleation, i.e. controlling the conditions at which these cavities fill with water. Thus for more hydrophobic particles pore filling occurs at higher relative humidity, and therefore freezing of pore water and ice crystal growth. Future work focusses on testing the cloud processing ability of soot particles and water adsorption isotherms of the different soot samples to support the hydrophobicity inferences from the ice nucleation results.
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Homogeneous nucleation of water in synthetic air
Fransen, M.A.L.J.; Sachteleben, E.; Hruby, J.; Smeulders, D.M.J.; DeMott, P.J.; O'Dowd, C.D.
2013-01-01
Homogeneous nucleation rates for water vapor in synthetic air are measured by means of a Pulse-Expansion Wave Tube (PEWT). A comparison of the experimental nucleation rates with the Classical Nucleation Theory (CNT) shows that a more elaborated model is necessary to describe supercooled water
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Nucleation in Synoptically Forced Cirrostratus
Lin, R.-F.; Starr, D. OC.; Reichardt, J.; DeMott, P. J.
2004-01-01
Formation and evolution of cirrostratus in response to weak, uniform and constant synoptic forcing is simulated using a one-dimensional numerical model with explicit microphysics, in which the particle size distribution in each grid box is fully resolved. A series of tests of the model response to nucleation modes (homogeneous-freezing-only/heterogeneous nucleation) and heterogeneous nucleation parameters are performed. In the case studied here, nucleation is first activated in the prescribed moist layer. A continuous cloud-top nucleation zone with a depth depending on the vertical humidity gradient and one of the nucleation parameters is developed afterward. For the heterogeneous nucleation cases, intermittent nucleation zones in the mid-upper portion of the cloud form where the relative humidity is on the rise, because existent ice crystals do not uptake excess water vapor efficiently, and ice nuclei (IN) are available. Vertical resolution as fine as 1 m is required for realistic simulation of the homogeneous-freezing-only scenario, while the model resolution requirement is more relaxed in the cases where heterogeneous nucleation dominates. Bulk microphysical and optical properties are evaluated and compared. Ice particle number flux divergence, which is due to the vertical gradient of the gravity-induced particle sedimentation, is constantly and rapidly changing the local ice number concentration, even in the nucleation zone. When the depth of the nucleation zone is shallow, particle number concentration decreases rapidly as ice particles grow and sediment away from the nucleation zone. When the depth of the nucleation zone is large, a region of high ice number concentration can be sustained. The depth of nucleation zone is an important parameter to be considered in parametric treatments of ice cloud generation.
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Ice nucleation in sulfuric acid/organic aerosols: implications for cirrus cloud formation
Directory of Open Access Journals (Sweden)
M. R. Beaver
2006-01-01
Full Text Available Using an aerosol flow tube apparatus, we have studied the effects of aliphatic aldehydes (C3 to C10 and ketones (C3 and C9 on ice nucleation in sulfuric acid aerosols. Mixed aerosols were prepared by combining an organic vapor flow with a flow of sulfuric acid aerosols over a small mixing time (~60 s at room temperature. No acid-catalyzed reactions were observed under these conditions, and physical uptake was responsible for the organic content of the sulfuric acid aerosols. In these experiments, aerosol organic content, determined by a Mie scattering analysis, was found to vary with the partial pressure of organic, the flow tube temperature, and the identity of the organic compound. The physical properties of the organic compounds (primarily the solubility and melting point were found to play a dominant role in determining the inferred mode of nucleation (homogenous or heterogeneous and the specific freezing temperatures observed. Overall, very soluble, low-melting organics, such as acetone and propanal, caused a decrease in aerosol ice nucleation temperatures when compared with aqueous sulfuric acid aerosol. In contrast, sulfuric acid particles exposed to organic compounds of eight carbons and greater, of much lower solubility and higher melting temperatures, nucleate ice at temperatures above aqueous sulfuric acid aerosols. Organic compounds of intermediate carbon chain length, C4-C7, (of intermediate solubility and melting temperatures nucleated ice at the same temperature as aqueous sulfuric acid aerosols. Interpretations and implications of these results for cirrus cloud formation are discussed.
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Failor, K C; Schmale, D G; Vinatzer, B A; Monteil, C L
2017-12-01
A growing body of circumstantial evidence suggests that ice nucleation active (Ice + ) bacteria contribute to the initiation of precipitation by heterologous freezing of super-cooled water in clouds. However, little is known about the concentration of Ice + bacteria in precipitation, their genetic and phenotypic diversity, and their relationship to air mass trajectories and precipitation chemistry. In this study, 23 precipitation events were collected over 15 months in Virginia, USA. Air mass trajectories and water chemistry were determined and 33 134 isolates were screened for ice nucleation activity (INA) at -8 °C. Of 1144 isolates that tested positive during initial screening, 593 had confirmed INA at -8 °C in repeated tests. Concentrations of Ice + strains in precipitation were found to range from 0 to 13 219 colony forming units per liter, with a mean of 384±147. Most Ice + bacteria were identified as members of known and unknown Ice + species in the Pseudomonadaceae, Enterobacteriaceae and Xanthomonadaceae families, which nucleate ice employing the well-characterized membrane-bound INA protein. Two Ice + strains, however, were identified as Lysinibacillus, a Gram-positive genus not previously known to include Ice + bacteria. INA of the Lysinibacillus strains is due to a nanometer-sized molecule that is heat resistant, lysozyme and proteinase resistant, and secreted. Ice + bacteria and the INA mechanisms they employ are thus more diverse than expected. We discuss to what extent the concentration of culturable Ice + bacteria in precipitation and the identification of a new heat-resistant biological INA mechanism support a role for Ice + bacteria in the initiation of precipitation.
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Homogeneous nucleation in 4He: A corresponding-states analysis
International Nuclear Information System (INIS)
Sinha, D.N.; Semura, J.S.; Brodie, L.C.
1982-01-01
We report homogeneous-nucleation-temperature measurements in liquid 4 He over a bath-temperature range 2.31 4 He, in a region far from the critical point. A simple empirical form is presented for estimating the homogeneous nucleation temperatures for any liquid with a spherically symmetric interatomic potential. The 4 He data are compared with nucleation data for Ar, Kr, Xe, and H; theoretical predictions for 3 He are given in terms of reduced quantities. It is shown that the nucleation data for both quantum and classical liquids obey a quantum law of corresponding states (QCS). On the basis of this QCS analysis, predictions of homogeneous nucleation temperatures are made for hydrogen isotopes such as HD, DT, HT, and T 2
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International Workshop on Comparing Ice Nucleation Measuring Systems 2014
Energy Technology Data Exchange (ETDEWEB)
Cziczo, Daniel [Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
2016-04-30
The relationship of ambient aerosol particles to the formation of ice-containing clouds is one of the largest uncertainties in understanding the Earth’s climate. The uncertainty is due to several poorly understood processes and measurements including, but not limited to: (1) the microphysics of how particles nucleate ice, (2) the number of ice forming particles as a function of atmospheric properties such as temperature and relative humidity, (3) the atmospheric distribution of ice forming particles and (4) the role of anthropogenic activities in producing or changing the behavior of ice forming particles. The ways in which ice forming particles can impact climate is also multi-faceted. More ice forming particles can lead to clouds with more ice crystals and different optical properties than clouds with less ice forming particles. More effective ice forming particles can lead to ice at higher temperature and/or lower saturation, resulting in clouds at lower altitude or latitude which also changes the Earth’s radiative balance. Ice nucleation also initiates most of the Earth’s precipitation, even in the mid- and low-latitudes, since cloud-top temperatures are often below freezing. The limited measurements and lack of understanding directly translates to restrictions in our ability to model atmospheric ice formation and project changes into the future. The importance of ice nucleation research is further exemplified by Figure 1 which shows the publications per decade and citations per year on the topic of ice nucleation [DeMott et al., 2011]. After a lull at the end of the last century, there has been a dramatic increase in both publications and citations related to ice nucleation; this directly corresponds to the importance of ice nucleation on the Earth’s climate and the uncertainty in this area noted by the Solomon [2007].
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Spray structure as generated under homogeneous flash boiling nucleation regime
International Nuclear Information System (INIS)
Levy, M.; Levy, Y.; Sher, E.
2014-01-01
We show the effect of the initial pressure and temperature on the spatial distribution of droplets size and their velocity profile inside a spray cloud that is generated by a flash boiling mechanism under homogeneous nucleation regime. We used TSI's Phase Doppler Particle Analyzer (PDPA) to characterize the spray. We conclude that the homogeneous nucleation process is strongly affected by the initial liquid temperature while the initial pressure has only a minor effect. The spray shape is not affected by temperature or pressure under homogeneous nucleation regime. We noted that the only visible effect is in the spray opacity. Finally, homogeneous nucleation may be easily achieved by using a simple atomizer construction, and thus is potentially suitable for fuel injection systems in combustors and engines. - Highlights: • We study the characteristics of a spray that is generated by a flash boiling process. • In this study, the flash boiling process occurs under homogeneous nucleation regime. • We used Phase Doppler Particle Analyzer (PDPA) to characterize the spray. • The SMD has been found to be strongly affected by the initial liquid temperature. • Homogeneous nucleation may be easily achieved by using a simple atomizer unit
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Heterogeneous ice nucleation and phase transition of viscous α-pinene secondary organic aerosol
Ignatius, Karoliina; Kristensen, Thomas B.; Järvinen, Emma; Nichman, Leonid; Fuchs, Claudia; Gordon, Hamish; Herenz, Paul; Hoyle, Christopher R.; Duplissy, Jonathan; Baltensperger, Urs; Curtius, Joachim; Donahue, Neil M.; Gallagher, Martin W.; Kirkby, Jasper; Kulmala, Markku; Möhler, Ottmar; Saathoff, Harald; Schnaiter, Martin; Virtanen, Annele; Stratmann, Frank
2016-04-01
There are strong indications that particles containing secondary organic aerosol (SOA) exhibit amorphous solid or semi-solid phase states in the atmosphere. This may facilitate deposition ice nucleation and thus influence cirrus cloud properties. Global model simulations of monoterpene SOA particles suggest that viscous biogenic SOA are indeed present in regions where cirrus cloud formation takes place. Hence, they could make up an important contribution to the global ice nucleating particle (INP) budget. However, experimental ice nucleation studies of biogenic SOA are scarce. Here, we investigated the ice nucleation ability of viscous SOA particles at the CLOUD (Cosmics Leaving OUtdoor Droplets) experiment at CERN (Ignatius et al., 2015, Järvinen et al., 2015). In the CLOUD chamber, the SOA particles were produced from the ozone initiated oxidation of α-pinene at temperatures in the range from -38 to -10° C at 5-15 % relative humidity with respect to water (RHw) to ensure their formation in a highly viscous phase state, i.e. semi-solid or glassy. We found that particles formed and grown in the chamber developed an asymmetric shape through coagulation. As the RHw was increased to between 35 % at -10° C and 80 % at -38° C, a transition to spherical shape was observed with a new in-situ optical method. This transition confirms previous modelling of the viscosity transition conditions. The ice nucleation ability of SOA particles was investigated with a new continuous flow diffusion chamber SPIN (Spectrometer for Ice Nuclei) for different SOA particle sizes. For the first time, we observed heterogeneous ice nucleation of viscous α-pinene SOA in the deposition mode for ice saturation ratios between 1.3 and 1.4, significantly below the homogeneous freezing limit. The maximum frozen fractions found at temperatures between -36.5 and -38.3° C ranged from 6 to 20 % and did not depend on the particle surface area. References Ignatius, K. et al., Heterogeneous ice
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Budke, Carsten; Dreischmeier, Katharina; Koop, Thomas
2014-05-01
Homogeneous ice nucleation is a stochastic process, implying that it is not only temperature but also time dependent. For heterogeneous ice nucleation it is still under debate whether there is a significant time dependence or not. In case of minor time dependence it is probably sufficient to use a singular or slightly modified singular approach, which mainly supposes temperature dependence and just small stochastic variations. We contribute to this discussion using a novel optical freezing array termed BINARY (Bielefeld Ice Nucleation ARraY). The setup consists of an array of microliter-sized droplets on a Peltier cooling stage. The droplets are separated from each other with a polydimethylsiloxane (PDMS) spacer to prevent a Bergeron-Findeisen process, in which the first freezing droplets grow at the expense of the remaining liquid ones due to their vapor pressure differences. An automatic detection of nucleation events is realized optically by the change in brightness during freezing. Different types of ice nucleating agents were tested with the presented setup, e. g. pollen and clay mineral dust. Exemplarily, cooling rate dependent measurements are shown for the heterogeneous ice nucleation induced by Snomax®. The authors gratefully acknowledge funding by the German Research Foundation (DFG) through the project BIOCLOUDS (KO 2944/1-1) and through the research unit INUIT (FOR 1525) under KO 2944/2-1. We particularly thank our INUIT partners for fruitful collaboration and sharing of ideas and IN samples.
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Ice nucleation efficiency of AgI: review and new insights
Directory of Open Access Journals (Sweden)
C. Marcolli
2016-07-01
Full Text Available AgI is one of the best-investigated ice-nucleating substances. It has relevance for the atmosphere since it is used for glaciogenic cloud seeding. Theoretical and experimental studies over the last 60 years provide a complex picture of silver iodide as an ice-nucleating agent with conflicting and inconsistent results. This review compares experimental ice nucleation studies in order to analyze the factors that influence the ice nucleation ability of AgI. 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. The ice nucleation by particles with surfaces exposed to air depends on water adsorption. AgI surfaces seem to be most efficient at nucleating ice when they are exposed to relative humidity at or even above water saturation. For AgI particles that are completely immersed in water, the freezing temperature increases with increasing AgI surface area. Higher threshold freezing temperatures 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 for ice nucleation in cloud chambers with short residence times.
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Freezing nucleation apparatus puts new slant on study of biological ice nucleators in precipitation
Stopelli, E.; Conen, F.; Zimmermann, L.; Alewell, C.; Morris, C. E.
2014-01-01
For decades, drop-freezing instruments have contributed to a better understanding of biological ice nucleation and its likely implications for cloud and precipitation development. Yet, current instruments have limitations. Drops analysed on a cold stage are subject to evaporation and potential contamination. The use of closed tubes provides a partial solution to these problems, but freezing events are still difficult to be clearly detected. Here, we present a new apparatus where freezing in closed tubes is detected automatically by a change in light transmission upon ice development, caused by the formation of air bubbles and crystal facets that scatter light. Risks of contamination and introduction of biases linked to detecting the freezing temperature of a sample are then minimized. To illustrate the performance of the new apparatus we show initial results of two assays with snow samples. In one, we repeatedly analysed the sample (208 tubes) over the course of a month with storage at +4 °C, during which evidence for biological ice nucleation activity emerged through an increase in the number of ice nucleators active around -4 °C. In the second assay, we indicate the possibility of increasingly isolating a single ice nucleator from a precipitation sample, potentially determining the nature of a particle responsible for a nucleation activity measured directly in the sample. These two seminal approaches highlight the relevance of this handy apparatus for providing new points of view in biological ice nucleation research.
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Chlorine-containing salts as water ice nucleating particles on Mars
Santiago-Materese, D. L.; Iraci, L. T.; Clapham, M. E.; Chuang, P. Y.
2018-03-01
Water ice cloud formation on Mars largely is expected to occur on the most efficient ice nucleating particle available. Salts have been observed on the Martian surface and have been known to facilitate water cloud formation on Earth. We examined heterogeneous ice nucleation onto sodium chloride and sodium perchlorate substrates under Martian atmospheric conditions, in the range of 150 to 180 K and 10-7 to 10-5 Torr water partial pressure. Sub-155 K data for the critical saturation ratio (Scrit) suggests an exponential model best describes the temperature-dependence of nucleation onset of water ice for all substrates tested. While sodium chloride does not facilitate water ice nucleation more easily than bare silicon, sodium perchlorate does support depositional nucleation at lower saturation levels than other substrates shown and is comparable to smectite-rich clay in its ability to support cloud initiation. Perchlorates could nucleate water ice at partial pressures up to 40% lower than other substrates examined to date under Martian atmospheric conditions. These findings suggest air masses on Mars containing uplifted salts such as perchlorates could form water ice clouds at lower saturation ratios than in air masses absent similar particles.
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Heterogeneous nucleation of ice in the atmosphere
International Nuclear Information System (INIS)
Nicosia, A; Piazza, M; Santachiara, G; Belosi, F
2017-01-01
The occurrence of ice-nucleating aerosols in the atmosphere has a profound impact on the properties of clouds, and in turn, influences our understanding on weather and climate. Research on this topic has grown constantly over the last decades, driven by advances in online and offline instruments capable of measuring the characteristics of these cloud-modifying aerosol particles. This article presents different aspects to the understanding of how aerosol particles can trigger the nucleation of ice in clouds. In addition, we present some experimental results obtained with the Dynamic Filter Processing Chamber, an off-line instrument that has been applied extensively in the last years and that circumvents some of the problems related to the measurement of Ice Nucleating Particles properties. (paper)
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Bioinspired Materials for Controlling Ice Nucleation, Growth, and Recrystallization.
He, Zhiyuan; Liu, Kai; Wang, Jianjun
2018-05-15
Ice formation, mainly consisting of ice nucleation, ice growth, and ice recrystallization, is ubiquitous and crucial in wide-ranging fields from cryobiology to atmospheric physics. Despite active research for more than a century, the mechanism of ice formation is still far from satisfactory. Meanwhile, nature has unique ways of controlling ice formation and can provide resourceful avenues to unravel the mechanism of ice formation. For instance, antifreeze proteins (AFPs) protect living organisms from freezing damage via controlling ice formation, for example, tuning ice nucleation, shaping ice crystals, and inhibiting ice growth and recrystallization. In addition, AFP mimics can have applications in cryopreservation of cells, tissues, and organs, food storage, and anti-icing materials. Therefore, continuous efforts have been made to understand the mechanism of AFPs and design AFP inspired materials. In this Account, we first review our recent research progress in understanding the mechanism of AFPs in controlling ice formation. A Janus effect of AFPs on ice nucleation was discovered, which was achieved via selectively tethering the ice-binding face (IBF) or the non-ice-binding face (NIBF) of AFPs to solid surfaces and investigating specifically the effect of the other face on ice nucleation. Through molecular dynamics (MD) simulation analysis, we observed ordered hexagonal ice-like water structure atop the IBF and disordered water structure atop the NIBF. Therefore, we conclude that the interfacial water plays a critical role in controlling ice formation. Next, we discuss the design and fabrication of AFP mimics with capabilities in tuning ice nucleation and controlling ice shape and growth, as well as inhibiting ice recrystallization. For example, we tuned ice nucleation via modifying solid surfaces with supercharged unfolded polypeptides (SUPs) and polyelectrolyte brushes (PBs) with different counterions. We found graphene oxide (GO) and oxidized quasi
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The enhancement and suppression of immersion mode heterogeneous ice-nucleation by solutes.
Whale, Thomas F; Holden, Mark A; Wilson, Theodore W; O'Sullivan, Daniel; Murray, Benjamin J
2018-05-07
Heterogeneous nucleation of ice from aqueous solutions is an important yet poorly understood process in multiple fields, not least the atmospheric sciences where it impacts the formation and properties of clouds. In the atmosphere ice-nucleating particles are usually, if not always, mixed with soluble material. However, the impact of this soluble material on ice nucleation is poorly understood. In the atmospheric community the current paradigm for freezing under mixed phase cloud conditions is that dilute solutions will not influence heterogeneous freezing. By testing combinations of nucleators and solute molecules we have demonstrated that 0.015 M solutions (predicted melting point depression nucleate ice up to around 3 °C warmer than they do in pure water. In contrast, dilute solutions of certain alkali metal halides can dramatically depress freezing points for the same nucleators. At 0.015 M, solutes can enhance or deactivate the ice-nucleating ability of a microcline feldspar across a range of more than 10 °C, which corresponds to a change in active site density of more than a factor of 10 5 . This concentration was chosen for a survey across multiple solutes-nucleant combinations since it had a minimal colligative impact on freezing and is relevant for activating cloud droplets. Other nucleators, for instance a silica gel, are unaffected by these 'solute effects', to within experimental uncertainty. This split in response to the presence of solutes indicates that different mechanisms of ice nucleation occur on the different nucleators or that surface modification of relevance to ice nucleation proceeds in different ways for different nucleators. These solute effects on immersion mode ice nucleation may be of importance in the atmosphere as sea salt and ammonium sulphate are common cloud condensation nuclei (CCN) for cloud droplets and are internally mixed with ice-nucleating particles in mixed-phase clouds. In addition, we propose a pathway dependence where
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Kobayashi, Atsuko; Horikawa, Masamoto; Kirschvink, Joseph L; Golash, Harry N
2018-05-22
In supercooled water, ice nucleation is a stochastic process that requires ∼250-300 molecules to transiently achieve structural ordering before an embryonic seed crystal can nucleate. This happens most easily on crystalline surfaces, in a process termed heterogeneous nucleation; without such surfaces, water droplets will supercool to below -30 °C before eventually freezing homogeneously. A variety of fundamental processes depends on heterogeneous ice nucleation, ranging from desert-blown dust inducing precipitation in clouds to frost resistance in plants. Recent experiments have shown that crystals of nanophase magnetite (Fe 3 O 4 ) are powerful nucleation sites for this heterogeneous crystallization of ice, comparable to other materials like silver iodide and some cryobacterial peptides. In natural materials containing magnetite, its ferromagnetism offers the possibility that magneto-mechanical motion induced by external oscillating magnetic fields could act to disrupt the water-crystal interface, inhibiting the heterogeneous nucleation process in subfreezing water and promoting supercooling. For this to act, the magneto-mechanical rotation of the particles should be higher than the magnitude of Brownian motions. We report here that 10-Hz precessing magnetic fields, at strengths of 1 mT and above, on ∼50-nm magnetite crystals dispersed in ultrapure water, meet these criteria and do indeed produce highly significant supercooling. Using these rotating magnetic fields, we were able to elicit supercooling in two representative plant and animal tissues (celery and bovine muscle), both of which have detectable, natural levels of ferromagnetic material. Tailoring magnetic oscillations for the magnetite particle size distribution in different tissues could maximize this supercooling effect. Copyright © 2018 the Author(s). Published by PNAS.
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Directory of Open Access Journals (Sweden)
K. Diehl
2018-03-01
Full Text Available In deep convective clouds, heavy rain is often formed involving the ice phase. Simulations were performed using the 3-D cloud resolving model COSMO-SPECS with detailed spectral microphysics including parameterizations of homogeneous and three heterogeneous freezing modes. The initial conditions were selected to result in a deep convective cloud reaching 14 km of altitude with strong updrafts up to 40 m s−1. At such altitudes with corresponding temperatures below −40 °C the major fraction of liquid drops freezes homogeneously. The goal of the present model simulations was to investigate how additional heterogeneous freezing will affect ice formation and precipitation although its contribution to total ice formation may be rather low. In such a situation small perturbations that do not show significant effects at first sight may trigger cloud microphysical responses. Effects of the following small perturbations were studied: (1 additional ice formation via immersion, contact, and deposition modes in comparison to solely homogeneous freezing, (2 contact and deposition freezing in comparison to immersion freezing, and (3 small fractions of biological ice nucleating particles (INPs in comparison to higher fractions of mineral dust INP. The results indicate that the modification of precipitation proceeds via the formation of larger ice particles, which may be supported by direct freezing of larger drops, the growth of pristine ice particles by riming, and by nucleation of larger drops by collisions with pristine ice particles. In comparison to the reference case with homogeneous freezing only, such small perturbations due to additional heterogeneous freezing rather affect the total precipitation amount. It is more likely that the temporal development and the local distribution of precipitation are affected by such perturbations. This results in a gradual increase in precipitation at early cloud stages instead of a strong increase at
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Homogeneous nucleation limit on the bulk formation of metallic glasses
International Nuclear Information System (INIS)
Drehman, A.J.
1983-01-01
Glassy Pd 82 Si 18 spheres, of up to 1 mm diameter, were formed in a drop tube filled with He gas. The largest spheres were successfully cooled to a glass using a cooling rate of less than 800 K/sec. Even at this low cooling rate, crystallization (complete or partial) was the result of heterogeneous nucleation at a high temperature, relative to the temperature at which copious homogeneous nucleation would commence. Bulk underscoring experiments demonstrated that this alloy could be cooled to 385 K below its eutectic melting temperature (1083 K) without the occurrence of crystallization. If heterogeneous nucleation can be avoided, it is estimated that a cooling rate of at most 100 K/sec would be required to form this alloy in the glassy state. Ingots of glassy Pd 40 Ni 40 P 20 were formed from the liquid by cooling at a rate of only 1 K/sec. It was found that glassy samples of this alloy could be heated well above the glass transition temperature without the occurrence of rapid divitrification. This is a result due, in part of the low density of pre-existing nuclei, but, more importantly, due to the low homogeneous nucleation rate and the slow crystal growth kinetics. Based on the observed devitrification kinetics, the steady-state homogeneous nucleation rate is approximately 1 nuclei/cm 3 sec at 590 K (the temperature at which the homogeneous nucleation rate is estimated to be a maximum). Two iron-nickel based glass-forming alloys (Fe 40 Ni 40 P 14 B 6 and Fe 40 Ni 40 B 20 , were not successfully formed into glassy spheres, however, microstructural examination indicates that crystallization was not the result of copious homogeneous nucleation. In contrast, glass forming iron based alloys (Fe 80 B 20 and Fe/sub 79.3/B/sub 16.4/Si/sub 4.0/C/sub 0.3/) exhibit copious homogeneous nucleation when cooled at approximately the same rate
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Glatz, Brittany; Sarupria, Sapna
2018-01-23
Ice is ubiquitous in nature, and heterogeneous ice nucleation is the most common pathway of ice formation. How surface properties affect the propensity to observe ice nucleation on that surface remains an open question. We present results of molecular dynamics studies of heterogeneous ice nucleation on model surfaces. The models surfaces considered emulate the chemistry of kaolinite, an abundant component of mineral dust. We investigate the interplay of surface lattice and hydrogen bonding properties in affecting ice nucleation. We find that lattice matching and hydrogen bonding are necessary but not sufficient conditions for observing ice nucleation at these surfaces. We correlate this behavior to the orientations sampled by the metastable supercooled water in contact with the surfaces. We find that ice is observed in cases where water molecules not only sample orientations favorable for bilayer formation but also do not sample unfavorable orientations. This distribution depends on both surface-water and water-water interactions and can change with subtle modifications to the surface properties. Our results provide insights into the diverse behavior of ice nucleation observed at different surfaces and highlight the complexity in elucidating heterogeneous ice nucleation.
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Controlled ice nucleation using freeze-dried Pseudomonas syringae encapsulated in alginate beads.
Weng, Lindong; Tessier, Shannon N; Swei, Anisa; Stott, Shannon L; Toner, Mehmet
2017-04-01
The control of ice nucleation is of fundamental significance in many process technologies related to food and pharmaceutical science and cryobiology. Mechanical perturbation, electromagnetic fields and ice-nucleating agents (INAs) have been known to induce ice nucleation in a controlled manner. But these ice-nucleating methods may suffer from cumbersome manual operations, safety concerns of external fields, and biocompatibility and recovery issues of INA particles, especially when used in living systems. Given the automatic ice-seeding nature of INAs, a promising solution to overcome some of the above limitations is to engineer a biocomposite that accommodates the INA particles but minimizes their interactions with biologics, as well as enabling the recovery of used particles. In this study, freeze-dried Pseudomonas syringae, a model ice-nucleating agent, was encapsulated into microliter-sized alginate beads. We evaluated the performance of the bacterial hydrogel beads to initiate ice nucleation in water and aqueous glycerol solution by investigating factors including the size and number of the beads and the local concentration of INA particles. In the aqueous sample of a fixed volume, the total mass of the INA particles (m) was found to be the governing parameter that is solely responsible for determining the ice nucleation performance of the bacterial hydrogel beads. The freezing temperature has a strong positive linear correlation with log 10 m. The findings in this study provide an effective, predictable approach to control ice nucleation, which can improve the outcome and standardization of many ice-assisted process technologies. Copyright © 2017 Elsevier Inc. All rights reserved.
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Molecular sizes of lichen ice nucleation sites determined by gamma radiation inactivation analysis
International Nuclear Information System (INIS)
Kieft, T.L.; Ruscetti, T.
1992-01-01
It has previously been shown that some species of lichen fungi contain proteinaceous ice nuclei which are active at temperatures as warm as −2 °C. This experiment was undertaken to determine the molecular sizes of ice nuclei in the lichen fungus Rhizoplaca chrysoleuca and to compare them to bacterial ice nuclei from Pseudomonas syringae. Gamma radiation inactivation analysis was used to determine molecular weights. Radiation inactivation analysis is based on target theory, which states that the likelihood of a molecule being inactivated by gamma rays increases as its size increases. Three different sources of ice nuclei from the lichen R. chrysoleuca were tested: field-collected lichens, extract of lichen fungus, and a pure culture of the fungus R. chrysoleuca. P. syringae strain Cit7 was used as a source of bacterial ice nuclei. Samples were lyophilized, irradiated with gamma doses ranging from 0 to 10.4 Mrads, and then tested for ice nucleation activity using a droplet-freezing assay. Data for all four types of samples were in rough agreement; sizes of nucleation sites increased logarithmically with increasing temperatures of ice nucleation activity. Molecular weights of nucleation sites active between −3 and −4 °C from the bacteria and from the field-collected lichens were approximately 1.0 × 10 6 Da. Nuclei from the lichen fungus and in the lichen extract appeared to be slightly smaller but followed the same log-normal pattern with temperature of ice nucleation activity. The data for both the bacterial and lichen ice nuclei are in agreement with ice nucleation theory which states that the size of ice nucleation sites increases logarithmically as the temperature of nucleation increases linearly. This suggests that although some differences exist between bacterial and lichen ice nucleation sites, their molecular sizes are quite similar
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Investigation of heterogeneous ice nucleation in pollen suspensions and washing water
Dreischmeier, Katharina; Budke, Carsten; Koop, Thomas
2014-05-01
Biological particles such as pollen often show ice nucleation activity at temperatures higher than -20 °C. Immersion freezing experiments of pollen washing water demonstrate comparable ice nucleation behaviour as water containing the whole pollen bodies (Pummer et al., 2012). It was suggested that polysaccharide molecules leached from the grains are responsible for the ice nucleation. Here, heterogeneous ice nucleation in birch pollen suspensions and their washing water was investigated by two different experimental methods. The optical freezing array BINARY (Bielefeld Ice Nucleation ARraY) allows the direct observation of freezing of microliter-sized droplets. The IN spectra obtained from such experiments with birch pollen suspensions over a large concentration range indicate several different ice nucleation active species, two of which are present also in the washing water. The latter was probed also in differential scanning calorimeter (DSC) experiments of emulsified sub-picoliter droplets. Due to the small droplet size in the emulsion samples and at small concentration of IN in the washing water, such DSC experiments can exhibit the ice nucleation behaviour of a single nucleus. The two heterogeneous freezing signals observed in the DSC thermograms can be assigned to two different kinds of ice nuclei, confirming the observation from the BINARY measurements, and also previous studies on Swedish birch pollen washing water (Augustin et al., 2012). The authors gratefully acknowledge funding by the German Research Foundation (DFG) through the project BIOCLOUDS (KO 2944/1-1) and through the research unit INUIT (FOR 1525) under KO 2944/2-1. We particularly thank our INUIT partners for fruitful collaboration and sharing of ideas and IN samples. S. Augustin, H. Wex, D. Niedermeier, B. Pummer, H. Grothe, S. Hartmann, L. Tomsche, T. Clauss, J. Voigtländer, K. Ignatius, and F. Stratmann, Immersion freezing of birch pollen washing water, Atmos. Chem. Phys., 13, 10989
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The Effect of Volcanic Ash Composition on Ice Nucleation Affinity
Genareau, K. D.; Cloer, S.; Primm, K.; Woods, T.; Tolbert, M. A.
2017-12-01
Understanding the role that volcanic ash plays in ice nucleation is important for knowledge of lightning generation in both volcanic plumes and in clouds developing downwind from active volcanoes. Volcanic ash has long been suggested to influence heterogeneous ice nucleation following explosive eruptions, but determining precisely how composition and mineralogy affects ice nucleation affinity (INA) is poorly constrained. For the study presented here, volcanic ash samples with different compositions and mineral/glass contents were tested in both the deposition and immersion modes, following the methods presented in Schill et al. (2015). Bulk composition was determined with X-ray fluorescence (XRF), grain size distribution was determined with laser diffraction particle size analysis (LDPSA), and mineralogy was determined with X-ray diffraction (XRD) and scanning electron microscopy (SEM). Results of the deposition-mode experiments reveal that there is no relationship between ice saturation ratios (Sice) and either mineralogy or bulk ash composition, as all samples have similar Sice ratios. In the immersion-mode experiments, frozen fractions were determined from -20 °C to -50 °C using three different amounts of ash (0.5, 1.0, and 2.0 wt% of slurry). Results from the immersion freezing reveal that the rhyolitic samples (73 wt% SiO2) nucleate ice at higher temperatures compared to the basaltic samples (49 wt% SiO2). There is no observed correlation between frozen fractions and mineral content of ash samples, but the two most efficient ice nuclei are rhyolites that contain the greatest proportion of amorphous glass (> 90 %), and are enriched in K2O relative to transition metals (MnO and TiO2), the latter of which show a negative correlation with frozen fraction. Higher ash abundance in water droplets increases the frozen fraction at all temperatures, indicating that ash amount plays the biggest role in ice nucleation. If volcanic ash can reach sufficient abundance (
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Yang, Fan
Ice particles in atmospheric clouds play an important role in determining cloud lifetime, precipitation and radiation. It is therefore important to understand the whole life cycle of ice particles in the atmosphere, e.g., where they come from (nucleation), how they evolve (growth), and where they go (precipitation). Ice nucleation is the crucial step for ice formation, and in this study, we will mainly focus on ice nucleation in the lab and its effect on mixed-phase stratiform clouds. In the first half of this study, we investigate the relevance of moving contact lines (i.e., the region where three or more phases meet) on the phenomenon of contact nucleation. High speed video is used to investigate heterogeneous ice nucleation in supercooled droplets resting on cold substrates under two different dynamic conditions: droplet electrowetting and droplet vibration. The results show that contact-line motion is not a sufficient condition to trigger ice nucleation, while locally curved contact lines that can result from contact-line motion are strongly related to ice nucleation. We propose that pressure perturbations due to locally curved contact lines can strongly enhance the ice nucleation rate, which gives another interpretation for the mechanism for contact nucleation. Corresponding theoretical results provide a quantitative connection between pressure perturbations and temperature, providing a useful tool for ice nucleation calculations in atmospheric models. In this second half of the study, we build a minimalist model for long lifetime mixed-phase stratiform clouds based on stochastic ice nucleation. Our result shows that there is a non-linear relationship between ice water contact and ice number concentration in the mixed-phase cloud, as long as the volume ice nucleation rate is constant. This statistical property may help identify the source of ice nuclei in mixed-phase clouds. In addition, results from Lagrangian ice particle tracking in time dependent fields
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Using Ice Nucleating Particles to Enable Desublimation on Chilled Substrates
O'Brien, Julia; Failor, Kevin; Bisbano, Caitlin; Mulroe, Megan; Nath, Saurabh; Vinatzer, Boris; Boreyko, Jonathan
2017-11-01
On a subfreezing surface, nucleating embryos usually form as supercooled condensate that later freeze into ice, as opposed to desublimation. Ice nucleating particles (INPs) have been widely used to freeze existing water; however, nobody has studied how they might affect the initial mode of nucleation. Here, we show that INPs deposited on a substrate can switch the mode of embryo nucleation to desublimation, rather than supercooled condensation. Deposition was achieved by evaporating a water droplet containing INPs on a hydrophobic silicon wafer. A Peltier stage was used to cool the wafer down inside of a controlled humidity chamber, such that the desired set point temperature correlated with the dew point and onset of nucleation. Beneath a critical surface temperature, microscopy indicated that desublimation occurred on the circular patch of deposited INPs, compared to supercooled condensation outside the circle. The hydrophobic surface was then patterned with hydrophilic stripe arrays, which facilitated the deposition of stripes of INPs via the same evaporation method. The resulting array of desublimating ice stripes created dry zones free of condensation or frost in the intermediate areas, as the hygroscopic ice stripes served as overlapping humidity sinks.
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Measurements of ice nucleating particle concentrations at 242 K in the free troposphere
Lacher, L.; Lohmann, U.; Boose, Y.; Zipori, A.; Herrmann, E.; Bukowiecki, N.; Steinbacher, M.; Gute, E.; Kanji, Z. A.
2017-12-01
Clouds containing ice play an important role in the Earth's system, but some fundamental knowledge on their formation and further development is still missing. The phase change from vapor or liquid to ice in the atmosphere can occur heterogeneously in the presence of ice nucleating particles (INPs) at temperatures warmer, and supersaturations lower than required for homogeneous freezing. Only a small fraction of particles in an environment relevant for the occurrence of ice- and mixed-phase clouds are INPs, and their identification and quantification remains challenging. We measure INP concentrations with the ETH Horizontal Ice Nucleation Chamber (HINC) at the High Altitude Research Station Jungfraujoch (JFJ) during several field campaigns in different seasons and years. The measurements are performed at 242 K and above water saturation, representing ice- and mixed-phase clouds conditions. Due to its elevation of 3580 m a.s.l. the site encounters mostly free tropospheric conditions, and is influenced by boundary layer injections up to 80% of the time in summer. JFJ regularly encounters Saharan dust events and receives air masses of marine origin, which can both occur within the free troposphere. Our measurements show that INP concentrations in the free troposphere do not follow a seasonal cycle. They are remarkably constant, with concentrations from 0.5 - 8 L-1 (interquartile range), which compares well to measurements performed under the same conditions at another location within the free troposphere, the Izaña Atmospheric Research Station in Tenerife. At JFJ, correlations with parameters of physical properties of ambient particles, meteorology and air mass characteristics do not show a single best estimator to predict INP concentrations, emphasizing the complexity of ice nucleation in the free troposphere. Increases in INP concentrations of a temporary nature were observed in the free troposphere during Saharan dust events and marine air mass influence, which
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Savre, J.; Ekman, A. M. L.
2015-05-01
A new parameterization for heterogeneous ice nucleation constrained by laboratory data and based on classical nucleation theory is introduced. Key features of the parameterization include the following: a consistent and modular modeling framework for treating condensation/immersion and deposition freezing, the possibility to consider various potential ice nucleating particle types (e.g., dust, black carbon, and bacteria), and the possibility to account for an aerosol size distribution. The ice nucleating ability of each aerosol type is described using a contact angle (θ) probability density function (PDF). A new modeling strategy is described to allow the θ PDF to evolve in time so that the most efficient ice nuclei (associated with the lowest θ values) are progressively removed as they nucleate ice. A computationally efficient quasi Monte Carlo method is used to integrate the computed ice nucleation rates over both size and contact angle distributions. The parameterization is employed in a parcel model, forced by an ensemble of Lagrangian trajectories extracted from a three-dimensional simulation of a springtime low-level Arctic mixed-phase cloud, in order to evaluate the accuracy and convergence of the method using different settings. The same model setup is then employed to examine the importance of various parameters for the simulated ice production. Modeling the time evolution of the θ PDF is found to be particularly crucial; assuming a time-independent θ PDF significantly overestimates the ice nucleation rates. It is stressed that the capacity of black carbon (BC) to form ice in the condensation/immersion freezing mode is highly uncertain, in particular at temperatures warmer than -20°C. In its current version, the parameterization most likely overestimates ice initiation by BC.
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Ice Nucleation Activity of Various Agricultural Soil Dust Aerosol Particles
Schiebel, Thea; Höhler, Kristina; Funk, Roger; Hill, Thomas C. J.; Levin, Ezra J. T.; Nadolny, Jens; Steinke, Isabelle; Suski, Kaitlyn J.; Ullrich, Romy; Wagner, Robert; Weber, Ines; DeMott, Paul J.; Möhler, Ottmar
2016-04-01
Recent investigations at the cloud simulation chamber AIDA (Aerosol Interactions and Dynamics in the Atmosphere) suggest that agricultural soil dust has an ice nucleation ability that is enhanced up to a factor of 10 compared to desert dust, especially at temperatures above -26 °C (Steinke et al., in preparation for submission). This enhancement might be caused by the contribution of very ice-active biological particles. In addition, soil dust aerosol particles often contain a considerably higher amount of organic matter compared to desert dust particles. To test agricultural soil dust as a source of ice nucleating particles, especially for ice formation in warm clouds, we conducted a series of laboratory measurements with different soil dust samples to extend the existing AIDA dataset. The AIDA has a volume of 84 m3 and operates under atmospherically relevant conditions over wide ranges of temperature, pressure and humidity. By controlled adiabatic expansions, the ascent of an air parcel in the troposphere can be simulated. As a supplement to the AIDA facility, we use the INKA (Ice Nucleation Instrument of the KArlsruhe Institute of Technology) continuous flow diffusion chamber based on the design by Rogers (1988) to expose the sampled aerosol particles to a continuously increasing saturation ratio by keeping the aerosol temperature constant. For our experiments, soil dust was dry dispersed into the AIDA vessel. First, fast saturation ratio scans at different temperatures were performed with INKA, sampling soil dust aerosol particles directly from the AIDA vessel. Then, we conducted the AIDA expansion experiment starting at a preset temperature. The combination of these two different methods provides a robust data set on the temperature-dependent ice activity of various agriculture soil dust aerosol particles with a special focus on relatively high temperatures. In addition, to extend the data set, we investigated the role of biological and organic matter in more
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Inhibition of ice nucleation by slippery liquid-infused porous surfaces (SLIPS).
Wilson, Peter W; Lu, Weizhe; Xu, Haojun; Kim, Philseok; Kreder, Michael J; Alvarenga, Jack; Aizenberg, Joanna
2013-01-14
Ice repellent coatings have been studied and keenly sought after for many years, where any advances in the durability of such coatings will result in huge energy savings across many fields. Progress in creating anti-ice and anti-frost surfaces has been particularly rapid since the discovery and development of slippery, liquid infused porous surfaces (SLIPS). Here we use SLIPS-coated differential scanning calorimeter (DSC) pans to investigate the effects of the surface modification on the nucleation of supercooled water. This investigation is inherently different from previous studies which looked at the adhesion of ice to SLIPS surfaces, or the formation of ice under high humidity conditions. Given the stochastic nature of nucleation of ice from supercooled water, multiple runs on the same sample are needed to determine if a given surface coating has a real and statistically significant effect on the nucleation temperature. We have cycled supercooling to freezing and then thawing of deionized water in hydrophilic (untreated aluminum), hydrophobic, superhydrophobic, and SLIPS-treated DSC pans multiple times to determine the effects of surface treatment on the nucleation and subsequent growth of ice. We find that SLIPS coatings lower the nucleation temperature of supercooled water in contact with statistical significance and show no deterioration or change in the coating performance even after 150 freeze-thaw cycles.
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Modelling of cirrus clouds – Part 2: Competition of different nucleation mechanisms
Directory of Open Access Journals (Sweden)
P. Spichtinger
2009-04-01
Full Text Available We study the competition of two different freezing mechanisms (homogeneous and heterogeneous freezing in the same environment for cold cirrus clouds. To this goal we use the recently developed and validated ice microphysics scheme (Spichtinger and Gierens, 2009a which distinguishes between ice classes according to their formation process. We investigate cases with purely homogeneous ice formation and compare them with cases where background ice nuclei in varying concentration heterogeneously form ice prior to homogeneous nucleation. We perform additionally a couple of sensitivity studies regarding threshold humidity for heterogeneous freezing, uplift speed, and ambient temperature, and we study the influence of random motions induced by temperature fluctuations in the clouds. We find three types of cloud evolution, homogeneously dominated, heterogeneously dominated, and a mixed type where neither nucleation process dominates. The latter case is prone to long–lasting in–cloud ice supersaturation of the order 30% and more.
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Immersion Freezing of Aluminas: The Effect of Crystallographic Properties on Ice Nucleation
King, M.; Chong, E.; Freedman, M. A.
2017-12-01
Atmospheric aerosol particles serve as the nuclei for heterogeneous ice nucleation, a process that allows for ice to form at higher temperatures and lower supersaturations with respect to ice. This process is essential to the formation of ice in cirrus clouds. Heterogeneous ice nucleation is affected by many factors including the composition, crystal structure, porosity, and surface area of the particles. However, these factors are not well understood and, as such, are difficult to account for in climate models. To test the effects of crystal structure on ice nucleation, a system of transition aluminas (Al2O3) that differ only in their crystal structure, despite being compositionally similar, were tested using immersion freezing. Particles were immersed in water and placed into a temperature controlled chamber. Freezing events were then recorded as the chamber was cooled to negative 30 °. Alpha-alumina, which is a member of the hexagonal crystal system, showed a significantly higher temperature at which all particles froze in comparison to other samples. This supports the hypothesis that, since a hexagonal crystal structure is the lowest energy state for ice, hexagonal surface structures would best facilitate ice nucleation. However, a similar sample of hexagonal chi-alumina did not show the same results. Further analysis of the samples will be done to characterize surface structures and composition. These conflicting data sets raise interesting questions about the effect of other surface features, such as surface area and porosity, on ice nucleation.
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A new temperature and humidity dependent surface site density approach for deposition ice nucleation
I. Steinke; C. Hoose; O. Möhler; P. Connolly; T. Leisner
2014-01-01
Deposition nucleation experiments with Arizona Test Dust (ATD) as a surrogate for mineral dusts were conducted at the AIDA cloud chamber at temperatures between 220 and 250 K. The influence of the aerosol size distribution and the cooling rate on the ice nucleation efficiencies was investigated. Ice nucleation active surface site (INAS) densities were calculated to quantify the ice nucleation efficiency as a function of temperature, humidity and the aerosol ...
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The relevance of nanoscale biological fragments for ice nucleation in clouds
O‧Sullivan, D.; Murray, B. J.; Ross, J. F.; Whale, T. F.; Price, H. C.; Atkinson, J. D.; Umo, N. S.; Webb, M. E.
2015-01-01
Most studies of the role of biological entities as atmospheric ice-nucleating particles have focused on relatively rare supermicron particles such as bacterial cells, fungal spores and pollen grains. However, it is not clear that there are sufficient numbers of these particles in the atmosphere to strongly influence clouds. Here we show that the ice-nucleating activity of a fungus from the ubiquitous genus Fusarium is related to the presence of nanometre-scale particles which are far more numerous, and therefore potentially far more important for cloud glaciation than whole intact spores or hyphae. In addition, we quantify the ice-nucleating activity of nano-ice nucleating particles (nano-INPs) washed off pollen and also show that nano-INPs are present in a soil sample. Based on these results, we suggest that there is a reservoir of biological nano-INPs present in the environment which may, for example, become aerosolised in association with fertile soil dust particles.
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An improved model for nucleation-limited ice formation in living cells during freezing.
Directory of Open Access Journals (Sweden)
Jingru Yi
Full Text Available Ice formation in living cells is a lethal event during freezing and its characterization is important to the development of optimal protocols for not only cryopreservation but also cryotherapy applications. Although the model for probability of ice formation (PIF in cells developed by Toner et al. has been widely used to predict nucleation-limited intracellular ice formation (IIF, our data of freezing Hela cells suggest that this model could give misleading prediction of PIF when the maximum PIF in cells during freezing is less than 1 (PIF ranges from 0 to 1. We introduce a new model to overcome this problem by incorporating a critical cell volume to modify the Toner's original model. We further reveal that this critical cell volume is dependent on the mechanisms of ice nucleation in cells during freezing, i.e., surface-catalyzed nucleation (SCN and volume-catalyzed nucleation (VCN. Taken together, the improved PIF model may be valuable for better understanding of the mechanisms of ice nucleation in cells during freezing and more accurate prediction of PIF for cryopreservation and cryotherapy applications.
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Glassy aerosols with a range of compositions nucleate ice heterogeneously at cirrus temperatures
Directory of Open Access Journals (Sweden)
T. W. Wilson
2012-09-01
Full Text Available Atmospheric secondary organic aerosol (SOA is likely to exist in a semi-solid or glassy state, particularly at low temperatures and humidities. Previously, it has been shown that glassy aqueous citric acid aerosol is able to nucleate ice heterogeneously under conditions relevant to cirrus in the tropical tropopause layer (TTL. In this study we test if glassy aerosol distributions with a range of chemical compositions heterogeneously nucleate ice under cirrus conditions. Three single component aqueous solution aerosols (raffinose, 4-hydroxy-3-methoxy-DL-mandelic acid (HMMA and levoglucosan and one multi component aqueous solution aerosol (raffinose mixed with five dicarboxylic acids and ammonium sulphate were studied in both the liquid and glassy states at a large cloud simulation chamber. The investigated organic compounds have similar functionality to oxidised organic material found in atmospheric aerosol and have estimated temperature/humidity induced glass transition thresholds that fall within the range predicted for atmospheric SOA. A small fraction of aerosol particles of all compositions were found to nucleate ice heterogeneously in the deposition mode at temperatures relevant to the TTL (<200 K. Raffinose and HMMA, which form glasses at higher temperatures, nucleated ice heterogeneously at temperatures as high as 214.6 and 218.5 K respectively. We present the calculated ice active surface site density, ns, of the aerosols tested here and also of glassy citric acid aerosol as a function of relative humidity with respect to ice (RHi. We also propose a parameterisation which can be used to estimate heterogeneous ice nucleation by glassy aerosol for use in cirrus cloud models up to ~220 K. Finally, we show that heterogeneous nucleation by glassy aerosol may compete with ice nucleation on mineral dust particles in mid-latitudes cirrus.
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Nonthermal ice nucleation observed at distorted contact lines of supercooled water drops.
Yang, Fan; Cruikshank, Owen; He, Weilue; Kostinski, Alex; Shaw, Raymond A
2018-02-01
Ice nucleation is the crucial step for ice formation in atmospheric clouds and therefore underlies climatologically relevant precipitation and radiative properties. Progress has been made in understanding the roles of temperature, supersaturation, and material properties, but an explanation for the efficient ice nucleation occurring when a particle contacts a supercooled water drop has been elusive for over half a century. Here, we explore ice nucleation initiated at constant temperature and observe that mechanical agitation induces freezing of supercooled water drops at distorted contact lines. Results show that symmetric motion of supercooled water on a vertically oscillating substrate does not freeze, no matter how we agitate it. However, when the moving contact line is distorted with the help of trace amounts of oil or inhomogeneous pinning on the substrate, freezing can occur at temperatures much higher than in a static droplet, equivalent to ∼10^{10} increase in nucleation rate. Several possible mechanisms are proposed to explain the observations. One plausible explanation among them, decreased pressure due to interface curvature, is explored theoretically and compared with the observational results quasiquantitatively. Indeed, the observed freezing-temperature increase scales with contact line speed in a manner consistent with the pressure hypothesis. Whatever the mechanism, the experiments demonstrate a strong preference for ice nucleation at three-phase contact lines compared to the two-phase interface, and they also show that movement and distortion of the contact line are necessary contributions to stimulating the nucleation process.
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Small particles big effect? - Investigating ice nucleation abilities of soot particles
Mahrt, Fabian; David, Robert O.; Lohmann, Ulrike; Stopford, Chris; Wu, Zhijun; Kanji, Zamin A.
2017-04-01
Atmospheric soot particles are primary particles produced by incomplete combustion of biomass and/or fossil fuels. Thus soot mainly originates from anthropogenic emissions, stemming from combustion related processes in transport vehicles, industrial and residential uses. Such soot particles are generally complex mixtures of black carbon (BC) and organic matter (OM) (Bond et al., 2013; Petzold et al., 2013), depending on the sources and the interaction of the primary particles with other atmospheric matter and/or gases BC absorbs solar radiation having a warming effect on global climate. It can also act as a heterogeneous ice nucleating particle (INP) and thus impact cloud-radiation interactions, potentially cooling the climate (Lohmann, 2002). Previous studies, however, have shown conflicting results concerning the ice nucleation ability of soot, limiting the ability to predict its effects on Earth's radiation budget. Here we present a laboratory study where we systematically investigate the ice nucleation behavior of different soot particles. Commercial soot samples are used, including an amorphous, industrial carbon frequently used in coatings and coloring (FW 200, Orion Engineered Carbons) and a fullerene soot (572497 ALDRICH), e.g. used as catalyst. In addition, we use soot generated from a propane flame Combustion Aerosol Standard Generator (miniCAST, JING AG), as a proxy for atmospheric soot particles. The ice nucleation ability of these soot types is tested on size-selected particles for a wide temperature range from 253 K to 218 K, using the Horizontal Ice Nucleation Chamber (HINC), a Continuous Flow Diffusion Chamber (CFDC) (Kanji and Abbatt, 2009). Ice nucleation results from these soot surrogates will be compared to chemically more complex real world samples, collected on filters. Filters will be collected during the 2016/2017 winter haze periods in Beijing, China and represent atmospheric soot particles with sources from both industrial and residential
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Sullivan, Sylvia C.; Betancourt, Ricardo Morales; Barahona, Donifan; Nenes, Athanasios
2016-01-01
Along with minimizing parameter uncertainty, understanding the cause of temporal and spatial variability of the nucleated ice crystal number, Ni, is key to improving the representation of cirrus clouds in climate models. To this end, sensitivities of Ni to input variables like aerosol number and diameter provide valuable information about nucleation regime and efficiency for a given model formulation. Here we use the adjoint model of the adjoint of a cirrus formation parameterization (Barahona and Nenes, 2009b) to understand Ni variability for various ice-nucleating particle (INP) spectra. Inputs are generated with the Community Atmosphere Model version 5, and simulations are done with a theoretically derived spectrum, an empirical lab-based spectrum and two field-based empirical spectra that differ in the nucleation threshold for black carbon particles and in the active site density for dust. The magnitude and sign of Ni sensitivity to insoluble aerosol number can be directly linked to nucleation regime and efficiency of various INP. The lab-based spectrum calculates much higher INP efficiencies than field-based ones, which reveals a disparity in aerosol surface properties. Ni sensitivity to temperature tends to be low, due to the compensating effects of temperature on INP spectrum parameters; this low temperature sensitivity regime has been experimentally reported before but never deconstructed as done here.
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Identification & Characterization of Fungal Ice Nucleation Proteins
Scheel, Jan Frederik; Kunert, Anna Theresa; Kampf, Christopher Johannes; Mauri, Sergio; Weidner, Tobias; Pöschl, Ulrich; Fröhlich-Nowoisky, Janine
2016-04-01
Freezing of water at relatively warm subfreezing temperatures is dependent on ice nucleation catalysis facilitated by ice nuclei (IN). These IN can be of various origins and although extensive research was done and progress was achieved, the nature and mechanisms leading to an effective IN are to date still poorly understood. Some of the most important processes of our geosphere like the water cycle are highly dependent on effective ice nucleation at temperatures between -2°C - -8°C, a temperature range which is almost exclusively covered by biological IN (BioIN). BioIN are usually macromolecular structures of biological polymers. Sugars as well as proteins have been reported to serve as IN and the best characterized BioIN are ice nucleation proteins (IN-P) from gram negative bacteria. Fungal strains from Fusarium spp. were described to be effective IN at subfreezing temperatures up to -2°C already 25 years ago and more and more fungal species are described to serve as efficient IN. Fungal IN are also thought to be proteins or at least contain a proteinaceous compound, but to date the fungal IN-P primary structure as well as their coding genetic elements of all IN active fungi are unknown. The aim of this study is a.) to identify the proteins and their coding genetic elements from IN active fungi (F. acuminatum, F. avenaceum, M. alpina) and b.) to characterize the mechanisms by which fungal IN serve as effective IN. We designed an interdisciplinary approach using biological, analytical and physical methods to identify fungal IN-P and describe their biological, chemical, and physical properties.
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Functional display of ice nucleation protein InaZ on the surface of bacterial ghosts.
Kassmannhuber, Johannes; Rauscher, Mascha; Schöner, Lea; Witte, Angela; Lubitz, Werner
2017-09-03
In a concept study the ability to induce heterogeneous ice formation by Bacterial Ghosts (BGs) from Escherichia coli carrying ice nucleation protein InaZ from Pseudomonas syringae in their outer membrane was investigated by a droplet-freezing assay of ultra-pure water. As determined by the median freezing temperature and cumulative ice nucleation spectra it could be demonstrated that both the living recombinant E. coli and their corresponding BGs functionally display InaZ on their surface. Under the production conditions chosen both samples belong to type II ice-nucleation particles inducing ice formation at a temperature range of between -5.6 °C and -6.7 °C, respectively. One advantage for the application of such BGs over their living recombinant mother bacteria is that they are non-living native cell envelopes retaining the biophysical properties of ice nucleation and do no longer represent genetically modified organisms (GMOs).
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Ice nucleation active particles are efficiently removed by precipitating clouds
Emiliano Stopelli; Franz Conen; Cindy E. Morris; Erik Herrmann; Nicolas Bukowiecki; Christine Alewell
2015-01-01
Ice nucleation in cold clouds is a decisive step in the formation of rain and snow. Observations and modelling suggest that variations in the concentrations of ice nucleating particles (INPs) affect timing, location and amount of precipitation. A quantitative description of the abundance and variability of INPs is crucial to assess and predict their influence on precipitation. Here we used the hydrological indicator δ(18)O to derive the fraction of water vapour lost from precipitating clouds ...
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Effect of photochemical ageing on the ice nucleation properties of diesel and wood burning particles
Directory of Open Access Journals (Sweden)
C. Chou
2013-01-01
Full Text Available A measurement campaign (IMBALANCE conducted in 2009 was aimed at characterizing the physical and chemical properties of freshly emitted and photochemically aged combustion particles emitted from a log wood burner and diesel vehicles: a EURO3 Opel Astra with a diesel oxidation catalyst (DOC but no particle filter and a EURO2 Volkswagen Transporter TDI Syncro without emission aftertreatment. Ice nucleation experiments in the deposition and condensation freezing modes were conducted with the Portable Ice Nucleation Chamber (PINC at three nominal temperatures, −30 °C, −35 °C and −40 °C. Freshly emitted diesel particles showed ice formation only at −40 °C in the deposition mode at 137% relative humidity with respect to ice (RHi and 92% relative humidity with respect to water (RHw, and photochemical ageing did not play a role in modifying their ice nucleation behaviour. Only one diesel experiment where α-pinene was added for the ageing process, showed an ice nucleation enhancement at −35 °C. Wood burning particles also act as ice nuclei (IN at −40 °C in the deposition mode at the same conditions as for diesel particles and photochemical ageing also did not alter the ice formation properties of the wood burning particles. Unlike diesel particles, wood burning particles form ice via condensation freezing at −35 °C whereas no ice nucleation was observed at −30 °C. Photochemical ageing did not affect the ice nucleation ability of the diesel and wood burning particles at the three different temperatures investigated but a broader range of temperatures below −40 °C need to be investigated in order to draw an overall conclusion on the effect of photochemical ageing on deposition/condensation ice nucleation across the entire temperature range relevant to cold clouds.
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How important is biological ice nucleation in clouds on a global scale?
International Nuclear Information System (INIS)
Hoose, C; Kristjansson, J E; Burrows, S M
2010-01-01
The high ice nucleating ability of some biological particles has led to speculations about living and dead organisms being involved in cloud ice and precipitation formation, exerting a possibly significant influence on weather and climate. In the present study, the role of primary biological aerosol particles (PBAPs) as heterogeneous ice nuclei is investigated with a global model. Emission parametrizations for bacteria, fungal spores and pollen based on recent literature are introduced, as well as an immersion freezing parametrization based on classical nucleation theory and laboratory measurements. The simulated contribution of PBAPs to the global average ice nucleation rate is only 10 -5 %, with an uppermost estimate of 0.6%. At the same time, observed PBAP concentrations in air and biological ice nucleus concentrations in snow are reasonably well captured by the model. This implies that 'bioprecipitation' processes (snow and rain initiated by PBAPs) are of minor importance on the global scale.
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Pummer, B. G.; Atanasova, L.; Bauer, H.; Bernardi, J.; Druzhinina, I. S.; Fröhlich-Nowoisky, J.; Grothe, H.
2013-12-01
Fungal spores are ubiquitous biological aerosols, which are considered to act as ice nuclei. In this study the ice nucleation (IN) activity of spores harvested from 29 fungal strains belonging to 21 different species was tested in the immersion freezing mode by microscopic observation of water-in-oil emulsions. Spores of 8 of these strains were also investigated in a microdroplet freezing array instrument. The focus was laid on species of economical, ecological or sanitary significance. Besides common molds (Ascomycota), some representatives of the widespread group of mushrooms (Basidiomycota) were also investigated. Fusarium avenaceum was the only sample showing IN activity at relatively high temperatures (about 264 K), while the other investigated fungal spores showed no freezing above 248 K. Many of the samples indeed froze at homogeneous ice nucleation temperatures (about 237 K). In combination with other studies, this suggests that only a limited number of species may act as atmospheric ice nuclei. This would be analogous to what is already known for the bacterial ice nuclei. Apart from that, we selected a set of fungal strains from different sites and exposed them to occasional freezing stress during their cultivation. This was in order to test if the exposure to a cold environment encourages the expression of ice nuclei during growth as a way of adaptation. Although the total protein expression was altered by this treatment, it had no significant impact on the IN activity.
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Ice nucleation properties of fine ash particles from the Eyjafjallajökull eruption in April 2010
Directory of Open Access Journals (Sweden)
I. Steinke
2011-12-01
Full Text Available 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
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Hiron, T.; Hoffmann, N.; Peckhaus, A.; Kiselev, A. A.; Leisner, T.; Flossmann, A. I.
2016-12-01
One of the main challenges in understanding the evolution of Earth's climate resides in the understanding the role of ice nucleation on the development of tropospheric clouds as well as its initiation. K-feldspar is known to be a very active ice nucleating particle and this study focuses on the characterization of its activity in two heterogeneous nucleation modes, immersion and deposition freezing.We use a newly built humidity-controlled cold stage allowing the simultaneous observation of up to 2000 identical 0.6-nanoliter droplets containing suspension of mineral dust particles. The droplets are first cooled down to observe immersion freezing, the obtained ice crystals are then evaporated and finally, the residual particles are exposed to the water vapor supersaturated with respect to ice.The ice nucleation abilities for the individual residual particles are then compared for the different freezing modes and correlation between immersion ice nuclei and deposition ice nuclei is investigated.Based on the electron microscopy analysis of the residual particles, we discuss the possible relationship between the ice nucleation properties of feldspar and its microstructure. Finally, we discuss the atmospheric implications of our experimental results, using DESCAM, a 1.5D bin-resolved microphysics model.
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Heterogeneous Ice Nucleation by Soufriere Hills Volcanic Ash Immersed in Water Droplets.
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T P Mangan
Full Text Available Fine particles of ash emitted during volcanic eruptions may sporadically influence cloud properties on a regional or global scale as well as influencing the dynamics of volcanic clouds and the subsequent dispersion of volcanic aerosol and gases. It has been shown that volcanic ash can trigger ice nucleation, but ash from relatively few volcanoes has been studied for its ice nucleating ability. In this study we quantify the efficiency with which ash from the Soufriere Hills volcano on Montserrat nucleates ice when immersed in supercooled water droplets. Using an ash sample from the 11th February 2010 eruption, we report ice nucleating efficiencies from 246 to 265 K. This wide range of temperatures was achieved using two separate droplet freezing instruments, one employing nanolitre droplets, the other using microlitre droplets. Soufriere Hills volcanic ash was significantly more efficient than all other ash samples that have been previously examined. At present the reasons for these differences are not understood, but may be related to mineralogy, amorphous content and surface chemistry.
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Heterogeneous Ice Nucleation by Soufriere Hills Volcanic Ash Immersed in Water Droplets.
Mangan, T P; Atkinson, J D; Neuberg, J W; O'Sullivan, D; Wilson, T W; Whale, T F; Neve, L; Umo, N S; Malkin, T L; Murray, B J
2017-01-01
Fine particles of ash emitted during volcanic eruptions may sporadically influence cloud properties on a regional or global scale as well as influencing the dynamics of volcanic clouds and the subsequent dispersion of volcanic aerosol and gases. It has been shown that volcanic ash can trigger ice nucleation, but ash from relatively few volcanoes has been studied for its ice nucleating ability. In this study we quantify the efficiency with which ash from the Soufriere Hills volcano on Montserrat nucleates ice when immersed in supercooled water droplets. Using an ash sample from the 11th February 2010 eruption, we report ice nucleating efficiencies from 246 to 265 K. This wide range of temperatures was achieved using two separate droplet freezing instruments, one employing nanolitre droplets, the other using microlitre droplets. Soufriere Hills volcanic ash was significantly more efficient than all other ash samples that have been previously examined. At present the reasons for these differences are not understood, but may be related to mineralogy, amorphous content and surface chemistry.
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Homogeneous nucleation, growth and recrystallization of discharge products on electrodes
Energy Technology Data Exchange (ETDEWEB)
Kappus, W.
1983-11-01
The early stage of discharge of electrodes with an electrodissolution/precipitation mechanism is investigated. A theory is proposed for quasi-classical homogeneous nucleation and the subsequent growth. Based on this theory the radii distribution function was calculated for the diffusion-controlled growth of crystallites. Recrystallization was included. The nucleation overpotential was calculated as a function of time for discharges under various conditions.
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Directory of Open Access Journals (Sweden)
C. Budke
2015-02-01
Full Text Available 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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Budke, C.; Koop, T.
2015-02-01
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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Effects of streptomycin, desiccation, and UV radiation on ice nucleation by Pseudomonas viridiflava
International Nuclear Information System (INIS)
Anderson, J.A.; Ashworth, E.N.
1986-01-01
Streptomycin (100 micrograms per milliliter), desiccation (over CaSO 4 ), and ultraviolet radiation (4500 microwatts per square centimeter at 254 nonometers for 15 minutes) reduced ice nucleation activity by Pseudomonas viridiflava strain W-1 as determined by freezing drops of the bacterial suspensions. Highest residual ice nucleation activity by dead cells was obtained by desiccation, although no freezing above -3.5 0 C was detected. The rate and extent of loss of ice nucleation activity following streptomycin and ultraviolet treatment was affected by preconditioning temperature. At 21 0 C and above, loss of activity by dead cells was rapid and irreversible
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Screening of plant resources with anti-ice nucleation activity for frost damage prevention.
Suzuki, Shingo; Fukuda, Satoshi; Fukushi, Yukiharu; Arakawa, Keita
2017-11-01
Previous studies have shown that some polyphenols have anti-ice nucleation activity (anti-INA) against ice-nucleating bacteria that contribute to frost damage. In the present study, leaf disk freezing assay, a test of in vitro application to plant leaves, was performed for the screening of anti-INA, which inhibits the ice nucleation activity of an ice-nucleating bacterium Erwinia ananas in water droplets on the leaf surfaces. The application of polyphenols with anti-INA, kaempferol 7-O-β-glucoside and (-)-epigallocatechin gallate, to the leaf disk freezing assay by cooling at -4--6 °C for 3 h, revealed that both the compounds showed anti-INAs against E. ananas in water droplets on the leaf surfaces. Further, this assay also revealed that the extracts of five plant leaves showed high anti-INA against E. ananas in water droplets on leaf surfaces, indicating that they are the candidate resources to protect crops from frost damage.
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Homogeneous Nucleation Rate Measurements in Supersaturated Water Vapor
Czech Academy of Sciences Publication Activity Database
Brus, David; Ždímal, Vladimír; Smolík, Jiří
2008-01-01
Roč. 129, č. 17 (2008), , 174501-1-174501-8 ISSN 0021-9606 R&D Projects: GA ČR GA101/05/2214 Institutional research plan: CEZ:AV0Z40720504 Keywords : homogeneous nucleation * water * diffusion chamber Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 3.149, year: 2008
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Investigation of nucleation processes during dynamic recrystallization of ice using cryo-EBSD.
Chauve, T; Montagnat, M; Barou, F; Hidas, K; Tommasi, A; Mainprice, D
2017-02-13
Nucleation mechanisms occurring during dynamic recrystallization play a crucial role in the evolution of microstructures and textures during high temperature deformation. In polycrystalline ice, the strong viscoplastic anisotropy induces high strain heterogeneities between grains which control the recrystallization mechanisms. Here, we study the nucleation mechanisms occurring during creep tests performed on polycrystalline columnar ice at high temperature and stress (T=-5°C;σ=0.5 MPa) by post-mortem analyses of deformation microstructures using cryogenic electron backscatter diffraction. The columnar geometry of the samples enables discrimination of the nuclei from the initial grains. Various nucleation mechanisms are deduced from the analysis of the nuclei relations with the dislocation sub-structures within grains and at grain boundaries. Tilt sub-grain boundaries and kink bands are the main structures responsible for development of polygonization and mosaic sub-structures. Nucleation by bulging at serrated grain boundaries is also an efficient nucleation mechanism near the grain boundaries where strain incompatibilities are high. Observation of nuclei with orientations not related to the 'parent' ones suggests the possibility of 'spontaneous' nucleation driven by the relaxation of the dislocation-related internal stress field. The complexity of the nucleation mechanisms observed here emphasizes the impact of stress and strain heterogeneities on dynamic recrystallization mechanisms.This article is part of the themed issue 'Microdynamics of ice'. © 2016 The Author(s).
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Ice nucleating particles in the Saharan Air Layer
Directory of Open Access Journals (Sweden)
Y. Boose
2016-07-01
Full Text Available This study aims at quantifying the ice nucleation properties of desert dust in the Saharan Air Layer (SAL, the warm, dry and dust-laden layer that expands from North Africa to the Americas. By measuring close to the dust's emission source, before aging processes during the transatlantic advection potentially modify the dust properties, the study fills a gap between in situ measurements of dust ice nucleating particles (INPs far away from the Sahara and laboratory studies of ground-collected soil. Two months of online INP concentration measurements are presented, which were part of the two CALIMA campaigns at the Izaña observatory in Tenerife, Spain (2373 m a.s.l., in the summers of 2013 and 2014. INP concentrations were measured in the deposition and condensation mode at temperatures between 233 and 253 K with the Portable Ice Nucleation Chamber (PINC. Additional aerosol information such as bulk chemical composition, concentration of fluorescent biological particles as well as the particle size distribution was used to investigate observed variations in the INP concentration. The concentration of INPs was found to range between 0.2 std L−1 in the deposition mode and up to 2500 std L−1 in the condensation mode at 240 K. It correlates well with the abundance of aluminum, iron, magnesium and manganese (R: 0.43–0.67 and less with that of calcium, sodium or carbonate. These observations are consistent with earlier results from laboratory studies which showed a higher ice nucleation efficiency of certain feldspar and clay minerals compared to other types of mineral dust. We find that an increase of ammonium sulfate, linked to anthropogenic emissions in upwind distant anthropogenic sources, mixed with the desert dust has a small positive effect on the condensation mode INP per dust mass ratio but no effect on the deposition mode INP. Furthermore, the relative abundance of biological particles was found to be significantly higher
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Bodzewski, Kentaro Y.; Caylor, Ryan L.; Comstock, Ashley M.; Hadley, Austin T.; Imholt, Felisha M.; Kirwan, Kory D.; Oyama, Kira S.; Wise, Matthew E.
2016-01-01
A differential scanning calorimeter was used to study homogeneous nucleation of ice from micron-sized aqueous ammonium sulfate aerosol particles. It is important to understand the conditions at which these particles nucleate ice because of their connection to cirrus cloud formation. Additionally, the concept of freezing point depression, a topic…
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The ice nucleation activity of extremophilic algae
Czech Academy of Sciences Publication Activity Database
Kvíderová, Jana; Hájek, J.; Worland, M. R.
2013-01-01
Roč. 34, č. 2 (2013), s. 137-148 ISSN 0143-2044 R&D Projects: GA AV ČR KJB601630808; GA AV ČR KJB600050708 Institutional support: RVO:67985939 Keywords : Ice nucleation * snow algae * lichen photobionts Subject RIV: EF - Botanics Impact factor: 0.640, year: 2013
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Directory of Open Access Journals (Sweden)
J. B. McQuaid
2009-06-01
Full Text Available A new Thermal Gradient ice nucleation Diffusion Chamber (TGDC capable of investigating ice nucleation efficiency of atmospherically important aerosols, termed Ice Nuclei (IN, has been designed, constructed and validated. The TGDC can produce a range of supersaturations with respect to ice (SSi over the temperature range of −10 to −34°C for sufficiently long time needed to observe the ice nucleation by the particles. The novel aspect of this new TGDC is that the chamber is run in static mode with aerosol particles supported on a Teflon substrate, which can be raised and lowered in a controlled way through the SSi profile within the chamber, and nucleation events are directly observed using digital photography. The TGDC consists of two ice coated plates to which a thermal gradient is applied to produce the range of SSi. The design of the TGDC gives the ability to understand time-related ice nucleation event information and to perform experiments at different temperatures and SSi conditions for different IN without changing the thermal gradient within the TGDC. The temperature and SSi conditions of the experimental system are validated by observing (NH42SO4 deliquescence and the results are in good agreement with the literature data. First results are presented of the onset ice nucleation for mineral dust sampled from the Saharan Desert, including images of nucleation and statistical distributions of onset ice nucleation SSi as a function of temperature. This paper illustrates how useful this new TGDC is for process level studies of ice nucleation and more experimental investigations are needed to better quantify the role of ice formation in the atmosphere.
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The Ice Nucleation Activity of Surface Modified Soot
Häusler, Thomas; Witek, Lorenz; Felgitsch, Laura; Hitzenberger, Regina; Grothe, Hinrich
2017-04-01
The ice nucleation efficiency of many important atmospheric particles remains poorly understood. Since soot is ubiquitous in the Earth's troposphere, they might have the potential to significantly impact the Earth's climate (Finlayson-Pitts and Pitts, 2000; Seinfeld and Pandis, 1998). Here we present the ice nucleation activity (INA) in immersion freezing mode of different types of soot. Therefor a CAST (combustion aerosol standard) generator was used to produce different kinds of soot samples. The CAST generator combusts a propane-air-mixture and deposits thereby produced soot on a polyvinyl fluoride filter. By varying the propane to air ratio, the amount of organic portion of the soot can be varied from black carbon (BC) with no organic content to brown carbon (BrC) with high organic content. To investigate the impact of functional sites of ice nuclei (IN), the soot samples were exposed to NO2 gas for a certain amount of time (30 to 360 minutes) to chemically modify the surface. Immersion freezing experiments were carried out in a unique reaction gadget. In this device a water-in-oil suspension (with the soot suspended in the aqueous phase) was cooled till the freezing point and was observed through a microscope (Pummer et al., 2012; Zolles et al., 2015) It was found that neither modified nor unmodified BC shows INA. On the contrary, unmodified BrC shows an INA at -32˚ C, which can be increased up to -20˚ C. The INA of BrC depends on the duration of NO2- exposure. To clarify the characteristics of the surface modifications, surface sensitive analysis like infrared spectroscopy and X-ray photoelectron spectroscopy were carried out. Finlayson-Pitts, B. J. and Pitts, J. N. J.: Chemistry of the Upper and Lower Atmosphere, Elsevier, New York, 2000. Pummer, B. G., Bauer, H., Bernardi, J., Bleicher, S., and Grothe, H.: Suspendable macromolecules are responsible for ice nucleation activity of birch and conifer pollen, Atmos Chem Phys, 12, 2541-2550, 2012. Seinfeld, J
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Ice nucleation of ammonia gas exposed montmorillonite mineral dust particles
Directory of Open Access Journals (Sweden)
A. Salam
2007-07-01
Full Text Available The ice nucleation characteristics of montmorillonite mineral dust aerosols with and without exposure to ammonia gas were measured at different atmospheric temperatures and relative humidities with a continuous flow diffusion chamber. The montmorillonite particles were exposed to pure (100% and diluted ammonia gas (25 ppm at room temperature in a stainless steel chamber. There was no significant change in the mineral dust particle size distribution due to the ammonia gas exposure. 100% pure ammonia gas exposure enhanced the ice nucleating fraction of montmorillonite mineral dust particles 3 to 8 times at 90% relative humidity with respect to water (RHw and 5 to 8 times at 100% RHw for 120 min exposure time compared to unexposed montmorillonite within our experimental conditions. The percentages of active ice nuclei were 2 to 8 times higher at 90% RHw and 2 to 7 times higher at 100% RHw in 25 ppm ammonia exposed montmorillonite compared to unexposed montmorillonite. All montmorillonite particles are more efficient as ice nuclei with increasing relative humidities and decreasing temperatures. The activation temperature of montmorillonite exposed to 100% pure ammonia was 15°C higher than for unexposed montmorillonite particles at 90% RHw. In the 25 ppm ammonia exposed montmorillonite experiments, the activation temperature was 10°C warmer than unexposed montmorillonite at 90% RHw. Degassing does not reverse the ice nucleating ability of ammonia exposed montmorillonite mineral dust particles suggesting that the ammonia is chemically bound to the montmorillonite particle. This is the first experimental evidence that ammonia gas exposed montmorillonite mineral dust particles can enhance its activation as ice nuclei and that the activation can occur at temperatures warmer than –10°C where natural atmospheric ice nuclei are very scarce.
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Ebert, Martin; Worringen, Annette; Kandler, Konrad; Weinbruch, Stephan; Schenk, Ludwig; Mertes, Stephan; Schmidt, Susan; Schneider, Johannes; Frank, Fabian; Nilius, Björn; Danielczok, Anja; Bingemer, Heinz
2014-05-01
An intense field campaign from the Ice Nuclei Research Unit (INUIT) was performed in January and February of 2013 at the High-Alpine Research Station Jungfraujoch (3580 m a.s.l., Switzerland). Main goal was the assessment of microphysical and chemical properties of free-tropospheric ice-nucelating particles. The ice-nucleating particles were discriminated from the total aerosol with the 'Fast Ice Nucleation CHamber' (FINCH; University Frankfurt) and the 'Ice-Selective Inlet' (ISI, Paul Scherer Institute) followed by a pumped counter-stream virtual impactor. The separated ice-nucleating particles were then collected with a nozzle-type impactor. With the 'FRankfurt Ice nuclei Deposition freezinG Experiment' (FRIDGE), aerosol particles are sampled on a silicon wafer, which is than exposed to ice-activating conditions in a static diffusion chamber. The locations of the growing ice crystals are recorded for later analysis. Finally, with the ICE Counter-stream Virtual Impactor (ICE-CVI) atmospheric ice crystals are separated from the total aerosol and their water content is evaporated to retain the ice residual particles, which are then collected also by impactor sampling. All samples were analyzed in a high-resolution scanning electron microscope. By this method, for each particle its size, morphology, mixing-state and chemical composition is obtained. In total approximately 1700 ice nucleating particles were analyzed. Based on their chemical composition, the particles were classified into seven groups: silicates, metal oxides, Ca-rich particles, (aged) sea-salt, soot, sulphates and carbonaceous matter. Sea-salt is considered as artifact and is not regarded as ice nuclei here. The most frequent ice nucleating particles/ice residuals at the Jungfraujoch station are silicates > carbonaceous particles > metal oxides. Calcium-rich particles and soot play a minor role. Similar results are obtained by quasi-parallel measurements with an online single particle laser ablation
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Directory of Open Access Journals (Sweden)
Z. A. Kanji
2013-09-01
Full Text Available Ice nucleation in the atmosphere is central to the understanding the microphysical properties of mixed-phase and cirrus clouds. Ambient conditions such as temperature (T and relative humidity (RH, as well as aerosol properties such as chemical composition and mixing state play an important role in predicting ice formation in the troposphere. Previous field studies have reported the absence of sulfate and organic compounds on mineral dust ice crystal residuals sampled at mountain top stations or aircraft based measurements despite the long-range transport mineral dust is subjected to. We present laboratory studies of ice nucleation for immersion and deposition mode on ozone aged mineral dust particles for 233 T ns are reported and observed to increase as a function of decreasing temperature. We present first results that demonstrate enhancement of the ice nucleation ability of aged mineral dust particles in both the deposition and immersion mode due to ageing. We also present the first results to show a suppression of heterogeneous ice nucleation activity without the condensation of a coating of (inorganic material. In immersion mode, low ozone exposed Ka particles showed enhanced ice activity requiring a median freezing temperature of 1.5 K warmer than that of untreated Ka, whereas high ozone exposed ATD particles showed suppressed ice nucleation requiring a median freezing temperature of 3 K colder than that of untreated ATD. In deposition mode, low exposure Ka had ice active fractions of an order of magnitude higher than untreated Ka, whereas high ozone exposed ATD had ice active fractions up to a factor of 4 lower than untreated ATD. From our results, we derive and present parameterizations in terms of ns(T that can be used in models to predict ice nuclei concentrations based on available aerosol surface area.
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Homogeneous SPC/E water nucleation in large molecular dynamics simulations.
Angélil, Raymond; Diemand, Jürg; Tanaka, Kyoko K; Tanaka, Hidekazu
2015-08-14
We perform direct large molecular dynamics simulations of homogeneous SPC/E water nucleation, using up to ∼ 4 ⋅ 10(6) molecules. Our large system sizes allow us to measure extremely low and accurate nucleation rates, down to ∼ 10(19) cm(-3) s(-1), helping close the gap between experimentally measured rates ∼ 10(17) cm(-3) s(-1). We are also able to precisely measure size distributions, sticking efficiencies, cluster temperatures, and cluster internal densities. We introduce a new functional form to implement the Yasuoka-Matsumoto nucleation rate measurement technique (threshold method). Comparison to nucleation models shows that classical nucleation theory over-estimates nucleation rates by a few orders of magnitude. The semi-phenomenological nucleation model does better, under-predicting rates by at worst a factor of 24. Unlike what has been observed in Lennard-Jones simulations, post-critical clusters have temperatures consistent with the run average temperature. Also, we observe that post-critical clusters have densities very slightly higher, ∼ 5%, than bulk liquid. We re-calibrate a Hale-type J vs. S scaling relation using both experimental and simulation data, finding remarkable consistency in over 30 orders of magnitude in the nucleation rate range and 180 K in the temperature range.
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The influence of organic-containing soil dust on ice nucleation and cloud properties
Hummel, Matthias; Grini, Alf; Berntsen, Terje K.; Ekman, Annica
2017-04-01
Natural mineral dust from desert regions is known to be the most important contributor to atmospheric ice-nucleating particles (INP) which induce heterogeneous ice nucleation in mixed-phase clouds. Its ability to nucleate ice effectively is shown by various laboratory (Hoose and Möhler 2012) and field results (DeMott et al. 2015) and its abundance in ice crystal residuals has also been shown (Cziczo et al. 2013). Thus it is an important player when representing mixed-phase clouds in climate models. MODIS satellite data indicate that 1 /4 of the global dust emission originates from semi-arid areas rather than from arid deserts (Ginoux et al. 2012). Here, organic components can mix with minerals within the soil and get into the atmosphere. These so-called 'soil dust' particles are ice-nucleating active at high sub-zero temperatures, i.e. at higher temperatures than pure desert dust (Steinke et al. 2016). In this study, soil dust is incorporated into the Norwegian Earth System Model (NorESM, Bentsen et al. 2013) and applied to a modified ice nucleation parameterization (Steinke et al. 2016). Its influence on the cloud ice phase is evaluated by comparing a control run, where only pure desert dust is considered, and a sensitivity experiment, where a fraction of the dust emissions are classified as soil dust. Both simulations are nudged to ERA-interim meteorology and they have the same loading of dust emissions. NorESM gives a lower annual soil dust emission flux compared to Ginoux et al. (2012), but the desert dust flux is similar to the MODIS-retrieved data. Although soil dust concentrations are much lower than desert dust, the NorESM simulations indicate that the annual INP concentrations from soil dust are on average lower by a just a factor of 4 than INP concentrations from pure desert dust. The highest soil dust INP concentrations occur at a lower height than for desert dust, i.e at warmer temperatures inside mixed-phase clouds. Furthermore, soil dust INP
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Analysis of the Effect of Water Activity on Ice Formation Using a New Theory of Nucleation
Barahona, Donifan
2013-01-01
In this work a new theory of nucleation is developed and used to investigate the effect of water activity on the formation of ice within super-cooled droplets. The new theory is based on a novel concept where the interface is assumed to be made of liquid molecules trapped by the solid matrix. Using this concept new expressions are developed for the critical ice germ size and the nucleation work, with explicit dependencies on temperature and water activity. However unlike previous approaches, the new theory does not depend on the interfacial tension between liquid and ice. Comparison against experimental results shows that the new theory is able to reproduce the observed effect of water activity on nucleation rate and freezing temperature. It allows for the first time a theoretical derivation of the constant shift in water activity between melting and nucleation. The new theory offers a consistent thermodynamic view of ice nucleation, simple enough to be applied in atmospheric models of cloud formation.
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Laboratory measurements and model sensitivity studies of dust deposition ice nucleation
Directory of Open Access Journals (Sweden)
G. Kulkarni
2012-08-01
Full Text Available We investigated the ice nucleating properties of mineral dust particles to understand the sensitivity of simulated cloud properties to two different representations of contact angle in the Classical Nucleation Theory (CNT. These contact angle representations are based on two sets of laboratory deposition ice nucleation measurements: Arizona Test Dust (ATD particles of 100, 300 and 500 nm sizes were tested at three different temperatures (−25, −30 and −35 °C, and 400 nm ATD and kaolinite dust species were tested at two different temperatures (−30 and −35 °C. These measurements were used to derive the onset relative humidity with respect to ice (RHice required to activate 1% of dust particles as ice nuclei, from which the onset single contact angles were then calculated based on CNT. For the probability density function (PDF representation, parameters of the log-normal contact angle distribution were determined by fitting CNT-predicted activated fraction to the measurements at different RHice. Results show that onset single contact angles vary from ~18 to 24 degrees, while the PDF parameters are sensitive to the measurement conditions (i.e. temperature and dust size. Cloud modeling simulations were performed to understand the sensitivity of cloud properties (i.e. ice number concentration, ice water content, and cloud initiation times to the representation of contact angle and PDF distribution parameters. The model simulations show that cloud properties are sensitive to onset single contact angles and PDF distribution parameters. The comparison of our experimental results with other studies shows that under similar measurement conditions the onset single contact angles are consistent within ±2.0 degrees, while our derived PDF parameters have larger discrepancies.
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Single-particle levitation system for automated study of homogeneous solute nucleation
Olsen, Adam P.; Flagan, Richard C.; Kornfield, Julia A.
2006-01-01
We present an instrument that addresses two critical requirements for quantitative measurements of the homogeneous crystal nucleation rate in supersaturated aqueous solution. First, the need to perform repeated measurements of nucleation incubation times is met by automating experiments to enable programmable cycling of thermodynamic conditions. Second, the need for precise and robust control of the chemical potential in supersaturated aqueous solution is met by implementing a novel technique...
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Directory of Open Access Journals (Sweden)
R. Wagner
2010-08-01
Full Text Available The heterogeneous ice nucleation potential of airborne oxalic acid dihydrate and sodium oxalate particles in the deposition and condensation mode has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 244 and 228 K. Previous laboratory studies have highlighted the particular role of oxalic acid dihydrate as the only species amongst a variety of other investigated dicarboxylic acids to be capable of acting as a heterogeneous ice nucleus in both the deposition and immersion mode. We could confirm a high deposition mode ice activity for 0.03 to 0.8 μm sized oxalic acid dihydrate particles that were either formed by nucleation from a gaseous oxalic acid/air mixture or by rapid crystallisation of highly supersaturated aqueous oxalic acid solution droplets. The critical saturation ratio with respect to ice required for deposition nucleation was found to be less than 1.1 and the size-dependent ice-active fraction of the aerosol population was in the range from 0.1 to 22%. In contrast, oxalic acid dihydrate particles that had crystallised from less supersaturated solution droplets and had been allowed to slowly grow in a supersaturated environment from still unfrozen oxalic acid solution droplets over a time period of several hours were found to be much poorer heterogeneous ice nuclei. We speculate that under these conditions a crystal surface structure with less-active sites for the initiation of ice nucleation was generated. Such particles partially proved to be almost ice-inactive in both the deposition and condensation mode. At times, the heterogeneous ice nucleation ability of oxalic acid dihydrate significantly changed when the particles had been processed in preceding cloud droplet activation steps. Such behaviour was also observed for the second investigated species, namely sodium oxalate. Our experiments address the atmospheric scenario
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Wagner, R.; Möhler, O.; Saathoff, H.; Schnaiter, M.; Leisner, T.
2010-08-01
The heterogeneous ice nucleation potential of airborne oxalic acid dihydrate and sodium oxalate particles in the deposition and condensation mode has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 244 and 228 K. Previous laboratory studies have highlighted the particular role of oxalic acid dihydrate as the only species amongst a variety of other investigated dicarboxylic acids to be capable of acting as a heterogeneous ice nucleus in both the deposition and immersion mode. We could confirm a high deposition mode ice activity for 0.03 to 0.8 μm sized oxalic acid dihydrate particles that were either formed by nucleation from a gaseous oxalic acid/air mixture or by rapid crystallisation of highly supersaturated aqueous oxalic acid solution droplets. The critical saturation ratio with respect to ice required for deposition nucleation was found to be less than 1.1 and the size-dependent ice-active fraction of the aerosol population was in the range from 0.1 to 22%. In contrast, oxalic acid dihydrate particles that had crystallised from less supersaturated solution droplets and had been allowed to slowly grow in a supersaturated environment from still unfrozen oxalic acid solution droplets over a time period of several hours were found to be much poorer heterogeneous ice nuclei. We speculate that under these conditions a crystal surface structure with less-active sites for the initiation of ice nucleation was generated. Such particles partially proved to be almost ice-inactive in both the deposition and condensation mode. At times, the heterogeneous ice nucleation ability of oxalic acid dihydrate significantly changed when the particles had been processed in preceding cloud droplet activation steps. Such behaviour was also observed for the second investigated species, namely sodium oxalate. Our experiments address the atmospheric scenario that coating layers
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Sahyoun, Maher; Korsholm, Ulrik S.; Sørensen, Jens H.; Šantl-Temkiv, Tina; Finster, Kai; Gosewinkel, Ulrich; Nielsen, Niels W.
2017-12-01
Bacterial ice-nucleating particles (INP) have the ability to facilitate ice nucleation from super-cooled cloud droplets at temperatures just below the melting point. Bacterial INP have been detected in cloud water, precipitation, and dry air, hence they may have an impact on weather and climate. In modeling studies, the potential impact of bacteria on ice nucleation and precipitation formation on global scale is still uncertain due to their small concentration compared to other types of INP, i.e. dust. Those earlier studies did not account for the yet undetected high concentration of nanoscale fragments of bacterial INP, which may be found free or attached to soil dust in the atmosphere. In this study, we investigate the sensitivity of modeled cloud ice, precipitation and global solar radiation in different weather scenarios to changes in the fraction of cloud droplets containing bacterial INP, regardless of their size. For this purpose, a module that calculates the probability of ice nucleation as a function of ice nucleation rate and bacterial INP fraction was developed and implemented in a numerical weather prediction model. The threshold value for the fraction of cloud droplets containing bacterial INP needed to produce a 1% increase in cloud ice was determined at 10-5 to 10-4. We also found that increasing this fraction causes a perturbation in the forecast, leading to significant differences in cloud ice and smaller differences in convective and total precipitation and in net solar radiation reaching the surface. These effects were most pronounced in local convective events. Our results show that bacterial INP can be considered as a trigger factor for precipitation, but not an enhancement factor.
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New species of ice nucleating fungi in soil and air
Fröhlich-Nowoisky, Janine; Hill, Thomas C. J.; Pummer, Bernhard G.; Franc, Gray D.; Pöschl, Ulrich
2014-05-01
Primary biological aerosol particles (PBAP) are ubiquitous in the atmosphere (1,2). Several types of PBAP have been identified as ice nuclei (IN) that can initiate the formation of ice at relatively high temperatures (3, 4). The best-known biological IN are common plant-associated bacteria. The IN activity of these bacteria is due to a surface protein on the outer cell membrane that catalyses ice formation, for which the corresponding gene has been identified and detected by DNA analysis (3). Fungal spores or hyphae can also act as IN, but the biological structures responsible for their IN activity have not yet been elucidated. Furthermore, the abundance, diversity, sources, seasonality, properties, and effects of fungal IN in the atmosphere have neither been characterized nor quantified. Recent studies have shown that airborne fungi are highly diverse (1), and that atmospheric transport leads to efficient exchange of species among different ecosystems (5, 6). The results presented in Fröhlich-Nowoisky et al. 2012 (7) clearly demonstrate the presence of geographic boundaries in the global distribution of microbial taxa in air, and indicate that regional differences may be important for the effects of microorganisms on climate and public health. DNA analyses of aerosol samples collected during rain events showed higher diversity and frequency of occurrence for fungi belonging to the Sordariomycetes, than samples that were collected under dry conditions (8). Sordariomycetes is the class that comprises known ice nucleation active species (Fusarium spp.). By determination of freezing ability of fungal colonies isolated from air samples two species of ice nucleation active fungi that were not previously known as biological ice nucleators were found. By DNA-analysis they were identified as Isaria farinosa and Acremonium implicatum. Both fungi belong to the phylum Ascomycota, produce fluorescent spores in the range of 1-4 µm in diameter, and induced freezing at -4 and
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Directory of Open Access Journals (Sweden)
S. Unterstrasser
2010-02-01
Full Text Available Simulations of contrail-to-cirrus transition were performed with an LES model. In Part 1 the impact of relative humidity, temperature and vertical wind shear was explored in a detailed parametric study. Here, we study atmospheric parameters like stratification and depth of the supersaturated layer and processes which may affect the contrail evolution. We consider contrails in various radiation scenarios herein defined by the season, time of day and the presence of lower-level cloudiness which controls the radiance incident on the contrail layer. Under suitable conditions, controlled by the radiation scenario and stratification, radiative heating lifts the contrail-cirrus and prolongs its lifetime. The potential of contrail-driven secondary nucleation is investigated. We consider homogeneous nucleation and heterogeneous nucleation of preactivated soot cores released from sublimated contrail ice crystals. In our model the contrail dynamics triggered by radiative heating does not suffice to force homogeneous freezing of ambient liquid aerosol particles. Furthermore, our model results suggest that heterogeneous nucleation of preactivated soot cores is unimportant. Contrail evolution is not controlled by the depth of the supersaturated layer as long as it exceeds roughly 500 m. Deep fallstreaks however need thicker layers. A variation of the initial ice crystal number is effective during the whole evolution of a contrail. A cut of the soot particle emission by two orders of magnitude can reduce the contrail timescale by one hour and the optical thickness by a factor of 5. Hence future engines with lower soot particle emissions could potentially lead to a reduction of the climate impact of aviation.
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Inhibition of ice crystallisation in highly viscous aqueous organic acid droplets
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B. J. Murray
2008-09-01
Full Text Available Homogeneous nucleation of ice within aqueous solution droplets and their subsequent crystallisation is thought to play a significant role in upper tropospheric ice cloud formation. It is normally assumed that homogeneous nucleation will take place at a threshold supersaturation, irrespective of the identity of the solute, and that rapid growth of ice particles will follow immediately after nucleation. However, it is shown here through laboratory experiments that droplets may not readily freeze in the very cold tropical tropopause layer (TTL, typical temperatures of 186–200 K. In these experiments ice crystal growth in citric acid solution droplets did not occur when ice nucleated below 197±6 K. Citric acid, 2-hydroxypropane-1,2,3-tricarboxyllic acid, is a molecule with similar functionality to oxygenated organic compounds which are ubiquitous in atmospheric aerosol. It is therefore thought to be a sensible proxy for atmospheric organic material. Evidence is presented that suggests citric acid solution droplets become ultra-viscous and form glassy solids under atmospherically relevant conditions. Diffusion of liquid water molecules to ice nuclei is expected to be very slow in ultra-viscous solution droplets and nucleation is negligible in glassy droplets; this most likely provides an explanation for the experimentally observed inhibition of ice crystallisation. The implications of ultra-viscous and glassy solution droplets for ice cloud formation and supersaturations in the TTL are discussed.
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High-density amorphous ice: nucleation of nanosized low-density amorphous ice
Tonauer, Christina M.; Seidl-Nigsch, Markus; Loerting, Thomas
2018-01-01
The pressure dependence of the crystallization temperature of different forms of expanded high-density amorphous ice (eHDA) was scrutinized. Crystallization at pressures 0.05-0.30 GPa was followed using volumetry and powder x-ray diffraction. eHDA samples were prepared via isothermal decompression of very high-density amorphous ice at 140 K to different end pressures between 0.07-0.30 GPa (eHDA0.07-0.3). At 0.05-0.17 GPa the crystallization line T x (p) of all eHDA variants is the same. At pressures >0.17 GPa, all eHDA samples decompressed to pressures <0.20 GPa exhibit significantly lower T x values than eHDA0.2 and eHDA0.3. We rationalize our findings with the presence of nanoscaled low-density amorphous ice (LDA) seeds that nucleate in eHDA when it is decompressed to pressures <0.20 GPa at 140 K. Below ~0.17 GPa, these nanosized LDA domains are latent within the HDA matrix, exhibiting no effect on T x of eHDA<0.2. Upon heating at pressures ⩾0.17 GPa, these nanosized LDA nuclei transform to ice IX nuclei. They are favored sites for crystallization and, hence, lower T x . By comparing crystallization experiments of bulk LDA with the ones involving nanosized LDA we are able to estimate the Laplace pressure and radius of ~0.3-0.8 nm for the nanodomains of LDA. The nucleation of LDA in eHDA revealed here is evidence for the first-order-like nature of the HDA → LDA transition, supporting water’s liquid-liquid transition scenarios.
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Hudait, Arpa; Molinero, Valeria
2014-06-04
Atmospheric aerosols have a strong influence on Earth's climate. Elucidating the physical state and internal structure of atmospheric aqueous aerosols is essential to predict their gas and water uptake, and the locus and rate of atmospherically important heterogeneous reactions. Ultrafine aerosols with sizes between 3 and 15 nm have been detected in large numbers in the troposphere and tropopause. Nanoscopic aerosols arising from bubble bursting of natural and artificial seawater have been identified in laboratory and field experiments. The internal structure and phase state of these aerosols, however, cannot yet be determined in experiments. Here we use molecular simulations to investigate the phase behavior and internal structure of liquid, vitrified, and crystallized water-salt ultrafine aerosols with radii from 2.5 to 9.5 nm and with up to 10% moles of ions. We find that both ice crystallization and vitrification of the nanodroplets lead to demixing of pure water from the solutions. Vitrification of aqueous nanodroplets yields nanodomains of pure low-density amorphous ice in coexistence with vitrified solute rich aqueous glass. The melting temperature of ice in the aerosols decreases monotonically with an increase of solute fraction and decrease of radius. The simulations reveal that nucleation of ice occurs homogeneously at the subsurface of the water-salt nanoparticles. Subsequent ice growth yields phase-segregated, internally mixed, aerosols with two phases in equilibrium: a concentrated water-salt amorphous mixture and a spherical cap-like ice nanophase. The surface of the crystallized aerosols is heterogeneous, with ice and solution exposed to the vapor. Free energy calculations indicate that as the concentration of salt in the particles, the advance of the crystallization, or the size of the particles increase, the stability of the spherical cap structure increases with respect to the alternative structure in which a core of ice is fully surrounded by
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Inhibition of nucleation and growth of ice by poly(vinyl alcohol) in vitrification solution.
Wang, Hai-Yan; Inada, Takaaki; Funakoshi, Kunio; Lu, Shu-Shen
2009-08-01
Control of ice formation is crucial in cryopreservation of biological substances. Successful vitrification using several additives that inhibit ice nucleation in vitrification solutions has previously been reported. Among these additives, here we focused on a synthetic polymer, poly(vinyl alcohol) (PVA), and investigated the effects of PVA on nucleation and growth of ice in 35% (w/w) aqueous 1,2-propanediol solution by using a differential scanning calorimetry (DSC) system equipped with a cryomicroscope. First, the freezing temperature of the solution was measured using the DSC system, and then the change in ice fraction in the solution during cooling was evaluated based on images obtained using the cryomicroscope, at different concentrations of PVA between 0% and 3% (w/w). Based on the ice fraction, the change in residual solution concentration during cooling was also evaluated and then plotted on the state diagram of aqueous 1,2-propanediol solution. Results indicated that, when the partially glassy and partially frozen state was intentionally allowed, the addition of PVA effectively inhibited not only ice nucleation but also ice growth in the vitrification solution. The effect of PVA on ice growth in the vitrification solution was explained based on kinetic limitations mainly due to mass transport. The interfacial kinetics also might limit ice growth in the vitrification solution only when the ice growth rate decreased below a critical value. This coincides with the fact that PVA exhibits a unique antifreeze activity in the same manner as antifreeze proteins when ice growth rate is lower than a critical value.
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Directory of Open Access Journals (Sweden)
S. Dobbie
2010-01-01
Full Text Available A newly developed ice nucleation experimental set up was used to investigate the heterogeneous ice nucleation properties of three Saharan and one Spanish dust particle samples. It was observed that the spread in the onset relative humidities with respect to ice (RHi for Saharan dust particles varied from 104% to 110%, whereas for the Spanish dust from 106% to 110%. The elemental composition analysis shows a prominent Ca feature in the Spanish dust sample which could potentially explain the differences in nucleation threshold. Although the spread in the onset RHi for the three Saharan dust samples were in agreement, the active fractions and nucleation time-lags calculated at various temperature and RHi conditions were found to differ. This could be due to the subtle variation in the elemental composition of the dust samples, and surface irregularities like steps, cracks, cavities etc. A combination of classical nucleation theory and active site theory is used to understand the importance of these surface irregularities on the nucleability parameter, contact angle that is widely used in ice cloud modeling. These calculations show that the surface irregularities can reduce the contact angle by approximately 10 degrees.
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Engineering functional nanothin multilayers on food packaging: ice-nucleating polyethylene films.
Gezgin, Zafer; Lee, Tung-Ching; Huang, Qingrong
2013-05-29
Polyethylene is the most prevalent plastic and is commonly used as a packaging material. Despite its common use, there are not many studies on imparting functionalities to those films which can make them more desirable for frozen food packaging. Here, commercial low-density polyethylene (LDPE) films were oxidized by UV-ozone (UVO) treatment to obtain a negatively charged hydrophilic surface to allow fabrication of functional multilayers. An increase in hydrophilicity was observed when films were exposed to UVO for 4 min and longer. Thin multilayers were formed by dipping the UVO-treated films into biopolymer solutions, and extracellular ice nucleators (ECINs) were immobilized onto the film surface to form a functional top layer. Polyelectrolyte adsorption was studied and confirmed on silicon wafers by measuring the water contact angles of the layers and investigating the surface morphology via atomic force microscopy. An up to 4-5 °C increase in ice nucleation temperatures and an up to 10 min decrease in freezing times were observed with high-purity deionized water samples frozen in ECIN-coated LDPE films. Films retained their ice nucleation activity up to 50 freeze-thaw cycles. Our results demonstrate the potential of using ECIN-coated polymer films for frozen food application.
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Zhao, Bingge; Yang, Bin; Abyzov, Alexander S; Schmelzer, Jürn W P; Rodríguez-Viejo, Javier; Zhai, Qijie; Schick, Christoph; Gao, Yulai
2017-12-13
In this paper, the amorphous Ce 68 Al 10 Cu 20 Co 2 (atom %) alloy was in situ prepared by nanocalorimetry. The high cooling and heating rates accessible with this technique facilitate the suppression of crystallization on cooling and the identification of homogeneous nucleation. Different from the generally accepted notion that metallic glasses form just by avoiding crystallization, the role of nucleation and growth in the crystallization behavior of amorphous alloys is specified, allowing an access to the ideal metallic glass free of nuclei. Local atomic configurations are fundamentally significant to unravel the glass forming ability (GFA) and phase transitions in metallic glasses. For this reason, isothermal annealing near T g from 0.001 s to 25,000 s following quenching becomes the strategy to tune local atomic configurations and facilitate an amorphous alloy, a mixed glassy-nanocrystalline state, and a crystalline sample successively. On the basis of the evolution of crystallization enthalpy and overall latent heat on reheating, we quantify the underlying mechanism for the isothermal nucleation and crystallization of amorphous alloys. With Johnson-Mehl-Avrami method, it is demonstrated that the coexistence of homogeneous and heterogeneous nucleation contributes to the isothermal crystallization of glass. Heterogeneous rather than homogeneous nucleation dominates the isothermal crystallization of the undercooled liquid. For the mixed glassy-nanocrystalline structure, an extraordinary kinetic stability of the residual glass is validated, which is ascribed to the denser packed interface between amorphous phase and ordered nanocrystals. Tailoring the amorphous structure by nanocalorimetry permits new insights into unraveling GFA and the mechanism that correlates local atomic configurations and phase transitions in metallic glasses.
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Ice-nucleating particle concentrations unaffected by urban air pollution in Beijing, China
Chen, Jie; Wu, Zhijun; Augustin-Bauditz, Stefanie; Grawe, Sarah; Hartmann, Markus; Pei, Xiangyu; Liu, Zirui; Ji, Dongsheng; Wex, Heike
2018-03-01
Exceedingly high levels of PM2.5 with complex chemical composition occur frequently in China. It has been speculated whether anthropogenic PM2.5 may significantly contribute to ice-nucleating particles (INP). However, few studies have focused on the ice-nucleating properties of urban particles. In this work, two ice-nucleating droplet arrays have been used to determine the atmospheric number concentration of INP (NINP) in the range from -6 to -25 °C in Beijing. No correlations between NINP and either PM2.5 or black carbon mass concentrations were found, although both varied by more than a factor of 30 during the sampling period. Similarly, there were no correlations between NINP and either total particle number concentration or number concentrations for particles with diameters > 500 nm. Furthermore, there was no clear difference between day and night samples. All these results indicate that Beijing air pollution did not increase or decrease INP concentrations in the examined temperature range above values observed in nonurban areas; hence, the background INP concentrations might not be anthropogenically influenced as far as urban air pollution is concerned, at least in the examined temperature range.
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Uncertainty in counting ice nucleating particles with continuous flow diffusion chambers
Garimella, Sarvesh; Rothenberg, Daniel A.; Wolf, Martin J.; David, Robert O.; Kanji, Zamin A.; Wang, Chien; Rösch, Michael; Cziczo, Daniel J.
2017-09-01
This study investigates the measurement of ice nucleating particle (INP) concentrations and sizing of crystals using continuous flow diffusion chambers (CFDCs). CFDCs have been deployed for decades to measure the formation of INPs under controlled humidity and temperature conditions in laboratory studies and by ambient aerosol populations. These measurements have, in turn, been used to construct parameterizations for use in models by relating the formation of ice crystals to state variables such as temperature and humidity as well as aerosol particle properties such as composition and number. We show here that assumptions of ideal instrument behavior are not supported by measurements made with a commercially available CFDC, the SPectrometer for Ice Nucleation (SPIN), and the instrument on which it is based, the Zurich Ice Nucleation Chamber (ZINC). Non-ideal instrument behavior, which is likely inherent to varying degrees in all CFDCs, is caused by exposure of particles to different humidities and/or temperatures than predicated from instrument theory of operation. This can result in a systematic, and variable, underestimation of reported INP concentrations. We find here variable correction factors from 1.5 to 9.5, consistent with previous literature values. We use a machine learning approach to show that non-ideality is most likely due to small-scale flow features where the aerosols are combined with sheath flows. Machine learning is also used to minimize the uncertainty in measured INP concentrations. We suggest that detailed measurement, on an instrument-by-instrument basis, be performed to characterize this uncertainty.
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Uncertainty in counting ice nucleating particles with continuous flow diffusion chambers
Directory of Open Access Journals (Sweden)
S. Garimella
2017-09-01
Full Text Available This study investigates the measurement of ice nucleating particle (INP concentrations and sizing of crystals using continuous flow diffusion chambers (CFDCs. CFDCs have been deployed for decades to measure the formation of INPs under controlled humidity and temperature conditions in laboratory studies and by ambient aerosol populations. These measurements have, in turn, been used to construct parameterizations for use in models by relating the formation of ice crystals to state variables such as temperature and humidity as well as aerosol particle properties such as composition and number. We show here that assumptions of ideal instrument behavior are not supported by measurements made with a commercially available CFDC, the SPectrometer for Ice Nucleation (SPIN, and the instrument on which it is based, the Zurich Ice Nucleation Chamber (ZINC. Non-ideal instrument behavior, which is likely inherent to varying degrees in all CFDCs, is caused by exposure of particles to different humidities and/or temperatures than predicated from instrument theory of operation. This can result in a systematic, and variable, underestimation of reported INP concentrations. We find here variable correction factors from 1.5 to 9.5, consistent with previous literature values. We use a machine learning approach to show that non-ideality is most likely due to small-scale flow features where the aerosols are combined with sheath flows. Machine learning is also used to minimize the uncertainty in measured INP concentrations. We suggest that detailed measurement, on an instrument-by-instrument basis, be performed to characterize this uncertainty.
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Alpert, Peter A.; Knopf, Daniel A.
2016-02-01
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
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Directory of Open Access Journals (Sweden)
R. W. Saunders
2010-02-01
Full Text Available Nanoparticles of iron oxide (crystalline and amorphous, silicon oxide and magnesium oxide were investigated for their propensity to nucleate ice over the temperature range 180–250 K, using the AIDA chamber in Karlsruhe, Germany.
All samples were observed to initiate ice formation via the deposition mode at threshold ice super-saturations (RHithresh ranging from 105% to 140% for temperatures below 220 K. Approximately 10% of amorphous Fe2O3 particles (modal diameter = 30 nm generated in situ from a photochemical aerosol reactor, led to ice nucleation at RHithresh = 140% at an initial chamber temperature of 182 K. Quantitative analysis using a singular hypothesis treatment provided a fitted function [ns(190 K=10(3.33×sice+8.16] for the variation in ice-active surface site density (ns:m−2 with ice saturation (sice for Fe2O3 nanoparticles. This was implemented in an aerosol-cloud model to determine a predicted deposition (mass accommodation coefficient for water vapour on ice of 0.1 at temperatures appropriate for the upper atmosphere. Classical nucleation theory was used to determine representative contact angles (θ for the different particle compositions. For the in situ generated Fe2O3 particles, a slight inverse temperature dependence was observed with θ = 10.5° at 182 K, decreasing to 9.0° at 200 K (compared with 10.2° and 11.4° respectively for the SiO2 and MgO particle samples at the higher temperature.
These observations indicate that such refractory nanoparticles are relatively efficient materials for the nucleation of ice under the conditions studied in the chamber which correspond to cirrus cloud formation in the upper troposphere. The results also show that Fe2O3 particles do not act as ice -
Homogeneous nucleation in liquid nitrogen at negative pressures
Energy Technology Data Exchange (ETDEWEB)
Baidakov, V. G., E-mail: baidakov@itp.uran.ru; Vinogradov, V. E.; Pavlov, P. A. [Russian Academy of Sciences, Institute of Thermal Physics, Ural Branch (Russian Federation)
2016-10-15
The kinetics of spontaneous cavitation in liquid nitrogen at positive and negative pressures has been studied in a tension wave formed by a compression pulse reflected from the liquid–vapor interface on a thin platinum wire heated by a current pulse. The limiting tensile stresses (Δp = p{sub s}–p, where p{sub s} is the saturation pressure), the corresponding bubble nucleation frequencies J (10{sup 20}–10{sup 22} s{sup –1} m{sup –3}), and temperature induced nucleation frequency growth rate G{sub T} = dlnJ/dT have been experimentally determined. At T = 90 K, the limiting tensile stress was Δp = 8.3 MPa, which was 4.9 MPa lower than the value corresponding to the boundary of thermodynamic stability of the liquid phase (spinodal). The measurement results were compared to classical (homogeneous) nucleation theory (CNT) with and without neglect of the dependence of the surface tension of critical bubbles on their dimensions. In the latter case, the properties of new phase nuclei were described in terms of the Van der Waals theory of capillarity. The experimental data agree well with the CNT theory when it takes into account the “size effect.”.
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International Nuclear Information System (INIS)
Kanji, Zamin A; Florea, Octavian; Abbatt, Jonathan P D
2008-01-01
We present ice nucleation results for Arizona test dust, kaolinite, montmorillonite, silica, silica coated with a hydrophobic octyl chain, oxalic acid dihydrate, Gascoyne leonardite (a humic material), and Aldrich humic acid (sodium salt). The focus was on deposition mode nucleation below water saturation at 233 K. Particles were deposited onto a hydrophobic cold stage by atomization of a slurry/solution and exposed to a constant partial pressure of water vapor. By lowering the temperature of the stage, the relative humidity with respect to ice (RH i ) was gradually increased until ice nucleation was observed using digital photography. Different numbers of particles were deposited onto the cold stage by varying the atomization solution concentration and deposition time. For the same total particulate surface area, mineral dust particles nucleated ice at lower supersaturations than all other materials. The most hydrophobic materials, i.e. Gascoyne leonardite and octyl silica, were the least active. For our limit of detection of one ice crystal, the ice onset RH i values were dependent on the total surface area of the particulates, indicating that no unique threshold RH i for ice nucleation prevails
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Energy Technology Data Exchange (ETDEWEB)
Kanji, Zamin A; Florea, Octavian; Abbatt, Jonathan P D [Department of Chemistry, University of Toronto, 80 St George Street, Toronto, ON, M5S 3H6 (Canada)], E-mail: zkanji@chem.utoronto.ca
2008-04-15
We present ice nucleation results for Arizona test dust, kaolinite, montmorillonite, silica, silica coated with a hydrophobic octyl chain, oxalic acid dihydrate, Gascoyne leonardite (a humic material), and Aldrich humic acid (sodium salt). The focus was on deposition mode nucleation below water saturation at 233 K. Particles were deposited onto a hydrophobic cold stage by atomization of a slurry/solution and exposed to a constant partial pressure of water vapor. By lowering the temperature of the stage, the relative humidity with respect to ice (RH{sub i}) was gradually increased until ice nucleation was observed using digital photography. Different numbers of particles were deposited onto the cold stage by varying the atomization solution concentration and deposition time. For the same total particulate surface area, mineral dust particles nucleated ice at lower supersaturations than all other materials. The most hydrophobic materials, i.e. Gascoyne leonardite and octyl silica, were the least active. For our limit of detection of one ice crystal, the ice onset RH{sub i} values were dependent on the total surface area of the particulates, indicating that no unique threshold RH{sub i} for ice nucleation prevails.
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Forward flux sampling calculation of homogeneous nucleation rates from aqueous NaCl solutions.
Jiang, Hao; Haji-Akbari, Amir; Debenedetti, Pablo G; Panagiotopoulos, Athanassios Z
2018-01-28
We used molecular dynamics simulations and the path sampling technique known as forward flux sampling to study homogeneous nucleation of NaCl crystals from supersaturated aqueous solutions at 298 K and 1 bar. Nucleation rates were obtained for a range of salt concentrations for the Joung-Cheatham NaCl force field combined with the Extended Simple Point Charge (SPC/E) water model. The calculated nucleation rates are significantly lower than the available experimental measurements. The estimates for the nucleation rates in this work do not rely on classical nucleation theory, but the pathways observed in the simulations suggest that the nucleation process is better described by classical nucleation theory than an alternative interpretation based on Ostwald's step rule, in contrast to some prior simulations of related models. In addition to the size of NaCl nucleus, we find that the crystallinity of a nascent cluster plays an important role in the nucleation process. Nuclei with high crystallinity were found to have higher growth probability and longer lifetimes, possibly because they are less exposed to hydration water.
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Deviation from equilibrium conditions in molecular dynamic simulations of homogeneous nucleation.
Halonen, Roope; Zapadinsky, Evgeni; Vehkamäki, Hanna
2018-04-28
We present a comparison between Monte Carlo (MC) results for homogeneous vapour-liquid nucleation of Lennard-Jones clusters and previously published values from molecular dynamics (MD) simulations. Both the MC and MD methods sample real cluster configuration distributions. In the MD simulations, the extent of the temperature fluctuation is usually controlled with an artificial thermostat rather than with more realistic carrier gas. In this study, not only a primarily velocity scaling thermostat is considered, but also Nosé-Hoover, Berendsen, and stochastic Langevin thermostat methods are covered. The nucleation rates based on a kinetic scheme and the canonical MC calculation serve as a point of reference since they by definition describe an equilibrated system. The studied temperature range is from T = 0.3 to 0.65 ϵ/k. The kinetic scheme reproduces well the isothermal nucleation rates obtained by Wedekind et al. [J. Chem. Phys. 127, 064501 (2007)] using MD simulations with carrier gas. The nucleation rates obtained by artificially thermostatted MD simulations are consistently lower than the reference nucleation rates based on MC calculations. The discrepancy increases up to several orders of magnitude when the density of the nucleating vapour decreases. At low temperatures, the difference to the MC-based reference nucleation rates in some cases exceeds the maximal nonisothermal effect predicted by classical theory of Feder et al. [Adv. Phys. 15, 111 (1966)].
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Yordanova, Petya; Maier, Stefanie; Lang-Yona, Naama; Tamm, Alexandra; Meusel, Hannah; Pöschl, Ulrich; Weber, Bettina; Fröhlich-Nowoisky, Janine
2017-04-01
Atmospheric aerosol particles, including desert and soil dust as well as marine aerosols, are well known to act as ice nuclei (IN) and thus have been investigated in numerous ice nucleation studies. Based on their cloud condensation nuclei potential and their impacts on radiative properties of clouds (via scattering and absorption of solar radiation), aerosol particles may significantly affect the cloud and precipitation development. Atmospheric aerosols of the Eastern Mediterranean have been described to be dominated by desert dust, but only little is known on their composition and ice nucleating properties. In this study we investigated the ice nucleating ability of total suspended particles (TSP), collected at the remote site Agia Marina Xyliatou on Cyprus during a field campaign in April 2016. Airborne TSP samples containing air masses of various types such as African (Saharan) and Arabian dust and European and Middle Eastern pollution were collected on glass fiber filters at 24 h intervals. Sampling was performed ˜5 m above ground level and ˜521 m above sea level. During the sampling period, two major dust storms (PM 10max 118 μg/m3 and 66 μg/m3) and a rain event (rainfall amount: 3.4 mm) were documented. Chemical and physical characterizations of the particles were analyzed experimentally through filtration, thermal, chemical and enzyme treatments. Immersion freezing experiments were performed at relatively high subzero temperatures (-1 to -15˚ C) using the mono ice nucleation array. Preliminary results indicate that highest IN particle numbers (INPs) occurred during the second dust storm event with lower particle concentrations. Treatments at 60˚ C lead to a gradual IN deactivation, indicating the presence of biological INPs, which were observed to be larger than 300 kDa. Additional results originating from this study will be shown. Acknowledgement: This work was funded by the DFG Ice Nuclei Research Unit (INUIT).
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Overview: Homogeneous nucleation from the vapor phase-The experimental science.
Wyslouzil, Barbara E; Wölk, Judith
2016-12-07
Homogeneous nucleation from the vapor phase has been a well-defined area of research for ∼120 yr. In this paper, we present an overview of the key experimental and theoretical developments that have made it possible to address some of the fundamental questions first delineated and investigated in C. T. R. Wilson's pioneering paper of 1897 [C. T. R. Wilson, Philos. Trans. R. Soc., A 189, 265-307 (1897)]. We review the principles behind the standard experimental techniques currently used to measure isothermal nucleation rates, and discuss the molecular level information that can be extracted from these measurements. We then highlight recent approaches that interrogate the vapor and intermediate clusters leading to particle formation, more directly.
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Hill, T. C.; DeMott, P. J.; Garcia, E.; Moffett, B. F.; Prenni, A. J.; Kreidenweis, S. M.; Franc, G. D.
2013-12-01
Ice nucleation active (INA) bacteria are a potentially prodigious source of highly active (≥-12°C) atmospheric ice nuclei, especially from agricultural land. However, we know little about the conditions that promote their release (eg, daily or seasonal cycles, precipitation, harvesting or post-harvest decay of litter) or their typical contribution to the pool of boundary layer ice nucleating particles (INP). To initiate these investigations we developed a quantitative Polymerase Chain Reaction (qPCR) test of the ina gene, the gene that codes for the ice nucleating protein, to directly count INA bacteria in environmental samples. The qPCR test amplifies most forms of the gene and is highly sensitive, able to detect perhaps a single gene copy (ie, a single bacterium) in DNA extracted from precipitation. Direct measurement of the INA bacteria is essential because environmental populations will be a mixture of living, viable-but-not culturable, moribund and dead cells, all of which may retain ice nucleating proteins. Using the qPCR test on leaf washings of plants from three farms in Wyoming, Colorado and Nebraska we found INA bacteria to be abundant on crops, especially on cereals. Mid-summer populations on wheat and barley were ~108/g fresh weigh of foliage. Broadleaf crops, such as corn, alfalfa, sugar beet and potato supported 105-107/g. Unexpectedly, however, in the absence of a significant physical disturbance, such as harvesting, we were unable to detect the ina gene in aerosols sampled above the crops. Likewise, in fresh snow samples taken over two winters, ina genes from a range of INA bacteria were detected in about half the samples but at abundances that equated to INA bacterial numbers that accounted for only a minor proportion of INP active at -10°C. By contrast, in a hail sample from a summer thunderstorm we found 0.3 INA bacteria per INP at -10°C and ~0.5 per hail stone. Although the role of the INA bacteria as warm-temperature INP in these samples
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Correlation between thermodynamic anomalies and pathways of ice nucleation in supercooled water
International Nuclear Information System (INIS)
Singh, Rakesh S.; Bagchi, Biman
2014-01-01
The well-known classical nucleation theory (CNT) for the free energy barrier towards formation of a nucleus of critical size of the new stable phase within the parent metastable phase fails to take into account the influence of other metastable phases having density/order intermediate between the parent metastable phase and the final stable phase. This lacuna can be more serious than capillary approximation or spherical shape assumption made in CNT. This issue is particularly significant in ice nucleation because liquid water shows rich phase diagram consisting of two (high and low density) liquid phases in supercooled state. The explanations of thermodynamic and dynamic anomalies of supercooled water often invoke the possible influence of a liquid-liquid transition between two metastable liquid phases. To investigate both the role of thermodynamic anomalies and presence of distinct metastable liquid phases in supercooled water on ice nucleation, we employ density functional theoretical approach to find nucleation free energy barrier in different regions of phase diagram. The theory makes a number of striking predictions, such as a dramatic lowering of nucleation barrier due to presence of a metastable intermediate phase and crossover in the dependence of free energy barrier on temperature near liquid-liquid critical point. These predictions can be tested by computer simulations as well as by controlled experiments
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International Nuclear Information System (INIS)
Hoose, C; Lohmann, U; Erdin, R; Tegen, I
2008-01-01
Mineral dust is the dominant natural ice nucleating aerosol. Its ice nucleation efficiency depends on the mineralogical composition. We show the first sensitivity studies with a global climate model and a three-dimensional dust mineralogy. Results show that, depending on the dust mineralogical composition, coating with soluble material from anthropogenic sources can lead to quasi-deactivation of natural dust ice nuclei. This effect counteracts the increased cloud glaciation by anthropogenic black carbon particles. The resulting aerosol indirect effect through the glaciation of mixed-phase clouds by black carbon particles is small (+0.1 W m -2 in the shortwave top-of-the-atmosphere radiation in the northern hemisphere)
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Directory of Open Access Journals (Sweden)
P. A. Alpert
2016-02-01
Full Text Available 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
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Directory of Open Access Journals (Sweden)
O. Möhler
2008-10-01
Full Text Available The ice nucleation activities of five different Pseudomonas syringae, Pseudomonas viridiflava and Erwinia herbicola bacterial species and of Snomax™ were investigated in the temperature range between −5 and −15°C. Water suspensions of these bacteria were directly sprayed into the cloud chamber of the AIDA facility of Forschungszentrum Karlsruhe at a temperature of −5.7°C. At this temperature, about 1% of the Snomax™ cells induced immersion freezing of the spray droplets before the droplets evaporated in the cloud chamber. The living cells didn't induce any detectable immersion freezing in the spray droplets at −5.7°C. After evaporation of the spray droplets the bacterial cells remained as aerosol particles in the cloud chamber and were exposed to typical cloud formation conditions in experiments with expansion cooling to about −11°C. During these experiments, the bacterial cells first acted as cloud condensation nuclei to form cloud droplets. Then, only a minor fraction of the cells acted as heterogeneous ice nuclei either in the condensation or the immersion mode. The results indicate that the bacteria investigated in the present study are mainly ice active in the temperature range between −7 and −11°C with an ice nucleation (IN active fraction of the order of 10−4. In agreement to previous literature results, the ice nucleation efficiency of Snomax™ cells was much larger with an IN active fraction of 0.2 at temperatures around −8°C.
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Influence of the homogenization pressure on the ice cream mix quality
Directory of Open Access Journals (Sweden)
Iva Murgić
2008-08-01
Full Text Available In this paper the suitability of different homogenization pressures on appearance and quality of ice cream mix was determined. The ice cream mix were taken from ageing tank, and depending on the source of fat in ice cream mix (butter, vegetable fat or cream they were homogenized under different pressures. Afterwards, by microscope with scalar, fat globule size was determined. The homogenization pressures reduce the fat globule size to 1-2 μm without clumping and these pressures have been characterized as adequate pressures for specific type of fat and specific portion of fat in the ice cream mixture. The higher the fat in the mixture, the lower the pressure should be. The optimal pressure for ice cream mixture containing 2% vegetable fat was 200 bars, for 6% 190-200 bars, and for 8% 170 bars. The optimal pressure for ice cream mixture that contained 8% butter was 190-200 bars, for 10% 150, and for 12% 135 bars. For ice cream mixture containing 8% of cream, optimal pressure was 200 bars, 10% cream was 190, 12% cream was 125 bars and 14% cream was 90 bars.
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Ladino, Luis A.; Korolev, Alexei; Heckman, Ivan; Wolde, Mengistu; Fridlind, Ann M.; Ackerman, Andrew S.
2018-01-01
Over decades, the cloud physics community has debated the nature and role of aerosol particles in ice initiation. The present study shows that the measured concentration of ice crystals in tropical mesoscale convective systems exceeds the concentration of ice nucleating particles (INPs) by several orders of magnitude. The concentration of INPs was assessed from the measured aerosol particles concentration in the size range of 0.5 to 1 µm. The observations from this study suggest that primary ice crystals formed on INPs make only a minor contribution to the total concentration of ice crystals in tropical mesoscale convective systems. This is found by comparing the predicted INP number concentrations with in-situ ice particle number concentrations. The obtained measurements suggest that ice multiplication is the likely explanation for the observed high concentrations of ice crystals in this type of convective system. PMID:29551842
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In-situ measurements of ice nucleating particles with FINCH (Fast Ice Nucleus Chamber)
Kohl, Rebecca; Frank, Fabian; Curtius, Joachim; Rose, Diana
2017-04-01
Ice nucleating particles (INPs), which are a small fraction of the total aerosol population, are capable of triggering ice formation under atmospheric conditions. Since INPs play an important role for the radiative properties of clouds as well as for the formation of precipitation it is important to get quantitative information on the ice activity of various atmospheric aerosol species. With the Fast Ice Nucleus Chamber (FINCH; Bundke et al., 2008) the number concentration of INP is determined at different freezing temperatures and supersaturations. In contrast to other commonly used INP counters, i.e., continuous flow diffusion chambers (CFDCs, DeMott et al., 2011), in FINCH the supersaturation is reached by mixing the sample flow of ambient aerosol with a warm moist as well as a cold dry airflow. By changing the flow rates and temperatures of the individual airflows the freezing temperature (down to -50°C) and supersaturation (up to above water saturation) can be varied relatively quickly. Particles that are ice active at the prescribed freezing temperature and supersaturation grow to crystals and are counted by a home-built optical particle counter (OPC) mounted below the chamber (Bundke et al., 2010). FINCH was operated during the four-week INUIT-BACCHUS-ACTRIS field campaign in Cyprus in April 2016. The measuring site was the location of the Cyprus Atmospheric Observatory (CAO) at Agia Marina Xyliatou, which is typically influenced by dust from the Sahara and the Middle East, an aerosol that is known to have relatively good ice nucleating ability. First results from this campaign will be presented. Acknowledgements: The authors thank the entire INUIT-BACCHUS-ACTRIS campaign team for their cooperation and support. The INUIT-2 project is financed by the German Research Foundation DFG (FOR 1525). The INUIT-Cyprus campaign is a cooperation with the EU-funded project BACCHUS and is also funded by ACTRIS-TNA. References: Bundke, U., Nillius, B., Jaenicke, R
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Cavitation in a metallic liquid: homogeneous nucleation and growth of nanovoids.
Cai, Y; Wu, H A; Luo, S N
2014-06-07
Large-scale molecular dynamics (MD) simulations are performed to investigate homogeneous nucleation and growth of nanovoids during cavitation in liquid Cu. We characterize in detail the atomistic cavitation processes by following the temporal evolution of cavities or voids, analyze the nucleation behavior with the mean first-passage time (MFPT) and survival probability (SP) methods, and discuss the results against classical nucleation theory (CNT), the Tolman equation for surface energy, independent calculation of surface tension via integrating the stress profiles, the Johnson-Mehl-Avrami (JMA) growth law, and the power law for nucleus size distributions. Cavitation in this representative metallic liquid is a high energy barrier Poisson processes, and the steady-state nucleation rates obtained from statistical runs with the MFPT and SP methods are in agreement. The MFPT method also yields the critical nucleus size and the Zeldovich factor. Fitting with the Tolman's equation to the MD simulations yields the surface energy of a planar interface (~0.9 J m⁻²) and the Tolman length (0.4-0.5 Å), and those values are in accord with those from integrating the stress profiles of a planar interface. Independent CNT predictions of the nucleation rate (10(33 - 34) s(-1) m(-3)) and critical size (3-4 Å in radius) are in agreement with the MFPT and SP results. The JMA law can reasonably describe the nucleation and growth process. The size distribution of subcritical nuclei appears to follow a power law with an exponent decreasing with increasing tension owing to coupled nucleation and growth, and that of the supercritical nuclei becomes flattened during further stress relaxation due to void coalescence.
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Cavitation in a metallic liquid: Homogeneous nucleation and growth of nanovoids
International Nuclear Information System (INIS)
Cai, Y.; Wu, H. A.; Luo, S. N.
2014-01-01
Large-scale molecular dynamics (MD) simulations are performed to investigate homogeneous nucleation and growth of nanovoids during cavitation in liquid Cu. We characterize in detail the atomistic cavitation processes by following the temporal evolution of cavities or voids, analyze the nucleation behavior with the mean first-passage time (MFPT) and survival probability (SP) methods, and discuss the results against classical nucleation theory (CNT), the Tolman equation for surface energy, independent calculation of surface tension via integrating the stress profiles, the Johnson-Mehl-Avrami (JMA) growth law, and the power law for nucleus size distributions. Cavitation in this representative metallic liquid is a high energy barrier Poisson processes, and the steady-state nucleation rates obtained from statistical runs with the MFPT and SP methods are in agreement. The MFPT method also yields the critical nucleus size and the Zeldovich factor. Fitting with the Tolman's equation to the MD simulations yields the surface energy of a planar interface (∼0.9 J m −2 ) and the Tolman length (0.4–0.5 Å), and those values are in accord with those from integrating the stress profiles of a planar interface. Independent CNT predictions of the nucleation rate (10 33−34 s −1 m −3 ) and critical size (3–4 Å in radius) are in agreement with the MFPT and SP results. The JMA law can reasonably describe the nucleation and growth process. The size distribution of subcritical nuclei appears to follow a power law with an exponent decreasing with increasing tension owing to coupled nucleation and growth, and that of the supercritical nuclei becomes flattened during further stress relaxation due to void coalescence
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Ice-nucleating particle emissions from photochemically aged diesel and biodiesel exhaust
Schill, G. P.; Jathar, S. H.; Kodros, J. K.; Levin, E. J. T.; Galang, A. M.; Friedman, B.; Link, M. F.; Farmer, D. K.; Pierce, J. R.; Kreidenweis, S. M.; DeMott, P. J.
2016-05-01
Immersion-mode ice-nucleating particle (INP) concentrations from an off-road diesel engine were measured using a continuous-flow diffusion chamber at -30°C. Both petrodiesel and biodiesel were utilized, and the exhaust was aged up to 1.5 photochemically equivalent days using an oxidative flow reactor. We found that aged and unaged diesel exhaust of both fuels is not likely to contribute to atmospheric INP concentrations at mixed-phase cloud conditions. To explore this further, a new limit-of-detection parameterization for ice nucleation on diesel exhaust was developed. Using a global-chemical transport model, potential black carbon INP (INPBC) concentrations were determined using a current literature INPBC parameterization and the limit-of-detection parameterization. Model outputs indicate that the current literature parameterization likely overemphasizes INPBC concentrations, especially in the Northern Hemisphere. These results highlight the need to integrate new INPBC parameterizations into global climate models as generalized INPBC parameterizations are not valid for diesel exhaust.
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Hill, T. C. J.; DeMott, P. J.; Fröhlich-Nowoisky, J.; Tobo, Y.; Suski, K. J.; Levin, E. J.; Kreidenweis, S. M.; Franc, G. D.
2014-12-01
Soil and plant surfaces emit ice nucleating particles (INP) to the atmosphere, especially when disturbed by wind, harvesting, rain or fire. Organic (biogenic) INP are abundant in most soils and dominate the population that nucleate >-15°C. For example, the sandy topsoil of sagebrush shrubland, a widespread ecotype prone to wind erosion after fire, contains ~106 organic INP g-1 at -6°C. The relevance of organic INP may also extend to colder temperatures than previously thought: Particles of soil organic matter (SOM) have been shown to be more important than mineral particles for the ice nucleating ability of agricultural soil dusts to -34°C. While the abundance of ice nucleation active (INA) bacteria on plants has been established, the identity of the organic INP in and emitted by soils remains a 40-year-old mystery. The need to understand their production and release is highlighted by recent findings that INA bacteria (measured with qPCR) account for few, if any, of the warm-temperature organic INP that predominate in boundary layer aerosols and snow; organic INP lofted with soil dusts seem a likely source. The complexity of SOM hinders its investigation. It contains decomposing plant materials, a diverse microbial and microfaunal community, humus, and inert organic matter. All are biochemically complex and all may contain ice nucleating constituents, either by design or by chance. Indeed the smoothness of the INP temperature spectra of soils is indicative of numerous, overlapping distributions of INP. We report recent progress in identifying and quantifying the organic INP in soils and boundary layer aerosols representative of West Central U.S. ecosystems, and how their characteristics may affect their dispersal. Chemical, enzymatic and DNA-based tests were used to assess contributions of INP from plant tissues, INA bacteria, INA fungi, organic crystals, monolayers of aliphatic alcohols, carbohydrates, and humic substances, while heat- and peroxide-based tests
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On the effect of pressure and carrier gas on homogeneous water nucleation
Czech Academy of Sciences Publication Activity Database
Fransen, M. A. L. J.; Hrubý, Jan; Smeulders, D. M. J.; Dongen, M. E. H.
2015-01-01
Roč. 142, č. 16 (2015), 164307_1-164307_7 ISSN 0021-9606 R&D Projects: GA ČR(CZ) GAP101/11/1593 Institutional support: RVO:61388998 Keywords : homogeneous nucleation * water * pressure effect Subject RIV: BJ - Thermodynamics Impact factor: 2.894, year: 2015 http://dx.doi.org/10.1063/1.4919249
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Rangel-Alvarado, Rodrigo Benjamin; Nazarenko, Yevgen; Ariya, Parisa A.
2015-11-01
Physicochemical processes of nucleation constitute a major uncertainty in understanding aerosol-cloud interactions. To improve the knowledge of the ice nucleation process, we characterized physical, chemical, and biological properties of fresh snow using a suite of state-of-the-art techniques based on mass spectrometry, electron microscopy, chromatography, and optical particle sizing. Samples were collected at two North American Arctic sites, as part of international campaigns (2006 and 2009), and in the city of Montreal, Canada, over the last decade. Particle size distribution analyses, in the range of 3 nm to 10 µm, showed that nanosized particles are the most numerous (38-71%) in fresh snow, with a significant portion (11 to 19%) less than 100 nm in size. Particles with diameters less than 200 nm consistently exhibited relatively high ice-nucleating properties (on average ranged from -19.6 ± 2.4 to -8.1 ± 2.6°C). Chemical analysis of the nanosized fraction suggests that they contain bioorganic materials, such as amino acids, as well as inorganic compounds with similar characteristics to mineral dust. The implication of nanoparticle ubiquity and abundance in diverse snow ecosystems are discussed in the context of their importance in understanding atmospheric nucleation processes.
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Alpert, P. A.; Knopf, D. A.
2015-05-01
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
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Cavitation in a metallic liquid: Homogeneous nucleation and growth of nanovoids
Energy Technology Data Exchange (ETDEWEB)
Cai, Y. [Department of Modern Mechanics, CAS Key Laboratory of Materials Behavior and Design, University of Science and Technology of China, Hefei, Anhui 230027 (China); The Peac Institute of Multiscale Sciences, Chengdu, Sichuan 610207 (China); Wu, H. A., E-mail: wuha@ustc.edu.cn [Department of Modern Mechanics, CAS Key Laboratory of Materials Behavior and Design, University of Science and Technology of China, Hefei, Anhui 230027 (China); Luo, S. N., E-mail: sluo@pims.ac.cn [The Peac Institute of Multiscale Sciences, Chengdu, Sichuan 610207 (China)
2014-06-07
Large-scale molecular dynamics (MD) simulations are performed to investigate homogeneous nucleation and growth of nanovoids during cavitation in liquid Cu. We characterize in detail the atomistic cavitation processes by following the temporal evolution of cavities or voids, analyze the nucleation behavior with the mean first-passage time (MFPT) and survival probability (SP) methods, and discuss the results against classical nucleation theory (CNT), the Tolman equation for surface energy, independent calculation of surface tension via integrating the stress profiles, the Johnson-Mehl-Avrami (JMA) growth law, and the power law for nucleus size distributions. Cavitation in this representative metallic liquid is a high energy barrier Poisson processes, and the steady-state nucleation rates obtained from statistical runs with the MFPT and SP methods are in agreement. The MFPT method also yields the critical nucleus size and the Zeldovich factor. Fitting with the Tolman's equation to the MD simulations yields the surface energy of a planar interface (∼0.9 J m{sup −2}) and the Tolman length (0.4–0.5 Å), and those values are in accord with those from integrating the stress profiles of a planar interface. Independent CNT predictions of the nucleation rate (10{sup 33−34} s{sup −1} m{sup −3}) and critical size (3–4 Å in radius) are in agreement with the MFPT and SP results. The JMA law can reasonably describe the nucleation and growth process. The size distribution of subcritical nuclei appears to follow a power law with an exponent decreasing with increasing tension owing to coupled nucleation and growth, and that of the supercritical nuclei becomes flattened during further stress relaxation due to void coalescence.
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Boundary layer new particle formation over East Antarctic sea ice – possible Hg-driven nucleation?
Directory of Open Access Journals (Sweden)
R. S. Humphries
2015-12-01
Full Text Available Aerosol observations above the Southern Ocean and Antarctic sea ice are scarce. Measurements of aerosols and atmospheric composition were made in East Antarctic pack ice on board the Australian icebreaker Aurora Australis during the spring of 2012. One particle formation event was observed during the 32 days of observations. This event occurred on the only day to exhibit extended periods of global irradiance in excess of 600 W m−2. Within the single air mass influencing the measurements, number concentrations of particles larger than 3 nm (CN3 reached almost 7700 cm−3 within a few hours of clouds clearing, and grew at rates of 5.6 nm h−1. Formation rates of 3 nm particles were in the range of those measured at other Antarctic locations at 0.2–1.1 ± 0.1 cm−3 s−1. Our investigations into the nucleation chemistry found that there were insufficient precursor concentrations for known halogen or organic chemistry to explain the nucleation event. Modelling studies utilising known sulfuric acid nucleation schemes could not simultaneously reproduce both particle formation or growth rates. Surprising correlations with total gaseous mercury (TGM were found that, together with other data, suggest a mercury-driven photochemical nucleation mechanism may be responsible for aerosol nucleation. Given the very low vapour pressures of the mercury species involved, this nucleation chemistry is likely only possible where pre-existing aerosol concentrations are low and both TGM concentrations and solar radiation levels are relatively high (∼ 1.5 ng m−3 and ≥ 600 W m−2, respectively, such as those observed in the Antarctic sea ice boundary layer in this study or in the global free troposphere, particularly in the Northern Hemisphere.
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Energy Technology Data Exchange (ETDEWEB)
Moehler, O; Benz, S; Saathoff, H; Schnaiter, M; Wagner, R [Forschungszentrum Karlsruhe, Institute for Meteorology and Climate Research, 76021 Karlsruhe (Germany); Schneider, J; Walter, S [Max Planck Institute for Chemistry, 55128 Mainz (Germany); Ebert, V; Wagner, S [University of Heidelberg, Institute for Physical Chemistry, 69120 Heidelberg (Germany)], E-mail: Ottmar.Moehler@imk.fzk.de
2008-04-15
The effect of organic coating on the heterogeneous ice nucleation (IN) efficiency of dust particles was investigated at simulated cirrus cloud conditions in the AIDA cloud chamber of Forschungszentrum Karlsruhe. Arizona test dust (ATD) and the clay mineral illite were used as surrogates for atmospheric dust aerosols. The dry dust samples were dispersed into a 3.7 m{sup 3} aerosol vessel and either directly transferred into the 84 m{sup 3} cloud simulation chamber or coated before with the semi-volatile products from the reaction of {alpha}-pinene with ozone in order to mimic the coating of atmospheric dust particles with secondary organic aerosol (SOA) substances. The ice-active fraction was measured in AIDA expansion cooling experiments as a function of the relative humidity with respect to ice, RHi, in the temperature range from 205 to 210 K. Almost all uncoated dust particles with diameters between 0.1 and 1.0 {mu}m acted as efficient deposition mode ice nuclei at RHi between 105 and 120%. This high ice nucleation efficiency was markedly suppressed by coating with SOA. About 20% of the ATD particles coated with a SOA mass fraction of 17 wt% were ice-active at RHi between 115 and 130%, and only 10% of the illite particles coated with an SOA mass fraction of 41 wt% were ice-active at RHi between 160 and 170%. Only a minor fraction of pure SOA particles were ice-active at RHi between 150 and 190%. Strong IN activation of SOA particles was observed only at RHi above 200%, which is clearly above water saturation at the given temperature. The IN suppression and the shift of the heterogeneous IN onset to higher RHi seem to depend on the coating thickness or the fractional surface coverage of the mineral particles. The results indicate that the heterogeneous ice nucleation potential of atmospheric mineral particles may also be suppressed if they are coated with secondary organics.
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International Nuclear Information System (INIS)
Moehler, O; Benz, S; Saathoff, H; Schnaiter, M; Wagner, R; Schneider, J; Walter, S; Ebert, V; Wagner, S
2008-01-01
The effect of organic coating on the heterogeneous ice nucleation (IN) efficiency of dust particles was investigated at simulated cirrus cloud conditions in the AIDA cloud chamber of Forschungszentrum Karlsruhe. Arizona test dust (ATD) and the clay mineral illite were used as surrogates for atmospheric dust aerosols. The dry dust samples were dispersed into a 3.7 m 3 aerosol vessel and either directly transferred into the 84 m 3 cloud simulation chamber or coated before with the semi-volatile products from the reaction of α-pinene with ozone in order to mimic the coating of atmospheric dust particles with secondary organic aerosol (SOA) substances. The ice-active fraction was measured in AIDA expansion cooling experiments as a function of the relative humidity with respect to ice, RHi, in the temperature range from 205 to 210 K. Almost all uncoated dust particles with diameters between 0.1 and 1.0 μm acted as efficient deposition mode ice nuclei at RHi between 105 and 120%. This high ice nucleation efficiency was markedly suppressed by coating with SOA. About 20% of the ATD particles coated with a SOA mass fraction of 17 wt% were ice-active at RHi between 115 and 130%, and only 10% of the illite particles coated with an SOA mass fraction of 41 wt% were ice-active at RHi between 160 and 170%. Only a minor fraction of pure SOA particles were ice-active at RHi between 150 and 190%. Strong IN activation of SOA particles was observed only at RHi above 200%, which is clearly above water saturation at the given temperature. The IN suppression and the shift of the heterogeneous IN onset to higher RHi seem to depend on the coating thickness or the fractional surface coverage of the mineral particles. The results indicate that the heterogeneous ice nucleation potential of atmospheric mineral particles may also be suppressed if they are coated with secondary organics
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Characterization of Ice Nucleating Particles at the Western US Coast
Rocci, K.; McCluskey, C. S.; Hill, T. C. J.; DeMott, P. J.; Kreidenweis, S. M.
2015-12-01
In temperate climates, ice nucleating particles (INPs) are vital for precipitation initiation. Because INPs may affect precipitation efficiency, and thereby the supply of water resources, it is paramount to have a clear understanding of both natural and anthropogenic sources of INPs. This is especially important to understand in California where drought continues to be a major problem. The CalWater 2015 field campaign, which took place in California from January 15 - March 9, 2015, included comprehensive characterizations of aerosols and their ice nucleating ability via ground-, air-, and ship-based measurements. As part of this campaign, we characterized and analyzed the intra-air mass differences of INPs at a coastal site (Bodega Bay) using immersion freezing measurements of particles collected on filters. Aerosol filters collected throughout the campaign were characterized by their loading and dominant type using meteorology, aerosol size distributions, aerosol composition, and trace gas concentration data. Samples contained a variety of aerosol influences, including biomass burning, nitrogen pollution, sulfur pollution, and sea spray. This study had a particular focus on the INP activity spectra of sea spray aerosol (SSA). We used the online aerosol data to infer variations in SSA types and heat-treated specific samples to look for the presence of heat-labile biological INPs. Furthermore, we ran the NOAA HYSPLIT model to obtain back trajectories for samples dominated by SSA. We found that air masses dominated by distinct terrestrial source types are not well distinguished by their INP number concentrations. However, we did see significantly higher (up to 5000-fold) INP number concentrations in SSA samples taken at the coast compared with number concentrations in samples obtained over open ocean. This difference could be attributable to differences in overall aerosol abundance, which will be evaluated in future studies. Overall, our findings suggest that an
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Creamean, J.; Spada, N. J.; Kirpes, R.; Pratt, K.
2017-12-01
Aerosols that serve as ice nucleating particles (INPs) have the potential to modulate cloud microphysical properties. INPs can thus subsequently impact cloud radiative forcing in addition to modification of precipitation formation processes. In regions such as the Arctic, aerosol-cloud interactions are severely understudied yet have significant implications for surface radiation reaching the sea ice and snow surfaces. Further, uncertainties in model representations of heterogeneous ice nucleation are a significant hindrance to simulating Arctic mixed-phase cloud processes. Characterizing a combination of aerosol chemical, physical, and ice nucleating properties is pertinent to evaluating of the role of aerosols in altering Arctic cloud microphysics. We present preliminary results from an aerosol sampling campaign called INPOP (Ice Nucleating Particles at Oliktok Point), which took place at a U.S. Department of Energy's Atmospheric Radiation Measurement (DOE ARM) facility on the North Slope of Alaska. Three time- and size-resolved aerosol samplers were deployed from 1 Mar to 31 May 2017 and were co-located with routine measurements of aerosol number, size, chemical, and radiative property measurements conducted by DOE ARM at their Aerosol Observing System (AOS). Offline analysis of samples collected at a daily time resolution included composition and morphology via single-particle analysis and drop freezing measurements for INP concentrations, while analysis of 12-hourly samples included mass, optical, and elemental composition. We deliberate the possible influences on the aerosol and INP population from the Prudhoe Bay oilfield resource extraction and daily operations in addition to what may be local background or long-range transported aerosol. To our knowledge our results represent some of the first INP characterization measurements in an Arctic oilfield location and can be used as a benchmark for future INP characterization studies in Arctic locations impacted
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Directory of Open Access Journals (Sweden)
R. J. Cotton
2007-01-01
Full Text Available The AIDA (Aerosol Interactions and Dynamics in the Atmosphere aerosol and cloud chamber of Forschungszentrum Karlsruhe can be used to test the ice forming ability of aerosols. The AIDA chamber is extensively instrumented including pressure, temperature and humidity sensors, and optical particle counters. Expansion cooling using mechanical pumps leads to ice supersaturation conditions and possible ice formation. In order to describe the evolving chamber conditions during an expansion, a parcel model was modified to account for diabatic heat and moisture interactions with the chamber walls. Model results are shown for a series of expansions where the initial chamber temperature ranged from −20°C to −60°C and which used desert dust as ice forming nuclei. During each expansion, the initial formation of ice particles was clearly observed. For the colder expansions there were two clear ice nucleation episodes. In order to test the ability of the model to represent the changing chamber conditions and to give confidence in the observations of chamber temperature and humidity, and ice particle concentration and mean size, ice particles were simply added as a function of time so as to reproduce the observations of ice crystal concentration. The time interval and chamber conditions over which ice nucleation occurs is therefore accurately known, and enables the model to be used as a test bed for different representations of ice formation.
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Ice nucleating particles in the high Arctic at the beginning of the melt season
Hartmann, M.; Gong, X.; Van Pinxteren, M.; Welti, A.; Zeppenfeld, S.; Herrmann, H.; Stratmann, F.
2017-12-01
Ice nucleating particles (INPs) initiate the ice crystal formation in persistent Arctic mixed-phase clouds and are important for the formation of precipitation, which affects the radiative properties of the Arctic pack ice as well as the radiative properties of clouds. Sources of Arctic INP have been suggested to be local emissions from the marine boundary and long-range transport. To what extent local marine sources contribute to the INP population or if the majority of INPs originate from long-range transport is not yet known. Ship-based INP measurements in the PASCAL framework are reported. The field campaign took place from May 24 to July 20 2017 around and north of Svalbard (up to 84°N, between 0° and 35°E) onboard the RV Polarstern. INP concentrations were determined applying in-situ measurements (DMT Spectrometer for Ice Nuclei, SPIN) and offline filter techniques (filter sampling on both quartz fiber and polycarbonate filters with subsequent analysis of filter pieces and water suspension from particles collected on filters by means of immersion freezing experiments on cold stage setups). Additionally the compartments sea-surface micro layer (SML), bulk sea water, snow, sea ice and fog water were sampled and their ice nucleation potential quantified, also utilizing cold stages. The measurements yield comprehensive picture of the spatial and temporal distribution of INPs around Svalbard for the different compartments. The dependence of the INP concentration on meteorological conditions (e.g. wind speed) and the geographical situation (sea ice cover, distance to the ice edge) are investigated. Potential sources of INP are identified by the comparison of INP concentrations in the compartments and by back trajectory analysis.
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Energy Technology Data Exchange (ETDEWEB)
Diehl, K; Mitra, S K; Pruppacher, H R [Johannes Gutenberg Univ., Mainz (Germany). Inst. fuer Physik der Atmosphaere
1998-12-31
Laboratory experiments are described during which the influence of the exhausts of a kerosene burner on microphysical processes were studied. In one experimental investigation the evaporation rates of polluted ice crystals were compared with the evaporation rates of pure ice crystals. During another experimental investigation the ice nucleating ability of the exhaust particles was studied. The results show that the evaporation rate of polluted ice crystals was significantly reduced and also that ice nucleation takes place between -20 and -38 deg C. (author) 7 refs.
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Energy Technology Data Exchange (ETDEWEB)
Diehl, K.; Mitra, S.K.; Pruppacher, H.R. [Johannes Gutenberg Univ., Mainz (Germany). Inst. fuer Physik der Atmosphaere
1997-12-31
Laboratory experiments are described during which the influence of the exhausts of a kerosene burner on microphysical processes were studied. In one experimental investigation the evaporation rates of polluted ice crystals were compared with the evaporation rates of pure ice crystals. During another experimental investigation the ice nucleating ability of the exhaust particles was studied. The results show that the evaporation rate of polluted ice crystals was significantly reduced and also that ice nucleation takes place between -20 and -38 deg C. (author) 7 refs.
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Peckhaus, Andreas; Bachmann, Felix; Hoffmann, Nadine; Koch, Michael; Kiselev, Alexei; Leisner, Thomas
2015-04-01
Recently K-feldspar was identified as one of the most active atmospheric ice nucleating particles (INP) of mineral origin [1]. Seeking the explanation to this phenomena we have conducted extensive experimental investigation of the ice nucleating efficiency of K-feldspar in three heterogeneous freezing modes. The immersion freezing of K-feldspar was investigated with the cold stage using arrays of nanoliter-size droplets containing aqueous suspension of polydisperse feldspar particles. For contact freezing, the charged droplets of supercooled water were suspended in the laminar flow of the DMA-selected feldspar-containing particles, allowing for determination of freezing probability on a single particle-droplet contact [2]. The nucleation and growth of ice via vapor deposition on the crystalline surfaces of macroscopic feldspar particles have been investigated in the Environmental Scanning Electron Microscope (ESEM) under humidified nitrogen atmosphere. The ice nucleation experiments were supplemented with measurements of effective surface area of feldspar particles and ion chromatography (IC) analysis of the leached framework cations (K+, Na+, Ca2+, Mg2+). In this contribution we focus on the role of surface chemistry influencing the IN efficiency of K-feldspar, in particular the connection between the degree of surface hydroxylation and its ability to induce local structural ordering in the interfacial layer in water molecules (as suggested by recent modeling efforts). We mimic the natural process of feldspar ageing by suspending it in water or weak aqueous solution of carbonic acid for different time periods, from minutes to months, and present its freezing efficiency as a function of time. Our immersion freezing experiments show that ageing have a nonlinear effect on the freezing behavior of feldspar within the investigated temperature range (-40°C to -10°C). On the other hand, deposition nucleation of ice observed in the ESEM reveals clear different pattern
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Beall, Charlotte M.; Stokes, M. Dale; Hill, Thomas C.; DeMott, Paul J.; DeWald, Jesse T.; Prather, Kimberly A.
2017-07-01
Ice nucleating particles (INPs) influence cloud properties and can affect the overall precipitation efficiency. Developing a parameterization of INPs in global climate models has proven challenging. More INP measurements - including studies of their spatial distribution, sources and sinks, and fundamental freezing mechanisms - must be conducted in order to further improve INP parameterizations. In this paper, an immersion mode INP measurement technique is modified and automated using a software-controlled, real-time image stream designed to leverage optical changes of water droplets to detect freezing events. For the first time, heat transfer properties of the INP measurement technique are characterized using a finite-element-analysis-based heat transfer simulation to improve accuracy of INP freezing temperature measurement. The heat transfer simulation is proposed as a tool that could be used to explain the sources of bias in temperature measurements in INP measurement techniques and ultimately explain the observed discrepancies in measured INP freezing temperatures between different instruments. The simulation results show that a difference of +8.4 °C between the well base temperature and the headspace gas results in an up to 0.6 °C stratification of the aliquot, whereas a difference of +4.2 °C or less results in a thermally homogenous water volume within the error of the thermal probe, ±0.2 °C. The results also show that there is a strong temperature gradient in the immediate vicinity of the aliquot, such that without careful placement of temperature probes, or characterization of heat transfer properties of the water and cooling environment, INP measurements can be biased toward colder temperatures. Based on a modified immersion mode technique, the Automated Ice Spectrometer (AIS), measurements of the standard test dust illite NX are reported and compared against six other immersion mode droplet assay techniques featured in Hiranuma et al. (2015) that used
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Directory of Open Access Journals (Sweden)
Thomas Häusler
2018-04-01
Full Text Available We are presenting a new approach to analyze the freezing behavior of aqueous droplets containing ice nucleating particles. The freezing chip consists of an etched and sputtered (15 × 15 × 1 mm gold-plated silicon or pure gold chip, enabling the formation of droplets with defined diameters between 20 and 80 µm. Several applications like an automated process control and an automated image evaluation were implemented to improve the quality of heterogeneous freezing experiments. To show the functionality of the setup, we compared freezing temperatures of aqueous droplets containing ice nucleating particles (i.e., microcline, birch pollen washing water, juniper pollen, and Snomax® solution measured with our setup, with literature data. The ice nucleation active surface/mass site density (ns/m of microcline, juniper pollen, and birch pollen washing water are shown to be in good agreement with literature data. Minor variations can be explained by slight differences in composition and droplet generation technique. The nm values of Snomax® differ by up to one order of magnitude at higher subzero temperatures when compared with fresh samples but are in agreement when compared with reported data of aged Snomax® samples.
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Palaiomylitou, M A; Kalimanis, A; Koukkou, A I; Drainas, C; Anastassopoulos, E; Panopoulos, N J; Ekateriniadou, L V; Kyriakidis, D A
1998-08-01
Ice nucleation protein was partially purified from the membrane fraction of E. coli carrying inaZ from Pseudomonas syringae. The ice nucleation protein was totally localized in the bacterial envelope and was extracted by either salt (0.25 M NH4Cl) or the nonionic detergent Tween 20. The extracted protein was partially purified by sequential passage through DEAE-52 cellulose and Sephacryl-S400 columns. The activity of the purified protein was lost after treatment with phospholipase C, and its activity was subsequently restored by addition of the naturally occurring lipid phosphatidylethanolamine. These results suggest that ice nucleation proteins have a requirement for lipids that reconstitute a physiological hydrophobic environment similar to the one existing in vivo, to attain and maintain a structure that enables ice catalysis. Copyright 1998 Academic Press.
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Directory of Open Access Journals (Sweden)
D. Barahona
2009-01-01
Full Text Available We present a parameterization of cirrus cloud formation that computes the ice crystal number and size distribution under the presence of homogeneous and heterogeneous freezing. The parameterization is very simple to apply and is derived from the analytical solution of the cloud parcel equations, assuming that the ice nuclei population is monodisperse and chemically homogeneous. In addition to the ice distribution, an analytical expression is provided for the limiting ice nuclei number concentration that suppresses ice formation from homogeneous freezing. The parameterization is evaluated against a detailed numerical parcel model, and reproduces numerical simulations over a wide range of conditions with an average error of 6±33%. The parameterization also compares favorably against other formulations that require some form of numerical integration.
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Heterogeneous nucleation from a supercooled ionic liquid on a carbon surface.
He, Xiaoxia; Shen, Yan; Hung, Francisco R; Santiso, Erik E
2016-12-07
Classical molecular dynamics simulations were used to study the nucleation of the crystal phase of the ionic liquid [dmim + ][Cl - ] from its supercooled liquid phase, both in the bulk and in contact with a graphitic surface of D = 3 nm. By combining the string method in collective variables [Maragliano et al., J. Chem. Phys. 125, 024106 (2006)], with Markovian milestoning with Voronoi tessellations [Maragliano et al., J. Chem. Theory Comput. 5, 2589-2594 (2009)] and order parameters for molecular crystals [Santiso and Trout, J. Chem. Phys. 134, 064109 (2011)], we computed minimum free energy paths, the approximate size of the critical nucleus, the free energy barrier, and the rates involved in these nucleation processes. For homogeneous nucleation, the subcooled liquid phase has to overcome a free energy barrier of ∼85 kcal/mol to form a critical nucleus of size ∼3.6 nm, which then grows into the monoclinic crystal phase. This free energy barrier becomes about 42% smaller (∼49 kcal/mol) when the subcooled liquid phase is in contact with a graphitic disk, and the critical nucleus formed is about 17% smaller (∼3.0 nm) than the one observed for homogeneous nucleation. The crystal formed in the heterogeneous nucleation scenario has a structure that is similar to that of the bulk crystal, with the exception of the layers of ions next to the graphene surface, which have larger local density and the cations lie with their imidazolium rings parallel to the graphitic surface. The critical nucleus forms near the graphene surface separated only by these layers of ions. The heterogeneous nucleation rate (∼4.8 × 10 11 cm -3 s -1 ) is about one order of magnitude faster than the homogeneous rate (∼6.6 × 10 10 cm -3 s -1 ). The computed free energy barriers and nucleation rates are in reasonable agreement with experimental and simulation values obtained for the homogeneous and heterogeneous nucleation of other systems (ice, urea, Lennard-Jones spheres, and oxide
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Overview: Nucleation of clathrate hydrates.
Warrier, Pramod; Khan, M Naveed; Srivastava, Vishal; Maupin, C Mark; Koh, Carolyn A
2016-12-07
Molecular level knowledge of nucleation and growth of clathrate hydrates is of importance for advancing fundamental understanding on the nature of water and hydrophobic hydrate formers, and their interactions that result in the formation of ice-like solids at temperatures higher than the ice-point. The stochastic nature and the inability to probe the small length and time scales associated with the nucleation process make it very difficult to experimentally determine the molecular level changes that lead to the nucleation event. Conversely, for this reason, there have been increasing efforts to obtain this information using molecular simulations. Accurate knowledge of how and when hydrate structures nucleate will be tremendously beneficial for the development of sustainable hydrate management strategies in oil and gas flowlines, as well as for their application in energy storage and recovery, gas separation, carbon sequestration, seawater desalination, and refrigeration. This article reviews various aspects of hydrate nucleation. First, properties of supercooled water and ice nucleation are reviewed briefly due to their apparent similarity to hydrates. Hydrate nucleation is then reviewed starting from macroscopic observations as obtained from experiments in laboratories and operations in industries, followed by various hydrate nucleation hypotheses and hydrate nucleation driving force calculations based on the classical nucleation theory. Finally, molecular simulations on hydrate nucleation are discussed in detail followed by potential future research directions.
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Overview: Nucleation of clathrate hydrates
Warrier, Pramod; Khan, M. Naveed; Srivastava, Vishal; Maupin, C. Mark; Koh, Carolyn A.
2016-12-01
Molecular level knowledge of nucleation and growth of clathrate hydrates is of importance for advancing fundamental understanding on the nature of water and hydrophobic hydrate formers, and their interactions that result in the formation of ice-like solids at temperatures higher than the ice-point. The stochastic nature and the inability to probe the small length and time scales associated with the nucleation process make it very difficult to experimentally determine the molecular level changes that lead to the nucleation event. Conversely, for this reason, there have been increasing efforts to obtain this information using molecular simulations. Accurate knowledge of how and when hydrate structures nucleate will be tremendously beneficial for the development of sustainable hydrate management strategies in oil and gas flowlines, as well as for their application in energy storage and recovery, gas separation, carbon sequestration, seawater desalination, and refrigeration. This article reviews various aspects of hydrate nucleation. First, properties of supercooled water and ice nucleation are reviewed briefly due to their apparent similarity to hydrates. Hydrate nucleation is then reviewed starting from macroscopic observations as obtained from experiments in laboratories and operations in industries, followed by various hydrate nucleation hypotheses and hydrate nucleation driving force calculations based on the classical nucleation theory. Finally, molecular simulations on hydrate nucleation are discussed in detail followed by potential future research directions.
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Liu, X.; Shi, Y.; Wu, M.; Zhang, K.
2017-12-01
Mixed-phase clouds frequently observed in the Arctic and mid-latitude storm tracks have the substantial impacts on the surface energy budget, precipitation and climate. In this study, we first implement the two empirical parameterizations (Niemand et al. 2012 and DeMott et al. 2015) of heterogeneous ice nucleation for mixed-phase clouds in the NCAR Community Atmosphere Model Version 5 (CAM5) and DOE Accelerated Climate Model for Energy Version 1 (ACME1). Model simulated ice nucleating particle (INP) concentrations based on Niemand et al. and DeMott et al. are compared with those from the default ice nucleation parameterization based on the classical nucleation theory (CNT) in CAM5 and ACME, and with in situ observations. Significantly higher INP concentrations (by up to a factor of 5) are simulated from Niemand et al. than DeMott et al. and CNT especially over the dust source regions in both CAM5 and ACME. Interestingly the ACME model simulates higher INP concentrations than CAM5, especially in the Polar regions. This is also the case when we nudge the two models' winds and temperature towards the same reanalysis, indicating more efficient transport of aerosols (dust) to the Polar regions in ACME. Next, we examine the responses of model simulated cloud liquid water and ice water contents to different INP concentrations from three ice nucleation parameterizations (Niemand et al., DeMott et al., and CNT) in CAM5 and ACME. Changes in liquid water path (LWP) reach as much as 20% in the Arctic regions in ACME between the three parameterizations while the LWP changes are smaller and limited in the Northern Hemispheric mid-latitudes in CAM5. Finally, the impacts on cloud radiative forcing and dust indirect effects on mixed-phase clouds are quantified with the three ice nucleation parameterizations in CAM5 and ACME.
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Liu, X.; Wang, Y.; Zhang, D.; Wang, Z.
2016-12-01
Mixed-phase clouds consisting of both liquid and ice water occur frequently at high-latitudes and in mid-latitude storm track regions. This type of clouds has been shown to play a critical role in the surface energy balance, surface air temperature, and sea ice melting in the Arctic. Cloud phase partitioning between liquid and ice water determines the cloud optical depth of mixed-phase clouds because of distinct optical properties of liquid and ice hydrometeors. The representation and simulation of cloud phase partitioning in state-of-the-art global climate models (GCMs) are associated with large biases. In this study, the cloud phase partition in mixed-phase clouds simulated from the NCAR Community Atmosphere Model version 5 (CAM5) is evaluated against satellite observations. Observation-based supercooled liquid fraction (SLF) is calculated from CloudSat, MODIS and CPR radar detected liquid and ice water paths for clouds with cloud-top temperatures between -40 and 0°C. Sensitivity tests with CAM5 are conducted for different heterogeneous ice nucleation parameterizations with respect to aerosol influence (Wang et al., 2014), different phase transition temperatures for detrained cloud water from shallow convection (Kay et al., 2016), and different CAM5 model configurations (free-run versus nudged winds and temperature, Zhang et al., 2015). A classical nucleation theory-based ice nucleation parameterization in mixed-phase clouds increases the SLF especially at temperatures colder than -20°C, and significantly improves the model agreement with observations in the Arctic. The change of transition temperature for detrained cloud water increases the SLF at higher temperatures and improves the SLF mostly over the Southern Ocean. Even with the improved SLF from the ice nucleation and shallow cumulus detrainment, the low SLF biases in some regions can only be improved through the improved circulation with the nudging technique. Our study highlights the challenges of
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Perlwitz, J. P.; Knopf, D. A.; Fridlind, A. M.; Miller, R. L.; Pérez García-Pando, C.; DeMott, P. J.
2016-12-01
The effect of aerosol particles on the radiative properties of clouds, the so-called, indirect effect of aerosols, is recognized as one of the largest sources of uncertainty in climate prediction. The distribution of water vapor, precipitation, and ice cloud formation are influenced by the atmospheric ice formation, thereby modulating cloud albedo and thus climate. It is well known that different particle types possess different ice formation propensities with mineral dust being a superior ice nucleating particle (INP) compared to soot particles. Furthermore, some dust mineral types are more proficient INP than others, depending on temperature and relative humidity.In recent work, we have presented an improved dust aerosol module in the NASA GISS Earth System ModelE2 with prognostic mineral composition of the dust aerosols. Thus, there are regional variations in dust composition. We evaluated the predicted mineral fractions of dust aerosols by comparing them to measurements from a compilation of about 60 published literature references. Additionally, the capability of the model to reproduce the elemental composition of the simulated dusthas been tested at Izana Observatory at Tenerife, Canary Islands, which is located off-shore of Africa and where frequent dust events are observed. We have been able to show that the new approach delivers a robust improvement of the predicted mineral fractions and elemental composition of dust.In the current study, we use three-dimensional dust mineral fields and thermodynamic conditions, which are simulated using GISS ModelE, to calculate offline the INP concentrations derived using different ice nucleation parameterizations that are currently discussed. We evaluate the calculated INP concentrations from the different parameterizations by comparing them to INP concentrations from field measurements.
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Ahern, H. E.; Walsh, K. A.; Hill, T. C. J.; Moffett, B. F.
2006-10-01
Microorganisms were discovered in clouds over 100 years ago but information on bacterial community structure and function is limited. Clouds may not only be a niche within which bacteria could thrive but they might also influence dynamic processes using ice nucleating and cloud condensing abilities. Cloud and rain samples were collected from two mountains in the Outer Hebrides, NW Scotland, UK. Community composition was determined using a combination of amplified 16S ribosomal DNA restriction analysis and sequencing. 256 clones yielded 100 operational taxonomic units (OTUs) of which half were related to bacteria from terrestrial psychrophilic environments. Cloud samples were dominated by a mixture of fluorescent Pseudomonas spp., some of which have been reported to be ice nucleators. It was therefore possible that these bacteria were using the ice nucleation (IN) gene to trigger the Bergeron-Findeisen process of raindrop formation as a mechanism for dispersal. In this study the IN gene was not detected in any of the isolates using both polymerase chain reaction (PCR) and differential scanning calorimetry (DSC). Instead 55% of the total isolates from both cloud and rain samples displayed significant biosurfactant activity when analyzed using the drop-collapse technique. All were characterised as fluorescent pseudomonads. Surfactants have been found to be very important in lowering atmospheric critical supersaturations required for the activation of aerosols into cloud condensation nuclei (CCN). It is also known that surfactants influence cloud droplet size and increase cloud lifetime and albedo. Some bacteria are known to act as CCN and so it is conceivable that these fluorescent pseudomonads are using surfactants to facilitate their activation from aerosols into CCN. This would allow water scavenging, countering desiccation, and assist in their widespread dispersal.
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Growth Kinetics of the Homogeneously Nucleated Water Droplets: Simulation Results
International Nuclear Information System (INIS)
Mokshin, Anatolii V; Galimzyanov, Bulat N
2012-01-01
The growth of homogeneously nucleated droplets in water vapor at the fixed temperatures T = 273, 283, 293, 303, 313, 323, 333, 343, 353, 363 and 373 K (the pressure p = 1 atm.) is investigated on the basis of the coarse-grained molecular dynamics simulation data with the mW-model. The treatment of simulation results is performed by means of the statistical method within the mean-first-passage-time approach, where the reaction coordinate is associated with the largest droplet size. It is found that the water droplet growth is characterized by the next features: (i) the rescaled growth law is unified at all the considered temperatures and (ii) the droplet growth evolves with acceleration and follows the power law.
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Ice Nucleation and Dehydration in the Tropical Tropopause Layer
Jensen, Eric J.; Diskin, Glenn S.; Lawson, R Paul; Lance, Sara; Bui, Thaopaul Van; Hlavka, Dennis L.; Mcgill, Matthew J.; Pfister, Leonhard; Toon, Owen B.; Gao, Rushan
2013-01-01
Optically thin cirrus near the tropical tropopause regulate the humidity of air entering the stratosphere, which in turn has a strong influence on the Earth's radiation budget and climate. Recent highaltitude, unmanned aircraft measurements provide evidence for two distinct classes of cirrus formed in the tropical tropopause region: (i) vertically extensive cirrus with low ice number concentrations, low extinctions, and large supersaturations (up to approx. 70%) with respect to ice; and (ii) vertically thin cirrus layers with much higher ice concentrations that effectively deplete the vapor in excess of saturation. The persistent supersaturation in the former class of cirrus is consistent with the long time-scales (several hours or longer) for quenching of vapor in excess of saturation given the low ice concentrations and cold tropical tropopause temperatures. The low-concentration clouds are likely formed on a background population of insoluble particles with concentrations less than 100 L-1 (often less than 20 L-1), whereas the high ice concentration layers (with concentrations up to 10,000 L-1) can only be produced by homogeneous freezing of an abundant population of aqueous aerosols. These measurements, along with past high-altitude aircraft measurements, indicate that the low-concentration cirrus occur frequently in the tropical tropopause region, whereas the high-concentration cirrus occur infrequently. The predominance of the low-concentration clouds means cirrus near the tropical tropopause may typically allow entry of air into the stratosphere with as much as approx. 1.7 times the ice saturation mixing ratio.
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Kandler, Konrad; Worringen, Annette; Benker, Nathalie; Dirsch, Thomas; Mertes, Stephan; Schenk, Ludwig; Kästner, Udo; Frank, Fabian; Nillius, Björn; Bundke, Ulrich; Rose, Diana; Curtius, Joachim; Kupiszewski, Piotr; Weingartner, Ernest; Vochezer, Paul; Schneider, Johannes; Schmidt, Susan; Weinbruch, Stephan; Ebert, Martin
2015-04-01
During January/February 2013, at the High Alpine Research Station Jungfraujoch a measurement campaign was carried out, which was centered on atmospheric ice-nucleating particles (INP) and ice particle residuals (IPR). Three different techniques for separation of INP and IPR from the non-ice-active particles are compared. The Ice Selective Inlet (ISI) and the Ice Counterflow Virtual Impactor (Ice-CVI) sample ice particles from mixed phase clouds and allow for the analysis of the residuals. The combination of the Fast Ice Nucleus Chamber (FINCH) and the Ice Nuclei Pumped Counterflow Virtual Impactor (IN-PCVI) provides ice-activating conditions to aerosol particles and extracts the activated INP for analysis. Collected particles were analyzed by scanning electron microscopy and energy-dispersive X-ray microanalysis to determine size, chemical composition and mixing state. All INP/IPR-separating techniques had considerable abundances (median 20 - 70 %) of instrumental contamination artifacts (ISI: Si-O spheres, probably calibration aerosol; Ice-CVI: Al-O particles; FINCH+IN-PCVI: steel particles). Also, potential sampling artifacts (e.g., pure soluble material) occurred with a median abundance of separated by all three techniques. Soot was a minor contributor. Lead was detected in less than 10 % of the particles, of which the majority were internal mixtures with other particle types. Sea-salt and sulfates were identified by all three methods as INP/IPR. Most samples showed a maximum of the INP/IPR size distribution at 400 nm geometric diameter. In a few cases, a second super-micron maximum was identified. Soot/carbonaceous material and metal oxides were present mainly in the submicron range. ISI and FINCH yielded silicates and Ca-rich particles mainly with diameters above 1 µm, while the Ice-CVI also separated many submicron IPR. As strictly parallel sampling could not be performed, a part of the discrepancies between the different techniques may result from
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Properties of subvisible cirrus clouds formed by homogeneous freezing
Directory of Open Access Journals (Sweden)
B. Kärcher
2002-01-01
Full Text Available Number concentrations and mean sizes of ice crystals and derived microphysical and optical properties of subvisible cirrus clouds (SVCs formed by homogeneous freezing of supercooled aerosols are investigated as a function of temperature and updraft speed of adiabatically ascending air parcels. The properties of such clouds are insensitive to variations of the aerosol number and size distribution. Based on criteria constraining the optical extinction, sedimentation time, and existence time of SVCs, longer-lived (>10min clouds, capable of exerting a measurable radiative or chemical impact, are generated within a narrow range of updraft speeds below 1-2cm s-1 at temperatures below about 215K, with concentrations of ice crystals not exceeding 0.1cm-3. The clouds do not reach an equilibrium state because the ice crystals sediment out of the formation layer typically before the supersaturation is removed. Two important conclusions emerge from this work. First, the above characteristics of SVCs may provide an explanation for why SVCs are more common in the cold tropical than in the warmer midlatitude tropopause region. Second, it seems likely that a limited number (-3 of effective heterogeneous freezing nuclei that nucleate ice below the homogeneous freezing threshold can control the formation and properties of SVCs, although homogeneous freezing nuclei are far more abundant.
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Onischuk, A A; Purtov, P A; Baklanov, A M; Karasev, V V; Vosel, S V
2006-01-07
Zinc and silver vapor homogeneous nucleations are studied experimentally at the temperature from 600 to 725 and 870 K, respectively, in a laminar flow diffusion chamber with Ar as a carrier gas at atmospheric pressure. The size, shape, and concentration of aerosol particles outcoming the diffusion chamber are analyzed by a transmission electron microscope and an automatic diffusion battery. The wall deposit is studied by a scanning electron microscope (SEM). Using SEM data the nucleation rate for both Zn and Ag is estimated as 10(10) cm(-3) s(-1). The dependence of critical supersaturation on temperature for Zn and Ag measured in this paper as well as Li, Na, Cs, Ag, Mg, and Hg measured elsewhere is analyzed. To this aim the classical nucleation theory is extended by the dependence of surface tension on the nucleus radius. The preexponent in the formula for the vapor nucleation rate is derived using the formula for the work of formation of noncritical embryo [obtained by Nishioka and Kusaka [J. Chem. Phys. 96, 5370 (1992)] and later by Debenedetti and Reiss [J. Chem. Phys. 108, 5498 (1998)
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Temperature Dependence in Homogeneous and Heterogeneous Nucleation
Energy Technology Data Exchange (ETDEWEB)
McGraw R. L.; Winkler, P. M.; Wagner, P. E.
2017-08-01
Heterogeneous nucleation on stable (sub-2 nm) nuclei aids the formation of atmospheric cloud condensation nuclei (CCN) by circumventing or reducing vapor pressure barriers that would otherwise limit condensation and new particle growth. Aerosol and cloud formation depend largely on the interaction between a condensing liquid and the nucleating site. A new paper published this year reports the first direct experimental determination of contact angles as well as contact line curvature and other geometric properties of a spherical cap nucleus at nanometer scale using measurements from the Vienna Size Analyzing Nucleus Counter (SANC) (Winkler et al., 2016). For water nucleating heterogeneously on silver oxide nanoparticles we find contact angles around 15 degrees compared to around 90 degrees for the macroscopically measured equilibrium angle for water on bulk silver. The small microscopic contact angles can be attributed via the generalized Young equation to a negative line tension that becomes increasingly dominant with increasing curvature of the contact line. These results enable a consistent theoretical description of heterogeneous nucleation and provide firm insight to the wetting of nanosized objects.
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Kumar, A.; Marcolli, C.; Luo, B.; Krieger, U. K.; Peter, T.
2017-12-01
Semivolatile species present in the atmosphere are prone to adhere to mineral dust particle surfaces during long range transport, and could potentially change the particle surface properties and its ice nucleation (IN) efficiency. Immersion freezing experiments were performed with microcline (K-feldspar), known to be highly IN active, suspended in aqueous solutions of ammonia, (NH4)2SO4, NH4HSO4, NH4NO3, NH4Cl, Na2SO4, H2SO4, K2SO4 and KCl to investigate the effect of solutes on the IN efficiency. Freezing of emulsified droplets investigated with a differential scanning calorimeter (DSC) showed that the heterogeneous ice nucleation temperatures deviate from the water activity-based IN theory, describing heterogeneous ice nucleation temperatures as a function of solution water activity by a constant offset with respect to the ice melting point curve (Zobrist et al. 2008). IN temperatures enhanced up to 4.5 K were observed for very dilute NH3 and NH4+-containing solutions while a decrease was observed as the concentration was further increased. For all solutes with cations other than NH4+, the IN efficiency decreased. An increase of the IN efficiency in very dilute NH3 and NH4+-containing solutions followed by a decrease with increasing concentration was also observed for sanidine (K-feldspar) and andesine (Na/Ca-feldspar). This is an important indication towards specific chemical interactions between solutes and the feldspar surface which is not captured by the water activity-based IN theory. A similar trend is present but less pronounced in case of kaolinite and mica, while quartz is barely affected. We hypothesize that the hydrogen bonding of NH3 molecules with surface -OH groups could be the reason for the enhanced freezing temperatures in dilute ammonia and ammonium containing solutions as they could form an ice-like overlayer providing hydrogen bonding groups for ice to nucleate on top of it. This implies to possibilities of enhanced IN efficiency, especially
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The Gibbs free energy of homogeneous nucleation: From atomistic nuclei to the planar limit.
Cheng, Bingqing; Tribello, Gareth A; Ceriotti, Michele
2017-09-14
In this paper we discuss how the information contained in atomistic simulations of homogeneous nucleation should be used when fitting the parameters in macroscopic nucleation models. We show how the number of solid and liquid atoms in such simulations can be determined unambiguously by using a Gibbs dividing surface and how the free energy as a function of the number of solid atoms in the nucleus can thus be extracted. We then show that the parameters (the chemical potential, the interfacial free energy, and a Tolman correction) of a model based on classical nucleation theory can be fitted using the information contained in these free-energy profiles but that the parameters in such models are highly correlated. This correlation is unfortunate as it ensures that small errors in the computed free energy surface can give rise to large errors in the extrapolated properties of the fitted model. To resolve this problem we thus propose a method for fitting macroscopic nucleation models that uses simulations of planar interfaces and simulations of three-dimensional nuclei in tandem. We show that when the chemical potentials and the interface energy are pinned to their planar-interface values, more precise estimates for the Tolman length are obtained. Extrapolating the free energy profile obtained from small simulation boxes to larger nuclei is thus more reliable.
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Kishimoto, Tadashi; Yamazaki, Hideyuki; Saruwatari, Atsushi; Murakawa, Hiroki; Sekozawa, Yoshihiko; Kuchitsu, Kazuyuki; Price, William S.; Ishikawa, Masaya
2014-01-01
Controlled ice nucleation is an important mechanism in cold-hardy plant tissues for avoiding excessive supercooling of the protoplasm, for inducing extracellular freezing and/or for accommodating ice crystals in specific tissues. To understand its nature, it is necessary to characterize the ice nucleation activity (INA), defined as the ability of a tissue to induce heterogeneous ice nucleation. Few studies have addressed the precise localization of INA in wintering plant tissues in respect of its function. For this purpose, we recently revised a test tube INA assay and examined INA in various tissues of over 600 species. Extremely high levels of INA (−1 to −4 °C) in two wintering blueberry cultivars of contrasting freezing tolerance were found. Their INA was much greater than in other cold-hardy species and was found to be evenly distributed along the stems of the current year's growth. Concentrations of active ice nuclei in the stem were estimated from quantitative analyses. Stem INA was localized mainly in the bark while the xylem and pith had much lower INA. Bark INA was located mostly in the cell wall fraction (cell walls and intercellular structural components). Intracellular fractions had much less INA. Some cultivar differences were identified. The results corresponded closely with the intrinsic freezing behaviour (extracellular freezing) of the bark, icicle accumulation in the bark and initial ice nucleation in the stem under dry surface conditions. Stem INA was resistant to various antimicrobial treatments. These properties and specific localization imply that high INA in blueberry stems is of intrinsic origin and contributes to the spontaneous initiation of freezing in extracellular spaces of the bark by acting as a subfreezing temperature sensor. PMID:25082142
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Homogeneous nucleation in phase separation of solid 3He-4He mixtures
International Nuclear Information System (INIS)
Poole, M.; Smith, A.; Maidanov, V.A.; Rudavskii, E.Ya.; Grigor'ev, V.N.; Slezov, V.V.; Saunders, J.; Cowan, B.
2003-01-01
NMR and pressure have been measured during phase separation in solid 3 He- 4 He mixtures. Spin echoes were used to observe bounded diffusion and to estimate the diffusion coefficient, size and nuclei concentration in the 3 He-enriched phase. The characteristic phase separation time constant of the mixture was found from pressure measurements. The results argue convincingly for homogeneous nucleation. The surface tension of the nuclei is found independently from NMR and from pressure measurements; the two determinations agree well and yield a surface tension coefficient of 4.9x10 -6 J m -2
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Ice nucleation and dehydration in the Tropical Tropopause Layer.
Jensen, Eric J; Diskin, Glenn; Lawson, R Paul; Lance, Sara; Bui, T Paul; Hlavka, Dennis; McGill, Matthew; Pfister, Leonhard; Toon, Owen B; Gao, Rushan
2013-02-05
Optically thin cirrus near the tropical tropopause regulate the humidity of air entering the stratosphere, which in turn has a strong influence on the Earth's radiation budget and climate. Recent high-altitude, unmanned aircraft measurements provide evidence for two distinct classes of cirrus formed in the tropical tropopause region: (i) vertically extensive cirrus with low ice number concentrations, low extinctions, and large supersaturations (up to ∼70%) with respect to ice; and (ii) vertically thin cirrus layers with much higher ice concentrations that effectively deplete the vapor in excess of saturation. The persistent supersaturation in the former class of cirrus is consistent with the long time-scales (several hours or longer) for quenching of vapor in excess of saturation given the low ice concentrations and cold tropical tropopause temperatures. The low-concentration clouds are likely formed on a background population of insoluble particles with concentrations less than 100 L(-1) (often less than 20 L(-1)), whereas the high ice concentration layers (with concentrations up to 10,000 L(-1)) can only be produced by homogeneous freezing of an abundant population of aqueous aerosols. These measurements, along with past high-altitude aircraft measurements, indicate that the low-concentration cirrus occur frequently in the tropical tropopause region, whereas the high-concentration cirrus occur infrequently. The predominance of the low-concentration clouds means cirrus near the tropical tropopause may typically allow entry of air into the stratosphere with as much as ∼1.7 times the ice saturation mixing ratio.
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Weber, Daniel; Schrod, Jann; Curtius, Joachim; Haunold, Werner; Thomson, Erik; Bingemer, Heinz
2016-04-01
The measurement of atmospheric ice nucleating particles (INP) is still challenging. In the absence of easily applicable INP standards the intercomparison of different methods during collaborative laboratory and field workshops is a valuable tool that can shine light on the performance of individual methods for the measurement of INP [1]. FIN-2 was conducted in March 2015 at the AIDA facility in Karlsruhe as an intercomparison of mobile instruments for measuring INP [2]. FIN-3 was a field campaign at the Desert Research Institutes Storm Peak Laboratory in Colorado in September 2015 [3]. The FRankfurt Ice nucleation Deposition freezinG Experiment (FRIDGE) participated in both experiments. FRIDGE measures ice nucleating particles by electrostatic precipitation of aerosol particles onto Si-wafers in a collection unit, followed by activation, growth, and optical detection of ice crystals on the substrate in an isostatic diffusion chamber [4,5]. We will present and discuss results of our measurements of deposition/condensation INP and of immersion INP with FRIDGE during FIN-2 and FIN-3. Acknowledgements: The valuable contributions of the FIN organizers and their institutions, and of the FIN Workshop Science team are gratefully acknowledged. Our work was supported by Deutsche Forschungsgemeinschaft (DFG) under the Research Unit FOR 1525 (INUIT) and the EU FP7-ENV- 2013 BACCHUS project under Grant Agreement 603445.
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Ice nucleation efficiency of clay minerals in the immersion mode
Directory of Open Access Journals (Sweden)
V. Pinti
2012-07-01
Full Text Available Emulsion and bulk freezing experiments were performed to investigate immersion ice nucleation on clay minerals in pure water, using various kaolinites, montmorillonites, illites as well as natural dust from the Hoggar Mountains in the Saharan region. Differential scanning calorimeter measurements were performed on three different kaolinites (KGa-1b, KGa-2 and K-SA, two illites (Illite NX and Illite SE and four natural and acid-treated montmorillonites (SWy-2, STx-1b, KSF and K-10. The emulsion experiments provide information on the average freezing behaviour characterized by the average nucleation sites. These experiments revealed one to sometimes two distinct heterogeneous freezing peaks, which suggest the presence of a low number of qualitatively distinct average nucleation site classes. We refer to the peak at the lowest temperature as "standard peak" and to the one occurring in only some clay mineral types at higher temperatures as "special peak". Conversely, freezing in bulk samples is not initiated by the average nucleation sites, but by a very low number of "best sites". The kaolinites and montmorillonites showed quite narrow standard peaks with onset temperatures 238 K<Tonstd<242 K and best sites with averaged median freezing temperature Tmedbest=257 K, but only some featuring a special peak (i.e. KSF, K-10, K-SA and SWy-2 with freezing onsets in the range 240–248 K. The illites showed broad standard peaks with freezing onsets at 244 K Tonstd<246 K and best sites with averaged median freezing temperature Tmedbest=262 K. The large difference between freezing temperatures of standard and best sites shows that characterizing ice nucleation efficiencies of dust particles on the basis of freezing onset temperatures from bulk experiments, as has been done in some atmospheric studies, is not appropriate. Our investigations
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Czech Academy of Sciences Publication Activity Database
Neitola, K.; Hyvärinen, A.-P.; Lihavainen, H.; Wölk, J.; Strey, R.; Brus, David
2014-01-01
Roč. 140, č. 17 (2014), č. článku 174301. ISSN 0021-9606 Grant - others:AFCE(FI) 1118615 Institutional support: RVO:67985858 Keywords : carbon-chain length * equilibrium vapor * homogenous nucleation Subject RIV: CF - Physical ; Theoretical Chemistry OBOR OECD: Physical chemistry Impact factor: 2.952, year: 2014
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Directory of Open Access Journals (Sweden)
T. Maki
2018-06-01
Full Text Available The westerly wind travelling at high altitudes over eastern Asia transports aerosols from the Asian deserts and urban areas to downwind areas such as Japan. These long-range-transported aerosols include not only mineral particles but also microbial particles (bioaerosols, that impact the ice-cloud formation processes as ice nuclei. However, the detailed relations of airborne bacterial dynamics to ice nucleation in high-elevation aerosols have not been investigated. Here, we used the aerosol particles captured in the snow cover at altitudes of 2450 m on Mt Tateyama to investigate sequential changes in the ice-nucleation activities and bacterial communities in aerosols and elucidate the relationships between the two processes. After stratification of the snow layers formed on the walls of a snow pit on Mt Tateyama, snow samples, including aerosol particles, were collected from 70 layers at the lower (winter accumulation and upper (spring accumulation parts of the snow wall. The aerosols recorded in the lower parts mainly came from Siberia (Russia, northern Asia and the Sea of Japan, whereas those in the upper parts showed an increase in Asian dust particles originating from the desert regions and industrial coasts of Asia. The snow samples exhibited high levels of ice nucleation corresponding to the increase in Asian dust particles. Amplicon sequencing analysis using 16S rRNA genes revealed that the bacterial communities in the snow samples predominately included plant associated and marine bacteria (phyla Proteobacteria during winter, whereas during spring, when dust events arrived frequently, the majority were terrestrial bacteria of phyla Actinobacteria and Firmicutes. The relative abundances of Firmicutes (Bacilli showed a significant positive relationship with the ice nucleation in snow samples. Presumably, Asian dust events change the airborne bacterial communities over Mt Tateyama and carry terrestrial bacterial populations, which
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Maki, Teruya; Furumoto, Shogo; Asahi, Yuya; Lee, Kevin C.; Watanabe, Koichi; Aoki, Kazuma; Murakami, Masataka; Tajiri, Takuya; Hasegawa, Hiroshi; Mashio, Asami; Iwasaka, Yasunobu
2018-06-01
The westerly wind travelling at high altitudes over eastern Asia transports aerosols from the Asian deserts and urban areas to downwind areas such as Japan. These long-range-transported aerosols include not only mineral particles but also microbial particles (bioaerosols), that impact the ice-cloud formation processes as ice nuclei. However, the detailed relations of airborne bacterial dynamics to ice nucleation in high-elevation aerosols have not been investigated. Here, we used the aerosol particles captured in the snow cover at altitudes of 2450 m on Mt Tateyama to investigate sequential changes in the ice-nucleation activities and bacterial communities in aerosols and elucidate the relationships between the two processes. After stratification of the snow layers formed on the walls of a snow pit on Mt Tateyama, snow samples, including aerosol particles, were collected from 70 layers at the lower (winter accumulation) and upper (spring accumulation) parts of the snow wall. The aerosols recorded in the lower parts mainly came from Siberia (Russia), northern Asia and the Sea of Japan, whereas those in the upper parts showed an increase in Asian dust particles originating from the desert regions and industrial coasts of Asia. The snow samples exhibited high levels of ice nucleation corresponding to the increase in Asian dust particles. Amplicon sequencing analysis using 16S rRNA genes revealed that the bacterial communities in the snow samples predominately included plant associated and marine bacteria (phyla Proteobacteria) during winter, whereas during spring, when dust events arrived frequently, the majority were terrestrial bacteria of phyla Actinobacteria and Firmicutes. The relative abundances of Firmicutes (Bacilli) showed a significant positive relationship with the ice nucleation in snow samples. Presumably, Asian dust events change the airborne bacterial communities over Mt Tateyama and carry terrestrial bacterial populations, which possibly induce ice-nucleation
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Knopf, Daniel A; Alpert, Peter A
2013-01-01
Immersion freezing of water and aqueous solutions by particles acting as ice nuclei (IN) is a common process of heterogeneous ice nucleation which occurs in many environments, especially in the atmosphere where it results in the glaciation of clouds. Here we experimentally show, using a variety of IN types suspended in various aqueous solutions, that immersion freezing temperatures and kinetics can be described solely by temperature, T, and solution water activity, a(w), which is the ratio of the vapour pressure of the solution and the saturation water vapour pressure under the same conditions and, in equilibrium, equivalent to relative humidity (RH). This allows the freezing point and corresponding heterogeneous ice nucleation rate coefficient, J(het), to be uniquely expressed by T and a(w), a result we term the a(w) based immersion freezing model (ABIFM). This method is independent of the nature of the solute and accounts for several varying parameters, including cooling rate and IN surface area, while providing a holistic description of immersion freezing and allowing prediction of freezing temperatures, J(het), frozen fractions, ice particle production rates and numbers. Our findings are based on experimental freezing data collected for various IN surface areas, A, and cooling rates, r, of droplets variously containing marine biogenic material, two soil humic acids, four mineral dusts, and one organic monolayer acting as IN. For all investigated IN types we demonstrate that droplet freezing temperatures increase as A increases. Similarly, droplet freezing temperatures increase as the cooling rate decreases. The log10(J(het)) values for the various IN types derived exclusively by Tand a(w), provide a complete description of the heterogeneous ice nucleation kinetics. Thus, the ABIFM can be applied over the entire range of T, RH, total particulate surface area, and cloud activation timescales typical of atmospheric conditions. Lastly, we demonstrate that ABIFM can
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Energy Technology Data Exchange (ETDEWEB)
Qin, F.G.F.; Jian Chao Zhao; Russell, A.B.; Xiao Dong Chen; Chen, J.J. [University of Auckland (New Zealand). Dept. of Chemical and Materials Engineering; Robertson, L. [Fonterra Research Centre, Palmerston North (New Zealand)
2003-08-01
Heat transfer is an unsteady process in the initial period of ice nucleation or phase transition from aqueous solution. During this period the latent heat of freezing increases the temperature in bulk solution monotonously until the system reaches equilibrium. Meanwhile heat can transfer from the solution to the environment or vise versa. The analysis of this unsteady heat transfer process leads to the establishment of a mathematical model, which is represented by two simultaneous differential equations. Using the Laplace transform and inverse transform, and incorporating the initial condition of ice nucleation, we obtained an analytical solution of this model. Further discussion of the model's fitness by comparing to the experimental data leads to a recognition that ice fouling (or ice adhesion) on the cooler wall should be highlighted in estimating the heat transfer resistance at the very beginning of the ice formation. The model fits to the experimental data satisfactorily. (author)
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Isolating and identifying atmospheric ice-nucleating aerosols: a new technique
Kreidenweis, S. M.; Chen, Y.; Rogers, D. C.; DeMott, P. J.
Laboratory studies examined two key aspects of the performance of a continuous-flow diffusion chamber (CFD) instrument that detects ice nuclei (IN) concentrations in air samples: separating IN from non-IN, and collecting IN aerosols to determine chemical composition. In the first study, submicron AgI IN particles were mixed in a sample stream with submicron non-IN salt particles, and the sample stream was processed in the CFD at -19°C and 23% supersaturation with respect to ice. Examination of the residual particles from crystals nucleated in the CFD confirmed that only AgI particles served as IN in the mixed stream. The second study applied this technique to separate and analyze IN and non-IN particles in a natural air sample. Energy-dispersive X-ray analyses (EDS) of the elemental composition of selected particles from the IN and non-IN fractions in ambient air showed chemical differences: Si and Ca were present in both, but S, Fe and K were also detected in the non-IN fraction.
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Croteau, T; Bertram, A K; Patey, G N
2008-10-30
Grand canonical Monte Carlo calculations are used to determine water adsorption and structure on defect-free kaolinite surfaces as a function of relative humidity at 235 K. This information is then used to gain insight into ice nucleation on kaolinite surfaces. Results for both the SPC/E and TIP5P-E water models are compared and demonstrate that the Al-surface [(001) plane] and both protonated and unprotonated edges [(100) plane] strongly adsorb at atmospherically relevant relative humidities. Adsorption on the Al-surface exhibits properties of a first-order process with evidence of collective behavior, whereas adsorption on the edges is essentially continuous and appears dominated by strong water lattice interactions. For the protonated and unprotonated edges no structure that matches hexagonal ice is observed. For the Al-surface some of the water molecules formed hexagonal rings. However, the a o lattice parameter for these rings is significantly different from the corresponding constant for hexagonal ice ( Ih). A misfit strain of 14.0% is calculated between the hexagonal pattern of water adsorbed on the Al-surface and the basal plane of ice Ih. Hence, the ring structures that form on the Al-surface are not expected to be good building-blocks for ice nucleation due to the large misfit strain.
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Perlwitz, J. P.; Fridlind, A. M.; Knopf, D. A.; Miller, R. L.; Pérez García-Pando, C.
2017-12-01
The effect of aerosol particles on ice nucleation and, in turn, the formation of ice and mixed phase clouds is recognized as one of the largest sources of uncertainty in climate prediction. We apply an improved dust mineral specific aerosol module in the NASA GISS Earth System ModelE, which takes into account soil aggregates and their fragmentation at emission as well as the emission of large particles. We calculate ice nucleating particle concentrations from K-feldspar abundance for an active site parameterization for a range of activation temperatures and external and internal mixing assumption. We find that the globally averaged INP concentration is reduced by a factor of two to three, compared to a simple assumption on the size distribution of emitted dust minerals. The decrease can amount to a factor of five in some geographical regions. The results vary little between external and internal mixing and different activation temperatures, except for the coldest temperatures. In the sectional size distribution, the size range 2-4 μm contributes the largest INP number.
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Perlwitz, Jan P.; Fridlind, Ann M.; Knopf, Daniel A.; Miller, Ron L.; García-Pando, Carlos Perez
2017-01-01
The effect of aerosol particles on ice nucleation and, in turn, the formation of ice and mixed phase clouds is recognized as one of the largest sources of uncertainty in climate prediction. We apply an improved dust mineral specific aerosol module in the NASA GISS Earth System ModelE, which takes into account soil aggregates and their fragmentation at emission as well as the emission of large particles. We calculate ice nucleating particle concentrations from K-feldspar abundance for an active site parameterization for a range of activation temperatures and external and internal mixing assumption. We find that the globally averaged INP concentration is reduced by a factor of two to three, compared to a simple assumption on the size distribution of emitted dust minerals. The decrease can amount to a factor of five in some geographical regions. The results vary little between external and internal mixing and different activation temperatures, except for the coldest temperatures. In the sectional size distribution, the size range 24 micrometer contributes the largest INP number.
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Costanzo, Jon P; Baker, Patrick J; Dinkelacker, Stephen A; Lee, Richard E
2003-02-01
Hatchlings of the painted turtle (Chrysemys picta) commonly hibernate in their shallow, natal nests. Survival at temperatures below the limit of freeze tolerance (approximately -4 degrees C) apparently depends on their ability to remain supercooled, and, whereas previous studies have reported that supercooling capacity improves markedly with cold acclimation, the mechanistic basis for this change is incompletely understood. We report that the crystallization temperature (T(c)) of recently hatched (summer) turtles acclimated to 22 degrees C and reared on a substratum of vermiculite or nesting soil was approximately 5 degrees C higher than the T(c) determined for turtles acclimated to 4 degrees C and tested in winter. This increase in supercooling capacity coincided with elimination of substratum (and, in fewer cases, eggshell) that the hatchlings had ingested; however, this association was not necessarily causal because turtles reared on a paper-covered substratum did not ingest exogenous matter but nevertheless showed a similar increase in supercooling capacity. Our results for turtles reared on paper revealed that seasonal development of supercooling capacity fundamentally requires elimination of ice-nucleating agents (INA) of endogenous origin: summer turtles, but not winter turtles, produced feces (perhaps derived from residual yolk) that expressed ice-nucleating activity. Ingestion of vermiculite or eggshell, which had modest ice-nucleating activity, had no effect on the T(c), whereas ingestion of nesting soil, which contained two classes of potent INA, markedly reduced the supercooling capacity of summer turtles. This effect persisted long after the turtles had purged their guts of soil particles, because the T(c) of winter turtles reared on nesting soil (mean +/- S.E.M.=-11.6+/-1.4 degrees C) was approximately 6 degrees C higher than the T(c) of winter turtles reared on vermiculite or paper. Experiments in which winter turtles were fed INA commonly found in
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Ice Nucleating Particle Properties in the Saharan Air Layer Close to the Dust Source
Boose, Y.; Garcia, I. M.; Rodríguez, S.; Linke, C.; Schnaiter, M.; Nickovic, S.; Lohmann, U.; Kanji, Z. A.; Sierau, B.
2015-12-01
In August 2013 and 2014 measurements of ice nucleating particle (INP) concentrations, aerosol particle size distributions, chemistry and fluorescence were conducted at the Izaña Atmospheric Observatory located at 2373 m asl on Tenerife, west off the African shore. During summer, the observatory is frequently within the Saharan Air Layer and thus often exposed to dust. Absolute INP concentrations and activated fractions at T=-40 to -15°C and RHi=100-150 % were measured. In this study, we discuss the in-situ measured INP properties with respect to changes in the chemical composition, the biological content, the source regions as well as transport pathways and thus aging processes of the dust aerosol. For the first time, ice crystal residues were also analyzed with regard to biological content by means of their autofluorescence signal close to a major dust source region. Airborne dust samples were collected with a cyclone for additional offline analysis in the laboratory under similar conditions as in the field. Both, in-situ and offline dust samples were chemically characterized using single-particle mass spectrometry. The DREAM8 dust model extended with dust mineral fractions was run to simulate meteorological and dust aerosol conditions for ice nucleation. Results show that the background aerosol at Izaña was dominated by carbonaceous particles, which were hardly ice-active under the investigated conditions. When Saharan dust was present, INP concentrations increased by up to two orders of magnitude even at water subsaturated conditions at T≤-25°C. Differences in the ice-activated fraction were found between different dust periods which seem to be linked to variations in the aerosol chemical composition (dust mixed with changing fractions of sea salt and differences in the dust aerosol itself). Furthermore, two biomass burning events in 2014 were identified which led to very low INP concentrations under the investigated temperature and relative humidity
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Energy Technology Data Exchange (ETDEWEB)
Kerminen, V.M.
1995-12-31
Production of new sulfur derived particles via homogeneous nucleation between sulfuric acid and water vapors, and other related aerosol processes taking place in a variety of tropospheric environments, were studied using theoretical and model approaches. For nucleation to occur in the lower troposphere, cool and humid conditions combined with relatively strong solar radiation were usually required. Regardless of the system concerned, production of nuclei was found to be favored also by high SO{sub 2}(g) to fine particulate matter ratios. Urban post-fog situations, which are encountered commonly during severe air pollution episodes, were shown to favor new particle production considerably above the corresponding `background` conditions. A simple procedure for evaluating post-fog nucleation probabilities from routinely obtained data was developed and applied to real aerosol systems. Nucleation in the remote marine environment, which is an essential phenomenon in linking natural sulfur emissions to global climate change, was studied from a dynamic point of view. It was demonstrated that new particle production occurs more often in association with relative humidity transitions typical for many boundary layer processes than under averaged or steady conditions of the kind assumed explicitly in most earlier model studies. Power plant plumes were shown to be a particularly significant source of atmospheric nuclei, due primarily to their frequently high SO{sub 2}-to-particulate matter ratios. Factors affecting the probability of nucleation during plume dispersion were examined in detail, and finally, strategies for the control of in-plume particle production were analyzed. (author)
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Hazra, Anupam; Padmakumari, B.; Maheskumar, R. S.; Chen, Jen-Ping
2016-05-01
This study investigates the influence of different ice nuclei (IN) species and their number concentrations on cloud ice production. The numerical simulation with different species of ice nuclei is investigated using an explicit bulk-water microphysical scheme in a Mesoscale Meteorological Model version 5 (MM5). The species dependent ice nucleation parameterization that is based on the classical nucleation theory has been implemented into the model. The IN species considered include dust and soot with two different concentrations (Low and High). The simulated cloud microphysical properties like droplet number concentration and droplet effective radii as well as macro-properties (equivalent potential temperature and relative humidity) are comparable with aircraft observations. When higher dust IN concentrations are considered, the simulation results showed good agreement with the cloud ice and cloud water mixing ratio from aircraft measurements during Cloud Aerosol Interactions and Precipitation Enhancement Experiment (CAIPEEX) and Modern Era Retrospective Analysis for Research and Applications (MERRA) reanalysis. Relative importance of IN species is shown as compared to the homogeneous freezing nucleation process. The tendency of cloud ice production rates is also analyzed and found that dust IN is more efficient in producing cloud ice when compared to soot IN. The dust IN with high concentration can produce more surface precipitation than soot IN at the same concentration. This study highlights the need to improve the ice nucleation parameterization in numerical models.
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Czech Academy of Sciences Publication Activity Database
Hajek, J.; Kvíderová, Jana; Worland, R.; Barták, M.; Elster, Josef; Vaczi, P.
2009-01-01
Roč. 48, č. 4 (2009), s. 37-38 ISSN 0031-8884. [International Phycological Congress /9./. 02.08.2009-08.08.2009, Tokyo] R&D Projects: GA AV ČR IAA600050702; GA AV ČR KJB601630808 Institutional research plan: CEZ:AV0Z60050516 Keywords : ice nucleation * algae * freezing Subject RIV: EF - Botanics
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Effect of freeze-thaw repetitions upon the supercooling release ability of ice-nucleating bacteria
International Nuclear Information System (INIS)
Tsuchiya, Yooko; Hasegawa, Hiromi; Sasaki, Kazuhiro
2004-01-01
We have studied the durability of ice-nucleating bacteria with a potent supercooling release capacity through repeated freeze-thaw cycles. Through experiment, we confirmed that UV sterilized Erwinia ananas maintains a superior supercooling release capacity at around -1degC through 2000 freeze-thaw cycles. We also found that γ-ray sterilization, which is more suitable than UV for large-scale sterilization treatment, has a similar effect at appropriately selected doses. (author)
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Bacterial Ice Crystal Controlling Proteins
Lorv, Janet S. H.; Rose, David R.; Glick, Bernard R.
2014-01-01
Across the world, many ice active bacteria utilize ice crystal controlling proteins for aid in freezing tolerance at subzero temperatures. Ice crystal controlling proteins include both antifreeze and ice nucleation proteins. Antifreeze proteins minimize freezing damage by inhibiting growth of large ice crystals, while ice nucleation proteins induce formation of embryonic ice crystals. Although both protein classes have differing functions, these proteins use the same ice binding mechanisms. Rather than direct binding, it is probable that these protein classes create an ice surface prior to ice crystal surface adsorption. Function is differentiated by molecular size of the protein. This paper reviews the similar and different aspects of bacterial antifreeze and ice nucleation proteins, the role of these proteins in freezing tolerance, prevalence of these proteins in psychrophiles, and current mechanisms of protein-ice interactions. PMID:24579057
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Planková, Barbora; Vinš, Václav; Hrubý, Jan
2017-10-28
Homogeneous droplet nucleation has been studied for almost a century but has not yet been fully understood. In this work, we used the density gradient theory (DGT) and considered the influence of capillary waves (CWs) on the predicted size-dependent surface tensions and nucleation rates for selected n-alkanes. The DGT model was completed by an equation of state (EoS) based on the perturbed-chain statistical associating fluid theory and compared to the classical nucleation theory and the Peng-Robinson EoS. It was found that the critical clusters are practically free of CWs because they are so small that even the smallest wavelengths of CWs do not fit into their finite dimensions. The CWs contribute to the entropy of the system and thus decrease the surface tension. A correction for the effect of CWs on the surface tension is presented. The effect of the different EoSs is relatively small because by a fortuitous coincidence their predictions are similar in the relevant range of critical cluster sizes. The difference of the DGT predictions to the classical nucleation theory computations is important but not decisive. Of the effects investigated, the most pronounced is the suppression of CWs which causes a sizable decrease of the predicted nucleation rates. The major difference between experimental nucleation rate data and theoretical predictions remains in the temperature dependence. For normal alkanes, this discrepancy is much stronger than observed, e.g., for water. Theoretical corrections developed here have a minor influence on the temperature dependency. We provide empirical equations correcting the predicted nucleation rates to values comparable with experiments.
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Planková, Barbora; Vinš, Václav; Hrubý, Jan
2017-10-01
Homogeneous droplet nucleation has been studied for almost a century but has not yet been fully understood. In this work, we used the density gradient theory (DGT) and considered the influence of capillary waves (CWs) on the predicted size-dependent surface tensions and nucleation rates for selected n-alkanes. The DGT model was completed by an equation of state (EoS) based on the perturbed-chain statistical associating fluid theory and compared to the classical nucleation theory and the Peng-Robinson EoS. It was found that the critical clusters are practically free of CWs because they are so small that even the smallest wavelengths of CWs do not fit into their finite dimensions. The CWs contribute to the entropy of the system and thus decrease the surface tension. A correction for the effect of CWs on the surface tension is presented. The effect of the different EoSs is relatively small because by a fortuitous coincidence their predictions are similar in the relevant range of critical cluster sizes. The difference of the DGT predictions to the classical nucleation theory computations is important but not decisive. Of the effects investigated, the most pronounced is the suppression of CWs which causes a sizable decrease of the predicted nucleation rates. The major difference between experimental nucleation rate data and theoretical predictions remains in the temperature dependence. For normal alkanes, this discrepancy is much stronger than observed, e.g., for water. Theoretical corrections developed here have a minor influence on the temperature dependency. We provide empirical equations correcting the predicted nucleation rates to values comparable with experiments.
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Infrared thermography has been used to visualize the freezing process in plants and has greatly enhanced our knowledge of ice nucleation and propagation in plants. The majority of IR analyses have been conducted under controlled rather than natural conditions and often on plant parts instead of wh...
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Wisniewski, Michael; Neuner, Gilbert; Gusta, Lawrence V
2015-05-08
Freezing events that occur when plants are actively growing can be a lethal event, particularly if the plant has no freezing tolerance. Such frost events often have devastating effects on agricultural production and can also play an important role in shaping community structure in natural populations of plants, especially in alpine, sub-arctic, and arctic ecosystems. Therefore, a better understanding of the freezing process in plants can play an important role in the development of methods of frost protection and understanding mechanisms of freeze avoidance. Here, we describe a protocol to visualize the freezing process in plants using high-resolution infrared thermography (HRIT). The use of this technology allows one to determine the primary sites of ice formation in plants, how ice propagates, and the presence of ice barriers. Furthermore, it allows one to examine the role of extrinsic and intrinsic nucleators in determining the temperature at which plants freeze and evaluate the ability of various compounds to either affect the freezing process or increase freezing tolerance. The use of HRIT allows one to visualize the many adaptations that have evolved in plants, which directly or indirectly impact the freezing process and ultimately enables plants to survive frost events.
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Ahern, H. E.; Walsh, K. A.; Hill, T. C. J.; Moffett, B. F.
2007-02-01
Microorganisms were discovered in clouds over 100 years ago but information on bacterial community structure and function is limited. Clouds may not only be a niche within which bacteria could thrive but they might also influence dynamic processes using ice nucleating and cloud condensing abilities. Cloud and rain samples were collected from two mountains in the Outer Hebrides, NW Scotland, UK. Community composition was determined using a combination of amplified 16S ribosomal DNA restriction analysis and sequencing. 256 clones yielded 100 operational taxonomic units (OTUs) of which half were related to bacteria from terrestrial psychrophilic environments. Cloud samples were dominated by a mixture of fluorescent Pseudomonas spp., some of which have been reported to be ice nucleators. It was therefore possible that these bacteria were using the ice nucleation (IN) gene to trigger the Bergeron-Findeisen process of raindrop formation as a mechanism for dispersal. In this study the IN gene was not detected in any of the isolates using both polymerase chain reaction (PCR) and differential scanning calorimetry (DSC). Instead 55% of the total isolates from both cloud and rain samples displayed significant biosurfactant activity when analyzed using the drop-collapse technique. All isolates were characterised as fluorescent pseudomonads. Surfactants have been found to be very important in lowering atmospheric critical supersaturations required for the activation of aerosols into cloud condensation nuclei (CCN). It is also known that surfactants influence cloud droplet size and increase cloud lifetime and albedo. Some bacteria are known to act as CCN and so it is conceivable that these fluorescent pseudomonads are using surfactants to facilitate their activation from aerosols into CCN. This would allow water scavenging,~countering desiccation, and assist in their widespread dispersal.
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Ladino, L. A.; Yakobi-Hancock, J. D.; Kilthau, W. P.; Mason, R. H.; Si, M.; Li, J.; Miller, L. A.; Schiller, C. L.; Huffman, J. A.; Aller, J. Y.; Knopf, D. A.; Bertram, A. K.; Abbatt, J. P. D.
2016-05-01
This study addresses, through two types of experiments, the potential for the oceans to act as a source of atmospheric ice-nucleating particles (INPs). The INP concentration via deposition mode nucleation was measured in situ at a coastal site in British Columbia in August 2013. The INP concentration at conditions relevant to cirrus clouds (i.e., -40 °C and relative humidity with respect to ice, RHice = 139%) ranged from 0.2 L-1 to 3.3 L-1. Correlations of the INP concentrations with levels of anthropogenic tracers (i.e., CO, SO2, NOx, and black carbon) and numbers of fluorescent particles do not indicate a significant influence from anthropogenic sources or submicron bioaerosols, respectively. Additionally, the INPs measured in the deposition mode showed a poor correlation with the concentration of particles with sizes larger than 500 nm, which is in contrast with observations made in the immersion freezing mode. To investigate the nature of particles that could have acted as deposition INP, laboratory experiments with potential marine aerosol particles were conducted under the ice-nucleating conditions used in the field. At -40 °C, no deposition activity was observed with salt aerosol particles (sodium chloride and two forms of commercial sea salt: Sigma-Aldrich and Instant Ocean), particles composed of a commercial source of natural organic matter (Suwannee River humic material), or particle mixtures of sea salt and humic material. In contrast, exudates from three phytoplankton (Thalassiosira pseudonana, Nanochloris atomus, and Emiliania huxleyi) and one marine bacterium (Vibrio harveyi) exhibited INP activity at low RHice values, down to below 110%. This suggests that the INPs measured at the field site were of marine biological origins, although we cannot rule out other sources, including mineral dust.
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Cloud chamber experiments on the origin of ice crystal complexity in cirrus clouds
Directory of Open Access Journals (Sweden)
M. Schnaiter
2016-04-01
Full Text Available This study reports on the origin of small-scale ice crystal complexity and its influence on the angular light scattering properties of cirrus clouds. Cloud simulation experiments were conducted at the AIDA (Aerosol Interactions and Dynamics in the Atmosphere cloud chamber of the Karlsruhe Institute of Technology (KIT. A new experimental procedure was applied to grow and sublimate ice particles at defined super- and subsaturated ice conditions and for temperatures in the −40 to −60 °C range. The experiments were performed for ice clouds generated via homogeneous and heterogeneous initial nucleation. Small-scale ice crystal complexity was deduced from measurements of spatially resolved single particle light scattering patterns by the latest version of the Small Ice Detector (SID-3. It was found that a high crystal complexity dominates the microphysics of the simulated clouds and the degree of this complexity is dependent on the available water vapor during the crystal growth. Indications were found that the small-scale crystal complexity is influenced by unfrozen H2SO4 / H2O residuals in the case of homogeneous initial ice nucleation. Angular light scattering functions of the simulated ice clouds were measured by the two currently available airborne polar nephelometers: the polar nephelometer (PN probe of Laboratoire de Métérologie et Physique (LaMP and the Particle Habit Imaging and Polar Scattering (PHIPS-HALO probe of KIT. The measured scattering functions are featureless and flat in the side and backward scattering directions. It was found that these functions have a rather low sensitivity to the small-scale crystal complexity for ice clouds that were grown under typical atmospheric conditions. These results have implications for the microphysical properties of cirrus clouds and for the radiative transfer through these clouds.
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Lacher, Larissa; Lohmann, Ulrike; Boose, Yvonne; Zipori, Assaf; Herrmann, Erik; Bukowiecki, Nicolas; Steinbacher, Martin; Kanji, Zamin A.
2017-12-01
In this work we describe the Horizontal Ice Nucleation Chamber (HINC) as a new instrument to measure ambient ice-nucleating particle (INP) concentrations for conditions relevant to mixed-phase clouds. Laboratory verification and validation experiments confirm the accuracy of the thermodynamic conditions of temperature (T) and relative humidity (RH) in HINC with uncertainties in T of ±0.4 K and in RH with respect to water (RHw) of ±1.5 %, which translates into an uncertainty in RH with respect to ice (RHi) of ±3.0 % at T > 235 K. For further validation of HINC as a field instrument, two measurement campaigns were conducted in winters 2015 and 2016 at the High Altitude Research Station Jungfraujoch (JFJ; Switzerland, 3580 m a. s. l. ) to sample ambient INPs. During winters 2015 and 2016 the site encountered free-tropospheric conditions 92 and 79 % of the time, respectively. We measured INP concentrations at 242 K at water-subsaturated conditions (RHw = 94 %), relevant for the formation of ice clouds, and in the water-supersaturated regime (RHw = 104 %) to represent ice formation occurring under mixed-phase cloud conditions. In winters 2015 and 2016 the median INP concentrations at RHw = 94 % was below the minimum detectable concentration. At RHw = 104 %, INP concentrations were an order of magnitude higher, with median concentrations in winter 2015 of 2.8 per standard liter (std L-1; normalized to standard T of 273 K and pressure, p, of 1013 hPa) and 4.7 std L-1 in winter 2016. The measurements are in agreement with previous winter measurements obtained with the Portable Ice Nucleation Chamber (PINC) of 2.2 std L-1 at the same location. During winter 2015, two events caused the INP concentrations at RHw = 104 % to significantly increase above the campaign average. First, an increase to 72.1 std L-1 was measured during an event influenced by marine air, arriving at the JFJ from the North Sea and the Norwegian Sea. The contribution from anthropogenic or other
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Pietsch, Renée B.; Hanlon, Regina; Bohland, Cynthia; Schmale, David G., III
2016-01-01
This article describes an interdisciplinary unit in which students explore biological "ice nucleation"--by particles that cause water to freeze at temperatures above -38°C--through the lens of the microbial ice nucleator "Pseudomonas syringae." Such This activity, which aligns with the "Next Generation Science…
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Global model comparison of heterogeneous ice nucleation parameterizations in mixed phase clouds
Yun, Yuxing; Penner, Joyce E.
2012-04-01
A new aerosol-dependent mixed phase cloud parameterization for deposition/condensation/immersion (DCI) ice nucleation and one for contact freezing are compared to the original formulations in a coupled general circulation model and aerosol transport model. The present-day cloud liquid and ice water fields and cloud radiative forcing are analyzed and compared to observations. The new DCI freezing parameterization changes the spatial distribution of the cloud water field. Significant changes are found in the cloud ice water fraction and in the middle cloud fractions. The new DCI freezing parameterization predicts less ice water path (IWP) than the original formulation, especially in the Southern Hemisphere. The smaller IWP leads to a less efficient Bergeron-Findeisen process resulting in a larger liquid water path, shortwave cloud forcing, and longwave cloud forcing. It is found that contact freezing parameterizations have a greater impact on the cloud water field and radiative forcing than the two DCI freezing parameterizations that we compared. The net solar flux at top of atmosphere and net longwave flux at the top of the atmosphere change by up to 8.73 and 3.52 W m-2, respectively, due to the use of different DCI and contact freezing parameterizations in mixed phase clouds. The total climate forcing from anthropogenic black carbon/organic matter in mixed phase clouds is estimated to be 0.16-0.93 W m-2using the aerosol-dependent parameterizations. A sensitivity test with contact ice nuclei concentration in the original parameterization fit to that recommended by Young (1974) gives results that are closer to the new contact freezing parameterization.
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R. Wagner; O. Möhler; H. Saathoff; M. Schnaiter; T. Leisner
2010-01-01
The heterogeneous ice nucleation potential of airborne oxalic acid dihydrate and sodium oxalate particles in the deposition and condensation mode has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 244 and 228 K. Previous laboratory studies have highlighted the particular role of oxalic acid dihydrate as the only species amongst a variety of other investigated dicarboxylic acids to ...
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Worringen, A.; Kandler, K.; Benker, N.; Dirsch, T.; Mertes, S.; Schenk, L.; Kästner, U.; Frank, F.; Nillius, B.; Bundke, U.; Rose, D.; Curtius, J.; Kupiszewski, P.; Weingartner, E.; Vochezer, P.; Schneider, J.; Schmidt, S.; Weinbruch, S.; Ebert, M.
2015-04-01
In the present work, three different techniques to separate ice-nucleating particles (INPs) as well as ice particle residuals (IPRs) from non-ice-active particles are compared. The Ice Selective Inlet (ISI) and the Ice Counterflow Virtual Impactor (Ice-CVI) sample ice particles from mixed-phase clouds and allow after evaporation in the instrument for the analysis of the residuals. The Fast Ice Nucleus Chamber (FINCH) coupled with the Ice Nuclei Pumped Counterflow Virtual Impactor (IN-PCVI) provides ice-activating conditions to aerosol particles and extracts the activated particles for analysis. The instruments were run during a joint field campaign which took place in January and February 2013 at the High Alpine Research Station Jungfraujoch (Switzerland). INPs and IPRs were analyzed offline by scanning electron microscopy and energy-dispersive X-ray microanalysis to determine their size, chemical composition and mixing state. Online analysis of the size and chemical composition of INP activated in FINCH was performed by laser ablation mass spectrometry. With all three INP/IPR separation techniques high abundances (median 20-70%) of instrumental contamination artifacts were observed (ISI: Si-O spheres, probably calibration aerosol; Ice-CVI: Al-O particles; FINCH + IN-PCVI: steel particles). After removal of the instrumental contamination particles, silicates, Ca-rich particles, carbonaceous material and metal oxides were the major INP/IPR particle types obtained by all three techniques. In addition, considerable amounts (median abundance mostly a few percent) of soluble material (e.g., sea salt, sulfates) were observed. As these soluble particles are often not expected to act as INP/IPR, we consider them as potential measurement artifacts. Minor types of INP/IPR include soot and Pb-bearing particles. The Pb-bearing particles are mainly present as an internal mixture with other particle types. Most samples showed a maximum of the INP/IPR size distribution at 200
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Vapour–to–liquid nucleation: Nucleation theorems for nonisothermal–nonideal case
Energy Technology Data Exchange (ETDEWEB)
Malila, J.; McGraw, R.; Napari, I.; Laaksonen, A.
2010-08-29
Homogeneous vapour-to-liquid nucleation, a basic process of aerosol formation, is often considered as a type example of nucleation phenomena, while most treatment of the subject introduce several simplifying assumptions (ideal gas phase, incompressible nucleus, isothermal kinetics, size-independent surface free energy...). During last decades, nucleation theorems have provided new insights into properties of critical nuclei facilitating direct comparison between laboratory experiments and molecular simulations. These theorems are, despite of their generality, often applied in forms where the aforementioned assumptions are made. Here we present forms of nucleation theorems that explicitly take into account these effects and allow direct estimation of their importance. Only assumptions are Arrhenius-type kinetics of nucleation process and exclusion carrier gas molecules from the critical nucleus.
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Sea spray as a source of ice nucleating particles - results from the AIDA Ocean03 campaign
Salter, M. E.; Ickes, L.; Adams, M.; Bierbauer, S.; Bilde, M.; Christiansen, S.; Ekman, A.; Gorokhova, E.; Höhler, K.; Kiselev, A. A.; Leck, C.; Mohr, C.; Mohler, O.; Murray, B. J.; Porter, G.; Ullrich, R.; Wagner, R.
2017-12-01
Clouds and their radiative effects are one of the major influences on the radiative fluxes in the atmosphere, but at the same time they remain the largest uncertainty in climate models. This lack of understanding is especially pronounced in the high Arctic. Summertime clouds can persist over long periods in this region, which is difficult to replicate in models based on our current understanding. The clouds most often encountered in the summertime high Arctic consist of a mixture of ice crystals and super-cooled water droplets, so-called mixed-phase clouds. This cloud type is sensitive to the availability of aerosol particles, which can act as cloud condensation nuclei and ice nuclei. However, since the high Arctic is a pristine region, aerosol particles are not very abundant, and the hypothesis of open leads in the Arctic as a potentially important source of cloud and ice nucleating particles via bubble bursting has emerged. In this context, we have conducted a series of experiments at the AIDA chamber at KIT, designed to investigate the mechanisms linking marine biology, seawater chemistry and aerosol physics/potential cloud impacts. During this campaign, two marine diatom species (Melosira arctica and Skeletonema marinoi) as well as sea surface microlayer samples collected during several Arctic Ocean research cruises were investigated. To aerosolize the samples, a variety of methods were used including a sea spray simulation chamber to mimic the process of bubble-bursting. The ice nucleating efficiency (mixed-phase cloud regime) of the samples was determined either directly in the AIDA chamber during adiabatic expansions, or using the INKA continuous flow diffusion chamber, or a cold stage. Results from the campaign along with the potential implications are presented.
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What controls the low ice number concentration in the upper troposphere?
Directory of Open Access Journals (Sweden)
C. Zhou
2016-10-01
Full Text Available Cirrus clouds in the tropical tropopause play a key role in regulating the moisture entering the stratosphere through their dehydrating effect. Low ice number concentrations ( < 200 L−1 and high supersaturations (150–160 % have been observed in these clouds. Different mechanisms have been proposed to explain these low ice number concentrations, including the inhibition of homogeneous freezing by the deposition of water vapour onto pre-existing ice crystals, heterogeneous ice formation on glassy organic aerosol ice nuclei (IN, and limiting the formation of ice number from high-frequency gravity waves. In this study, we examined the effect from three different representations of updraft velocities, the effect from pre-existing ice crystals, the effect from different water vapour deposition coefficients (α = 0.1 or 1, and the effect of 0.1 % of the total secondary organic aerosol (SOA particles acting as IN. Model-simulated ice crystal numbers are compared against an aircraft observational dataset.Including the effect from water vapour deposition on pre-existing ice particles can effectively reduce simulated in-cloud ice number concentrations for all model setups. A larger water vapour deposition coefficient (α = 1 can also efficiently reduce ice number concentrations at temperatures below 205 K, but less so at higher temperatures. SOA acting as IN is most effective at reducing ice number concentrations when the effective updraft velocities are moderate ( ∼ 0.05–0.2 m s−1. However, the effects of including SOA as IN and using (α = 1 are diminished when the effect from pre-existing ice is included.When a grid-resolved large-scale updraft velocity ( < 0.1 m s−1 is used, the ice nucleation parameterization with homogeneous freezing only or with both homogeneous freezing and heterogeneous nucleation is able to generate low ice number concentrations in good agreement
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Directory of Open Access Journals (Sweden)
E. Stopelli
2016-07-01
Full Text Available Nucleation of ice affects the properties of clouds and the formation of precipitation. Quantitative data on how ice nucleating particles (INPs determine the distribution, occurrence and intensity of precipitation are still scarce. INPs active at −8 °C (INPs−8 were observed for 2 years in precipitation samples at the High-Altitude Research Station Jungfraujoch (Switzerland at 3580 m a.s.l. Several environmental parameters were scanned for their capability to predict the observed abundance and variability of INPs−8. Those singularly presenting the best correlations with observed number of INPs−8 (residual fraction of water vapour, wind speed, air temperature, number of particles with diameter larger than 0.5 µm, season, and source region of particles were implemented as potential predictor variables in statistical multiple linear regression models. These models were calibrated with 84 precipitation samples collected during the first year of observations; their predictive power was successively validated on the set of 15 precipitation samples collected during the second year. The model performing best in calibration and validation explains more than 75 % of the whole variability of INPs−8 in precipitation and indicates that a high abundance of INPs−8 is to be expected whenever high wind speed coincides with air masses having experienced little or no precipitation prior to sampling. Such conditions occur during frontal passages, often accompanied by precipitation. Therefore, the circumstances when INPs−8 could be sufficiently abundant to initiate the ice phase in clouds may frequently coincide with meteorological conditions favourable to the onset of precipitation events.
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Weber, Daniel; Schrod, Jann; Drücke, Jaqueline; Keleshis, Christos; Pikridas, Michael; Ebert, Martin; Cvetkovic, Bojan; Nickovic, Slobodan; Baars, Holger; Marinou, Eleni; Vrekoussis, Mihalis; Sciare, Jean; Mihalopoulos, Nikos; Curtius, Joachim; Bingemer, Heinz G.
2017-04-01
During the intensive INUIT-BACCHUS-ACTRIS field campaign focusing on aerosols, clouds and ice nucleation in the Eastern Mediterranean in April 2016, we have measured the abundance of ice nucleating particles (INP) in the lower troposphere both with unmanned aircraft systems (UAS) as well as from the ground. Aerosol samples were collected by miniaturized electrostatic precipitators onboard the UAS and were analyzed immediately after collection on site in the ice nucleus counter FRIDGE for INP active at -20˚ C to -30˚ C in the deposition/condensation mode (INPD). Immersion freezing INP (INPI) were sampled on membrane filters and were analysed in aqueous extracts by the drop freezing method on the cold stage of FRIDGE. Ground samples were collected at the Cyprus Atmospheric Observatory (CAO) in Agia Marina Xyliatou (Latitude; 35˚ 2' 8" N; Longitude: 33˚ 3' 26" E; Altitude: 532 m a.s.l.). During the one-month campaign, we encountered a series of Saharan dust plumes that traveled at several kilometers altitude. Here we present INP data from 42 individual flights, together with OPC aerosol number concentrations, backscatter and depolarization retrievals from the Polly-XT Raman Lidar, dust concentrations derived by the dust transport model DREAM (Dust Regional Atmospheric Model), and results from scanning electron microscopy. The effect of the dust plumes is reflected by the coincidence of INP with the particulate mass (PM), the Lidar retrievals and the predicted dust mass of the model. This suggests that mineral dust or a constituent related to dust was a major contributor to the ice nucleating properties of the aerosol. Peak concentrations of above 100 INP std.l-1 were measured at -30˚ C. The INPD concentration in elevated plumes was on average a factor of 10 higher than at ground level. The INPI concentration at ground also agreed with PM levels and exceeded the ground-based INPD concentration by more than one order of magnitude. Since desert dust is transported
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Directory of Open Access Journals (Sweden)
L. Lacher
2017-12-01
Full Text Available In this work we describe the Horizontal Ice Nucleation Chamber (HINC as a new instrument to measure ambient ice-nucleating particle (INP concentrations for conditions relevant to mixed-phase clouds. Laboratory verification and validation experiments confirm the accuracy of the thermodynamic conditions of temperature (T and relative humidity (RH in HINC with uncertainties in T of ±0.4 K and in RH with respect to water (RHw of ±1.5 %, which translates into an uncertainty in RH with respect to ice (RHi of ±3.0 % at T > 235 K. For further validation of HINC as a field instrument, two measurement campaigns were conducted in winters 2015 and 2016 at the High Altitude Research Station Jungfraujoch (JFJ; Switzerland, 3580 m a. s. l. to sample ambient INPs. During winters 2015 and 2016 the site encountered free-tropospheric conditions 92 and 79 % of the time, respectively. We measured INP concentrations at 242 K at water-subsaturated conditions (RHw = 94 %, relevant for the formation of ice clouds, and in the water-supersaturated regime (RHw = 104 % to represent ice formation occurring under mixed-phase cloud conditions. In winters 2015 and 2016 the median INP concentrations at RHw = 94 % was below the minimum detectable concentration. At RHw = 104 %, INP concentrations were an order of magnitude higher, with median concentrations in winter 2015 of 2.8 per standard liter (std L−1; normalized to standard T of 273 K and pressure, p, of 1013 hPa and 4.7 std L−1 in winter 2016. The measurements are in agreement with previous winter measurements obtained with the Portable Ice Nucleation Chamber (PINC of 2.2 std L−1 at the same location. During winter 2015, two events caused the INP concentrations at RHw = 104 % to significantly increase above the campaign average. First, an increase to 72.1 std L−1 was measured during an event influenced by marine air, arriving at the JFJ
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Directory of Open Access Journals (Sweden)
M. L. López
2016-01-01
Full Text Available This study reports measurements of deposition-mode ice-nucleating particle (INP concentrations at ground level during the period July–December 2014 in Córdoba, Argentina. Ambient air was sampled into a cloud chamber where the INP concentration was measured at a temperature of −25 °C and a 15 % supersaturation over ice. Measurements were performed on days with different thermodynamic conditions, including rainy days. The effect of the relative humidity at ground level (RHamb on the INP concentration was analyzed. The number of INPs activated varied from 1 L−1 at RHamb of 25 % to 30 L−1 at RHamb of 90 %. In general, a linear trend between the INP concentration and the RHamb was found, suggesting that this variability must be related to the effectiveness of the aerosols acting as INPs. From the backward trajectories analysis, it was found that the link between INP concentration and RHamb is independent of the origin of the air masses. The role of biological INPs and nucleation occurring in pores and cavities was discussed as a possible mechanism to explain the increase of the INP concentration during high ambient relative humidity events. This work provides valuable measurements of deposition-mode INP concentrations from the Southern Hemisphere where INP data are sparse so far.
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Ice condensation on sulfuric acid tetrahydrate: Implications for polar stratospheric ice clouds
Directory of Open Access Journals (Sweden)
T. J. Fortin
2003-01-01
Full Text Available The mechanism of ice nucleation to form Type 2 PSCs is important for controlling the ice particle size and hence the possible dehydration in the polar winter stratosphere. This paper probes heterogeneous ice nucleation on sulfuric acid tetrahydrate (SAT. Laboratory experiments were performed using a thin-film, high-vacuum apparatus in which the condensed phase is monitored via Fourier transform infrared spectroscopy and water pressure is monitored with the combination of an MKS baratron and an ionization gauge. Results show that SAT is an efficient ice nucleus with a critical ice saturation ratio of S*ice = 1.3 to 1.02 over the temperature range 169.8-194.5 K. This corresponds to a necessary supercooling of 0.1-1.3 K below the ice frost point. The laboratory data is used as input for a microphysical/photochemical model to probe the effect that this heterogeneous nucleation mechanism could have on Type 2 PSC formation and stratospheric dehydration. In the model simulations, even a very small number of SAT particles (e.g., 10-3 cm-3 result in ice nucleation on SAT as the dominant mechanism for Type 2 PSC formation. As a result, Type 2 PSC formation is more widespread, leading to larger-scale dehydration. The characteristics of the clouds are controlled by the assumed number of SAT particles present, demonstrating that a proper treatment of SAT is critical for correctly modeling Type 2 PSC formation and stratospheric dehydration.
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Frazil-ice growth rate and dynamics in mixed layers and sub-ice-shelf plumes
Rees Jones, David W.; Wells, Andrew J.
2018-01-01
The growth of frazil or granular ice is an important mode of ice formation in the cryosphere. Recent advances have improved our understanding of the microphysical processes that control the rate of ice-crystal growth when water is cooled beneath its freezing temperature. These advances suggest that crystals grow much faster than previously thought. In this paper, we consider models of a population of ice crystals with different sizes to provide insight into the treatment of frazil ice in large-scale models. We consider the role of crystal growth alongside the other physical processes that determine the dynamics of frazil ice. We apply our model to a simple mixed layer (such as at the surface of the ocean) and to a buoyant plume under a floating ice shelf. We provide numerical calculations and scaling arguments to predict the occurrence of frazil-ice explosions, which we show are controlled by crystal growth, nucleation, and gravitational removal. Faster crystal growth, higher secondary nucleation, and slower gravitational removal make frazil-ice explosions more likely. We identify steady-state crystal size distributions, which are largely insensitive to crystal growth rate but are affected by the relative importance of secondary nucleation to gravitational removal. Finally, we show that the fate of plumes underneath ice shelves is dramatically affected by frazil-ice dynamics. Differences in the parameterization of crystal growth and nucleation give rise to radically different predictions of basal accretion and plume dynamics, and can even impact whether a plume reaches the end of the ice shelf or intrudes at depth.
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Spores of most common airborne fungi reveal no ice nucleation activity
Pummer, B. G.; Atanasova, L.; Bauer, H.; Bernardi, J.; Druzhinina, I. S.; Grothe, H.
2013-06-01
Fungal spores are ubiquitous biological aerosols, which are considered to show ice nucleation (IN) activity. In this study the respective IN activity was tested in oil emulsion in the immersion freezing mode. The focus was laid on species of economical, ecological or sanitary significance. For the first time, not only common moulds, but also edible mushrooms (Basidiomycota, Agaricomycetes) were investigated, as they contribute massively to the total amount of fungal spores in the atmosphere. Only Fusarium avenaceum showed freezing events at low subzero-temperatures, while the other investigated fungal spores showed no significant IN activity. Furthermore, we selected a set of fungal strains from different sites and exposed them to occasional freezing stress during cultivation. Although the total protein expression was altered by this treatment, it had no significant impact on the IN activity.
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Directory of Open Access Journals (Sweden)
I. Crawford
2011-09-01
Full Text Available The ice nucleation efficiency of propane flame soot particles with and without a sulphuric acid coating was investigated using the aerosol and cloud chamber facility AIDA (Aerosol Interaction and Dynamics in the Atmosphere. The test soot for cloud formation simulations was produced using a propane flame Combustion Aerosol Standard generator (CAST, Jing-CAST Technologies. The organic carbon content (OC of the test soot was altered in a reproducible fashion by changing the fuel/air mixture of the generator. The soot content of ice nuclei was subsequently investigated using a combination of a pumped counterflow virtual impactor (PCVI to separate and evaporate the ice crystals, and a DMT single particle soot photometer (SP2 to examine the mixing state of the BC containing ice residuals.
Ice nucleation was found to be most efficient for uncoated soot of low organic carbon content (~5 % organic carbon content where deposition freezing occurred at an ice saturation ratio Sice ~ 1.22 at a temperature T = 226.6 K with 25 % of the test soot becoming active as ice nuclei. Propane flame soot of higher organic carbon content (~30 % and ~70 % organic carbon content showed significantly lower ice nucleation efficiency (an activated fraction of the order of a few percent in the experiments than the low organic carbon content soot, with water saturation being required for freezing to occur. Ice nucleation occurred over the range Sice = 1.22–1.70, and T = 223.2–226.6 K. Analysis of the SP2 data showed that the 5 % organic carbon content soot had an undetectable OC coating whereas the 30 % organic carbon content soot had a thicker or less volatile OC coating.
The application of a sulphuric acid coating to the flame soot shifted the threshold of the onset of freezing towards that of the homogeneous freezing of sulphuric acid; for the minimum OC flame soot this inhibited nucleation since the -
Kanji, Z A; Abbatt, J P D
2010-01-21
The University of Toronto Continuous Flow Diffusion Chamber (UT-CFDC) was used to study ice formation onto monodisperse Arizona Test Dust (ATD) particles. The onset relative humidity with respect to ice (RH(i)) was measured as a function of temperature in the range 251-223 K for 100 nm ATD particles. It was found that for 0.1% of the particles to freeze, water saturation was required at all temperatures except 223 K where particles activated at RH(i) below water saturation. At this temperature, where deposition mode freezing is occurring, we find that the larger the particle size, the lower the onset RH(i). We also demonstrate that the total number of particles present may influence the onset RH(i) observed. The surface area for ice activation, aerosol size, and temperature must all be considered when reporting onset values of ice formation onto ATD mineral dust particles. In addition, we calculate nucleation rates and contact angles of ice germs with ATD aerosols which indicate that there exists a range of active sites on the surface with different efficiencies for activating ice formation.
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Binary Homogeneous Nucleation in Selected Aqueous
Czech Academy of Sciences Publication Activity Database
Maršík, František; Němec, Tomáš; Hrubý, Jan; Demo, Pavel; Kožíšek, Zdeněk; Petr, V.; Kolovratník, M.
2008-01-01
Roč. 37, č. 12 (2008), s. 1671-1708 ISSN 0095-9782 R&D Projects: GA ČR(CZ) GA101/05/2524; GA AV ČR KJB400760701; GA MŠk(CZ) 1M06031; GA AV ČR IBS2076003 Institutional research plan: CEZ:AV0Z20760514; CEZ:AV0Z10100520 Keywords : nucleation * steam * theory Subject RIV: BJ - Thermodynamics Impact factor: 1.241, year: 2008 http://www.springerlink.com/content/104381/
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Energy Technology Data Exchange (ETDEWEB)
Nejad, Pajand
2005-03-01
To find out whether bacteria isolated from diseased plant parts can be the main causal agent for the dieback appearing in Salix energy forestry plantations in Sweden during the last few years, and if the joint effects of bacteria and frost injury are synergistic, extensive sampling of shoots from diseased Salix plants was performed. We performed several laboratory and greenhouse investigations and used evaluation techniques on the functions of the Ice-Nucleation Active (INA) bacteria. We carried out a comparison between spring and autumn bacterial communities isolated from within (endophytically) and surface (epiphytically) plant tissues of Salix viminalis. Seasonal variation of bacteria in willow clones with different levels of frost sensitivity and symptoms of bacterial damage was also investigated. We further focussed on possible effect of fertilisation and nutrient availability on the bacterial community in relation to plant dieback in Estonian willow plantations. The identification and detection of INA bacteria which cause damage in combination with frost to willow (Salix spp) plants in late fall, winter and spring was performed using BIOLOG MicroPlate, biochemical tests, selective INA primers and 16S rDNA analysis. To distinguish the character for differentiation between these bacteria morphologically and with respect to growing ability different culture media were used. We studied the temperature, at which ice nucleation occurred for individual bacteria, estimated the population of INA bacteria, effect of growth limiting factors, and evaluated the effect of chemical and physical agents for disruption and possible inhibition of INA among individual bacterial strains. The concentration of carbon, nitrogen and phosphorus on INA is discussed. We demonstrate that among the bacterial isolates recovered from the willow plantations, there were many that were capable of ice nucleation at temperatures between -2 and -10 deg C, many that were capable of inducing a
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Schill, Gregory P.; DeMott, Paul J.; Levin, Ezra J. T.; Kreidenweis, Sonia M.
2018-05-01
Ice nucleation is a fundamental atmospheric process that impacts precipitation, cloud lifetimes, and climate. Challenges remain to identify and quantify the compositions and sources of ice-nucleating particles (INPs). Assessment of the role of black carbon (BC) as an INP is particularly important due to its anthropogenic sources and abundance at upper-tropospheric cloud levels. The role of BC as an INP, however, is unclear. This is, in part, driven by a lack of techniques that directly determine the contribution of refractory BC (rBC) to INP concentrations. One previously developed technique to measure this contribution uses the Single Particle Soot Photometer (SP2) as a pre-filter to an online ice-nucleating particle counter. In this technique, rBC particles are selectively heated to their vaporization temperature in the SP2 cavity by a 1064 nm laser. From previous work, however, it is unclear under what SP2 conditions, if any, the original rBC particles were fully vaporized. Furthermore, previous work also left questions about the effect of the SP2 laser on the ice-nucleating properties of several INP proxies and their mixtures with rBC.To answer these questions, we sampled the exhaust of an SP2 with a Scanning Mobility Particle Sizer and a Continuous Flow Diffusion Chamber. Using Aquadag® as an rBC proxy, the effect of several SP2 instrument parameters on the size distribution and physical properties of particles in rBC SP2 exhaust were explored. We found that a high SP2 laser power (930 nW/(220 nm PSL)) is required to fully vaporize a ˜ 0.76 fg rBC particle. We also found that the exhaust particle size distribution is minimally affected by the SP2 sheath-to-sample ratio; the size of the original rBC particle, however, greatly influences the size distribution of the SP2 exhaust. The effect of the SP2 laser on the ice nucleation efficiency of Snomax®, NX-illite, and Suwannee River Fulvic Acid was studied; these particles acted as proxies for biological, illite
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International Nuclear Information System (INIS)
Hegg, D A; Baker, M B
2009-01-01
Small particles play major roles in modulating radiative and hydrological fluxes in the atmosphere and thus they impact both climate (IPCC 2007) and weather. Most atmospheric particles outside clouds are created in situ through nucleation from gas phase precursors and most ice particles within clouds are formed by nucleation, usually from the liquid. Thus, the nucleation process is of great significance in the Earth's atmosphere. The theoretical examination of nucleation in the atmosphere has been based mostly on classical nucleation theory. While diagnostically very useful, the prognostic skill demonstrated by this approach has been marginal. Microscopic approaches such as molecular dynamics and density functional theory have also proven useful in elucidating various aspects of the process but are not yet sufficiently refined to offer a significant prognostic advantage to the classical approach, due primarily to the heteromolecular nature of atmospheric nucleation. An important aspect of the nucleation process in the atmosphere is that the degree of metastability of the parent phase for the nucleation is modulated by a number of atmospheric processes such as condensation onto pre-existing particles, updraft velocities that are the main driving force for supersaturation of water (a major factor in all atmospheric nucleation), and photochemical production rates of nucleation precursors. Hence, atmospheric nucleation is both temporally and spatially inhomogeneous
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Numerical simulations of homogeneous freezing processes in the aerosol chamber AIDA
Directory of Open Access Journals (Sweden)
W. Haag
2003-01-01
Full Text Available The homogeneous freezing of supercooled H2SO4/H2O aerosols in an aerosol chamber is investigated with a microphysical box model using the activity parameterization of the nucleation rate by Koop et al. (2000. The simulations are constrained by measurements of pressure, temperature, total water mixing ratio, and the initial aerosol size distribution, described in a companion paper Möhler et al. (2003. Model results are compared to measurements conducted in the temperature range between 194 and 235 K, with cooling rates in the range between 0.5 and 2.6 K min-1, and at air pressures between 170 and 1000 hPa. The simulations focus on the time history of relative humidity with respect to ice, aerosol size distribution, partitioning of water between gas and particle phase, onset times of freezing, freezing threshold relative humidities, aerosol chemical composition at the onset of freezing, and the number of nucleated ice crystals. The latter four parameters can be inferred from the experiments, the former three aid in interpreting the measurements. Sensitivity studies are carried out to address the relative importance of uncertainties of basic quantities such as temperature, total H2O mixing ratio, aerosol size spectrum, and deposition coefficient of H2O molecules on ice. The ability of the numerical simulations to provide detailed explanations of the observations greatly increases confidence in attempts to model this process under real atmospheric conditions, for instance with regard to the formation of cirrus clouds or polar stratospheric ice clouds, provided that accurate temperature and humidity measurements are available.
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On the Role of Ammonia in Arctic Aerosol Nucleation and Cloud Formation
Browse, J.; Dall'Osto, M.; Geels, C.; Skov, H.; Massling, A.; Boertmann, D.; Beddows, D.; Gordon, H.; Pringle, K.
2017-12-01
This study investigates the importance of ammonia in Arctic aerosol nucleation and the formation of cloud condensation nuclei (CCN) at high-latitudes. The importance of atmospheric nucleation processes to summertime Arctic aerosol concentration has been frequently noted at ground-stations, during campaigns and within models (which typically predict that the majority of aerosol in the Arctic summertime boundary layer derives from nucleation). However, as nucleation mechanisms in global models have increased in complexity (improving model skill globally) our skill in the Arctic has generally decreased. This decrease in model skill is likely due to a lack of organic compounds (monterpenes etc.) in the modelled high Arctic which have been identified as a key component in atmospheric nucleation in the mid-latitudes and thus incorporated into many global nucleation parametrisations. Recently it has been suggested that ammonia (also identified as a potentially important component in atmospheric nucleation) may control nucleation processes in the Arctic. However, the source (or sources) of Arctic ammonia remain unclear. Here, we use modelling, long-term aerosol in-situ observations, high resolution sea-ice satellite observations and new emission inventories to investigate the link between ammonia sources (including bird colonies, sea-ice melt and open ocean in the marginal ice zones) and nucleation events in the mid-to-high Arctic, and thus quantify the importance of individual ammonia sources to Arctic-wide CCN and cloud droplet populations.
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Schill, G. P.; DeMott, P. J.; Suski, K. J.; Emerson, E. W.; Rauker, A. M.; Kodros, J.; Levin, E. J.; Hill, T. C. J.; Farmer, D.; Pierce, J. R.; Kreidenweis, S. M.
2017-12-01
Black carbon (BC) has been implicated as a potential immersion-mode ice nucleating particle (INP) because of its relative abundance in the upper troposphere. Furthermore, several field and aircraft measurements have observed positive correlations between BC and INP concentrations. Despite this, the efficiency of BC to act as an immersion-mode INP is poorly constrained. Indeed, previous results from laboratory studies are in conflict, with estimates of BC's impact on INP ranging from no impact to being efficient enough to rival the well-known INP mineral dust. It is, however, becoming clear that the ice nucleation activity of BC may depend on both its fuel type and combustion conditions. For example, previous work has shown that diesel exhaust BC is an extremely poor immersion-mode INP, but laboratory burns of biomass fuels indicate that BC can contribute up to 70% of all INP for some fuel types. Given these dependencies, we propose that sampling from real-world biomass burning sources would provide the most useful new information on the contribution of BC to atmospheric INP. In this work, we will present recent results looking at the sources of INP from prescribed burns and wildfires. To determine the specific contribution of refractory black carbon (rBC) to INP concentrations, we utilized a new technique that couples the Single Particle Soot Photometer (SP2) to the Colorado State University Continuous Flow Diffusion Chamber (CFDC). The SP2 utilizes laser-induced incandescence to quantify rBC mass on a particle-by-particle basis; in doing so, it also selectively destroys rBC particles by heating them to their vaporization temperature. Thus, the SP2 can be used as a selective pre-filter for rBC into the CFDC. Furthermore, we have also used a filter-based technique for measuring INP, the Ice Spectrometer, which can employ pretreatments such as heating and digestion by H2O2 to determine the contribution of heat-labile and organic particles, respectively.
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Lintunen, A.; Hölttä, T.; Kulmala, M.
2013-01-01
Water in the xylem, the water transport system of plants, is vulnerable to freezing and cavitation, i.e. to phase change from liquid to ice or gaseous phase. The former is a threat in cold and the latter in dry environmental conditions. Here we show that a small xylem conduit diameter, which has previously been shown to be associated with lower cavitation pressure thus making a plant more drought resistant, is also associated with a decrease in the temperature required for ice nucleation in the xylem. Thus the susceptibility of freezing and cavitation are linked together in the xylem of plants. We explain this linkage by the regulation of the sizes of the nuclei catalysing freezing and drought cavitation. Our results offer better understanding of the similarities of adaption of plants to cold and drought stress, and offer new insights into the ability of plants to adapt to the changing environment. PMID:23778457
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Directory of Open Access Journals (Sweden)
DIANA ELIZABETH WATURANGI
2009-06-01
Full Text Available Ice nucleation active (INA bacteria is a group of bacteria with the ability to catalyze the ice formation at temperature above -10 °C and causing frost injury in plants. Since, most of the literature on INA bacteria were from subtropical area, studies of INA bacteria from tropical area are needed. We sampled eight fruits and 36 leaves of 21 plant species, and then identified through biochemical and genetic analysis. INA bacteria were characterized for INA protein classification, pH stability, and optimization of heat endurance. We discovered 15 INA bacteria from seven plants species. Most of bacteria are oxidase and H2S negative, catalase and citrate positive, gram negative, and cocoid formed. These INA bacteria were classified in to three classes based on their freezing temperature. Most of the isolates were active in heat and pH stability assay. Some isolates were analysed for 16S rRNA gene. We observed that isolates from Morinda citrifolia shared 97% similiarity with Pseudomonas sp. Isolate from Piper betle shared 93% similarity with P. pseudoalcaligenes. Isolate from Carica papaya shared 94% similarity with Pseudomonas sp. While isolate from Fragaria vesca shared 90% similarity with Sphingomonas sp.
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Directory of Open Access Journals (Sweden)
DIANA ELIZABETH WATURANGI
2009-06-01
Full Text Available Ice nucleation active (INA bacteria is a group of bacteria with the ability to catalyze the ice formation at temperature above -10 oC and causing frost injury in plants. Since, most of the literature on INA bacteria were from subtropical area, studies of INA bacteria from tropical area are needed. We sampled eight fruits and 36 leaves of 21 plant species, and then identified through biochemical and genetic analysis. INA bacteria were characterized for INA protein classification, pH stability, and optimization of heat endurance. We discovered 15 INA bacteria from seven plants species. Most of bacteria are oxidase and H2S negative, catalase and citrate positive, gram negative, and cocoid formed. These INA bacteria were classified in to three classes based on their freezing temperature. Most of the isolates were active in heat and pH stability assay. Some isolates were analysed for 16S rRNA gene. We observed that isolates from Morinda citrifolia shared 97% similiarity with Pseudomonas sp. Isolate from Piper betle shared 93% similarity with P. pseudoalcaligenes. Isolate from Carica papaya shared 94% similarity with Pseudomonas sp. While isolate from Fragaria vesca shared 90% similarity with Sphingomonas sp.
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Langenbach, K.; Heilig, M.; Horsch, M.; Hasse, H.
2018-03-01
A new method for predicting homogeneous bubble nucleation rates of pure compounds from vapor-liquid equilibrium (VLE) data is presented. It combines molecular dynamics simulation on the one side with density gradient theory using an equation of state (EOS) on the other. The new method is applied here to predict bubble nucleation rates in metastable liquid carbon dioxide (CO2). The molecular model of CO2 is taken from previous work of our group. PC-SAFT is used as an EOS. The consistency between the molecular model and the EOS is achieved by adjusting the PC-SAFT parameters to VLE data obtained from the molecular model. The influence parameter of density gradient theory is fitted to the surface tension of the molecular model. Massively parallel molecular dynamics simulations are performed close to the spinodal to compute bubble nucleation rates. From these simulations, the kinetic prefactor of the hybrid nucleation theory is estimated, whereas the nucleation barrier is calculated from density gradient theory. This enables the extrapolation of molecular simulation data to the whole metastable range including technically relevant densities. The results are tested against available experimental data and found to be in good agreement. The new method does not suffer from typical deficiencies of classical nucleation theory concerning the thermodynamic barrier at the spinodal and the bubble size dependence of surface tension, which is typically neglected in classical nucleation theory. In addition, the density in the center of critical bubbles and their surface tension is determined as a function of their radius. The usual linear Tolman correction to the capillarity approximation is found to be invalid.
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Langenbach, K; Heilig, M; Horsch, M; Hasse, H
2018-03-28
A new method for predicting homogeneous bubble nucleation rates of pure compounds from vapor-liquid equilibrium (VLE) data is presented. It combines molecular dynamics simulation on the one side with density gradient theory using an equation of state (EOS) on the other. The new method is applied here to predict bubble nucleation rates in metastable liquid carbon dioxide (CO 2 ). The molecular model of CO 2 is taken from previous work of our group. PC-SAFT is used as an EOS. The consistency between the molecular model and the EOS is achieved by adjusting the PC-SAFT parameters to VLE data obtained from the molecular model. The influence parameter of density gradient theory is fitted to the surface tension of the molecular model. Massively parallel molecular dynamics simulations are performed close to the spinodal to compute bubble nucleation rates. From these simulations, the kinetic prefactor of the hybrid nucleation theory is estimated, whereas the nucleation barrier is calculated from density gradient theory. This enables the extrapolation of molecular simulation data to the whole metastable range including technically relevant densities. The results are tested against available experimental data and found to be in good agreement. The new method does not suffer from typical deficiencies of classical nucleation theory concerning the thermodynamic barrier at the spinodal and the bubble size dependence of surface tension, which is typically neglected in classical nucleation theory. In addition, the density in the center of critical bubbles and their surface tension is determined as a function of their radius. The usual linear Tolman correction to the capillarity approximation is found to be invalid.
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A novel approach to the theory of homogeneous and heterogeneous nucleation.
Ruckenstein, Eli; Berim, Gersh O; Narsimhan, Ganesan
2015-01-01
A new approach to the theory of nucleation, formulated relatively recently by Ruckenstein, Narsimhan, and Nowakowski (see Refs. [7-16]) and developed further by Ruckenstein and other colleagues, is presented. In contrast to the classical nucleation theory, which is based on calculating the free energy of formation of a cluster of the new phase as a function of its size on the basis of macroscopic thermodynamics, the proposed theory uses the kinetic theory of fluids to calculate the condensation (W(+)) and dissociation (W(-)) rates on and from the surface of the cluster, respectively. The dissociation rate of a monomer from a cluster is evaluated from the average time spent by a surface monomer in the potential well as obtained from the solution of the Fokker-Planck equation in the phase space of position and momentum for liquid-to-solid transition and the phase space of energy for vapor-to-liquid transition. The condensation rates are calculated using traditional expressions. The knowledge of those two rates allows one to calculate the size of the critical cluster from the equality W(+)=W(-) as well as the rate of nucleation. The developed microscopic approach allows one to avoid the controversial application of classical thermodynamics to the description of nuclei which contain a few molecules. The new theory was applied to a number of cases, such as the liquid-to-solid and vapor-to-liquid phase transitions, binary nucleation, heterogeneous nucleation, nucleation on soluble particles and protein folding. The theory predicts higher nucleation rates at high saturation ratios (small critical clusters) than the classical nucleation theory for both solid-to-liquid as well as vapor-to-liquid transitions. As expected, at low saturation ratios for which the size of the critical cluster is large, the results of the new theory are consistent with those of the classical one. The present approach was combined with the density functional theory to account for the density
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Iwata, Ayumi; Matsuki, Atsushi
2018-02-01
In order to better characterize ice nucleating (IN) aerosol particles in the atmosphere, we investigated the chemical composition, mixing state, and morphology of atmospheric aerosols that nucleate ice under conditions relevant for mixed-phase clouds. Five standard mineral dust samples (quartz, K-feldspar, Na-feldspar, Arizona test dust, and Asian dust source particles) were compared with actual aerosol particles collected from the west coast of Japan (the city of Kanazawa) during Asian dust events in February and April 2016. Following droplet activation by particles deposited on a hydrophobic Si (silicon) wafer substrate under supersaturated air, individual IN particles were located using an optical microscope by gradually cooling the temperature to -30 °C. For the aerosol samples, both the IN active particles and non-active particles were analyzed individually by atomic force microscopy (AFM), micro-Raman spectroscopy, and scanning electron microscopy (SEM) coupled with energy dispersive X-ray spectroscopy (EDX). Heterogeneous ice nucleation in all standard mineral dust samples tested in this study was observed at consistently higher temperatures (e.g., -22.2 to -24.2 °C with K-feldspar) than the homogeneous freezing temperature (-36.5 °C). Meanwhile, most of the IN active atmospheric particles formed ice below -28 °C, i.e., at lower temperatures than the standard mineral dust samples of pure components. The most abundant IN active particles above -30 °C were predominantly irregular solid particles that showed clay mineral characteristics (or mixtures of several mineral components). Other than clay, Ca-rich particles internally mixed with other components, such as sulfate, were also regarded as IN active particle types. Moreover, sea salt particles were predominantly found in the non-active fraction, and internal mixing with sea salt clearly acted as a significant inhibiting agent for the ice nucleation activity of mineral dust particles. Also, relatively
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Survival and ice nucleation activity of bacteria as aerosols in a cloud simulation chamber
Amato, P.; Joly, M.; Schaupp, C.; Attard, E.; Möhler, O.; Morris, C. E.; Brunet, Y.; Delort, A.-M.
2015-06-01
The residence time of bacterial cells in the atmosphere is predictable by numerical models. However, estimations of their aerial dispersion as living entities are limited by a lack of information concerning survival rates and behavior in relation to atmospheric water. Here we investigate the viability and ice nucleation (IN) activity of typical atmospheric ice nucleation active bacteria (Pseudomonas syringae and P. fluorescens) when airborne in a cloud simulation chamber (AIDA, Karlsruhe, Germany). Cell suspensions were sprayed into the chamber and aerosol samples were collected by impingement at designated times over a total duration of up to 18 h, and at some occasions after dissipation of a cloud formed by depressurization. Aerosol concentration was monitored simultaneously by online instruments. The cultivability of airborne cells decreased exponentially over time with a half-life time of 250 ± 30 min (about 3.5 to 4.5 h). In contrast, IN activity remained unchanged for several hours after aerosolization, demonstrating that IN activity was maintained after cell death. Interestingly, the relative abundance of IN active cells still airborne in the chamber was strongly decreased after cloud formation and dissipation. This illustrates the preferential precipitation of IN active cells by wet processes. Our results indicate that from 106 cells aerosolized from a surface, one would survive the average duration of its atmospheric journey estimated at 3.4 days. Statistically, this corresponds to the emission of 1 cell that achieves dissemination every ~ 33 min m-2 of cultivated crops fields, a strong source of airborne bacteria. Based on the observed survival rates, depending on wind speed, the trajectory endpoint could be situated several hundreds to thousands of kilometers from the emission source. These results should improve the representation of the aerial dissemination of bacteria in numeric models.
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Leisner, T.; Abdelmonem, A.; Benz, S.; Brinkmann, M.; Möhler, O.; Rzesanke, D.; Saathoff, H.; Schnaiter, M.; Wagner, R.
2009-04-01
The formation of ice in tropospheric clouds controls the evolution of precipitation and thereby influences climate and weather via a complex network of dynamical and microphysical processes. At higher altitudes, ice particles in cirrus clouds or contrails modify the radiative energy budget by direct interaction with the shortwave and longwave radiation. In order to improve the parameterisation of the complex microphysical and dynamical processes leading to and controlling the evolution of tropospheric ice, laboratory experiments are performed at the IMK Karlsruhe both on a single particle level and in the aerosol and cloud chamber AIDA. Single particle experiments in electrodynamic levitation lend themselves to the study of the interaction between cloud droplets and aerosol particles under extremely well characterized and static conditions in order to obtain microphysical parameters as freezing nucleation rates for homogeneous and heterogeneous ice formation. They also allow the observation of the freezing dynamics and of secondary ice formation and multiplication processes under controlled conditions and with very high spatial and temporal resolution. The inherent droplet charge in these experiments can be varied over a wide range in order to assess the influence of the electrical state of the cloud on its microphysics. In the AIDA chamber on the other hand, these processes are observable under the realistic dynamic conditions of an expanding and cooling cloud- parcel with interacting particles and are probed simultaneously by a comprehensive set of analytical instruments. By this means, microphysical processes can be studied in their complex interplay with dynamical processes as for example coagulation or particle evaporation and growth via the Bergeron - Findeisen process. Shortwave scattering and longwave absorption properties of the nucleating and growing ice crystals are probed by in situ polarised laser light scattering measurements and infrared extinction
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DEFF Research Database (Denmark)
Toxværd, Søren
2016-01-01
temperature Ttr.p. crystallizes via a liquid droplet is an example of Ostwald's step rule. The homogeneous nucleation in the supersaturated gas is not to a crystal, but to a liquid-like critical nucleus. We have for the first time performed constant energy (NVE) Molecular Dynamics (MD) of homogeneous...... nucleation without the use of a thermostat. The simulations of homogeneous nucleation in a Lennard-Jones system from supersaturated vapor at temperatures below Ttr.p. reveals that the nucleation to a liquid-like critical nucleus is initiated by a small cold cluster [S. Toxvaerd, J. Chem. Phys. \\textbf{143...
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Sassen, Kenneth; Arnott, W. Patrick; O'C. Starr, David; Mace, Gerald G.; Wang, Zhien; Poellot, Michael R.
2003-04-01
Hurricane Nora traveled up the Baja Peninsula coast in the unusually warm El Niño waters of September 1997 until rapidly decaying as it approached southern California on 24 September. The anvil cirrus blowoff from the final surge of tropical convection became embedded in subtropical flow that advected the cirrus across the western United States, where it was studied from the Facility for Atmospheric Remote Sensing (FARS) in Salt Lake City, Utah, on 25 September. A day later, the cirrus shield remnants were redirected southward by midlatitude circulations into the southern Great Plains, providing a case study opportunity for the research aircraft and ground-based remote sensors assembled at the Clouds and Radiation Testbed (CART) site in northern Oklahoma. Using these comprehensive resources and new remote sensing cloud retrieval algorithms, the microphysical and radiative cloud properties of this unusual cirrus event are uniquely characterized.Importantly, at both the FARS and CART sites the cirrus generated spectacular halos and arcs, which acted as a tracer for the hurricane cirrus, despite the limited lifetimes of individual ice crystals. Lidar depolarization data indicate widespread regions of uniform ice plate orientations, and in situ particle replicator data show a preponderance of pristine, solid hexagonal plates and columns. It is suggested that these unusual aspects are the result of the mode of cirrus particle nucleation, presumably involving the lofting of sea salt nuclei in strong thunderstorm updrafts into the upper troposphere. This created a reservoir of haze particles that continued to produce halide-salt-contaminated ice crystals during the extended period of cirrus cloud maintenance. The inference that marine microbiota are embedded in the replicas of some ice crystals collected over the CART site points to the longevity of marine effects. Various nucleation scenarios proposed for cirrus clouds based on this and other studies, and the
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Pietsch, Renée B; Vinatzer, Boris A; Schmale, David G
2017-01-01
The bacterium Pseudomonas syringae is found in a variety of terrestrial and aquatic environments. Some strains of P. syringae express an ice nucleation protein (hereafter referred to as Ice+) allowing them to catalyze the heterogeneous freezing of water. Though P. syringae has been sampled intensively from freshwater sources in France, little is known about the genetic diversity of P. syringae in natural aquatic habitats in North America. We collected samples of freshwater from three different depths in Claytor Lake, Virginia, USA between November 2015 and June 2016. Samples were plated on non-selective medium (TSA) and on medium selective for Pseudomonas (KBC) and closely related species to estimate the total number of culturable bacteria and of Pseudomonas , respectively. A droplet freezing assay was used to screen colonies for the Ice+ phenotype. Ice+ colonies were then molecularly identified based on the cts (citrate synthase) gene and the 16S rDNA gene. Phylogenetic analysis of cts sequences showed a surprising diversity of phylogenetic subgroups of P. syringae . Frequencies of Ice+ isolates on P. syringae selective medium ranged from 0 to 15% per sample with the highest frequency being found in spring. Our work shows that freshwater lakes can be a significant reservoir of Ice+ P. syringae . Future work is needed to determine the contribution of P. syringae from freshwater lakes to the P. syringae populations present in the atmosphere and on plants and, in particular, if freshwater lakes could be an inoculum source of P. syringae -caused plant disease outbreaks.
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Major new sources of biological ice nuclei
Moffett, B. F.; Hill, T.; Henderson-Begg, S. K.
2009-12-01
Almost all research on biological ice nucleation has focussed on a limited number of bacteria. Here we characterise several major new sources of biogenic ice nuclei. These include mosses, hornworts, liverworts and cyanobacteria. Ice nucleation in the eukaryotic bryophytes appears to be ubiquitous. The temperature at which these organisms nucleate is that at which the difference in vapour pressure over ice and water is at or close to its maximum. At these temperatures (-8 to -18 degrees C) ice will grow at the expense of supercooled water. These organisms are dependent for their water on occult precipitation - fog, dew and cloudwater which by its nature is not collected in conventional rain gauges. Therefore we suggest that these organism produce ice nuclei as a water harvesting mechanism. Since the same mechanism would also drive the Bergeron-Findeisen process, and as moss is known to become airborne, these nuclei may have a role in the initiation of precipitation. The properties of these ice nuclei are very different from the well characterised bacterial nuclei. We will also present DNA sequence data showing that, although related, the proteins responsible are only very distantly related to the classical bacterial ice nuclei.
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Nucleation and Growth Kinetics from LaMer Burst Data.
Chu, Daniel B K; Owen, Jonathan S; Peters, Baron
2017-10-12
In LaMer burst nucleation, the individual nucleation events happen en masse, quasi-simultaneously, and at nearly identical homogeneous conditions. These properties make LaMer burst nucleation important for applications that require monodispersed particles and also for theoretical analyses. Sugimoto and co-workers predicted that the number of nuclei generated during a LaMer burst depends only on the solute supply rate and the growth rate, independent of the nucleation kinetics. Some experiments confirm that solute supply kinetics control the number of nuclei, but flaws in the original theoretical analysis raise questions about the predicted roles of growth and nucleation kinetics. We provide a rigorous analysis of the coupled equations that govern concentrations of nuclei and solutes. Our analysis confirms that the number of nuclei is largely determined by the solute supply and growth rates, but our predicted relationship differs from that of Sugimoto et al. Moreover, we find that additional nucleus size dependent corrections should emerge in systems with slow growth kinetics. Finally, we show how the nucleation kinetics determine the particle size distribution. We suggest that measured particle size distributions might therefore provide ways to test theoretical models of homogeneous nucleation kinetics.
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What experiments on pinned nanobubbles can tell about the critical nucleus for bubble nucleation.
Xiao, Qianxiang; Liu, Yawei; Guo, Zhenjiang; Liu, Zhiping; Frenkel, Daan; Dobnikar, Jure; Zhang, Xianren
2017-12-22
The process of homogeneous bubble nucleation is almost impossible to probe experimentally, except near the critical point or for liquids under large negative tension. Elsewhere in the phase diagram, the bubble nucleation barrier is so high as to be effectively insurmountable. Consequently, there is a severe lack of experimental studies of homogenous bubble nucleation under conditions of practical importance (e.g., cavitation). Here we use a simple geometric relation to show that we can obtain information about the homogeneous nucleation process from Molecular Dynamics studies of bubble formation in solvophobic nanopores on a solid surface. The free energy of pinned nanobubbles has two extrema as a function of volume: one state corresponds to a free-energy maximum ("the critical nucleus"), the other corresponds to a free-energy minimum (the metastable, pinned nanobubble). Provided that the surface tension does not depend on nanobubble curvature, the radius of the curvature of the metastable surface nanobubble is independent of the radius of the pore and is equal to the radius of the critical nucleus in homogenous bubble nucleation. This observation opens the way to probe the parameters that determine homogeneous bubble nucleation under experimentally accessible conditions, e.g. with AFM studies of metastable nanobubbles. Our theoretical analysis also indicates that a surface with pores of different sizes can be used to determine the curvature corrections to the surface tension. Our conclusions are not limited to bubble nucleation but suggest that a similar approach could be used to probe the structure of critical nuclei in crystal nucleation.
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Energy Technology Data Exchange (ETDEWEB)
Cambours, M.A.
2004-07-01
During the past decade, important dieback has been observed in short-rotation forestry plantations of Salix viminalis and S. dasyclados in Sweden and Estonia, plantations from which the isolation of ice nucleation-active (INA) and pathogenic bacteria has also been reported. This thesis investigates the connection between bacterial infection and frost as a possible cause for such damage, and the role played by internal and external factors (e.g. plant frost sensitivity, fertilisation) in the dieback observed. Bacterial floras isolated from ten Salix clones growing on fertilised/unfertilised mineral soil or nitrogen-rich organic soil, were studied. Culturable bacterial communities present both in internal necrotic tissues and on the plant surface (i.e. epiphytes) were isolated on two occasions (spring and autumn). The strains were biochemically characterised (with gram, oxidase and fluorescence tests), and tested for ice nucleation-activity. Their pathogenic properties were studied with and without association to a freezing stress. Certain strains were eventually identified with BIOLOG plates and 16S rRNA analysis. A high number of culturable bacterial strains was found in the plant samplings, belonging mainly to Erwinia and Sphingomonas spp.; pathogenic and INA communities being mostly Erwinia-, Sphingomonas- and Xanthomonas-like. The generally higher plant dieback noted in the field on nutrient-rich soils and for frost sensitive clones was found connected to higher numbers of pathogenic and INA bacteria in the plants. We thus confirm Salix dieback to be related to a synergistic effect of frost and bacterial infection, possibly aggravated by fertilisation.
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Directory of Open Access Journals (Sweden)
A. Iwata
2018-02-01
Full Text Available In order to better characterize ice nucleating (IN aerosol particles in the atmosphere, we investigated the chemical composition, mixing state, and morphology of atmospheric aerosols that nucleate ice under conditions relevant for mixed-phase clouds. Five standard mineral dust samples (quartz, K-feldspar, Na-feldspar, Arizona test dust, and Asian dust source particles were compared with actual aerosol particles collected from the west coast of Japan (the city of Kanazawa during Asian dust events in February and April 2016. Following droplet activation by particles deposited on a hydrophobic Si (silicon wafer substrate under supersaturated air, individual IN particles were located using an optical microscope by gradually cooling the temperature to −30 °C. For the aerosol samples, both the IN active particles and non-active particles were analyzed individually by atomic force microscopy (AFM, micro-Raman spectroscopy, and scanning electron microscopy (SEM coupled with energy dispersive X-ray spectroscopy (EDX. Heterogeneous ice nucleation in all standard mineral dust samples tested in this study was observed at consistently higher temperatures (e.g., −22.2 to −24.2 °C with K-feldspar than the homogeneous freezing temperature (−36.5 °C. Meanwhile, most of the IN active atmospheric particles formed ice below −28 °C, i.e., at lower temperatures than the standard mineral dust samples of pure components. The most abundant IN active particles above −30 °C were predominantly irregular solid particles that showed clay mineral characteristics (or mixtures of several mineral components. Other than clay, Ca-rich particles internally mixed with other components, such as sulfate, were also regarded as IN active particle types. Moreover, sea salt particles were predominantly found in the non-active fraction, and internal mixing with sea salt clearly acted as a significant inhibiting agent for the ice nucleation activity of mineral
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Kim, J; Yli-Juuti, T; Lawler, M; Keskinen, H; Tröstl, J; Schobesberger, S; Duplissy, J; Amorim, A; Bianchi, F; Donahue, N M; Flagan, R C; Hakala, J; Heinritzi, M; Jokinen, T; Kürten, A; Laaksonen, A; Lehtipalo, K; Miettinen, P; Petäjä, T; Rissanen, M P; Rondo, L; Sengupta, K; Simon, M; Tomé, A; Williamson, C; Wimmer, D; Winkler, P M; Ehrhart, S; Ye, P; Kirkby, J; Curtius, J; Baltensperger, U; Kulmala, M; Lehtinen, K E J; Smith, J N; Riipinen, I; Virtanen, A
2016-01-01
Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e., particles that have grown to diameters of 10 and 15 nm following nucleation, and measure their water uptake. Water uptake is useful information for indirectly obtaining chemical composition of aerosol particles. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) at subsaturated conditions (ca. 90 % relative humidity at 293 K) to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7) campaign performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was meas...
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A dynamical theory of nucleation
Lutsko, James F.
2013-05-01
A dynamical theory of nucleation based on fluctuating hydrodynamics is described. It is developed in detail for the case of diffusion-limited nucleation appropriate to colloids and macro-molecules in solution. By incorporating fluctuations, realistic fluid-transport and realistic free energy models the theory is able to give a unified treatment of both the pre-critical development of fluctuations leading to a critical cluster as well as of post-critical growth. Standard results from classical nucleation theory are shown to follow in the weak noise limit while the generality of the theory allows for many extensions including the description of very high supersaturations (small clusters), multiple order parameters and strong-noise effects to name a few. The theory is applied to homogeneous and heterogeneous nucleation of a model globular protein in a confined volume and it is found that nucleation depends critically on the existence of long-wavelength, small-amplitude density fluctuations.
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Application of nonequilibrium quantum statistical mechanics to homogeneous nucleation
International Nuclear Information System (INIS)
Larson, A.R.; Cantrell, C.D.
1978-01-01
The master equation for cluster growth and evaporation is derived from many-body quantum mechanics and from a modified version of quantum damping theory used in laser physics. For application to nucleation theory, the quantum damping theory has been generalized to include system and reservoir states that are not separate entities. Formulae for rate constants are obtained. Solutions of the master equation yield equations of state and system-averaged quantities recognized as thermodynamic variables. Formulae for Helmholtz free energies of clusters in a Debye approximation are derived. Coexistence-line equations for pressure volume, and number of clusters are obtained from equations-of-state analysis. Coexistence-line and surface-tension data are used to obtain values of parameters for the Debye approximation. These data are employed in calculating both the nucleation current in diffusion cloud chamber experiments and the onset of condensation in expansion nozzle experiments. Theoretical and experimental results are similar for both cloud-chamber and nozzle experiments, which measure water
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International Nuclear Information System (INIS)
Mikheev, Vladimir B.; Laulainen, Nels S.; Barlow, Stephan E.; Knott, Michael; Ford, Ian J.
2000-01-01
A laminar flow tube reactor was designed and constructed to provide an accurate, quantitative measurement of a nucleation rate as a function of supersaturation and temperature. Measurements of nucleation of a supersaturated vapor of dibutylphthalate have been made for the temperature range from -30.3 to +19.1 degree sign C. A thorough analysis of the possible sources of experimental uncertainties (such as defining the correct value of the initial vapor concentration, temperature boundary conditions on the reactor walls, accuracy of the calculations of the thermodynamic parameters of the nucleation zone, and particle concentration measurement) is given. Both isothermal and the isobaric nucleation rates were measured. The experimental data obtained were compared with the measurements of other experimental groups and with theoretical predictions made on the basis of the self-consistency correction nucleation theory. Theoretical analysis, based on the first and the second nucleation theorems, is also presented. The critical cluster size and the excess of internal energy of the critical cluster are obtained. (c) 2000 American Institute of Physics
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Heterogeneous primary nucleation of ice in water and aqueous solutions
Thijssen, H.A.C.; Vorstman, M.A.G.; Roels, J.A.
1968-01-01
The effect of the volume of the liquid sample, the degree of turbulence in the liquid, and the rate of cooling upon the probability of nucleation has been studied for water and aqueous solutions. Nucleation rates were measured for droplets nearly instantaneously cooled to a predetermined
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Implications of the Homogeneous Nucleation Barrier for Top-Down Crystallization in Mercury's Core
Huguet, L.; Hauck, S. A.; Van Orman, J. A.; Jing, Z.
2018-05-01
Crystallization of solids in planetary cores depends both on ambient temperatures falling below the liquidus and on the ability to nucleate crystal growth. We discuss the implications of the nucleation barrier for thermal evolution of Mercury's core.
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Initiation of secondary ice production in clouds
Directory of Open Access Journals (Sweden)
S. C. Sullivan
2018-02-01
Full Text Available Disparities between the measured concentrations of ice-nucleating particles (INPs and in-cloud ice crystal number concentrations (ICNCs have led to the hypothesis that mechanisms other than primary nucleation form ice in the atmosphere. Here, we model three of these secondary production mechanisms – rime splintering, frozen droplet shattering, and ice–ice collisional breakup – with a six-hydrometeor-class parcel model. We perform three sets of simulations to understand temporal evolution of ice hydrometeor number (Nice, thermodynamic limitations, and the impact of parametric uncertainty when secondary production is active. Output is assessed in terms of the number of primarily nucleated ice crystals that must exist before secondary production initiates (NINP(lim as well as the ICNC enhancement from secondary production and the timing of a 100-fold enhancement. Nice evolution can be understood in terms of collision-based nonlinearity and the phasedness of the process, i.e., whether it involves ice hydrometeors, liquid ones, or both. Ice–ice collisional breakup is the only process for which a meaningful NINP(lim exists (0.002 up to 0.15 L−1. For droplet shattering and rime splintering, a warm enough cloud base temperature and modest updraft are the more important criteria for initiation. The low values of NINP(lim here suggest that, under appropriate thermodynamic conditions for secondary ice production, perturbations in cloud concentration nuclei concentrations are more influential in mixed-phase partitioning than those in INP concentrations.
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Directory of Open Access Journals (Sweden)
Masaya eIshikawa
2015-03-01
Full Text Available Wintering flower buds of cold hardy Rhododendron japonicum cooled slowly to subfreezing temperatures are known to undergo extraorgan freezing, whose mechanisms remain obscure. We revisited this material to demonstrate why bud scales freeze first in spite of their lower water content, why florets remain deeply supercooled and how seasonal adaptive responses occur in regard to extraorgan freezing in flower buds. We determined ice nucleation activity (INA of various flower bud tissues of using a test tube-based assay. Irrespective of collection sites, outer and inner bud scales that function as ice sinks in extraorgan freezing had high INA levels whilst florets that remain supercooled and act as a water source lacked INA. The INA level of bud scales was not high in late August when flower bud formation was ending, but increased to reach the highest level in late October just before the first autumnal freeze. The results support the following hypothesis: the high INA in bud scales functions as the subfreezing sensor, ensuring the primary freezing in bud scales at warmer subzero temperatures, which likely allows the migration of floret water to the bud scales and accumulation of icicles within the bud scales. The low INA in the florets helps them remain unfrozen by deep supercooling. The INA in the bud scales was resistant to grinding and autoclaving at 121°C for 15 min, implying the intrinsic nature of the INA rather than of microbial origin, whilst the INA in stem bark was autoclaving labile. Anti-nucleation activity (ANA was implicated in the leachate of autoclaved bud scales, which suppresses the INA at millimolar levels of concentration and likely differs from the colligative effects of the solutes. The tissue INA levels likely contribute to the establishment of freezing behaviors by ensuring the order of freezing in the tissues: from the primary freeze to the last tissue remaining unfrozen.
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Energy Technology Data Exchange (ETDEWEB)
Mitchell, David L. [Desert Research Institute, Reno, NV (United States)
2013-09-05
than simply using the 2D-S measurements to directly calculate Vm. By calculating Vm directly from the measured PSD, ice particle projected area and estimated mass, more accurate estimates of Vm are obtained. These Vm values were then parameterized for climate models by relating them to (1) sampling temperature and ice water content (IWC) and (2) the effective diameter (De) of the ice PSD. Parameterization (1) is appropriate for climate models having single-moment microphysical schemes whereas (2) is appropriate for double-moment microphysical schemes and yields more accurate Vm estimates. These parameterizations were developed for tropical cirrus clouds, Arctic cirrus, mid-latitude synoptic cirrus and mid-latitude anvil cirrus clouds based on field campaigns in these regions. An important but unexpected result of this research was the discovery of microphysical evidence indicating the mechanisms by which ice crystals are produced in cirrus clouds. This evidence, derived from PSD measurements, indicates that homogeneous freezing ice nucleation dominates in mid-latitude synoptic cirrus clouds, whereas heterogeneous ice nucleation processes dominate in mid-latitude anvil cirrus. Based on these findings, De was parameterized in terms of temperature (T) for conditions dominated by (1) homo- and (2) heterogeneous ice nucleation. From this, an experiment was designed for global climate models (GCMs). The net radiative forcing from cirrus clouds may be affected by the means ice is produced (homo- or heterogeneously), and this net forcing contributes to climate sensitivity (i.e. the change in mean global surface temperature resulting from a doubling of CO2). The objective of this GCM experiment was to determine how a change in ice nucleation mode affects the predicted global radiation balance. In the first simulation (Run 1), the De-T relationship for homogeneous nucleation is
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Morris, Cindy E; Conen, Franz; Alex Huffman, J; Phillips, Vaughan; Pöschl, Ulrich; Sands, David C
2014-02-01
Landscapes influence precipitation via the water vapor and energy fluxes they generate. Biologically active landscapes also generate aerosols containing microorganisms, some being capable of catalyzing ice formation and crystal growth in clouds at temperatures near 0 °C. The resulting precipitation is beneficial for the growth of plants and microorganisms. Mounting evidence from observations and numerical simulations support the plausibility of a bioprecipitation feedback cycle involving vegetated landscapes and the microorganisms they host. Furthermore, the evolutionary history of ice nucleation-active bacteria such as Pseudomonas syringae supports that they have been part of this process on geological time scales since the emergence of land plants. Elucidation of bioprecipitation feedbacks involving landscapes and their microflora could contribute to appraising the impact that modified landscapes have on regional weather and biodiversity, and to avoiding inadvertent, negative consequences of landscape management. © 2013 John Wiley & Sons Ltd.
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Nucleation mechanisms in high energy ion beam induced dewetting
Energy Technology Data Exchange (ETDEWEB)
Haag, Michael; Garmatter, Daniel; Ferhati, Redi; Amirthapandian, Sankarakumar; Bolse, Wolfgang [Institut fuer Halbleiteroptik und Funktionelle Grenzflaechen, Universitaet Stuttgart (Germany)
2011-07-01
Solid coatings, when heated above their melting points, often break up by forming small round holes, which then grow, coalesce and finally turn the initially contiguous film into a pattern of isolated droplets. Such dewetting has been intensively studied using thin polymer films on Si. Three different hole nucleation mechanisms were discovered: homogeneous (spontaneous) nucleation, heterogeneous nucleation at defects, and spinodal dewetting by self-amplifying capillary waves. We have recently found that swift heavy ion (SHI) irradiation of thin oxide films on Si results in similar dewetting patterns, even though the films were kept far below their melting points. Using our new in-situ SEM at the UNILAC accelerator of GSI, we were now able to identify the mechanisms behind this SHI induced dewetting phenomenon. By varying the film thickness and introducing defects at the interface, we can directly address the hole nucleation processes. Besides homogeneous and heterogeneous nucleation, we also found a process, which very much resembles the spinodal mechanism found for liquid polymers, although in the present case the instable wavy surface is not generated by capillary waves, but by ion beam induced stresses.
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Nucleation and cavitation in parahydrogen
International Nuclear Information System (INIS)
Pi, Martí; Barranco, Manuel; Navarro, Jesús; Ancilotto, Francesco
2012-01-01
Highlights: ► We have constructed a density functional (DF) for parahydrogen between 14 and 32 K. ► The experimental equation of state and the surface tension are well reproduced. ► We have investigated nucleation and cavitations processes in the metastable phase. ► We have obtained the electron bubble explosion within the capillary model. - Abstract: We have used a density functional approach to investigate thermal homogeneous nucleation and cavitation in parahydrogen. The effect of electrons as seeds of heterogeneous cavitation in liquid parahydrogen is also discussed within the capillary model.
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Dumitrescu, Lucia R; Smeulders, David M J; Dam, Jacques A M; Gaastra-Nedea, Silvia V
2017-02-28
Molecular dynamics (MD) simulations were conducted to study nucleation of water at 350 K in argon using TIP4P and TIP4P/2005 water models. We found that the stability of any cluster, even if large, strongly depends on the energetic interactions with its vicinity, while the stable clusters change their composition almost entirely during nucleation. Using the threshold method, direct nucleation rates are obtained. Our nucleation rates are found to be 1.08×10 27 cm -3 s -1 for TIP4P and 2.30×10 27 cm -3 s -1 for TIP4P/2005. The latter model prescribes a faster dynamics than the former, with a nucleation rate two times larger due to its higher electrostatic charges. The non-equilibrium water densities derived from simulations and state-of-art equilibrium parameters from Vega and de Miguel [J. Chem. Phys. 126, 154707 (2007)] are used for the classical nucleation theory (CNT) prediction. The CNT overestimates our results for both water models, where TIP4P/2005 shows largest discrepancy. Our results complement earlier data at high nucleation rates and supersaturations in the Hale plot [Phys. Rev. A 33, 4156 (1986)], and are consistent with MD data on the SPC/E and the TIP4P/2005 model.
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Maloney, C.; Toon, B.; Bardeen, C.
2017-12-01
Recent studies indicate that heterogeneous nucleation may play a large role in cirrus cloud formation in the UT/LS, a region previously thought to be primarily dominated by homogeneous nucleation. As a result, it is beneficial to ensure that general circulation models properly represent heterogeneous nucleation in ice cloud simulations. Our work strives towards addressing this issue in the NSF/DOE Community Earth System Model's atmospheric model, CAM. More specifically we are addressing the role of heterogeneous nucleation in the coupled sectional microphysics cloud model, CARMA. Currently, our CAM/CARMA cirrus model only performs homogenous ice nucleation while ignoring heterogeneous nucleation. In our work, we couple the CAM/CARMA cirrus model with the Modal Aerosol Model (MAM). By combining the aerosol model with CAM/CARMA we can both account for heterogeneous nucleation, as well as directly link the sulfates used for homogeneous nucleation to computed fields instead of the current static field being utilized. Here we present our initial results and compare our findings to observations from the long running CALIPSO and MODIS satellite missions.
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Patterns of ice nuclei from natural water sources in the mountains of Tirol, Austria
Baloh, Philipp; Hanlon, Regina; Pietsch, Renee; Anderson, Christopher; Schmale, David G., III; Grothe, Hinrich
2017-04-01
Heterogeneous ice nucleation—the process by which particles can nucleate ice between 0 and -35°C—is important for generating artificial snow. Though abiotic and biotic ice nuclei are present in many different natural and managed ecosystems, little is known about their nature, sources, and ecological roles. We collected samples of water and snow from the mountains of Tyrol, Austria in June, July, and November, 2016. The collected water was mostly from sources with minimal anthropogenic pollution, since most of the water from the sampled streams came from glacial melt. The samples were filtered through a 0.22μm filter, and microorganisms were cultured on different types of media. Resulting colonies were tested for their ice nucleation ability using a droplet freezing assay and identified to the level of the species. The unfiltered water and the filtered water will be subjected to additional assays using cryo microscopy and vibrational microscopy (IR and Raman- spectroscopy). Preliminary analyses suggested that the percentage of ice-nucleating microbes varied with season; greater percentages of ice nucleating microbes were present during colder months. The glacial melt also varies strongly over the year with the fraction of mineral dust suspended in it which serves as an inorganic ice nucleation agent. Further investigation of these samples may help to show the combined ice nuleation abilities of biological and non biological particles present in the mountains of Tirol, Austria. Future work may shed light on how the nucleation properties of the natural water changes with the time of the year and what may be responsible for these changes.
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Ion irradiation enhanced crystal nucleation in amorphous Si thin films
International Nuclear Information System (INIS)
Im, J.S.; Atwater, H.A.
1990-01-01
The nucleation kinetics of the amorphous-to-crystal transition of Si films under 1.5 MeV Xe + irradiation have been investigated by means of in situ transmission electron microscopy in the temperature range T=500--580 degree C. After an incubation period during which negligible nucleation occurs, a constant nucleation rate was observed in steady state, suggesting that homogeneous nucleation occurred. Compared to thermal crystallization, a significant enhancement in the nucleation rate during high-energy ion irradiation (five to seven orders of magnitude) was observed with an apparent activation energy of 3.9±0.75 eV
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Sensitivity of warm-frontal processes to cloud-nucleating aerosol concentrations
Igel, Adele L.; Van Den Heever, Susan C.; Naud, Catherine M.; Saleeby, Stephen M.; Posselt, Derek J.
2013-01-01
An extratropical cyclone that crossed the United States on 9-11 April 2009 was successfully simulated at high resolution (3-km horizontal grid spacing) using the Colorado State University Regional Atmospheric Modeling System. The sensitivity of the associated warm front to increasing pollution levels was then explored by conducting the same experiment with three different background profiles of cloud-nucleating aerosol concentration. To the authors' knowledge, no study has examined the indirect effects of aerosols on warm fronts. The budgets of ice, cloud water, and rain in the simulation with the lowest aerosol concentrations were examined. The ice mass was found to be produced in equal amounts through vapor deposition and riming, and the melting of ice produced approximately 75% of the total rain. Conversion of cloud water to rain accounted for the other 25%. When cloud-nucleating aerosol concentrations were increased, significant changes were seen in the budget terms, but total precipitation remained relatively constant. Vapor deposition onto ice increased, but riming of cloud water decreased such that there was only a small change in the total ice production and hence there was no significant change in melting. These responses can be understood in terms of a buffering effect in which smaller cloud droplets in the mixed-phase region lead to both an enhanced vapor deposition and decreased riming efficiency with increasing aerosol concentrations. Overall, while large changes were seen in the microphysical structure of the frontal cloud, cloud-nucleating aerosols had little impact on the precipitation production of the warm front.
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Aqueous aerosol may build up large upper tropospheric ice supersaturation
Bogdan, Anatoli; Molina, Mario J.
2010-05-01
Keywords: ice supersaturation, upper tropospheric cirrus clouds, freezing of aqueous aerosol. Observations often reveal enhanced and persistent upper tropospheric (UT) ice supersaturation, Si up to 100%, independently of whether cirrus ice clouds are present or not (Krämer et al., 2009; Lawson et al., 2008). However, a water activity criterion (WAC) (Koop et al., 2000) does not allow the formation of Si > ~67% by the homogeneous freezing of aqueous droplets even at the lowest atmospheric temperature of ~185 K. For aqueous aerosol the WAC predicts the existence of a so called homogeneous ice nucleation threshold which, being expressed as Si, is between ~52 and 67% in the temperature range of ~220 - 185 K. The nature of the formation of large Si remains unclear. Since water vapor is the dominant greenhouse gas it is important to know the nature of the accumulation and persistence of water vapor in the UT. We studied the freezing behavior of micrometer-scaled 3-, 4-, and 5-component droplets, which contain different weight fractions of H2O, H2SO4, HNO3, (NH4)2SO4, (NH4)HSO4, NH4NO3, and (NH4)3H(SO4)2. The study was performed between 133 and 278 K at cooling rates of 3, 0.1, and 0.05 K/min using differential scanning calorimetry (DSC) (Bogdan and Molina, 2010). The cooling rates of 0.1 and 0.05 K/min (6 and 3 K/h) are similar to the smallest reported synoptic temperature change of ~2 K/h (Carslaw et al., 1998). Using the measured freezing temperature of ice, Ti, and the thermodynamic E-AIM model of the system of H+ - NH4+ - SO42-- NO3-- H2O (Clegg et al., 1998), we calculated the corresponding clear-sky Si which would be built up immediately prior to the formation of ice cirrus clouds by the homogeneous freezing of aqueous aerosol of similar composition. We found that our calculated values of Si are both larger and smaller than the homogeneous ice nucleation threshold. For example, for the droplets of compositions of 15/10 and 20/10 wt % (NH4)3H(SO4)2/H2SO4, which
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Homogeneous nucleation: a problem in nonequilibrium quantum statistical mechanics
International Nuclear Information System (INIS)
1978-08-01
The master equation for cluster growth and evaporation is derived for many-body quantum mechanics and from a modified version of quantum damping theory used in laser physics. For application to nucleation theory, the quantum damping theory is generalized to include system and reservoir states that are not separate entities. Formulas for rate constants are obtained. Solutions of the master equation yield equations of state and system-averaged quantities recognized as thermodynamic variables. Formulas for Helmholtz free energies of clusters in a Debye approximation are derived. Coexistence-line equations for pressure, volume, and number of clusters are obtained from equations-of-state analysis. Coexistence-line and surface-tension data are used to obtain values of parameters for the Debye approximation. These data are employed in calculating both the nucleation current in diffusion cloud chamber experiments and the onset of condensation in expansion nozzle experiments. Theoretical and experimental results are similar for both cloud chamber and nozzle experiments, which measure water. Comparison with other theories reveals that classical theory only accidently agrees with experiment and that the Helmholtz free-energy formula used in the Lothe--Pound theory is incomplete. 27 figures, 3 tables, 149 references
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Overview: Understanding nucleation phenomena from simulations of lattice gas models
International Nuclear Information System (INIS)
Binder, Kurt; Virnau, Peter
2016-01-01
Monte Carlo simulations of homogeneous and heterogeneous nucleation in Ising/lattice gas models are reviewed with an emphasis on the general insight gained on the mechanisms by which metastable states decay. Attention is paid to the proper distinction of particles that belong to a cluster (droplet), that may trigger a nucleation event, from particles in its environment, a problem crucial near the critical point. Well below the critical point, the lattice structure causes an anisotropy of the interface tension, and hence nonspherical droplet shapes result, making the treatment nontrivial even within the conventional classical theory of homogeneous nucleation. For temperatures below the roughening transition temperature facetted crystals rather than spherical droplets result. The possibility to find nucleation barriers from a thermodynamic analysis avoiding a cluster identification on the particle level is discussed, as well as the question of curvature corrections to the interfacial tension. For the interpretation of heterogeneous nucleation at planar walls, knowledge of contact angles and line tensions is desirable, and methods to extract these quantities from simulations will be mentioned. Finally, also the problem of nucleation near the stability limit of metastable states and the significance of the spinodal curve will be discussed, in the light of simulations of Ising models with medium range interactions.
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Sahyoun, Maher; Woetmann Nielsen, Niels; Havskov Sørensen, Jens; Finster, Kai; Bay Gosewinkel Karlson, Ulrich; Šantl-Temkiv, Tina; Smith Korsholm, Ulrik
2014-05-01
Bacteria, e.g. Pseudomonas syringae, have previously been found efficient in nucleating ice heterogeneously at temperatures close to -2°C in laboratory tests. Therefore, ice nucleation active (INA) bacteria may be involved in the formation of precipitation in mixed phase clouds, and could potentially influence weather and climate. Investigations into the impact of INA bacteria on climate have shown that emissions were too low to significantly impact the climate (Hoose et al., 2010). The goal of this study is to clarify the reason for finding the marginal impact on climate when INA bacteria were considered, by investigating the usability of ice nucleation rate parameterization based on classical nucleation theory (CNT). For this purpose, two parameterizations of heterogeneous ice nucleation were compared. Both parameterizations were implemented and tested in a 1-d version of the operational weather model (HIRLAM) (Lynch et al., 2000; Unden et al., 2002) in two different meteorological cases. The first parameterization is based on CNT and denoted CH08 (Chen et al., 2008). This parameterization is a function of temperature and the size of the IN. The second parameterization, denoted HAR13, was derived from nucleation measurements of SnomaxTM (Hartmann et al., 2013). It is a function of temperature and the number of protein complexes on the outer membranes of the cell. The fraction of cloud droplets containing each type of IN as percentage in the cloud droplets population were used and the sensitivity of cloud ice production in each parameterization was compared. In this study, HAR13 produces more cloud ice and precipitation than CH08 when the bacteria fraction increases. In CH08, the increase of the bacteria fraction leads to decreasing the cloud ice mixing ratio. The ice production using HAR13 was found to be more sensitive to the change of the bacterial fraction than CH08 which did not show a similar sensitivity. As a result, this may explain the marginal impact of
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Ice Nucleation Activity of Black Carbon and Organic Aerosol Emitted from Biomass Burning
Rauker, A. M.; Schill, G. P.; Hill, T. C. J.; Levin, E. J.; DeMott, P. J.; Kreidenweis, S. M.
2017-12-01
Ice-nucleating particles (INPs) must be present in clouds warmer than approximately -36 °C for initial ice crystal formation to occur. Although rare, they modify the lifetime, albedo and precipitation rates of clouds. Black carbon (BC) particles are present in the upper troposphere, and have been implicated as possible INPs, but recent research has not led to a consensus on their importance as INPs. Biomass burning is known to be a source of INPs as well as a major contributor to BC concentrations. Preliminary research from both prescribed burns (Manhattan, Kanas) and wildfires (Boise, Idaho and Weldon, Colorado), using the Colorado State University Continuous Flow Diffusion Chamber (CSU-CFDC) coupled to a Single Particle Soot Photometer (SP2), suggest that BC contributed ≤ 10% to INP concentrations in biomass burning conditions. To evaluate the identity of non-BC as an INP, filters were collected downwind from the same prescribed burns and wildfires, and particles re-suspended in water were subjected to the immersion freezing method to quantify INP concentrations. The contributions of biological and total organic species to INP concentrations were determined through heat and hydrogen peroxide pre-treatments. Total INPs ranged from 0.88 - 31 L-1 air at -20 °C with 82 - 99 % of the INPs at that temperature being organic (i.e., deactivated by H2O2 digestion). Results are consistent with CSU-CFDC-SP2 derived rBC INP contributions from the same fires. The results from the study also support previous findings that prescribed burns and wildfires produce plumes enriched in INPs.
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Kumar, Anand; Marcolli, Claudia; Luo, Beiping; Peter, Thomas
2018-05-01
Potassium-containing feldspars (K-feldspars) have been considered as 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 IN onset temperatures, Thet(aw), deviate strongly from ThetΔawhet(aw), the values calculated from the water-activity-based approach (where ThetΔawhet(aw) = Tmelt(aw + Δawhet) with a constant offset Δawhet with respect to the ice melting point curve). Surprisingly, for very dilute solutions of NH3 and NH4+ salts (molalities ≲1 mol kg-1 corresponding to aw ≳ 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 ThetΔawhet(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 ThetΔawhet(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) NH4+). However, the presence of a similar increase in IN efficiency in dilute ammonia solutions indicates that the cation exchange cannot explain the increase in IN temperatures. Instead, we hypothesize that NH3 molecules hydrogen bonded on the microcline surface form an ice-like overlayer, which provides hydrogen bonding favorable for ice to nucleate on, thus enhancing both the freezing temperatures and the
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Development of a Capacitive Ice Sensor to Measure Ice Growth in Real Time
Directory of Open Access Journals (Sweden)
Xiang Zhi
2015-03-01
Full Text Available This paper presents the development of the capacitive sensor to measure the growth of ice on a fuel pipe surface in real time. The ice sensor consists of pairs of electrodes to detect the change in capacitance and a thermocouple temperature sensor to examine the ice formation situation. In addition, an environmental chamber was specially designed to control the humidity and temperature to simulate the ice formation conditions. From the humidity, a water film is formed on the ice sensor, which results in an increase in capacitance. Ice nucleation occurs, followed by the rapid formation of frost ice that decreases the capacitance suddenly. The capacitance is saturated. The developed ice sensor explains the ice growth providing information about the icing temperature in real time.
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Development of a capacitive ice sensor to measure ice growth in real time.
Zhi, Xiang; Cho, Hyo Chang; Wang, Bo; Ahn, Cheol Hee; Moon, Hyeong Soon; Go, Jeung Sang
2015-03-19
This paper presents the development of the capacitive sensor to measure the growth of ice on a fuel pipe surface in real time. The ice sensor consists of pairs of electrodes to detect the change in capacitance and a thermocouple temperature sensor to examine the ice formation situation. In addition, an environmental chamber was specially designed to control the humidity and temperature to simulate the ice formation conditions. From the humidity, a water film is formed on the ice sensor, which results in an increase in capacitance. Ice nucleation occurs, followed by the rapid formation of frost ice that decreases the capacitance suddenly. The capacitance is saturated. The developed ice sensor explains the ice growth providing information about the icing temperature in real time.
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Effects of shear flow on phase nucleation and crystallization.
Mura, Federica; Zaccone, Alessio
2016-04-01
Classical nucleation theory offers a good framework for understanding the common features of new phase formation processes in metastable homogeneous media at rest. However, nucleation processes in liquids are ubiquitously affected by hydrodynamic flow, and there is no satisfactory understanding of whether shear promotes or slows down the nucleation process. We developed a classical nucleation theory for sheared systems starting from the molecular level of the Becker-Doering master kinetic equation and we analytically derived a closed-form expression for the nucleation rate. The theory accounts for the effect of flow-mediated transport of molecules to the nucleus of the new phase, as well as for the mechanical deformation imparted to the nucleus by the flow field. The competition between flow-induced molecular transport, which accelerates nucleation, and flow-induced nucleus straining, which lowers the nucleation rate by increasing the nucleation energy barrier, gives rise to a marked nonmonotonic dependence of the nucleation rate on the shear rate. The theory predicts an optimal shear rate at which the nucleation rate is one order of magnitude larger than in the absence of flow.
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Directory of Open Access Journals (Sweden)
A. Wiacek
2010-09-01
Full Text Available This modelling study explores the availability of mineral dust particles as ice nuclei for interactions with ice, mixed-phase and liquid water clouds, also tracking the particles' history of cloud-processing. We performed 61 320 one-week forward trajectory calculations originating near the surface of major dust emitting regions in Africa and Asia using high-resolution meteorological analysis fields for the year 2007. Dust-bearing trajectories were assumed to be those coinciding with known dust emission seasons, without explicitly modelling dust emission and deposition processes. We found that dust emissions from Asian deserts lead to a higher potential for interactions with high ice clouds, despite being the climatologically much smaller dust emission source. This is due to Asian regions experiencing significantly more ascent than African regions, with strongest ascent in the Asian Taklimakan desert at ~25%, ~40% and 10% of trajectories ascending to 300 hPa in spring, summer and fall, respectively. The specific humidity at each trajectory's starting point was transported in a Lagrangian manner and relative humidities with respect to water and ice were calculated in 6-h steps downstream, allowing us to estimate the formation of liquid, mixed-phase and ice clouds. Downstream of the investigated dust sources, practically none of the simulated air parcels reached conditions of homogeneous ice nucleation (T≲−40 °C along trajectories that have not experienced water saturation first. By far the largest fraction of cloud forming trajectories entered conditions of mixed-phase clouds, where mineral dust will potentially exert the biggest influence. The majority of trajectories also passed through atmospheric regions supersaturated with respect to ice but subsaturated with respect to water, where so-called "warm ice clouds" (T≳−40 °C theoretically may form prior to supercooled water or mixed-phase clouds. The importance of "warm ice
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Lipovsky, Bradley Paul; Dunham, Eric M.
2017-04-01
The Whillans Ice Plain (WIP), Antarctica, experiences twice daily tidally modulated stick-slip cycles. Slip events last about 30 min, have sliding velocities as high as ˜0.5 mm/s (15 km/yr), and have total slip ˜0.5 m. Slip events tend to occur during falling ocean tide: just after high tide and just before low tide. To reproduce these characteristics, we use rate-and-state friction, which is commonly used to simulate tectonic faulting, as an ice stream sliding law. This framework describes the evolving strength of the ice-bed interface throughout stick-slip cycles. We present simulations that resolve the cross-stream dimension using a depth-integrated treatment of an elastic ice layer loaded by tides and steady ice inflow. Steady sliding with rate-weakening friction is conditionally stable with steady sliding occurring for sufficiently narrow ice streams relative to a nucleation length. Stick-slip cycles occur when the ice stream is wider than the nucleation length or, equivalently, when effective pressures exceed a critical value. Ice streams barely wider than the nucleation length experience slow-slip events, and our simulations suggest that the WIP is in this slow-slip regime. Slip events on the WIP show a sense of propagation, and we reproduce this behavior by introducing a rate-strengthening region in the center of the otherwise rate-weakening ice stream. If pore pressures are raised above a critical value, our simulations predict that the WIP would exhibit quasi-steady tidally modulated sliding as observed on other ice streams. This study validates rate-and-state friction as a sliding law to describe ice stream sliding styles.
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International Nuclear Information System (INIS)
Smith, P.M.; Elmer, J.W.
1996-01-01
In recent rapid solidification experiments on Al-5%Be alloys, a Liquid Phase Nucleation (LPN) model was developed to explain the formation of periodic arrays of randomly-oriented Be-rich particles in an Al-rich matrix. In the LPN model, Be droplets were assumed to nucleate in the liquid ahead of the solid-liquid interface, but no justification for this was given. Here the authors present a model which considers the geometric constraints (imposed by proximity to the interface) on the number of solute atoms available to form a nucleus. Calculations based on this model predict that nucleation of second-phase particles can be most likely a short distance ahead of the interface in immiscible binary systems such as Al-Be. As part of the nucleation calculations, a semi-empirical method of calculating solid-liquid surface tensions in binary systems was developed, and is presented in the Appendix
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Understanding nanoparticle-mediated nucleation pathways of anisotropic nanoparticles
Laramy, Christine R.; Fong, Lam-Kiu; Jones, Matthew R.; O'Brien, Matthew N.; Schatz, George C.; Mirkin, Chad A.
2017-09-01
Several seed-mediated syntheses of low symmetry anisotropic nanoparticles yield broad product distributions with multiple defect structures. This observation challenges the role of the nanoparticle precursor as a seed for certain syntheses and suggests the possibility of alternate nucleation pathways. Herein, we report a method to probe the role of the nanoparticle precursor in anisotropic nanoparticle nucleation with compositional and structural 'labels' to track their fate. We use the synthesis of gold triangular nanoprisms (Au TPs) as a model system. We propose a mechanism in which, rather than acting as a template, the nanoparticle precursor catalyzes homogenous nucleation of Au TPs.
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Homogeneous bubble nucleation in binary systems of liquid solvent and dissolved gas
Czech Academy of Sciences Publication Activity Database
Němec, Tomáš
2016-01-01
Roč. 467, March (2016), s. 26-37 ISSN 0301-0104 R&D Projects: GA ČR GAP101/10/1819; GA ČR GA13-23550S Institutional support: RVO:61388998 Keywords : bubble nucleation * binary nucleation theory * dissolved gas Subject RIV: BJ - Thermodynamics Impact factor: 1.767, year: 2016 http://ac.els-cdn.com/S0301010416000124/1-s2.0-S0301010416000124-main.pdf?_tid=7797c8a0-fb13-11e5-ba55-00000aab0f6c&acdnat=1459849853_b9a5413fefc3e9199e844a9ccc97f514
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Effect of wetting on nucleation and growth of D2 in confinement
Zepeda-Ruiz, L. A.; Sadigh, B.; Shin, S. J.; Kozioziemski, B. J.; Chernov, A. A.
2018-04-01
We have performed a computational study to determine how the wetting of liquid deuterium to the walls of the material influences nucleation. We present the development of a pair-wise interatomic potential that includes zero-point motion of molecular deuterium. Deuterium is used in this study because of its importance to inertial confinement fusion and the potential to generate a superfluid state if the solidification can be suppressed. Our simulations show that wetting dominates undercooling compared to the pore geometries. We observe a transition from heterogeneous nucleation at the confining wall to homogeneous nucleation at the bulk of the liquid (and intermediate cases) as the interaction with the confining wall changes from perfect wetting to non-wetting. When nucleation is heterogeneous, the temperature needed for solidification changes by 4 K with decreasing deuterium-wall interaction, but it remains independent (and equal to the one from bulk samples) when homogeneous nucleation dominates. We find that growth and quality of the resulting microstructure also depends on the magnitude of liquid deuterium-wall interaction strength.
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The competition between mineral dust and soot ice nuclei in mixed-phase clouds (Invited)
Murray, B. J.; Atkinson, J.; Umo, N.; Browse, J.; Woodhouse, M. T.; Whale, T.; Baustian, K. J.; Carslaw, K. S.; Dobbie, S.; O'Sullivan, D.; Malkin, T. L.
2013-12-01
The amount of ice present in mixed-phase clouds, which contain both supercooled liquid water droplets and ice particles, affects cloud extent, lifetime, particle size and radiative properties. The freezing of cloud droplets can be catalysed by the presence of aerosol particles known as ice nuclei. In this talk our recent laboratory and global aerosol modelling work on mineral dust and soot ice nuclei will be presented. We have performed immersion mode experiments to quantify ice nucleation by the individual minerals which make up desert mineral dusts and have shown that the feldspar component, rather than the clay component, is most important for ice nucleation (Atkinson et al. 2013). Experiments with well-characterised soot generated with eugenol, an intermediate in biomass burning, and n-decane show soot has a significant ice nucleation activity in mixed-phase cloud conditions. Our results for soot are in good agreement with previous results for acetylene soot (DeMott, 1990), but extend the efficiency to much higher temperatures. We then use a global aerosol model (GLOMAP) to map the distribution of soot and feldspar particles on a global basis. We show that below about -15oC that dust and soot together can explain most observed ice nuclei in the Earth's atmosphere, while at warmer temperatures other ice nuclei types are needed. We show that in some regions soot is the most important ice nuclei (below -15oC), while in others feldspar dust dominates. Our results suggest that there is a strong anthropogenic contribution to the ice nuclei population, since a large proportion of soot aerosol in the atmosphere results from human activities. Atkinson, J. D., Murray, B. J., Woodhouse, M. T., Carslaw, K. S., Whale, T. F., Baustian, K. J., Dobbie, S., O'Sullivan, D., and Malkin, T. L.: The importance of feldspar for ice nucleation by mineral dust in mixed-phase clouds, Nature, 10.1038/nature12278, (2013). Demott, P. J. 1990. An Exploratory-Study of Ice Nucleation by Soot
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Concentration and variability of ice nuclei in the subtropical maritime boundary layer
Welti, André; Müller, Konrad; Fleming, Zoë L.; Stratmann, Frank
2018-04-01
Measurements of the concentration and variability of ice nucleating particles in the subtropical maritime boundary layer are reported. Filter samples collected in Cabo Verde over the period 2009-2013 are analyzed with a drop freezing experiment with sensitivity to detect the few rare ice nuclei active at low supercooling. The data set is augmented with continuous flow diffusion chamber measurements at temperatures below -24 °C from a 2-month field campaign in Cabo Verde in 2016. The data set is used to address the following questions: what are typical concentrations of ice nucleating particles active at a certain temperature? What affects their concentration and where are their sources? Concentration of ice nucleating particles is found to increase exponentially by 7 orders of magnitude from -5 to -38 °C. Sample-to-sample variation in the steepness of the increase indicates that particles of different origin, with different ice nucleation properties (size, composition), contribute to the ice nuclei concentration at different temperatures. The concentration of ice nuclei active at a specific temperature varies over a range of up to 4 orders of magnitude. The frequency with which a certain ice nuclei concentration is measured within this range is found to follow a lognormal distribution, which can be explained by random dilution during transport. To investigate the geographic origin of ice nuclei, source attribution of air masses from dispersion modeling is used to classify the data into seven typical conditions. While no source could be attributed to the ice nuclei active at temperatures higher than -12 °C, concentrations at lower temperatures tend to be elevated in air masses originating from the Sahara.
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Energy Technology Data Exchange (ETDEWEB)
Feiden, P
2007-09-15
This work deals with the study of nano-particles formation in gas phase and their dissociation pathways after an optical excitation. The clusters formation decomposes in two steps: a seed is formed (nucleation phase) and sticks atoms during its propagation in a sodium atomic vapor (growth phase). Those two steps have been observed separately for homogeneous Na{sub n} and heterogeneous Na{sub n}X particles (X = (NaOH){sub 2} or (Na{sub 2}O){sub 2}). The growth mechanism is well interpreted by a Monte Carlo simulation taking into account an accretion mechanism with hard-sphere cross section. The homogeneous nucleation mechanism has been highlighted by a direct comparison with the Classical Nucleation Theory predictions. The clusters fragmentation of ionic Na{sup +}(NaOH){sub p} et Na{sup +}(NaF){sub p} particles is studied in the second part. The way clusters fragment with size when they are excited optically is compared with theoretical previsions: this highlights the existence of an energetic barrier for special size of clusters. Finally, the fragmentation of doubly charged Na{sup +} Na{sup +} (NaOH){sub p} clusters shows a competition between the fission into two single charged fragments and the unimolecular evaporation of a neutral fragment. (author)
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Modelling the role of compositional fluctuations in nucleation kinetics
International Nuclear Information System (INIS)
Ženíšek, J.; Kozeschnik, E.; Svoboda, J.; Fischer, F.D.
2015-01-01
The classical nucleation theory of precipitate nucleation in interstitial/substitutional alloys is applied to account for the influence of spatial A–B composition fluctuations in an A–B–C matrix on the kinetics of nucleation of (A,B) 3 C precipitates. A and B are substitutional elements in the matrix and C is an interstitial component, assumed to preferentially bind to B atoms. All lattice sites are considered as potential nucleation sites. The fluctuations of chemical composition result in a local variation of the nucleation probability. The nucleation sites are eliminated from the system if they are located in a C-depleted diffusion zone belonging to an already nucleated and growing precipitate. The chemistry is that of an Fe–Cr–C system, and the specific interface energy is treated as a free parameter. Random, regular and homogeneous A–B distributions in the matrix are simulated and compared for various values of the interface energy. An increasing enhancement of the role of compositional fluctuations on nucleation kinetics with increasing interface energy and decreasing chemical driving force is observed
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A one-dimensional ice structure built from pentagons
Carrasco, Javier; Michaelides, Angelos
2010-03-01
Heterogeneous nucleation of water plays a key role in fields as diverse as atmospheric chemistry, astrophysics, and biology. Ice nucleation on metal surfaces offers an opportunity to watch this process unfold, providing a molecular-scale description at a well-defined, planar interface. We discuss a density-functional theory study on a metal surface specifically designed to understand such phenomena. Together with our colleges at the University of Liverpool, we found that the nanometer wide water-ice chains experimentally observed to nucleate and grow on Cu(110) are built from a face sharing arrangement of water pentagons [1]. The novel one-dimensional pentagon structure maximizes the water-metal bonding whilst simultaneously maintaining a strong hydrogen bonding network. These results reveal an unanticipated structural adaptability of water-ice films, demonstrating that the presence of the substrate can be sufficient to favor non-conventional structural units. [4pt] [1] J. Carrasco et al., Nature Mater. 8, 427 (2009).
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Harrington, J. Y.
2017-12-01
Parameterizing the growth of ice particles in numerical models is at an interesting cross-roads. Most parameterizations developed in the past, including some that I have developed, parse model ice into numerous categories based primarily on the growth mode of the particle. Models routinely possess smaller ice, snow crystals, aggregates, graupel, and hail. The snow and ice categories in some models are further split into subcategories to account for the various shapes of ice. There has been a relatively recent shift towards a new class of microphysical models that predict the properties of ice particles instead of using multiple categories and subcategories. Particle property models predict the physical characteristics of ice, such as aspect ratio, maximum dimension, effective density, rime density, effective area, and so forth. These models are attractive in the sense that particle characteristics evolve naturally in time and space without the need for numerous (and somewhat artificial) transitions among pre-defined classes. However, particle property models often require fundamental parameters that are typically derived from laboratory measurements. For instance, the evolution of particle shape during vapor depositional growth requires knowledge of the growth efficiencies for the various axis of the crystals, which in turn depends on surface parameters that can only be determined in the laboratory. The evolution of particle shapes and density during riming, aggregation, and melting require data on the redistribution of mass across a crystals axis as that crystal collects water drops, ice crystals, or melts. Predicting the evolution of particle properties based on laboratory-determined parameters has a substantial influence on the evolution of some cloud systems. Radiatively-driven cirrus clouds show a broader range of competition between heterogeneous nucleation and homogeneous freezing when ice crystal properties are predicted. Even strongly convective squall
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Hygroscopicity of nanoparticles produced from homogeneous nucleation in the CLOUD experiments
Directory of Open Access Journals (Sweden)
J. Kim
2016-01-01
Full Text Available Sulfuric acid, amines and oxidized organics have been found to be important compounds in the nucleation and initial growth of atmospheric particles. Because of the challenges involved in determining the chemical composition of objects with very small mass, however, the properties of the freshly nucleated particles and the detailed pathways of their formation processes are still not clear. In this study, we focus on a challenging size range, i.e., particles that have grown to diameters of 10 and 15 nm following nucleation, and measure their water uptake. Water uptake is useful information for indirectly obtaining chemical composition of aerosol particles. We use a nanometer-hygroscopicity tandem differential mobility analyzer (nano-HTDMA at subsaturated conditions (ca. 90 % relative humidity at 293 K to measure the hygroscopicity of particles during the seventh Cosmics Leaving OUtdoor Droplets (CLOUD7 campaign performed at CERN in 2012. In CLOUD7, the hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid–dimethylamine, and sulfuric acid–organics derived from α-pinene oxidation. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles. No clear effect of the sulfuric acid concentration on the hygroscopicity of 10 nm particles produced from sulfuric acid and dimethylamine was observed, whereas the hygroscopicity of 15 nm particles sharply decreased with decreasing sulfuric acid concentrations. In particular, when the concentration of sulfuric acid was 5.1 × 106 molecules cm−3 in the gas phase, and the dimethylamine mixing ratio was 11.8 ppt, the measured κ of 15 nm particles was 0.31 ± 0.01: close to the value reported for dimethylaminium sulfate (DMAS (κDMAS ∼ 0.28. Furthermore, the difference in κ between sulfuric acid and sulfuric acid–imethylamine experiments increased with increasing particle
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Simple improvements to classical bubble nucleation models.
Tanaka, Kyoko K; Tanaka, Hidekazu; Angélil, Raymond; Diemand, Jürg
2015-08-01
We revisit classical nucleation theory (CNT) for the homogeneous bubble nucleation rate and improve the classical formula using a correct prefactor in the nucleation rate. Most of the previous theoretical studies have used the constant prefactor determined by the bubble growth due to the evaporation process from the bubble surface. However, the growth of bubbles is also regulated by the thermal conduction, the viscosity, and the inertia of liquid motion. These effects can decrease the prefactor significantly, especially when the liquid pressure is much smaller than the equilibrium one. The deviation in the nucleation rate between the improved formula and the CNT can be as large as several orders of magnitude. Our improved, accurate prefactor and recent advances in molecular dynamics simulations and laboratory experiments for argon bubble nucleation enable us to precisely constrain the free energy barrier for bubble nucleation. Assuming the correction to the CNT free energy is of the functional form suggested by Tolman, the precise evaluations of the free energy barriers suggest the Tolman length is ≃0.3σ independently of the temperature for argon bubble nucleation, where σ is the unit length of the Lennard-Jones potential. With this Tolman correction and our prefactor one gets accurate bubble nucleation rate predictions in the parameter range probed by current experiments and molecular dynamics simulations.
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Nichman, Leonid; Järvinen, Emma; Dorsey, James; Connolly, Paul; Duplissy, Jonathan; Fuchs, Claudia; Ignatius, Karoliina; Sengupta, Kamalika; Stratmann, Frank; Möhler, Ottmar; Schnaiter, Martin; Gallagher, Martin
2017-09-01
Optical probes are frequently used for the detection of microphysical cloud particle properties such as liquid and ice phase, size and morphology. These properties can eventually influence the angular light scattering properties of cirrus clouds as well as the growth and accretion mechanisms of single cloud particles. In this study we compare four commonly used optical probes to examine their response to small cloud particles of different phase and asphericity. Cloud simulation experiments were conducted at the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at European Organisation for Nuclear Research (CERN). The chamber was operated in a series of multi-step adiabatic expansions to produce growth and sublimation of ice particles at super- and subsaturated ice conditions and for initial temperatures of -30, -40 and -50 °C. The experiments were performed for ice cloud formation via homogeneous ice nucleation. We report the optical observations of small ice particles in deep convection and in situ cirrus simulations. Ice crystal asphericity deduced from measurements of spatially resolved single particle light scattering patterns by the Particle Phase Discriminator mark 2 (PPD-2K, Karlsruhe edition) were compared with Cloud and Aerosol Spectrometer with Polarisation (CASPOL) measurements and image roundness captured by the 3View Cloud Particle Imager (3V-CPI). Averaged path light scattering properties of the simulated ice clouds were measured using the Scattering Intensity Measurements for the Optical detectioN of icE (SIMONE) and single particle scattering properties were measured by the CASPOL. We show the ambiguity of several optical measurements in ice fraction determination of homogeneously frozen ice in the case where sublimating quasi-spherical ice particles are present. Moreover, most of the instruments have difficulties of producing reliable ice fraction if small aspherical ice particles are present, and all of the instruments cannot separate perfectly
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Jensen, Eric
2018-01-01
One of the proposed concepts for mitigating the warming effect of increasing greenhouse gases is seeding cirrus cloud with ice nuclei (IN) in order to reduce the lifetime and coverage of cold cirrus that have a net warming impact on the earth's surface. Global model simulations of the net impact of changing upper tropospheric IN have given widely disparate results, partly as a result of poor understanding of ice nucleation processes in the current atmosphere, and partly as a result of poor representation of these processes in global models. Here, we present detailed process-model simulations of tropical tropopause layer (TTL) transport and cirrus formation with ice nuclei properties based on recent laboratory nucleation experiments and field measurements of aerosol composition. The model is used to assess the sensitivity of TTL cirrus occurrence frequency and microphysical properties to the abundance and efficacy of ice nuclei. The simulated cloud properties compared with recent high-altitude aircraft measurements of TTL cirrus and ice supersaturation. We find that abundant effective IN (either from glassy organic aerosols or crystalline ammonium sulfate with concentrations greater than about 100/L) prevent the occurrences of large ice concentration and large ice supersaturations, both of which are clearly indicated by the in situ observations. We find that concentrations of effective ice nuclei larger than about 50/L can drive significant changes in cirrus microphysical properties and occurrence frequency. However, the cloud occurrence frequency can either increase or decrease, depending on the efficacy and abundance of IN added to the TTL. We suggest that our lack of information about ice nuclei properties in the current atmosphere, as well as uncertainties in ice nucleation processes and their representations in global models, preclude meaningful estimates of climate impacts associated with addition of ice nuclei in the upper troposphere. We will briefly discuss
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Rinaldi, M.; Santachiara, G.; Nicosia, A.; Piazza, M.; Decesari, S.; Gilardoni, S.; Paglione, M.; Cristofanelli, P.; Marinoni, A.; Bonasoni, P.; Belosi, F.
2017-12-01
Measurement campaigns at the high mountain Observatory Mt. Cimone (CMN; 2165 m a.s.l.) were performed during May 2014 and October 2015. The concentration of Ice Nucleating Particles (INPs) were measured offline with a dynamic filter processing chamber (DFPC), in the deposition and condensation mode, after collecting PM1 and PM10 aerosol samples. Presented INP data are the first ever published for a high mountain site in the Mediterranean basin. During the May campaign, parallel INP measurements were also carried out at San Pietro Capofiume (SPC), a low altitude rural background area within the Po Valley basin, by the same offline technique. The average INPPM10 concentration at CMN was 86 m-3 (saturation ratio Sw = 1.01; T = -18 °C) during the May 2014 campaign, while it was 171 m-3 at SPC, in the same period. A lower average INPPM10 concentration was observed at CMN during October 2015 (43 m-3). A significantly higher activated fraction (AF) characterized the October 2015 campaign, suggesting that the seasonal changes in the aerosol sources have an impact on the INP efficiency of the aerosol at CMN. Super-micrometer INP contributed for ∼30% of total INP in the May 2014 campaign, at both sites, and for ∼70% in the October 2015 campaign, showing the importance of coarse particles in the INP population. The analysis of meteorological parameters, gaseous tracers concentrations and backwards trajectories suggests that the INP population at CMN is contributed by transport processes occurring at diverse spatial scales, from the local to the synoptic scale. During the Saharan Dust transport Event observed in May 2014, a reduction of the AF was observed, suggesting, for this case, a limited ice nucleating activity for Saharan dust particles. This may be due to physico-chemical aging of the Saharan dust particles during transport or to the relatively high activation temperature at which the experiments were performed in this study.
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International Nuclear Information System (INIS)
Costa, Tassio S; Gonçalves, Fábio L T; Yamasoe, Marcia A; Martins, Jorge A; Morris, Cindy E
2014-01-01
This study examines the effect of the bacterial species Pseudomonas syringae acting as ice nuclei (IN) on cloud properties to understand its impact on local radiative budget and heating rates. These bacteria may become active IN at temperatures as warm as −2 °C. Numerical simulations were developed using the Brazilian Regional Atmospheric Model System (BRAMS). To investigate the isolated effect of bacterial IN, four scenarios were created considering only homogeneous and bacterial ice nucleation, with 1, 10 and 100 IN per cubic meter of cloud volume and one with no bacteria. Moreover, two other scenarios were generated: the BRAMS default parameterization and its combination with bacterial IN. The model reproduced a strong convective cell over São Paulo on 3 March 2003. Results showed that bacterial IN may change cloud evolution as well as its microphysical properties, which in turn influence cloud radiative properties. For example, the reflected shortwave irradiance over an averaged domain in a scenario considering bacterial IN added to the BRAMS default parameterization was 14% lower than if bacteria were not considered. Heating rates can also be impacted, especially due to differences in cloud lifetime. Results suggest that the omission of bacterial IN in numerical models, including global cloud models, could neglect relevant ice nucleation processes that potentially influence cloud radiative properties. (letter)
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Nucleation reactions during deformation and crystallization of metallic glass
International Nuclear Information System (INIS)
Perepezko, J.H.; Imhoff, S.D.; Chen, M.W.; Gonzalez, S.; Inoue, A.
2012-01-01
Highlights: ► New approach to the examination and analysis of shear band nucleation. ► Discovery of multiple shear band nucleation sites. ► Identification of a method of using transient kinetic behavior to provide a more realistic evaluation of the diffusivity that is relevant to nucleation. - Abstract: Nucleation reactions play a central role in the synthesis of both bulk metallic glasses and nanostructured materials. For nanostructured materials it is necessary to promote a high nucleation density without significant growth or coarsening. Beyond crystallization reactions nucleation of shear bands is critical for promoting a homogeneous flow and useful ductility for structural applications of bulk metallic glass. The study and analysis of nucleation reactions for these different situations requires a consideration of the stochastic nature of nucleation, the influence of heterogeneous sites, and the controlling transport properties. For shear band nucleation, the stochastic nature can be effectively probed by instrumented nanoindentation tests. The analysis of a statistically significant number of measurements of the first pop-in shear band nucleation events reveals at least two main nucleation sites. In nanostructured composites, the initial nucleation stage is influenced by transient effects as reflected in the delay time prior to steady state nucleation and by heterogeneous nucleation sites that are related to medium range order regions in Al-base amorphous alloys. Moreover, the early growth characteristics are linked to the maximum achievable particle density. The new developments and insight on the fundamental understanding of nanostructure reaction mechanisms offer valuable guidance for control of nanoscale microstructures and for promoting ductile deformation behavior.
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Determination of critical nucleation number for a single nucleation amyloid-β aggregation model.
Ghosh, Preetam; Vaidya, Ashwin; Kumar, Amit; Rangachari, Vijayaraghavan
2016-03-01
Aggregates of amyloid-β (Aβ) peptide are known to be the key pathological agents in Alzheimer disease (AD). Aβ aggregates to form large, insoluble fibrils that deposit as senile plaques in AD brains. The process of aggregation is nucleation-dependent in which the formation of a nucleus is the rate-limiting step, and controls the physiochemical fate of the aggregates formed. Therefore, understanding the properties of nucleus and pre-nucleation events will be significant in reducing the existing knowledge-gap in AD pathogenesis. In this report, we have determined the plausible range of critical nucleation number (n(*)), the number of monomers associated within the nucleus for a homogenous aggregation model with single unique nucleation event, by two independent methods: A reduced-order stability analysis and ordinary differential equation based numerical analysis, supported by experimental biophysics. The results establish that the most likely range of n(*) is between 7 and 14 and within, this range, n(*) = 12 closely supports the experimental data. These numbers are in agreement with those previously reported, and importantly, the report establishes a new modeling framework using two independent approaches towards a convergent solution in modeling complex aggregation reactions. Our model also suggests that the formation of large protofibrils is dependent on the nature of n(*), further supporting the idea that pre-nucleation events are significant in controlling the fate of larger aggregates formed. This report has re-opened an old problem with a new perspective and holds promise towards revealing the molecular events in amyloid pathologies in the future. Copyright © 2015 Elsevier Inc. All rights reserved.
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Nucleation of voids. Final report, October 1, 1971--January 31, 1977
International Nuclear Information System (INIS)
Katz, J.L.
1977-10-01
The successful prediction of the conditions under which nucleation occurs in metals, as a result of the high concentrations of vacancies and interstitial atoms (and gas atoms) present in reactor environments, has been accomplished by (1) generalizing homogeneous nucleation theory to account for nucleation of matter (i.e., vacancies) in the presence of its antimatter (i.e., interstitials), (2) further generalizing the theory to account for the effects of both trapped and soluble gas, and (3) modifying the theory to describe interstitial loop formation and including the effects of external stress
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Condensed-phase biogenic-anthropogenic interactions with implications for cold cloud formation.
Charnawskas, Joseph C; Alpert, Peter A; Lambe, Andrew T; Berkemeier, Thomas; O'Brien, Rachel E; Massoli, Paola; Onasch, Timothy B; Shiraiwa, Manabu; Moffet, Ryan C; Gilles, Mary K; Davidovits, Paul; Worsnop, Douglas R; Knopf, Daniel A
2017-08-24
Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil fuel combustion can acquire a coating of SOA. We investigate SOA-soot biogenic-anthropogenic interactions and their impact on ice nucleation in relation to the particles' organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without the presence of sulfate or soot particles. Corresponding particle glass transition (T g ) and full deliquescence relative humidity (FDRH) were estimated using a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfate mixtures exhibit a core-shell configuration (i.e. a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation, in agreement with respective T g and FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid, inducing ice nucleation. Naphthalene SOA coated soot particles acted as ice nuclei above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate renders this even less likely. However, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during pre-industrial times or in pristine areas.
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Duman, John G
2015-06-01
Ice-binding proteins (IBPs) assist in subzero tolerance of multiple cold-tolerant organisms: animals, plants, fungi, bacteria etc. IBPs include: (1) antifreeze proteins (AFPs) with high thermal hysteresis antifreeze activity; (2) low thermal hysteresis IBPs; and (3) ice-nucleating proteins (INPs). Several structurally different IBPs have evolved, even within related taxa. Proteins that produce thermal hysteresis inhibit freezing by a non-colligative mechanism, whereby they adsorb onto ice crystals or ice-nucleating surfaces and prevent further growth. This lowers the so-called hysteretic freezing point below the normal equilibrium freezing/melting point, producing a difference between the two, termed thermal hysteresis. True AFPs with high thermal hysteresis are found in freeze-avoiding animals (those that must prevent freezing, as they die if frozen) especially marine fish, insects and other terrestrial arthropods where they function to prevent freezing at temperatures below those commonly experienced by the organism. Low thermal hysteresis IBPs are found in freeze-tolerant organisms (those able to survive extracellular freezing), and function to inhibit recrystallization - a potentially damaging process whereby larger ice crystals grow at the expense of smaller ones - and in some cases, prevent lethal propagation of extracellular ice into the cytoplasm. Ice-nucleator proteins inhibit supercooling and induce freezing in the extracellular fluid at high subzero temperatures in many freeze-tolerant species, thereby allowing them to control the location and temperature of ice nucleation, and the rate of ice growth. Numerous nuances to these functions have evolved. Antifreeze glycolipids with significant thermal hysteresis activity were recently identified in insects, frogs and plants. © 2015. Published by The Company of Biologists Ltd.
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Nanoscale-Agglomerate-Mediated Heterogeneous Nucleation.
Cha, Hyeongyun; Wu, Alex; Kim, Moon-Kyung; Saigusa, Kosuke; Liu, Aihua; Miljkovic, Nenad
2017-12-13
Water vapor condensation on hydrophobic surfaces has received much attention due to its ability to rapidly shed water droplets and enhance heat transfer, anti-icing, water harvesting, energy harvesting, and self-cleaning performance. However, the mechanism of heterogeneous nucleation on hydrophobic surfaces remains poorly understood and is attributed to defects in the hydrophobic coating exposing the high surface energy substrate. Here, we observe the formation of high surface energy nanoscale agglomerates on hydrophobic coatings after condensation/evaporation cycles in ambient conditions. To investigate the deposition dynamics, we studied the nanoscale agglomerates as a function of condensation/evaporation cycles via optical and field emission scanning electron microscopy (FESEM), microgoniometric contact angle measurements, nucleation statistics, and energy dispersive X-ray spectroscopy (EDS). The FESEM and EDS results indicated that the nanoscale agglomerates stem from absorption of sulfuric acid based aerosol particles inside the droplet and adsorption of volatile organic compounds such as methanethiol (CH 3 SH), dimethyl disulfide (CH 3 SSCH), and dimethyl trisulfide (CH 3 SSSCH 3 ) on the liquid-vapor interface during water vapor condensation, which act as preferential sites for heterogeneous nucleation after evaporation. The insights gained from this study elucidate fundamental aspects governing the behavior of both short- and long-term heterogeneous nucleation on hydrophobic surfaces, suggest previously unexplored microfabrication and air purification techniques, and present insights into the challenges facing the development of durable dropwise condensing surfaces.
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Atmospheric ice nuclei: No detectable effects from a coal-fired powerplant plume
International Nuclear Information System (INIS)
Schnell, R.C.; Van Valin, C.C.; Pueschel, R.F.
1976-01-01
Atmospheric ice nuclei were measured upwind and within the effluent plume of a coalfired powerplant during February 1976. Aerosol particles were captured on two types of membrane filters (Nuclepore and Millipore) and processed in two different thermal diffusion chambers, one calibrated to produce a 100% saturation relative to water and the other to produce a slight supersaturation relative to water. Consequently, the ice nuclei measured were active in the modes that are dominant in diffusion chambers, viz., deposition nucleation and condensation-followed-by-freezing nucleation. Results indicate that plume particles do not act as ice nuclei between the temperatures of -10 and -20degreeC, nor do combustion gases in the plume deactivate natural ice nuclei
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Classical nucleation theory in the phase-field crystal model.
Jreidini, Paul; Kocher, Gabriel; Provatas, Nikolas
2018-04-01
A full understanding of polycrystalline materials requires studying the process of nucleation, a thermally activated phase transition that typically occurs at atomistic scales. The numerical modeling of this process is problematic for traditional numerical techniques: commonly used phase-field methods' resolution does not extend to the atomic scales at which nucleation takes places, while atomistic methods such as molecular dynamics are incapable of scaling to the mesoscale regime where late-stage growth and structure formation takes place following earlier nucleation. Consequently, it is of interest to examine nucleation in the more recently proposed phase-field crystal (PFC) model, which attempts to bridge the atomic and mesoscale regimes in microstructure simulations. In this work, we numerically calculate homogeneous liquid-to-solid nucleation rates and incubation times in the simplest version of the PFC model, for various parameter choices. We show that the model naturally exhibits qualitative agreement with the predictions of classical nucleation theory (CNT) despite a lack of some explicit atomistic features presumed in CNT. We also examine the early appearance of lattice structure in nucleating grains, finding disagreement with some basic assumptions of CNT. We then argue that a quantitatively correct nucleation theory for the PFC model would require extending CNT to a multivariable theory.
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Classical nucleation theory in the phase-field crystal model
Jreidini, Paul; Kocher, Gabriel; Provatas, Nikolas
2018-04-01
A full understanding of polycrystalline materials requires studying the process of nucleation, a thermally activated phase transition that typically occurs at atomistic scales. The numerical modeling of this process is problematic for traditional numerical techniques: commonly used phase-field methods' resolution does not extend to the atomic scales at which nucleation takes places, while atomistic methods such as molecular dynamics are incapable of scaling to the mesoscale regime where late-stage growth and structure formation takes place following earlier nucleation. Consequently, it is of interest to examine nucleation in the more recently proposed phase-field crystal (PFC) model, which attempts to bridge the atomic and mesoscale regimes in microstructure simulations. In this work, we numerically calculate homogeneous liquid-to-solid nucleation rates and incubation times in the simplest version of the PFC model, for various parameter choices. We show that the model naturally exhibits qualitative agreement with the predictions of classical nucleation theory (CNT) despite a lack of some explicit atomistic features presumed in CNT. We also examine the early appearance of lattice structure in nucleating grains, finding disagreement with some basic assumptions of CNT. We then argue that a quantitatively correct nucleation theory for the PFC model would require extending CNT to a multivariable theory.
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Directory of Open Access Journals (Sweden)
A. Kumar
2018-05-01
Full Text Available Potassium-containing feldspars (K-feldspars have been considered as 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, (NH42SO4, 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 IN onset temperatures, Thet(aw, deviate strongly from ThetΔawhet(aw, the values calculated from the water-activity-based approach (where ThetΔawhet(aw = Tmelt(aw + Δawhet with a constant offset Δawhet with respect to the ice melting point curve. Surprisingly, for very dilute solutions of NH3 and NH4+ salts (molalities ≲1 mol kg−1 corresponding to aw ≳ 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 ThetΔawhet(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 ThetΔawhet(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 < ThetΔawhet(aw even at very small solute concentrations. In all these cases, the heterogeneous freezing peak displays a decrease as solute concentration increases. This deviation from Δawhet = const. indicates specific chemical interactions between particular solutes and the microcline surface not captured by the water-activity-based approach. One
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Nucleation and dissociation of nano-particles in gas phase
International Nuclear Information System (INIS)
Feiden, P.
2007-09-01
This work deals with the study of nano-particles formation in gas phase and their dissociation pathways after an optical excitation. The clusters formation decomposes in two steps: a seed is formed (nucleation phase) and sticks atoms during its propagation in a sodium atomic vapor (growth phase). Those two steps have been observed separately for homogeneous Na n and heterogeneous Na n X particles (X = (NaOH) 2 or (Na 2 O) 2 ). The growth mechanism is well interpreted by a Monte Carlo simulation taking into account an accretion mechanism with hard-sphere cross section. The homogeneous nucleation mechanism has been highlighted by a direct comparison with the Classical Nucleation Theory predictions. The clusters fragmentation of ionic Na + (NaOH) p et Na + (NaF) p particles is studied in the second part. The way clusters fragment with size when they are excited optically is compared with theoretical previsions: this highlights the existence of an energetic barrier for special size of clusters. Finally, the fragmentation of doubly charged Na + Na + (NaOH) p clusters shows a competition between the fission into two single charged fragments and the unimolecular evaporation of a neutral fragment. (author)
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Schwarzenböck, A.; Mertes, S.; Heintzenberg, J.; Wobrock, W.; Laj, P.
The paper focuses on the redistribution of aerosol particles (APs) during the artificial nucleation and subsequent growth of ice crystals in a supercooled cloud. A significant number of the supercooled cloud droplets during icing periods (seeding agents: C 3H 8, CO 2) did not freeze as was presumed prior to the experiment but instead evaporated. The net mass flux of water vapour from the evaporating droplets to the nucleating ice crystals (Bergeron-Findeisen mechanism) led to the release of residual particles that simultaneously appeared in the interstitial phase. The strong decrease of the droplet residuals confirms the nucleation of ice particles on seeding germs without natural aerosol particles serving as ice nuclei. As the number of residual particles during the seedings did not drop to zero, other processes such as heterogeneous ice nucleation, spontaneous freezing, entrainment of supercooled droplets and diffusion to the created particle-free ice germs must have contributed to the experimental findings. During the icing periods, residual mass concentrations in the condensed phase dropped by a factor of 1.1-6.7, as compared to the unperturbed supercooled cloud. As the Bergeron-Findeisen process also occurs without artificial seeding in the atmosphere, this study demonstrated that the hydrometeors in mixed-phase clouds might be much cleaner than anticipated for the simple freezing process of supercooled droplets in tropospheric mid latitude clouds.
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Surface Assisted Formation of methane Hydrates on Ice and Na Montmorillonite Clay
Energy Technology Data Exchange (ETDEWEB)
Gordon, Margaret Ellen [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Teich-McGoldrick, Stephanie [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Cygan, Randall Timothy [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Meserole, Stephen P. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Rodriguez, Mark A. [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
2015-07-01
Methane hydrates are extremely important naturally-occurring crystalline materials that impact climate change, energy resources, geological hazards, and other major environmental issues. Whereas significant experimental effort has been completed to understanding the bulk thermodynamics of methane hydrate assemblies, little is understood on heterogeneous nucleation and growth of methane hydrates in clay-rich environments. Controlled synthesis experiments were completed at 265-285 K and 6.89 MPa to examine the impact of montmorillonite surfaces in clay-ice mixtures to nucleate and form methane hydrate. The results suggest that the hydrophilic and methane adsorbing properties of Namontmorillonite reduce the nucleation period of methane hydrate formation in pure ice systems.
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Clustering of amines and hydrazines in atmospheric nucleation
Li, Siyang; Qu, Kun; Zhao, Hailiang; Ding, Lei; Du, Lin
2016-06-01
It has been proved that the presence of amines in the atmosphere can enhance aerosol formation. Hydrazine (HD) and its substituted derivatives, monomethylhydrazine (MMH) and unsymmetrical dimethylhydrazine (UDMH), which are organic derivatives of amine and ammonia, are common trace atmospheric species that may contribute to the growth of nucleation clusters. The structures of the hydrazine and amine clusters containing one or two common nucleation molecules (ammonia, water, methanol and sulfuric acid) have been optimized using density functional theory (DFT) methods. The clusters growth mechanism has been explored from the thermochemistry by calculating the Gibbs free energies of adding an ammonia, water, methanol or sulfuric acid molecule step by step at room temperature, respectively. The results show that hydrazine and its derivatives could enhance heteromolecular homogeneous nucleation in the earth's atmosphere.
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Competition for water vapour results in suppression of ice formation in mixed-phase clouds
Directory of Open Access Journals (Sweden)
E. L. Simpson
2018-05-01
Full Text Available The formation of ice in clouds can initiate precipitation and influence a cloud's reflectivity and lifetime, affecting climate to a highly uncertain degree. Nucleation of ice at elevated temperatures requires an ice nucleating particle (INP, which results in so-called heterogeneous freezing. Previously reported measurements for the ability of a particle to nucleate ice have been made in the absence of other aerosol which will act as cloud condensation nuclei (CCN and are ubiquitous in the atmosphere. Here we show that CCN can outcompete INPs for available water vapour thus suppressing ice formation, which has the potential to significantly affect the Earth's radiation budget. The magnitude of this suppression is shown to be dependent on the mass of condensed water required for freezing. Here we show that ice formation in a state-of-the-art cloud parcel model is strongly dependent on the criteria for heterogeneous freezing selected from those previously hypothesised. We have developed an alternative criteria which agrees well with observations from cloud chamber experiments. This study demonstrates the dominant role that competition for water vapour can play in ice formation, highlighting both a need for clarity in the requirements for heterogeneous freezing and for measurements under atmospherically appropriate conditions.
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Competition for water vapour results in suppression of ice formation in mixed-phase clouds
Simpson, Emma L.; Connolly, Paul J.; McFiggans, Gordon
2018-05-01
The formation of ice in clouds can initiate precipitation and influence a cloud's reflectivity and lifetime, affecting climate to a highly uncertain degree. Nucleation of ice at elevated temperatures requires an ice nucleating particle (INP), which results in so-called heterogeneous freezing. Previously reported measurements for the ability of a particle to nucleate ice have been made in the absence of other aerosol which will act as cloud condensation nuclei (CCN) and are ubiquitous in the atmosphere. Here we show that CCN can outcompete INPs for available water vapour thus suppressing ice formation, which has the potential to significantly affect the Earth's radiation budget. The magnitude of this suppression is shown to be dependent on the mass of condensed water required for freezing. Here we show that ice formation in a state-of-the-art cloud parcel model is strongly dependent on the criteria for heterogeneous freezing selected from those previously hypothesised. We have developed an alternative criteria which agrees well with observations from cloud chamber experiments. This study demonstrates the dominant role that competition for water vapour can play in ice formation, highlighting both a need for clarity in the requirements for heterogeneous freezing and for measurements under atmospherically appropriate conditions.
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Anti-icing/frosting and self-cleaning performance of superhydrophobic aluminum alloys
Feng, Libang; Yan, Zhongna; Shi, Xueting; Sultonzoda, Firdavs
2018-02-01
Ice formation and frost deposition on cryogenic equipment and systems can result in serious problems and huge economic loss. Hence, it is quite necessary to develop new materials to prevent icing and frosting on cold surfaces in engineering fields. Here, a superhydrophobic aluminum alloy with enhanced anti-frosting, anti-icing, and self-cleaning performance has been developed by a facile one-step method. The anti-frosting/icing performance of superhydrophobic aluminum alloys is confirmed by frosting/icing time delay, consolidating and freezing temperature reduction, and lower amount of frost/ice adhesion. Meanwhile, the excellent self-cleaning performance is authenticated by the fact that simulated pollution particles can be cleaned out by rolling water droplets completely. Finally, based on the classical nucleation theory, anti-icing and anti-frosting mechanisms of the superhydrophobic aluminum alloys are deduced. Results show that grounded on "air cushion" and "heat insulation" effect, a larger nucleation barrier and a lower crystal growth rate can be observed, which, hence, inhibit ice formation and frost deposition. It can be concluded that preparing superhydrophobic surfaces would be an effective strategy for improving anti-icing, anti-frosting, and self-cleaning performance of aluminum alloys.
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Investigating heterogeneous nucleation in peritectic materials via the phase-field method
International Nuclear Information System (INIS)
Emmerich, Heike; Siquieri, Ricardo
2006-01-01
Here we propose a phase-field approach to investigate the influence of convection on peritectic growth as well as the heterogeneous nucleation kinetics of peritectic systems. For this purpose we derive a phase-field model for peritectic growth taking into account fluid flow in the melt, which is convergent to the underlying sharp interface problem in the thin interface limit (Karma and Rappel 1996 Phys. Rev. E 53 R3017). Moreover, we employ our new phase-field model to study the heterogeneous nucleation kinetics of peritectic material systems. Our approach is based on a similar approach towards homogeneous nucleation in Granasy et al (2003 Interface and Transport Dynamics (Springer Lecture Notes in Computational Science and Engineering vol 32) ed Emmerich et al (Berlin: Springer) p 190). We applied our model successfully to extend the nucleation rate predicted by classical nucleation theory for an additional morphological term relevant for peritectic growth. Further applications to understand the mechanisms and consequences of heterogeneous nucleation kinetics in more detail are discussed
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Directory of Open Access Journals (Sweden)
L. Nichman
2017-09-01
Full Text Available Optical probes are frequently used for the detection of microphysical cloud particle properties such as liquid and ice phase, size and morphology. These properties can eventually influence the angular light scattering properties of cirrus clouds as well as the growth and accretion mechanisms of single cloud particles. In this study we compare four commonly used optical probes to examine their response to small cloud particles of different phase and asphericity. Cloud simulation experiments were conducted at the Cosmics Leaving OUtdoor Droplets (CLOUD chamber at European Organisation for Nuclear Research (CERN. The chamber was operated in a series of multi-step adiabatic expansions to produce growth and sublimation of ice particles at super- and subsaturated ice conditions and for initial temperatures of −30, −40 and −50 °C. The experiments were performed for ice cloud formation via homogeneous ice nucleation. We report the optical observations of small ice particles in deep convection and in situ cirrus simulations. Ice crystal asphericity deduced from measurements of spatially resolved single particle light scattering patterns by the Particle Phase Discriminator mark 2 (PPD-2K, Karlsruhe edition were compared with Cloud and Aerosol Spectrometer with Polarisation (CASPOL measurements and image roundness captured by the 3View Cloud Particle Imager (3V-CPI. Averaged path light scattering properties of the simulated ice clouds were measured using the Scattering Intensity Measurements for the Optical detectioN of icE (SIMONE and single particle scattering properties were measured by the CASPOL. We show the ambiguity of several optical measurements in ice fraction determination of homogeneously frozen ice in the case where sublimating quasi-spherical ice particles are present. Moreover, most of the instruments have difficulties of producing reliable ice fraction if small aspherical ice particles are present, and all of the instruments cannot
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Experimental study of ion-induced nucleation by radon decay
International Nuclear Information System (INIS)
He, F.; Hopke, P.K.
1993-01-01
In the environment, the presence of ions from natural radioactivity may increase the rate of new particle formation through ion-induced nucleation. A thermal diffusion cloud chamber (TDCC) has been built to experimentally study ion-induced nucleation where the ions are produced by gaseous radioactive sources. The critical supersaturation values and nucleation rates for methanol, ethanol, 1-propanol, and 1-butanol vapors on ions produced within the volume of the chamber by alpha decay of 222 Rn have been measured quantitatively at various radioactivity concentrations and supersaturations. The presence of ion tracks and the effect of an external electric field were also investigated. The alpha tracks and ion-induced nucleation formed by 222 Rn decay become visible at the critical supersaturation that is below the value needed for homogeneous nucleation. At this supersaturation, the nucleation rates increase substantially with increasing 222 Rn at low activity concentrations, but attain limiting values at higher concentrations. The experimental results indicate that the ionization by radon decay will promote ion-cluster formation and lower the free energy barriers. The formation of visible droplets is strongly dependent on the supersaturation. This study also confirms that the external electric field has a significant effect on the observed rates of nucleation
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Laboratory Investigation of Contact Freezing and the Aerosol to Ice Crystal Transformation Process
Energy Technology Data Exchange (ETDEWEB)
Shaw, Raymond A. [Michigan Technological Univ., Houghton, MI (United States)
2014-10-28
This project has been focused on the following objectives: 1. Investigations of the physical processes governing immersion versus contact nucleation, specifically surface-induced crystallization; 2. Development of a quadrupole particle trap with full thermodynamic control over the temperature range 0 to –40 °C and precisely controlled water vapor saturation ratios for continuous, single-particle measurement of the aerosol to ice crystal transformation process for realistic ice nuclei; 3. Understanding the role of ice nucleation in determining the microphysical properties of mixed-phase clouds, within a framework that allows bridging between laboratory and field measurements.
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Longwave indirect effect of mineral dusts on ice clouds
Directory of Open Access Journals (Sweden)
Q. Min
2010-08-01
Full Text Available In addition to microphysical changes in clouds, changes in nucleation processes of ice cloud due to aerosols would result in substantial changes in cloud top temperature as mildly supercooled clouds are glaciated through heterogenous nucleation processes. Measurements from multiple sensors on multiple observing platforms over the Atlantic Ocean show that the cloud effective temperature increases with mineral dust loading with a slope of +3.06 °C per unit aerosol optical depth. The macrophysical changes in ice cloud top distributions as a consequence of mineral dust-cloud interaction exert a strong cooling effect (up to 16 Wm−2 of thermal infrared radiation on cloud systems. Induced changes of ice particle size by mineral dusts influence cloud emissivity and play a minor role in modulating the outgoing longwave radiation for optically thin ice clouds. Such a strong cooling forcing of thermal infrared radiation would have significant impacts on cloud systems and subsequently on climate.
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Directory of Open Access Journals (Sweden)
Anil S Thakur
2007-10-01
Full Text Available Crystallization is a major bottleneck in the process of macromolecular structure determination by X-ray crystallography. Successful crystallization requires the formation of nuclei and their subsequent growth to crystals of suitable size. Crystal growth generally occurs spontaneously in a supersaturated solution as a result of homogenous nucleation. However, in a typical sparse matrix screening experiment, precipitant and protein concentration are not sampled extensively, and supersaturation conditions suitable for nucleation are often missed.We tested the effect of nine potential heterogenous nucleating agents on crystallization of ten test proteins in a sparse matrix screen. Several nucleating agents induced crystal formation under conditions where no crystallization occurred in the absence of the nucleating agent. Four nucleating agents: dried seaweed; horse hair; cellulose and hydroxyapatite, had a considerable overall positive effect on crystallization success. This effect was further enhanced when these nucleating agents were used in combination with each other.Our results suggest that the addition of heterogeneous nucleating agents increases the chances of crystal formation when using sparse matrix screens.
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Availability analysis for heterogeneous nucleation in a uniform electric field
Saidi, M H
2003-01-01
Industrial demands for more compact heat exchangers are a motivation to find new technology features. Electrohydrodynamics (EHD) is introduced as a promising phenomenon for heat transfer enhancement mechanisms. Similar to any new technology, EHD has not been understood completely yet and require more fundamental studies. In boiling phase change phenomena, nucleation is the dominant mechanism in heat transfer. Because of higher performance in heat transfer, nucleate boiling is considered as the main regime in thermal components. Hence, bubble dynamic investigation is a means to evaluate heat transfer. This study investigate bubble formation, including homogeneous and heterogeneous nucleation, from a thermodynamic point of view. Change in availability due to bubble embryo nucleation is discussed. Stability criteria for these systems are theoretically studied and results are discussed considering experimental data. In addition, a conceptual discussion on entropy generation in a thermodynamic system under electri...
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Directory of Open Access Journals (Sweden)
O. Möhler
2006-01-01
Full Text Available Activation energies ΔGact for the nucleation of nitric acid dihydrate (NAD in supercooled binary HNO3/H2O solution droplets were calculated from volume-based nucleation rate measurements using the AIDA (Aerosol, Interactions, and Dynamics in the Atmosphere aerosol chamber of Forschungszentrum Karlsruhe. The experimental conditions covered temperatures T between 192 and 197 K, NAD saturation ratios SNAD between 7 and 10, and nitric acid molar fractions of the nucleating sub-micron sized droplets between 0.26 and 0.28. Based on classical nucleation theory, a new parameterisation for ΔGact=A×(T ln SNAD−2+B is fitted to the experimental data with A=2.5×106 kcal K2 mol−1 and B=11.2−0.1(T−192 kcal mol−1. A and B were chosen to also achieve good agreement with literature data of ΔGact. The parameter A implies, for the temperature and composition range of our analysis, a mean interface tension σsl=51 cal mol−1 cm−2 between the growing NAD germ and the supercooled solution. A slight temperature dependence of the diffusion activation energy is represented by the parameter B. Investigations with a detailed microphysical process model showed that literature formulations of volume-based (Salcedo et al., 2001 and surface-based (Tabazadeh et al., 2002 nucleation rates significantly overestimate NAD formation rates when applied to the conditions of our experiments.
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Directory of Open Access Journals (Sweden)
N. Reicher
2018-01-01
Full Text Available 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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Knopf, D. A.; Alpert, P. A.; Wang, B.; OBrien, R. E.; Moffet, R. C.; Aller, J. Y.; Laskin, A.; Gilles, M.
2013-12-01
Atmospheric ice formation represents one of the least understood atmospheric processes with important implications for the hydrological cycle and climate. Current freezing descriptions assume that ice active sites on the particle surface initiate ice nucleation, however, the nature of these sites remains elusive. Here, we present a new experimental method that allows us to relate physical and chemical properties of individual particles with observed water uptake and ice nucleation ability using a combination of micro-spectroscopic and optical single particle analytical techniques. We apply this method to field-collected particles and particles generated via bursting of bubbles produced by glass frit aeration and plunging water impingement jets in a mesocosm containing artificial sea water and bacteria and/or phytoplankton. The most efficient ice nuclei (IN) within a particle population are identified and characterized. Single particle characterization is achieved by computer controlled scanning electron microscopy with energy dispersive analysis of X-rays (CCSEM/EDX) and scanning transmission X-ray microscopy with near edge X-ray absorption fine structure spectroscopy. A vapor controlled cooling-stage coupled to an optical microscope is used to determine the onsets of water uptake, immersion freezing, and deposition ice nucleation of the individual particles as a function of temperature (T) as low as 200 K and relative humidity (RH) up to water saturation. In addition, we perform CCSEM/EDX to obtain on a single particle level the elemental composition of the entire particle population. Thus, we can determine if the IN are exceptional in nature or belong to a major particle type class with respect to composition and size. We find that ambient and sea spray particles are coated by organic material and can induce ice formation under tropospheric relevant conditions. Micro-spectroscopic single particle analysis of the investigated particle samples invokes a potential
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Schrod, Jann; Weber, Daniel; Thomson, Erik S.; Pöhlker, Christopher; Saturno, Jorge; Artaxo, Paulo; Curtius, Joachim; Bingemer, Heinz
2017-04-01
The number concentration of ice nucleating particles (INP) is an important, yet under quantified atmospheric parameter. The temporal and geographic extent of observations worldwide remains relatively small, with many regions of the world (even whole continents and oceans), almost completely unrepresented by observational data. Measurements at pristine sites are particularly rare, but all the more valuable because such observations are necessary to estimate the pre-industrial baseline of aerosol and cloud related parameters that are needed to better understand the climate system and forecast future scenarios. As a partner of BACCHUS we began in September 2014 to operate an INP measurement network of four sampling stations, with a global geographic distribution. The stations are located at unique sites reaching from the Arctic to the equator: the Amazonian Tall Tower Observatory ATTO in Brazil, the Observatoire Volcanologique et Sismologique on the island of Martinique in the Caribbean Sea, the Zeppelin Observatory at Svalbard in the Norwegian Arctic and the Taunus Observatory near Frankfurt, Germany. Since 2014 samples were collected regularly by electrostatic precipitation of aerosol particles onto silicon substrates. The INP on the substrate are activated and analyzed in the isothermal static diffusion chamber FRIDGE at temperatures between -20°C and -30°C and relative humidity with respect to ice from 115 to 135%. Here we present data from the years 2015 and 2016 from this novel INP network and from selected campaign-based measurements from remote sites, including the Mt. Kenya GAW station. Acknowledgements The research leading to these results has received funding from the European Union's Seventh Framework Programme (FP7/2007-2013) project BACCHUS under grant agreement No 603445 and the Deutsche Forschungsgemeinschaft (DFG) under the Research Unit FOR 1525 (INUIT).
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Heterogeneous Nucleation of Colloidal Crystals on a Glass Substrate with Depletion Attraction.
Guo, Suxia; Nozawa, Jun; Hu, Sumeng; Koizumi, Haruhiko; Okada, Junpei; Uda, Satoshi
2017-10-10
The heterogeneous nucleation of colloidal crystals with attractive interactions has been investigated via in situ observations. We have found two types of nucleation processes: a cluster that overcomes the critical size for nucleation with a monolayer, and a method that occurs with two layers. The Gibbs free energy changes (ΔG) for these two types of nucleation processes are evaluated by taking into account the effect of various interfacial energies. In contrast to homogeneous nucleation, the change in interfacial free energy, Δσ, is generated for colloidal nucleation on a foreign substrate such as a cover glass in the present study. The Δσ and step free energy of the first layer, γ 1 , are obtained experimentally based on the equation deduced from classical nucleation theory (CNT). It is concluded that the ΔG of q-2D nuclei is smaller than of monolayer nuclei, provided that the same number of particles are used, which explains the experimental result that the critical size in q-2D nuclei is smaller than that in monolayer nuclei.
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Crystal nucleation and dendrite growth of metastable phases in undercooled melts
International Nuclear Information System (INIS)
Herlach, Dieter
2011-01-01
Research highlights: → Homogenous nucleation. → Effects of convection on dendrite growth kinetics. → Description of disorder trapping validated by experiment. - Abstract: An undercooled melt possesses an enhanced free enthalpy that opens up the possibility to crystallize metastable crystalline solids in competition with their stable counterparts. Crystal nucleation selects the crystallographic phase whereas the growth dynamics controls microstructure evolution. We apply containerless processing techniques such as electromagnetic and electrostatic levitation to containerlesss undercool and solidify metallic melts. Owing to the complete avoidance of heterogeneous nucleation on container-walls a large undercooling range becomes accessible with the extra benefit that the freely suspended drop is direct accessible for in situ observation of crystallization far away from equilibrium. Results of investigations of maximum undercoolability on pure zirconium are presented showing the limit of maximum undercoolability set by the onset of homogeneous nucleation. Rapid dendrite growth is measured as a function of undercooling by a high-speed camera and analysed within extended theories of non-equilibrium solidification. In such both supersaturated solid solutions and disordered superlattice structure of intermetallics are formed at high growth velocities. A sharp interface theory of dendrite growth is capable to describe the non-equilibrium solidification phenomena during rapid crystallization of deeply undercooled melts. Eventually, anomalous growth behaviour of Al-rich Al-Ni alloys is presented, which may be caused by forced convection.
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Bundke, U.; Jaenicke, R.; Klein, H.; Nillius, B.; Reimann, B.; Wetter, T.; Bingemer, H.
2009-04-01
Ice formation in clouds is a subject of great practical and fundamental importance since the occurrence of ice particle initializes dramatic changes in the microphysical structure of the cloud, which finally ends in the formation of precipitation. The initially step of ice formation is largely unknown. Homogenous nucleation of ice occurs only below -40 °C. If an ice nucleus (IN) is present, heterogeneous nucleation may occur at higher temperature. Here deposition freezing, condensation and immersion freezing as well as contact freezing are known. Also growth rates of ice particles are known as function of crystal surface properties, temperature and super saturation. Timescales for homogenous freezing activation in the order of 0.01 seconds and nucleation rates have been measured by Anderson et al. (1980) and Hagen et al., (1981) using their expansion cloud chamber. This contribution of deposition mode freezing measurements by the ice nucleus counter FINCH presents evidence that the activation timescale of this freezing mode is in the order of 1E-3 seconds. FINCH is an Ice Nucleus counter which activates IN in a supersaturated environment at freezing temperatures. The activation conditions are actively controlled by mixing three gas flows (aerosol, particle-free cold-dry and warm-humid flows).See Bundke et al. 2008 for details. In a special operation mode of FINCH we are able to produce a controlled peak super saturation in the order of 1 ms duration. For several test aerosols the results observed in this particular mode are comparable to normal mode operations, where the maximum super saturation remains for more than a second, thus leading to the conclusion that the time for activation is in the order of 1ms or less. References: R.J. Anderson et al, "A Study of Homogeneous Condensation Freezing Nucleation of Small Water Droplets in an Expansion Cloud Chamber, Journal of the Atmospheric Sciences, Vol. 37, 2508-2520, 1980 U.Bundke et al., "The fast Ice Nucleus
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Strategies to initiate and control the nucleation behavior of bimetallic nanoparticles.
Krishnan, Gopi; de Graaf, Sytze; Ten Brink, Gert H; Persson, Per O Å; Kooi, Bart J; Palasantzas, George
2017-06-22
In this work we report strategies to nucleate bimetallic nanoparticles (NPs) made by gas phase synthesis of elements showing difficulty in homogeneous nucleation. It is shown that the nucleation assisted problem of bimetallic NP synthesis can be solved via the following pathways: (i) selecting an element which can itself nucleate and act as a nucleation center for the synthesis of bimetallic NPs; (ii) introducing H 2 or CH 4 as an impurity/trace gas to initiate nucleation during the synthesis of bimetallic NPs. The latter can solve the problem if none of the elements in a bimetallic NP can initiate nucleation. We illustrate the abovementioned strategies for the case of Mg based bimetallic NPs, which are interesting as hydrogen storage materials and exhibit both nucleation and oxidation issues even under ultra-high vacuum conditions. In particular, it is shown that adding H 2 in small proportions favors the formation of a solid solution/alloy structure even in the case of immiscible Mg and Ti, where normally phase separation occurs during synthesis. In addition, we illustrate the possibility of improving the nucleation rate, and controlling the structure and size distribution of bimetallic NPs using H 2 /CH 4 as a reactive/nucleating gas. This is shown to be associated with the dimer bond energies of the various formed species and the vapor pressures of the metals, which are key factors for NP nucleation.
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Directory of Open Access Journals (Sweden)
M. Kulmala
2008-08-01
Full Text Available Binary homogeneous nucleation (BHN of sulphuric acid and water (H2SO4/H2O is one of the most important atmospheric nucleation processes, but laboratory observations of this nucleation process are very limited and there are also large discrepancies between different laboratory studies. The difficulties associated with these experiments include wall loss of H2SO4 and uncertainties in estimation of H2SO4 concentration ([H2SO4] involved in nucleation. We have developed a new laboratory nucleation setup to study H2SO4/H2O BHN kinetics and provide relatively constrained [H2SO4] needed for nucleation. H2SO4 is produced from the SO2+OH→HSO3 reaction and OH radicals are produced from water vapor UV absorption. The residual [H2SO4] were measured at the end of the nucleation reactor with a chemical ionization mass spectrometer (CIMS. Wall loss factors (WLFs of H2SO4 were estimated by assuming that wall loss is diffusion limited and these calculated WLFs were in good agreement with simultaneous measurements of the initial and residual [H2SO4] with two CIMSs. The nucleation zone was estimated from numerical simulations based on the measured aerosol sizes (particle diameter, Dp and [H2SO4]. The measured BHN rates (J ranged from 0.01–220 cm−3 s−1 at the initial and residual [H2SO4] from 108−1010 cm−3, a temperature of 288 K and relative humidity (RH from 11–23%; J increased with increasing [H2SO4] and RH. J also showed a power dependence on [H2SO4] with the exponential power of 3–8. These power dependences are consistent with other laboratory studies under similar [H2SO4] and RH, but different from atmospheric field observations which showed that particle number concentrations are often linearly dependent on [H2SO4]. These results, together with a higher [H2SO4] threshold (108–109 cm−3 needed to produce the unit J measured from the laboratory studies compared to the atmospheric conditions (106–107 cm−3, imply that H2SO4/H2O BHN alone is
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International Nuclear Information System (INIS)
Deinum, Eva E; Tindemans, Simon H; Mulder, Bela M
2011-01-01
The highly aligned cortical microtubule array of interphase plant cells is a key regulator of anisotropic cell expansion. Recent computational and analytical work has shown that the non-equilibrium self-organization of this structure can be understood on the basis of experimentally observed collisional interactions between dynamic microtubules attached to the plasma membrane. Most of these approaches assumed that new microtubules are homogeneously and isotropically nucleated on the cortical surface. Experimental evidence, however, shows that nucleation mostly occurs from other microtubules and under specific relative angles. Here, we investigate the impact of directed microtubule-bound nucleations on the alignment process using computer simulations. The results show that microtubule-bound nucleations can increase the degree of alignment achieved, decrease the timescale of the ordering process and widen the regime of dynamic parameters for which the system can self-organize. We establish that the major determinant of this effect is the degree of co-alignment of the nucleations with the parent microtubule. The specific role of sideways branching nucleations appears to allow stronger alignment while maintaining a measure of overall spatial homogeneity. Finally, we investigate the suggestion that observed persistent rotation of microtubule domains can be explained through a handedness bias in microtubule-bound nucleations, showing that this is possible only for an extreme bias and over a limited range of parameters
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Deinum, Eva E.; Tindemans, Simon H.; Mulder, Bela M.
2011-10-01
The highly aligned cortical microtubule array of interphase plant cells is a key regulator of anisotropic cell expansion. Recent computational and analytical work has shown that the non-equilibrium self-organization of this structure can be understood on the basis of experimentally observed collisional interactions between dynamic microtubules attached to the plasma membrane. Most of these approaches assumed that new microtubules are homogeneously and isotropically nucleated on the cortical surface. Experimental evidence, however, shows that nucleation mostly occurs from other microtubules and under specific relative angles. Here, we investigate the impact of directed microtubule-bound nucleations on the alignment process using computer simulations. The results show that microtubule-bound nucleations can increase the degree of alignment achieved, decrease the timescale of the ordering process and widen the regime of dynamic parameters for which the system can self-organize. We establish that the major determinant of this effect is the degree of co-alignment of the nucleations with the parent microtubule. The specific role of sideways branching nucleations appears to allow stronger alignment while maintaining a measure of overall spatial homogeneity. Finally, we investigate the suggestion that observed persistent rotation of microtubule domains can be explained through a handedness bias in microtubule-bound nucleations, showing that this is possible only for an extreme bias and over a limited range of parameters.
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Nucleation and microstructure development in Cr-Mo-V tool steel during gas atomization
Behúlová, M.; Grgač, P.; Čička, R.
2017-11-01
Nucleation studies of undercooled metallic melts are of essential interest for the understanding of phase selection, growth kinetics and microstructure development during their rapid non-equilibrium solidification. The paper deals with the modelling of nucleation processes and microstructure development in the hypoeutectic tool steel Ch12MF4 with the chemical composition of 2.37% C, 12.06 % Cr, 1.2% Mo, 4.0% V and balance Fe [wt. %] in the process of nitrogen gas atomization. Based on the classical theory of homogeneous nucleation, the nucleation temperature of molten rapidly cooled spherical particles from this alloy with diameter from 40 μm to 600 μm in the gas atomization process is calculated using various estimations of parameters influencing the nucleation process - the Gibbs free energy difference between solid and liquid phases and the solid/liquid interfacial energy. Results of numerical calculations are compared with experimentally measured nucleation temperatures during levitation experiments and microstructures developed in rapidly solidified powder particles from the investigated alloy.
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Directory of Open Access Journals (Sweden)
Florian Steinbach
2017-09-01
Full Text Available The flow of ice depends on the properties of the aggregate of individual ice crystals, such as grain size or lattice orientation distributions. Therefore, an understanding of the processes controlling ice micro-dynamics is needed to ultimately develop a physically based macroscopic ice flow law. We investigated the relevance of the process of grain dissection as a grain-size-modifying process in natural ice. For that purpose, we performed numerical multi-process microstructure modeling and analyzed microstructure and crystallographic orientation maps from natural deep ice-core samples from the North Greenland Eemian Ice Drilling (NEEM project. Full crystallographic orientations measured by electron backscatter diffraction (EBSD have been used together with c-axis orientations using an optical technique (Fabric Analyser. Grain dissection is a feature of strain-induced grain boundary migration. During grain dissection, grain boundaries bulge into a neighboring grain in an area of high dislocation energy and merge with the opposite grain boundary. This splits the high dislocation-energy grain into two parts, effectively decreasing the local grain size. Currently, grain size reduction in ice is thought to be achieved by either the progressive transformation from dislocation walls into new high-angle grain boundaries, called subgrain rotation or polygonisation, or bulging nucleation that is assisted by subgrain rotation. Both our time-resolved numerical modeling and NEEM ice core samples show that grain dissection is a common mechanism during ice deformation and can provide an efficient process to reduce grain sizes and counter-act dynamic grain-growth in addition to polygonisation or bulging nucleation. Thus, our results show that solely strain-induced boundary migration, in absence of subgrain rotation, can reduce grain sizes in polar ice, in particular if strain energy gradients are high. We describe the microstructural characteristics that can be
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Steinbach, Florian; Kuiper, Ernst-Jan N.; Eichler, Jan; Bons, Paul D.; Drury, Martyn R.; Griera, Albert; Pennock, Gill M.; Weikusat, Ilka
2017-09-01
The flow of ice depends on the properties of the aggregate of individual ice crystals, such as grain size or lattice orientation distributions. Therefore, an understanding of the processes controlling ice micro-dynamics is needed to ultimately develop a physically based macroscopic ice flow law. We investigated the relevance of the process of grain dissection as a grain-size-modifying process in natural ice. For that purpose, we performed numerical multi-process microstructure modelling and analysed microstructure and crystallographic orientation maps from natural deep ice-core samples from the North Greenland Eemian Ice Drilling (NEEM) project. Full crystallographic orientations measured by electron backscatter diffraction (EBSD) have been used together with c-axis orientations using an optical technique (Fabric Analyser). Grain dissection is a feature of strain-induced grain boundary migration. During grain dissection, grain boundaries bulge into a neighbouring grain in an area of high dislocation energy and merge with the opposite grain boundary. This splits the high dislocation-energy grain into two parts, effectively decreasing the local grain size. Currently, grain size reduction in ice is thought to be achieved by either the progressive transformation from dislocation walls into new high-angle grain boundaries, called subgrain rotation or polygonisation, or bulging nucleation that is assisted by subgrain rotation. Both our time-resolved numerical modelling and NEEM ice core samples show that grain dissection is a common mechanism during ice deformation and can provide an efficient process to reduce grain sizes and counter-act dynamic grain-growth in addition to polygonisation or bulging nucleation. Thus, our results show that solely strain-induced boundary migration, in absence of subgrain rotation, can reduce grain sizes in polar ice, in particular if strain energy gradients are high. We describe the microstructural characteristics that can be used to
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Czech Academy of Sciences Publication Activity Database
Planková, Barbora; Vinš, Václav; Hrubý, Jan
2017-01-01
Roč. 147, č. 16 (2017), č. článku 164702. ISSN 0021-9606 R&D Projects: GA MŠk(CZ) 7F14466; GA ČR(CZ) GJ15-07129Y Institutional support: RVO:61388998 Keywords : nucleation * classical nucleation theory * density gradient theory Subject RIV: BJ - Thermodynamics OBOR OECD: Thermodynamics Impact factor: 2.965, year: 2016
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Main features of nucleation in model solutions of oral cavity
Golovanova, O. A.; Chikanova, E. S.; Punin, Yu. O.
2015-05-01
The regularities of nucleation in model solutions of oral cavity have been investigated, and the induction order and constants have been determined for two systems: saliva and dental plaque fluid (DPF). It is shown that an increase in the initial supersaturation leads to a transition from the heterogeneous nucleation of crystallites to a homogeneous one. Some additives are found to enhance nucleation: HCO{3/-} > C6H12O6 > F-, while others hinder this process: protein (casein) > Mg2+. It is established that crystallization in DPF occurs more rapidly and the DPF composition is favorable for the growth of small (52.6-26.1 μm) crystallites. On the contrary, the conditions implemented in the model saliva solution facilitate the formation of larger (198.4-41.8 μm) crystals.
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Non-equilibrium Quasi-Chemical Nucleation Model
Gorbachev, Yuriy E.
2018-04-01
Quasi-chemical model, which is widely used for nucleation description, is revised on the basis of recent results in studying of non-equilibrium effects in reacting gas mixtures (Kolesnichenko and Gorbachev in Appl Math Model 34:3778-3790, 2010; Shock Waves 23:635-648, 2013; Shock Waves 27:333-374, 2017). Non-equilibrium effects in chemical reactions are caused by the chemical reactions themselves and therefore these contributions should be taken into account in the corresponding expressions for reaction rates. Corrections to quasi-equilibrium reaction rates are of two types: (a) spatially homogeneous (caused by physical-chemical processes) and (b) spatially inhomogeneous (caused by gas expansion/compression processes and proportional to the velocity divergency). Both of these processes play an important role during the nucleation and are included into the proposed model. The method developed for solving the generalized Boltzmann equation for chemically reactive gases is applied for solving the set of equations of the revised quasi-chemical model. It is shown that non-equilibrium processes lead to essential deviation of the quasi-stationary distribution and therefore the nucleation rate from its traditional form.
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The location of the second critical point of water
Kanno, Hitoshi; Miyata, Kuniharu
2006-05-01
Based on the DTA data for homogeneous ice nucleation of emulsified liquid water at low temperatures and high pressures, the location of the second critical point (SCP) of water, which is expected to exist in addition to the normal liquid-vapor critical point, is estimated to be at 145 K pressure). It is shown that SCP is closely associated with the break point of the curve for the homogeneous ice nucleation temperature ( TH) of liquid water and with the transition between low density and high density amorphous solid water (LDA and HDA). Although the existence of SCP has become more realistic, the location seems to be less favorable to the water model of the second-critical-point interpretation.
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The Nucleation of Protein Aggregates - From Crystals to Amyloid Fibrils.
Buell, Alexander K
2017-01-01
The condensation and aggregation of individual protein molecules into dense insoluble phases is of relevance in such diverse fields as materials science, medicine, structural biology and pharmacology. A common feature of these condensation phenomena is that they usually are nucleated processes, i.e. the first piece of the condensed phase is energetically costly to create and hence forms slowly compared to its subsequent growth. Here we give a compact overview of the differences and similarities of various protein nucleation phenomena, their theoretical description in the framework of colloid and polymer science and their experimental study. Particular emphasis is put on the nucleation of a specific type of filamentous protein aggregates, amyloid fibrils. The current experimentally derived knowledge on amyloid fibril nucleation is critically assessed, and we argue that it is less advanced than is generally believed. This is due to (I) the lack of emphasis that has been put on the distinction between homogeneous and heterogeneous nucleation in experimental studies (II) the use of oversimplifying and/or inappropriate theoretical frameworks for the analysis of kinetic data of amyloid fibril nucleation. A strategy is outlined and advocated of how our understanding of this important class of processes can be improved in the future. © 2017 Elsevier Inc. All rights reserved.
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Two-Dimensional Nucleation on the Terrace of Colloidal Crystals with Added Polymers.
Nozawa, Jun; Uda, Satoshi; Guo, Suxia; Hu, Sumeng; Toyotama, Akiko; Yamanaka, Junpei; Okada, Junpei; Koizumi, Haruhiko
2017-04-04
Understanding nucleation dynamics is important both fundamentally and technologically in materials science and other scientific fields. Two-dimensional (2D) nucleation is the predominant growth mechanism in colloidal crystallization, in which the particle interaction is attractive, and has recently been regarded as a promising method to fabricate varieties of complex nanostructures possessing innovative functionality. Here, polymers are added to a colloidal suspension to generate a depletion attractive force, and the detailed 2D nucleation process on the terrace of the colloidal crystals is investigated. In the system, we first measured the nucleation rate at various area fractions of particles on the terrace, ϕ area . In situ observations at single-particle resolution revealed that nucleation behavior follows the framework of classical nucleation theory (CNT), such as single-step nucleation pathway and existence of critical size. Characteristic nucleation behavior is observed in that the nucleation and growth stage are clearly differentiated. When many nuclei form in a small area of the terrace, a high density of kink sites of once formed islands makes growth more likely to occur than further nucleation because nucleation has a higher energy barrier than growth. The steady-state homogeneous 2D nucleation rate, J, and the critical size of nuclei, r*, are measured by in situ observations based on the CNT, which enable us to obtain the step free energy, γ, which is an important parameter for characterizing the nucleation process. The γ value is found to change according to the strength of attraction, which is tuned by the concentration of the polymer as a depletant.
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Horsch, Martin; Vrabec, Jadran; Bernreuther, Martin; Grottel, Sebastian; Reina, Guido; Wix, Andrea; Schaber, Karlheinz; Hasse, Hans
2008-04-28
Molecular dynamics (MD) simulation is applied to the condensation process of supersaturated vapors of methane, ethane, and carbon dioxide. Simulations of systems with up to a 10(6) particles were conducted with a massively parallel MD program. This leads to reliable statistics and makes nucleation rates down to the order of 10(30) m(-3) s(-1) accessible to the direct simulation approach. Simulation results are compared to the classical nucleation theory (CNT) as well as the modification of Laaksonen, Ford, and Kulmala (LFK) which introduces a size dependence of the specific surface energy. CNT describes the nucleation of ethane and carbon dioxide excellently over the entire studied temperature range, whereas LFK provides a better approach to methane at low temperatures.
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Alpert, P. A.; Radway, J.; Kilthau, W.; Bothe, D.; Knopf, D. A.; Aller, J. Y.
2013-12-01
The oceans cover the majority of the earth's surface, host nearly half the total global primary productivity and are a major source of atmospheric aerosol particles. However, effects of biological activity on sea spray generation and composition, and subsequent cloud formation are not well understood. Our goal is to elucidate these effects which will be particularly important over nutrient rich seas, where microorganisms can reach concentrations of 10^9 per mL and along with transparent exopolymer particles (TEP) can become aerosolized. Here we report the results of mesocosm experiments in which bubbles were generated by two methods, either recirculating impinging water jets or glass frits, in natural or artificial seawater containing bacteria and unialgal cultures of three representative phytoplankton species, Thalassiosira pseudonana, Emiliania huxleyi, and Nannochloris atomus. Over time we followed the size distribution of aerosolized particles as well as their hygroscopicity, heterogeneous ice nucleation potential, and individual physical-chemical characteristics. Numbers of cells and the mass of dissolved and particulate organic carbon (DOC, POC), TEP (which includes polysaccharide-containing microgels and nanogels >0.4 μm in diameter) were determined in the bulk water, the surface microlayer, and aerosolized material. Aerosolized particles were also impacted onto substrates for ice nucleation and water uptake experiments, elemental analysis using computer controlled scanning electron microscopy and energy dispersive analysis of X-rays (CCSEM/EDX), and determination of carbon bonding with scanning transmission X-ray microscopy and near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Regardless of bubble generation method, the overall concentration of aerosol particles, TEP, POC and DOC increased as concentrations of bacterial and phytoplankton cells increased, stabilized, and subsequently declined. Particles cloud formation and potential
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Mechanism of supercooled droplet freezing on surfaces.
Jung, Stefan; Tiwari, Manish K; Doan, N Vuong; Poulikakos, Dimos
2012-01-10
Understanding ice formation from supercooled water on surfaces is a problem of fundamental importance and general utility. Superhydrophobic surfaces promise to have remarkable 'icephobicity' and low ice adhesion. Here we show that their icephobicity can be rendered ineffective by simple changes in environmental conditions. Through experiments, nucleation theory and heat transfer physics, we establish that humidity and/or the flow of a surrounding gas can fundamentally switch the ice crystallization mechanism, drastically affecting surface icephobicity. Evaporative cooling of the supercooled liquid can engender ice crystallization by homogeneous nucleation at the droplet-free surface as opposed to the expected heterogeneous nucleation at the substrate. The related interplay between droplet roll-off and rapid crystallization is also studied. Overall, we bring a novel perspective to icing and icephobicity, unveiling the strong influence of environmental conditions in addition to the accepted effects of the surface conditions and hydrophobicity.
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Corona-producing ice clouds: A case study of a cold mid-latitude cirrus layer
International Nuclear Information System (INIS)
Sassen, K.; Mace, G.G.; Hallett, J.; Poellot, M.R.
1998-01-01
A high (14.0-km), cold (-71.0thinsp degree C) cirrus cloud was studied by ground-based polarization lidar and millimeter radar and aircraft probes on the night of 19 April 1994 from the Cloud and Radiation Testbed site in northern Oklahoma. A rare cirrus cloud lunar corona was generated by this 1 - 2-km-deep cloud, thus providing an opportunity to measure the composition in situ, which had previously been assumed only on the basis of lidar depolarization data and simple diffraction theory for spheres. In this case, corona ring analysis indicated an effective particle diameter of ∼22 μm. A variety of in situ data corroborates the approximate ice-particle size derived from the passive retrieval method, especially near the cloud top, where impacted cloud samples show simple solid crystals. The homogeneous freezing of sulfuric acid droplets of stratospheric origin is assumed to be the dominant ice-particle nucleation mode acting in corona-producing cirrus clouds. It is speculated that this process results in a previously unrecognized mode of acid-contaminated ice-particle growth and that such small-particle cold cirrus clouds are potentially a radiatively distinct type of cloud. copyright 1998 Optical Society of America
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Heterogeneous Nucleation and Growth of Nanoparticles at Environmental Interfaces.
Jun, Young-Shin; Kim, Doyoon; Neil, Chelsea W
2016-09-20
water chemistry and substrate identity on heterogeneously and homogeneously formed nanoscale precipitate size dimensions and total particle volume. Using this technique, we also provided a new platform for quantitatively comparing between heterogeneous and homogeneous nucleation and growth of nanoparticles and obtaining undiscovered interfacial energies between nuclei and surfaces. In addition, nanoscale surface characterization tools, such as in situ atomic force microscopy (AFM), were utilized to support and complement our findings. With these powerful nanoscale tools, we systematically evaluated the influences of environmentally abundant (oxy)anions and cations and the properties of environmental surfaces, such as surface charge and hydrophobicity. The findings, significantly enhanced by in situ observations, can lead to a more accurate prediction of the behaviors of nanoparticles in the environment and enable better control of the physicochemical properties of nanoparticles in engineered systems, such as catalytic reactions and energy storage.
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Onset of runaway nucleation in aerosol reactors
Wu, Jin Jwang; Flagan, Richard C.
1987-01-01
The onset of homogeneous nucleation of new particles from the products of gas phase chemical reactions was explored using an aerosol reactor in which seed particles of silicon were grown by silane pyrolysis. The transition from seed growth by cluster deposition to catastrophic nucleation was extremely abrupt, with as little as a 17 percent change in the reactant concentration leading to an increase in the concentration of measurable particles of four orders of magnitude. From the structure of the particles grown near this transition, it is apparent that much of the growth occurs by the accumulation of clusters on the growing seed particles. The time scale for cluster diffusion indicates, however, that the clusters responsible for growth must be much smaller than the apparent fine structure of the product particles.
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Energy Technology Data Exchange (ETDEWEB)
Klein, William [Boston Univ., MA (United States)
2016-09-12
Over the 21 years of funding we have pursued several projects related to earthquakes, damage and nucleation. We developed simple models of earthquake faults which we studied to understand Gutenburg-Richter scaling, foreshocks and aftershocks, the effect of spatial structure of the faults and its interaction with underlying self organization and phase transitions. In addition we studied the formation of amorphous solids via the glass transition. We have also studied nucleation with a particular concentration on transitions in systems with a spatial symmetry change. In addition we investigated the nucleation process in models that mimic rock masses. We obtained the structure of the droplet in both homogeneous and heterogeneous nucleation. We also investigated the effect of defects or asperities on the nucleation of failure in simple models of earthquake faults.
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On the growth of homogeneously nucleated water droplets in nitrogen: an experimental study
Czech Academy of Sciences Publication Activity Database
Fransen, M. A. L. J.; Sachteleben, E.; Hrubý, Jan; Smeulders, D. M. J.
2014-01-01
Roč. 55, č. 7 (2014), s. 1780-1780 ISSN 0723-4864 R&D Projects: GA ČR(CZ) GAP101/11/1593 Institutional support: RVO:61388998 Keywords : droplet nucleation * droplet growth * water Subject RIV: BJ - Thermodynamics Impact factor: 1.670, year: 2014 http://link.springer.com/article/10.1007%2Fs00348-014-1780-y
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Sosso, Gabriele C; Chen, Ji; Cox, Stephen J; Fitzner, Martin; Pedevilla, Philipp; Zen, Andrea; Michaelides, Angelos
2016-06-22
The nucleation of crystals in liquids is one of nature's most ubiquitous phenomena, playing an important role in areas such as climate change and the production of drugs. As the early stages of nucleation involve exceedingly small time and length scales, atomistic computer simulations can provide unique insights into the microscopic aspects of crystallization. In this review, we take stock of the numerous molecular dynamics simulations that, in the past few decades, have unraveled crucial aspects of crystal nucleation in liquids. We put into context the theoretical framework of classical nucleation theory and the state-of-the-art computational methods by reviewing simulations of such processes as ice nucleation and the crystallization of molecules in solutions. We shall see that molecular dynamics simulations have provided key insights into diverse nucleation scenarios, ranging from colloidal particles to natural gas hydrates, and that, as a result, the general applicability of classical nucleation theory has been repeatedly called into question. We have attempted to identify the most pressing open questions in the field. We believe that, by improving (i) existing interatomic potentials and (ii) currently available enhanced sampling methods, the community can move toward accurate investigations of realistic systems of practical interest, thus bringing simulations a step closer to experiments.
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Adsorption of dysprosium on the graphite (0001) surface: Nucleation and growth at 300 K
International Nuclear Information System (INIS)
Kwolek, Emma J.; Lii-Rosales, Ann; Lei, Huaping; Wang, Cai-Zhuang; Tringides, Michael C.; Evans, James W.; Wallingford, Mark; Zhou, Yinghui; Thiel, Patricia A.
2016-01-01
We have studied nucleation and growth of Dy islands on the basal plane of graphite at 300 K using scanning tunneling microscopy, density functional theory (DFT) in a form that includes van der Waals interactions, and analytic theory. The interaction of atomic Dy with graphite is strong, while the diffusion barrier is small. Experiment shows that at 300 K, the density of nucleated islands is close to the value predicted for homogeneous nucleation, using critical nucleus size of 1 and the DFT-derived diffusion barrier. Homogeneous nucleation is also supported by the monomodal shape of the island size distributions. Comparison with the published island density of Dy on graphene shows that the value is about two orders of magnitude smaller on graphite, which can be attributed to more effective charge screening in graphite. The base of each island is 3 atomic layers high and atomically ordered, forming a coincidence lattice with the graphite. Islands resist coalescence, probably due to multiple rotational orientations associated with the coincidence lattice. Upper levels grow as discernible single-atom layers. Analysis of the level populations reveals significant downward interlayer transport, which facilitates growth of the base. This island shape is metastable, since more compact three-dimensional islands form at elevated growth temperature.
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Adsorption of dysprosium on the graphite (0001) surface: Nucleation and growth at 300 K
Energy Technology Data Exchange (ETDEWEB)
Kwolek, Emma J.; Lii-Rosales, Ann [The Ames Laboratory, Ames, Iowa 50011 (United States); Department of Chemistry, Iowa State University, Ames, Iowa 50011 (United States); Lei, Huaping; Wang, Cai-Zhuang; Tringides, Michael C.; Evans, James W. [The Ames Laboratory, Ames, Iowa 50011 (United States); Department of Physics and Astronomy, Iowa State University, Ames, Iowa 50011 (United States); Wallingford, Mark; Zhou, Yinghui [The Ames Laboratory, Ames, Iowa 50011 (United States); Thiel, Patricia A., E-mail: pthiel@iastate.edu [The Ames Laboratory, Ames, Iowa 50011 (United States); Department of Chemistry, Iowa State University, Ames, Iowa 50011 (United States); Department of Materials Science and Engineering, Iowa State University, Ames, Iowa 50011 (United States)
2016-12-07
We have studied nucleation and growth of Dy islands on the basal plane of graphite at 300 K using scanning tunneling microscopy, density functional theory (DFT) in a form that includes van der Waals interactions, and analytic theory. The interaction of atomic Dy with graphite is strong, while the diffusion barrier is small. Experiment shows that at 300 K, the density of nucleated islands is close to the value predicted for homogeneous nucleation, using critical nucleus size of 1 and the DFT-derived diffusion barrier. Homogeneous nucleation is also supported by the monomodal shape of the island size distributions. Comparison with the published island density of Dy on graphene shows that the value is about two orders of magnitude smaller on graphite, which can be attributed to more effective charge screening in graphite. The base of each island is 3 atomic layers high and atomically ordered, forming a coincidence lattice with the graphite. Islands resist coalescence, probably due to multiple rotational orientations associated with the coincidence lattice. Upper levels grow as discernible single-atom layers. Analysis of the level populations reveals significant downward interlayer transport, which facilitates growth of the base. This island shape is metastable, since more compact three-dimensional islands form at elevated growth temperature.
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Atmospheric nucleation: highlights of the EUCAARI project and future directions
Directory of Open Access Journals (Sweden)
V.-M. Kerminen
2010-11-01
Full Text Available Within the project EUCAARI (European Integrated project on Aerosol Cloud Climate and Air Quality interactions, atmospheric nucleation was studied by (i developing and testing new air ion and cluster spectrometers, (ii conducting homogeneous nucleation experiments for sulphate and organic systems in the laboratory, (iii investigating atmospheric nucleation mechanism under field conditions, and (iv applying new theoretical and modelling tools for data interpretation and development of parameterisations. The current paper provides a synthesis of the obtained results and identifies the remaining major knowledge gaps related to atmospheric nucleation. The most important technical achievement of the project was the development of new instruments for measuring sub-3 nm particle populations, along with the extensive application of these instruments in both the laboratory and the field. All the results obtained during EUCAARI indicate that sulphuric acid plays a central role in atmospheric nucleation. However, also vapours other than sulphuric acid are needed to explain the nucleation and the subsequent growth processes, at least in continental boundary layers. Candidate vapours in this respect are some organic compounds, ammonia, and especially amines. Both our field and laboratory data demonstrate that the nucleation rate scales to the first or second power of the nucleating vapour concentration(s. This agrees with the few earlier field observations, but is in stark contrast with classical thermodynamic nucleation theories. The average formation rates of 2-nm particles were found to vary by almost two orders of magnitude between the different EUCAARI sites, whereas the formation rates of charged 2-nm particles varied very little between the sites. Overall, our observations are indicative of frequent, yet moderate, ion-induced nucleation usually outweighed by much stronger neutral nucleation events in the continental lower troposphere. The most concrete
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Microbial production of ice crystals in clouds as a novel atmospheric biosignature
Santl-Temkiv, T.; Sahyoun, M.; Kjeldsen, H.; Ling, M.; Boesen, T.; Karlson, U. G.; Finster, K.
2014-03-01
A diverse assembly of exoplanets has been discovered during recent decades (Howard 2013), their atmospheres providing some of the most accessible evidence for the presence of biological activity on these planets. Metabolic gases have been commonly proposed as atmospheric biosignatures (Seager et al 2012). However, airborne microbes are also involved in cloud- and precipitation formation on Earth. Thus, meteorological phenomena may serve as alternative atmospheric biosignatures, for which appropriate observational techniques have yet to be developed. The atmospheric part of the Earth's water cycle heavily relies on the presence of nucleating particles, which promote the condensation and freezing of atmospheric water, both potentially leading to precipitation. While cloud condensation nuclei are diverse and relatively common, ice nuclei are poorly understood and comparably rare airborne particles. According to current knowledge, most ice nucleation below ñ15∞C is driven by the presence of inorganic dust particles, which are considered inactive at higher temperatures. Biogenic IN are the only reported particles that promote ice formation above ñ10∞C. Some bacteria, e.g. Pseudomonas syringae, produce Ice Nucleation Active (INA) proteins that are most efficient ice nuclei currently known. These INA bacteria are common in the atmosphere, and may thus be involved in precipitation processes of mixed phase clouds (Möhler et al 2007). We investigate the relevance of bacterial INA proteins for atmospheric processes using three approaches: (i) study of the presence of INA bacteria and their INA proteins in the atmosphere, (ii) a detailed molecular and physical study of isolated INA proteins, and finally (iii) a modeling study of the importance of INA proteins for ice-path in clouds as well as their importance for precipitation. During 14 precipitation events, we observed that 12% of isolated bacteria carried INA genes. INA bacteria had likely been emitted to the
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Rosa, Mónica; Tiago, João M; Singh, Satish K; Geraldes, Vítor; Rodrigues, Miguel A
2016-10-01
The quality of lyophilized products is dependent of the ice structure formed during the freezing step. Herein, we evaluate the importance of the air gap at the bottom of lyophilization vials for consistent nucleation, ice structure, and cake appearance. The bottom of lyophilization vials was modified by attaching a rectified aluminum disc with an adhesive material. Freezing was studied for normal and converted vials, with different volumes of solution, varying initial solution temperature (from 5°C to 20°C) and shelf temperature (from -20°C to -40°C). The impact of the air gap on the overall heat transfer was interpreted with the assistance of a computational fluid dynamics model. Converted vials caused nucleation at the bottom and decreased the nucleation time up to one order of magnitude. The formation of ice crystals unidirectionally structured from bottom to top lead to a honeycomb-structured cake after lyophilization of a solution with 4% mannitol. The primary drying time was reduced by approximately 35%. Converted vials that were frozen radially instead of bottom-up showed similar improvements compared with normal vials but very poor cake quality. Overall, the curvature of the bottom of glass vials presents a considerable threat to consistency by delaying nucleation and causing radial ice growth. Rectifying the vials bottom with an adhesive material revealed to be a relatively simple alternative to overcome this inconsistency.
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Shaposhnikov, Dmitry S.; Rodin, Alexander V.; Medvedev, Alexander S.; Fedorova, Anna A.; Kuroda, Takeshi; Hartogh, Paul
2018-02-01
We present a new implementation of the hydrological cycle scheme into a general circulation model of the Martian atmosphere. The model includes a semi-Lagrangian transport scheme for water vapor and ice and accounts for microphysics of phase transitions between them. The hydrological scheme includes processes of saturation, nucleation, particle growth, sublimation, and sedimentation under the assumption of a variable size distribution. The scheme has been implemented into the Max Planck Institute Martian general circulation model and tested assuming monomodal and bimodal lognormal distributions of ice condensation nuclei. We present a comparison of the simulated annual variations, horizontal and vertical distributions of water vapor, and ice clouds with the available observations from instruments on board Mars orbiters. The accounting for bimodality of aerosol particle distribution improves the simulations of the annual hydrological cycle, including predicted ice clouds mass, opacity, number density, and particle radii. The increased number density and lower nucleation rates bring the simulated cloud opacities closer to observations. Simulations show a weak effect of the excess of small aerosol particles on the simulated water vapor distributions.
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Directory of Open Access Journals (Sweden)
H.-W. Wong
2013-10-01
Full Text Available Contrails and contrail-induced cirrus clouds are identified as the most uncertain components in determining aviation impacts on global climate change. Parameters affecting contrail ice particle formation immediately after the engine exit plane (< 5 s in plume age may be critical to ice particle properties used in large-scale models predicting contrail radiative forcing. Despite this, detailed understanding of these parametric effects is still limited. In this paper, we present results from recent laboratory and modeling studies conducted to investigate the effects of water and soot emissions and ambient conditions on near-field formation of contrail ice particles and ice particle properties. The Particle Aerosol Laboratory (PAL at the NASA Glenn Research Center and the Aerodyne microphysical parcel model for contrail ice particle formation were employed. Our studies show that exhaust water concentration has a significant impact on contrail ice particle formation and properties. When soot particles were introduced, ice particle formation was observed only when exhaust water concentration was above a critical level. When no soot or sulfuric acid was introduced, no ice particle formation was observed, suggesting that ice particle formation from homogeneous nucleation followed by homogeneous freezing of liquid water was unfavorable. Soot particles were found to compete for water vapor condensation, and higher soot concentrations emitted into the chamber resulted in smaller ice particles being formed. Chamber conditions corresponding to higher cruising altitudes were found to favor ice particle formation. The microphysical model captures trends of particle extinction measurements well, but discrepancies between the model and the optical particle counter measurements exist as the model predicts narrower ice particle size distributions and ice particle sizes nearly a factor of two larger than measured. These discrepancies are likely due to particle
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Energy Technology Data Exchange (ETDEWEB)
Ni, Yicun; Skinner, J. L. [Theoretical Chemistry Institute and Department of Chemistry, University of Wisconsin, Madison, Wisconsin 53706 (United States)
2016-06-07
Supercooled water exhibits many thermodynamic anomalies, and several scenarios have been proposed to interpret them, among which the liquid-liquid critical point (LLCP) hypothesis is the most commonly discussed. We investigated Widom lines and the LLCP of deeply supercooled water, by using molecular dynamics simulation with a newly reparameterized water model that explicitly includes three-body interactions. Seven isobars are studied from ambient pressure to 2.5 kbar, and Widom lines are identified by calculating maxima in the coefficient of thermal expansion and the isothermal compressibility (both with respect to temperature). From these data we estimate that the LLCP of the new water model is at 180 K and 2.1 kbar. The oxygen radial distribution function is calculated along the 2 kbar isobar. It shows a steep change in the height of its second peak between 180 and 185 K, which indicates a transition between the high-density liquid and low-density liquid phases and which is consistent with the ascribed location of the critical point. The good agreement of the height of the second peak of the radial distribution function between simulation and experiment at 1 bar, as a function of temperature, supports the validity of the model. The location of the LLCP within the model is close to the kink in the experimental homogeneous nucleation line. We use existing experimental data to argue that the experimental LLCP is at 168 K and 1.95 kbar and speculate how this LLCP and its Widom line might be responsible for the kink in the homogeneous nucleation line.
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Effect of particle surface area on ice active site densities retrieved from droplet freezing spectra
Directory of Open Access Journals (Sweden)
H. Beydoun
2016-10-01
Full Text Available 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
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Betancourt, R. Morales; Lee, D.; Oreopoulos, L.; Sud, Y. C.; Barahona, D.; Nenes, A.
2012-01-01
The salient features of mixed-phase and ice clouds in a GCM cloud scheme are examined using the ice formation parameterizations of Liu and Penner (LP) and Barahona and Nenes (BN). The performance of LP and BN ice nucleation parameterizations were assessed in the GEOS-5 AGCM using the McRAS-AC cloud microphysics framework in single column mode. Four dimensional assimilated data from the intensive observation period of ARM TWP-ICE campaign was used to drive the fluxes and lateral forcing. Simulation experiments where established to test the impact of each parameterization in the resulting cloud fields. Three commonly used IN spectra were utilized in the BN parameterization to described the availability of IN for heterogeneous ice nucleation. The results show large similarities in the cirrus cloud regime between all the schemes tested, in which ice crystal concentrations were within a factor of 10 regardless of the parameterization used. In mixed-phase clouds there are some persistent differences in cloud particle number concentration and size, as well as in cloud fraction, ice water mixing ratio, and ice water path. Contact freezing in the simulated mixed-phase clouds contributed to transfer liquid to ice efficiently, so that on average, the clouds were fully glaciated at T approximately 260K, irrespective of the ice nucleation parameterization used. Comparison of simulated ice water path to available satellite derived observations were also performed, finding that all the schemes tested with the BN parameterization predicted 20 average values of IWP within plus or minus 15% of the observations.
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Arctic sea ice melt leads to atmospheric new particle formation.
Dall Osto, M; Beddows, D C S; Tunved, P; Krejci, R; Ström, J; Hansson, H-C; Yoon, Y J; Park, Ki-Tae; Becagli, S; Udisti, R; Onasch, T; O Dowd, C D; Simó, R; Harrison, Roy M
2017-06-12
Atmospheric new particle formation (NPF) and growth significantly influences climate by supplying new seeds for cloud condensation and brightness. Currently, there is a lack of understanding of whether and how marine biota emissions affect aerosol-cloud-climate interactions in the Arctic. Here, the aerosol population was categorised via cluster analysis of aerosol size distributions taken at Mt Zeppelin (Svalbard) during a 11 year record. The daily temporal occurrence of NPF events likely caused by nucleation in the polar marine boundary layer was quantified annually as 18%, with a peak of 51% during summer months. Air mass trajectory analysis and atmospheric nitrogen and sulphur tracers link these frequent nucleation events to biogenic precursors released by open water and melting sea ice regions. The occurrence of such events across a full decade was anti-correlated with sea ice extent. New particles originating from open water and open pack ice increased the cloud condensation nuclei concentration background by at least ca. 20%, supporting a marine biosphere-climate link through sea ice melt and low altitude clouds that may have contributed to accelerate Arctic warming. Our results prompt a better representation of biogenic aerosol sources in Arctic climate models.
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Analysis of supercooling activity of tannin-related polyphenols.
Kuwabara, Chikako; Wang, Donghui; Endoh, Keita; Fukushi, Yukiharu; Arakawa, Keita; Fujikawa, Seizo
2013-08-01
Based on the discovery of novel supercooling-promoting hydrolyzable gallotannins from deep supercooling xylem parenchyma cells (XPCs) in Katsura tree (see Wang et al. (2012) [38]), supercooling capability of a wide variety of tannin-related polyphenols (TRPs) was examined in order to find more effective supercooling-promoting substances for their applications. The TRPs examined were single compounds including six kinds of hydrolyzable tannins, 11 kinds of catechin derivatives, two kinds of structural analogs of catechin and six kinds of phenolcarboxylic acid derivatives, 11 kinds of polyphenol mixtures and five kinds of crude plant tannin extracts. The effects of these TRPs on freezing were examined by droplet freezing assays using various solutions containing different kinds of identified ice nucleators such as the ice nucleation bacterium (INB) Erwinia ananas, the INB Xanthomonas campestris, silver iodide and phloroglucinol as well as a solution containing only unintentionally included unidentified airborne ice nucleators. Among the 41 kinds of TRPs examined, all of the hydrolyzable tannins, catechin derivatives, polyphenol mixtures and crude plant tannin extracts as well as a few structural analogs of catechin and phenolcarboxylic acid derivatives exhibited supercooling-promoting activity (SCA) with significant differences (p>0.05) from at least one of the solutions containing different kinds of ice nucleators. It should be noted that there were no TRPs exhibiting ice nucleation-enhancing activity (INA) in all solutions containing identified ice nucleators, whereas there were many TRPs exhibiting INA with significant differences in solutions containing unidentified ice nucleators alone. An emulsion freezing assay confirmed that these TRPs did not essentially affect homogeneous ice nucleation temperatures. It is thought that not only SCA but also INA in the TRPs are produced by interactions with heterogeneous ice nucleators, not by direct interaction with water
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Possible influence of anthropogenic aerosols on cirrus clouds and anthropogenic forcing
Directory of Open Access Journals (Sweden)
J. E. Penner
2009-02-01
Full Text Available Cirrus clouds have a net warming effect on the atmosphere and cover about 30% of the Earth's area. Aerosol particles initiate ice formation in the upper troposphere through modes of action that include homogeneous freezing of solution droplets, heterogeneous nucleation on solid particles immersed in a solution, and deposition nucleation of vapor onto solid particles. Here, we examine the possible change in ice number concentration from anthropogenic soot originating from surface sources of fossil fuel and biomass burning, from anthropogenic sulfate aerosols, and from aircraft that deposit their aerosols directly in the upper troposphere. We use a version of the aerosol model that predicts sulfate number and mass concentrations in 3-modes and includes the formation of sulfate aerosol through homogeneous binary nucleation as well as a version that only predicts sulfate mass. The 3-mode version best represents the Aitken aerosol nuclei number concentrations in the upper troposphere which dominated ice crystal residues in the upper troposphere. Fossil fuel and biomass burning soot aerosols with this version exert a radiative forcing of −0.3 to −0.4 Wm−2 while anthropogenic sulfate aerosols and aircraft aerosols exert a forcing of −0.01 to 0.04 Wm−2 and −0.16 to −0.12 Wm−2, respectively, where the range represents the forcing from two parameterizations for ice nucleation. The sign of the forcing in the mass-only version of the model depends on which ice nucleation parameterization is used and can be either positive or negative. The magnitude of the forcing in cirrus clouds can be comparable to the forcing exerted by anthropogenic aerosols on warm clouds, but this forcing has not been included in past assessments of the total anthropogenic radiative forcing of climate.
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First passage times in homogeneous nucleation: Dependence on the total number of particles
International Nuclear Information System (INIS)
Yvinec, Romain; Bernard, Samuel; Pujo-Menjouet, Laurent; Hingant, Erwan
2016-01-01
Motivated by nucleation and molecular aggregation in physical, chemical, and biological settings, we present an extension to a thorough analysis of the stochastic self-assembly of a fixed number of identical particles in a finite volume. We study the statistics of times required for maximal clusters to be completed, starting from a pure-monomeric particle configuration. For finite volumes, we extend previous analytical approaches to the case of arbitrary size-dependent aggregation and fragmentation kinetic rates. For larger volumes, we develop a scaling framework to study the first assembly time behavior as a function of the total quantity of particles. We find that the mean time to first completion of a maximum-sized cluster may have a surprisingly weak dependence on the total number of particles. We highlight how higher statistics (variance, distribution) of the first passage time may nevertheless help to infer key parameters, such as the size of the maximum cluster. Finally, we present a framework to quantify formation of macroscopic sized clusters, which are (asymptotically) very unlikely and occur as a large deviation phenomenon from the mean-field limit. We argue that this framework is suitable to describe phase transition phenomena, as inherent infrequent stochastic processes, in contrast to classical nucleation theory
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Hoyle, C. R.; Engel, I.; Luo, B. P.; Pitts, M. C.; Poole, L. R.; Grooss, J.-U.; Peter, T.
2013-01-01
Satellite-based observations during the Arctic winter of 2009/2010 provide firm evidence that, in contrast to the current understanding, the nucleation of nitric acid trihydrate (NAT) in the polar stratosphere does not only occur on preexisting ice particles. In order to explain the NAT clouds observed over the Arctic in mid-December 2009, a heterogeneous nucleation mechanism is required, occurring via immersion freezing on the surface of solid particles, likely of meteoritic origin. For the first time, a detailed microphysical modelling of this NAT formation pathway has been carried out. Heterogeneous NAT formation was calculated along more than sixty thousand trajectories, ending at Cloud Aerosol Lidar with Orthogonal Polarization (CALIOP) observation points. Comparing the optical properties of the modelled NAT with these observations enabled a thorough validation of a newly developed NAT nucleation parameterisation, which has been built into the Zurich Optical and Microphysical box Model (ZOMM). The parameterisation is based on active site theory, is simple to implement in models and provides substantial advantages over previous approaches which involved a constant rate of NAT nucleation in a given volume of air. It is shown that the new method is capable of reproducing observed polar stratospheric clouds (PSCs) very well, despite the varied conditions experienced by air parcels travelling along the different trajectories. In a companion paper, ZOMM is applied to a later period of the winter, when ice PSCs are also present, and it is shown that the observed PSCs are also represented extremely well under these conditions.
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Stick-slip Cycles and Tidal Modulation of Ice Stream Flow
Lipovsky, B.; Dunham, E. M.
2016-12-01
The reactivation of a single dormant Antarctic ice stream would double the continent's mass imbalance. Despite importance of understanding the likelihood of such an event, direct observation of the basal processes that lead to the activation and stagnation of streaming ice are minimal. As the only ice stream undergoing stagnation, the Whillans Ice Plain (WIP) occupies a central role in our understanding of these subglacial processes. Complicating matters is the observation, from GPS records, that the WIP experiences most of its motion during episodes of rapid sliding. These sliding events are tidally modulated and separated by 12 hour periods of quiescence. We conduct numerical simulations of ice stream stick-slip cycles. Our simulations include rate- and state-dependent frictional sliding, tidal forcing, inertia, upstream loading in a cross-stream, thickness-averaged formulation. Our principal finding is that ice stream motion may respond to ocean tidal forcing with one of two end member behaviors. In one limit, tidally modulated slip events have rupture velocities that approach the shear wave speed and slip events have a duration that scales with the ice stream width divided by the shear wave speed. In the other limit, tidal modulation results in ice stream sliding velocities with lower amplitude variation but at much longer timescales, i.e. semi-diurnal and longer. This latter behavior more closely mimics the behavior of several active ice streams (Bindschadler, Rutford). We find that WIP slip events exist between these two end member behaviors: rupture velocities are far below the inertial limit yet sliding occurs only episodically. The continuum of sliding behaviors is governed by a critical ice stream width over which slip event nucleate. When the critical width is much longer than the ice stream width, slip events are unable to nucleate. The critical width depends on the subglacial effective pressure, ice thickness, and frictional and elastic constitutive
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STABLE ISOTOPE GEOCHEMISTRY OF MASSIVE ICE
Directory of Open Access Journals (Sweden)
Yurij K. Vasil’chuk
2016-01-01
Full Text Available The paper summarises stable-isotope research on massive ice in the Russian and North American Arctic, and includes the latest understanding of massive-ice formation. A new classification of massive-ice complexes is proposed, encompassing the range and variabilityof massive ice. It distinguishes two new categories of massive-ice complexes: homogeneousmassive-ice complexes have a similar structure, properties and genesis throughout, whereasheterogeneous massive-ice complexes vary spatially (in their structure and properties andgenetically within a locality and consist of two or more homogeneous massive-ice bodies.Analysis of pollen and spores in massive ice from Subarctic regions and from ice and snow cover of Arctic ice caps assists with interpretation of the origin of massive ice. Radiocarbon ages of massive ice and host sediments are considered together with isotope values of heavy oxygen and deuterium from massive ice plotted at a uniform scale in order to assist interpretation and correlation of the ice.
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Rainfall drives atmospheric ice-nucleating particles in the coastal climate of southern Norway
Directory of Open Access Journals (Sweden)
F. Conen
2017-09-01
Full Text Available Ice-nucleating particles (INPs active at modest supercooling (e.g. −8 °C; INP−8 can transform clouds from liquid to mixed phase, even at very small number concentrations (< 10 m−3. Over the course of 15 months, we found very similar patterns in weekly concentrations of INP−8 in PM10 (median = 1.7 m−3, maximum = 10.1 m−3 and weekly amounts of rainfall (median = 28 mm, maximum = 153 mm at Birkenes, southern Norway. Most INP−8 were probably aerosolised locally by the impact of raindrops on plant, litter and soil surfaces. Major snowfall and heavy rain onto snow-covered ground were not mirrored by enhanced numbers of INP−8. Further, transport model calculations for large (> 4 m−3 and small (< 4 m−3 numbers of INP−8 revealed that potential source regions likely to provide precipitation to southern Norway were associated with large numbers of INP−8. The proportion of land cover and land use type in potential source regions was similar for large and small numbers of INP−8. In PM2. 5 we found consistently about half as many INP−8 as in PM10. From mid-May to mid-September, INP−8 correlated positively with the fungal spore markers arabitol and mannitol, suggesting that some fraction of INP−8 during that period may consist of fungal spores. In the future, warmer winters with more rain instead of snow may enhance airborne concentrations of INP−8 during the cold season in southern Norway and in other regions with a similar climate.
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Nucleation Characteristics in Physical Experiments/explosions
International Nuclear Information System (INIS)
Henry, R.E.; Fauske, Hans K.
1976-01-01
Large-scale vapor explosion experiments have shown that intimate contact between hot and cold liquids, and a temperature upon contact that is greater than the spontaneous nucleation temperature of the system, are two necessary conditions for the onset of large scale vapor explosions. A model, based on spontaneous nucleation of the homogeneous type, has been proposed to describe the relevant processes and the resulting energetics for explosive boiling systems. The model considers that spontaneous nucleation cannot occur either during the relief time for constant volume heating or until the thermal boundary layer is sufficiently thick to support a vapor cavity of the critical size. After nucleation, bubble growth does not occur until an acoustic wave establishes a pressure gradient in the cold liquid. These considerations lead to the prediction that, for a given temperature, drops greater than a critical size will remain in film boiling due to coalescence of vapor nuclei and drops smaller than this value will wet and be captured by the hot liquid surface. These results are compared to small drop data for well-wetted systems and excellent agreement is obtained between the observed behavior and the model predictions. In conclusion: A model, based on spontaneous nucleation, has been proposed to describe vaporization potential and behavior upon contact in a liquid/liquid system. This behavior is determined by the size of the liquid mass, single-phase pressurization and acoustic relief, nucleation frequency due to random density fluctuations, the initiation of unstable growth and acoustic relief, and the development of the thermal boundary layer in the cold liquid. The proposed model predicts that the stability of a given size drop upon intimate contact with another liquid is extremely dependent upon the interface temperature. For low interface temperatures, large masses will be captured by the hot liquid and the resulting vaporization rates will be extremely low because
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Dumitrescu, Lucia R.; Smeulders, David M.J.; Dam, Jacques A.M.; Gaastra-Nedea, Silvia V.
2017-01-01
Molecular dynamics (MD) simulations were conducted to study nucleation of water at 350 K in argon using TIP4P and TIP4P/2005 water models. We found that the stability of any cluster, even if large, strongly depends on the energetic interactions with its vicinity, while the stable clusters change
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Kinetics of heterogeneous nucleation on intrinsic nucleants in pure fcc transition metals
International Nuclear Information System (INIS)
Wilde, G; Bokeloh, J; Santhaweesuk, C; Perepezko, J H; Sebright, J L
2009-01-01
Nucleation during solidification is heterogeneous in nature in an overwhelmingly large fraction of all solidification events. Yet, most often the identity of the heterogeneous nucleants that initiate nucleation remains a matter of speculation. In fact, a series of dedicated experiments needs to be designed in order to verify if nucleation of the material under study is based on one type of heterogeneous nucleant and if the potency of that nucleant is constant, e.g. for a population of individual droplets, or stays constant over time, e.g. throughout repeated melting/solidification cycles. In this work it is demonstrated that one way to circumvent ambiguities and analyze nucleation kinetics under well-defined conditions experimentally is given by performing statistically significant numbers of repeated single-droplet experiments. The application of proper statistics analyses based upon a non-homogeneous Poisson process is shown to yield nucleation rates that are independent of a specific nucleation model. Based upon this approach nucleation undercooling measurements on pure Au, Cu and Ni as model materials have confirmed that the experimental strategy and analysis method are valid. The results are comparable to those obtained by classical nucleation theory applied to experimental data that has been verified to comply with the assertions that are necessary for applying this model framework. However, the results reveal also other complex nucleant-sample interactions such as an initial transient undercooling behavior and impurity removal during repeated cycling treatments. The transient undercooling behavior has been analyzed by a nucleant refining model to provide new insight on the operation of melt fluxing treatments.
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Experimental Study on Ice Forming Process of Cryogenic Liquid Releasing underwater
Zhang, Bin; Wu, Wanqing; Zhang, Xingdong; Zhang, Yi; Zhang, Chuanlin; Zhang, Haoran; Wang, Peng
2017-11-01
Cryogenic liquid releasing into water would be a process combines hyperactive boiling with ice forming. There are still few researches on the experimental study on the environmental conditions for deciding ice forming speed and liquid surviving state. In this paper, to advance our understanding of ice forming deciding factors in the process of LN2 releasing underwater, a visualization experimental system is built. The results show that the pressure difference significantly influences the ice forming speed and liquid surviving distance, which is observed by the experiment and theoretically analysed by Kelvin-Helmholtz instability. Adding nucleating agent is helpful to provide ice nucleus which can accelerate the ice forming speed. Water flowing has some effect on changing pressure difference, which can affect the ice forming speed and liquid surviving distance.
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Nucleation of super-critical carbon dioxide in a venturi nozzle
Energy Technology Data Exchange (ETDEWEB)
Jarrahbashi, D., E-mail: dorrin.jarrahbashi@me.gatech.edu; Pidaparti, S.R.; Ranjan, D.
2016-12-15
Highlights: • Nucleation of S-CO{sub 2} in a nozzle near critical point has been computationally studied. • The nucleation behavior is very sensitive to the inlet pressure and temperature. • After nucleation, high liquid-content two-phase mixture near wall travels downstream. - Abstract: Pressure reduction at the entrance of the compressor in supercritical CO{sub 2} Brayton cycles may cause nucleation and create a mixture of vapor and liquid droplets due to operation near the saturation conditions. Transient behavior of the flow after nucleation may cause serious issues in operation of the cycle and degrade the materials used in the design. The nucleation behavior of supercritical carbon-dioxide inside a venturi nozzle near the critical point is computationally studied. A transient compressible 3D Navier–Stokes solver, coupled with continuity, and energy equations have been implemented. In order to expedite the simulations, Fluid property Interpolation Tables (FIT) based on a piecewise biquintic spline interpolation of Helmholtz energy have been integrated with OpenFOAM to model S-CO{sub 2} properties. The mass fraction of vapor created in the venturi nozzle has been calculated using homogeneous equilibrium model (HEM). Nucleation behavior has been shown to be very sensitive to the inlet pressure, inlet temperature, and flow rate. The flow conditions that led to nucleation were identified. Nucleation was observed in the throat area and divergent section of the nozzle for mass flow rates from 0.050 kg/s to 0.065 kg/s, inlet pressure from 7.8 to 7.4 MPa for fixed exit pressure equal to 7.28 MPa. The inception of high-vapor-content nucleation was first observed in the throat area away from the side walls that remained confined to the throat region in later times. However, near the walls, a high liquid-content two-phase region was detected, first in the divergent section. At later times, the two-phase region was convected downstream toward the nozzle exit
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Effects of homogeneous condensation in compressible flows: Ludwieg-tube experiments and simulations
Luo, X.; Lamanna, G.; Holten, A.P.C.; Dongen, van M.E.H.
2007-01-01
Effects of homogeneous nucleation and subsequent droplet growth in compressible flows in humid nitrogen are investigated numerically and exptl. A Ludwieg tube is employed to produce expansion flows. Corresponding to different configurations, three types of expt. are carried out in such a tube.
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Directory of Open Access Journals (Sweden)
J.-F. Gayet
2012-01-01
IWC up to 1 g m−3 may be observed near the cloud top. Extrapolating the relationship for stronger convective clouds with similar ice particles, IWC up to 5 g m−3 could be experienced with reflectivity factors no larger than about 20 dBZ. This means that for similar situations, indication of rather weak radar echo does not necessarily warn the occurrence of high ice water content carried by small ice crystals. All along the cloud penetration the shape of the ice crystals is dominated by chain-like aggregates of frozen droplets. Our results confirm previous observations that the chains of ice crystals are found in a continental deep convective systems which are known generally to generate intense electric fields causing efficient ice particle aggregation processes. Vigorous updrafts could lift supercooled droplets which are frozen extremely rapidly by homogeneous nucleation near the −37 °C level, producing therefore high concentrations of very small ice particles at upper altitudes. They are sufficient to deplete the water vapour and suppress further nucleation as confirmed by humidity measurements. These observations address scientific issues related to the microphysical properties and structure of deep convective clouds and confirm that particles smaller than 50 μm may control the radiative properties in convective-related clouds. These unusual observations may also provide some possible insights regarding engineering issues related to the failure of jet engines commonly used on commercial aircraft during flights through areas of high ice water content. However, large uncertainties of the measured and derived parameters limit our observations.
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Gayet, J.-F.; Mioche, G.; Bugliaro, L.; Protat, A.; Minikin, A.; Wirth, M.; Dörnbrack, A.; Shcherbakov, V.; Mayer, B.; Garnier, A.; Gourbeyre, C.
2012-01-01
. Extrapolating the relationship for stronger convective clouds with similar ice particles, IWC up to 5 g m-3 could be experienced with reflectivity factors no larger than about 20 dBZ. This means that for similar situations, indication of rather weak radar echo does not necessarily warn the occurrence of high ice water content carried by small ice crystals. All along the cloud penetration the shape of the ice crystals is dominated by chain-like aggregates of frozen droplets. Our results confirm previous observations that the chains of ice crystals are found in a continental deep convective systems which are known generally to generate intense electric fields causing efficient ice particle aggregation processes. Vigorous updrafts could lift supercooled droplets which are frozen extremely rapidly by homogeneous nucleation near the -37 °C level, producing therefore high concentrations of very small ice particles at upper altitudes. They are sufficient to deplete the water vapour and suppress further nucleation as confirmed by humidity measurements. These observations address scientific issues related to the microphysical properties and structure of deep convective clouds and confirm that particles smaller than 50 μm may control the radiative properties in convective-related clouds. These unusual observations may also provide some possible insights regarding engineering issues related to the failure of jet engines commonly used on commercial aircraft during flights through areas of high ice water content. However, large uncertainties of the measured and derived parameters limit our observations.
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Physical and chemical characterization of bioaerosols - Implications for nucleation processes
Ariya, P. A.; Sun, J.; Eltouny, N. A.; Hudson, E. D.; Hayes, C. T.; Kos, G.
The importance of organic compounds in the oxidative capacity of the atmosphere, and as cloud condensation and ice-forming nuclei, has been recognized for several decades. Organic compounds comprise a significant fraction of the suspended matter mass, leading to local (e.g. toxicity, health hazards) and global (e.g. climate change) impacts. The state of knowledge of the physical chemistry of organic aerosols has increased during the last few decades. However, due to their complex chemistry and the multifaceted processes in which they are involved, the importance of organic aerosols, particularly bioaerosols, in driving physical and chemical atmospheric processes is still very uncertain and poorly understood. Factors such as solubility, surface tension, chemical impurities, volatility, morphology, contact angle, deliquescence, wettability, and the oxidation process are pivotal in the understanding of the activation processes of cloud droplets, and their chemical structures, solubilities and even the molecular configuration of the microbial outer membrane, all impact ice and cloud nucleation processes in the atmosphere. The aim of this review paper is to assess the current state of knowledge regarding chemical and physical characterization of bioaerosols with a focus on those properties important in nucleation processes. We herein discuss the potential importance (or lack thereof) of physical and chemical properties of bioaerosols and illustrate how the knowledge of these properties can be employed to study nucleation processes using a modeling exercise. We also outline a list of major uncertainties due to a lack of understanding of the processes involved or lack of available data. We will also discuss key issues of atmospheric significance deserving future physical chemistry research in the fields of bioaerosol characterization and microphysics, as well as bioaerosol modeling. These fundamental questions are to be addressed prior to any definite conclusions on the
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Lamellipodia nucleation by filopodia depends on integrin occupancy and downstream Rac1 signaling
International Nuclear Information System (INIS)
Guillou, Herve; Depraz-Depland, Adeline; Planus, Emmanuelle; Vianay, Benoit; Chaussy, Jacques; Grichine, Alexei; Albiges-Rizo, Corinne; Block, Marc R.
2008-01-01
Time-lapse video-microscopy unambiguously shows that fibroblast filopodia are the scaffold of lamellipodia nucleation that allows anisotropic cell spreading. This process was dissected into elementary stages by monitoring cell adhesion on micropatterned extracellular matrix arrays of various pitches. Adhesion structures are stabilized by contact with the adhesive plots and subsequently converted into lamellipodia-like extensions starting at the filopodia tips. This mechanism progressively leads to full cell spreading. Stable expression of the dominant-negative Rac1 N17 impairs this change in membrane extension mode and stops cell spreading on matrix arrays. Similar expression of the dominant-negative Cdc42 N17 impairs cell spreading on homogenous and structured substrate, suggesting that filopodia extension is a prerequisite for cell spreading in this model. The differential polarity of the nucleation of lamellipodial structures by filopodia on homogenous and structured surfaces starting from the cell body and of filopodia tip, respectively, suggested that this process is triggered by areas that are in contact with extracellular matrix proteins for longer times. Consistent with this view, wild-type cells cannot spread on microarrays made of function blocking or neutral anti-β 1 integrin antibodies. However, stable expression of a constitutively active Rac1 mutant rescues the cell ability to spread on these integrin microarrays. Thereby, lamellipodia nucleation by filopodia requires integrin occupancy by matrix substrate and downstream Rac1 signaling
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International Nuclear Information System (INIS)
Bove, L.E.
2009-01-01
Full text: It is widely accepted that ice, no matter what phase, is unable to incorporate large amount of salt into its structure. This conclusion is based on the observation that upon freezing of saltwater, ice expels the salt almost entirely into brine, a fact which can be exploited to desalinate seawater. Here we show, by neutron diffraction under high pressure, that this behaviour is not an intrinsic physico-chemical property of ice phases. We demonstrate that substantial am mounts of dissolved LiCl can be built homogeneously into the ice VII structure if it is produced by recrystallisation of its glassy state under pressure [1]. Such highly doped or alloyed ice VII has significantly different structural properties compared to pure ice VII, such as a 8% larger unit cell volume, 5 times larger displacement factors, an absence of a transition to an ordered ice VIII structure, plasticity, and most likely ionic conductivity. Our study suggests that there could be a whole new class of salty ices based on various kinds of solutes and high pressure ice forms. (author)
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A note on the nucleation with multiple steps: Parallel and series nucleation
Iwamatsu, Masao
2012-01-01
Parallel and series nucleation are the basic elements of the complex nucleation process when two saddle points exist on the free-energy landscape. It is pointed out that the nucleation rates follow formulas similar to those of parallel and series connection of resistors or conductors in an electric circuit. Necessary formulas to calculate individual nucleation rates at the saddle points and the total nucleation rate are summarized and the extension to the more complex nucleation process is su...
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Thermally activated vapor bubble nucleation: The Landau-Lifshitz-Van der Waals approach
Gallo, Mirko; Magaletti, Francesco; Casciola, Carlo Massimo
2018-05-01
Vapor bubbles are formed in liquids by two mechanisms: evaporation (temperature above the boiling threshold) and cavitation (pressure below the vapor pressure). The liquid resists in these metastable (overheating and tensile, respectively) states for a long time since bubble nucleation is an activated process that needs to surmount the free energy barrier separating the liquid and the vapor states. The bubble nucleation rate is difficult to assess and, typically, only for extremely small systems treated at an atomistic level of detail. In this work a powerful approach, based on a continuum diffuse interface modeling of the two-phase fluid embedded with thermal fluctuations (fluctuating hydrodynamics), is exploited to study the nucleation process in homogeneous conditions, evaluating the bubble nucleation rates and following the long-term dynamics of the metastable system, up to the bubble coalescence and expansion stages. In comparison with more classical approaches, this methodology allows us on the one hand to deal with much larger systems observed for a much longer time than possible with even the most advanced atomistic models. On the other, it extends continuum formulations to thermally activated processes, impossible to deal with in a purely determinist setting.
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A note on the nucleation with multiple steps: parallel and series nucleation.
Iwamatsu, Masao
2012-01-28
Parallel and series nucleation are the basic elements of the complex nucleation process when two saddle points exist on the free-energy landscape. It is pointed out that the nucleation rates follow formulas similar to those of parallel and series connection of resistors or conductors in an electric circuit. Necessary formulas to calculate individual nucleation rates at the saddle points and the total nucleation rate are summarized, and the extension to the more complex nucleation process is suggested. © 2012 American Institute of Physics
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Properties of liquid clusters in large-scale molecular dynamics nucleation simulations
International Nuclear Information System (INIS)
Angélil, Raymond; Diemand, Jürg; Tanaka, Kyoko K.; Tanaka, Hidekazu
2014-01-01
We have performed large-scale Lennard-Jones molecular dynamics simulations of homogeneous vapor-to-liquid nucleation, with 10 9 atoms. This large number allows us to resolve extremely low nucleation rates, and also provides excellent statistics for cluster properties over a wide range of cluster sizes. The nucleation rates, cluster growth rates, and size distributions are presented in Diemand et al. [J. Chem. Phys. 139, 74309 (2013)], while this paper analyses the properties of the clusters. We explore the cluster temperatures, density profiles, potential energies, and shapes. A thorough understanding of the properties of the clusters is crucial to the formulation of nucleation models. Significant latent heat is retained by stable clusters, by as much as ΔkT = 0.1ε for clusters with size i = 100. We find that the clusters deviate remarkably from spherical—with ellipsoidal axis ratios for critical cluster sizes typically within b/c = 0.7 ± 0.05 and a/c = 0.5 ± 0.05. We examine cluster spin angular momentum, and find that it plays a negligible role in the cluster dynamics. The interfaces of large, stable clusters are thinner than planar equilibrium interfaces by 10%−30%. At the critical cluster size, the cluster central densities are between 5% and 30% lower than the bulk liquid expectations. These lower densities imply larger-than-expected surface areas, which increase the energy cost to form a surface, which lowers nucleation rates
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Pulsed ion-beam induced nucleation and growth of Ge nanocrystals on SiO2
International Nuclear Information System (INIS)
Stepina, N. P.; Dvurechenskii, A. V.; Armbrister, V. A.; Kesler, V. G.; Novikov, P. L.; Gutakovskii, A. K.; Kirienko, V. V.; Smagina, Zh. V.; Groetzschel, R.
2007-01-01
Pulsed low-energy (200 eV) ion-beam induced nucleation during Ge deposition on thin SiO 2 film was used to form dense homogeneous arrays of Ge nanocrystals. The ion-beam action is shown to stimulate the nucleation of Ge nanocrystals when being applied after thin Ge layer deposition. Temperature and flux variation was used to optimize the nanocrystal size and array density required for memory device. Kinetic Monte Carlo simulation shows that ion impacts open an additional channel of atom displacement from a nanocrystal onto SiO 2 surface. This results both in a decrease in the average nanocrystal size and in an increase in nanocrystal density
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High density amorphous ice and its phase transition to ice XII
International Nuclear Information System (INIS)
Kohl, I.
2001-07-01
1998 Lobban et al. reported the neutron diffraction data of a new phase of ice, called ice XII, which formed at 260 K on compression of water within the domain of ice V at a pressure of 0.5 GPa. Surprisingly ice XII forms as an incidental product in the preparation of high-density amorphous ice (HDA) on compression of hexagonale ice (ice Ih) at 77 K up to pressures = 1.3 GPa. A decisive experimental detail is the use of an indium container: when compressing ice Ih in a pressure vessel with indium linings, then reproducibly HDA (high density amorphous ice) forms, but without indium randomly scattered relative amounts of ice XII and HDA form. Ice XII forms on compression of ice Ih at 77 K only via HDA, and not directly from ice Ih. Its formation requires a sudden pronounced apparent pressure drop of ca 0.18 GPa at pressures ca 1.1 GPa. These apparent pressure drops can be caused by buildup friction between the piston and the pressure vessel and its sudden release on further compression. I propose that shock-waves generated by apparent pressure drops cause transient local heating and that this induces nucleation and crystal growth. A specific reproducible method to prepare ice XII is heating HDA in a pressure vessel with indium linings at constant pressures (or constant volume). The ice XII (meta-)stability domain extends between ca 158 and 212 K from ca 0.7 to ca 1.5 GPa. DSC (differential scanning calorimetry) and x-ray powder diffraction revealed, that on heating at atmospheric pressure ice XII transforms directly into cubic ice (ice Ic) at 154 K (heating rate 10 K min - 1) and not into an amorphous form before transition to ice Ic. The enthalpy of the ice XII - ice Ic transition is -1.21 ± 0.07 kJ mol -1 . An estimation of the Gibbs free energy at atmospheric pressure and about 140 K results that ice XII is thermodynamically more stable than ice VI. In the heating curve of ice XII a reversible endothermic step can be found at the onset temperature (heating rate
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Li, Ruipeng
2012-09-04
A new way to investigate and control the growth of solution-cast thin films is presented. The combination of in situ quartz crystal microbalance measurements with dissipation capabilities (QCM-D) and in situ grazing-incidence wide-angle X-ray scattering (GIWAXS) in an environmental chamber provides unique quantitative insights into the time-evolution of the concentration of the solution, the onset of nucleation, and the mode of growth of the organic semiconductor under varied drying conditions. It is demonstrated that careful control over the kinetics of solution drying enhances carrier transport significantly by promoting phase transformation predominantly via heterogeneous nucleation and sustained surface growth of a highly lamellar structure at the solid-liquid interface at the expense of homogeneous nucleation. A new way to investigate and control the growth of drop-cast thin films is presented. The solution-processing of small-molecule thin films of TIPS-pentacene is investigated using time-resolved techniques to reveal the mechanisms of nucleation and growth leading to solid film formation. By tuning the drying speed of the solution, the balance between surface and bulk growth modes is altered, thereby controlling the lamellar formation and tuning the carrier mobility in organic field-effect transistors Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
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Aerosol-cloud interactions in Arctic mixed-phase stratocumulus
Solomon, A.
2017-12-01
Reliable climate projections require realistic simulations of Arctic cloud feedbacks. Of particular importance is accurately simulating Arctic mixed-phase stratocumuli (AMPS), which are ubiquitous and play an important role in regional climate due to their impact on the surface energy budget and atmospheric boundary layer structure through cloud-driven turbulence, radiative forcing, and precipitation. AMPS are challenging to model due to uncertainties in ice microphysical processes that determine phase partitioning between ice and radiatively important cloud liquid water. Since temperatures in AMPS are too warm for homogenous ice nucleation, ice must form through heterogeneous nucleation. In this presentation we discuss a relatively unexplored source of ice production-recycling of ice nuclei in regions of ice subsaturation. AMPS frequently have ice-subsaturated air near the cloud-driven mixed-layer base where falling ice crystals can sublimate, leaving behind IN. This study provides an idealized framework to understand feedbacks between dynamics and microphysics that maintain phase-partitioning in AMPS. In addition, the results of this study provide insight into the mechanisms and feedbacks that may maintain cloud ice in AMPS even when entrainment of IN at the mixed-layer boundaries is weak.
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International Nuclear Information System (INIS)
Subbotin, A.V.
1978-01-01
Nucleation of viable voids in irradiated materials is considered. The mechanism of evaporation and absorption of interstitials and vacancies disregarding the possibility of void merging is laid down into the basis of the discussion. The effect of irradiated material structure on void nucleation is separated from the effect of the properties of supersaturated solutions of vacancies and interstitials. An analytical expression for the nucleation rate is obtained and analyzed in different cases. The interstitials are concluded to effect severely the nucleation rate of viable voids
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Thermomechanical Mechanisms of Reducing Ice Adhesion on Superhydrophobic Surfaces.
Cohen, N; Dotan, A; Dodiuk, H; Kenig, S
2016-09-20
Superhydrophobic (SH) coatings have been shown to reduce freezing and ice nucleation rates, by means of low surface energy chemistry tailored with nano/micro roughness. Durability enhancement of SH surfaces is a crucial issue. Consequently, the present research on reducing ice adhesion is based on radiation-induced radical reaction for covalently bonding SiO2 nanoparticles to polymer coatings to obtain durable roughness. Results indicated that the proposed approach resulted in SH surfaces having high contact angles (>155°) and low sliding angles (reduction of shear adhesion to a variety of SH treated substrates having low thermal expansion coefficient (copper and aluminum) and high thermal expansion coefficient (polycarbonate and poly(methyl methacrylate)). It was concluded that the thermal mismatch between the adhering ice and the various substrates and its resultant interfacial thermal stresses affect the adhesion strength of the ice to the respective substrate.
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Nucleation of diindenoperylene and pentacene at thermal and hyperthermal incident kinetic energies
Energy Technology Data Exchange (ETDEWEB)
Kish, Edward R.; Desai, Tushar V.; Greer, Douglas R.; Engstrom, James R., E-mail: jre7@cornell.edu [School of Chemical and Biomolecular Engineering, Cornell University, Ithaca, New York 14853 (United States); Woll, Arthur R. [Cornell High Energy Synchrotron Source, Cornell University, Ithaca, New York 14853 (United States)
2015-05-15
The authors have examined the nucleation of diindenoperylene (DIP) on SiO{sub 2} employing primarily atomic force microscopy and focusing on the effect of incident kinetic energy employing both thermal and supersonic sources. For all incident kinetic energies examined (E{sub i} = 0.09–11.3 eV), the nucleation of DIP is homogeneous and the dependence of the maximum island density on the growth rate is described by a power law. A critical nucleus of approximately two molecules is implicated by our data. A re-examination of the nucleation of pentacene on SiO{sub 2} gives the same major result that the maximum island density is determined by the growth rate, and it is independent of the incident kinetic energy. These observations are readily understood by factoring in the size of the critical nucleus in each case, and the island density, which indicates that diffusive transport of molecules to the growing islands dominate the dynamics of growth in the submonolayer regime.
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Using the thermal diffusion cloud chamber to study the ion-induced nucleation by radon decay
International Nuclear Information System (INIS)
Wu, Yefei.
1991-01-01
Thermal diffusion cloud chamber is steady-state device and has been extensively used for nucleation research. In order to study the ion-induced nucleation by radon decay, a new chamber was designed with improved both upper and bottom plates, the system of circulating fluid, the gasketting, the temperature measurement and the insulation. An alternative method of using oxygen as carrier gas was examined. Therefore, the heavy carrier gas including nitrogen, oxygen, neon, argon and air can be used to study radon radiolysis-induced nucleation for the water or organic compounds in the TDCC. The effects of the pressure and temperature ranges on the density, supersaturation, temperature and partial pressure profile for the water-oxygen-helium in the TDCC have been examined. Based on the classical theory, the rate profile of ion-induced nucleation by radon decays was calculated and compared with the homogeneous nucleation. From measured indoor concentrations of Volatile Organic Compounds (VOC), thermodynamic theory models were used to assess the possibility that these compounds will form ultrafine particles in indoor air by ion-induced nucleation. The energy, number of molecules and equilibrium radius of clusters have been calculated based on Such and Thomson theories. These two sets of values have been compared. Ion cluster radii corresponding to 1--3 VOC molecules are in range of 3--5 x 10 -8 cm. 43 refs., 18 figs., 5 tabs
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McCluskey, Christina S.
Insufficient knowledge regarding the sources and number concentrations of atmospheric ice nucleating particles (INP) leads to large uncertainties in understanding the interaction of aerosols with cloud processes, such as cloud life time and precipitation rates. This study utilizes measurements of INP from a diverse set of biomass burning events to better understand INP associated with biomass burning in the U.S. Prescribed burns in Georgia and Colorado, two Colorado wildfires and two laboratory burns were monitored for INP number concentrations. The relationship between nINP and total particle number concentrations, evident within prescribed burning plumes, was degraded within aged smoke plumes from the wildfires, limiting the utility of this relationship for comparing laboratory and field data. Larger particles, represented by n500nm, are less vulnerable to plume processing and have previously been evaluated for their relation to nINP. Our measurements indicated that for a given n500nm, nINP associated with the wildfires were nearly an order of magnitude higher than nINP found in prescribed fire emissions. Reasons for the differences between INP characteristics in these emissions were explored, including variations in combustion efficiency, fuel type, transport time and environmental conditions. Combustion efficiency and fuel type were eliminated as controlling factors by comparing samples with contrasting combustion efficiencies and fuel types. Transport time was eliminated because the expected impact would be to reduce n500nm, thus resulting in the opposite effect from the observed change. Bulk aerosol chemical composition analyses support the potential role of elevated soil dust particle concentrations during the fires, contributing to the population of INP, but the bulk analyses do not target INP composition directly. It is hypothesized that both hardwood burning and soil lofting are responsible for the elevated production of INP in the Colorado wildfires in
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Schneider, Johannes
2014-05-01
Ice formation in mixed phase tropospheric clouds is an essential prerequisite for the formation of precipitation at mid-latitudes. Ice formation at temperatures warmer than -35°C is only possible via heterogeneous ice nucleation, but up to now the exact pathways of heterogeneous ice formation are not sufficiently well understood. The research unit INUIT (Ice NUcleation research unIT), funded by the Deutsche Forschungsgemeinschaft (DFG FOR 1525) has been established in 2012 with the objective to investigate heterogeneous ice nucleation by combination of laboratory studies, model calculation and field experiments. The main field campaign of the INUIT project (INUIT-JFJ) was conducted at the High Alpine Research Station Jungfraujoch (Swiss Alps, 3580 m asl) during January and February 2013, in collaboration with several international partners in the framework of CLACE2013. The instrumentation included a large set of aerosol chemical and physical analysis instruments (particle counters, particle sizers, particle mass spectrometers, cloud condensation nuclei counters, ice nucleus counters etc.), that were operated inside the Sphinx laboratory and sampled in mixed phase clouds through two ice selective inlets (Ice-CVI, ISI) as well as through a total aerosol inlet that was used for out-of-cloud aerosol measurements. Besides the on-line measurements, also samples for off-line analysis (ESEM, STXM) have been taken in and out of clouds. Furthermore, several cloud microphysics instruments were operated outside the Sphinx laboratory. First results indicate that a large fraction of ice residues sampled from mixed phase clouds contain organic material, but also mineral dust. Soot and lead were not found to be enriched in ice residues. The concentration of heterogeneous ice nuclei was found to be variable (ranging between 100 per liter) and to be strongly dependent on the operating conditions of the respective IN counter. The number size distribution of ice residues appears to
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Barcheck, C. Grace; Tulaczyk, Slawek; Schwartz, Susan Y.; Walter, Jacob I.; Winberry, J. Paul
2018-03-01
The Whillans Ice Plain (WIP) is unique among Antarctic ice streams because it moves by stick-slip. The conditions allowing stick-slip and its importance in controlling ice dynamics remain uncertain. Local basal seismicity previously observed during unstable slip is a clue to the mechanism of ice stream stick-slip and a window into current basal conditions, but the spatial extent and importance of this basal seismicity are unknown. We analyze data from a 2010-2011 ice-plain-wide seismic and GPS network to show that basal micro-seismicity correlates with large-scale patterns in ice stream slip behavior: Basal seismicity is common where the ice moves the least between unstable slip events, with small discrete basal micro-earthquakes happening within 10s of km of the central stick-slip nucleation area and emergent basal tremor occurring downstream of this area. Basal seismicity is largely absent in surrounding areas, where inter-slip creep rates are high. The large seismically active area suggests that a frictional sliding law that can accommodate stick-slip may be appropriate for ice stream beds on regional scales. Variability in seismic behavior over inter-station distances of 1-10 km indicates heterogeneity in local bed conditions and frictional complexity. WIP unstable slips may nucleate when stick-slip basal earthquake patches fail over a large area. We present a conceptual model in which basal seismicity results from slip-weakening frictional failure of over-consolidated till as it is eroded and mobilized into deforming till.
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Simulating gas-aerosol-cirrus interactions: Process-oriented microphysical model and applications
Directory of Open Access Journals (Sweden)
B. Kärcher
2003-01-01
Full Text Available This work describes a process-oriented, microphysical-chemical model to simulate the formation and evolution of aerosols and ice crystals under the conditions prevailing in the upper troposphere and lower stratosphere. The model can be run as a box model or along atmospheric trajectories, and considers mixing, gas phase chemistry of aerosol precursors, binary homogeneous aerosol nucleation, homogeneous and heterogeneous ice nucleation, coagulation, condensation and dissolution, gas retention during particle freezing, gas trapping in growing ice crystals, and reverse processes. Chemical equations are solved iteratively using a second order implicit integration method. Gas-particle interactions and coagulation are treated over various size structures, with fully mass conserving and non-iterative numerical solution schemes. Particle types include quinternary aqueous solutions composed of H2SO4, HNO3, HCl, and HBr with and without insoluble components, insoluble aerosol particles, and spherical or columnar ice crystals deriving from each aerosol type separately. Three case studies are discussed in detail to demonstrate the potential of the model to simulate real atmospheric processes and to highlight current research topics concerning aerosol and cirrus formation near the tropopause. Emphasis is placed on how the formation of cirrus clouds and the scavenging of nitric acid in cirrus depends on small-scale temperature fluctuations and the presence of efficient ice nuclei in the tropopause region, corroborating and partly extending the findings of previous studies.
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China, Swarup; Alpert, Peter A.; Zhang, Bo; Schum, Simeon; Dzepina, Katja; Wright, Kendra; Owen, R. Chris; Fialho, Paulo; Mazzoleni, Lynn R.; Mazzoleni, Claudio; Knopf, Daniel A.
2017-03-01
Long-range transported free tropospheric particles can play a significant role on heterogeneous ice nucleation. Using optical and electron microscopy we examine the physicochemical characteristics of ice nucleating particles (INPs). Particles were collected on substrates from the free troposphere at the remote Pico Mountain Observatory in the Azores Islands, after long-range transport and aging over the Atlantic Ocean. We investigate four specific events to study the ice formation potential by the collected particles with different ages and transport patterns. We use single-particle analysis, as well as bulk analysis to characterize particle populations. Both analyses show substantial differences in particle composition between samples from the four events; in addition, single-particle microscopy analysis indicates that most particles are coated by organic material. The identified INPs contained mixtures of dust, aged sea salt and soot, and organic material acquired either at the source or during transport. The temperature and relative humidity (RH) at which ice formed, varied only by 5% between samples, despite differences in particle composition, sources, and transport patterns. We hypothesize that this small variation in the onset RH may be due to the coating material on the particles. This study underscores and motivates the need to further investigate how long-range transported and atmospherically aged free tropospheric particles impact ice cloud formation.
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Possible significance of cubic water-ice, H2O-Ic, in the atmospheric water cycle of Mars
Gooding, James L.
1988-01-01
The possible formation and potential significance of the cubic ice polymorph on Mars is discussed. When water-ice crystallizes on Earth, the ambient conditions of temperature and pressure result in the formation of the hexagonal ice polymorph; however, on Mars, the much lower termperature and pressures may permit the crystallization of the cubic polymorph. Cubic ice has two properties of possible importance on Mars: it is an excellant nucleator of other volatiles (such as CO2), and it undergoes an exothermic transition to hexagonal ice at temperatures above 170 K. These properties may have significant implications for both martian cloud formation and the development of the seasonal polar caps.
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Heterogeneous condensation of ice mantle around silicate core grain in molecular cloud
International Nuclear Information System (INIS)
Hasegawa, H.
1984-01-01
Interstellar water ice grains are observed in the cold and dense regions such as molecular clouds, HII regions and protostellar objects. The water ice is formed from gas phase during the cooling stage of cosmic gas with solid grain surfaces of high temperature silicate minerals. It is a question whether the ice is formed through the homogeneous condensation process (as the ice alone) or the heterogeneous one (as the ice around the pre-existing high temperature mineral grains). (author)
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Schenk, Ludwig; Mertes, Stephan; Kästner, Udo; Schmidt, Susan; Schneider, Johannes; Frank, Fabian; Nillius, Björn; Worringen, Annette; Kandler, Konrad; Ebert, Martin; Stratmann, Frank
2014-05-01
In 2011, the German research foundation (DFG) research group called Ice Nuclei Research Unit (INUIT (FOR 1525, project STR 453/7-1) was established with the objective to achieve a better understanding concerning heterogeneous ice formation. The presented work is part of INUIT and aims for a better microphysical and chemical characterization of atmospheric aerosol particles that have the potential to act as ice nuclei (IN). For this purpose a counterflow virtual impactor (Kulkarni et al., 2011) system (IN-PCVI) was developed and characterized in order to separate and collect ice particles generated in the Fast Ice Nucleus Chamber (FINCH; Bundke et al., 2008) and to release their IN for further analysis. Here the IN-PCVI was used for the inertial separation of the IN counter produced ice particles from smaller drops and interstitial particles. This is realized by a counterflow that matches the FINCH output flow inside the IN-PCVI. The choice of these flows determines the aerodynamic cut-off diameter. The collected ice particles are transferred into the IN-PCVI sample flow where they are completely evaporated in a particle-free and dry carrier air. In this way, the aerosol particles detected as IN by the IN counter can be extracted and distributed to several particle sensors. This coupled setup FINCH, IN-PCVI and aerosol instrumentation was deployed during the INUIT-JFJ joint measurement field campaign at the research station Jungfraujoch (3580m asl). Downstream of the IN-PCVI, the Aircraft-based Laser Ablation Aerosol Mass Spectrometer (ALABAMA; Brands et al., 2011) was attached for the chemical analysis of the atmospheric IN. Also, number concentration and size distribution of IN were measured online (TROPOS) and IN impactor samples for electron microscopy (TU Darmstadt) were taken. Therefore the IN-PCVI was operated with different flow settings than known from literature (Kulkarni et al., 2011), which required a further characterisation of its cut
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Bhattacharjee, Amit Kumar
2017-01-01
For isotropic fluids, classical nucleation theory predicts the nucleation rate, barrier height and critical droplet size by ac- counting for the competition between bulk energy and interfacial tension. The nucleation process in liquid crystals is less understood. We numerically investigate nucleation in monolayered nematogenic films using a mesoscopic framework, in par- ticular, we study the morphology and kinetic pathway in spontaneous formation and growth of droplets of the stable phase in the metastable background. The parameter κ that quantifies the anisotropic elastic energy plays a central role in determining the geometric structure of the droplets. Noncircular nematic droplets with homogeneous director orientation are nucleated in a background of supercooled isotropic phase for small κ. For large κ, noncircular droplets with integer topological charge, accompanied by a biaxial ring at the outer surface, are nucleated. The isotropic droplet shape in a superheated nematic background is found to depend on κ in a similar way. Identical growth laws are found in the two cases, although an unusual two-stage mechanism is observed in the nucleation of isotropic droplets. Temporal distributions of successive events indi- cate the relevance of long-ranged elasticity-mediated interactions within the isotropic domains. Implications for a theoretical description of nucleation in anisotropic fluids are discussed.
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Barahona, Donifan; Molod, Andrea M.; Bacmeister, Julio; Nenes, Athanasios; Gettelman, Andrew; Morrison, Hugh; Phillips, Vaughan,; Eichmann, Andrew F.
2013-01-01
This work presents the development of a two-moment cloud microphysics scheme within the version 5 of the NASA Goddard Earth Observing System (GEOS-5). The scheme includes the implementation of a comprehensive stratiform microphysics module, a new cloud coverage scheme that allows ice supersaturation and a new microphysics module embedded within the moist convection parameterization of GEOS-5. Comprehensive physically-based descriptions of ice nucleation, including homogeneous and heterogeneous freezing, and liquid droplet activation are implemented to describe the formation of cloud particles in stratiform clouds and convective cumulus. The effect of preexisting ice crystals on the formation of cirrus clouds is also accounted for. A new parameterization of the subgrid scale vertical velocity distribution accounting for turbulence and gravity wave motion is developed. The implementation of the new microphysics significantly improves the representation of liquid water and ice in GEOS-5. Evaluation of the model shows agreement of the simulated droplet and ice crystal effective and volumetric radius with satellite retrievals and in situ observations. The simulated global distribution of supersaturation is also in agreement with observations. It was found that when using the new microphysics the fraction of condensate that remains as liquid follows a sigmoidal increase with temperature which differs from the linear increase assumed in most models and is in better agreement with available observations. The performance of the new microphysics in reproducing the observed total cloud fraction, longwave and shortwave cloud forcing, and total precipitation is similar to the operational version of GEOS-5 and in agreement with satellite retrievals. However the new microphysics tends to underestimate the coverage of persistent low level stratocumulus. Sensitivity studies showed that the simulated cloud properties are robust to moderate variation in cloud microphysical parameters
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Effect of CaCO3(S) nucleation modes on algae removal from alkaline water.
Choi, Jin Yong; Kinney, Kerry A; Katz, Lynn E
2016-02-29
The role of calcite heterogeneous nucleation was studied in a particle coagulation treatment process for removing microalgae from water. Batch experiments were conducted with Scenedesmus sp. and Chlorella sp. in the presence and absence of carbonate and in the presence and absence of Mg to delineate the role of CaCO 3(S) nucleation on microalgae removal. The results indicate that effective algae coagulation (e.g., up to 81 % algae removal efficiency) can be achieved via heterogeneous nucleation with CaCO 3(S) ; however, supersaturation ratios between 120 and 200 are required to achieve at least 50% algae removal, depending on ion concentrations. Algae removal was attributed to adsorption of Ca 2+ onto the cell surface which provides nucleation sites for CaCO 3(S) precipitation. Bridging of calcite particles between the algal cells led to rapid aggregation and formation of larger flocs. However, at higher supersaturation conditions, algae removal was diminished due to the dominance of homogeneous nucleation of CaCO 3(S) . Removal of algae in the presence of Ca 2+ and Mg 2+ required higher supersaturation values; however, the shift from heteronucleation to homonucleation with increasing supersaturation was still evident. The results suggest that water chemistry, pH, ionic strength, alkalinity and Ca 2+ concentration can be optimized for algae removal via coagulation-sedimentation.
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Paraskevov, A V; Zendrikov, D K
2017-03-23
We show that in model neuronal cultures, where the probability of interneuronal connection formation decreases exponentially with increasing distance between the neurons, there exists a small number of spatial nucleation centers of a network spike, from where the synchronous spiking activity starts propagating in the network typically in the form of circular traveling waves. The number of nucleation centers and their spatial locations are unique and unchanged for a given realization of neuronal network but are different for different networks. In contrast, if the probability of interneuronal connection formation is independent of the distance between neurons, then the nucleation centers do not arise and the synchronization of spiking activity during a network spike occurs spatially uniform throughout the network. Therefore one can conclude that spatial proximity of connections between neurons is important for the formation of nucleation centers. It is also shown that fluctuations of the spatial density of neurons at their random homogeneous distribution typical for the experiments in vitro do not determine the locations of the nucleation centers. The simulation results are qualitatively consistent with the experimental observations.
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Effects of different temperature treatments on biological ice nuclei in snow samples
Hara, Kazutaka; Maki, Teruya; Kakikawa, Makiko; Kobayashi, Fumihisa; Matsuki, Atsushi
2016-09-01
The heat tolerance of biological ice nucleation activity (INA) depends on their types. Different temperature treatments may cause varying degrees of inactivation on biological ice nuclei (IN) in precipitation samples. In this study, we measured IN concentration and bacterial INA in snow samples using a drop freezing assay, and compared the results for unheated snow and snow treated at 40 °C and 90 °C. At a measured temperature of -7 °C, the concentration of IN in untreated snow was 100-570 L-1, whereas the concentration in snow treated at 40 °C and 90 °C was 31-270 L-1 and 2.5-14 L-1, respectively. In the present study, heat sensitive IN inactivated by heating at 40 °C were predominant, and ranged 23-78% of IN at -7 °C compared with untreated samples. Ice nucleation active Pseudomonas strains were also isolated from the snow samples, and heating at 40 °C and 90 °C inactivated these microorganisms. Consequently, different temperature treatments induced varying degrees of inactivation on IN in snow samples. Differences in the concentration of IN across a range of treatment temperatures might reflect the abundance of different heat sensitive biological IN components.
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Decompression-induced melting of ice IV and the liquid-liquid transition in water
Mishima, Osamu; Stanley, H. Eugene
1998-03-01
Although liquid water has been the focus of intensive research for over 100 years, a coherent physical picture that unifies all of the known anomalies of this liquid, is still lacking. Some of these anomalies occur in the supercooled region, and have been rationalized on the grounds of a possible retracing of the liquid-gas spinodal (metastability limit) line into the supercooled liquid region, or alternatively the presence of a line of first-order liquid-liquid phase transitions in this region which ends in a critical point,. But these ideas remain untested experimentally, in part because supercooled water can be probed only above the homogeneous nucleation temperature TH at which water spontaneously crystallizes. Here we report an experimental approach that is not restricted by the barrier imposed by TH, involving measurement of the decompression-induced melting curves of several high-pressure phases of ice in small emulsified droplets. We find that the melting curve for ice IV seems to undergo a discontinuity at precisely the location proposed for the line of liquid-liquid phase transitions. This is consistent with, but does not prove, the coexistence of two different phases of (supercooled) liquid water. From the experimental data we calculate a possible Gibbs potential surface and a corresponding equation of state for water, from the forms of which we estimate the coordinates of the liquid-liquid critical point to be at pressure Pc ~ 0.1GPa and temperature Tc ~ 220K.
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Nakaoka, Yuki; Kimura, Akatsuki; Tani, Tomomi; Goshima, Gohta
2015-01-01
The mechanism underlying microtubule (MT) generation in plants has been primarily studied using the cortical MT array, in which fixed-angled branching nucleation and katanin-dependent MT severing predominate. However, little is known about MT generation in the endoplasm. Here, we explored the mechanism of endoplasmic MT generation in protonemal cells of Physcomitrella patens. We developed an assay that utilizes flow cell and oblique illumination fluorescence microscopy, which allowed visualization and quantification of individual MT dynamics. MT severing was infrequently observed, and disruption of katanin did not severely affect MT generation. Branching nucleation was observed, but it showed markedly variable branch angles and was occasionally accompanied by the transport of nucleated MTs. Cytoplasmic nucleation at seemingly random locations was most frequently observed and predominated when depolymerized MTs were regrown. The MT nucleator γ-tubulin was detected at the majority of the nucleation sites, at which a single MT was generated in random directions. When γ-tubulin was knocked down, MT generation was significantly delayed in the regrowth assay. However, nucleation occurred at a normal frequency in steady state, suggesting the presence of a γ-tubulin-independent backup mechanism. Thus, endoplasmic MTs in this cell type are generated in a less ordered manner, showing a broader spectrum of nucleation mechanisms in plants. PMID:25616870
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Mesoscopic surface roughness of ice crystals pervasive across a wide range of ice crystal conditions
Magee, N. B.; Miller, A.; Amaral, M.; Cumiskey, A.
2014-11-01
Here we show high-magnification images of hexagonal ice crystals acquired by environmental scanning electron microscopy (ESEM). Most ice crystals were grown and sublimated in the water vapor environment of an FEI-Quanta-200 ESEM, but crystals grown in a laboratory diffusion chamber were also transferred intact and imaged via ESEM. All of these images display prominent mesoscopic topography including linear striations, ridges, islands, steps, peaks, pits, and crevasses; the roughness is not observed to be confined to prism facets. The observations represent the most highly magnified images of ice surfaces yet reported and expand the range of conditions in which rough surface features are known to be conspicuous. Microscale surface topography is seen to be ubiquitously present at temperatures ranging from -10 °C to -40 °C, in supersaturated and subsaturated conditions, on all crystal facets, and irrespective of substrate. Despite the constant presence of surface roughness, the patterns of roughness are observed to be dramatically different between growing and sublimating crystals, and transferred crystals also display qualitatively different patterns of roughness. Crystals are also demonstrated to sometimes exhibit inhibited growth in moderately supersaturated conditions following exposure to near-equilibrium conditions, a phenomenon interpreted as evidence of 2-D nucleation. New knowledge about the characteristics of these features could affect the fundamental understanding of ice surfaces and their physical parameterization in the context of satellite retrievals and cloud modeling. Links to supplemental videos of ice growth and sublimation are provided.
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Bacon, Neil Julian
2001-12-01
I describe experiments to investigate the properties of microscopic ice particles. The goal of the work was to measure parameters that are important in cloud processes and radiative transfer, using a novel technique that avoids the use of substrates. The experiments were conducted in two separate electrodynamic balance chambers. Single, charged ice particles were formed from frost particles or from droplets frozen either homogeneously or heteroge neously with a bionucleant. The particles were trapped at temperatures between -38°C and -4°C and grown or sublimated according to the temperature gradient in the cham ber. I describe observations of breakup of sublimating frost particles, measurements of light scattering by hexagonal crystals, and observations of the morphology of ice particles grown from frozen water droplets and frost particles. The breaking strength of frost particles was an order of magnitude less than that of bulk ice. Light scattering features not previously observed were analyzed and related to crystal dimension. Initial results from a computer model failed to reproduce these features. The widths of scattering peaks suggest that surface roughness may play a role in determining the angular distribution of scattered light. Ice particle mass evolution was found to be consistent with diffusion- limited growth. Crystals grown slowly from frozen droplets adopted isometric habits, while faster growth resulted in thin side-planes, although there was not an exact correspondence between growth conditions and particle morphology. From the morphological transition, I infer lower limits for the critical supersaturation for layer nucleation on the prism face of 2.4% at -15°C, 4.4% at -20°C, and 3.1% at -25°C. Analytic expressions for the size dependence of facet stability are developed, indicating a strong dependence of stability on both crystal size and surface kinetics, and compared with data. I discuss the role of complex particle morphologies in
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The immersion freezing behavior of size-segregated soot and kaolinite particles
Hartmann, S.; Augustin, S.; Clauss, T.; Niedermeier, D.; Raddatz, M.; Wex, H.; Shaw, R. A.; Stratmann, F.
2011-12-01
Heterogeneous ice nucleation plays a crucial role for ice formation in mixed-phase and cirrus clouds and has an important impact on precipitation formation, global radiation balances, and therefore Earth's climate (Cantrell and Heymsfield, 2005). Mineral dust and soot particles are found to be a major component of ice crystal residues (e.g., Pratt et al., 2009) so these substances are potential sources of atmospheric ice nuclei (IN). Experimental studies investigating the immersion freezing behavior of size-segregated soot and kaolinite particles conducted at the Leipzig Aerosol Cloud Interaction Simulator (LACIS) are presented. In our measurements only one aerosol particle is immersed in an air suspended water droplet which can trigger ice nucleation. The method facilitates very precise examinations with respect to temperature, ice nucleation time and ice nucleus size. Considering laboratory studies, the picture of the IN ability of soot particles is quite heterogeneous. Our studies show that submicron flame, spark soot particles and optionally coated with sulfuric acid to simulate chemically aging do not act as IN at temperatures higher than homogeneous freezing taking place. Therefore soot particles might not be an important source of IN for immersion freezing in the atmosphere. In contrast, kaolinite being representative for natural mineral dust with a well known composition and structure is found to be very active in forming ice for all freezing modes (e.g., Mason and Maybank, 1958). Analyzing the immersion freezing behavior of different sized kaolinite particles (300, 500 and 700 nm in diameter) the size effect was clearly observed, i.e. the ice fraction (number of frozen droplets per total number) scales with particle surface, i.e. the larger the ice nucleus surface the higher the ice fraction. The slope of the logarithm of the ice fraction as function of temperature is similar for all particle sizes investigated and fits very well with the results of L
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DEFF Research Database (Denmark)
Möller, Per; Lubinski, David J.; Ingólfsson, Ólafur
2006-01-01
Quaternary glacial stratigraphy and relative sea-level changes reveal at least four expansions of the Kara Sea ice sheet over the Severnaya Zemlya Archipelago at 79°N in the Russian Arctic, as indicated from tills interbedded with marine sediments, exposed in stratigraphic superposition, and from......-5e and MIS 5d-3. The MIS 6-5e event, associated with the high marine limit, implies ice-sheet thickness of >2000 m only 200 km from the deep Arctic Ocean, consistent with published evidence of ice grounding at ~1000 m water depth in the central Arctic Ocean. Till fabrics and glacial tectonics record...... repeated expansions of local ice caps exclusively, suggesting wet-based ice cap advance followed by cold-based regional ice-sheet expansion. Local ice caps over highland sites along the perimeter of the shallow Kara Sea, including the Byrranga Mountains, appear to have repeatedly fostered initiation...
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Braun, S.; Kraska, T.; Kalikmanov, V.I.
2013-01-01
Binary clusters formed by vapor-liquid nucleation are frequently nonhomogeneous objects in which components are not well mixed. The structure of a cluster plays an important role in nucleation and cluster growth. We demonstrate structuring effects by studying high-pressure nucleation and cluster
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Directory of Open Access Journals (Sweden)
O. Möhler
2003-01-01
Full Text Available The homogeneous freezing of supercooled H2SO4/H2O solution droplets was investigated in the aerosol chamber AIDA (Aerosol Interactions and Dynamics in the Atmosphere of Forschungszentrum Karlsruhe. 24 freezing experiments were performed at temperatures between 189 and 235 K with aerosol particles in the diameter range 0.05 to 1 µm. Individual experiments started at homogeneous temperatures and ice saturation ratios between 0.9 and 0.95. Cloud cooling rates up to -2.8 K min-1 were simulated dynamically in the chamber by expansion cooling using a mechanical pump. Depending on the cooling rate and starting temperature, freezing threshold relative humidities were exceeded after expansion time periods between about 1 and 10 min. The onset of ice formation was measured with three independent methods showing good agreement among each other. Ice saturation ratios measured at the onset of ice formation increased from about 1.4 at 231 K to about 1.75 at 189 K. The experimental data set including thermodynamic parameters as well as physical and chemical aerosol analysis provides a good basis for microphysical model applications.
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Liu, Shanqiu; Eijkelenkamp, Rik; Duvigneau, Joost; Vancso, G Julius
2017-11-01
Core-shell nanoparticles consisting of silica as core and surface-grafted poly(dimethylsiloxane) (PDMS) as shell with different diameters were prepared and used as heterogeneous nucleation agents to obtain CO 2 -blown poly(methyl methacrylate) (PMMA) nanocomposite foams. PDMS was selected as the shell material as it possesses a low surface energy and high CO 2 -philicity. The successful synthesis of core-shell nanoparticles was confirmed by Fourier transform infrared spectroscopy, thermogravimetric analysis, and transmission electron microscopy. The cell size and cell density of the PMMA micro- and nanocellular materials were determined by scanning electron microscopy. The cell nucleation efficiency using core-shell nanoparticles was significantly enhanced when compared to that of unmodified silica. The highest nucleation efficiency observed had a value of ∼0.5 for nanoparticles with a core diameter of 80 nm. The particle size dependence of cell nucleation efficiency is discussed taking into account line tension effects. Complete engulfment by the polymer matrix of particles with a core diameter below 40 nm at the cell wall interface was observed corresponding to line tension values of approximately 0.42 nN. This line tension significantly increases the energy barrier of heterogeneous nucleation and thus reduces the nucleation efficiency. The increase of the CO 2 saturation pressure to 300 bar prior to batch foaming resulted in an increased line tension length. We observed a decrease of the heterogeneous nucleation efficiency for foaming after saturation with CO 2 at 300 bar, which we attribute to homogenous nucleation becoming more favorable at the expense of heterogeneous nucleation in this case. Overall, it is shown that the contribution of line tension to the free energy barrier of heterogeneous foam cell nucleation must be considered to understand foaming of viscoelastic materials. This finding emphasizes the need for new strategies including the use of
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Identification of Dust and Ice Cloud Formation from A-Train Datasets
Russell, D. S.; Liou, K. N.
2014-12-01
Dust aerosols are effective ice nuclei for clouds and instances of nucleation have been well studied in laboratory experiments. We used CALIOP/CALIPSO, MODIS/Aqua, and CloudSat on the A-Train to find collocated instances of clouds characterized as water by MODIS, but contain ice water as indicated by CloudSat. The vertical profiles of CALIPSO detect the presence of dust and polluted dust near clouds. This study concentrates on high dust aerosol areas including the regions surrounding the Sahara Desert as well as South Asia including the Tibetan Plateau. These cases display the effects of dust acting as ice nuclei in the time frame between MODIS overpass and CloudSat overpass (~45 seconds). Utilizing available datasets, we then carried out radiative transfer calculations to understand spectral radiative forcing differences between water and ice clouds, particularly over snow surfaces at the Tibetan Plateau.
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Directory of Open Access Journals (Sweden)
Zhen Zhang
Full Text Available Ice nucleation protein (INP is frequently used as a surface anchor for protein display in gram-negative bacteria. Here, MalE and TorA signal peptides, and three charged polypeptides, 6×Lys, 6×Glu and 6×Asp, were anchored to the N-terminus of truncated INP (InaK-N to improve its surface display efficiency for human Arginase1 (ARG1. Our results indicated that the TorA signal peptide increased the surface translocation of non-protein fused InaK-N and human ARG1 fused InaK-N (InaK-N/ARG1 by 80.7% and 122.4%, respectively. Comparably, the MalE signal peptide decreased the display efficiencies of both the non-protein fused InaK-N and InaK-N/ARG1. Our results also suggested that the 6×Lys polypeptide significantly increased the surface display efficiency of K6-InaK-N/ARG1 by almost 2-fold, while also practically abolishing the surface translocation of non-protein fused InaK-N, indicating the interesting roles of charged polypeptides in bacteria surface display systems. Cell surface-immobilized K6-InaK-N/ARG1 presented an arginase activity of 10.7 U/OD600 under the optimized conditions of 40°C, pH 10.0 and 1 mM Mn2+, which could convert more than 95% of L-Arginine (L-Arg to L-Ornithine (L-Orn in 16 hours. The engineered InaK-Ns expanded the INP surface display system, which aided in the surface immobilization of human ARG1 in E. coli cells.
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International Nuclear Information System (INIS)
Hubert, J; Cheng, M; Emmerich, H
2009-01-01
We contribute to the more detailed understanding of the phase-field crystal model recently developed by Elder et al (2002 Phys. Rev. Lett. 88 245701), by focusing on its noise term and examining its impact on the nucleation rate in a homogeneously solidifying system as well as on successively developing grain size distributions. In this context we show that principally the grain size decreases with increasing noise amplitude, resulting in both a smaller average grain size and a decreased maximum grain size. Despite this general tendency, which we interpret based on Panfilis and Filiponi (2000 J. Appl. Phys. 88 562), we can identify two different regimes in which nucleation and successive initial growth are governed by quite different mechanisms.
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Livingston, David P; Tuong, Tan D; Murphy, J Paul; Gusta, Lawrence V; Willick, Ian; Wisniewski, Micheal E
2018-04-01
An extremely high resolution infrared camera demonstrated various freezing events in wheat under natural conditions. Many of those events shed light on years of misunderstanding regarding freezing in small grains. Infrared thermography has enhanced our knowledge of ice nucleation and propagation in plants through visualization of the freezing process. The majority of infrared analyses have been conducted under controlled conditions and often on individual organs instead of whole plants. In the present study, high-definition (1280 × 720 pixel resolution) infrared thermography was used under natural conditions to visualize the freezing process of wheat plants during freezing events in 2016 and 2017. Plants within plots were found to freeze one at a time throughout the night and in an apparently random manner. Leaves on each plant also froze one at a time in an age-dependent pattern with oldest leaves freezing first. Contrary to a common assumption that freezing begins in the upper parts of leaves; freezing began at the base of the plant and spread upwards. The high resolution camera used was able to verify that a two stage sequence of freezing began within vascular bundles. Neither of the two stages was lethal to leaves, but a third stage was demonstrated at colder temperatures that was lethal and was likely a result of dehydration stress; this stage of freezing was not detectable by infrared. These results underscore the complexity of the freezing process in small grains and indicate that comprehensive observational studies are essential to identifying and selecting freezing tolerance traits in grain crops.
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Directory of Open Access Journals (Sweden)
D. P. Grosvenor
2012-12-01
lack of seeding ice crystals to act as rimers to initiate secondary ice particle production. This highlights the chaotic and spatially inhomogeneous nature of this process and indicates that the accurate representation of it in global models is likely to represent a challenge. However, the contrast between Hallett Mossop zone ice concentrations and the fairly low concentrations of heterogeneously nucleated ice suggests that the Hallet Mossop process has the potential to be very important in remote, pristine regions such as around the Antarctic coast.
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Superheating in nucleate boiling calculated by the heterogeneous nucleation theory
International Nuclear Information System (INIS)
Gerum, E.; Straub, J.; Grigull, U.
1979-01-01
With the heterogeneous nucleation theory the superheating of the liquid boundary layer in nucleate boiling is described not only for the onset of nuclear boiling but also for the boiling crisis. The rate of superheat depends on the thermodynamic stability of the metastable liquid, which is influenced by the statistical fluctuations in the liquid and the nucleation at the solid surface. Because of the fact that the cavities acting as nuclei are too small for microscopic observation, the size and distribution function of the nuclei on the surface necessary for the determination of the probability of bubble formation cannot be detected by measuring techniques. The work of bubble formation reduced by the nuclei can be represented by a simple empirical function whose coefficients are determined from boiling experiments. Using this the heterogeneous nucleation theory describes the superheating of the liquid. Several fluids including refrigerants, liquid gases, organic liquids and water were used to check the theory. (author)
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Lidar Ice nuclei estimates and how they relate with airborne in-situ measurements
Marinou, Eleni; Amiridis, Vassilis; Ansmann, Albert; Nenes, Athanasios; Balis, Dimitris; Schrod, Jann; Binietoglou, Ioannis; Solomos, Stavros; Mamali, Dimitra; Engelmann, Ronny; Baars, Holger; Kottas, Michael; Tsekeri, Alexandra; Proestakis, Emmanouil; Kokkalis, Panagiotis; Goloub, Philippe; Cvetkovic, Bojan; Nichovic, Slobodan; Mamouri, Rodanthi; Pikridas, Michael; Stavroulas, Iasonas; Keleshis, Christos; Sciare, Jean
2018-04-01
By means of available ice nucleating particle (INP) parameterization schemes we compute profiles of dust INP number concentration utilizing Polly-XT and CALIPSO lidar observations during the INUIT-BACCHUS-ACTRIS 2016 campaign. The polarization-lidar photometer networking (POLIPHON) method is used to separate dust and non-dust aerosol backscatter, extinction, mass concentration, particle number concentration (for particles with radius > 250 nm) and surface area concentration. The INP final products are compared with aerosol samples collected from unmanned aircraft systems (UAS) and analyzed using the ice nucleus counter FRIDGE.
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Lidar Ice nuclei estimates and how they relate with airborne in-situ measurements
Directory of Open Access Journals (Sweden)
Marinou Eleni
2018-01-01
Full Text Available By means of available ice nucleating particle (INP parameterization schemes we compute profiles of dust INP number concentration utilizing Polly-XT and CALIPSO lidar observations during the INUIT-BACCHUS-ACTRIS 2016 campaign. The polarization-lidar photometer networking (POLIPHON method is used to separate dust and non-dust aerosol backscatter, extinction, mass concentration, particle number concentration (for particles with radius > 250 nm and surface area concentration. The INP final products are compared with aerosol samples collected from unmanned aircraft systems (UAS and analyzed using the ice nucleus counter FRIDGE.
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Impact of aerosols on ice crystal size
Directory of Open Access Journals (Sweden)
B. Zhao
2018-01-01
Full Text Available The interactions between aerosols and ice clouds represent one of the largest uncertainties in global radiative forcing from pre-industrial time to the present. In particular, the impact of aerosols on ice crystal effective radius (Rei, which is a key parameter determining ice clouds' net radiative effect, is highly uncertain due to limited and conflicting observational evidence. Here we investigate the effects of aerosols on Rei under different meteorological conditions using 9-year satellite observations. We find that the responses of Rei to aerosol loadings are modulated by water vapor amount in conjunction with several other meteorological parameters. While there is a significant negative correlation between Rei and aerosol loading in moist conditions, consistent with the "Twomey effect" for liquid clouds, a strong positive correlation between the two occurs in dry conditions. Simulations based on a cloud parcel model suggest that water vapor modulates the relative importance of different ice nucleation modes, leading to the opposite aerosol impacts between moist and dry conditions. When ice clouds are decomposed into those generated from deep convection and formed in situ, the water vapor modulation remains in effect for both ice cloud types, although the sensitivities of Rei to aerosols differ noticeably between them due to distinct formation mechanisms. The water vapor modulation can largely explain the difference in the responses of Rei to aerosol loadings in various seasons. A proper representation of the water vapor modulation is essential for an accurate estimate of aerosol–cloud radiative forcing produced by ice clouds.
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Impact of aerosols on ice crystal size
Zhao, Bin; Liou, Kuo-Nan; Gu, Yu; Jiang, Jonathan H.; Li, Qinbin; Fu, Rong; Huang, Lei; Liu, Xiaohong; Shi, Xiangjun; Su, Hui; He, Cenlin
2018-01-01
The interactions between aerosols and ice clouds represent one of the largest uncertainties in global radiative forcing from pre-industrial time to the present. In particular, the impact of aerosols on ice crystal effective radius (Rei), which is a key parameter determining ice clouds' net radiative effect, is highly uncertain due to limited and conflicting observational evidence. Here we investigate the effects of aerosols on Rei under different meteorological conditions using 9-year satellite observations. We find that the responses of Rei to aerosol loadings are modulated by water vapor amount in conjunction with several other meteorological parameters. While there is a significant negative correlation between Rei and aerosol loading in moist conditions, consistent with the "Twomey effect" for liquid clouds, a strong positive correlation between the two occurs in dry conditions. Simulations based on a cloud parcel model suggest that water vapor modulates the relative importance of different ice nucleation modes, leading to the opposite aerosol impacts between moist and dry conditions. When ice clouds are decomposed into those generated from deep convection and formed in situ, the water vapor modulation remains in effect for both ice cloud types, although the sensitivities of Rei to aerosols differ noticeably between them due to distinct formation mechanisms. The water vapor modulation can largely explain the difference in the responses of Rei to aerosol loadings in various seasons. A proper representation of the water vapor modulation is essential for an accurate estimate of aerosol-cloud radiative forcing produced by ice clouds.
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de Leede, G.L.A.; Waal, de H.
1989-01-01
Nucleation rates were detd. in a ZrF4-BaF2-NaF-LaF3-AlF3 glass (ZBLAN) using an optical method. The results were compared with a similar glass having a slightly different compn. The difference in the nucleation rate is explained by classical nucleation theory using calcd. free-energy differences
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Nucleation phenomena at Suzuki phases
International Nuclear Information System (INIS)
Acosta-Najarro, D.; Jose Y, M.
1982-01-01
Crystal of NaCl doped with Mn present regions with an increase in nucleation densities when observed by surface gold decoration; this increase is related to the nucleation of the Suzuki phases which are induced by cooling of the crystal matrix. Calculations based on atomistic nucleation theory are developed to explain the increased nucleation density. Experiments were made to compare with the theoretical results. In particular the density of nuclei was measured as a function of the rate or arrival of atoms to the surface. Therefore, the changes in the nucleation densities are explained in terms of change in migration energies between the Suzuki phase and the NaCl matrix excluding the possibility of nucleation induced by point defects. (author)
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Gallet, Jean-Charles; Merkouriadi, Ioanna; Liston, Glen E.; Polashenski, Chris; Hudson, Stephen; Rösel, Anja; Gerland, Sebastian
2017-10-01
Snow is crucial over sea ice due to its conflicting role in reflecting the incoming solar energy and reducing the heat transfer so that its temporal and spatial variability are important to estimate. During the Norwegian Young Sea ICE (N-ICE2015) campaign, snow physical properties and variability were examined, and results from April until mid-June 2015 are presented here. Overall, the snow thickness was about 20 cm higher than the climatology for second-year ice, with an average of 55 ± 27 cm and 32 ± 20 cm on first-year ice. The average density was 350-400 kg m-3 in spring, with higher values in June due to melting. Due to flooding in March, larger variability in snow water equivalent was observed. However, the snow structure was quite homogeneous in spring due to warmer weather and lower amount of storms passing over the field camp. The snow was mostly consisted of wind slab, faceted, and depth hoar type crystals with occasional fresh snow. These observations highlight the more dynamic character of evolution of snow properties over sea ice compared to previous observations, due to more variable sea ice and weather conditions in this area. The snowpack was isothermal as early as 10 June with the first onset of melt clearly identified in early June. Based on our observations, we estimate than snow could be accurately represented by a three to four layers modeling approach, in order to better consider the high variability of snow thickness and density together with the rapid metamorphose of the snow in springtime.
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Protein crystal nucleation in pores.
Nanev, Christo N; Saridakis, Emmanuel; Chayen, Naomi E
2017-01-16
The most powerful method for protein structure determination is X-ray crystallography which relies on the availability of high quality crystals. Obtaining protein crystals is a major bottleneck, and inducing their nucleation is of crucial importance in this field. An effective method to form crystals is to introduce nucleation-inducing heterologous materials into the crystallization solution. Porous materials are exceptionally effective at inducing nucleation. It is shown here that a combined diffusion-adsorption effect can increase protein concentration inside pores, which enables crystal nucleation even under conditions where heterogeneous nucleation on flat surfaces is absent. Provided the pore is sufficiently narrow, protein molecules approach its walls and adsorb more frequently than they can escape. The decrease in the nucleation energy barrier is calculated, exhibiting its quantitative dependence on the confinement space and the energy of interaction with the pore walls. These results provide a detailed explanation of the effectiveness of porous materials for nucleation of protein crystals, and will be useful for optimal design of such materials.
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Oliver, Michael J.
2014-01-01
The Propulsion Systems Laboratory (PSL) is an existing altitude simulation jet engine test facility located at NASA Glenn Research Center in Cleveland, OH. It was modified in 2012 with the integration of an ice crystal cloud generation system. This paper documents the inaugural ice crystal cloud test in PSL--the first ever full scale, high altitude ice crystal cloud turbofan engine test to be conducted in a ground based facility. The test article was a Lycoming ALF502-R5 high bypass turbofan engine, serial number LF01. The objectives of the test were to validate the PSL ice crystal cloud calibration and engine testing methodologies by demonstrating the capability to calibrate and duplicate known flight test events that occurred on the same LF01 engine and to generate engine data to support fundamental and computational research to investigate and better understand the physics of ice crystal icing in a turbofan engine environment while duplicating known revenue service events and conducting test points while varying facility and engine parameters. During PSL calibration testing it was discovered than heated probes installed through tunnel sidewalls experienced ice buildup aft of their location due to ice crystals impinging upon them, melting and running back. Filtered city water was used in the cloud generation nozzle system to provide ice crystal nucleation sites. This resulted in mineralization forming on flow path hardware that led to a chronic degradation of performance during the month long test. Lacking internal flow path cameras, the response of thermocouples along the flow path was interpreted as ice building up. Using this interpretation, a strong correlation between total water content (TWC) and a weaker correlation between median volumetric diameter (MVD) of the ice crystal cloud and the rate of ice buildup along the instrumented flow path was identified. For this test article the engine anti-ice system was required to be turned on before ice crystal
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Dinh, Tra; Fueglistaler, Stephan
2016-04-01
Thin cirrus clouds in the tropical tropopause layer (TTL) are of great interest due to their role in the control of water vapor and temperature in the TTL. Previous research on TTL cirrus clouds has focussed mainly on microphysical processes, specifically the ice nucleation mechanism and dehydration efficiency. Here, we use a cloud resolving model to analyse the sensitivity of TTL cirrus characteristics and impacts with respect to microphysical and radiative processes. A steady-state TTL cirrus cloud field is obtained in the model forced with dynamical conditions typical for the TTL (2-dimensional setup with a Kelvin-wave temperature perturbation). Our model results show that the dehydration efficiency (as given by the domain average relative humidity in the layer of cloud occurrence) is relatively insensitive to the ice nucleation mechanism, i.e. homogeneous versus heterogeneous nucleation. Rather, TTL cirrus affect the water vapor entering the stratosphere via an indirect effect associated with the cloud radiative heating and dynamics. Resolving the cloud radiative heating and the radiatively induced circulations approximately doubles the domain average ice mass. The cloud radiative heating is proportional to the domain average ice mass, and the observed increase in domain average ice mass induces a domain average temperature increase of a few Kelvin. The corresponding increase in water vapor entering the stratosphere is estimated to be about 30 to 40%.
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Regions of open water and melting sea ice drive new particle formation in North East Greenland.
Dall Osto, M; Geels, C; Beddows, D C S; Boertmann, D; Lange, R; Nøjgaard, J K; Harrison, Roy M; Simo, R; Skov, H; Massling, A
2018-04-17
Atmospheric new particle formation (NPF) and growth significantly influences the indirect aerosol-cloud effect within the polar climate system. In this work, the aerosol population is categorised via cluster analysis of aerosol number size distributions (9-915 nm, 65 bins) taken at Villum Research Station, Station Nord (VRS) in North Greenland during a 7 year record (2010-2016). Data are clustered at daily averaged resolution; in total, we classified six categories, five of which clearly describe the ultrafine aerosol population, one of which is linked to nucleation events (up to 39% during summer). Air mass trajectory analyses tie these frequent nucleation events to biogenic precursors released by open water and melting sea ice regions. NPF events in the studied regions seem not to be related to bird colonies from coastal zones. Our results show a negative correlation (r = -0.89) between NPF events and sea ice extent, suggesting the impact of ultrafine Arctic aerosols is likely to increase in the future, given the likely increased sea ice melting. Understanding the composition and the sources of Arctic aerosols requires further integrated studies with joint multi-component ocean-atmosphere observation and modelling.
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The impact of dissolved fluorine on bubble nucleation in hydrous rhyolite melts
Gardner, James E.; Hajimirza, Sahand; Webster, James D.; Gonnermann, Helge M.
2018-04-01
Surface tension of hydrous rhyolitic melt is high enough that large degrees of supersaturation are needed to homogeneously nucleate H2O bubbles during eruptive magma ascent. This study examines whether dissolved fluorine lowers surface tension of hydrous rhyolite, and thus lowers the supersaturation required for bubble nucleation. Fluorine was targeted because it, like H2O, changes melt properties and is highly soluble, unlike all other common magmatic volatiles. Rhyolite melts were saturated at Ps = 245 MPa with H2O fluid that contained F, generating rhyolite with 6.7 ± 0.4 wt.% H2O and 1.1-1.3 wt.% F. When these melts were decompressed rapidly to Pf = 149-202 MPa and quenched after 60 s, bubbles nucleated at supersaturations of ΔP = Ps - Pf ≥52 MPa, and reached bubble number densities of NB = 1012-13 m-3 at ΔP = 78-101 MPa. In comparison, rhyolite saturated with 6.34 ± 0.09 wt.% H2O, but only 0.25 wt.% F, did not nucleate bubbles until ΔP ≥ 100-116 MPa, and even then, at significantly lower NB (<1010 m-3). Numerical modeling of bubble nucleation and growth was used to estimate the values of surface tension required to generate the observed values of NB. Slight differences in melt compositions (i.e., alkalinity and H2O content), H2O diffusivity, or melt viscosity cannot explain the observed differences in NB. Instead, surface tension of F-rich rhyolite must be lower by approximately 4% than that of F-poor rhyolite. This difference in surface tension is significant and, for example, exceeds that found between hydrous basaltic andesite and hydrous rhyolite. These results suggest that is likely that surface tension for F-rich magmas, such as topaz rhyolite, is significantly lower than for F-poor magmas.
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DEFF Research Database (Denmark)
Möller, Per; Lubinski, David J.; Ingólfsson, Ólafur
2006-01-01
Quaternary glacial stratigraphy and relative sea-level changes reveal at least four expansions of the Kara Sea ice sheet over the Severnaya Zemlya Archipelago at 79°N in the Russian Arctic, as indicated from tills interbedded with marine sediments, exposed in stratigraphic superposition, and from...... of a large Kara Sea ice sheet, with exception of the Last Glacial Maximum (MIS 2), when Kara Sea ice did not impact Severnaya Zemlya and barely graced northernmost Taymyr Peninsula.......Quaternary glacial stratigraphy and relative sea-level changes reveal at least four expansions of the Kara Sea ice sheet over the Severnaya Zemlya Archipelago at 79°N in the Russian Arctic, as indicated from tills interbedded with marine sediments, exposed in stratigraphic superposition, and from......-5e and MIS 5d-3. The MIS 6-5e event, associated with the high marine limit, implies ice-sheet thickness of >2000 m only 200 km from the deep Arctic Ocean, consistent with published evidence of ice grounding at ~1000 m water depth in the central Arctic Ocean. Till fabrics and glacial tectonics record...
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Principles of nucleation theory
International Nuclear Information System (INIS)
Clement, C.F.; Wood, M.H.
1980-01-01
The nucleation of small stable species is described in the problem of void growth by discrete rate equations. When gas is being produced the problem reduces to one of calculating the incubation dose for the gas bubble to void transition. A general expression for the steady state nucleation rate is derived for the case when voids are formed by vacancy fluctuations which enable an effective nucleation barrier to be crossed. (author)
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Energy Technology Data Exchange (ETDEWEB)
Pleše, P.; Higgins, M. D.; Mancini, L.; Lanzafame, G.; Brun, F.; Fife, J. L.; Casselman, J.; Baker, D. R.
2018-01-01
Bubble nucleation and growth control the explosivity of volcanic eruptions, and the kinetics of these processes are generally determined from examinations of natural samples and quenched experimental run products. These samples, however, only provide a view of the final state, from which the initial conditions of a time-evolving magmatic system are then inferred. The interpretations that follow are inexact due to the inability of determining the exact conditions of nucleation and the potential detachment of bubbles from their nucleation sites, an uncertainty that can obscure their nucleation location – either homogeneously within the melt or heterogeneously at the interface between crystals and melts. We present results of a series of dynamic, real-time 4D X-ray tomographic microscopy experiments where we observed the development of bubbles in crystal bearing silicate magmas. Experimentally synthesized andesitic glasses with 0.25–0.5 wt% H2O and seed silicate crystals were heated at 1 atm to induce bubble nucleation and track bubble growth and movement. In contrast to previous studies on natural and experimentally produced samples, we found that bubbles readily nucleated on plagioclase and clinopyroxene crystals, that their contact angle changes during growth and that they can grow to sizes many times that of the silicate on whose surface they originated. The rapid heterogeneous nucleation of bubbles at low degrees of supersaturation in the presence of silicate crystals demonstrates that silicates can affect when vesiculation ensues, influencing subsequent permeability development and effusive vs. explosive transition in volcanic eruptions.
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Pleše, P.; Higgins, M. D.; Mancini, L.; Lanzafame, G.; Brun, F.; Fife, J. L.; Casselman, J.; Baker, D. R.
2018-01-01
Bubble nucleation and growth control the explosivity of volcanic eruptions, and the kinetics of these processes are generally determined from examinations of natural samples and quenched experimental run products. These samples, however, only provide a view of the final state, from which the initial conditions of a time-evolving magmatic system are then inferred. The interpretations that follow are inexact due to the inability of determining the exact conditions of nucleation and the potential detachment of bubbles from their nucleation sites, an uncertainty that can obscure their nucleation location - either homogeneously within the melt or heterogeneously at the interface between crystals and melts. We present results of a series of dynamic, real-time 4D X-ray tomographic microscopy experiments where we observed the development of bubbles in crystal bearing silicate magmas. Experimentally synthesized andesitic glasses with 0.25-0.5 wt% H2O and seed silicate crystals were heated at 1 atm to induce bubble nucleation and track bubble growth and movement. In contrast to previous studies on natural and experimentally produced samples, we found that bubbles readily nucleated on plagioclase and clinopyroxene crystals, that their contact angle changes during growth and that they can grow to sizes many times that of the silicate on whose surface they originated. The rapid heterogeneous nucleation of bubbles at low degrees of supersaturation in the presence of silicate crystals demonstrates that silicates can affect when vesiculation ensues, influencing subsequent permeability development and effusive vs. explosive transition in volcanic eruptions.
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UAV applications for thermodynamic profiling: Emphasis on ice fog research
Gultepe, Ismail; Heymsfield, Andrew J.; Fernando, Harindra J. S.; Hoch, Sebastian W.; Ware, Randolph
2016-04-01
Ice fog occurs often over the Arctic, cold climatic, and mountainous regions for about 30% of time where temperature (T) can go down to -10°C or below. Ice Nucleation (IN) and cooling processes play an important role by the controlling the intensity of ice fog conditions that affect aviation application, transportation, and local climate. Ice fog can also occur at T above -10°C but close to 0°C it occurs due to freezing of supercooled droplets that include an IN. To better document ice fog conditions, observations from the ice fog events of the Indirect and Semi-Direct Aerosol effects on Climate (ISDAC) project, Barrow, Alaska, Fog Remote Sensing And Modeling (FRAM) project Yellowknife, Northwest Territories, and the Mountain Terrain Atmospheric Modeling and Observations (MATERHORN) project, Heber City, Utah, were analyzed.. Measurements difficulties of small ice fog particles at cold temperatures and low-level flying restrictions prevent observations from aircraft within the surface boundary layer. However, unmanned Aerial Vehicles (UAVs) can be operated safely to measure IN number concentration, Relative Humidity with respect to ice (RHi), T, horizontal wind speed (Uh) and direction, and ice crystal spectra less than about 500 micron. Thermodynamic profiling by a Radiometrics Profiling Microwave Radiometer (PMWR) and Vaisala CL51 ceilometer was used to describe ice fog conditions in the vertical and its time development. In this presentation, ice fog characteristics and its thermodynamic environment will be presented using both ground-based and airborne platforms such as a UAV with new sensors. Some examples of measurements from the UAV for future research, and challenges related to both ice fog measurements and visibility parameterization will also be presented.
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New trends in the nucleation research
Anisimov, M. P.; Hopke, P. K.
2017-09-01
During the last half of century the most of efforts have been directed towards small molecule system modeling using intermolecular potentials. Summarizing the nucleation theory, it can be concluded that the nowadays theory is far from complete. The vapor-gas nucleation theory can produce values that deviate from the experimental results by several orders of magnitude currently. Experiments on the vapor-gas nucleation rate measurements using different devices show significant inconsistencies in the measured rates as well. Theoretical results generally are quite reasonable for sufficiently low vapor nucleation rates where the capillary approximation is applicable. In the present research the advantages and current problems of the vapor-gas nucleation experiments are discussed briefly and a view of the future studies is presented. Using the brake points of the first derivative for the nucleation rate surface as markers of the critical embryos phase change is fresh idea to show the gas-pressure effect for the nucleating vapor-gas systems. To test the accuracy of experimental techniques, it is important to have a standard system that can be measured over a range of nucleation conditions. Several results illustrate that high-pressure techniques are needed to study multi-channel nucleation. In practical applications, parametric theories can be used for the systems of interest. However, experimental measurements are still the best source of information on nucleation rates. Experiments are labor intensive and costly, and thus, it is useful to extend the value of limited experimental measurements to a broader range of nucleation conditions. Only limited experimental data one needs for use in normalizing the slopes of the linearized nucleation rate surfaces. The nucleation rate surface is described in terms of steady-state nucleation rates. It is supposed that several new measuring systems, such as High Pressure Flow Diffusion Chamber for pressure limit up to 150 bar will be
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Time-Lapse, in Situ Imaging of Ice Crystal Growth Using Confocal Microscopy.
Marcellini, Moreno; Noirjean, Cecile; Dedovets, Dmytro; Maria, Juliette; Deville, Sylvain
2016-11-30
Ice crystals nucleate and grow when a water solution is cooled below its freezing point. The growth velocities and morphologies of the ice crystals depend on many parameters, such as the temperature of ice growth, the melting temperature, and the interactions of solutes with the growing crystals. Three types of morphologies may appear: dendritic, cellular (or fingerlike), or the faceted equilibrium form. Understanding and controlling which type of morphology is formed is essential in several domains, from biology to geophysics and materials science. Obtaining, in situ, three dimensional observations without introducing artifacts due to the experimental technique is nevertheless challenging. Here we show how we can use laser scanning confocal microscopy to follow in real-time the growth of smoothed and faceted ice crystals in zirconium acetate solutions. Both qualitative and quantitative observations can be made. In particular, we can precisely measure the lateral growth velocity of the crystals, a measure otherwise difficult to obtain. Such observations should help us understand the influence of the parameters that control the growth of ice crystals in various systems.
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Neil, Chelsea W; Lee, Byeongdu; Jun, Young-Shin
2014-10-21
Iron(III) (hydr)oxides play an important role in the geochemical cycling of contaminants in natural and engineered aquatic systems. The ability of iron(III) (hydr)oxides to immobilize contaminants can be related to whether the precipitates form heterogeneously (e.g., at mineral surfaces) or homogeneously in solution. Utilizing grazing incidence small-angle X-ray scattering (GISAXS), we studied heterogeneous iron(III) (hydr)oxide nucleation and growth on quartz substrates for systems containing arsenate and phosphate anions. For the iron(III) only system, the radius of gyration (Rg) of heterogeneously formed precipitates grew from 1.5 to 2.5 (± 1.0) nm within 1 h. For the system containing 10(-5) M arsenate, Rg grew from 3.6 to 6.1 (± 0.5) nm, and for the system containing 10(-5) M phosphate, Rg grew from 2.0 to 4.0 (± 0.2) nm. While the systems containing these oxyanions had more growth, the system containing only iron(III) had the most nucleation events on substrates. Ex situ analyses of homogeneously and heterogeneously formed precipitates indicated that precipitates in the arsenate system had the highest water content and that oxyanions may bridge iron(III) hydroxide polymeric embryos to form a structure similar to ferric arsenate or ferric phosphate. These new findings are important because differences in nucleation and growth rates and particle sizes will impact the number of available reactive sites and the reactivity of newly formed particles toward aqueous contaminants.
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Minimum energy path for the nucleation of misfit dislocations in Ge/Si(0 0 1) heteroepitaxy
International Nuclear Information System (INIS)
Trushin, O; Maras, E; Jónsson, H; Ala-Nissila, T; Stukowski, A; Granato, E; Ying, S C
2016-01-01
A possible mechanism for the formation of a 90° misfit dislocation at the Ge/Si(0 0 1) interface through homogeneous nucleation is identified from atomic scale calculations where a minimum energy path connecting the coherent epitaxial state and a final state with a 90° misfit dislocation is found using the nudged elastic band method. The initial path is generated using a repulsive bias activation procedure in a model system including 75 000 atoms. The energy along the path exhibits two maxima in the energy. The first maximum occurs as a 60° dislocation nucleates. The intermediate minimum corresponds to an extended 60° dislocation. The subsequent energy maximum occurs as a second 60° dislocation nucleates in a complementary, mirror glide plane, simultaneously starting from the surface and from the first 60° dislocation. The activation energy of the nucleation of the second dislocation is 30% lower than that of the first one showing that the formation of the second 60° dislocation is aided by the presence of the first one. The simulations represent a step towards unraveling the formation mechanism of 90° dislocations, an important issue in the design of growth procedures for strain released Ge overlayers on Si(1 0 0) surfaces, and more generally illustrate an approach that can be used to gain insight into the mechanism of complex nucleation paths of extended defects in solids. (paper)
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Indirect radiative forcing by ion-mediated nucleation of aerosol
Directory of Open Access Journals (Sweden)
F. Yu
2012-12-01
Full Text Available A clear understanding of particle formation mechanisms is critical for assessing aerosol indirect radiative forcing and associated climate feedback processes. Recent studies reveal the importance of ion-mediated nucleation (IMN in generating new particles and cloud condensation nuclei (CCN in the atmosphere. Here we implement the IMN scheme into the Community Atmosphere Model version 5 (CAM5. Our simulations show that, compared to globally averaged results based on H2SO4-H2O binary homogeneous nucleation (BHN, the presence of ionization (i.e., IMN halves H2SO4 column burden, but increases the column integrated nucleation rate by around one order of magnitude, total particle number burden by a factor of ~3, CCN burden by ~10% (at 0.2% supersaturation to 65% (at 1.0% supersaturation, and cloud droplet number burden by ~18%. Compared to BHN, IMN increases cloud liquid water path by 7.5%, decreases precipitation by 1.1%, and increases total cloud cover by 1.9%. This leads to an increase of total shortwave cloud radiative forcing (SWCF by 3.67 W m−2 (more negative and longwave cloud forcing by 1.78 W m−2 (more positive, with large spatial variations. The effect of ionization on SWCF derived from this study (3.67 W m−2 is a factor of ~3 higher that of a previous study (1.15 W m−2 based on a different ion nucleation scheme and climate model. Based on the present CAM5 simulation, the 5-yr mean impacts of solar cycle induced changes in ionization rates on CCN and cloud forcing are small (~−0.02 W m−2 but have larger inter-annual (from −0.18 to 0.17 W m−2 and spatial variations.
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A nanoscale temperature-dependent heterogeneous nucleation theory
International Nuclear Information System (INIS)
Cao, Y. Y.; Yang, G. W.
2015-01-01
Classical nucleation theory relies on the hypothetical equilibrium of the whole nucleation system, and neglects the thermal fluctuations of the surface; this is because the high entropic gains of the (thermodynamically extensive) surface would lead to multiple stable states. In fact, at the nanometer scale, the entropic gains of the surface are high enough to destroy the stability of the thermal equilibrium during nucleation, comparing with the whole system. We developed a temperature-dependent nucleation theory to elucidate the heterogeneous nucleation process, by considering the thermal fluctuations based on classical nucleation theory. It was found that the temperature not only affected the phase transformation, but also influenced the surface energy of the nuclei. With changes in the Gibbs free energy barrier, nucleation behaviors, such as the nucleation rate and the critical radius of the nuclei, showed temperature-dependent characteristics that were different from those predicted by classical nucleation theory. The temperature-dependent surface energy density of a nucleus was deduced based on our theoretical model. The agreement between the theoretical and experimental results suggested that the developed nucleation theory has the potential to contribute to the understanding and design of heterogeneous nucleation at the nanoscale
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Climate change drives expansion of Antarctic ice-free habitat
Lee, Jasmine R.; Raymond, Ben; Bracegirdle, Thomas J.; Chadès, Iadine; Fuller, Richard A.; Shaw, Justine D.; Terauds, Aleks
2017-07-01
Antarctic terrestrial biodiversity occurs almost exclusively in ice-free areas that cover less than 1% of the continent. Climate change will alter the extent and configuration of ice-free areas, yet the distribution and severity of these effects remain unclear. Here we quantify the impact of twenty-first century climate change on ice-free areas under two Intergovernmental Panel on Climate Change (IPCC) climate forcing scenarios using temperature-index melt modelling. Under the strongest forcing scenario, ice-free areas could expand by over 17,000 km2 by the end of the century, close to a 25% increase. Most of this expansion will occur in the Antarctic Peninsula, where a threefold increase in ice-free area could drastically change the availability and connectivity of biodiversity habitat. Isolated ice-free areas will coalesce, and while the effects on biodiversity are uncertain, we hypothesize that they could eventually lead to increasing regional-scale biotic homogenization, the extinction of less-competitive species and the spread of invasive species.
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Li, Tanghua; Wu, Patrick; Steffen, Holger; Wang, Hansheng
2018-05-01
Most models of Glacial Isostatic Adjustment (GIA) assume that the Earth is laterally homogeneous. However, seismic and geological observations clearly show that the Earth's mantle is laterally heterogeneous. Previous studies of GIA with lateral heterogeneity mostly focused on its effect or sensitivity on GIA predictions, and it is not clear to what extent can lateral heterogeneity solve the misfits between GIA predictions and observations. Our aim is to search for the best 3D viscosity models that can simultaneously fit the global relative sea-level (RSL) data, the peak uplift rates (u-dot from GNSS) and peak gravity-rate-of-change (g-dot from the GRACE satellite mission) in Laurentia and Fennoscandia. However, the search is dependent on the ice and viscosity model inputs - the latter depends on the background viscosity and the seismic tomography models used. In this paper, the ICE-6G_C ice model, with Bunge & Grand's seismic tomography model and background viscosity models close to VM5 will be assumed. A Coupled Laplace-Finite Element Method is used to compute gravitationally self-consistent sea level change with time dependent coastlines and rotational feedback in addition to changes in deformation, gravity and the state of stress. Several laterally heterogeneous models are found to fit the global sea level data better than laterally homogeneous models. Two of these laterally heterogeneous models also fit the ICE-6G_C peak g-dot and u-dot rates observed in Laurentia simultaneously. However, even with the introduction of lateral heterogeneity, no model that is able to fit the present-day g-dot and uplift rate data in Fennoscandia has been found. Therefore, either the ice history of ICE-6G_C in Fennoscandia and Barent Sea needs some modifications, or the sub-lithospheric property/non-thermal effect underneath northern Europe must be different from that underneath Laurentia.
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Mechanisms of nucleation in flashing flows
International Nuclear Information System (INIS)
Yan, F.; Giot, M.
1989-01-01
The mechanisms of nucleation have been analysed. Starting from the assumption that the activation of micro-cavities in the wall surfaces is the most probable nucleation mechanism in practical flashing system, the authors study in detail the nucleation in a micro-cavity. A three step nucleation criterion is proposed, namely: trapping cavity, activable cavity and active cavity. Then, a new nucleation model is presented. The output of the model is the prediction of the bubble departure frequency versus the thermodynamic state of the liquid and the geometry of the cavity. The model can also predict the nucleation site density if the nature of the wall and the surface roughness are know. The prediction have been successfully compared with some preliminary experimental results. By combining the present model with Jones'theory, the flashing inception is correctly predicted. The use of this nucleation model for the complete modelling of a flashing non-equilibrium flow is in progress
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Heat transfer enhancement on nucleate boiling
International Nuclear Information System (INIS)
Zhuang, M.; Guibai, L.
1990-01-01
This paper reports on enhancement of nucleate boiling heat transfer with additives that was investigated experimentally. More than fifteen kinds of additives were chosen and tested. Eight kinds of effective additives which can enhance nucleate boiling heat transfer were selected. Experimental results showed that boiling heat transfer coefficient of water was increased by 1 to 5 times and that of R-113 was increased by 1 to 4 times when trace amount additives were put in the two boiling liquids. There exist optimum concentrations for the additives, respectively, which can enhance nucleate boiling heat transfer rate best. In order to analyze the mechanism of the enhancement of boiling heat transfer with additives, the surface tension and the bubble departure diameter were measured. The nucleation sites were investigated by use of high-speed photograph. Experimental results showed that nucleation sites increase with additive amount increasing and get maximum. Increasing nucleation sites is one of the most important reason why nucleate boiling heat transfer can be enhanced with additives
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The role of sodium bicarbonate in the nucleation of noctilucent clouds
Directory of Open Access Journals (Sweden)
J. M. C. Plane
2000-07-01
Full Text Available It is proposed that a component of meteoric smoke, sodium bicarbonate (NaHCO3, provides particularly effective condensation nuclei for noctilucent clouds. This assertion is based on three conditions being met. The first is that NaHCO3 is present at sufficient concentration (±104 cm-3 in the upper mesosphere between 80 and 90 km. It is demonstrated that there is strong evidence for this based on recent laboratory measurements coupled with atmospheric modelling. The second condition is that the thermodynamics of NaHCO3(H2On cluster formation allow spontaneous nucleation to occur under mesospheric conditions at temperatures below 140 K. The Gibbs free energy changes for forming clusters with n = 1 and 2 were computed from quantum calculations using hybrid density functional/Hartree-Fock (B3LYP theory and a large basis set with added polarization and diffuse functions. The results were then extrapolated to higher n using an established dependence of the free energy on cluster size and the free energy for the sublimation of H2O to bulk ice. A 1-dimensional model of sodium chemistry was then employed to show that spontaneous nucleation to form ice particles (n >100 should occur between 84 and 89 km in the high-latitude summer mesosphere. The third condition is that other metallic components of meteoric smoke are less effective condensation nuclei, so that the total number of potential nuclei is small relative to the amount of available H2O. Quantum calculations indicate that this is probably the case for major constituents such as Fe(OH2, FeO3 and MgCO3.Key words: Atmospheric composition and structure (aerosols and particles; cloud physics and chemistry; middle atmosphere · composition and chemistry
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Role of nucleation in nanodiamond film growth
International Nuclear Information System (INIS)
Lifshitz, Y.; Lee, C.H.; Wu, Y.; Zhang, W.J.; Bello, I.; Lee, S.T.
2006-01-01
Nanodiamond films were deposited using different microwave plasma chemical vapor deposition schemes following several nucleation pretreatment methods. The nucleation efficiency and the films structure were investigated using scanning and transmission electron microscopy and Raman spectroscopy. C 2 dimer growth (CH 4 and H 2 in 90% Ar) cannot nucleate diamond and works only on existing diamond surfaces. The methyl radical process (up to 20% CH 4 in H 2 ) allows some nucleation probability on appropriate substrates. Prolonged bias enhanced nucleation initiates both diamond nucleation and growth. C 2 dimer growth results in pure nanodiamond free of amorphous carbon, while prolonged bias enhanced nucleation forms an amorphous carbon/nanodiamond composite
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DEFF Research Database (Denmark)
van den Berg, Roy; Elkjær, Christian Fink; Gommes, Cedric J.
2016-01-01
The understanding of processes leading to the formation of nanometer-sized particles is important for tailoring of their size, shape and location. The growth mechanisms and kinetics of nanoparticles from solid precursors are, however, often poorly described. Here we employ transmission electron...... microscopy (TEM) to examine the formation of copper nanoparticles on a silica support during the reduction by H2 of homogeneous copper phyllosilicate platelets, as a prototype precursor for a coprecipitated catalyst. Specifically, time-lapsed TEM image series acquired of the material during the reduction...... process provide a direct visualization of the growth dynamics of an ensemble of individual nanoparticles and enable a quantitative evaluation of the nucleation and growth of the nanoparticles. This quantitative information is compared with kinetic models and found to be best described by a nucleation...
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Immersion freezing by SnomaxTM particles: Comparison of results from different instruments
Wex, Heike; Stratmann, Frank; Rösch, Michael; Niedermeier, Dennis; Nilius, Björn; Möhler, Ottmar; Mitra, Subir K.; Koop, Thomas; Jantsch, Evelyn; Hiranuma, Naruki; Diehl, Karoline; Curtius, Joachim; Budke, Carsten; Boose, Yvonne; Augustin, Stefanie
2014-05-01
to work equally well, hence freezing by SnomaxTM can be considered to show no time dependence. Particularly data from LACIS and BINARY, i.e. from the "fastest" and "slowest" measurements, were found to agree very well. Acknowledgement: This work was done within the framework of the DFG funded Ice Nucleation research UnIT (INUIT, FOR 1525). Literature Budke et al. (2013), Investigation of Heterogeneous Ice Nucleation Using a Novel Optical Freezing Array, AIP Conference Proceedings, 1527, 949-951, doi: 10.1064/1.4803429. Bundke et al. (2008), The fast Ice Nucleus chamber FINCH, Atmos. Res. 90, 180-186. Chou et al. (2011), Ice nuclei properties within a Saharan dust event at the Jungfraujoch in the Swiss Alps, Atmos. Chem. Phys., 11, 4725-4738. Connolly, et al. (2009), Studies of heterogeneous freezing by three different desert dust samples, Atmos. Chem. Phys., 9, 2805-2824. Diehl et al. (2011), The Mainz vertical wind tunnel facility: A review of 25 years of laboratory experiments on cloud physics and chemistry. In: J.D. Pereira (Ed.), Wind tunnels: Aerodynamics, models, and experiments. Nova Science Publishers, Inc., Chapter 2. Diehl et al. (2009), Homogeneous freezing of single sulfuric and nitric acid solution drops levitated in an acoustic trap, Atm. Res., 94, 356-361, doi:10.1016/j.atmosres.2009.06.001. Hartmann et al. (2011), Homogeneous and heterogeneous ice nucleation at LACIS: Operating principle and theoretical studies, Atmos. Chem. Phys., 11, 1753-1767. Hartmann et al. (2013), Immersion freezing of ice nucleating active protein complexes, Atmos. Chem. Phys., 13, 5751-5766. Murray et al. (2012), Ice nucleation by particles immersed in supercooled cloud droplets, Chem. Soc. Rev., 41, 6519-6554. Niedermeier et al. (2014), A computationally-efficient description of heterogeneous freezing: A simplified version of the Soccer ball model, Geophys. Res. Lett., 10.1002/2013GL058684. Vali, G. (1971), Quantitative evaluation of experimental results on heterogeneous
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Diamond Nucleation Using Polyethene
Morell, Gerardo (Inventor); Makarov, Vladimir (Inventor); Varshney, Deepak (Inventor); Weiner, Brad (Inventor)
2013-01-01
The invention presents a simple, non-destructive and non-abrasive method of diamond nucleation using polyethene. It particularly describes the nucleation of diamond on an electrically viable substrate surface using polyethene via chemical vapor deposition (CVD) technique in a gaseous environment.
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Energy Technology Data Exchange (ETDEWEB)
Boakye Yiadom, Solomon, E-mail: boakyeys@cc.umanitoba.ca; Khaliq Khan, Abdul, E-mail: abdulkhaliq.khan@umanitoba.ca; Bassim, Nabil, E-mail: nabil.bassim@ad.umanitoba.ca
2014-10-06
While instability may occur homogenously during plastic deformation, the formation of adiabatic shear band (ASBs) does not follow a homogenous instability during impact. Geometrical stress concentration sites and/or microstructural inhomogeneities result in the nucleation and initiation of shear strain localization. In this study, initial microstructural inhomogeneity was found to produce nucleation sites for the initiation of ASBs. It was observed that double misfit interfaces and boundary layers with random arrangement of atomic columns are formed around precipitated carbides and they increase the volume fraction of dislocation sources within the specimens. The AISI 4340 steel specimens which were tempered at the lowest temperature had smaller precipitated carbides with high aspect ratios densely distributed within the matrix and were easily susceptible to the formation of ASBs. As the tempering temperature increased, the relative sizes of the carbides increased with a corresponding reduction in their aspect ratios and their distribution density within the matrix and thus were more resistant to the formation of ASBs. In this study, it is demonstrated that the intersection of an activated dislocation source with the direction of maximum shear (regions of stress concentrations) within the specimens during impact, is a necessary condition for the point of intersection to act as a possible site for the nucleation of ASBs, depending on the rate of dislocation generation, local strain and strain rate. At a constant carbide volume fraction, the higher susceptibility of the tempered specimens to the initiation of ASBs is attributed to the volume fraction of the points of intersection between activated dislocation sources and direction of maximum shear during impact. Additionally, the smaller carbides, with their higher aspect ratios and distribution densities, accentuate the effect of strain gradients and the microstructural inhomogeneities associated with the tempered
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Probabilistic approach to lysozyme crystal nucleation kinetics.
Dimitrov, Ivaylo L; Hodzhaoglu, Feyzim V; Koleva, Dobryana P
2015-09-01
Nucleation of lysozyme crystals in quiescent solutions at a regime of progressive nucleation is investigated under an optical microscope at conditions of constant supersaturation. A method based on the stochastic nature of crystal nucleation and using discrete time sampling of small solution volumes for the presence or absence of detectable crystals is developed. It allows probabilities for crystal detection to be experimentally estimated. One hundred single samplings were used for each probability determination for 18 time intervals and six lysozyme concentrations. Fitting of a particular probability function to experimentally obtained data made possible the direct evaluation of stationary rates for lysozyme crystal nucleation, the time for growth of supernuclei to a detectable size and probability distribution of nucleation times. Obtained stationary nucleation rates were then used for the calculation of other nucleation parameters, such as the kinetic nucleation factor, nucleus size, work for nucleus formation and effective specific surface energy of the nucleus. The experimental method itself is simple and adaptable and can be used for crystal nucleation studies of arbitrary soluble substances with known solubility at particular solution conditions.
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Void nucleation at heterogeneities
International Nuclear Information System (INIS)
Seyyedi, S.A.; Hadji-Mirzai, M.; Russell, K.C.
The energetics and kinetics of void nucleation at dislocations and interfaces are analyzed. These are potential void nucleation sites only when they are not point defect sinks. Both kinds of site are found to be excellent catalysts in the presence of inert gas
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Delort, Anne-Marie; Vaïtilingom, Mickael; Amato, Pierre; Sancelme, Martine; Parazols, Marius; Mailhot, Gilles; Laj, Paolo; Deguillaume, Laurent
2010-11-01
Recent studies showed that living microorganisms, including bacteria, fungi and yeasts, are present in the atmospheric water phase (fog and clouds) and their role in chemical processes may have been underestimated. At the interface between atmospheric science and microbiology, information about this field of science suffers from the fact that not all recent findings are efficiently conveyed to both scientific communities. The purpose of this paper is therefore to provide a short overview of recent work linked to living organisms in the atmospheric water phase, from their activation to cloud droplets and ice crystal, to their potential impact on atmospheric chemical processes. This paper is focused on the microorganisms present in clouds and on the role they could play in atmospheric chemistry and nucleation processes. First, the life cycle of microorganisms via the atmosphere is examined, including their aerosolization from sources, their integration into clouds and their wet deposition on the ground. Second, special attention is paid to the possible impacts of microorganisms on liquid and ice nucleation processes. Third, a short description of the microorganisms that have been found in clouds and their variability in numbers and diversity is presented, emphasizing some specific characteristics that could favour their occurrence in cloud droplets. In the last section, the potential role of microbial activity as an alternative route to photochemical reaction pathways in cloud chemistry is discussed.
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Using rheometry for determining nucleation density in colored system containing a nucleation agent
Ma, Z.; Steenbakkers, R.J.A.; Giboz, J.; Peters, G.W.M.
2011-01-01
A new suspension-based rheological method was applied to study experimentally the crystallization of a nucleating agent (NA) filled isotactic polypropylene. This method allows for determination of point-nucleation densities where other methods fail. For example, optical microscopy can fail because
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D’Alessandro, John J.; Diao, Minghui; Wu, Chenglai; Liu, Xiaohong; Chen, Ming; Morrison, Hugh; Eidhammer, Trude; Jensen, Jorgen B.; Bansemer, Aaron; Zondlo, Mark A.;
2017-01-01
Occurrence frequency and dynamical conditions of ice supersaturation (ISS, where relative humidity with respect to ice (RHi) greater than 100%) are examined in the upper troposphere around convective activity. Comparisons are conducted between in situ airborne observations and the Weather Research and Forecasting model simulations using four double-moment microphysical schemes at temperatures less than or or equal to -40degdegC. All four schemes capture both clear-sky and in-cloud ISS conditions. However, the clear-sky (in-cloud) ISS conditions are completely (significantly) limited to the RHi thresholds of the Cooper parameterization. In all of the simulations, ISS occurrence frequencies are higher by approximately 3-4 orders of magnitude at higher updraft speeds (greater than 1 m s(exp -1) than those at the lower updraft speeds when ice water content (IWC) greater than 0.01 gm(exp -3), while observations show smaller differences up to approximately 1-2 orders of magnitude. The simulated ISS also occurs less frequently at weaker updrafts and downdrafts than observed. These results indicate that the simulations have a greater dependence on stronger updrafts to maintain/generate ISS at higher IWC. At lower IWC (less than or equal or 0.01 gm(exp -3), simulations unexpectedly show lower ISS frequencies at stronger updrafts. Overall, the Thompson aerosol-aware scheme has the closest magnitudes and frequencies of ISS greater than 20% to the observations, and the modified Morrison has the closest correlations between ISS frequencies and vertical velocity at higher IWC and number density. The Cooper parameterization often generates excessive ice crystals and therefore suppresses the frequency and magnitude of ISS, indicating that it should be initiated at higher ISS (e.g.,lees than or equal to 25%).
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Nucleation in Polymers and Soft Matter
Xu, Xiaofei; Ting, Christina L.; Kusaka, Isamu; Wang, Zhen-Gang
2014-04-01
Nucleation is a ubiquitous phenomenon in many physical, chemical, and biological processes. In this review, we describe recent progress on the theoretical study of nucleation in polymeric fluids and soft matter, including binary mixtures (polymer blends, polymers in poor solvents, compressible polymer-small molecule mixtures), block copolymer melts, and lipid membranes. We discuss the methodological development for studying nucleation as well as novel insights and new physics obtained in the study of the nucleation behavior in these systems.
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Fridlind, A. M.; Atlas, R.; van Diedenhoven, B.; Ackerman, A. S.; Rind, D. H.; Harrington, J. Y.; McFarquhar, G. M.; Um, J.; Jackson, R.; Lawson, P.
2017-12-01
It has recently been suggested that seeding synoptic cirrus could have desirable characteristics as a geoengineering approach, but surprisingly large uncertainties remain in the fundamental parameters that govern cirrus properties, such as mass accommodation coefficient, ice crystal physical properties, aggregation efficiency, and ice nucleation rate from typical upper tropospheric aerosol. Only one synoptic cirrus model intercomparison study has been published to date, and studies that compare the shapes of observed and simulated ice size distributions remain sparse. Here we amend a recent model intercomparison setup using observations during two 2010 SPARTICUS campaign flights. We take a quasi-Lagrangian column approach and introduce an ensemble of gravity wave scenarios derived from collocated Doppler cloud radar retrievals of vertical wind speed. We use ice crystal properties derived from in situ cloud particle images, for the first time allowing smoothly varying and internally consistent treatments of nonspherical ice capacitance, fall speed, gravitational collection, and optical properties over all particle sizes in our model. We test two new parameterizations for mass accommodation coefficient as a function of size, temperature and water vapor supersaturation, and several ice nucleation scenarios. Comparison of results with in situ ice particle size distribution data, corrected using state-of-the-art algorithms to remove shattering artifacts, indicate that poorly constrained uncertainties in the number concentration of crystals smaller than 100 µm in maximum dimension still prohibit distinguishing which parameter combinations are more realistic. When projected area is concentrated at such sizes, the only parameter combination that reproduces observed size distribution properties uses a fixed mass accommodation coefficient of 0.01, on the low end of recently reported values. No simulations reproduce the observed abundance of such small crystals when the
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Arienti, Marco; Geier, Manfred; Yang, Xiaoyuan; Orcutt, John; Zenker, Jake; Brooks, Sarah D.
2018-05-01
We investigate the optical properties of ice crystals nucleated on atmospheric black carbon (BC). The parameters examined in this study are the shape of the ice crystal, the volume fraction of the BC inclusion, and its location inside the crystal. We report on new spectrometer measurements of forward scattering and backward polarization from ice crystals nucleated on BC particles and grown under laboratory-controlled conditions. Data from the Cloud and Aerosol Spectrometer with Polarization (CASPOL) are used for direct comparison with single-particle calculations of the scattering phase matrix. Geometrical optics and discrete dipole approximation techniques are jointly used to provide the best compromise of flexibility and accuracy over a broad range of size parameters. Together with the interpretation of the trends revealed by the CASPOL measurements, the numerical results confirm previous reports on absorption cross-section magnification in the visible light range. Even taking into account effects of crystal shape and inclusion position, the ratio between absorption cross-section of the compound particle and the absorption cross-section of the BC inclusion alone (the absorption magnification) has a lower bound of 1.5; this value increases to 1.7 if the inclusion is centered with respect to the crystal. The simple model of BC-ice particle presented here also offers new insights on the effect of the relative position of the BC inclusion with respect to the crystal's outer surfaces, the shape of the crystal, and its size.
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Computer simulation of chemical nucleation
International Nuclear Information System (INIS)
Turner, J.S.
1979-01-01
The problem of nucleation at chemical instabilities is investigated by means of microscopic computer simulation. The first-order transition of interest involves a new kind of nucleation arising from chemical transformations rather than physical forces. Here it is the chemical state of matter, and not matter itself, which is spatially localized to form the nucleus for transition between different chemical states. First, the concepts of chemical instability, nonequilibrium phase transition, and dissipative structure are reviewed briefly. Then recently developed methods of reactive molecular dynamics are used to study chemical nucleation in a simple model chemical reactions. Finally, the connection of these studies to nucleation and condensation processes involving physical and chemical interactions is explored. (orig.)
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A classical view on nonclassical nucleation
Smeets, P.J.M.; Finney, A.R.; Habraken, W.J.E.M.; Nudelman, F.; Friedrich, H.; Laven, J.; De Yoreo, J.J.; Rodger, P.M.; Sommerdijk, N.A.J.M.
2017-01-01
Understanding and controlling nucleation is important for many crystallization applications. Calcium carbonate (CaCO3) is often used as a model system to investigate nucleation mechanisms. Despite its great importance in geology, biology, and many industrial applications, CaCO3 nucleation is still a
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Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea-ice
Humphries, R. S.; Klekociuk, A. R.; Schofield, R.; Keywood, M.; Ward, J.; Wilson, S. R.
2015-10-01
The effect of aerosols on clouds and their radiative properties is one of the largest uncertainties in our understanding of radiative forcing. A recent study has concluded that better characterisation of pristine, natural aerosol processes leads to the largest reduction in these uncertainties. Antarctica, being far from anthropogenic activities, is an ideal location for the study of natural aerosol processes. Aerosol measurements in Antarctica are often limited to boundary layer air-masses at spatially sparse coastal and continental research stations, with only a handful of studies in the sea ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the ice-breaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3) concentrations exhibited a five-fold increase moving across the Polar Front, with mean Polar Cell concentrations of 1130 cm-3 - higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air-masses quickly from the free-troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea ice boundary layer air-masses travelled equator-ward into the low albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei where, after growth, may potentially impact on the region's radiative balance. The high aerosol concentrations and
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Icing conditions over Northern Eurasia in changing climate
International Nuclear Information System (INIS)
Bulygina, Olga N; Arzhanova, Natalia M; Groisman, Pavel Ya
2015-01-01
Icing conditions, particularly in combination with wind, affect greatly the operation of overhead communication and transmission lines causing serious failures, which result in tremendous economic damage. Icing formation is dangerous to agriculture, forestry, high seas fishery, for land and off coast man-made infrastructure. Quantitative icing characteristics such as weight, thickness, and duration are very important for the economy and human wellbeing when their maximum values exceed certain thresholds. Russian meteorological stations perform both visual and instrumental monitoring of icing deposits. Visual monitoring is ocular estimation of the type and intensity of icing and the date of ice appearance and disappearance. Instrumental monitoring is performed by ice accretion indicator that in addition to the type, intensity and duration of ice deposits reports also their weight and size. We used observations at 958 Russian stations for the period 1977–2013 to analyze changes in the ice formation frequency at individual meteorological stations and on the territory of quasi-homogeneous climatic regions in Russia. It was found that hoar frosts are observed in most parts of Russia, but icing only occurs in European Russia and the Far East. On the Arctic coast of Russia, this phenomenon can even be observed in summer months. Statistically significant decreasing trends in occurrence of icing and hoar frost events are found over most of Russia. An increasing trend in icing weights (IWs) was found in the Atlantic Arctic region in autumn. Statistically significant large negative trends in IWs were found in the Pacific Arctic in winter and spring. (letter)
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Regular network model for the sea ice-albedo feedback in the Arctic.
Müller-Stoffels, Marc; Wackerbauer, Renate
2011-03-01
The Arctic Ocean and sea ice form a feedback system that plays an important role in the global climate. The complexity of highly parameterized global circulation (climate) models makes it very difficult to assess feedback processes in climate without the concurrent use of simple models where the physics is understood. We introduce a two-dimensional energy-based regular network model to investigate feedback processes in an Arctic ice-ocean layer. The model includes the nonlinear aspect of the ice-water phase transition, a nonlinear diffusive energy transport within a heterogeneous ice-ocean lattice, and spatiotemporal atmospheric and oceanic forcing at the surfaces. First results for a horizontally homogeneous ice-ocean layer show bistability and related hysteresis between perennial ice and perennial open water for varying atmospheric heat influx. Seasonal ice cover exists as a transient phenomenon. We also find that ocean heat fluxes are more efficient than atmospheric heat fluxes to melt Arctic sea ice.
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Lifanov, Yuri; Vorselaars, Bart; Quigley, David
2016-12-07
We study a three-species analogue of the Potts lattice gas model of nucleation from solution in a regime where partially disordered solute is a viable thermodynamic phase. Using a multicanonical sampling protocol, we compute phase diagrams for the system, from which we determine a parameter regime where the partially disordered phase is metastable almost everywhere in the temperature-fugacity plane. The resulting model shows non-trivial nucleation and growth behaviour, which we examine via multidimensional free energy calculations. We consider the applicability of the model in capturing the multi-stage nucleation mechanisms of polymorphic biominerals (e.g., CaCO 3 ). We then quantitatively explore the kinetics of nucleation in our model using the increasingly popular "seeding" method. We compare the resulting free energy barrier heights to those obtained via explicit free energy calculations over a wide range of temperatures and fugacities, carefully considering the propagation of statistical error. We find that the ability of the "seeding" method to reproduce accurate free energy barriers is dependent on the degree of supersaturation, and severely limited by the use of a nucleation driving force Δμ computed for bulk phases. We discuss possible reasons for this in terms of underlying kinetic assumptions, and those of classical nucleation theory.
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Chemically assisted crack nucleation in zircaloy
International Nuclear Information System (INIS)
Williford, R.E.
1985-01-01
Stress corrosion cracking models (proposed to explain fuel rod failures) generally address crack propagation and cladding rupture, but frequently neglect the necessary nucleation stage for microcracks small enough to violate fracture mechanics continuum requirements. Intergranular microcrack nucleation was modeled with diffusion-controlled grain-boundary cavitation concepts, including the effects of metal embrittlement by iodine species. Computed microcrack nucleation times and strains agree with experimental observation, but the predicted grain-boundary cavities are so small that detection may be difficult. Without a protective oxide film intergranular microcracks can nucleate within 30 s at even low stresses when the embrittler concentration exceeds a threshold value. Indications were found that intergranular microcrack nucleation may be caused by combined corrosive and embrittlement phenomena. (orig.)
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The influence of ions on atmospheric aerosol processes
DEFF Research Database (Denmark)
Enghoff, Martin
2008-01-01
Considering the big climate changes of the recent centuries and the predictions of future changes, it becomes increasingly important to understand what mechanisms drive climate. One such mechanism, that has been held responsible for changes in cloud cover during the last 25 years, for the Little...... Ice Age, the Medieval Warmth, and other climate phenomena going further back in time, is that of Ion Induced Nucleation { the ability of ions to enhance the formation of aerosol particles in the atmosphere. Several nucleation events that cannot be explained with the standard theory of homogeneous...... nucleation have been speculated to be caused by ions. Correlations between ionisation sources and climate parameters have been put forth, and experiments with extreme gas or ion concentrations have shown an eect of the ions. The relevance of Ion Induced Nucleation is, however, still undergoing debate [1, p...
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A classical density functional investigation of nucleation
International Nuclear Information System (INIS)
Ghosh, Satinath; Ghosh, Swapan K.
2009-01-01
Study of nucleation and growth phenomena in condensation is of prime importance in various applications such as crystal growth, nanoparticle synthesis, pattern formation etc. The knowledge of nucleation barrier in condensation is necessary to control the nucleation kinetics, size of the nanoparticles etc. Classical nucleation theory (CNT) assumes the density of the drop as bulk density irrespective of the size of the drop and overestimates the nucleation barrier. Here we are interested in solving the problem analytically using density functional theory (DFT) with square gradient approximation along the lines of Cahn and Hilliard. Nucleation barrier and density profile obtained in this work are consistent with other works based on nonclassical theory. (author)
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On Sea Ice Characterisation By Multi-Frequency SAR
Grahn, Jakob; Brekke, Camilla; Eltoft, Torbjorn; Holt, Benjamin
2013-12-01
By means of polarimetric target decomposition, quad-pol SAR data of sea ice is analysed at two frequency bands. In particular, the non negative eigenvalue decomposition (NNED) is applied on L- and C-band NASA/JPL AIR- SAR data acquired over the Beaufort sea in 2004. The de- composition separates the scattered radar signal into three types, dominated by double, volume and single bounce scattering respectively. Using ground truth derived from RADARSAT-1 and meteorological data, we investigate how the different frequency bands compare in terms of these scattering types. The ground truth contains multi year ice and three types of first year ice of different age and thickness. We find that C-band yields a higher scattered intensity in most ice and scattering types, as well as a more homogeneous intensity. L-band on the other hand yields more pronounced deformation features, such as ridges. The mean intensity contrast between the two thinnest ice types is highest in the double scattering component of C- band, although the contrast of the total signal is greater in L-band. This may indicate that the choice of polarimetric parameters is important for discriminating thin ice types.
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Nucleation of voids - the impurity effect
International Nuclear Information System (INIS)
Chen, I-W; Taiwo, A.
1984-01-01
Nucleation of voids under irradiation in multicomponent alloys remains an unsolved theoretical problem. Of particular interest are the effects of nonequilibrium solute segregation phenomena on the critical nucleus and the nucleation rate. The resolution of the multicomponent nucleation in a dissipative system also has broader implication to the field of irreversible thermodynamics. The present paper describes a recent study of solute segregation effects in void nucleation. We begin with a thermodynamic model for a nonequilibrium void with interfacial segregation. The thermodynamic model is coupled with kinetic considerations of solute/solvent diffusion under a bias, which is itself related to segregation by the coating effect, to assess the stability of void embryos. To determine nucleation rate, we develop a novel technique by extending the most probable path method in statistical mechanics for nonequilibrium steady state to simulate large fluctuation with nonlinear dissipation. The path of nucleation is determined by solving an analogous problem on particle trajectory in classical dynamics. The results of both the stability analysis and the fluctuation analysis establish the paramount significance of the impurity effect via the mechanism of nonequilibrium segregation. We conclude that over-segregation is probably the most general cause for the apparently low nucleation barriers that are responsible for nearly ubiquitous occurrence of void swelling in common metals
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Murata, K.; Tobo, Y.; Taketani, F.; Miyakawa, T.; Kanaya, Y.
2017-12-01
Measurement of ice-nucleating particles (INPs) was performed using aerosol samples collected during a cruise of R/V Mirai across the western North Pacific, Bering Sea, and Arctic Ocean from August to October, 2016. We used the National Institute of Polar Research Cryogenic Refrigerator Applied to Freezing Test (NIPR-CRAFT) device to examine the immersion freezing efficiency of the collected aerosols in the temperature range of -25°C to 0°C and measured the number concentration of atmospheric INPs. The INP concentrations varied over about three orders of magnitude during the cruise. Over the Arctic Ocean (i.e., >70°N), the INPs were simulations, extremely high concentrations of INPs during the returning leg would be attributed to transport of smoke from fires in Siberia. Different INP concentrations during the cruise indicates that INPs in marine air can vary dramatically in response to long-range transport of continental aerosols, such as smoke, in addition to local emissions from the sea surface. The observed concentrations of INPs were reasonably well expressed by power law fits with the number concentration of fluorescent biological aerosol particles simultaneously measured with a Waveband Integrated Bioaerosol Sensor (WIBS-4) during the cruise, which suggests that biological aerosol particles may play a role in determining INP populations in the marine air of this case.
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Directory of Open Access Journals (Sweden)
Piyush Kumar Jha
2017-10-01
Full Text Available Ice nucleation is a stochastic process and it is very difficult to be controlled. Freezing technologies and more specifically crystallisation assisted by magnetic, electric and electromagnetic fields have the capability to interact with nucleation. Static magnetic field (SMF may affect matter crystallisation; however, this is still under debate in the literature. Static electric field (SEF has a significant effect on crystallisation; this has been evidenced experimentally and confirmed by the theory. Oscillating magnetic field induces an oscillating electric field and is also expected to interact with water crystallisation. Oscillating electromagnetic fields interact with water, perturb and even disrupt hydrogen bonds, which in turn are thought to increase the degree of supercooling and to generate numerous fine ice crystals. Based on the literature, it seems that the frequency has an influence on the above-mentioned phenomena. This review article summarizes the fundamentals of freezing under magnetic, electric and electromagnetic fields, as well as their applicability and potentials within the food industry.
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Bao, Luyao; Huang, Zhaoyuan; Priezjev, Nikolai V.; Chen, Shaoqiang; Luo, Kai; Hu, Haibao
2018-04-01
It is well recognized that excessive ice accumulation at low-temperature conditions can cause significant damage to civil infrastructure. The passive anti-icing surfaces provide a promising solution to suppress ice nucleation and enhance ice removal. However, despite extensive efforts, it remains a challenge to design anti-icing surfaces with low ice adhesion. Using all-atom molecular dynamics (MD) simulations, we show that surfaces with single-walled carbon nanotube array (CNTA) significantly reduce ice adhesion due to the extremely low solid areal fraction. It was found that the CNTA surface exhibits up to a 45% decrease in the ice adhesion strength in comparison with the atomically smooth graphene surface. The details of the ice detachment from the CNTA surface were examined for different water-carbon interaction energies and temperatures of the ice cube. Remarkably, the results of MD simulations demonstrate that the ice detaching strength depends linearly on the ratio of the ice-surface interaction energy and the ice temperature. These results open the possibility for designing novel robust surfaces with low ice adhesion for passive anti-icing applications.
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Physical and chemical properties of ice residuals during the 2013 and 2014 CLACE campaigns
Kupiszewski, Piotr; Weingartner, Ernest; Vochezer, Paul; Hammer, Emanuel; Gysel, Martin; Färber, Raphael; Fuchs, Claudia; Schnaiter, Martin; Baltensperger, Urs; Schmidt, Susan; Schneider, Johannes; Bigi, Alessandro; Toprak, Emre; Linke, Claudia; Klimach, Thomas
2014-05-01
The shortcomings in our understanding and, thus, representation of aerosol-cloud interactions are one of the major sources of uncertainty in climate model projections. Among the poorly understood processes is mixed-phase cloud formation via heterogeneous nucleation, and the subsequent spatial and temporal evolution of such clouds. Cloud glaciation augments precipitation formation, resulting in decreased cloud cover and lifetime, and affects cloud radiative properties. Meanwhile, the physical and chemical properties of atmospherically relevant ice nuclei (IN), the sub-population of aerosol particles which enable heterogeneous nucleation, are not well known. Extraction of ice residuals (IR) in mixed-phase clouds is a difficult task, requiring separation of the few small, freshly formed ice crystals (the IR within such crystals can be deemed representative of the original IN) not only from interstitial particles, but also from the numerous supercooled droplets which have aerodynamic diameters similar to those of the ice crystals. In order to address the difficulties with ice crystal sampling and IR extraction in mixed-phase clouds, the new Ice Selective Inlet (ISI) has been designed and deployed at the Jungfraujoch field site. Small ice crystals are selectively sampled via the inlet with simultaneous counting, sizing and imaging of hydrometeors contained in the cloud by a set of optical particle spectrometers, namely Welas optical particle counters (OPC) and a Particle Phase Discriminator (PPD). The heart of the ISI is a droplet evaporation unit with ice-covered inner walls, resulting in removal of droplets using the Wegener-Bergeron-Findeisen process, while transmitting a relatively high fraction of small ice crystals. The ISI was deployed in the winters of 2013 and 2014 at the high alpine Jungfraujoch site (3580 m.a.s.l) during the intensive CLACE field campaigns. The measurements focused on analysis of the physical and chemical characteristics of IR and the
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Interaction of the nucleation phenomena at adjacent sites in nucleate boiling
International Nuclear Information System (INIS)
Sultan, M.; Judd, R.L.
1983-01-01
The present investigation is an original study in nucleate pool boiling heat transfer combining theory and experiment in which water boiling at atmospheric pressure on a single copper surface at two different levels of heat and different levels of subcooling was studied. Cross spectral analysis of the signals generated by the emission of bubbles at adjacent nucleation sites was used to determine the relationship of the time elapsed between the start of bubble growth at the two neighbouring active sites with the distance separating them. The experimental results obtained indicated that for the lower level of heat flux at three different levels of subcooling, the elapsed time and distance were directly related. Theoretical predictions of a temperature disturbance propagating through the heating surface in the radial direction gave good agreement with the experimental findings, suggesting that this is the mechanism responsible for the activation of the surrounding nucleation sites
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Radiation induced homogeneous precipitation in undersaturated solid-solutions
International Nuclear Information System (INIS)
Cauvin, Richard; Martin, Georges.
1978-01-01
The stability of various types of solid solutions under irradiation is studied. In this paper, observations made on AlZn solid solutions under 1 MeV electron irradiation are reported. Al-Zn was chosen as a prototype of solid solutions with a simple miscibility gap. It is shown that under appropriate irradiation conditions undersaturated AnZn solid solutions give rise to a homogeneous precipitation of coherent G.P. zones and of incoherent Zn precipitates the atomic volume of which is smaller than that of the matrix. We propose a more general treatment of solute concentration heterogeneities in solid solutions under irradiation and suggest how it might account for the nucleation of the observed phases. The growth of the observed precipitates is studied
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The nucleation process and the roles of structure and density fluctuations in supercooled liquid Fe
International Nuclear Information System (INIS)
Li, Rong; Wu, Yongquan; Xiao, Junjiang
2014-01-01
We observed homogeneous nucleation process of supercooled liquid Fe by molecular dynamics simulations. Using bond-orientational order parameters together with Voronoi polyhedron method, we characterized local structure, calculated the volume of Voronoi polyhedra of atoms and identified the structure and density fluctuations. We monitored the formation of nucleus and analyzed its inner structure. The birth and growth of the pre-nucleus and nucleus are accompanied with aggregating and disaggregating processes in the time scale of femtosecond. Only the initial solid-like clusters (ISLC), ranging from 1 to 7 atoms, pop up directly from liquid. The relation between the logarithm of number of clusters and the cluster size was found to be linear for ISLCs and was observed to be parabolic for all solid-like clusters (SLC) due to aggregating and disaggregating effects. The nucleus and pre-nuclei mainly consist of body centered cubic (BCC) and hexagonal close packed atoms, while the BCC atoms tend to be located at the surface. Medium-range structure fluctuations induce the birth of ISLCs, benefit the aggregation of embryos and remarkably promote the nucleation. But density fluctuations contribute little to nucleation. The lifetime of most icosahedral-like atoms (ICO) is shorter than 0.7 ps. No obvious relationship was found between structure/density fluctuations and the appearance of ICO atoms
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International Nuclear Information System (INIS)
Escobedo, Fernando A.
2016-01-01
The phase behavior and the homogeneous nucleation of an equimolar mixture of octahedra and cuboctahedra are studied using thermodynamic integration, Gibbs-Duhem integration, and umbrella sampling simulations. The components of this mixture are modeled as polybead objects of equal edge lengths so that they can assemble into a space-filling compound with the CsCl crystal structure. Taking as reference the hard-core system where the compound crystal does not spontaneously nucleate, we quantified the effect of inter-species selective interactions on facilitating the disorder-to-order transition. Facet selective and facet non-selective inter-species attractions were considered, and while the former was expectedly more favorable toward the target tessellating structure, the latter was found to be similarly effective in nucleating the crystal compound. Ranges for the strength of attractions and degree of supersaturation were identified where the nucleation free-energy barrier was small enough to foretell a fast process but large enough to prevent spinodal fluctuations that can trap the system in dense metastable states lacking long-range order. At those favorable conditions, the tendency toward the local orientational order favored by packing entropy is amplified and found to play a key role seeding nuclei with the CsCl structure.
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From glass to crystal - Nucleation, growth and de-mixing, from research to applications
International Nuclear Information System (INIS)
Neuville, Daniel R.; Cormier, Laurent; Caurant, Daniel; Montagne, Lionel; Charpentier, Thibault; Chevalier, Jerome; Comte, Monique; Dargaud, Olivier; Ligny, Dominique de; Deniard, Philippe; Dussardier, Bernard; Dussauze, Marc; Fargin, Evelyne; Gremillard, Laurent; Gredin, Patrick; Jousseaume, Cecile; Lafait, Jacques; Lancry, Mathieu; Lefebvre, Leila; Levelut, Claire; Magallanes-Pedromo, Marlin; Massiot, Dominique; Mear, Francois O.; Meille, Sylvain; Meng, Nicolas; Mortier, Michel; Papin, Sophie; Papon, Gautier; Pastouret, Main; Petit, Yannick; Poumellec, Bertrand; Pradel, Annie; Reillon, Vincent; Rodriguez, Vincent; Rogez, Jacques; Roussel, Pascal; Royon, Arnaud; Schuller, Sophie; Tricot, Gregory; Vigouroux, Helene
2013-01-01
This book first presents the conventional nucleation theory: vitrification, homogeneous and heterogeneous nucleation, induction time, crystal growth, Oswald law. The second part addresses the evolutions beyond this theory: cluster dynamics, validity of the Stokes-Einstein relationship, non conventional germ system, Gibbs generalized approach, two-stage model. The third part addresses the thermodynamic stability and the global kinetics of transformation: thermodynamic stability and instability of a vitreous system, phenomenological approach to transformation kinetics. The fourth part addresses the de-mixing process on glasses: thermodynamic description of phase separation, de-mixing kinetics, influence of glass structure on de-mixing trend, de-mixing characterisation. The next parts describe the crystal-chemical approach to the main crystalline phases noticed in glass-ceramics (silicate phases and phosphates), the elaboration and control of glass-ceramic microstructure (controllable parameters, elaboration processes, characterization methods, microstructure types, design of glass-ceramics with desired properties by control of crystallisation mechanisms), X ray diffraction in the case of glass-ceramics, calorimetry and differential thermal analysis for the study of glass ceramics, the application of electronic microscopy to the study of nucleation and crystallisation in glasses, small-angle scattering of X rays and neutrons, the use of nuclear magnetic resonance to understand the disorder and crystallisation in vitreous materials, the use of Raman spectrometry to study mechanisms of nucleation and crystal growth, large instruments aimed at an in situ approaches to crystallisation, commercial applications of glass-ceramics, applications of biomaterials in glass and glass-ceramics, the coloration of metal nanoparticles, transparent glass-ceramics, the formation and applications of nanoparticles in silica-based optic fibres, the both-way relationship between non linear
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Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea ice
Directory of Open Access Journals (Sweden)
R. S. Humphries
2016-02-01
Full Text Available Better characterisation of aerosol processes in pristine, natural environments, such as Antarctica, have recently been shown to lead to the largest reduction in uncertainties in our understanding of radiative forcing. Our understanding of aerosols in the Antarctic region is currently based on measurements that are often limited to boundary layer air masses at spatially sparse coastal and continental research stations, with only a handful of studies in the vast sea-ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the icebreaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3 concentrations exhibited a five-fold increase moving across the polar front, with mean polar cell concentrations of 1130 cm−3 – higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low-pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air masses quickly from the free troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea-ice boundary layer air masses travelled equatorward into the low-albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei which, after growth, may potentially impact on the region's radiative balance. The high aerosol concentrations and their transport pathways described here, could help reduce the discrepancy currently present between
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Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea ice
Humphries, R. S.; Klekociuk, A. R.; Schofield, R.; Keywood, M.; Ward, J.; Wilson, S. R.
2016-02-01
Better characterisation of aerosol processes in pristine, natural environments, such as Antarctica, have recently been shown to lead to the largest reduction in uncertainties in our understanding of radiative forcing. Our understanding of aerosols in the Antarctic region is currently based on measurements that are often limited to boundary layer air masses at spatially sparse coastal and continental research stations, with only a handful of studies in the vast sea-ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the icebreaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3) concentrations exhibited a five-fold increase moving across the polar front, with mean polar cell concentrations of 1130 cm-3 - higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low-pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air masses quickly from the free troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea-ice boundary layer air masses travelled equatorward into the low-albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei which, after growth, may potentially impact on the region's radiative balance. The high aerosol concentrations and their transport pathways described here, could help reduce the discrepancy currently present between simulations and observations of
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A theoretical analysis of flow through the nucleating stage in a low pressure steam turbine
International Nuclear Information System (INIS)
Skillings, S.A.; Walters, P.T.; Jackson, R.
1989-01-01
In order to improve steam turbine efficiency and reliability, the phenomena associated with the formation and growth of water droplets must be understood. This report describes a theoretical investigation into flow behaviour in the nucleating stage, where the predictions of a one-dimensional theory are compared with measured turbine data. Results indicate that droplet sizes predicted by homogeneous condensation theory cannot be reconciled with measurements unless fluctuating shock waves arise. Heterogeneous effects and flow turbulence are also discussed along with their implications for the condensation process. (author)
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Modelling ice microphysics of mixed-phase clouds
Ahola, J.; Raatikainen, T.; Tonttila, J.; Romakkaniemi, S.; Kokkola, H.; Korhonen, H.
2017-12-01
The low-level Arctic mixed-phase clouds have a significant role for the Arctic climate due to their ability to absorb and reflect radiation. Since the climate change is amplified in polar areas, it is vital to apprehend the mixed-phase cloud processes. From a modelling point of view, this requires a high spatiotemporal resolution to capture turbulence and the relevant microphysical processes, which has shown to be difficult.In order to solve this problem about modelling mixed-phase clouds, a new ice microphysics description has been developed. The recently published large-eddy simulation cloud model UCLALES-SALSA offers a good base for a feasible solution (Tonttila et al., Geosci. Mod. Dev., 10:169-188, 2017). The model includes aerosol-cloud interactions described with a sectional SALSA module (Kokkola et al., Atmos. Chem. Phys., 8, 2469-2483, 2008), which represents a good compromise between detail and computational expense.Newly, the SALSA module has been upgraded to include also ice microphysics. The dynamical part of the model is based on well-known UCLA-LES model (Stevens et al., J. Atmos. Sci., 56, 3963-3984, 1999) which can be used to study cloud dynamics on a fine grid.The microphysical description of ice is sectional and the included processes consist of formation, growth and removal of ice and snow particles. Ice cloud particles are formed by parameterized homo- or heterogeneous nucleation. The growth mechanisms of ice particles and snow include coagulation and condensation of water vapor. Autoconversion from cloud ice particles to snow is parameterized. The removal of ice particles and snow happens by sedimentation and melting.The implementation of ice microphysics is tested by initializing the cloud simulation with atmospheric observations from the Indirect and Semi-Direct Aerosol Campaign (ISDAC). The results are compared to the model results shown in the paper of Ovchinnikov et al. (J. Adv. Model. Earth Syst., 6, 223-248, 2014) and they show a good
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Lushnikov, A. A.; Kulmala, M.
1998-09-01
The dimer stage of nucleation may affect considerably the rate of the nucleation process at high supersaturation of the nucleating vapor. Assuming that the dimer formation limits the nucleation rate, the kinetics of the particle formation-growth process is studied starting with the definition of dimers as bound states of two associating molecules. The partition function of dimer states is calculated by summing the Boltzmann factor over all classical bound states, and the equilibrium population of dimers is found for two types of intermolecular forces: the Lennard-Jones (LJ) and rectangular well+hard core (RW) potentials. The principle of detailed balance is used for calculating the evaporation rate of dimers. The kinetics of the particle formation-growth process is then investigated under the assumption that the trimers are stable with respect to evaporation and that the condensation rate is a power function of the particle mass. If the power exponent λ=n/(n+1) (n is a non-negative integer), the kinetics of the process is described by a finite set of moments of particle mass distribution. When the characteristic time of the particle formation by nucleation is much shorter than that of the condensational growth, n+2 universal functions of a nondimensional time define the kinetic process. These functions are calculated for λ=2/3 (gas-to-particle conversion in the free molecular regime) and λ=1/2 (formation of islands on surfaces).
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Kiani, Hossein; Sun, Da-Wen; Delgado, Adriana; Zhang, Zhihang
2012-05-01
Nucleation, as an important stage of freezing process, can be induced by the irradiation of power ultrasound. In this study, the effect of irradiation temperature (-2 °C, -3 °C, -4 °C and -5 °C), irradiation duration (0s, 1s, 3s, 5s, 10s or 15s) and ultrasound intensity (0.07 W cm(-2), 0.14 W cm(-2), 0.25 W cm(-2), 0.35 W cm(-2) and 0.42 W cm(-2)) on the dynamic nucleation of ice in agar gel samples was studied. The samples were frozen in an ethylene glycol-water mixture (-20 °C) in an ultrasonic bath system after putting them into tubing vials. Results indicated that ultrasound irradiation is able to initiate nucleation at different supercooled temperatures (from -5 °C to -2 °C) in agar gel if optimum intensity and duration of ultrasound were chosen. Evaluation of the effect of 0.25 W cm(-2) ultrasound intensity and different durations of ultrasound application on agar gels showed that 1s was not long enough to induce nucleation, 3s induced the nucleation repeatedly but longer irradiation durations resulted in the generation of heat and therefore nucleation was postponed. Investigation of the effect of ultrasound intensity revealed that higher intensities of ultrasound were effective when a shorter period of irradiation was used, while lower intensities only resulted in nucleation when a longer irradiation time was applied. In addition to this, higher intensities were not effective at longer irradiation times due to the heat generated in the samples by the heating effect of ultrasound. In conclusion, the use of ultrasound as a means to control the crystallization process offers promising application in freezing of solid foods, however, optimum conditions should be selected. Copyright © 2011 Elsevier B.V. All rights reserved.
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Heterogeneous nucleation of calcium oxalate on native oxide surfaces
International Nuclear Information System (INIS)
Song, L.; Pattillo, M.J.; Graff, G.L.; Campbell, A.A.; Bunker, B.C.
1994-04-01
The aqueous deposition of calcium oxalate onto colloidal oxides has been studied as a model system for understanding heterogeneous nucleation processes of importance in biomimetic synthesis of ceramic thin films. Calcium oxalate nucleation has been monitored by measuring induction times for nucleation using Constant Composition techniques and by measuring nucleation densities on extended oxide surfaces using an atomic force microscope. Results show that the dependence of calcium oxalate nucleation on solution supersaturation fits the functional form predicted by classical nucleation theories. Anionic surfaces appear to promote nucleation better than cationic surfaces, lowering the effective energy barrier to heterogeneous nucleation
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Control of nucleation and crystal growth of a silicate apatitic phase in a glassy matrix
International Nuclear Information System (INIS)
Ligny, D.; Caurant, D.; Bardez, I.; Dussossoy, J.L.; Loiseau, P.; Neuville, D.R.
2004-01-01
Nucleation and growth of crystal in an oxide glass was studied in a Si B Al Zr Nd Ca Na O system. The nucleation and growth process were monitored by thermal analysis and isothermal experiments. The effect of the network modifier was studied. Therefore for a Ca rich sample the crystallization is homogeneous in the bulk showing a slow increase of crystallinity as temperature increases. On the other hand, a Na rich sample undergoes several crystallization processes in the bulk or from the surface, leading to bigger crystals. The activation energy of the viscous flow and the glass transition are of same magnitude when that of crystallization is a lot smaller. Early diffusion of element is done with a mechanism different than the configurational rearrangements of the liquid sate. The global density and small size of the crystals within the Ca rich matrix confirmed that it would be a profitable waste form for minor actinides. (authors)
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Non-classical homogeneous precipitation mediated by compositional fluctuations in titanium alloys
International Nuclear Information System (INIS)
Nag, S.; Zheng, Y.; Williams, R.E.A.; Devaraj, A.; Boyne, A.; Wang, Y.; Collins, P.C.; Viswanathan, G.B.; Tiley, J.S.; Muddle, B.C.; Banerjee, R.
2012-01-01
This paper presents experimental evidence of homogeneous precipitation of the α-phase within the β matrix of a titanium alloy, and then accounts for this phase transformation by a new, non-classical mechanism involving compositional fluctuations, based on the pseudo-spinodal concept [1]. This mechanism involves local compositional fluctuations of small amplitude which, when of a certain magnitude, can favor thermodynamically certain regions of the β matrix to transform congruently to the α-phase but with compositions far from equilibrium. Subsequently, as measured experimentally using the tomographical atom probe, continuous diffusional partitioning between the parent β- and product α-phases during isothermal annealing drives their compositions towards equilibrium. For a given alloy composition, the decomposition mechanism is strongly temperature dependent, which would be expected for homogeneous precipitation via the compositional fluctuation-mediated mechanism but not necessarily for one based on classical nucleation theory. The applicability of this mechanism to phase transformations in general is noted.
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Nucleation behavior of glutathione polymorphs in water
International Nuclear Information System (INIS)
Chen, Zhi; Dang, Leping; Li, Shuai; Wei, Hongyuan
2013-01-01
Nucleation behavior of glutathione (GSH) polymorphs in water was investigated by experimental method combined with classical nucleation theory. The solubility of α and β forms GSH in water at different temperatures, and the nucleation induction period at various supersaturations and temperatures were determined experimentally. The results show that, in a certain range of supersaturation, the nucleation of β form predominates at relatively higher temperature, while α form will be obtained at lower temperature. The nucleation kinetics parameters of α and β form were then calculated. To understand the crucial role of temperature on crystal forms, “hypothetic” nucleation parameters of β form at 283.15 K were deduced based on extrapolation method. The results show that the interfacial tension, critical free energy, critical nucleus radius and nucleus number of α form are smaller than that of β form in the same condition at 283.15 K, which implies that α form nucleates easier than β form at low temperature. This work may be useful for the control and optimization of GSH crystallization process in industry
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Nucleation in an ultra low ionization environment
DEFF Research Database (Denmark)
Pedersen, Jens Olaf Pepke; Enghoff, Martin Andreas Bødker; Paling, Sean
Atmospheric ions can enhance the nucleation of aerosols, as has been established by experiments, observation, and theory. In the clean marine atmosphere ionization is mainly caused by cosmic rays which in turn are controlled by the activity of the Sun, thus providing a potential link between solar...... activity and climate. In order to understand the effect ions may have on the production of cloud condensation nuclei the overall contribution of ion induced nucleation to the global production of secondary aerosols must be determined. One issue with determining this contribution is that several mechanisms...... for nucleation exist and it can be difficult to determine the relative importance of the various mechanisms in a given nucleation event when both ion induced and electrically neutral nucleation mechanisms are at work at the same time. We have carried out nucleation experiments in the Boulby Underground...