Effect of ageing of K-feldspar on its ice nucleating efficiency in immersion, deposition and contact freezing modes

Science.gov (United States)

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

High variability of the heterogeneous ice nucleation potential of oxalic acid dihydrate and sodium oxalate

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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

High variability of the heterogeneous ice nucleation potential of oxalic acid dihydrate and sodium oxalate

Science.gov (United States)

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

Role of stacking disorder in ice nucleation.

Science.gov (United States)

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.

Influence of the ambient humidity on the concentration of natural deposition-mode ice-nucleating particles

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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.

Modelling heterogeneous ice nucleation on mineral dust and soot with parameterizations based on laboratory experiments

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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.

Heterogeneous ice nucleation

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.)

Ice nucleating particles in the Saharan Air Layer

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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

Heterogeneous Ice Nucleation Ability of NaCl and Sea Salt Aerosol Particles at Cirrus Temperatures

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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.

Janus effect of antifreeze proteins on ice nucleation.

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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.

A theory-based parameterization for heterogeneous ice nucleation and implications for the simulation of ice processes in atmospheric models

Science.gov (United States)

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.

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).

Immersion freezing of ice nucleation active protein complexes

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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

Tuning Ice Nucleation with Supercharged Polypeptides

NARCIS (Netherlands)

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

Heterogeneous ice nucleation and phase transition of viscous α-pinene secondary organic aerosol

Science.gov (United States)

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

Glassy aerosols with a range of compositions nucleate ice heterogeneously at cirrus temperatures

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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, n_s, of the aerosols tested here and also of glassy citric acid aerosol as a function of relative humidity with respect to ice (RH_i. 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.

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

Dynamics of ice nucleation on water repellent surfaces.

Science.gov (United States)

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.

Urediospores of rust fungi are ice nucleation active at > -10 °C and harbor ice nucleation active bacteria

Science.gov (United States)

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 �

Urediospores of Puccinia spp. and other rusts are warm-temperature ice nucleators and harbor ice nucleation active bacteria

Science.gov (United States)

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

Impact of surface nanostructure on ice nucleation.

Science.gov (United States)

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.

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.

Ice nucleation activity of polysaccharides

Science.gov (United States)

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

Probing Individual Ice Nucleation Events with Environmental Scanning Electron Microscopy

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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.

Ice nucleation active bacteria in precipitation are genetically diverse and nucleate ice by employing different mechanisms.

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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.

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].

Homogeneous ice nucleation from aqueous inorganic/organic particles representative of biomass burning: water activity, freezing temperatures, nucleation rates.

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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

Ice nucleation efficiency of AgI: review and new insights

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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.

Freezing nucleation apparatus puts new slant on study of biological ice nucleators in precipitation

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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.

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)

Bioinspired Materials for Controlling Ice Nucleation, Growth, and Recrystallization.

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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

Chemical composition, mixing state, size and morphology of Ice nucleating particles at the Jungfraujoch research station, Switzerland

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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

The enhancement and suppression of immersion mode heterogeneous ice-nucleation by solutes.

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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

An aerosol chamber investigation of the heterogeneous ice nucleating potential of refractory nanoparticles

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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 (RHi_thresh 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 RHi_thresh = 140% at an initial chamber temperature of 182 K. Quantitative analysis using a singular hypothesis treatment provided a fitted function [n_s(190 K=10^{(3.33×s_ice+8.16}] for the variation in ice-active surface site density (n_s:m⁻² with ice saturation (s_ice 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

The effects of ice on methane hydrate nucleation: a microcanonical molecular dynamics study.

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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.

The Ice Nucleation Activity of Surface Modified Soot

Science.gov (United States)

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

Thermodynamic Derivation of the Activation Energy for Ice Nucleation

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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

Heterogeneous ice nucleation in aqueous solutions: the role of water activity.

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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.

Heterogeneous Ice Nucleation: Interplay of Surface Properties and Their Impact on Water Orientations.

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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.

Controlled ice nucleation using freeze-dried Pseudomonas syringae encapsulated in alginate beads.

Science.gov (United States)

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.

Ice cloud processing of ultra-viscous/glassy aerosol particles leads to enhanced ice nucleation ability

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

A simulation study of homogeneous ice nucleation in supercooled salty water

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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.

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

Investigation of heterogeneous ice nucleation in pollen suspensions and washing water

Science.gov (United States)

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

Laboratory, Computational and Theoretical Investigations of Ice Nucleation and its Implications for Mixed Phase Clouds

Science.gov (United States)

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

Ice Nucleation Activity of Various Agricultural Soil Dust Aerosol Particles

Science.gov (United States)

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

Inhibition of ice nucleation by slippery liquid-infused porous surfaces (SLIPS).

Science.gov (United States)

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.

Immersion Freezing of Aluminas: The Effect of Crystallographic Properties on Ice Nucleation

Science.gov (United States)

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.

The barrier to ice nucleation in monatomic water

Science.gov (United States)

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.

The relevance of nanoscale biological fragments for ice nucleation in clouds

Science.gov (United States)

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.

Effect of Controlled Ice Nucleation on Stability of Lactate Dehydrogenase During Freeze-Drying.

Science.gov (United States)

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.

Understanding ice nucleation characteristics of selective mineral dusts suspended in solution

Science.gov (United States)

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

Understanding the ice nucleation characteristics of feldspars suspended in solution

Science.gov (United States)

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

Ice nucleation on nanotextured surfaces: the influence of surface fraction, pillar height and wetting states.

Science.gov (United States)

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.

Ice nucleating particles measured during the laboratory and field intercomparisons FIN-2 and FIN-3 by the diffusion chamber FRIDGE

Science.gov (United States)

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.

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.

Single Particle Laser Mass Spectrometry Applied to Differential Ice Nucleation Experiments at the AIDA Chamber

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

Nonthermal ice nucleation observed at distorted contact lines of supercooled water drops.

Science.gov (United States)

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.

Small particles big effect? - Investigating ice nucleation abilities of soot particles

Science.gov (United States)

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

Understanding Cirrus Ice Crystal Number Variability for Different Heterogeneous Ice Nucleation Spectra

Science.gov (United States)

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.

Identification & Characterization of Fungal Ice Nucleation Proteins

Science.gov (United States)

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.

Functional display of ice nucleation protein InaZ on the surface of bacterial ghosts.

Science.gov (United States)

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).

Heterogeneous ice nucleation of viscous secondary organic aerosol produced from ozonolysis of α-pinene

Science.gov (United States)

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.

Cloud condensation nuclei and ice nucleation activity of hydrophobic and hydrophilic soot particles.

Science.gov (United States)

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.

Ice nucleation active particles are efficiently removed by precipitating clouds

OpenAIRE

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 ...

submitter Heterogeneous ice nucleation of viscous secondary organic aerosol produced from ozonolysis of α-pinene

CERN Document Server

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...

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.

The effect of organic coating on the heterogeneous ice nucleation efficiency of mineral dust aerosols

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.

The effect of organic coating on the heterogeneous ice nucleation efficiency of mineral dust aerosols

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

Pre-activation of ice-nucleating particles by the pore condensation and freezing mechanism

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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.

Ice nucleation rates near ˜225 K

Science.gov (United States)

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.

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.

Heterogeneous Ice Nucleation by Soufriere Hills Volcanic Ash Immersed in Water Droplets.

Science.gov (United States)

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.

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

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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.

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

Science.gov (United States)

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.

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

Ice nucleation and cloud microphysical properties in tropical tropopause layer cirrus

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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.

Direct calculation of ice homogeneous nucleation rate for a molecular model of water

Science.gov (United States)

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

Screening of plant resources with anti-ice nucleation activity for frost damage prevention.

Science.gov (United States)

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.

Investigation of nucleation processes during dynamic recrystallization of ice using cryo-EBSD.

Science.gov (United States)

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).

High variability of the heterogeneous ice nucleation potential of oxalic acid dihydrate and sodium oxalate

OpenAIRE

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 ...

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

On the Importance of High Frequency Gravity Waves for Ice Nucleation in the Tropical Tropopause Layer

Science.gov (United States)

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.

A new thermal gradient ice nucleation diffusion chamber instrument: design, development and first results using Saharan mineral dust

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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 (SS_i 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 SS_i 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 SS_i. The design of the TGDC gives the ability to understand time-related ice nucleation event information and to perform experiments at different temperatures and SS_i conditions for different IN without changing the thermal gradient within the TGDC. The temperature and SS_i 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 SS_i 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.

Ice Nucleation of Soot Particles in the Cirrus Regime: Is Pore Condensation and Freezing Relevant for Soot?

Science.gov (United States)

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.

Ice nucleation of ammonia gas exposed montmorillonite mineral dust particles

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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.

Model simulations with COSMO-SPECS: impact of heterogeneous freezing modes and ice nucleating particle types on ice formation and precipitation in a deep convective cloud

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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

Ice nucleation in sulfuric acid/organic aerosols: implications for cirrus cloud formation

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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.

Parametrization of the homogeneous ice nucleation rate for the numerical simulation of multiphase flow

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

The influence of organic-containing soil dust on ice nucleation and cloud properties

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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

Analysis of the Effect of Water Activity on Ice Formation Using a New Theory of Nucleation

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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.

Impact of bacterial ice nucleating particles on weather predicted by a numerical weather prediction model

Science.gov (United States)

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.

New species of ice nucleating fungi in soil and air

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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

High-density amorphous ice: nucleation of nanosized low-density amorphous ice

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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.

Inhibition of nucleation and growth of ice by poly(vinyl alcohol) in vitrification solution.

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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.

A novel optical freezing array for the examination of cooling rate dependence in heterogeneous ice nucleation

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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.

Ice nucleation properties of mineral dust particles: determination of onset RHi, IN active fraction, nucleation time-lag, and the effect of active sites on contact angles

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.

Engineering functional nanothin multilayers on food packaging: ice-nucleating polyethylene films.

Science.gov (United States)

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.

Ice-nucleating particle concentrations unaffected by urban air pollution in Beijing, China

Science.gov (United States)

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.

Uncertainty in counting ice nucleating particles with continuous flow diffusion chambers

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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.

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.

Analysis of isothermal and cooling-rate-dependent immersion freezing by a unifying stochastic ice nucleation model

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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

Magnetic control of heterogeneous ice nucleation with nanophase magnetite: Biophysical and agricultural implications.

Science.gov (United States)

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.

Viscous organic aerosol particles in the upper troposphere: diffusivity-controlled water uptake and ice nucleation?

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.

Ice nucleation properties of atmospheric aerosol particles collected during a field campaign in Cyprus

Science.gov (United States)

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).

Direct Quantification of Ice Nucleation Active Bacteria in Aerosols and Precipitation: Their Potential Contribution as Ice Nuclei

Science.gov (United States)

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

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

Ice nucleation onto Arizona test dust at cirrus temperatures: effect of temperature and aerosol size on onset relative humidity.

Science.gov (United States)

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.

The global influence of dust mineralogical composition on heterogeneous ice nucleation in mixed-phase clouds

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)

Analysis of isothermal and cooling-rate-dependent immersion freezing by a unifying stochastic ice nucleation model

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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

Sensitivity of warm-frontal processes to cloud-nucleating aerosol concentrations

Science.gov (United States)

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.

Heterogeneous ice nucleation activity of bacteria: new laboratory experiments at simulated cloud conditions

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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.

Global model comparison of heterogeneous ice nucleation parameterizations in mixed phase clouds

Science.gov (United States)

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.

On the role of ice-nucleating aerosol in the formation of ice particles in tropical mesoscale convective systems

Science.gov (United States)

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

Nucleation in Synoptically Forced Cirrostratus

Science.gov (United States)

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.

Ice nucleation by surrogates for atmospheric mineral dust and mineral dust/sulfate particles at cirrus temperatures

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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.

Measurements of ice nucleating particle concentrations at 242 K in the free troposphere

Science.gov (United States)

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

In-situ measurements of ice nucleating particles with FINCH (Fast Ice Nucleus Chamber)

Science.gov (United States)

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

Ice Nucleation in the Tropical Tropopause Layer: Implications for Cirrus Occurrence, Cirrus Microphysical Properties, and Dehydration of Air Entering the Stratosphere

Science.gov (United States)

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.

Ice-nucleating particle emissions from photochemically aged diesel and biodiesel exhaust

Science.gov (United States)

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.

Progress Towards Identifying and Quantifying the Organic Ice Nucleating Particles in Soils and Aerosols

Science.gov (United States)

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

Snow-borne nanosized particles: Abundance, distribution, composition, and significance in ice nucleation processes

Science.gov (United States)

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.

Analysis of isothermal and cooling rate dependent immersion freezing by a unifying stochastic ice nucleation model

Science.gov (United States)

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

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.

Characterization of Ice Nucleating Particles at the Western US Coast

Science.gov (United States)

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

Characterization of ice nucleating particles during continuous springtime measurements in Prudhoe Bay: an Arctic oilfield location

Science.gov (United States)

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

Ice nucleation activity of diesel soot particles at cirrus relevant temperature conditions: Effects of hydration, secondary organics coating, soot morphology, and coagulation

Science.gov (United States)

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.

Ice nucleating particles over the Eastern Mediterranean measured at ground and by unmanned aircraft systems

Science.gov (United States)

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

Technical Note: A numerical test-bed for detailed ice nucleation studies in the AIDA cloud simulation chamber

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.

Ice nucleating particles in the high Arctic at the beginning of the melt season

Science.gov (United States)

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.

A laboratory investigation on the influence of adsorbed gases and particles from the exhaust of a kerosene burner on the evaporation rate of ice crystals and the ice nucleating ability of the exhaust particles

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.

A laboratory investigation on the influence of adsorbed gases and particles from the exhaust of a kerosene burner on the evaporation rate of ice crystals and the ice nucleating ability of the exhaust particles

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.

Effect of pretreatment and deposition parameters on diamond nucleation in CVD

International Nuclear Information System (INIS)

Nazim, E.; Izman, S.; Ourdjini, A.; Shaharoun, A.M.

2007-01-01

Chemical vapour deposition (CVD) of diamond films on cemented carbide (WC) has aroused great interest in recent years. The combination of toughness from the WC and the high hardness of diamond results in outstanding wear resistance. This will increase the lifetime and better technical performance of the components made of diamond coated carbide. One of the important steps in the growth of diamond film is the nucleation of diamond as its density strongly influences the diamond growth process, film quality and morphology. In this paper the various effects of surface pretreatment and diamond deposition conditions on the diamond nucleation density are reviewed. (author)

Anomalous Behavior of the Homogeneous Ice Nucleation Rate in “No-Man’s Land”

Science.gov (United States)

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

Freezing on a Chip—A New Approach to Determine Heterogeneous Ice Nucleation of Micrometer-Sized Water Droplets

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.

Phospholipid analysis and fractional reconstitution of the ice nucleation protein activity purified from Escherichia coli overexpressing the inaZ gene of Pseudomonas syringae.

Science.gov (United States)

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.

Anti-icing/frosting and self-cleaning performance of superhydrophobic aluminum alloys

Science.gov (United States)

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.

Nucleation and growth of copper phthalocyanine aggregates deposited from solution on planar surfaces

Energy Technology Data Exchange (ETDEWEB)

Ghani, Fatemeh [Department of Theory & Bio-Systems, Max Planck Institute of Colloids and Interfaces, Am Mühlenberg 1 Golm, 14476 Potsdam (Germany); Gojzewski, Hubert, E-mail: hubert.gojzewski@put.poznan.pl [Department of Theory & Bio-Systems, Max Planck Institute of Colloids and Interfaces, Am Mühlenberg 1 Golm, 14476 Potsdam (Germany); Institute of Physics, Poznan University of Technology, Piotrowo 3, 60-965 Poznan (Poland); Riegler, Hans [Department of Theory & Bio-Systems, Max Planck Institute of Colloids and Interfaces, Am Mühlenberg 1 Golm, 14476 Potsdam (Germany)

2015-10-01

Graphical abstract: - Highlights: • Copper phthalocyanine deposited on planar surfaces by 3 solution process methods. • Aggregate morphology examined for coverage extending over 3 orders of magnitude. • Morphologies vary from small individual domains to mesh-like multilayers. • Nucleation and growth model explains the observed deposit morphologies. - Abstract: Copper phthalocyanine (CuPc) dissolved in trifluoroacetic acid (TFA) is deposited on solid SiO{sub 2} surfaces by solvent evaporation. The deposited CuPc aggregates are investigated by atomic force microscopy (AFM). The CuPc deposits were prepared by spin casting, dip coating, and spray deposition. Depending on the amount of deposited CuPc the aggregate morphology ranges from small individual domains to mesh-like multilayers. Each domain/layer consists of many parallel stacks of CuPc molecules with the square, plate-like molecules piled face-wise within each stack. The parallel stacks are attached sideways (i.e., edgewise attachment molecularly) to the substrate forming “nanoribbons” with uniform thickness of about 1 nm and varying width. The thickness reflects the length of a molecular edge, the width the number of stacks. A nucleation and growth model is presented that explains the observed aggregate and multilayer morphologies as result of the combination of nucleation, transport processes and a consequence of the anisotropic intermolecular interactions due to the shape of the CuPc molecule.

Overview: Nucleation of clathrate hydrates.

Science.gov (United States)

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.

Overview: Nucleation of clathrate hydrates

Science.gov (United States)

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.

Responses of Mixed-Phase Cloud Condensates and Cloud Radiative Effects to Ice Nucleating Particle Concentrations in NCAR CAM5 and DOE ACME Climate Models

Science.gov (United States)

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.

Spores of many common airborne fungi reveal no ice nucleation activity in oil immersion freezing experiments

Science.gov (United States)

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.

Contributions of Heterogeneous Ice Nucleation, Large-Scale Circulation, and Shallow Cumulus Detrainment to Cloud Phase Transition in Mixed-Phase Clouds with NCAR CAM5

Science.gov (United States)

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

Evaluating Ice Nucleating Particle Concentrations From Prognostic Dust Minerals in an Earth System Model

Science.gov (United States)

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.

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

Ice-nucleation negative fluorescent pseudomonads isolated from Hebridean cloud and rain water produce biosurfactants

Science.gov (United States)

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.

Single-particle characterization of ice-nucleating particles and ice particles residuals sampled by three different techniques

Science.gov (United States)

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

Ice crystallization in ultrafine water-salt aerosols: nucleation, ice-solution equilibrium, and internal structure.

Science.gov (United States)

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

Increase in Ice Nucleation Efficiency of Feldspars, Kaolinite and Mica in Dilute NH3 and NH4+-containing Solutions

Science.gov (United States)

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

High ice nucleation activity located in blueberry stem bark is linked to primary freeze initiation and adaptive freezing behaviour of the bark

Science.gov (United States)

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

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<T_on^std<242 K and best sites with averaged median freezing temperature T_med^best=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 T_on^std<246 K and best sites with averaged median freezing temperature T_med^best=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

Long-range-transported bioaerosols captured in snow cover on Mount Tateyama, Japan: impacts of Asian-dust events on airborne bacterial dynamics relating to ice-nucleation activities

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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

Long-range-transported bioaerosols captured in snow cover on Mount Tateyama, Japan: impacts of Asian-dust events on airborne bacterial dynamics relating to ice-nucleation activities

Science.gov (United States)

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

A water activity based model of heterogeneous ice nucleation kinetics for freezing of water and aqueous solution droplets.

Science.gov (United States)

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

Simulation and experiment of the unsteady heat transport in the onset time of nucleation and crystallization of ice from the subcooled solution

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)

Sea ice dynamics influence halogen deposition to Svalbard

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A. Spolaor

2013-10-01

Full Text Available Sea ice is an important parameter in the climate system and its changes impact upon the polar albedo and atmospheric and oceanic circulation. Iodine (I and bromine (Br have been measured in a shallow firn core drilled at the summit of the Holtedahlfonna glacier (Northwest Spitsbergen, Svalbard. Changing I concentrations can be linked to the March–May maximum sea ice extension. Bromine enrichment, indexed to the Br / Na sea water mass ratio, appears to be influenced by changes in the seasonal sea ice area. I is emitted from marine biota and so the retreat of March–May sea ice coincides with enlargement of the open-ocean surface which enhances marine primary production and consequent I emission. The observed Br enrichment could be explained by greater Br emissions during the Br explosions that have been observed to occur mainly above first year sea ice during the early springtime. In this work we present the first comparison between halogens in surface snow and Arctic sea ice extension. Although further investigation is required to characterize potential depositional and post-depositional processes, these preliminary findings suggest that I and Br can be linked to variability in the spring maximum sea ice extension and seasonal sea ice surface area.

Isolating and identifying atmospheric ice-nucleating aerosols: a new technique

Science.gov (United States)

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.

Adsorption and structure of water on kaolinite surfaces: possible insight into ice nucleation from grand canonical monte carlo calculations.

Science.gov (United States)

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.

How the Emitted Size Distribution and Mixing State of Feldspar Affect Ice Nucleating Particles in a Global Model

Science.gov (United States)

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.

How the Emitted Size Distribution and Mixing State of Feldspar Affect Ice Nucleating Particles in a Global Model

Science.gov (United States)

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.

Endogenous and exogenous ice-nucleating agents constrain supercooling in the hatchling painted turtle.

Science.gov (United States)

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

Ice Nucleating Particle Properties in the Saharan Air Layer Close to the Dust Source

Science.gov (United States)

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

Interannual observations and quantification of summertime H2O ice deposition on the Martian CO2 ice south polar cap

Science.gov (United States)

Brown, Adrian J.; Piqueux, Sylvain; Titus, Timothy N.

2014-01-01

The spectral signature of water ice was observed on Martian south polar cap in 2004 by the Observatoire pour l'Mineralogie, l'Eau les Glaces et l'Activite (OMEGA) ( Bibring et al., 2004). Three years later, the OMEGA instrument was used to discover water ice deposited during southern summer on the polar cap ( Langevin et al., 2007). However, temporal and spatial variations of these water ice signatures have remained unexplored, and the origins of these water deposits remains an important scientific question. To investigate this question, we have used observations from the Compact Reconnaissance Imaging Spectrometer for Mars (CRISM) instrument on the Mars Reconnaissance Orbiter (MRO) spacecraft of the southern cap during austral summer over four Martian years to search for variations in the amount of water ice. We report below that for each year we have observed the cap, the magnitude of the H2O ice signature on the southern cap has risen steadily throughout summer, particularly on the west end of the cap. The spatial extent of deposition is in disagreement with the current best simulations of deposition of water ice on the south polar cap (Montmessin et al., 2007). This increase in water ice signatures is most likely caused by deposition of atmospheric H2O ice and a set of unusual conditions makes the quantification of this transport flux using CRISM close to ideal. We calculate a ‘minimum apparent‘ amount of deposition corresponding to a thin H2O ice layer of 0.2 mm (with 70% porosity). This amount of H2O ice deposition is 0.6–6% of the total Martian atmospheric water budget. We compare our ‘minimum apparent’ quantification with previous estimates. This deposition process may also have implications for the formation and stability of the southern CO2 ice cap, and therefore play a significant role in the climate budget of modern day Mars.

Glaciochemical investigations of the ice deposit of Vukušić Ice Cave, Velebit Mountain, Croatia

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Z. Kern

2011-06-01

Full Text Available The ³H activity and the concentration of 23 metals and metalloids have been analysed in cave ice samples from the perennial cave ice deposit of Vukušić Ice Cave, Velebit Mt., Croatia. The results of tritium measurements exclude a secular age for the upper 2.4 m of ice deposition, and provide clear arguments that the sampled ice sequence consists of frozen post-1950 precipitation. Measured concentrations of most of the analysed elements have largely surmounted reported concentrations of similar elements from local precipitation or Alpine snow/firn/ice records, whereas three metals (Cr, Cu, Pb show concentrations comparable to them. Principal component analysis was used to select three groups of elements. The Ca-Mg-governed group (PC1 encompasses the bedrock-related components; their fluctuation might thus reflect the past intensity of dissolution in the epikarst. PC2, with the most characteristic elements being Na, Cr and Pb, probably preserved an atmospheric depositional signal. PC3 is governed by Al and Fe. This probably carries the distal, non-karstic crustal signal and hence might be related to atmospheric circulation (i.e., wind direction and speed.

Nucleation/Growth Mechanisms and Morphological Evolution of Porous MnO2 Coating Deposited on Graphite for Supercapacitor

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Wenxin Huang

2017-10-01

Full Text Available The nucleation and growth mechanisms of porous MnO2 coating deposited on graphite in MnSO4 solution were investigated in detail by cyclic voltammetry, chronoamperometry and scanning electron microscopy. The electrochemical properties of honeycomb-like MnO2 were evaluated by cycle voltammetry and galvanostatic charge-discharge. Results indicated that MnO2 was synthesized by the following steps: Mn2+→ Mn3++ e-, Mn3++2H2O → MnOOH + 3H+, and MnOOH → MnO2 + H++ e-. The deposition of MnO2 was divided into four stages. A short incubation period (approximately 1.5 s was observed, prior to nucleation. The decreasing trend of the current slowed as time increased due to nucleation and MnO2 growth in the second stage. A huge number of nuclei were formed by instantaneous nucleation, and these nuclei grew and connected with one another at an exceedingly short time (0.5 s. In the third stage, the gaps in-between initial graphite flakes were filled with MnO2 until the morphology of the flakes gradually became similar to that of the MnO2-deposited layer. In the fourth stage, the graphite electrode was covered completely with a thick and dense layer of MnO2 deposits. All MnO2 electrodes at different deposition times obtained nearly the same specific capacitance of approximately 186 F/g, thus indicating that the specific capacitance of the electrodes is not related with deposition time.

Snow algae and lichen algae differ in their resistance to freezing temperature: An ice nucleation study

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

Experiments in Ice Contaminant Remanent Magnetization of Dusty Frost Deposits

Science.gov (United States)

Grossman, Y.; Aharonson, O.; Shaar, R.

2017-12-01

Sedimentary rocks can acquire magnetization in the presence of an external field as grains settle out of suspension in a water column - a process known as Depositional Remanent Magnetization (DRM). In analogy with this, here we propose and experimentally demonstrate a new mechanism for acquisition of magnetization by ice and particulate mixtures which we term Ice Contaminant Remanent Magnetization (ICRM). This phenomenon results from the settling of atmospheric dust containing magnetic particles (e.g. magnetite or other iron oxides). Upon freezing, magnetic dust particles assume a preferential orientation that depends on the external planetary field, resulting in bulk magnetization of the dusty ice. Hence over geologic timescales, the ice stratigraphy is expected to record the geomagnetic history. To test this hypothesis, we designed a set of experiments in which mixtures of ice and dust were deposited in a controlled ambient magnetic field environment. We measured the ratio between the volume normalized magnetization of the dusty ice (m) and the applied field (H) during deposition of the mixture, which is expressed as the effective ICRM susceptibility: m=χICRMH. A magnetic field was applied by a 3-axis Helmholtz coil at the Weizmann Simulating Planetary Ices & Environments Laboratory, and the frozen samples were analyzed in a 2G-Entreprises SQUID Rock Magnetometer at the Hebrew University Institute for Earth Sciences. We measured a clear correlation in amplitude and direction between the ambient magnetic field applied during deposition and the remanent magnetic moment of the resulting samples. We studied various concentrations and particle sizes (diameters 5 µm to 50 µm) of iron and magnetite particles. Effective bulk susceptibilities show a range of values, starting from 10-3 and up to values that saturate the analytical instrument. Our preliminary results indicate that natural ice deposits may acquire variable magnetization due to ICRM, which may in turn be

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)

Bacterial Ice Crystal Controlling Proteins

Science.gov (United States)

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

Nanoscale-Agglomerate-Mediated Heterogeneous Nucleation.

Science.gov (United States)

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.

High-definition infrared thermography of ice nucleation and propagation in wheat under natural frost conditions and controlled freezing

Science.gov (United States)

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...

The use of high-resolution infrared thermography (HRIT) for the study of ice nucleation and ice propagation in plants.

Science.gov (United States)

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.

Fluorescent pseudomonads isolated from Hebridean cloud and rain water produce biosurfactants but do not cause ice nucleation

Science.gov (United States)

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.

The Horizontal Ice Nucleation Chamber (HINC): INP measurements at conditions relevant for mixed-phase clouds at the High Altitude Research Station Jungfraujoch

Science.gov (United States)

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

Turning into Ice

Science.gov (United States)

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…

Does deposition freezing really exist? At least different as we thought

Science.gov (United States)

Abdelmonem, Ahmed

2017-04-01

The structural and chemical properties of the surface of an IN-particle (INP) play a major role in its IN ability. This role is not well explored in terms of water/INP-surface molecular-level interactions. Recent MD simulations on deposition freezing showed that water first deposits as liquid clusters and then crystallize isothermally from there [1]. We probe freezing of water on INPs of different structural and chemical properties under varying supersaturation conditions using non-linear optical spectroscopy, mainly second harmonic generation (SHG) and sum frequency generation (SFG) [2, 3]. This presentation will show very recent preliminary experimental results comparing deposition, condensation and immersion freezing (DF, CF and IF respectively) on an atmospheric relevant metal oxide surface (mica) using supercooled SHG measurements. It is found that the signal drops upon the formation of a thin film regardless of 1) the freezing path (DF or CF), 2) the formed phase (ice or liquid), indicating a similar molecular structuring. The observed structuring similarity between DF, CF and LC films is a kick-off experimental confirmation of those computational results. References 1. Lupi, L., N. Kastelowitz, and V. Molinero, Vapor deposition of water on graphitic surfaces: Formation of amorphous ice, bilayer ice, ice I, and liquid water. The Journal of Chemical Physics, 2014. 141(18): p. 18C508. 2. Abdelmonem, A., J. Lützenkirchen, and T. Leisner, Probing ice-nucleation processes on the molecular level using second harmonic generation spectroscopy. Atmospheric Measurement Techniques, 2015. 8(8): p. 3519-3526. 3. Abdelmonem, A., et al., Surface charge-induced orientation of interfacial water suppresses heterogeneous ice nucleation on α-alumina (0001). Angewandte Chemie (Submitted), 2017.

Single-particle characterization of ice-nucleating particles and ice particle residuals sampled by three different techniques

Science.gov (United States)

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

What controls the low ice number concentration in the upper troposphere?

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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

Sea spray as a source of ice nucleating particles - results from the AIDA Ocean03 campaign

Science.gov (United States)

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.

Rate of Homogenous Nucleation of Ice in Supercooled Water.

Science.gov (United States)

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.

Atmospheric Ice Nucleating Particle measurements at the high mountain observatory Mt. Cimone (2165 m a.s.l., Italy)

Science.gov (United States)

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.

Predicting abundance and variability of ice nucleating particles in precipitation at the high-altitude observatory Jungfraujoch

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.

The Horizontal Ice Nucleation Chamber (HINC: INP measurements at conditions relevant for mixed-phase clouds at the High Altitude Research Station Jungfraujoch

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

Ice condensation on sulfuric acid tetrahydrate: Implications for polar stratospheric ice clouds

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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.

Frazil-ice growth rate and dynamics in mixed layers and sub-ice-shelf plumes

Science.gov (United States)

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.

Spores of most common airborne fungi reveal no ice nucleation activity

Science.gov (United States)

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.

Diamond-coated three-dimensional GaN micromembranes: effect of nucleation and deposition techniques

Czech Academy of Sciences Publication Activity Database

Ižák, Tibor; Vanko, G.; Babchenko, Oleg; Potocký, Štěpán; Marton, M.; Vojs, M.; Choleva, P.; Kromka, Alexander

2015-01-01

Roč. 252, č. 11 (2015), s. 2585-2590 ISSN 0370-1972 R&D Projects: GA ČR(CZ) GP14-16549P Institutional support: RVO:68378271 Keywords : diamond film * GaN micromembranes * microwave chemical vapour deposition * polymer-based nucleation Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 1.522, year: 2015

Nucleation and growth of microdroplets of ionic liquids deposited by physical vapor method onto different surfaces

Science.gov (United States)

Costa, José C. S.; Coelho, Ana F. S. M. G.; Mendes, Adélio; Santos, Luís M. N. B. F.

2018-01-01

Nanoscience and technology has generated an important area of research in the field of properties and functionality of ionic liquids (ILs) based materials and their thin films. This work explores the deposition process of ILs droplets as precursors for the fabrication of thin films, by means of physical vapor deposition (PVD). It was found that the deposition (by PVD on glass, indium tin oxide, graphene/nickel and gold-coated quartz crystal surfaces) of imidazolium [C4mim][NTf2] and pyrrolidinium [C4C1Pyrr][NTf2] based ILs generates micro/nanodroplets with a shape, size distribution and surface coverage that could be controlled by the evaporation flow rate and deposition time. No indication of the formation of a wetting-layer prior to the island growth was found. Based on the time-dependent morphological analysis of the micro/nanodroplets, a simple model for the description of the nucleation process and growth of ILs droplets is presented. The proposed model is based on three main steps: minimum free area to promote nucleation; first order coalescence; second order coalescence.

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

Pathogenic and Ice-Nucleation Active (INA) Bacteria causing Dieback of Willows in Short Rotation Forestry

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

Use of the Single Particle Soot Photometer (SP2) as a pre-filter for ice nucleation measurements: effect of particle mixing state and determination of SP2 conditions to fully vaporize refractory black carbon

Science.gov (United States)

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

Nucleation in the atmosphere

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

The potential influence of Asian and African mineral dust on ice, mixed-phase and liquid water clouds

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

Modeling the Sulfate Deposition to the Greenland Ice Sheet From the Laki Eruption

Science.gov (United States)

Oman, L.; Robock, A.; Stenchikov, G.; Thordarson, T.; Gao, C.

2005-12-01

Using the state of the art Goddard Institute for Space Studies (GISS) modelE general circulation model, simulations were conducted of the chemistry and transport of aerosols resulting from the 1783-84 Laki (64°N) flood lava eruption. A set of 3 ensemble simulations from different initial conditions were conducted by injecting our estimate of the SO2 gas into the atmosphere by the 10 episodes of the eruption and allowing the sulfur chemistry model to convert this gas into sulfate aerosol. The SO2 gas and sulfate aerosol is transported by the model and wet and dry deposition is calculated over each grid box during the simulation. We compare the resulting sulfate deposition to the Greenland Ice Sheet in the model to 23 ice core measurements and find very good agreement. The model simulation deposits a range of 169 to over 300 kg/km2 over interior Greenland with much higher values along the coastal areas. This compares to a range of 62 to 324 kg/km2 for the 23 ice core measurements with an average value of 158 kg/km2. This comparison is one important model validation tool. Modeling and observations show fairly large spatial variations in the deposition of sulfate across the Greenland Ice Sheet for the Laki eruption, but the patterns are similar to those we modeled for the 1912 Katmai and 1991 Pinatubo eruptions. Estimates of sulfate loading based on single ice cores can show significant differences, so ideally several ice cores should be combined in reconstructing the sulfate loading of past volcanic eruptions, taking into account the characteristic spatial variations in the deposition pattern.

Micro-Spectroscopic Chemical Imaging of Individual Identified Marine Biogenic and Ambient Organic Ice Nuclei (Invited)

Science.gov (United States)

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

On the Role of Ammonia in Arctic Aerosol Nucleation and Cloud Formation

Science.gov (United States)

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.

Diamond Nucleation Using Polyethene

Science.gov (United States)

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.

Studies of propane flame soot acting as heterogeneous ice nuclei in conjunction with single particle soot photometer measurements

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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 S_ice ~ 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 S_ice = 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

The Contribution of Black Carbon to Ice Nucleating Particle Concentrations from Prescribed Burns and Wildfires

Science.gov (United States)

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.

Anatomical regulation of ice nucleation and cavitation helps trees to survive freezing and drought stress

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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

Isolation, Characterization, and Genetic Diversity of Ice Nucleation Active Bacteria on Various Plants

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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.

Isolation, Characterization, and Genetic Diversity of Ice Nucleation Active Bacteria on Various Plants

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.

Investigation of the nucleation process of chemical vapour deposited diamond films

International Nuclear Information System (INIS)

Katai, S.

2001-01-01

The primary aim of this work was to contribute to the understanding of the bias enhanced nucleation (BEN) process during the chemical vapour deposition (CVD) of diamond on silicon. The investigation of both the gas phase environment above the substrate surface, by in situ mass selective energy analysis of ions, and of the surface composition and structure by in vacuo surface analytic methods (XPS, EELS) have been carried out. In both cases, the implementation of these measurements required the development and construction of special experimental apparatus as well. The secondary aim of this work was to give orientation to our long term goal of growing diamond films with improved quality. For this reason, (1) contaminant levels at the diamond-silicon interface after growth were studied by SIMS, (2) the internal stress distribution of highly oriented free-standing diamond films were studied by Raman spectroscopy, and (3) an attempt was made to produce spatially regular oriented nuclei formation by nucleating on a pattern created by laser treatment on silicon substrates. (orig.)

Survival and ice nucleation activity of bacteria as aerosols in a cloud simulation chamber

Science.gov (United States)

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.

Subaqueous ice-contact fans: Depositional systems characterised by highly aggradational supercritical flow conditions

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Lang, Joerg; Winsemann, Jutta

2015-04-01

Subaqueous ice-contact fans are deposited by high-energy plane-wall jets from subglacial conduits into standing water bodies. Highly aggradational conditions during flow expansion and deceleration allow for the preservation of bedforms related to supercritical flows, which are commonly considered rare in the depositional record. We present field examples from gravelly and sandy subaqueous ice-contact fan successions, which indicate that deposition by supercritical flows might be considered as a characteristic feature of these depositional systems. The studied successions were deposited in deep ice-dammed lakes, which formed along the margins of the Middle Pleistocene Scandinavian ice sheets across Northern Germany. The gravel-rich subaqueous fan deposits are dominated by large scour-fills (up to 25 m wide and 3 m) deep and deposits of turbulent hyperconcentrated flows, which are partly attributed to supercritical flow conditions (Winsemann et al., 2009). Scours (up to 4.5 m wide and 0.9 m deep) infilled by gravelly backsets are observed above laterally extensive erosional surfaces and are interpreted as deposits of cyclic steps. Laterally discontinuous beds of low-angle cross-stratified gravel are interpreted as antidune deposits. Downflow and up-section the gravel-rich deposits pass into sand-rich successions, which include deposits of chutes-and-pools, breaking antidunes, stationary antidunes and humpback dunes (Lang and Winsemann, 2013). Deposits of chutes-and-pools and breaking antidunes are characterised by scour-fills (up to 4 m wide and 1.2 m deep) comprising backsets or gently dipping sigmoidal foresets. Stationary antidune deposits consist of laterally extensive sinusoidal waveforms with long wavelengths (1-12 m) and low amplitudes (0.1-0.5 m), which formed under quasi-steady flows at the lower limit of the supercritical flow stage and high rates of sedimentation. Humpback dunes are characterised by divergent sigmoidal foresets and are interpreted as

NUCLEATION STUDIES OF GOLD ON CARBON ELECTRODES

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S. SOBRI

2008-04-01

Full Text Available Interest has grown in developing non-toxic electrolytes for gold electrodeposition to replace the conventional cyanide-based bath for long term sustainability of gold electroplating. A solution containing thiosulphate and sulphite has been developed specially for microelectronics applications. However, at the end of the electrodeposition process, the spent electrolyte can contain a significant amount of gold in solution. This study has been initiated to investigate the feasibility of gold recovery from a spent thiosulphate-sulphite electrolyte. We have used flat-plate glassy carbon and graphite electrodes to study the mechanism of nucleation and crystal growth of gold deposition from the spent electrolyte. It was found that at the early stages of reduction process, the deposition of gold on glassy carbon exhibits an instantaneous nucleation of non-overlapping particles. At longer times, the particles begin to overlap and the deposition follows a classic progressive nucleation phenomenon. On the other hand, deposition of gold on graphite does not follow the classical nucleation phenomena.

Deposition uniformity, particle nucleation and the optimum conditions for CVD in multi-wafer furnaces

Energy Technology Data Exchange (ETDEWEB)

Griffiths, S.K.; Nilson, R.H.

1996-06-01

A second-order perturbation solution describing the radial transport of a reactive species and concurrent deposition on wafer surfaces is derived for use in optimizing CVD process conditions. The result is applicable to a variety of deposition reactions and accounts for both diffusive and advective transport, as well as both ordinary and Knudsen diffusion. Based on the first-order approximation, the deposition rate is maximized subject to a constraint on the radial uniformity of the deposition rate. For a fixed reactant mole fraction, the optimum pressure and optimum temperature are obtained using the method of Lagrange multipliers. This yields a weak one-sided maximum; deposition rates fall as pressures are reduced but remain nearly constant at all pressures above the optimum value. The deposition rate is also maximized subject to dual constraints on the uniformity and particle nucleation rate. In this case, the optimum pressure, optimum temperature and optimum reactant fraction are similarly obtained, and the resulting maximum deposition rate is well defined. These results are also applicable to CVI processes used in composites manufacturing.

Synthesis of Functional Ceramic Supports by Ice Templating and Atomic Layer Deposition

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Michaela Klotz

2018-05-01

Full Text Available In this work, we report an innovative route for the manufacturing of functional ceramic supports, by combining ice templating of yttria stabilized zirconia (YSZ and atomic layer deposition (ALD of Al2O3 processes. Ceramic YSZ monoliths are prepared using the ice-templating process, which is based on the controlled crystallization of water following a thermal gradient. Sublimation of the ice and the sintering of the material reveal the straight micrometer sized pores shaped by the ice crystal growth. The high temperature sintering allows for the ceramic materials to present excellent mechanical strength and porosities of 67%. Next, the conformality benefit of ALD is used to deposit an alumina coating at the surface of the YSZ pores, in order to obtain a functional material. The Al2O3 thin films obtained by ALD are 100 nm thick and conformally deposited within the macroporous ceramic supports, as shown by SEM and EDS analysis. Mercury intrusion experiments revealed a reduction of the entrance pore diameter, in line with the growth per cycle of 2 Å of the ALD process. In addition to the manufacture of the innovative ceramic nanomaterials, this article also describes the fine characterization of the coatings obtained using mercury intrusion, SEM and XRD analysis.

Midlatitude Cirrus Clouds Derived from Hurricane Nora: A Case Study with Implications for Ice Crystal Nucleation and Shape.

Science.gov (United States)

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

Numerical simulations of contrail-to-cirrus transition – Part 2: Impact of initial ice crystal number, radiation, stratification, secondary nucleation and layer depth

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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.

Diversity and Abundance of Ice Nucleating Strains of Pseudomonas syringae in a Freshwater Lake in Virginia, USA.

Science.gov (United States)

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.

Investigating Freezing Point Depression and Cirrus Cloud Nucleation Mechanisms Using a Differential Scanning Calorimeter

Science.gov (United States)

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…

Major new sources of biological ice nuclei

Science.gov (United States)

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.

Automation and heat transfer characterization of immersion mode spectroscopy for analysis of ice nucleating particles

Science.gov (United States)

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

The impact of atmospheric mineral aerosol deposition on the albedo of snow & sea ice: are snow and sea ice optical properties more important than mineral aerosol optical properties?

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M. L. Lamare

2016-01-01

Full Text Available Knowledge of the albedo of polar regions is crucial for understanding a range of climatic processes that have an impact on a global scale. Light-absorbing impurities in atmospheric aerosols deposited on snow and sea ice by aeolian transport absorb solar radiation, reducing albedo. Here, the effects of five mineral aerosol deposits reducing the albedo of polar snow and sea ice are considered. Calculations employing a coupled atmospheric and snow/sea ice radiative-transfer model (TUV-snow show that the effects of mineral aerosol deposits are strongly dependent on the snow or sea ice type rather than the differences between the aerosol optical characteristics. The change in albedo between five different mineral aerosol deposits with refractive indices varying by a factor of 2 reaches a maximum of 0.0788, whereas the difference between cold polar snow and melting sea ice is 0.8893 for the same mineral loading. Surprisingly, the thickness of a surface layer of snow or sea ice loaded with the same mass ratio of mineral dust has little effect on albedo. On the contrary, the surface albedo of two snowpacks of equal depth, containing the same mineral aerosol mass ratio, is similar, whether the loading is uniformly distributed or concentrated in multiple layers, regardless of their position or spacing. The impact of mineral aerosol deposits is much larger on melting sea ice than on other types of snow and sea ice. Therefore, the higher input of shortwave radiation during the summer melt cycle associated with melting sea ice accelerates the melt process.

Parameterizing the competition between homogeneous and heterogeneous freezing in ice cloud formation – polydisperse ice nuclei

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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.

Impact of air pollution on deposition of mineral dust: Implications for ocean productivity

Science.gov (United States)

Fan, S.; Horrowitz, L. W.; Levy, H.; Moxim, W. J.

2003-12-01

Atmospheric dust aerosols originating from arid regions are simulated in an atmospheric global chemical transport model. Based on model results and observations of dust oncentration, we hypothesize that Asian dust over the North Pacific is mostly hydrophilic and removed efficiently by both ice and droplet nucleation processes. By contrast, African dust over the tropical Atlantic is mostly hydrophobic and removed by ice, but not droplet, nucleation. We suggest that Asian dust is transformed into hydrophilic aerosols by chemical reactions with air pollutants over East Asia, which produce high levels of readily soluble materials on the surface of dust particles. A model of chemical aging will be presented for the hygroscopic transformation of mineral dust in the atmosphere. The model predicts that evolving air pollution in East Asia could have caused an increase of dust deposition to the coastal oceans off Asia and a decrease by as much as 50 percent in the eastern North Pacific. Insofar as iron from dust deposition fuels diatom blooms in the North Pacific Ocean, this decrease could have potential consequences on ocean biology.

Characterization of individual ice residual particles by the single droplet freezing method: a case study in the Asian dust outflow region

Science.gov (United States)

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

Massive CO2 Ice Deposits Sequestered in the South Polar Layered Deposits of Mars

Science.gov (United States)

Phillips, Roger J.; Davis, Brian J.; Tanaka, Kenneth L.; Byrne, Shane; Mellon, Michael T.; Putzig, Nathaniel E.; Haberle, Robert M.; Kahre, Melinda A.; Campbell, Bruce A.; Carter, Lynn M.; Smith, Isaac B.; Holt, John W.; Smrekar, Suzanne E.; Nunes, Daniel C.; Plaut, Jeffrey J.; Egan, Anthony F.; Titus, Timothy N.; Seu, Roberto

2011-01-01

Shallow Radar soundings from the Mars Reconnaissance Orbiter reveal a buried deposit of carbon dioxide (CO2) ice within the south polar layered deposits of Mars with a volume of 9500 to 12,500 cubic kilometers, about 30 times that previously estimated for the south pole residual cap. The deposit occurs within a stratigraphic unit that is uniquely marked by collapse features and other evidence of interior CO2 volatile release. If released into the atmosphere at times of high obliquity, the CO2 reservoir would increase the atmospheric mass by up to 80%, leading to more frequent and intense dust storms and to more regions where liquid water could persist without boiling.

Inhibition of ice crystallisation in highly viscous aqueous organic acid droplets

Directory of Open Access Journals (Sweden)

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.

Frost-related dieback of Swedish and Estonian Salix plantations due to pathogenic and ice nucleation-active bacteria

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.

Constraining the thickness of polar ice deposits on Mercury using the Mercury Laser Altimeter and small craters in permanently shadowed regions

Science.gov (United States)

Deutsch, Ariel N.; Head, James W.; Chabot, Nancy L.; Neumann, Gregory A.

2018-05-01

Radar-bright deposits at the poles of Mercury are located in permanently shadowed regions, which provide thermally stable environments for hosting and retaining water ice on the surface or in the near subsurface for geologic timescales. While the areal distribution of these radar-bright deposits is well characterized, their thickness, and thus their total mass and volume, remain poorly constrained. Here we derive thickness estimates for selected water-ice deposits using small, simple craters visible within the permanently shadowed, radar-bright deposits. We examine two endmember scenarios: in Case I, these craters predate the emplacement of the ice, and in Case II, these craters postdate the emplacement of the ice. In Case I, we find the difference between estimated depths of the original unfilled craters and the measured depths of the craters to find the estimated infill of material. The average estimated infilled material for 9 craters assumed to be overlain with water ice is ∼ 41-14+30 m, where 1-σ standard error of the mean is reported as uncertainty. Reported uncertainties are for statistical errors only. Additional systematic uncertainty may stem from georeferencing the images and topographic datasets, from the radial accuracy of the altimeter measurements, or from assumptions in our models including (1) ice is flat in the bowl-shaped crater and (2) there is negligible ice at the crater rims. In Case II, we derive crater excavation depths to investigate the thickness of the ice layer that may have been penetrated by the impact. While the absence of excavated regolith associated with the small craters observed suggests that impacts generally do not penetrate through the ice deposit, the spatial resolution and complex illumination geometry of images may limit the observations. Therefore, it is not possible to conclude whether the small craters in this study penetrate through the ice deposit, and thus Case II does not provide a constraint on the ice thickness

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.

Copper Benzenetricarboxylate Metal-Organic Framework Nucleation Mechanisms on Metal Oxide Powders and Thin Films formed by Atomic Layer Deposition.

Science.gov (United States)

Lemaire, Paul C; Zhao, Junjie; Williams, Philip S; Walls, Howard J; Shepherd, Sarah D; Losego, Mark D; Peterson, Gregory W; Parsons, Gregory N

2016-04-13

Chemically functional microporous metal-organic framework (MOF) crystals are attractive for filtration and gas storage applications, and recent results show that they can be immobilized on high surface area substrates, such as fiber mats. However, fundamental knowledge is still lacking regarding initial key reaction steps in thin film MOF nucleation and growth. We find that thin inorganic nucleation layers formed by atomic layer deposition (ALD) can promote solvothermal growth of copper benzenetricarboxylate MOF (Cu-BTC) on various substrate surfaces. The nature of the ALD material affects the MOF nucleation time, crystal size and morphology, and the resulting MOF surface area per unit mass. To understand MOF nucleation mechanisms, we investigate detailed Cu-BTC MOF nucleation behavior on metal oxide powders and Al2O3, ZnO, and TiO2 layers formed by ALD on polypropylene substrates. Studying both combined and sequential MOF reactant exposure conditions, we find that during solvothermal synthesis ALD metal oxides can react with the MOF metal precursor to form double hydroxy salts that can further convert to Cu-BTC MOF. The acidic organic linker can also etch or react with the surface to form MOF from an oxide metal source, which can also function as a nucleation agent for Cu-BTC in the mixed solvothermal solution. We discuss the implications of these results for better controlled thin film MOF nucleation and growth.

Nucleation and growth kinetics for intercalated islands during deposition on layered materials with isolated pointlike surface defects

International Nuclear Information System (INIS)

Han, Yong; Lii-Rosales, A.; Zhou, Y.; Wang, C.-J.

2017-01-01

Theory and stochastic lattice-gas modeling is developed for the formation of intercalated metal islands in the gallery between the top layer and the underlying layer at the surface of layered materials. Our model for this process involves deposition of atoms, some fraction of which then enter the gallery through well-separated pointlike defects in the top layer. Subsequently, these atoms diffuse within the subsurface gallery leading to nucleation and growth of intercalated islands nearby the defect point source. For the case of a single point defect, continuum diffusion equation analysis provides insight into the nucleation kinetics. However, complementary tailored lattice-gas modeling produces a more comprehensive and quantitative characterization. We analyze the large spread in nucleation times and positions relative to the defect for the first nucleated island. We also consider the formation of subsequent islands and the evolution of island growth shapes. The shapes reflect in part our natural adoption of a hexagonal close-packed island structure. As a result, motivation and support for the model is provided by scanning tunneling microscopy observations of the formation of intercalated metal islands in highly-ordered pyrolytic graphite at higher temperatures.

Heterogeneous primary nucleation of ice in water and aqueous solutions

NARCIS (Netherlands)

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

Copper Oxidation through Nucleation Sites of Chemical Vapor Deposited Graphene

DEFF Research Database (Denmark)

Luo, Birong; Whelan, Patrick Rebsdorf; Shivayogimath, Abhay

2016-01-01

We investigate the nucleation defect-triggered oxidation of Cu covered by CVD graphene during postannealing in air. The results reveal that different growth conditions may induce imperfect nucleation of graphene, and cause creation of defects near the nucleation point such as pin holes...... and amorphous carbon. These defects would serve as a pathway for the diffusion of 02 during thermal annealing, allowing oxidation of Cu to progress gradually from the nucleation center toward the growth edge. The oxidation process follows the graphene morphology closely; the shape of the oxidized area of Cu has...... a striking resemblance to that of the graphene flakes. Our work demonstrates that inferior graphene nucleation in CVD processes can compromise the oxidation resistance of a graphene-coated Cu substrate, and indirectly reveal the structure and integrity of graphene, which is of fundamental importance...

Simulation of nucleation and growth of atomic layer deposition phosphorus for doping of advanced FinFETs

International Nuclear Information System (INIS)

Seidel, Thomas E.; Goldberg, Alexander; Halls, Mat D.; Current, Michael I.

2016-01-01

Simulations for the nucleation and growth of phosphorus films were carried out using density functional theory. The surface was represented by a Si 9 H 12 truncated cluster surface model with 2 × 1-reconstructured (100) Si-OH terminations for the initial reaction sites. Chemistries included phosphorous halides (PF 3 , PCl 3 , and PBr 3 ) and disilane (Si 2 H 6 ). Atomic layer deposition (ALD) reaction sequences were illustrated with three-dimensional molecular models using sequential PF 3 and Si 2 H 6 reactions and featuring SiFH 3 as a byproduct. Exothermic reaction pathways were developed for both nucleation and growth for a Si-OH surface. Energetically favorable reactions for the deposition of four phosphorus atoms including lateral P–P bonding were simulated. This paper suggests energetically favorable thermodynamic reactions for the growth of elemental phosphorus on (100) silicon. Phosphorus layers made by ALD are an option for doping advanced fin field-effect transistors (FinFETs). Phosphorus may be thermally diffused into the silicon or recoil knocked in; simulations of the recoil profile of phosphorus into a FinFET surface are illustrated

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.

Ice nucleation activity in various tissues of Rhododendron flower buds: their relevance to extraorgan freezing

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.

Volcanic flows versus water- and ice-related outburst deposits in eastern Hellas: A comparison

Science.gov (United States)

Voelker, M.; Hauber, E.; Stephan, K.; Jaumann, R.

2018-06-01

Hellas Planitia is one of the major topographic sinks on Mars for the deposition of any kind of sediments. We report on our observations of sheet deposits in the eastern part of the basin that are apparently related to the Dao Vallis outflow channel. The deposits have lobate flow fronts and a thickness of a few decameters. Despite their generally smooth surface, some distinctive textures and patterns can be identified, such as longitudinal lineations, distributive channels, and polygons. We compared these deposits to other sheet deposits on Mars and tested three hypotheses of their origin: volcanic flows as well as water- and ice-related mass wastings. Despite some similarities to volcanic sheet flows on Mars, we found several morphological characteristics that are not known for sheet lava flows; for example conically arranged lineations and channel systems very similar to fluvial incisions. We also reject an ice-related formation similar to terrestrial rock-ice avalanches, as there is no sufficient relief energy to explain their extent and location. A water-related origin appears most consistent with our observations, and we favor an emplacement by fluvially-driven mass wasting processes, e.g., debris flows. Assuming a water-related origin, we calculated the amount of water that would be required to deposit such large sedimentary bodies for different flow types. Our calculations show a large range of possible water volumes, from 64 to 2,042 km³, depending on the specific flow mechanism. The close link to Dao Vallis makes these deposits a unique place to study the deposition of outflow channel sediments, as the deposits of other outflow channels on Mars, such as those around Chryse Planitia, are mostly buried by younger sediments and volcanic flows.

Nucleation and strain-stabilization during organic semiconductor thin film deposition.

Science.gov (United States)

Li, Yang; Wan, Jing; Smilgies, Detlef-M; Bouffard, Nicole; Sun, Richard; Headrick, Randall L

2016-09-07

The nucleation mechanisms during solution deposition of organic semiconductor thin films determine the grain morphology and may influence the crystalline packing in some cases. Here, in-situ optical spectromicroscopy in reflection mode is used to study the growth mechanisms and thermal stability of 6,13-bis(trisopropylsilylethynyl)-pentacene thin films. The results show that the films form in a supersaturated state before transforming to a solid film. Molecular aggregates corresponding to subcritical nuclei in the crystallization process are inferred from optical spectroscopy measurements of the supersaturated region. Strain-free solid films exhibit a temperature-dependent blue shift of optical absorption peaks due to a continuous thermally driven change of the crystalline packing. As crystalline films are cooled to ambient temperature they become strained although cracking of thicker films is observed, which allows the strain to partially relax. Below a critical thickness, cracking is not observed and grazing incidence X-ray diffraction measurements confirm that the thinnest films are constrained to the lattice constants corresponding to the temperature at which they were deposited. Optical spectroscopy results show that the transition temperature between Form I (room temperature phase) and Form II (high temperature phase) depends on the film thickness, and that Form I can also be strain-stabilized up to 135 °C.

Bioprecipitation: a feedback cycle linking earth history, ecosystem dynamics and land use through biological ice nucleators in the atmosphere.

Science.gov (United States)

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.

Characterization of individual ice residual particles by the single droplet freezing method: a case study in the Asian dust outflow region

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

Patterns of ice nuclei from natural water sources in the mountains of Tirol, Austria

Science.gov (United States)

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.

The Big Science Questions About Mercury's Ice-Bearing Polar Deposits After MESSENGER

Science.gov (United States)

Chabot, N. L.; Lawrence, D. J.

2018-05-01

Mercury’s polar deposits provide many well-characterized locations that are known to have large expanses of exposed water ice and/or other volatile materials — presenting unique opportunities to address fundamental science questions.

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

The impact of atmospheric mineral aerosol deposition on the albedo of snow and sea ice: are snow and sea ice optical properties more important than mineral aerosol optical properties?

OpenAIRE

M. L. Lamare; J. Lee-Taylor; M. D. King

2015-01-01

Knowledge of the albedo of polar regions is crucial for understanding a range of climatic processes that have an impact on a global scale. Light absorbing impurities in atmospheric aerosols deposited on snow and sea ice by aeolian transport absorb solar radiation, reducing albedo. Here, the effects of five mineral aerosol deposits reducing the albedo of polar snow and sea ice are considered. Calculations employing a coupled atmospheric and snow/sea ice radiative-transfer model (TUV-snow) show...

Nucleation and adhesion of diamond films on Co cemented tungsten carbide

Energy Technology Data Exchange (ETDEWEB)

Polini, R.; Santarelli, M.; Traversa, E.

1999-12-01

Diamond deposits were grown using hot filament chemical vapor deposition (CVD) on pretreated Co cemented tungsten carbide (WC-Co) substrates with an average grain size of 6 {micro}m. Depositions were performed with 0.5 or 1.0% methane concentration and with substrate temperatures ranging from 750 to 1,000 C. Diamond nucleation densities were measured by scanning electron microscopy. Scratched and bias-enhanced nucleation pretreated substrates showed the larger nucleation densities. Etching of the WC performed by Murakami's reagent, followed by surface-Co dissolution (MP pretreatment), led to a roughened but scarcely nucleating surface. The performance of a scratching prior to the MP pretreatment allowed one to increase the nucleation density, due scratching-induced defects, confined in the outermost layer of WC grains, which act as nucleation sites. Smaller nucleation densities were observed with increasing the substrate temperature and reducing the methane concentration, confirming that diamond nucleates via a heterogeneous process. The adhesion of continuous films was evaluated by the reciprocal of the slope of crack radius-indentation load functions. The substrate pretreatments mainly affected the film adhesion, while the influence of CVD process conditions was minor. The two main factors that improve the diamond film adhesion are the coating-substrate contact area and the surface-Co removal.

On the usage of classical nucleation theory in predicting the impact of bacteria on weather and climate

Science.gov (United States)

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

Ice Nucleation Activity of Black Carbon and Organic Aerosol Emitted from Biomass Burning

Science.gov (United States)

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.

Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions - Part 1: The K-feldspar microcline

Science.gov (United States)

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

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.

Development of a capacitive ice sensor to measure ice growth in real time.

Science.gov (United States)

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.

Slow-slip events on the Whillans Ice Plain, Antarctica, described using rate-and-state friction as an ice stream sliding law

Science.gov (United States)

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.

Nucleation and growth mechanism of Co–Pt alloy nanowires electrodeposited within alumina template

Energy Technology Data Exchange (ETDEWEB)

Srivastav, Ajeet K., E-mail: srivastav.ajeet.kumar@gmail.com, E-mail: mm09d004@smail.iitm.ac.in [Indian Institute of Technology Madras, Department of Metallurgical and Materials Engineering (India); Shekhar, Rajiv [Indian Institute of Technology Kanpur, Department of Materials Science and Engineering (India)

2015-01-15

Co–Pt alloy nanowires were electrodeposited by direct current electrodeposition within nanoporous alumina templates with varying deposition potentials. The effect of deposition potential on nucleation and growth mechanisms during electrodeposition of Co–Pt alloy nanowires was investigated. The less negative deposition potential (−0.9 V) favours the instantaneous nucleation mechanism. The positive deviation from theoretical instantaneous and progressive nucleation mechanisms occurs at higher negative deposition potentials. The hysteresis behaviour and magnetic properties of electrodeposited Co–Pt alloy nanowires altered with varying deposition potential. The easy magnetization direction was in direction perpendicular to the wire axis. The deposition potential dependent change in hysteresis behaviour with increased coercivity and scattered remanence ratio was observed. This is attributed to better crystallinity with reduced defect density and hydrogen evolution causing structural changes at more negative deposition potentials.

Communication: Disorder-suppressed vibrational relaxation in vapor-deposited high-density amorphous ice

Science.gov (United States)

Shalit, Andrey; Perakis, Fivos; Hamm, Peter

2014-04-01

We apply two-dimensional infrared spectroscopy to differentiate between the two polyamorphous forms of glassy water, low-density (LDA) and high-density (HDA) amorphous ices, that were obtained by slow vapor deposition at 80 and 11 K, respectively. Both the vibrational lifetime and the bandwidth of the 1-2 transition of the isolated OD stretch vibration of HDO in H2O exhibit characteristic differences when comparing hexagonal (Ih), LDA, and HDA ices, which we attribute to the different local structures - in particular the presence of interstitial waters in HDA ice - that cause different delocalization lengths of intermolecular phonon degrees of freedom. Moreover, temperature dependent measurements show that the vibrational lifetime closely follows the structural transition between HDA and LDA phases.

The competition between mineral dust and soot ice nuclei in mixed-phase clouds (Invited)

Science.gov (United States)

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

Concentration and variability of ice nuclei in the subtropical maritime boundary layer

Science.gov (United States)

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.

Constraining the Depth of Polar Ice Deposits and Evolution of Cold Traps on Mercury with Small Craters in Permanently Shadowed Regions

Science.gov (United States)

Deutsch, Ariel N.; Head, James W.; Neumann, Gregory A.; Chabot, Nancy L.

2017-01-01

Earth-based radar observations revealed highly reflective deposits at the poles of Mercury [e.g., 1], which collocate with permanently shadowed regions (PSRs) detected from both imagery and altimetry by the MErcury Surface, Space ENvironment, GEochemistry, and Ranging (MESSENGER) spacecraft [e.g., 2]. MESSENGER also measured higher hydrogen concentrations at the north polar region, consistent with models for these deposits to be composed primarily of water ice [3]. Enigmatic to the characterization of ice deposits on Mercury is the thickness of these radar-bright features. A current minimum bound of several meters exists from the radar measurements, which show no drop in the radar cross section between 13- and 70-cm wavelength observations [4, 5]. A maximum thickness of 300 m is based on the lack of any statistically significant difference between the height of craters that host radar-bright deposits and those that do not [6]. More recently, this upper limit on the depth of a typical ice deposit has been lowered to approximately 150 m, in a study that found a mean excess thickness of 50 +/- 35 m of radar-bright deposits for 6 craters [7]. Refining such a constraint permits the derivation of a volumetric estimate of the total polar ice on Mercury, thus providing insight into possible sources of water ice on the planet. Here, we take a different approach to constrain the thickness of water-ice deposits. Permanently shadowed surfaces have been resolved in images acquired with the broadband filter on MESSENGER's wide-angle camera (WAC) using low levels of light scattered by crater walls and other topography [8]. These surfaces are not featureless and often host small craters (less than a few km in diameter). Here we utilize the presence of these small simple craters to constrain the thickness of the radar-bright ice deposits on Mercury. Specifically, we compare estimated depths made from depth-to-diameter ratios and depths from individual Mercury Laser Altimeter (MLA

A one-dimensional ice structure built from pentagons

Science.gov (United States)

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).

Impact of climate fluctuations on deposition of DDT and hexachlorocyclohexane in mountain glaciers: Evidence from ice core records

International Nuclear Information System (INIS)

Wang Xiaoping; Gong Ping; Zhang, Qianggong; Yao Tandong

2010-01-01

How do climate fluctuations affect DDT and hexachlorocyclohexane (HCH) distribution in the global scale? In this study, the interactions between climate variations and depositions of DDT and HCH in ice cores from Mt. Everest (the Tibetan Plateau), Mt. Muztagata (the eastern Pamirs) and the Rocky Mountains were investigated. All data regarding DDT/HCH deposition were obtained from the published results. Concentrations of DDT and HCH in an ice core from Mt. Everest were associated with the El Nino-Southern Oscillation. Concentrations of DDT in an ice core from Mt. Muztagata were significantly correlated with the Siberia High pattern. Concentrations of HCH in an ice core from Snow Dome of the Rocky Mountains responded to the North Atlantic Oscillation. These associations suggested that there are some linkages between climate variations and the global distribution of persistent organic pollutants. - Our study approves the potential contribution of ice core records of POPs to transport mechanisms of POPs.

LiF enhanced nucleation of the low temperature microcrystalline silicon prepared by plasma enhanced chemical vapour deposition

Czech Academy of Sciences Publication Activity Database

Stuchlík, Jiří; Ledinský, Martin; Honda, Shinya; Drbohlav, Ivo; Mates, Tomáš; Fejfar, Antonín; Hruška, Karel; Stuchlíková, The-Ha; Kočka, Jan

2009-01-01

Roč. 517, č. 24 (2009), s. 6829-6832 ISSN 0040-6090 R&D Projects: GA AV ČR KAN400100701; GA ČR(CZ) GD202/05/H003; GA MŠk LC510; GA AV ČR IAA1010413 Institutional research plan: CEZ:AV0Z10100521 Keywords : amorphous hydrogenated silicon * atomic force microscopy * plasma-enhanced chemical vapour deposition, * nucleation * Raman scattering * lithium fluoride Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 1.727, year: 2009

Ice Nucleation and Dehydration in the Tropical Tropopause Layer

Science.gov (United States)

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.

Reaction and nucleation mechanisms of copper electrodeposition on disposable pencil graphite electrode

Energy Technology Data Exchange (ETDEWEB)

Majidi, M.R. [Department of Analytical Chemistry, Faculty of Chemistry, University of Tabriz, 29th Bahman Bolvard, Tabriz 51664 (Iran, Islamic Republic of)], E-mail: sr.majidi@gmail.com; Asadpour-Zeynali, K.; Hafezi, B. [Department of Analytical Chemistry, Faculty of Chemistry, University of Tabriz, 29th Bahman Bolvard, Tabriz 51664 (Iran, Islamic Republic of)

2009-01-01

The reaction and nucleation mechanism of copper electrodeposition on disposable pencil graphite electrode (PGE) in acidic sulphate solution were investigated using cyclic voltammetry (CV) and chronoamperometry (CA) techniques, respectively. Electrochemical experiments were followed by morphological studies with scanning electron microscopy (SEM). The effect of some experimental parameters, namely copper concentration, pH, scan rate, background electrolyte, deposition potential, and conditioning surface of the electrode were described. At the surface of PGE, Cu{sup 2+} ions were reduced at -250 mV vs. SCE. It was found that electrodeposition of copper is affected by rough surface of PGE. The nucleation mechanisms were examined by fitting the experimental CA data into Scharifker-Hills nucleation models. The nuclei population densities were also determined by means of two common fitting models developed for three-dimensional nucleation and growth (Scharifker-Mostany and Mirkin-Nilov-Herrman-Tarallo). It was found that deposition potential and background electrolyte affect the distribution of the deposited copper. The morphology of the deposited copper is affected by background electrolyte.

Ice nucleation and dehydration in the Tropical Tropopause Layer.

Science.gov (United States)

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.

Cirrus Susceptibility to Changes in Ice Nuclei: Physical Processes, Model Uncertainties, and Measurement Needs

Science.gov (United States)

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

A short overview of the microbial population in clouds: Potential roles in atmospheric chemistry and nucleation processes

Science.gov (United States)

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.

High laser-fluence deposition of organic materials in water ice matrices by ''MAPLE''

DEFF Research Database (Denmark)

Christensen, Bo Toftmann; Rodrigo, K.; Schou, Jørgen

2005-01-01

Matrix assisted pulsed laser evaporation (MAPLE) is a deposition technique for organic material. Water ice was used as a matrix for the biotechnologically important guest material, polyethylene glycol (PEG), for concentrations from 0.5 to 4 wt.%. The target was irradiated with 6 ns laser pulses...

Animal ice-binding (antifreeze) proteins and glycolipids: an overview with emphasis on physiological function.

Science.gov (United States)

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.

Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions – Part 1: The K-feldspar microcline

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

Impact of the Bergeron-Findeisen process on the release of aerosol particles during the evolution of cloud ice

Science.gov (United States)

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.

On The Importance of Connecting Laboratory Measurements of Ice Crystal Growth with Model Parameterizations: Predicting Ice Particle Properties

Science.gov (United States)

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

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.

Competition for water vapour results in suppression of ice formation in mixed-phase clouds

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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.

Competition for water vapour results in suppression of ice formation in mixed-phase clouds

Science.gov (United States)

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.

Kinetic Monte Carlo simulations of water ice porosity: extrapolations of deposition parameters from the laboratory to interstellar space

Science.gov (United States)

Clements, Aspen R.; Berk, Brandon; Cooke, Ilsa R.; Garrod, Robin T.

2018-02-01

Using an off-lattice kinetic Monte Carlo model we reproduce experimental laboratory trends in the density of amorphous solid water (ASW) for varied deposition angle, rate and surface temperature. Extrapolation of the model to conditions appropriate to protoplanetary disks and interstellar dark clouds indicate that these ices may be less porous than laboratory ices.

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.

Selective deposition of polycrystalline diamond films using photolithography with addition of nanodiamonds as nucleation centers

International Nuclear Information System (INIS)

Okhotnikov, V V; Linnik, S A; Gaidaichuk, A V; Shashev, D V; Nazarova, G Yu; Yurchenko, V I

2016-01-01

A new method of selective deposition of polycrystalline diamond has been developed and studied. The diamond coatings with a complex, predetermined geometry and resolution up to 5 μm were obtained. A high density of polycrystallites in the coating area was reached (up to 32·10 7 pcs/cm 2 ). The uniformity of the film reached 100%, and the degree of the surface contamination by parasitic crystals did not exceed 2%. The technology was based on the application of the standard photolithography with an addition of nanodiamond suspension into the photoresist that provided the creation of the centers of further nucleation in the areas which require further overgrowth. The films were deposited onto monocrystalline silicon substrates using the method of “hot filaments” in the CVD reactor. The properties of the coating and the impact of the nanodiamond suspension concentration in the photoresist were also studied. The potential use of the given method includes a high resolution, technological efficiency, and low labor costs compared to the standard methods (laser treatment, chemical etching in aggressive environments,). (paper)

Selective deposition of polycrystalline diamond films using photolithography with addition of nanodiamonds as nucleation centers

Science.gov (United States)

Okhotnikov, V. V.; Linnik, S. A.; Gaidaichuk, A. V.; Shashev, D. V.; Nazarova, G. Yu; Yurchenko, V. I.

2016-02-01

A new method of selective deposition of polycrystalline diamond has been developed and studied. The diamond coatings with a complex, predetermined geometry and resolution up to 5 μm were obtained. A high density of polycrystallites in the coating area was reached (up to 32·107 pcs/cm2). The uniformity of the film reached 100%, and the degree of the surface contamination by parasitic crystals did not exceed 2%. The technology was based on the application of the standard photolithography with an addition of nanodiamond suspension into the photoresist that provided the creation of the centers of further nucleation in the areas which require further overgrowth. The films were deposited onto monocrystalline silicon substrates using the method of “hot filaments” in the CVD reactor. The properties of the coating and the impact of the nanodiamond suspension concentration in the photoresist were also studied. The potential use of the given method includes a high resolution, technological efficiency, and low labor costs compared to the standard methods (laser treatment, chemical etching in aggressive environments,).

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.

Global Distribution of Solid Ammonium Sulfate Aerosols and their Climate Impact Acting as Ice Nuclei

Science.gov (United States)

Zhou, C.; Penner, J.

2017-12-01

Laboratory experiments show that liquid ammonium sulfate particles effloresce when RHw is below 34% to become solid and dissolve when RHw is above 79%. Solid ammonium sulfate aerosols can act as heterogeneous ice nuclei particles (INPs) to form ice particles in deposition mode when the relative humidity over ice is above 120%. In this study we used the coupled IMPACT/CAM5 model to track the efflorescence and deliquescence processes of ammonium sulfate. Results show that about 20% of the total simulated pure sulfate aerosol mass is in the solid state and is mainly distributed in the northern hemisphere (NH) from 50 hPa to 200 hPa. When these solid ammonium sulfate aerosols are allowed to act as ice nuclei particles, they act to increase the ice water path in the NH and reduce ice water path in the tropics. The addition of these particles leads to a positive net radiative effect at the TOA ranging from 0.5-0.9 W/m2 depending on the amounts of other ice nuclei particles (e.g., dust, soot) used in the ice nucleation process. The short-term climate feedback shows that the ITCZ shifts northwards and precipitation increases in the NH. There is also an average warming of 0.05-0.1 K near the surface (at 2 meter) in the NH which is most obvious in the Arctic region.

Nucleation on a stepped surface with an Ehrlich–Schwöbel barrier

International Nuclear Information System (INIS)

Chromcova, Z; Chvoj, Z; Tringides, M C

2013-01-01

During deposition on a stepped surface the growth mode depends on the conditions such as temperature T, deposition rate F and width of the terraces w. In this work we studied the influence of all the above mentioned characteristics using the kinetic Monte Carlo (kMC) technique. We concentrated on the conditions on the terrace at the moment of the first nucleation. The critical density of monomers for nucleation η m decreases with the width of the terrace and the nucleation starts at surprisingly low densities of monomers. We tested several definitions of the critical width for nucleation w c used in various articles in the past and we compared our results with results of the analytical steady-state mean-field model (Ranguelov and Altman 2007 Phys. Rev. B 75 245419). To check how the simplified assumption about the steady-state regime during deposition influences the resulting dependence of w c ≃ (D/F) κ , we set and also solved a time-dependent analytical model. This analytical model as well as kMC predict that w c ≃ (D/F) 1/5 . kMC simulation also shows that the Ehrlich–Schwöbel barrier has only limited influence on the nucleation on the stepped surface at conditions close to the nucleation regime. For all widths of terraces there is a critical value of the Ehrlich–Schwöbel barrier, and only below this critical value does the Ehrlich–Schwöbel barrier affect the final value of the density of nuclei. The results of the kMC are summarized in a semi-empirical analytical formula which describes the dependence of the step-flow growth and nucleation on the terrace width w, diffusion coefficient D and deposition rate F. In our simulations we tested two models of the stepped surface with different thicknesses of the step, both with an Ehrlich–Schwöbel barrier on the edge of the terrace. (paper)

The effect of mineral dust and soot aerosols on ice microphysics near the foothills of the Himalayas: A numerical investigation

Science.gov (United States)

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.

Evaluating and constraining ice cloud parameterizations in CAM5 using aircraft measurements from the SPARTICUS campaign

Directory of Open Access Journals (Sweden)

K. Zhang

2013-05-01

Full Text Available This study uses aircraft measurements of relative humidity and ice crystal size distribution collected during the SPARTICUS (Small PARTicles In CirrUS field campaign to evaluate and constrain ice cloud parameterizations in the Community Atmosphere Model version 5. About 200 h of data were collected during the campaign between January and June 2010, providing the longest aircraft measurements available so far for cirrus clouds in the midlatitudes. The probability density function (PDF of ice crystal number concentration (Ni derived from the high-frequency (1 Hz measurements features a strong dependence on ambient temperature. As temperature decreases from −35 °C to −62 °C, the peak in the PDF shifts from 10–20 L−1 to 200–1000 L−1, while Ni shows a factor of 6–7 increase. Model simulations are performed with two different ice nucleation schemes for pure ice-phase clouds. One of the schemes can reproduce a clear increase of Ni with decreasing temperature by using either an observation-based ice nuclei spectrum or a classical-theory-based spectrum with a relatively low (5–10% maximum freezing ratio for dust aerosols. The simulation with the other scheme, which assumes a high maximum freezing ratio (100%, shows much weaker temperature dependence of Ni. Simulations are also performed to test empirical parameters related to water vapor deposition and the autoconversion of ice crystals to snow. Results show that a value between 0.05 and 0.1 for the water vapor deposition coefficient, and 250 μm for the critical diameter that distinguishes ice crystals from snow, can produce good agreement between model simulation and the SPARTICUS measurements in terms of Ni and effective radius. The climate impact of perturbing these parameters is also discussed.

Ice nucleating particles from a large-scale sampling network: insight into geographic and temporal variability

Science.gov (United States)

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).

Effects of Surface Modification of Nanodiamond Particles for Nucleation Enhancement during Its Film Growth by Microwave Plasma Jet Chemical Vapour Deposition Technique

Directory of Open Access Journals (Sweden)

Chii-Ruey Lin

2014-01-01

Full Text Available The seedings of the substrate with a suspension of nanodiamond particles (NDPs were widely used as nucleation seeds to enhance the growth of nanostructured diamond films. The formation of agglomerates in the suspension of NDPs, however, may have adverse impact on the initial growth period. Therefore, this paper was aimed at the surface modification of the NDPs to enhance the diamond nucleation for the growth of nanocrystalline diamond films which could be used in photovoltaic applications. Hydrogen plasma, thermal, and surfactant treatment techniques were employed to improve the dispersion characteristics of detonation nanodiamond particles in aqueous media. The seeding of silicon substrate was then carried out with an optimized spin-coating method. The results of both Fourier transform infrared spectroscopy and dynamic light scattering measurements demonstrated that plasma treated diamond nanoparticles possessed polar surface functional groups and attained high dispersion in methanol. The nanocrystalline diamond films deposited by microwave plasma jet chemical vapour deposition exhibited extremely fine grain and high smooth surfaces (~6.4 nm rms on the whole film. These results indeed open up a prospect of nanocrystalline diamond films in solar cell applications.

Adherent nanoparticles-mediated micro- and nanobubble nucleation

Science.gov (United States)

Chan, Chon U.; Chen, Long Quan; Lippert, Alexander; Arora, Manish; Ohl, Claus-Dieter

2014-11-01

Surface nanobubbles are commonly nucleated through water-ethanol-water exchange. It is believed that the higher gas solubility in ethanol and exothermic mixing leads to a supersaturation of gas in water. However details of the nucleation dynamic are still unknown. Here we apply the exchange process onto a glass surface deposited with nanoparticles and monitor the dynamics optically at video frame rates. During exchange bubbles of a few micron in diameter nucleate at the sites of nanoparticles. These microbubbles eventually dissolve in ethanol but are stable in water. This agrees with the nucleation process observed for surface nanobubbles. Also we find a reduction of surface attached nanobubbles near the particles, which might be due to gas uptake from the microbubble growth. Finally, high speed recordings reveal stick-slip motion of the triple contact line during the growth process. We will discuss possibilities of utilizing the findings for contamination detection and ultrasonic cleaning.

Determination of critical nucleation number for a single nucleation amyloid-β aggregation model.

Science.gov (United States)

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.

The Dominant Snow-forming Process in Warm and Cold Mixed-phase Orographic Clouds: Effects of Cloud Condensation Nuclei and Ice Nuclei

Science.gov (United States)

Fan, J.; Rosenfeld, D.; Leung, L. R.; DeMott, P. J.

2014-12-01

Mineral dust aerosols often observed over California in winter and spring from long-range transport can be efficient ice nuclei (IN) and enhance snow precipitation in mixed-phase orographic clouds. On the other hand, local pollution particles can serve as good CCN and suppress warm rain, but their impacts on cold rain processes are uncertain. The main snow-forming mechanism in warm and cold mixed-phase orographic clouds (refer to as WMOC and CMOC, respectively) could be very different, leading to different precipitation response to CCN and IN. We have conducted 1-km resolution model simulations using the Weather Research and Forecasting (WRF) model coupled with a spectral-bin cloud microphysical model for WMOC and CMOC cases from CalWater2011. We investigated the response of cloud microphysical processes and precipitation to CCN and IN with extremely low to extremely high concentrations using ice nucleation parameterizations that connect with dust and implemented based on observational evidences. We find that riming is the dominant process for producing snow in WMOC while deposition plays a more important role than riming in CMOC. Increasing IN leads to much more snow precipitation mainly due to an increase of deposition in CMOC and increased rimming in WMOC. Increasing CCN decreases precipitation in WMOC by efficiently suppressing warm rain, although snow is increased. In CMOC where cold rain dominates, increasing CCN significantly increases snow, leading to a net increase in precipitation. The sensitivity of supercooled liquid to CCN and IN has also been analyzed. The mechanism for the increased snow by CCN and caveats due to uncertainties in ice nucleation parameterizations will be discussed.

Laboratory studies on the uptake of aromatic hydrocarbons by ice crystals during vapor depositional crystal growth

Science.gov (United States)

Fries, Elke; Starokozhev, Elena; Haunold, Werner; Jaeschke, Wolfgang; Mitra, Subir K.; Borrmann, Stephan; Schmidt, Martin U.

Uptake of aromatic hydrocarbons (AH) by ice crystals during vapor deposit growth was investigated in a walk-in cold chamber at temperatures of 242, 251, and 260 K, respectively. Ice crystals were grown from ambient air in the presence of gaseous AH namely: benzene (C 6H 6), toluene (methylbenzene, C 7H 8), the C 8H 10 isomers ethylbenzene, o-, m-, p-xylene (dimethylbenzenes), the C 9H 12 isomers n-propylbenzene, 4-ethyltoluene, 1,3,5-trimethylbenzene (1,3,5-TMB), 1,2,4-trimethylbenzene (1,2,4-TMB), 1,2,3-trimethylbenzene (1,2,3-TMB), and the C 10H 14 compound tert.-butylbenzene. Gas-phase concentrations calculated at 295 K were 10.3-20.8 μg m -3. Uptake of AH was detected by analyzing vapor deposited ice with a very sensitive method composed of solid-phase micro-extraction (SPME), followed by gas chromatography/mass spectrometry (GC/MS). Ice crystal size was lower than 1 cm. At water vapor extents of 5.8, 6.0 and 8.1 g m -3, ice crystal shape changed with decreasing temperatures from a column at a temperature of 260 K, to a plate at 251 K, and to a dendrite at 242 K. Experimentally observed ice growth rates were between 3.3 and 13.3×10 -3 g s -1 m -2 and decreased at lower temperatures and lower value of water vapor concentration. Predicted growth rates were mostly slightly higher. Benzene, toluene, ethylbenzene, and xylenes (BTEX) were not detected in ice above their detection limits (DLs) of 25 pg g ice-1 (toluene, ethylbenzene, xylenes) and 125 pg g ice-1 (benzene) over the entire temperature range. Median concentrations of n-propylbenzene, 4-ethyltoluene, 1,3,5-TMB, tert.-butylbenzene, 1,2,4-TMB, and 1,2,3-TMB were between 4 and 176 pg g ice-1 at gas concentrations of 10.3-10.7 μg m -3 calculated at 295 K. Uptake coefficients ( K) defined as the product of concentration of AH in ice and density of ice related to the product of their concentration in the gas phase and ice mass varied between 0.40 and 10.23. K increased with decreasing temperatures. Values of

Polymer-based nucleation for chemical vapour deposition of diamond

Czech Academy of Sciences Publication Activity Database

Domonkos, Mária; Ižák, Tibor; Kromka, Alexander; Varga, Marián

2016-01-01

Roč. 133, č. 29 (2016), 1-7, č. článku 43688. ISSN 0021-8995 R&D Projects: GA ČR GC15-22102J Institutional support: RVO:68378271 Keywords : copolymers * composites * diamond * nucleation Subject RIV: BM - Solid Matter Physics ; Magnetism Impact factor: 1.860, year: 2016

Luminescence dating of paleolake deltas and glacial deposits in Garwood Valley, Antarctica: Implications for climate, Ross ice sheet dynamics, and paleolake duration

Science.gov (United States)

Levy, Joseph S.; Rittenour, Tammy M.; Fountain, Andrew G.; O'Connor, Jim E.

2017-01-01

The formation of perched deltas and other lacustrine deposits in the McMurdo Dry Valleys of Antarctica is widely considered to be evidence of valley-filling lakes dammed by the grounded Ross Sea ice sheet during the local Last Glacial Maximum, with lake drainage interpreted as a record of grounding line retreat. We used luminescence dating to determine the age of paleolake deltas and glacial tills in Garwood Valley, a coastal dry valley that opens to the Ross Sea. Luminescence ages are stratigraphically consistent with radiocarbon results from algal mats within the same delta deposits but suggest radiocarbon dates from lacustrine carbonates may overestimate deposit ages by thousands of years. Results suggest that late Holocene delta deposition into paleolake Howard in Garwood Valley persisted until ca. 3.5 ka. This is significantly younger than the date when grounded ice is thought to have retreated from the Ross Sea. Our evidence suggests that the local, stranded ice-cored till topography in Garwood Valley, rather than regional ice-sheet dynamics, may have controlled lake levels for some McMurdo Dry Valleys paleolakes. Age control from the supraglacial Ross Sea drift suggests grounding and up-valley advance of the Ross Sea ice sheet into Garwood valley during marine oxygen isotope stage (MIS) 4 (71–78 ka) and the local Last Glacial Maximum (9–10 ka). This work demonstrates the power of combining luminescence dating with existing radiocarbon data sets to improve understanding of the relationships among paleolake formation, glacial position, and stream discharge in response to climate change.

Deposits related to supercritical flows in glacifluvial deltas and subaqueous ice-contact fans: Integrating facies analysis and ground-penetrating radar

Science.gov (United States)

Lang, Joerg; Sievers, Julian; Loewer, Markus; Igel, Jan; Winsemann, Jutta

2017-04-01

Bedforms related to supercritical flows have recently received much interest and the understanding of flow morphodynamics and depositional processes has been greatly advanced. However, outcrop studies of these bedforms are commonly hampered by their long wavelengths. Therefore, we combined outcrop-based facies analysis with extensive ground-penetrating radar (GPR) measurements. Different GPR antennas (200, 400 and 1500 MHz) were utilised to measure both long profiles and densely spaced grids in order to map the large-scale facies architecture and image the three-dimensional geometry of the deposits. The studied delta and subaqueous ice-contact fan successions were deposited within ice-dammed lakes, which formed along the margins of the Middle Pleistocene Scandinavian ice sheets across Northern Germany. These glacilacustrine depositional systems are characterised by high aggradation rates due to the rapid expansion and deceleration of high-energy sediment-laden flows, favouring the preservation of bedforms related to supercritical flows. In flow direction, delta foresets commonly display lenticular scours, which are 2 to 6 m wide and 0.15 to 0.5 m deep. Characteristically, scours are filled by upslope dipping backsets, consisting of pebbly sand. In a few cases, massive and deformed strata were observed, passing upflow into backsets. Across flow, scours are 2 to 3 m wide and typically display a concentric infill. The scour fills are commonly associated with subhorizontally or sinusoidal stratified pebbly sand. These facies types are interpreted as deposits of cyclic steps and antidunes, respectively, representing deposition from supercritical density flows, which formed during high meltwater discharge events or regressive slope failures (Winsemann et al., in review). The GPR-sections show that the scour fills form trains along the delta foresets, which can be traced for up to 15 m. The studied subaqueous ice-contact fan succession relates to the zone of flow

The Relevance of Grain Dissection for Grain Size Reduction in Polar Ice: Insights from Numerical Models and Ice Core Microstructure Analysis

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

The relevance of grain dissection for grain size reduction in polar ice: insights from numerical models and ice core microstructure analysis

Science.gov (United States)

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

Morphology evolution in spinel manganite films deposited from an aqueous solution

International Nuclear Information System (INIS)

Ko, Song Won; Li, Jing; Trolier-McKinstry, Susan

2012-01-01

Spinel manganite films were deposited by the spin spray technique at low deposition temperatures ( 1000, agglomeration of small particles was dominant, which suggests that homogeneous nucleation is dominant during deposition. Heterogeneous nucleation was critical to obtain dense films. - Highlights: ► Film microstructure depends on supersaturation. ► Heterogeneous nucleation induces dense and continuous films. ► The spin spray technique enables use of a variety of substrates.

Aerosolization, Chemical Characterization, Hygroscopicity and Ice Formation of Marine Biogenic Particles

Science.gov (United States)

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

Buried CO2 Ice traces in South Polar Layered Deposits of Mars detected by radar sounder

Science.gov (United States)

Castaldo, L.; Mège, D.; Orosei, R.; Séjourné, A.

2014-12-01

SHARAD (SHAllow RADar) is the subsurface sounding radar provided by the Italian Space Agency (ASI) as a facility instrument to NASA's 2005 Mars Reconnaissance Orbiter (MRO). The Reduced Data Record of SHARAD data covering the area of the South Polar Layered Deposits (SPLD), has been used. The elaboration and interpretation of the data, aimed to estimate electromagnetic properties of surface layers, has been performed in terms of permittivity. The theory of electromagnetic scattering from fractal surfaces, and the estimation of geometric parameters from topographic data by Mars Orbiter Laser Altimeter (MOLA) which was one of five instruments on board the Mars Global Surveyor (MGS) spacecraft, has been used. A deep analysis of inversion has been made on all Mars and extended to the South Polar Caps in order to extract the area with a permittivity constant of CO2 ice. Several corrections have been applied to the data, moreover the calibration of the signal requires the determination of a constant that takes into account the power gain due to the radar system and the surface in order to compensate the power losses due to the orbitographic phenomena. The determination of regions with high probability of buried CO2 ice in the first layer of the Martian surface, is obtained extracting the real part of the permittivity constant of the CO2 ice (~2), estimated by other means. The permittivity of CO2ice is extracted from the Global Permittivity Map of Mars using the global standard deviation of itself as following: ɛCO2ice=ɛCO2ice+ Σ (1)where Σ=±std(ɛMapMars)/2Figure 1(a) shows the south polar areas where the values of the permittivity point to the possibility of a CO2 ice layer. Figure 1(b) is the corresponding geologic map. The comparison between the two maps indicates that the area with probable buried CO2 overlaps Hesperian and Amazonian polar units (Hp, Hesperian plains-forming deposits marked by narrow sinuous, anabranching ridges and irregular depressions, and

The last Scandinavian ice sheet in northwestern Russia: ice flow patterns and decay dynamics

DEFF Research Database (Denmark)

Demidov, L.; Houmark-Nielsen, Michael; Kjær, Kurt Henrik

2006-01-01

in Russia than previously outlined and the time of termination at 18-16 cal. kyr BP was almost 10 kyr delayed compared to the southwestern part of the ice sheet. We argue that the lithology of the ice sheets' substrate, and especially the location of former proglacial lake basins, influenced the dynamics......Advance of the Late Weichselian (Valdaian) Scandinavian Ice Sheet (SIS) in northwestern Russia took place after a period of periglacial conditions. Till of the last SIS, Bobrovo till, overlies glacial deposits from the previous Barents and Kara Sea ice sheets and marine deposits of the Last...

Crystal Nucleation in Liquids: Open Questions and Future Challenges in Molecular Dynamics Simulations.

Science.gov (United States)

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.

Incorporating C60 as Nucleation Sites Optimizing PbI2 Films To Achieve Perovskite Solar Cells Showing Excellent Efficiency and Stability via Vapor-Assisted Deposition Method.

Science.gov (United States)

Chen, Hai-Bin; Ding, Xi-Hong; Pan, Xu; Hayat, Tasawar; Alsaedi, Ahmed; Ding, Yong; Dai, Song-Yuan

2018-01-24

To achieve high-quality perovskite solar cells (PSCs), the morphology and carrier transportation of perovskite films need to be optimized. Herein, C 60 is employed as nucleation sites in PbI 2 precursor solution to optimize the morphology of perovskite films via vapor-assisted deposition process. Accompanying the homogeneous nucleation of PbI 2 , the incorporation of C 60 as heterogeneous nucleation sites can lower the nucleation free energy of PbI 2 , which facilitates the diffusion and reaction between PbI 2 and organic source. Meanwhile, C 60 could enhance carrier transportation and reduce charge recombination in the perovskite layer due to its high electron mobility and conductivity. In addition, the grain sizes of perovskite get larger with C 60 optimizing, which can reduce the grain boundaries and voids in perovskite and prevent the corrosion because of moisture. As a result, we obtain PSCs with a power conversion efficiency (PCE) of 18.33% and excellent stability. The PCEs of unsealed devices drop less than 10% in a dehumidification cabinet after 100 days and remain at 75% of the initial PCE during exposure to ambient air (humidity > 60% RH, temperature > 30 °C) for 30 days.

Microbial production of ice crystals in clouds as a novel atmospheric biosignature

Science.gov (United States)

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

Improving Heat Transfer at the Bottom of Vials for Consistent Freeze Drying with Unidirectional Structured Ice.

Science.gov (United States)

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.

Patterned electrochemical deposition of copper using an electron beam

Directory of Open Access Journals (Sweden)

Mark den Heijer

2014-02-01

Full Text Available We describe a technique for patterning clusters of metal using electrochemical deposition. By operating an electrochemical cell in the transmission electron microscope, we deposit Cu on Au under potentiostatic conditions. For acidified copper sulphate electrolytes, nucleation occurs uniformly over the electrode. However, when chloride ions are added there is a range of applied potentials over which nucleation occurs only in areas irradiated by the electron beam. By scanning the beam we control nucleation to form patterns of deposited copper. We discuss the mechanism for this effect in terms of electron beam-induced reactions with copper chloride, and consider possible applications.

Modeling the Hydrological Cycle in the Atmosphere of Mars: Influence of a Bimodal Size Distribution of Aerosol Nucleation Particles

Science.gov (United States)

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.

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

Influences of in-cloud aerosol scavenging parameterizations on aerosol concentrations and wet deposition in ECHAM5-HAM

Directory of Open Access Journals (Sweden)

B. Croft

2010-02-01

Full Text Available A diagnostic cloud nucleation scavenging scheme, which determines stratiform cloud scavenging ratios for both aerosol mass and number distributions, based on cloud droplet, and ice crystal number concentrations, is introduced into the ECHAM5-HAM global climate model. This scheme is coupled with a size-dependent in-cloud impaction scavenging parameterization for both cloud droplet-aerosol, and ice crystal-aerosol collisions. The aerosol mass scavenged in stratiform clouds is found to be primarily (>90% scavenged by cloud nucleation processes for all aerosol species, except for dust (50%. The aerosol number scavenged is primarily (>90% attributed to impaction. 99% of this impaction scavenging occurs in clouds with temperatures less than 273 K. Sensitivity studies are presented, which compare aerosol concentrations, burdens, and deposition for a variety of in-cloud scavenging approaches: prescribed fractions, a more computationally expensive prognostic aerosol cloud processing treatment, and the new diagnostic scheme, also with modified assumptions about in-cloud impaction and nucleation scavenging. Our results show that while uncertainties in the representation of in-cloud scavenging processes can lead to differences in the range of 20–30% for the predicted annual, global mean aerosol mass burdens, and near to 50% for accumulation mode aerosol number burden, the differences in predicted aerosol mass concentrations can be up to one order of magnitude, particularly for regions of the middle troposphere with temperatures below 273 K where mixed and ice phase clouds exist. Different parameterizations for impaction scavenging changed the predicted global, annual mean number removal attributed to ice clouds by seven-fold, and the global, annual dust mass removal attributed to impaction by two orders of magnitude. Closer agreement with observations of black carbon profiles from aircraft (increases near to one order of magnitude for mixed phase clouds

Quantifying Black Carbon Deposition Over the Greenland Ice Sheet from Forest Fires in Canada

Science.gov (United States)

Thomas, J. L.; Polashenski, C. M.; Soja, Amber J.; Marelle, L.; Casey, K. A.; Choi, H. D.; Raut, J.-C.; Wiedinmyer, C.; Emmons, L. K.; Fast, J. D.;

Sensitivity of Cirrus and Mixed-phase Clouds to the Ice Nuclei Spectra in McRAS-AC: Single Column Model Simulations

Science.gov (United States)

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.

Arctic sea ice melt leads to atmospheric new particle formation.

Science.gov (United States)

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.

Fine-Scale Layering of Mars Polar Deposits and Signatures of Ice Content in Nonpolar Material From Multiband SHARAD Data Processing

Science.gov (United States)

Campbell, Bruce A.; Morgan, Gareth A.

2018-02-01

The variation of Shallow Radar (SHARAD) echo strength with frequency reveals material dielectric losses and polar layer properties. Loss tangents for Elysium and Amazonis Planitiae deposits are consistent with volcanic flows and sediments, while the Medusae Fossae Formation, lineated valley fill, and lobate debris aprons have low losses consistent with a major component of water ice. Mantling materials in Arcadia and Utopia Planitiae have higher losses, suggesting they are not dominated by ice over large fractions of their thickness. In Gemina Lingula, there are frequent deviations from a simple dependence of loss on depth. Within reflector packets, the brightest reflectors are often different among the frequency subbands, and there are cases of reflectors that occur in only the high- or low-frequency echoes. Many polar radar reflections must arise from multiple thin interfaces, or single deposits of appropriate thickness, that display resonant scattering behaviors. Reflector properties may be linked to climate-controlled polar dust deposition.

Ice flow Modelling of the Greenland Ice Sheet

DEFF Research Database (Denmark)

Nielsen, Lisbeth Tangaa

Models of ice flow have a range of application in glaciology, including investigating the large-scale response of ice sheets to changes in climate, assimilating data to estimate unknown conditions beneath the ice sheet, and in interpreting proxy records obtained from ice cores, among others. In t...... a steady state with respect to the reference climate at the end of the simulation and that the mass balance of the ice sheet at this time was more sensitive to recent climate fluctuations than the temperature forcing in the early or mid-Holocene.......Models of ice flow have a range of application in glaciology, including investigating the large-scale response of ice sheets to changes in climate, assimilating data to estimate unknown conditions beneath the ice sheet, and in interpreting proxy records obtained from ice cores, among others....... In this PhD project, the use of ice flow models for the interpretation of the age-structure of the Greenland ice sheet, i.e. the depth within the ice, at which ice deposited at given times are found at present day. Two different observational data sets of this archive were investigated. Further, paleo...

A FIRE-ACE/SHEBA Case Study of Mixed-Phase Arctic Boundary Layer Clouds: Entrainment Rate Limitations on Rapid Primary Ice Nucleation Processes

Science.gov (United States)

Fridlin, Ann; vanDiedenhoven, Bastiaan; Ackerman, Andrew S.; Avramov, Alexander; Mrowiec, Agnieszka; Morrison, Hugh; Zuidema, Paquita; Shupe, Matthew D.

2012-01-01

Observations of long-lived mixed-phase Arctic boundary layer clouds on 7 May 1998 during the First International Satellite Cloud Climatology Project (ISCCP) Regional Experiment (FIRE)Arctic Cloud Experiment (ACE)Surface Heat Budget of the Arctic Ocean (SHEBA) campaign provide a unique opportunity to test understanding of cloud ice formation. Under the microphysically simple conditions observed (apparently negligible ice aggregation, sublimation, and multiplication), the only expected source of new ice crystals is activation of heterogeneous ice nuclei (IN) and the only sink is sedimentation. Large-eddy simulations with size-resolved microphysics are initialized with IN number concentration N(sub IN) measured above cloud top, but details of IN activation behavior are unknown. If activated rapidly (in deposition, condensation, or immersion modes), as commonly assumed, IN are depleted from the well-mixed boundary layer within minutes. Quasi-equilibrium ice number concentration N(sub i) is then limited to a small fraction of overlying N(sub IN) that is determined by the cloud-top entrainment rate w(sub e) divided by the number-weighted ice fall speed at the surface v(sub f). Because w(sub c) 10 cm/s, N(sub i)/N(sub IN)<< 1. Such conditions may be common for this cloud type, which has implications for modeling IN diagnostically, interpreting measurements, and quantifying sensitivity to increasing N(sub IN) (when w(sub e)/v(sub f)< 1, entrainment rate limitations serve to buffer cloud system response). To reproduce observed ice crystal size distributions and cloud radar reflectivities with rapidly consumed IN in this case, the measured above-cloud N(sub IN) must be multiplied by approximately 30. However, results are sensitive to assumed ice crystal properties not constrained by measurements. In addition, simulations do not reproduce the pronounced mesoscale heterogeneity in radar reflectivity that is observed.

Nucleation of microwave plasma CVD diamond on molybdenum (Mo) substrate

International Nuclear Information System (INIS)

Inderjeet, K.; Ramesh, S.

2000-01-01

Molybdenum is a metal, which is gaining increasing significance in industrial applications. The main use of Mo is as all alloying element added in small amounts to steel, irons and non- ferrous alloys in order to enhance the strength, toughness and wear resistance. Mo is also vastly being employed in the automotive and aircraft industries, mainly due to its low coefficient of friction. Diamond, on be other hand, is a unique material for innumerable applications because of its usual combination of physical and chemical properties. Several potential applications can be anticipated for diamond in many sectors including electronics, optics, as protective corrosion resistant coatings, cutting tools, etc. With the enhancement in science and technology, diamond microcrystals and thin films are now being produced from the vapour phase by a variety of chemical vapour deposition (CVD) techniques; such as microwave plasma CVD. With such technology being made available, it is envisage that diamond-coated molybdenum would further enhance the performance and to open up new avenue for Mo in various industries. Therefore, it is the aim of the present work to study the nucleation and growth of diamond particles on Mo surface by employing microwave plasma CVD (MAPCVD). In the present work, diamond deposition was carried out in several stages by varying the deposition distance. The nucleation and growth rate were studied using scanning electron microscopy (SEM). In addition, the existence of diamond was verified by X-ray diffraction (XRD) analysis. It has been found that the nucleation and growth rate of diamond particles were influenced by the deposition height between the substrate and plasma. Under the optimum condition, well defined diamond crystallites distributed homogeneously throughout the surface, could be obtained. Some of the important parameters controlling the deposition and growth of diamond particles on Mo surface are discussed. (author)

A review of phosphate mineral nucleation in biology and geobiology.

Science.gov (United States)

Omelon, Sidney; Ariganello, Marianne; Bonucci, Ermanno; Grynpas, Marc; Nanci, Antonio

2013-10-01

Relationships between geological phosphorite deposition and biological apatite nucleation have often been overlooked. However, similarities in biological apatite and phosphorite mineralogy suggest that their chemical formation mechanisms may be similar. This review serves to draw parallels between two newly described phosphorite mineralization processes, and proposes a similar novel mechanism for biologically controlled apatite mineral nucleation. This mechanism integrates polyphosphate biochemistry with crystal nucleation theory. Recently, the roles of polyphosphates in the nucleation of marine phosphorites were discovered. Marine bacteria and diatoms have been shown to store and concentrate inorganic phosphate (Pi) as amorphous, polyphosphate granules. Subsequent release of these P reserves into the local marine environment as Pi results in biologically induced phosphorite nucleation. Pi storage and release through an intracellular polyphosphate intermediate may also occur in mineralizing oral bacteria. Polyphosphates may be associated with biologically controlled apatite nucleation within vertebrates and invertebrates. Historically, biological apatite nucleation has been attributed to either a biochemical increase in local Pi concentration or matrix-mediated apatite nucleation control. This review proposes a mechanism that integrates both theories. Intracellular and extracellular amorphous granules, rich in both calcium and phosphorus, have been observed in apatite-biomineralizing vertebrates, protists, and atremate brachiopods. These granules may represent stores of calcium-polyphosphate. Not unlike phosphorite nucleation by bacteria and diatoms, polyphosphate depolymerization to Pi would be controlled by phosphatase activity. Enzymatic polyphosphate depolymerization would increase apatite saturation to the level required for mineral nucleation, while matrix proteins would simultaneously control the progression of new biological apatite formation.

Surface poisoning in the nucleation and growth of palladium atomic layer deposition with Pd(hfac){sub 2} and formalin

Energy Technology Data Exchange (ETDEWEB)

Goldstein, D.N. [Department of Chemistry and Biochemistry, University of Colorado, 215 UCB, Boulder, CO 80309 (United States); George, S.M., E-mail: Steven.George@Colorado.Edu [Department of Chemistry and Biochemistry, University of Colorado, 215 UCB, Boulder, CO 80309 (United States); Department of Chemical and Biological Engineering, University of Colorado, 424 UCB, Boulder, CO (United States)

2011-06-01

Palladium (Pd) atomic layer deposition (ALD) can be performed with Pd(hfac){sub 2} (hfac = hexafluoroacetyl-acetone) and formalin as the reactants. For Pd ALD on oxide surfaces, the nucleation of Pd ALD has been observed to require between 20 and 100 ALD cycles. To understand the long nucleation periods, this study explored the surface reactions occurring during Pd ALD nucleation and growth on hydroxylated Al{sub 2}O{sub 3} substrates. In situ Fourier transform infrared (FTIR) spectroscopy on high surface area nanopowders was used to observe the surface species. The adsorption of Pd(hfac){sub 2} on hydroxylated Al{sub 2}O{sub 3} substrates was found to yield both Pd(hfac)* and Al(hfac)* surface species. The identity of the Al(hfac)* species was confirmed by separate FTIR studies of hfacH adsorption on the hydroxylated Al{sub 2}O{sub 3} substrates. Isothermal loss of the Al(hfac)* species revealed second-order kinetics at 448-523 K with an activation barrier of E{sub d} = 39.4 kcal/mol. The lack of correlation between Al(hfac)* and AlOH* species during the loss of Al(hfac)* species suggested that the Al(hfac)* species may desorb as Al(hfac){sub 3}. After Pd(hfac){sub 2} exposure and the subsequent formalin exposure on hydroxylated Al{sub 2}O{sub 3} substrates, only hfac ligands from Pd(hfac)* species were removed from the surface. In addition, the formalin exposure added formate species. The Al(hfac)* species was identified as the cause of the long nucleation period because Al(hfac)* behaves as a site blocker. The surface poisoning by Al(hfac)* species was corroborated by adsorbing hfacH prior to the Pd(hfac){sub 2} exposures. The amount of Pd(hfac)* species after Pd(hfac){sub 2} exposures decreased progressively versus the previous hfacH exposure. Pd ALD occurred gradually during the subsequent Pd ALD cycles as the Al(hfac)* species were slowly removed from the Al{sub 2}O{sub 3} surface. Ex situ transmission electron microscopy analysis revealed Pd nanoclusters

Results from the FIN-2 formal comparison

Science.gov (United States)

Connolly, Paul; Hoose, Corinna; Liu, Xiaohong; Moehler, Ottmar; Cziczo, Daniel; DeMott, Paul

2017-04-01

During the Fifth International Ice Nucleation Workshop (FIN-2) at the AIDA Ice Nucleation facility in Karlsruhe, Germany in March 2015, a formal comparison of ice nucleation measurement methods was conducted. During the experiments the samples of ice nucleating particles were not revealed to the instrument scientists, hence this was referred to as a "blind comparison". The two samples used were later revealed to be Arizona Test Dust and an Argentina soil sample. For these two samples seven mobile ice nucleating particle counters sampled directly from the AIDA chamber or from the aerosol preparation chamber at specified temperatures, whereas filter samples were taken for two offline deposition nucleation instruments. Wet suspension methods for determining IN concentrations were also used with 10 different methods employed. For the wet suspension methods experiments were conducted using INPs collected from the air inside the chambers (impinger sampling) and INPs taken from the bulk samples (vial sampling). Direct comparisons of the ice nucleating particle concentrations are reported as well as derived ice nucleation active site densities. The study highlights the difficulties in performing such analyses, but generally indicates that there is reasonable agreement between the wet suspension techniques. It is noted that ice nucleation efficiency derived from the AIDA chamber (quantified using the ice active surface site density approach) is higher than that for the cold stage techniques. This is both true for the Argentina soil sample and, to a lesser extent, for the Arizona Test Dust sample too. Other interesting effects were noted: for the ATD the impinger sampling demonstrated higher INP efficiency at higher temperatures (>255 K) than the vial sampling, but agreed at the lower temperatures (<255K), whereas the opposite was true for the Argentina soil sample. The results are analysed to better understand the performance of the various techniques and to address any

Heterogeneous Formation of Polar Stratospheric Clouds- Part 1: Nucleation of Nitric Acid Trihydrate (NAT)

Science.gov (United States)

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.

Effect of high temperature deposition on CoSi2 phase formation

International Nuclear Information System (INIS)

Comrie, C. M.; Ahmed, H.; Smeets, D.; Demeulemeester, J.; Vantomme, A.; Turner, S.; Van Tendeloo, G.; Detavernier, C.

2013-01-01

This paper discusses the nucleation behaviour of the CoSi to CoSi 2 transformation from cobalt silicide thin films grown by deposition at elevated substrate temperatures ranging from 375 °C to 600 °C. A combination of channelling, real-time Rutherford backscattering spectrometry, real-time x-ray diffraction, and transmission electron microscopy was used to investigate the effect of the deposition temperature on the subsequent formation temperature of CoSi 2 , its growth behaviour, and the epitaxial quality of the CoSi 2 thus formed. The temperature at which deposition took place was observed to exert a significant and systematic influence on both the formation temperature of CoSi 2 and its growth mechanism. CoSi films grown at the lowest temperatures were found to increase the CoSi 2 nucleation temperature above that of CoSi 2 grown by conventional solid phase reaction, whereas the higher deposition temperatures reduced the nucleation temperature significantly. In addition, a systematic change in growth mechanism of the subsequent CoSi 2 growth occurs as a function of deposition temperature. First, the CoSi 2 growth rate from films grown at the lower reactive deposition temperatures is substantially lower than that grown at higher reactive deposition temperatures, even though the onset of growth occurs at a higher temperature, Second, for deposition temperatures below 450 °C, the growth appears columnar, indicating nucleation controlled growth. Elevated deposition temperatures, on the other hand, render the CoSi 2 formation process layer-by-layer which indicates enhanced nucleation of the CoSi 2 and diffusion controlled growth. Our results further indicate that this observed trend is most likely related to stress and changes in microstructure introduced during reactive deposition of the CoSi film. The deposition temperature therefore provides a handle to tune the CoSi 2 growth mechanism.

Control of Reaction Surface in Low Temperature CVD to Enhance Nucleation and Conformal Coverage

Science.gov (United States)

Kumar, Navneet

2009-01-01

The Holy Grail in CVD community is to find precursors that can afford the following: good nucleation on a desired substrate and conformal deposition in high AR features. Good nucleation is not only necessary for getting ultra-thin films at low thicknesses; it also offers films that are smooth at higher thickness values. On the other hand,…

Stick-slip Cycles and Tidal Modulation of Ice Stream Flow

Science.gov (United States)

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

7YSZ coating prepared by PS-PVD based on heterogeneous nucleation

Directory of Open Access Journals (Sweden)

Ziqian DENG

2018-04-01

Full Text Available Plasma spray-physical vapor deposition (PS-PVD as a novel coating process based on low-pressure plasma spray (LPPS has been significantly used for thermal barrier coatings (TBCs. A coating can be deposited from liquid splats, nano-sized clusters, and the vapor phase forming different structured coatings, which shows obvious advantages in contrast to conventional technologies like atmospheric plasma spray (APS and electron beam-physical vapor deposition (EB-PVD. In addition, it can be used to produce thin, dense, and porous ceramic coatings for special applications because of its special characteristics, such as high power, very low pressure, etc. These provide new opportunities to obtain different advanced microstructures, thus to meet the growing requirements of modern functional coatings. In this work, focusing on exploiting the potential of gas-phase deposition from PS-PVD, a series of 7YSZ coating experiments with various process conditions was performed in order to better understand the deposition process in PS-PVD, where coatings were deposited on different substrates including graphite and zirconia. Meanwhile, various substrate temperatures were investigated for the same substrate. As a result, a deposition mechanism of heterogeneous nucleation has been presented showing that surface energy is an important influencing factor for coating structures. Besides, undercooling of the interface between substrate and vapor phase plays an important role in coating structures. Keywords: 7YSZ, Deposition mechanism, Heterogeneous nucleation, PS-PVD, TBC

Observed degradation stages of ring-mold craters (RMC): Geomorphic evidence for modification of ice-rich deposits in the transitions zone between Elysium and Utopia Basin, Mars

DEFF Research Database (Denmark)

Pedersen, Gro Birkefeldt Møller

Deposits with pits, depressions and RMCs observed north of Elysium rise are interpreted as degraded mixtures of ice and clastic material (CCF, LVF and LDA). Degradation stages of RMCs are an important tool for mapping dusty, deflated ice-rich units....

Prognostic parameterization of cloud ice with a single category in the aerosol-climate model ECHAM(v6.3.0)-HAM(v2.3)

Science.gov (United States)

Dietlicher, Remo; Neubauer, David; Lohmann, Ulrike

2018-04-01

A new scheme for stratiform cloud microphysics has been implemented in the ECHAM6-HAM2 general circulation model. It features a widely used description of cloud water with two categories for cloud droplets and raindrops. The unique aspect of the new scheme is the break with the traditional approach to describe cloud ice analogously. Here we parameterize cloud ice by a single category that predicts bulk particle properties (P3). This method has already been applied in a regional model and most recently also in the Community Atmosphere Model 5 (CAM5). A single cloud ice category does not rely on heuristic conversion rates from one category to another. Therefore, it is conceptually easier and closer to first principles. This work shows that a single category is a viable approach to describe cloud ice in climate models. Prognostic representation of sedimentation is achieved by a nested approach for sub-stepping the cloud microphysics scheme. This yields good results in terms of accuracy and performance as compared to simulations with high temporal resolution. Furthermore, the new scheme allows for a competition between various cloud processes and is thus able to unbiasedly represent the ice formation pathway from nucleation to growth by vapor deposition and collisions to sedimentation. Specific aspects of the P3 method are evaluated. We could not produce a purely stratiform cloud where rime growth dominates growth by vapor deposition and conclude that the lack of appropriate conditions renders the prognostic parameters associated with the rime properties unnecessary. Limitations inherent in a single category are examined.

Rainfall drives atmospheric ice-nucleating particles in the coastal climate of southern Norway

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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.

Electrochemical Deposition of Aluminum from NaCl-AlCl3 Melts

DEFF Research Database (Denmark)

Li, Qingfeng; Hjuler, H. A.; Berg, Rolf W.

1990-01-01

Electrochemical deposition of aluminum from NaAlCl4 melts saturated with NaCl onto a glassy carbon electrode at175°C has been studied by voltammetry, chronoamperometry, and constant current deposition. The deposition of aluminumwas found to proceed via a nucleation/growth mechanism, and the nucle......Electrochemical deposition of aluminum from NaAlCl4 melts saturated with NaCl onto a glassy carbon electrode at175°C has been studied by voltammetry, chronoamperometry, and constant current deposition. The deposition of aluminumwas found to proceed via a nucleation/growth mechanism......, and the nucleation process was found to be progressive.The morphology of aluminum deposits was examined with photomicroscopy. It was shown that depending on the currentdensities (c.d.) applied, three types of aluminum deposits could be obtained, namely, spongy deposits formed at lower c.d.(below 0.7 mA/cm2), smooth...... layers deposited at intermediate c.d. (between 2 and 10 mA/cm2), and dendritic or porous depositsobtained at high c.d. (above 15 mA/cm2). However, the smooth aluminum deposits were about five times more voluminousthan the theoretical value. The spongy deposits were formed due to difficulties...

Experimental Study on Ice Forming Process of Cryogenic Liquid Releasing underwater

Science.gov (United States)

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.

The role of surface defects in HOPG on the electrochemical and physical deposition of Ag

Directory of Open Access Journals (Sweden)

R. PETROVIC

1999-08-01

Full Text Available The role of defects on a substrate surface during the initial stages of nucleation and growth of Ag deposited electrochemically and physically on highly oriented pyrolytic graphite (HOPG has been observed ex situ by scanning tunneling microscopy (STM. The silver was electrodeposited under current controlled electrochemical conditions at 26 µA/cm2, which corresponded to a deposition rate of 0.1 monolayers (ML per second. For comparison, physical deposition of Ag on HOPG was performed by DC Ar+ ion sputtering, at the same deposition rate and for the same deposition times. In both cases, Ag grows in an island growth mode, but the distribution of the islands appears to be quite different. In physical deposition, the Ag islands are almost homogeneously distributed over the substrate surface and a slight accumulation of islands on steps does not contribute significantly to the overall morphology. This indicates the crucial role of point defects on the substrate in the initial stages of nucleation. In electrochemical deposition, more lined defects are observed after a flow of current, and their role in the beginning of the nucleation is more pronounced. Lined defects are responsible for the string-like shaped domains of deposited atoms. Also, the existence of string-like shaped nucleation exclusion zones is indicated. The problem of the formation of nucleation exclusion zones, which appear only in electrochemical deposition, has been reconsidered and a new explanaton of their formation is given. A mathematical model for the calculation of the radius of the nucleation exclusion zone has been developed.

IceCube systematic errors investigation: Simulation of the ice

Energy Technology Data Exchange (ETDEWEB)

Resconi, Elisa; Wolf, Martin [Max-Planck-Institute for Nuclear Physics, Heidelberg (Germany); Schukraft, Anne [RWTH, Aachen University (Germany)

2010-07-01

IceCube is a neutrino observatory for astroparticle and astronomy research at the South Pole. It uses one cubic kilometer of Antartica's deepest ice (1500 m-2500 m in depth) to detect Cherenkov light, generated by charged particles traveling through the ice, with an array of phototubes encapsulated in glass pressure spheres. The arrival time as well as the charge deposited of the detected photons represent the base measurements that are used for track and energy reconstruction of those charged particles. The optical properties of the deep antarctic ice vary from layer to layer. Measurements of the ice properties and their correct modeling in Monte Carlo simulation is then of primary importance for the correct understanding of the IceCube telescope behavior. After a short summary about the different methods to investigate the ice properties and to calibrate the detector, we show how the simulation obtained by using this information compares to the measured data and how systematic errors due to uncertain ice properties are determined in IceCube.

Simulating Aerosol Size Distribution and Mass Concentration with Simultaneous Nucleation, Condensation/Coagulation, and Deposition with the GRAPES-CUACE

Science.gov (United States)

Zhou, Chunhong; Shen, Xiaojing; Liu, Zirui; Zhang, Yangmei; Xin, Jinyuan

2018-04-01

A coupled aerosol-cloud model is essential for investigating the formation of haze and fog and the interaction of aerosols with clouds and precipitation. One of the key tasks of such a model is to produce correct mass and number size distributions of aerosols. In this paper, a parameterization scheme for aerosol size distribution in initial emission, which took into account the measured mass and number size distributions of aerosols, was developed in the GRAPES-CUACE [Global/Regional Assimilation and PrEdiction System-China Meteorological Administration (CMA) Unified Atmospheric Chemistry Environment model]—an online chemical weather forecast system that contains microphysical processes and emission, transport, and chemical conversion of sectional multi-component aerosols. In addition, the competitive mechanism between nucleation and condensation for secondary aerosol formation was improved, and the dry deposition was also modified to be in consistent with the real depositing length. Based on the above improvements, the GRAPES-CUACE simulations were verified against observational data during 1-31 January 2013, when a series of heavy regional haze-fog events occurred in eastern China. The results show that the aerosol number size distribution from the improved experiment was much closer to the observation, whereas in the old experiment the number concentration was higher in the nucleation mode and lower in the accumulation mode. Meanwhile, the errors in aerosol number size distribution as diagnosed by its sectional mass size distribution were also reduced. Moreover, simulations of organic carbon, sulfate, and other aerosol components were improved and the overestimation as well as underestimation of PM2.5 concentration in eastern China was significantly reduced, leading to increased correlation coefficient between simulated and observed PM2.5 by more than 70%. In the remote areas where bad simulation results were produced previously, the correlation coefficient

The effect of ion-beam induced strain on the nucleation density of chemical vapour deposited diamond

International Nuclear Information System (INIS)

Weiser, P.S.; Prawer, S.; Nugent, K.W.; Bettiol, A.A.; Kostidis, L.I.; Jamieson, D.N.

1995-01-01

The effect of ion implantation on the nucleation of CVD diamond on silicon and diamond substrates has been investigated. The strategy employed is to create laterally confined regions of strain in the substrates by focused MeV implantation of light ions. Raman Microscopy has been employed to obtain spatially resolved maps of the strain in these implanted regions. On diamond substrates a homo-epitaxial CVD diamond film was grown on top of both the implanted and unimplanted regions of the substrate. Raman analysis of the film grown on top of the implanted region revealed it to be under slightly tensile strain as compared to that grown on the unimplanted diamond substrate. The film deposited on the implanted portion of the diamond showed a lower fluorescence background; indicating a lower concentration of incorporated defects. These results suggest that the strain and defects in the diamond substrate material have an important influence on the quality of the homo-epitaxially grown diamond films. 6 refs., 5 figs

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

Nacre biomineralisation: A review on the mechanisms of crystal nucleation.

Science.gov (United States)

Nudelman, Fabio

2015-10-01

The wide diversity of biogenic minerals that is found in nature, each with its own morphology, mechanical properties and composition, is remarkable. In order to produce minerals that are optimally adapted for their function, biomineralisation usually occurs under strict cellular control. This control is exerted by specialised proteins and polysaccharides that assemble into a 3-dimensional organic matrix framework, forming a microenvironment where mineral deposition takes place. Molluscs are unique in that they use a striking variety of structural motifs to build their shells, each made of crystals with different morphologies and different calcium carbonate polymorphs. Much of want is known about mollusc shell formation comes from studies on the nacreous layer, or mother-of-pearl. In this review, we discuss two existing models on the nucleation of aragonite crystals during nacre formation: heteroepitaxial nucleation and mineral bridges. The heteroepitaxial nucleation model is based on the identification of chemical functional groups and aragonite-nucleating proteins at the centre of crystal imprints. It proposes that during nacre formation, each aragonite tablet nucleates independently on a nucleation site that is formed by acidic proteins and/or glycoproteins adsorbed on the chitin scaffold. The mineral bridges model is based on the identification of physical connections between the crystals in a stack, which results in a large number of crystals across several layers sharing the same crystallographic orientation. These observations suggest that there is one nucleation event per stack of tablets. Once the first crystal nucleates and reaches the top interlamellar matrix, it continues growing through pores, giving rise to the next layer of nacre, subsequently propagating into a stack. We compare both models and propose that they work in concert to control crystal nucleation in nacre. De novo crystal nucleation has to occur at least once per stack of aligned crystals

Comparison in Schemes for Simulating Depositional Growth of Ice Crystal between Theoretical and Laboratory Data

Science.gov (United States)

Zhai, Guoqing; Li, Xiaofan

2015-04-01

The Bergeron-Findeisen process has been simulated using the parameterization scheme for the depositional growth of ice crystal with the temperature-dependent theoretically predicted parameters in the past decades. Recently, Westbrook and Heymsfield (2011) calculated these parameters using the laboratory data from Takahashi and Fukuta (1988) and Takahashi et al. (1991) and found significant differences between the two parameter sets. There are two schemes that parameterize the depositional growth of ice crystal: Hsie et al. (1980), Krueger et al. (1995) and Zeng et al. (2008). In this study, we conducted three pairs of sensitivity experiments using three parameterization schemes and the two parameter sets. The pre-summer torrential rainfall event is chosen as the simulated rainfall case in this study. The analysis of root-mean-squared difference and correlation coefficient between the simulation and observation of surface rain rate shows that the experiment with the Krueger scheme and the Takahashi laboratory-derived parameters produces the best rain-rate simulation. The mean simulated rain rates are higher than the mean observational rain rate. The calculations of 5-day and model domain mean rain rates reveal that the three schemes with Takahashi laboratory-derived parameters tend to reduce the mean rain rate. The Krueger scheme together with the Takahashi laboratory-derived parameters generate the closest mean rain rate to the mean observational rain rate. The decrease in the mean rain rate caused by the Takahashi laboratory-derived parameters in the experiment with the Krueger scheme is associated with the reductions in the mean net condensation and the mean hydrometeor loss. These reductions correspond to the suppressed mean infrared radiative cooling due to the enhanced cloud ice and snow in the upper troposphere.

Ice Thickness, Melting Rates and Styles of Activity in Ice-Volcano Interaction

Science.gov (United States)

Gudmundsson, M. T.

2005-12-01

In most cases when eruptions occur within glaciers they lead to rapid ice melting, jokulhlaups and/or lahars. Many parameters influence the style of activity and its impact on the environment. These include ice thickness (size of glacier), bedrock geometry, magma flow rate and magma composition. The eruptions that have been observed can roughly be divided into: (1) eruptions under several hundred meters thick ice on a relatively flat bedrock, (2) eruptions on flat or sloping bed through relatively thin ice, and (3) volcanism where effects are limitied to confinement of lava flows or melting of ice by pyroclastic flows or surges. This last category (ice-contact volcanism) need not cause much ice melting. Many of the deposits formed by Pleistocene volcanism in Iceland, British Columbia and Antarctica belong to the first category. An important difference between this type of activity and submarine activity (where pressure is hydrostatic) is that pressure at vents may in many cases be much lower than glaciostatic due to partial support of ice cover over vents by the surrounding glacier. Reduced pressure favours explosive activity. Thus the effusive/explosive transition may occur several hundred metres underneath the ice surface. Explosive fragmentation of magma leads to much higher rates of heat transfer than does effusive eruption of pillow lavas, and hence much higher melting rates. This effect of reduced pressure at vents will be less pronounced in a large ice sheet than in a smaller glacier or ice cap, since the hydraulic gradient that drives water away from an eruption site will be lower in the large glacier. This may have implications for form and type of eruption deposits and their relationship with ice thickness and glacier size.