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Sample records for depositional ice nucleation

  1. Differences in ice nucleation behavior of arable and desert soil dust in deposition nucleation regime

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    Ullrich, Romy; Vogel, Franziska; Möhler, Ottmar; Höhler, Kristina; Schiebel, Thea

    2017-04-01

    Soil dust from arid and semi-arid regions is one of the most abundant aerosol types in the atmosphere with emission rates of about 1600 Tg per year (Andreae et al. (2009)). Therewith, soil dust plays an important role for the atmospheric radiative transfer and also for the formation of clouds. Soil dust refers to dust sampled from agricultural used areas, to dust from bare soil as well as to dust from desert regions. By mass-spectrometric measurements of the chemical composition of ice residuals, mineral dust as component of soil dust was found to be the major heterogeneous ice nucleating particle (INP) type (e.g. Cziczo et al. (2013)), in particular in the upper troposphere. Also in laboratory studies the ice nucleation efficiency of the different soil dusts was investigated. It was shown that desert dusts (Ullrich et al. (2017)) as well as soil dusts from arable regions (O'Sullivan et al. (2014), Tobo et al. (2014)) are efficient INP. However, there is still a lack of data for ice nucleation on soil dusts for temperatures below about 220 K. With the AIDA (Aerosol Interactions and Dynamics in the Atmosphere) cloud chamber, we are able to characterize the ice nucleation efficiency for different aerosol types to temperatures down to 180 K and high ice supersaturations. In order to extend the already existing AIDA data base for deposition nucleation on desert dusts and agricultural soil dusts, new experiments were done in the upper tropospheric temperature regime. This contribution will show the results of the new experiments with desert dust in comparison to existing data for higher temperatures. The first data analysis confirms the temperature dependent trend of the ice nucleation activity as discussed and parameterized in a recent paper by Ullrich et al. (2017). Furthermore, the update and extension of the recently published parameterization of deposition nucleation for desert dust to lower temperatures will be discussed. The experiments with agricultural soil

  2. Deposition and immersion-mode nucleation of ice by three distinct samples of volcanic ash

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    Schill, G. P.; Genareau, K.; Tolbert, M. A.

    2015-07-01

    Ice nucleation of volcanic ash controls both ash aggregation and cloud glaciation, which affect atmospheric transport and global climate. Previously, it has been suggested that there is one characteristic ice nucleation efficiency for all volcanic ash, regardless of its composition, when accounting for surface area; however, this claim is derived from data from only two volcanic eruptions. In this work, we have studied the depositional and immersion freezing efficiency of three distinct samples of volcanic ash using Raman microscopy coupled to an environmental cell. Ash from the Fuego (basaltic ash, Guatemala), Soufrière Hills (andesitic ash, Montserrat), and Taupo (Oruanui eruption, rhyolitic ash, New Zealand) volcanoes were chosen to represent different geographical locations and silica content. All ash samples were quantitatively analyzed for both percent crystallinity and mineralogy using X-ray diffraction. In the present study, we find that all three samples of volcanic ash are excellent depositional ice nuclei, nucleating ice from 225 to 235 K at ice saturation ratios of 1.05 ± 0.01, comparable to the mineral dust proxy kaolinite. Since depositional ice nucleation will be more important at colder temperatures, fine volcanic ash may represent a global source of cold-cloud ice nuclei. For immersion freezing relevant to mixed-phase clouds, however, only the Oruanui ash exhibited appreciable heterogeneous ice nucleation activity. Similar to recent studies on mineral dust, we suggest that the mineralogy of volcanic ash may dictate its ice nucleation activity in the immersion mode.

  3. Depositional ice nucleation on solid ammonium sulfate and glutaric acid particles

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    K. J. Baustian

    2010-03-01

    Full Text Available Heterogeneous ice nucleation on solid ammonium sulfate and glutaric acid particles was studied using optical microscopy and Raman spectroscopy. Optical microscopy was used to detect selective nucleation events as water vapor was slowly introduced into an environmental sample cell. Particles that nucleated ice were dried via sublimation and examined in detail using Raman spectroscopy. Depositional ice nucleation is highly selective and occurred preferentially on just a few ammonium sulfate and glutaric acid particles in each sample. For freezing temperatures between 214 K and 235 K an average ice saturation ratio of S = 1.10±0.07 for solid ammonium sulfate was observed. Over the same temperature range, S values observed for ice nucleation on glutaric acid particles increased from 1.2 at 235 K to 1.6 at 218 K. Experiments with externally mixed particles further show that ammonium sulfate is a more potent ice nucleus than glutaric acid. Our results suggest that heterogeneous nucleation on ammonium sulfate may be an important pathway for atmospheric ice nucleation and cirrus cloud formation when solid ammonium sulfate aerosol particles are available for ice formation. This pathway for ice formation may be particularly significant near the tropical tropopause region where sulfates are abundant and other species known to be good ice nuclei are depleted.

  4. Deposition-mode ice nucleation reexamined at temperatures below 200 K

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    Thomson, E. S.; Kong, X.; Papagiannakopoulos, P.; Pettersson, J. B. C.

    2015-02-01

    The environmental chamber of a molecular beam apparatus is used to study deposition nucleation of ice on graphite, alcohols and acetic and nitric acids at temperatures between 155 and 200 K. The critical supersaturations necessary to spontaneously nucleate water ice on six different substrate materials are observed to occur at higher supersaturations than are theoretically predicted. This contradictory result motivates more careful examination of the experimental conditions and the underlying basis of the current theories. An analysis based on classical nucleation theory supports the view that at these temperatures nucleation is primarily controlled by the rarification of the vapor and the strength of water's interaction with the substrate surface. The technique enables a careful probing of the underlying processes of ice nucleation and the substrate materials of study. The findings are relevant to atmospheric nucleation processes that are intrinsically linked to cold cloud formation and lifetime.

  5. Laboratory studies of immersion and deposition mode ice nucleation of ozone aged mineral dust particles

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    Z. A. Kanji

    2013-04-01

    Full Text Available Ice nucleation in the atmosphere is central to the understanding the microphysical properties of mixed-phase and cirrus clouds. Ambient conditions such as temperature (T and relative humidity (RH, as well as aerosol properties such as chemical composition and mixing state play an important role in predicting ice formation in the troposphere. Previous field studies have reported the absence of sulphate and organic compounds on mineral dust ice crystal residuals sampled at mountain top stations or aircraft based measurements despite the long range transport mineral dust is subjected to. We present laboratory studies of ice nucleation for immersion and deposition mode on ozone aged mineral dust particles for 233 T ns are reported and observed to increase as a function of temperature. We present first results that demonstrate enhancement of the ice nucleation ability of aged mineral dust particles in both the deposition and immersion mode due to ageing. Additionally, these are also the first results to show a suppression of heterogeneous ice nucleation without the condensation of a coating of (inorganic material. In immersion mode, low exposure Ka particles showed enhanced ice activity requiring a median freezing temperature of 1.5 K warmer than that of untreated Ka whereas high exposure ATD particles showed suppressed ice nucleation requiring a median freezing temperature of 3 K colder than that of untreated ATD. In deposition mode, low exposure Ka had ice active fractions of an order of magnitude higher than untreated Ka, where as high exposure ATD had ice active fractions up to a factor of 4 lower than untreated ATD. Based on our results, we present parameterizations in terms of ns(T that can represent ice nucleation of atmospherically aged and non-aged particles for both immersion and deposition mode. We find excellent agreement (to within less than a factor of 2 with field measurements when parameterizations derived from our results are used to

  6. Laboratory studies of immersion and deposition mode ice nucleation of ozone aged mineral dust particles

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    Kanji, Z. A.; Welti, A.; Chou, C.; Stetzer, O.; Lohmann, U.

    2013-09-01

    Ice nucleation in the atmosphere is central to the understanding the microphysical properties of mixed-phase and cirrus clouds. Ambient conditions such as temperature (T) and relative humidity (RH), as well as aerosol properties such as chemical composition and mixing state play an important role in predicting ice formation in the troposphere. Previous field studies have reported the absence of sulfate and organic compounds on mineral dust ice crystal residuals sampled at mountain top stations or aircraft based measurements despite the long-range transport mineral dust is subjected to. We present laboratory studies of ice nucleation for immersion and deposition mode on ozone aged mineral dust particles for 233 < T < 263 K. Heterogeneous ice nucleation of untreated kaolinite (Ka) and Arizona Test Dust (ATD) particles is compared to corresponding aged particles that are subjected to ozone concentrations of 0.4-4.3 ppmv in a stainless steel aerosol tank. The portable ice nucleation counter (PINC) and immersion chamber combined with the Zurich ice nucleation chamber (IMCA-ZINC) are used to conduct deposition and immersion mode measurements, respectively. Ice active fractions as well as ice active surface site densities (ns) are reported and observed to increase as a function of decreasing temperature. We present first results that demonstrate enhancement of the ice nucleation ability of aged mineral dust particles in both the deposition and immersion mode due to ageing. We also present the first results to show a suppression of heterogeneous ice nucleation activity without the condensation of a coating of (in)organic material. In immersion mode, low ozone exposed Ka particles showed enhanced ice activity requiring a median freezing temperature of 1.5 K warmer than that of untreated Ka, whereas high ozone exposed ATD particles showed suppressed ice nucleation requiring a median freezing temperature of 3 K colder than that of untreated ATD. In deposition mode, low

  7. Comparative study of ice nucleating efficiency of K-feldspar in immersion and deposition freezing modes

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    Hiron, T.; Hoffmann, N.; Peckhaus, A.; Kiselev, A. A.; Leisner, T.; Flossmann, A. I.

    2016-12-01

    One of the main challenges in understanding the evolution of Earth's climate resides in the understanding the role of ice nucleation on the development of tropospheric clouds as well as its initiation. K-feldspar is known to be a very active ice nucleating particle and this study focuses on the characterization of its activity in two heterogeneous nucleation modes, immersion and deposition freezing.We use a newly built humidity-controlled cold stage allowing the simultaneous observation of up to 2000 identical 0.6-nanoliter droplets containing suspension of mineral dust particles. The droplets are first cooled down to observe immersion freezing, the obtained ice crystals are then evaporated and finally, the residual particles are exposed to the water vapor supersaturated with respect to ice.The ice nucleation abilities for the individual residual particles are then compared for the different freezing modes and correlation between immersion ice nuclei and deposition ice nuclei is investigated.Based on the electron microscopy analysis of the residual particles, we discuss the possible relationship between the ice nucleation properties of feldspar and its microstructure. Finally, we discuss the atmospheric implications of our experimental results, using DESCAM, a 1.5D bin-resolved microphysics model.

  8. Laboratory studies of immersion and deposition mode ice nucleation of ozone aged mineral dust particles

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    Z. A. Kanji

    2013-09-01

    Full Text Available Ice nucleation in the atmosphere is central to the understanding the microphysical properties of mixed-phase and cirrus clouds. Ambient conditions such as temperature (T and relative humidity (RH, as well as aerosol properties such as chemical composition and mixing state play an important role in predicting ice formation in the troposphere. Previous field studies have reported the absence of sulfate and organic compounds on mineral dust ice crystal residuals sampled at mountain top stations or aircraft based measurements despite the long-range transport mineral dust is subjected to. We present laboratory studies of ice nucleation for immersion and deposition mode on ozone aged mineral dust particles for 233 T ns are reported and observed to increase as a function of decreasing temperature. We present first results that demonstrate enhancement of the ice nucleation ability of aged mineral dust particles in both the deposition and immersion mode due to ageing. We also present the first results to show a suppression of heterogeneous ice nucleation activity without the condensation of a coating of (inorganic material. In immersion mode, low ozone exposed Ka particles showed enhanced ice activity requiring a median freezing temperature of 1.5 K warmer than that of untreated Ka, whereas high ozone exposed ATD particles showed suppressed ice nucleation requiring a median freezing temperature of 3 K colder than that of untreated ATD. In deposition mode, low exposure Ka had ice active fractions of an order of magnitude higher than untreated Ka, whereas high ozone exposed ATD had ice active fractions up to a factor of 4 lower than untreated ATD. From our results, we derive and present parameterizations in terms of ns(T that can be used in models to predict ice nuclei concentrations based on available aerosol surface area.

  9. Efficiency of the deposition mode ice nucleation on mineral dust particles

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    O. Möhler

    2006-01-01

    Full Text Available The deposition mode ice nucleation efficiency of various dust aerosols was investigated at cirrus cloud temperatures between 196 and 223 K using the aerosol and cloud chamber facility AIDA (Aerosol Interaction and Dynamics in the Atmosphere. Arizona test dust (ATD as a reference material and two dust samples from the Takla Makan desert in Asia (AD1 and the Sahara (SD2 were used for the experiments at simulated cloud conditions. The dust particle sizes were almost lognormally distributed with mode diameters between 0.3 and 0.5 μm and geometric standard deviations between 1.6 and 1.9. Deposition ice nucleation was most efficient on ATD particles with ice-active particle fractions of about 0.6 and 0.8 at an ice saturation ratio SiSiSi. This indicates that deposition ice nucleation on mineral particles may not be treated in the same stochastic sense as homogeneous freezing. The suggested formulation of ice activation spectra may be used to calculate the formation rate of ice crystals in models, if the number concentration of dust particles is known. More experimental work is needed to quantify the variability of the ice activation spectra as function of the temperature and dust particle properties.

  10. Depositional and Immersion-Mode Ice Nucleation of Fine-Grained Volcanic Ash Samples

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    Cloer, S.; Woods, T.; Genareau, K. D.

    2016-12-01

    Volcanic lightning is a common phenomenon during explosive eruptions; occurring as vent discharges, near-vent discharges, and plume lightning. Plume lightning is most similar to thunderstorm lightning, where volcanic ash may act as ice nuclei. Volcanic ash samples derived from eight volcanoes: Augustine, Crater Peak, Katmai, Okmok, Redoubt (Alaska, U.S.A.), Lathrop Well (Nevada, U.S.A.), Taupo (New Zealand), and Valles Caldera (New Mexico, U.S.A.); were used to determine what roles ash mineralogy, particularly Fe-oxide-bearing minerals and silica-enriched minerals, grain shape, and grain size have in the nucleation of ice, which can generate plume lightning. Depositional and immersion-mode ice nucleation experiments were performed using a Nicolet Almega XR Dispersive Raman spectrometer, following the methods of Schill et al. (2015), where samples were shaken for 24 h prior to experiments in ultra-pure water, then nebulized to super micron droplets. Depositional nucleation experiments were conducted from 225-235 K, and immersion-mode nucleation experiments were conducted from 233-278 K. A JEOL JSM 6010 Plus/LA scanning electron microscope (SEM), along with Image-J freeware, was used to quantify the number density of Fe-oxide mineral phases in backscattered electron images, with an x-ray diffractometer (XRD) used to determine bulk mineral abundance and an x-ray fluorescence (XRF) spectrometer to determine bulk ash composition. Based on previous studies, we hypothesize that all ash samples will efficiently form depositional ice nuclei; however, certain mineral phases will dictate the efficiency of immersion-mode ice nucleation including K or Na / Ca feldspars, which have been shown to be efficient nuclei, and Fe-oxide-bearing minerals. These results will shed new light on volcanic cloud dynamics and add new parameters for atmospheric models, which currently only address effects of mineral dust as ice nuclei and overlook the potential role of volcanic ash.

  11. Laboratory measurements and model sensitivity studies of dust deposition ice nucleation

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    G. Kulkarni

    2012-08-01

    Full Text Available We investigated the ice nucleating properties of mineral dust particles to understand the sensitivity of simulated cloud properties to two different representations of contact angle in the Classical Nucleation Theory (CNT. These contact angle representations are based on two sets of laboratory deposition ice nucleation measurements: Arizona Test Dust (ATD particles of 100, 300 and 500 nm sizes were tested at three different temperatures (−25, −30 and −35 °C, and 400 nm ATD and kaolinite dust species were tested at two different temperatures (−30 and −35 °C. These measurements were used to derive the onset relative humidity with respect to ice (RHice required to activate 1% of dust particles as ice nuclei, from which the onset single contact angles were then calculated based on CNT. For the probability density function (PDF representation, parameters of the log-normal contact angle distribution were determined by fitting CNT-predicted activated fraction to the measurements at different RHice. Results show that onset single contact angles vary from ~18 to 24 degrees, while the PDF parameters are sensitive to the measurement conditions (i.e. temperature and dust size. Cloud modeling simulations were performed to understand the sensitivity of cloud properties (i.e. ice number concentration, ice water content, and cloud initiation times to the representation of contact angle and PDF distribution parameters. The model simulations show that cloud properties are sensitive to onset single contact angles and PDF distribution parameters. The comparison of our experimental results with other studies shows that under similar measurement conditions the onset single contact angles are consistent within ±2.0 degrees, while our derived PDF parameters have larger discrepancies.

  12. Laboratory measurements and model sensitivity studies of dust deposition ice nucleation

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    G. Kulkarni

    2012-01-01

    Full Text Available We investigated the ice nucleating properties of mineral dust particles to understand the sensitivity of modeled cloud properties to different representations of contact angle in the Classical Nucleation Theory (CNT: onset single angle and probability density function (PDF distribution approaches. These contact angle representations are based on two sets of laboratory deposition ice nucleation measurements: Arizona Test Dust (ATD particles of 100, 300, and 500 nm sizes were tested at three different temperatures (−25, −30 and −35 °C, and 400 nm ATD and Kaolinite dust species were tested at two different temperatures (−30 and −35 °C. These measurements were used to derive the onset relative humidity with respect to ice (RHice required to activate 1% of dust particles as ice nuclei, from which the onset single contact angles were then calculated based on the CNT. For the PDF representation, parameters of the log-normal contact angle distribution (mean and standard deviation were determined by fitting the CNT-predicted activated fraction to the measurements at different RHice. Results show that onset single contact angles are not much different between experiments, while the PDF parameters are sensitive to those environmental conditions (i.e., temperature and dust size. The cloud resolving model simulations show that cloud properties (i.e. ice number concentration, ice water content, and cloud initiation times are sensitive to onset single contact angles and PDF distribution parameters, particularly to the mean value. The comparison of our experimental results with other studies shows that under similar measurement conditions the onset single contact angles are consistent within ±2.0°, while our derived PDF parameters have discrepancies.

  13. Deposition and immersion mode nucleation of ice by three distinct samples of volcanic ash using Raman spectroscopy

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    Schill, G. P.; Genareau, K.; Tolbert, M. A.

    2015-01-01

    Ice nucleation on volcanic ash controls both ash aggregation and cloud glaciation, which affect atmospheric transport and global climate. Previously, it has been suggested that there is one characteristic ice nucleation efficiency for all volcanic ash, regardless of its composition, when accounting for surface area; however, this claim is derived from data from only two volcanic eruptions. In this work, we have studied the depositional and immersion freezing efficiency of three distinct samples of volcanic ash using Raman Microscopy coupled to an environmental cell. Ash from the Fuego (basaltic ash, Guatemala), Soufrière Hills (andesitic ash, Montserrat), and Taupo (Oruanui euption, rhyolitic ash, New Zealand) volcanoes were chosen to represent different geographical locations and silica content. All ash samples were quantitatively analyzed for both percent crystallinity and mineralogy using X-ray diffraction. In the present study, we find that all three samples of volcanic ash are excellent depositional ice nuclei, nucleating ice from 225-235 K at ice saturation ratios of 1.05 ± 0.01, comparable to the mineral dust proxy kaolinite. Since depositional ice nucleation will be more important at colder temperatures, fine volcanic ash may represent a global source of cold-cloud ice nuclei. For immersion freezing relevant to mixed-phase clouds, however, only the Oruanui ash exhibited heterogeneous ice nucleation activity. Similar to recent studies on mineral dust, we suggest that the mineralogy of volcanic ash may dictate its ice nucleation activity in the immersion mode.

  14. Ice Formation via Deposition Mode Nucleation on Bare and Alcohol-covered Graphite Surfaces

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    Kong, Xiangrui; Thomson, Erik S; Pettersson, Jan B C

    2013-01-01

    Deposition of water on aerosol particles contributes to ice cloud formation in the atmosphere with implications for the water cycle and climate on Earth. The heterogeneous ice nucleation process is influenced by physico-chemical properties of the substrate, but the mechanisms remain incompletely understood. Here, we report on ice formation on bare and alcohol-covered graphite at temperatures from 175 to 213 K, probed by elastic helium and light scattering. Water has a low wettability on bare and butanol-covered graphite resulting in the growth of rough ice surfaces. In contrast, pre-adsorbed methanol provides hydrophilic surface sites and results in the formation of smooth crystalline ice; an effect that is pronounced also for sub-monolayer methanol coverages. The alcohols primarily reside at the ice surface and at the ice-graphite interface with a minor fraction being incorporated into the growing ice structures. Methanol has no observable effect on gas/solid water vapor exchange whereas butanol acts as a tr...

  15. Ice Formation via Deposition Mode Nucleation Onto Dust Particulates: The University of Toronto Continuous Flow Diffusion Chamber

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    Kanji, Z. A.; Abbatt, J. P.; Cotton, R.; Demott, P.; Jones, H.; Möhler, O.; Stetzer, O.

    2008-12-01

    Laboratory studies are described whereby the heterogeneous ice nucleating ability of various dust samples were studied, for particles suspended in a newly built thermal gradient continuous flow diffusion chamber (TG-CFDC). Ice formation is observed using an optical particle counter (OPC) and the relative humidity (RH) and temperature conditions of the flow system are validated by observing homogenous freezing of H2SO4 aerosols. At the Fourth International Ice Nucleation Workshop (ICIS 07) in Karslruhe, Germany this system was used to investigate ice nucleation primarily in the vapor deposition mode, for Arizona Test Dust (ATD), Israeli Desert Dust (ID), Canary Island Dust (CID), Saharan Dust (SD), Graphite Spark Soot, Snomax® (dead bacteria) and live bacteria. The aerosol size was in the submicron range with an approximate cut off of 700 nm and a mode of 350 nm. Temperatures for nucleation were varied from 265 - 230 K. The dust aerosols were generally found to be more efficient than soot. At warmer temperatures (263 K) the bacteria were found to be active in the deposition mode which was not the case for dusts. Among the various dust types at 248 K, the CID was more efficient than ATD at nucleating ice when efficiency is based on lowest onset RH conditions for ice formation in our chamber. We also present preliminary results for the effect of total surface area versus size of aerosols on ice nucleation using ATD as a surrogate for naturally occurring mineral dust.

  16. Ice nucleation properties of agricultural soil dusts

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    Steinke, Isabelle; Funk, Roger; Busse, Jacqueline; Iturri, Antonela; Kirchen, Silke; Leue, Martin; Möhler, Ottmar; Schwartz, Thomas; Sierau, Berko; Toprak, Emre; Ulrich, Andreas; Hoose, Corinna; Leisner, Thomas

    2015-04-01

    Soil dust particles emitted from agricultural areas contain large amounts of organic material such as fungi, bacteria and plant debris. Being carrier for potentially highly ice-active biological particles, agricultural soil dusts are candidates for being very ice-active as well. In this work, we present ice nucleation experiments conducted in the AIDA cloud chamber. We investigated the ice nucleation efficiency of four types of soil dust from different regions of the world. Results are presented for the immersion freezing and the deposition nucleation mode: all soil dusts show higher ice nucleation efficiencies than desert dusts, especially at temperatures above 254 K. For one soil dust sample, the effect of heat treatments was investigated. Heat treatments did not affect the ice nucleation efficiency which presumably excludes primary biological particles as the only source of the increased ice nucleation efficiency. Therefore, organo-mineral complexes or organic compounds may contribute substantially to the high ice nucleation activity of agricultural soil dusts.

  17. Ice nucleation terminology

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    G. Vali

    2014-08-01

    Full Text Available Progress in the understanding of ice nucleation is being hampered by the lack of uniformity in how some terms are used in the literature. This even extends to some ambiguity of meanings attached to some terms. Suggestions are put forward here for common use of terms. Some are already well established and clear of ambiguities. Others are less engrained and will need a conscious effort in adoption. Evolution in the range of systems where ice nucleation is being studied enhances the need for a clear nomenclature. The ultimate limit in the clarity of definitions is, of course, the limited degree to which ice nucleation processes are understood.

  18. Nucleation of Ice

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    Molinero, Valeria

    2009-03-01

    The freezing of water into ice is a ubiquitous transformation in nature, yet the microscopic mechanism of homogeneous nucleation of ice has not yet been elucidated. One of the reasons is that nucleation happens in time scales that are too fast for an experimental characterization and two slow for a systematic study with atomistic simulations. In this work we use coarse-grained molecular dynamics simulations with the monatomic model of water mW[1] to shed light into the mechanism of homogeneous nucleation of ice and its relationship to the thermodynamics of supercooled water. Cooling of bulk water produces either crystalline ice or low- density amorphous ice (LDA) depending on the quenching rate. We find that ice crystallization occurs faster at temperatures close to the liquid-liquid transition, defined as the point of maximum inflection of the density with respect to the temperature. At the liquid-liquid transition, the time scale of nucleation becomes comparable to the time scale of relaxation within the liquid phase, determining --effectively- the end of the metastable liquid state. Our results imply that no ultraviscous liquid water can exist at temperatures just above the much disputed glass transition of water. We discuss how the scenario is changed when water is in confinement, and the relationship of the mechanism of ice nucleation to that of other liquids that present the same phase behavior, silicon [2] and germanium [3]. [4pt] [1] Molinero, V. & Moore, E. B. Water modeled as an intermediate element between carbon and silicon. Journal of Physical Chemistry B (2008). Online at http://pubs.acs.org/cgi- bin/abstract.cgi/jpcbfk/asap/abs/jp805227c.html [0pt] [2] Molinero, V., Sastry, S. & Angell, C. A. Tuning of tetrahedrality in a silicon potential yields a series of monatomic (metal-like) glass formers of very high fragility. Physical Review Letters 97, 075701 (2006).

  19. Addressing the ice nucleating abilities of marine aerosol: A combination of deposition mode laboratory and field measurements

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    Ladino, L. A.; Yakobi-Hancock, J. D.; Kilthau, W. P.; Mason, R. H.; Si, M.; Li, J.; Miller, L. A.; Schiller, C. L.; Huffman, J. A.; Aller, J. Y.; Knopf, D. A.; Bertram, A. K.; Abbatt, J. P. D.

    2016-05-01

    This study addresses, through two types of experiments, the potential for the oceans to act as a source of atmospheric ice-nucleating particles (INPs). The INP concentration via deposition mode nucleation was measured in situ at a coastal site in British Columbia in August 2013. The INP concentration at conditions relevant to cirrus clouds (i.e., -40 °C and relative humidity with respect to ice, RHice = 139%) ranged from 0.2 L-1 to 3.3 L-1. Correlations of the INP concentrations with levels of anthropogenic tracers (i.e., CO, SO2, NOx, and black carbon) and numbers of fluorescent particles do not indicate a significant influence from anthropogenic sources or submicron bioaerosols, respectively. Additionally, the INPs measured in the deposition mode showed a poor correlation with the concentration of particles with sizes larger than 500 nm, which is in contrast with observations made in the immersion freezing mode. To investigate the nature of particles that could have acted as deposition INP, laboratory experiments with potential marine aerosol particles were conducted under the ice-nucleating conditions used in the field. At -40 °C, no deposition activity was observed with salt aerosol particles (sodium chloride and two forms of commercial sea salt: Sigma-Aldrich and Instant Ocean), particles composed of a commercial source of natural organic matter (Suwannee River humic material), or particle mixtures of sea salt and humic material. In contrast, exudates from three phytoplankton (Thalassiosira pseudonana, Nanochloris atomus, and Emiliania huxleyi) and one marine bacterium (Vibrio harveyi) exhibited INP activity at low RHice values, down to below 110%. This suggests that the INPs measured at the field site were of marine biological origins, although we cannot rule out other sources, including mineral dust.

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

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    Peckhaus, Andreas; Bachmann, Felix; Hoffmann, Nadine; Koch, Michael; Kiselev, Alexei; Leisner, Thomas

    2015-04-01

    Recently K-feldspar was identified as one of the most active atmospheric ice nucleating particles (INP) of mineral origin [1]. Seeking the explanation to this phenomena we have conducted extensive experimental investigation of the ice nucleating efficiency of K-feldspar in three heterogeneous freezing modes. The immersion freezing of K-feldspar was investigated with the cold stage using arrays of nanoliter-size droplets containing aqueous suspension of polydisperse feldspar particles. For contact freezing, the charged droplets of supercooled water were suspended in the laminar flow of the DMA-selected feldspar-containing particles, allowing for determination of freezing probability on a single particle-droplet contact [2]. The nucleation and growth of ice via vapor deposition on the crystalline surfaces of macroscopic feldspar particles have been investigated in the Environmental Scanning Electron Microscope (ESEM) under humidified nitrogen atmosphere. The ice nucleation experiments were supplemented with measurements of effective surface area of feldspar particles and ion chromatography (IC) analysis of the leached framework cations (K+, Na+, Ca2+, Mg2+). In this contribution we focus on the role of surface chemistry influencing the IN efficiency of K-feldspar, in particular the connection between the degree of surface hydroxylation and its ability to induce local structural ordering in the interfacial layer in water molecules (as suggested by recent modeling efforts). We mimic the natural process of feldspar ageing by suspending it in water or weak aqueous solution of carbonic acid for different time periods, from minutes to months, and present its freezing efficiency as a function of time. Our immersion freezing experiments show that ageing have a nonlinear effect on the freezing behavior of feldspar within the investigated temperature range (-40°C to -10°C). On the other hand, deposition nucleation of ice observed in the ESEM reveals clear different pattern

  1. Climate Impacts of Ice Nucleation

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    Gettelman, Andrew; Liu, Xiaohong; Barahona, Donifan; Lohmann, Ulrike; Chen, Celia

    2012-01-01

    Several different ice nucleation parameterizations in two different General Circulation Models (GCMs) are used to understand the effects of ice nucleation on the mean climate state, and the Aerosol Indirect Effects (AIE) of cirrus clouds on climate. Simulations have a range of ice microphysical states that are consistent with the spread of observations, but many simulations have higher present-day ice crystal number concentrations than in-situ observations. These different states result from different parameterizations of ice cloud nucleation processes, and feature different balances of homogeneous and heterogeneous nucleation. Black carbon aerosols have a small (0.06 Wm(exp-2) and not statistically significant AIE when included as ice nuclei, for nucleation efficiencies within the range of laboratory measurements. Indirect effects of anthropogenic aerosols on cirrus clouds occur as a consequence of increasing anthropogenic sulfur emissions with different mechanisms important in different models. In one model this is due to increases in homogeneous nucleation fraction, and in the other due to increases in heterogeneous nucleation with coated dust. The magnitude of the effect is the same however. The resulting ice AIE does not seem strongly dependent on the balance between homogeneous and heterogeneous ice nucleation. Regional effects can reach several Wm2. Indirect effects are slightly larger for those states with less homogeneous nucleation and lower ice number concentration in the base state. The total ice AIE is estimated at 0.27 +/- 0.10 Wm(exp-2) (1 sigma uncertainty). This represents a 20% offset of the simulated total shortwave AIE for ice and liquid clouds of 1.6 Wm(sup-2).

  2. Ice Nucleation in Deep Convection

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    Jensen, Eric; Ackerman, Andrew; Stevens, David; Gore, Warren J. (Technical Monitor)

    2001-01-01

    The processes controlling production of ice crystals in deep, rapidly ascending convective columns are poorly understood due to the difficulties involved with either modeling or in situ sampling of these violent clouds. A large number of ice crystals are no doubt generated when droplets freeze at about -40 C. However, at higher levels, these crystals are likely depleted due to precipitation and detrainment. As the ice surface area decreases, the relative humidity can increase well above ice saturation, resulting in bursts of ice nucleation. We will present simulations of these processes using a large-eddy simulation model with detailed microphysics. Size bins are included for aerosols, liquid droplets, ice crystals, and mixed-phase (ice/liquid) hydrometers. Microphysical processes simulated include droplet activation, freezing, melting, homogeneous freezing of sulfate aerosols, and heterogeneous ice nucleation. We are focusing on the importance of ice nucleation events in the upper part of the cloud at temperatures below -40 C. We will show that the ultimate evolution of the cloud in this region (and the anvil produced by the convection) is sensitive to these ice nucleation events, and hence to the composition of upper tropospheric aerosols that get entrained into the convective column.

  3. 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

  4. Partitioning of ice nucleating particles: Which modes matter?

    Science.gov (United States)

    Hande, Luke; Hoose, Corinna

    2017-04-01

    Ice particles in clouds have a large impact on cloud lifetime, precipitation amount, and cloud radiative properties through the indirect aerosol effect. Thus, correctly modelling ice formation processes is important for simulations preformed on all spatial and temporal scales. Ice forms on aerosol particles through several different mechanisms, namely deposition nucleation, immersion freezing, and contact freezing. However there is conflicting evidence as to which mode dominates, and the relative importance of the three heterogeneous ice nucleation mechanisms, as well as homogeneous nucleation, remains an open question. The environmental conditions, and hence the cloud type, have a large impact on determining which nucleation mode dominates. In order to understand this, simulations were performed with the COSMO-LES model, utilising state of the art parameterisations to describe the different nucleation mechanisms for several semi-idealised cloud types commonly occurring over central Europe. The cloud types investigated include a semi-idealised, and an idealised convective cloud, an orographic cloud, and a stratiform cloud. Results show that immersion and contact freezing dominate at warmer temperatures, and under most conditions, deposition nucleation plays only a minor role. In clouds where sufficiently high levels of water vapour are present at colder temperatures, deposition nucleation can play a role, however in general homogeneous nucleation dominates at colder temperatures. Since contact nucleation depends on the environmental relative humidity, enhancements in this nucleation mode can be seen in areas of dry air entrainment. The results indicate that ice microphysical processes are somewhat sensitve to the environmental conditions and therefore the cloud type.

  5. Laboratory Studies of Ice Nucleation on Volcanic Ash

    Science.gov (United States)

    Tolbert, M. A.; Schill, G. P.; Genareau, K. D.

    2014-12-01

    Ice nucleation on volcanic ash controls both ash aggregation and cloud glaciation, which affect human respiratory health, atmospheric transport, and global climate. We have performed laboratory studies of the depositional and immersion freezing efficiency of three distinct samples of volcanic ash using Raman Microscopy coupled to an environmental cell. Ash from the Fuego (Basaltic Ash, Guatemala), Soufriere Hills (Andesetic Ash, Montserrat), and Taupo (Rhyolitic Ash, New Zealand) volcanoes were chosen to represent different geographical locations and silica content. All ash samples were quantitatively analyzed for both percent crystallinity and mineralogy using X-ray diffraction. We find that all three samples of volcanic ash are excellent depositional ice nuclei, nucleating ice at ice saturation ratios of 1.05 ± 0.1. For immersion freezing, however, only the Taupo ash exhibited efficient heterogeneous ice nucleation activity. Similar to recent studies on mineral dust, we suggest that the mineralogy of volcanic ash may dictate its ice nucleation activity in the immersion mode.

  6. Some ice nucleation characteristics of Asian and Saharan desert dust

    Directory of Open Access Journals (Sweden)

    P. R. Field

    2006-01-01

    Full Text Available The large (7 m×4 m cylinder, 84 m3 AIDA (Aerosol Interactions and Dynamics in the Atmosphere cloud chamber facility at Forschungszentrum, Karlsruhe, Germany was used to test the ice nucleating ability of two desert dust samples from the Sahara and Asia. Aerosol samples were lognormally distributed with a mode diameter of 0.4(±0.1 μm and geometric standard deviation of ~1.7(±0.2. At temperatures warmer than −40°C droplets were formed before ice crystals formed and there was generally no deposition nucleation observed. At temperatures colder than −40°C both dust samples exhibited dual nucleation events that were observed during the same expansion experiment. The primary nucleation event occurred at ice saturation ratios of 1.1 to 1.3 and is likely to be a deposition nucleation mode. The secondary nucleation event occurred at ice saturation ratios between 1.35 and 1.5. We cannot categorically determine whether this ice nucleation event is via a further deposition mode or a condensation mode, but the presence of some soluble material in the dust samples leads us to favour the latter process. The activated fractions of desert dust ranged from ~5–10% at −20°C to 20–40% at temperatures colder than −40°C. There was no obvious difference between the nucleation behaviour of the two dust samples.

  7. 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 S

  8. Molecular Ice Nucleation Activity of Birch Pollen

    Science.gov (United States)

    Felgitsch, Laura; Bichler, Magdalena; Häusler, Thomas; Weiss, Victor U.; Marchetti-Deschmann, Martina; Allmaier, Günter; Grothe, Hinrich

    2015-04-01

    Heterogeneous ice nucleation plays a major part in ecosystem and climate. Due to the triggering of ice cloud formation it influences the radiation balance of the earth, but also on the ground it can be found to be important in many processes of nature. So far the process of heterogeneous ice nucleation is not fully understood and many questions remain to be answered. Biological ice nucleation is hereby from great interest, because it shows the highest freezing temperatures. Several bacteria and fungi act as ice nuclei. A famous example is Pseudomonas syringae, a bacterium in commercial use (Snomax®), which increases the freezing from homogeneous freezing temperatures of approx. -40° C (for small volumes as in cloud droplets) to temperatures up to -2° C. In 2001 it was found that birch pollen can trigger ice nucleation (Diehl et al. 2001; Diehl et al. 2002). For a long time it was believed that this is due to macroscopic features of the pollen surface. Recent findings of Bernhard Pummer (2012) show a different picture. The ice nuclei are not attached on the pollen surface directly, but on surface material which can be easily washed off. This shows that not only the surface morphology, but also specific molecules or molecular structures are responsible for the ice nucleation activity of birch pollen. With various analytic methods we work on elucidating the structure of these molecules as well as the mechanism with which they trigger ice nucleation. To solve this we use various instrumental analytic techniques like Nuclear Magnetic Resonance spectroscopy (NMR), Matrix-Assisted Laser Desorption/Ionization Mass Spectrometry (MALDI-MS), and Gas-phase Electrophoretic Mobility Molecular Analysis (GEMMA). Also standard techniques like various chromatographic separation techniques and solvent extraction are in use. We state here that this feature might be due to the aggregation of small molecules, with agglomerates showing a specific surface structure. Our results

  9. The Leipzig Ice Nucleation chamber Comparison (LINC): An overview of ice nucleation measurements observed with four on-line ice nucleation devices

    Science.gov (United States)

    Kohn, Monika; Wex, Heike; Grawe, Sarah; Hartmann, Susan; Hellner, Lisa; Herenz, Paul; Welti, André; Stratmann, Frank; Lohmann, Ulrike; Kanji, Zamin A.

    2016-04-01

    Mixed-phase clouds (MPCs) are found to be the most relevant cloud type leading to precipitation in mid-latitudes. The formation of ice crystals in MPCs is not completely understood. To estimate the effect of aerosol particles on the radiative properties of clouds and to describe ice nucleation in models, the specific properties of aerosol particles acting as ice nucleating particles (INPs) still need to be identified. A number of devices are able to measure INPs in the lab and in the field. However, methods can be very different and need to be tested under controlled conditions with respect to aerosol generation and properties in order to standardize measurement and data analysis approaches for subsequent ambient measurements. Here, we present an overview of the LINC campaign hosted at TROPOS in September 2015. We compare four ice nucleation devices: PINC (Portable Ice Nucleation Chamber, Chou et al., 2011) and SPIN (SPectrometer for Ice Nuclei) are operated in deposition nucleation and condensation freezing mode. LACIS (Leipzig Aerosol Cloud Interaction Simulator, Hartmann et al., 2011) and PIMCA (Portable Immersion Mode Cooling chamber) measure in the immersion freezing mode. PIMCA is used as a vertical extension to PINC and allows activation and droplet growth prior to exposure to the investigated ice nucleation temperature. Size-resolved measurements of multiple aerosol types were performed including pure mineral dust (K-feldspar, kaolinite) and biological particles (Birch pollen washing waters) as well as some of them after treatment with sulfuric or nitric acid prior to experiments. LACIS and PIMCA-PINC operated in the immersion freezing mode showed very good agreement in the measured frozen fraction (FF). For the comparison between PINC and SPIN, which were scanning relative humidity from below to above water vapor saturation, an agreement was found for the obtained INP concentration. However, some differences were observed, which may result from ice

  10. Thermodynamics of ice nucleation in liquid water.

    Science.gov (United States)

    Wang, Xin; Wang, Shui; Xu, Qinzhi; Mi, Jianguo

    2015-01-29

    We present a density functional theory approach to investigate the thermodynamics of ice nucleation in supercooled water. Within the theoretical framework, the free-energy functional is constructed by the direct correlation function of oxygen-oxygen of the equilibrium water, and the function is derived from the reference interaction site model in consideration of the interactions of hydrogen-hydrogen, hydrogen-oxygen, and oxygen-oxygen. The equilibrium properties, including vapor-liquid and liquid-solid phase equilibria, local structure of hexagonal ice crystal, and interfacial structure and tension of water-ice are calculated in advance to examine the basis for the theory. The predicted phase equilibria and the water-ice surface tension are in good agreement with the experimental data. In particular, the critical nucleus radius and free-energy barrier during ice nucleation are predicted. The critical radius is similar to the simulation value, suggesting that the current theoretical approach is suitable in describing the thermodynamic properties of ice crystallization.

  11. Soot Aerosol Particles as Cloud Condensation Nuclei: from Ice Nucleation Activity to Ice Crystal Morphology

    Science.gov (United States)

    Pirim, Claire; Ikhenazene, Raouf; Ortega, Isamel Kenneth; Carpentier, Yvain; Focsa, Cristian; Chazallon, Bertrand; Ouf, François-Xavier

    2016-04-01

    Emissions of solid-state particles (soot) from engine exhausts due to incomplete fuel combustion is considered to influence ice and liquid water cloud droplet activation [1]. The activity of these aerosols would originate from their ability to be important centers of ice-particle nucleation, as they would promote ice formation above water homogeneous freezing point. Soot particles are reported to be generally worse ice nuclei than mineral dust because they activate nucleation at higher ice-supersaturations for deposition nucleation and at lower temperatures for immersion freezing than ratios usually expected for homogeneous nucleation [2]. In fact, there are still numerous opened questions as to whether and how soot's physico-chemical properties (structure, morphology and chemical composition) can influence their nucleation ability. Therefore, systematic investigations of soot aerosol nucleation activity via one specific nucleation mode, here deposition nucleation, combined with thorough structural and compositional analyzes are needed in order to establish any association between the particles' activity and their physico-chemical properties. In addition, since the morphology of the ice crystals can influence their radiative properties [3], we investigated their morphology as they grow over both soot and pristine substrates at different temperatures and humidity ratios. In the present work, Combustion Aerosol STandart soot samples were produced from propane using various experimental conditions. Their nucleation activity was studied in deposition mode (from water vapor), and monitored using a temperature-controlled reactor in which the sample's relative humidity is precisely measured with a cryo-hygrometer. Formation of water/ice onto the particles is followed both optically and spectroscopically, using a microscope coupled to a Raman spectrometer. Vibrational signatures of hydroxyls (O-H) emerge when the particle becomes hydrated and are used to characterize ice

  12. The ice nucleation activity of biological aerosols

    Science.gov (United States)

    Grothe, H.; Pummer, B.; Bauer, H.; Bernardi, J.

    2012-04-01

    Primary Biological Aerosol Particles (PBAPs), including bacteria, spores and pollen may be important for several atmospheric processes. Particularly, the ice nucleation caused by PBAPs is a topic of growing interest, since their impact on ice cloud formation and thus on radiative forcing, an important parameter in global climate is not yet fully understood. In laboratory model studies we investigated the ice nucleation activity of selected PBAPs. We studied the immersion mode freezing using water-oil emulsion, which we observed by optical microscopy. We particularly focused on pollen. We show that pollen of different species strongly differ in their ice nucleation behavior. The average freezing temperatures in laboratory experiments range from 240 K to 255 K. As the most efficient nuclei (silver birch, Scots pine and common juniper pollen) have a distribution area up to the Northern timberline, their ice nucleation activity might be a cryoprotective mechanism. For comparison the ice nucleation activity of Snomax, fungal spores, and mushrooms will be discussed as well. In the past, pollen have been rejected as important atmospheric IN, as they are not as abundant in the atmosphere as bacteria or mineral dust and are too heavy to reach higher altitudes. However, in our experiments (Pummer et al. 2011) it turned out that water, which had been in contact with pollen and then been separated from the bodies, nucleates as good as the pollen grains themselves. So the ice nuclei have to be easily-suspendable macromolecules (100-300 kDa) located on the pollen. Once extracted, they can be distributed further through the atmosphere than the heavy pollen grains and so augment the impact of pollen on ice cloud formation even in the upper troposphere. It is widely known, that material from the pollen, like allergens and sugars, can indeed leave the pollen body and be distributed independently. The most probable mechanism is the pollen grain bursting by rain, which releases

  13. Heterogeneous ice nucleation and water uptake by field-collected atmospheric particles below 273 K

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Bingbing; Laskin, Alexander; Roedel, Tobias R.; Gilles, Marry K.; Moffet, Ryan C.; Tivanski, Alexei V.; Knopf, Daniel A.

    2012-09-25

    Atmospheric ice formation induced by particles with complex chemical and physical properties through heterogeneous nucleation is not well understood. Heterogeneous ice nucleation and water uptake by ambient particles collected from urban environments in Los Angeles and Mexico City are presented. Using a vapour controlled cooling system equipped with an optical microscopy, the range of onset conditions for ice nucleation and water uptake by the collected particles was determined as a function of temperature (200{273 K) and relative humidity with respect to ice (RHice) up to water saturation. Three distinctly different types of authentic atmospheric particles were investigated including soot particles associated with organics/inorganics, inorganic particles of marine origin coated with organic material, and Pb/Zn containing inorganic particles apportioned to anthropogenic emissions relevant to waste incineration. Single particle characterization was provided by micro-spectroscopic analyses using 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 ne structure spectroscopy (STXM/NEXAFS). Above 230 K, signicant differences in water uptake and immersion freezing effciencies of the different particle types were observed. Below 230 K, the particles exhibited high deposition ice nucleation effciencies and formed ice at RHice values well below homogeneous ice nucleation limits. The data show that the chemical composition of these eld{collected particles plays an important role in determining water uptake and immersion freezing. Heterogeneous ice nucleation rate coeffcients, cumulative ice nuclei (IN) spectrum, and IN activated fraction for deposition ice nucleation are derived. The presented ice nucleation data demonstrate that anthropogenic and marine particles comprising of various chemical and physical properties exhibit distinctly different ice

  14. Effect of photochemical ageing on the ice nucleation properties of diesel and wood burning particles

    Science.gov (United States)

    Chou, C.; Kanji, Z. A.; Stetzer, O.; Tritscher, T.; Chirico, R.; Heringa, M. F.; Weingartner, E.; Prévôt, A. S. H.; Baltensperger, U.; Lohmann, U.

    2013-01-01

    A measurement campaign (IMBALANCE) conducted in 2009 was aimed at characterizing the physical and chemical properties of freshly emitted and photochemically aged combustion particles emitted from a log wood burner and diesel vehicles: a EURO3 Opel Astra with a diesel oxidation catalyst (DOC) but no particle filter and a EURO2 Volkswagen Transporter TDI Syncro without emission aftertreatment. Ice nucleation experiments in the deposition and condensation freezing modes were conducted with the Portable Ice Nucleation Chamber (PINC) at three nominal temperatures, -30 °C, -35 °C and -40 °C. Freshly emitted diesel particles showed ice formation only at -40 °C in the deposition mode at 137% relative humidity with respect to ice (RHi) and 92% relative humidity with respect to water (RHw), and photochemical ageing did not play a role in modifying their ice nucleation behaviour. Only one diesel experiment where α-pinene was added for the ageing process, showed an ice nucleation enhancement at -35 °C. Wood burning particles also act as ice nuclei (IN) at -40 °C in the deposition mode at the same conditions as for diesel particles and photochemical ageing also did not alter the ice formation properties of the wood burning particles. Unlike diesel particles, wood burning particles form ice via condensation freezing at -35 °C whereas no ice nucleation was observed at -30 °C. Photochemical ageing did not affect the ice nucleation ability of the diesel and wood burning particles at the three different temperatures investigated but a broader range of temperatures below -40 °C need to be investigated in order to draw an overall conclusion on the effect of photochemical ageing on deposition/condensation ice nucleation across the entire temperature range relevant to cold clouds.

  15. Effect of photochemical aging on the ice nucleation properties of diesel and wood burning particles

    Science.gov (United States)

    Chou, C.; Stetzer, O.; Tritscher, T.; Chirico, R.; Heringa, M. F.; Kanji, Z. A.; Weingartner, E.; Prévôt, A. S. H.; Baltensperger, U.; Lohmann, U.

    2012-06-01

    A measurement campaign (IMBALANCE) was conducted in 2009 and aimed at characterizing the physical and chemical properties of freshly emitted and photochemically aged combustion particles emitted from a log wood burner and diesel vehicles: a EURO3 Opel Astra with a diesel oxidation catalyst (DOC) but no particle filter and a EURO2 Volkswagen Transporter TDI Syncro with no emission after-treatment. Ice nucleation experiments in the deposition and condensation freezing modes were conducted with the Portable Ice Nucleation Chamber (PINC) at three nominal temperatures, -30 °C, -35 °C and -40 °C. Freshly emitted diesel particles showed ice formation only at -40 °C in the deposition mode at 137% relative humidity with respect to ice (RHi) and 92% relative humidity with respect to water (RHw), and photochemical aging did not play a role in modifying their ice nucleation behavior. Only one diesel experiment where α-pinene was added, showed an ice nucleation enhancement after the aging at -35 °C. Wood burning particles also act as ice nuclei (IN) at -40 °C in the deposition mode at the same conditions as for diesel particles and photochemical aging did also not alter the ice formation properties of the wood burning particles. Unlike diesel particles, wood burning particles form ice via condensation freezing at -35 °C with no ice nucleation observed at -30 °C for wood burning particles. Photochemical aging did not affect the ice nucleation ability of the diesel and wood burning particles at the three different temperatures investigated but a broader range of temperatures below -30 °C need to be investigated in order to draw an overall conclusion on the effect of photochemical aging on deposition/condensation ice nucleation across the entire temperature range relevant to cold clouds.

  16. Effect of photochemical aging on the ice nucleation properties of diesel and wood burning particles

    Directory of Open Access Journals (Sweden)

    C. Chou

    2012-06-01

    Full Text Available A measurement campaign (IMBALANCE was conducted in 2009 and aimed at characterizing the physical and chemical properties of freshly emitted and photochemically aged combustion particles emitted from a log wood burner and diesel vehicles: a EURO3 Opel Astra with a diesel oxidation catalyst (DOC but no particle filter and a EURO2 Volkswagen Transporter TDI Syncro with no emission after-treatment. Ice nucleation experiments in the deposition and condensation freezing modes were conducted with the Portable Ice Nucleation Chamber (PINC at three nominal temperatures, −30 °C, −35 °C and −40 °C. Freshly emitted diesel particles showed ice formation only at −40 °C in the deposition mode at 137% relative humidity with respect to ice (RHi and 92% relative humidity with respect to water (RHw, and photochemical aging did not play a role in modifying their ice nucleation behavior. Only one diesel experiment where α-pinene was added, showed an ice nucleation enhancement after the aging at −35 °C. Wood burning particles also act as ice nuclei (IN at −40 °C in the deposition mode at the same conditions as for diesel particles and photochemical aging did also not alter the ice formation properties of the wood burning particles. Unlike diesel particles, wood burning particles form ice via condensation freezing at −35 °C with no ice nucleation observed at −30 °C for wood burning particles. Photochemical aging did not affect the ice nucleation ability of the diesel and wood burning particles at the three different temperatures investigated but a broader range of temperatures below −30 °C need to be investigated in order to draw an overall conclusion on the effect of photochemical aging on deposition/condensation ice nucleation across the entire temperature range relevant to cold clouds.

  17. Effect of photochemical ageing on the ice nucleation properties of diesel and wood burning particles

    Directory of Open Access Journals (Sweden)

    C. Chou

    2013-01-01

    Full Text Available A measurement campaign (IMBALANCE conducted in 2009 was aimed at characterizing the physical and chemical properties of freshly emitted and photochemically aged combustion particles emitted from a log wood burner and diesel vehicles: a EURO3 Opel Astra with a diesel oxidation catalyst (DOC but no particle filter and a EURO2 Volkswagen Transporter TDI Syncro without emission aftertreatment. Ice nucleation experiments in the deposition and condensation freezing modes were conducted with the Portable Ice Nucleation Chamber (PINC at three nominal temperatures, −30 °C, −35 °C and −40 °C. Freshly emitted diesel particles showed ice formation only at −40 °C in the deposition mode at 137% relative humidity with respect to ice (RHi and 92% relative humidity with respect to water (RHw, and photochemical ageing did not play a role in modifying their ice nucleation behaviour. Only one diesel experiment where α-pinene was added for the ageing process, showed an ice nucleation enhancement at −35 °C. Wood burning particles also act as ice nuclei (IN at −40 °C in the deposition mode at the same conditions as for diesel particles and photochemical ageing also did not alter the ice formation properties of the wood burning particles. Unlike diesel particles, wood burning particles form ice via condensation freezing at −35 °C whereas no ice nucleation was observed at −30 °C. Photochemical ageing did not affect the ice nucleation ability of the diesel and wood burning particles at the three different temperatures investigated but a broader range of temperatures below −40 °C need to be investigated in order to draw an overall conclusion on the effect of photochemical ageing on deposition/condensation ice nucleation across the entire temperature range relevant to cold clouds.

  18. Heterogeneous ice nucleation: bridging stochastic and singular freezing behavior

    Directory of Open Access Journals (Sweden)

    D. Niedermeier

    2011-01-01

    Full Text Available Heterogeneous ice nucleation, a primary pathway for ice formation in the atmosphere, has been described alternately as being stochastic, in direct analogy with homogeneous nucleation, or singular, with ice nuclei initiating freezing at deterministic temperatures. We present an idealized model that bridges these stochastic and singular descriptions of heterogeneous ice nucleation. This "soccer ball" model treats statistically similar particles as being covered with surface sites (patches of finite area characterized by different nucleation barriers, but with each surface site following the stochastic nature of ice embryo formation. The model provides a phenomenological explanation for seemingly contradictory experimental results obtained in our research groups. We suggest that ice nucleation is fundamentally a stochastic process but that for realistic atmospheric particle populations this process can be masked by the heterogeneity of surface properties. Full evaluation of the model will require experiments with well characterized ice nucleating particles and the ability to vary both temperature and waiting time for freezing.

  19. 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.

  20. Ice nucleating particles in the Saharan Air Layer

    Science.gov (United States)

    Boose, Yvonne; Sierau, Berko; García, M. Isabel; Rodríguez, Sergio; Alastuey, Andrés; Linke, Claudia; Schnaiter, Martin; Kupiszewski, Piotr; Kanji, Zamin A.; Lohmann, Ulrike

    2016-07-01

    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 in INPs compared to the ambient

  1. Heterogeneous ice nucleation and water uptake by field-collected atmospheric particles below 273 K

    Science.gov (United States)

    Wang, Bingbing; Laskin, Alexander; Roedel, Tobias; Gilles, Mary K.; Moffet, Ryan C.; Tivanski, Alexei V.; Knopf, Daniel A.

    2012-09-01

    Ice formation induced by atmospheric particles through heterogeneous nucleation is not well understood. Onset conditions for heterogeneous ice nucleation and water uptake by particles collected in Los Angeles and Mexico City were determined as a function of temperature (200-273 K) and relative humidity with respect to ice (RHice). Four dominant particle types were identified including soot associated with organics, soot with organic and inorganics, inorganic particles of marine origin coated with organic material, and Pb/Zn-containing particles apportioned to emissions relevant to waste incineration. Single particle characterization was provided by micro-spectroscopic analyses using 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 (STXM/NEXAFS). Above 230 K, significant differences in onsets of water uptake and immersion freezing of different particle types were observed. Below 230 K, particles exhibited high deposition ice nucleation efficiencies and formed ice atRHicewell below homogeneous ice nucleation limits. The data suggest that water uptake and immersion freezing are more sensitive to changes in particle chemical composition compared to deposition ice nucleation. The data demonstrate that anthropogenic and marine influenced particles, exhibiting various chemical and physical properties, possess distinctly different ice nucleation efficiencies and can serve as efficient IN at atmospheric conditions typical for cirrus and mixed-phase clouds.

  2. Boreal pollen contain ice-nucleating as well as ice-binding ‘antifreeze’ polysaccharides

    Science.gov (United States)

    Dreischmeier, Katharina; Budke, Carsten; Wiehemeier, Lars; Kottke, Tilman; Koop, Thomas

    2017-01-01

    Ice nucleation and growth is an important and widespread environmental process. Accordingly, nature has developed means to either promote or inhibit ice crystal formation, for example ice-nucleating proteins in bacteria or ice-binding antifreeze proteins in polar fish. Recently, it was found that birch pollen release ice-nucleating macromolecules when suspended in water. Here we show that birch pollen washing water exhibits also ice-binding properties such as ice shaping and ice recrystallization inhibition, similar to antifreeze proteins. We present spectroscopic evidence that both the ice-nucleating as well as the ice-binding molecules are polysaccharides bearing carboxylate groups. The spectra suggest that both polysaccharides consist of very similar chemical moieties, but centrifugal filtration indicates differences in molecular size: ice nucleation occurs only in the supernatant of a 100 kDa filter, while ice shaping is strongly enhanced in the filtrate. This finding may suggest that the larger ice-nucleating polysaccharides consist of clusters of the smaller ice-binding polysaccharides, or that the latter are fragments of the ice-nucleating polysaccharides. Finally, similar polysaccharides released from pine and alder pollen also display both ice-nucleating as well as ice-binding ability, suggesting a common mechanism of interaction with ice among several boreal pollen with implications for atmospheric processes and antifreeze protection. PMID:28157236

  3. Boreal pollen contain ice-nucleating as well as ice-binding ‘antifreeze’ polysaccharides

    Science.gov (United States)

    Dreischmeier, Katharina; Budke, Carsten; Wiehemeier, Lars; Kottke, Tilman; Koop, Thomas

    2017-02-01

    Ice nucleation and growth is an important and widespread environmental process. Accordingly, nature has developed means to either promote or inhibit ice crystal formation, for example ice-nucleating proteins in bacteria or ice-binding antifreeze proteins in polar fish. Recently, it was found that birch pollen release ice-nucleating macromolecules when suspended in water. Here we show that birch pollen washing water exhibits also ice-binding properties such as ice shaping and ice recrystallization inhibition, similar to antifreeze proteins. We present spectroscopic evidence that both the ice-nucleating as well as the ice-binding molecules are polysaccharides bearing carboxylate groups. The spectra suggest that both polysaccharides consist of very similar chemical moieties, but centrifugal filtration indicates differences in molecular size: ice nucleation occurs only in the supernatant of a 100 kDa filter, while ice shaping is strongly enhanced in the filtrate. This finding may suggest that the larger ice-nucleating polysaccharides consist of clusters of the smaller ice-binding polysaccharides, or that the latter are fragments of the ice-nucleating polysaccharides. Finally, similar polysaccharides released from pine and alder pollen also display both ice-nucleating as well as ice-binding ability, suggesting a common mechanism of interaction with ice among several boreal pollen with implications for atmospheric processes and antifreeze protection.

  4. Probing Individual Ice Nucleation Events with Environmental Scanning Electron Microscopy

    Science.gov (United States)

    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.

  5. Ice Nucleation on Carbon Surface Supports the Classical Theory for Heterogeneous Nucleation

    CERN Document Server

    Cabriolu, Raffaela

    2015-01-01

    The prevalence of heterogeneous nucleation in nature was explained qualitatively by the classical theory for heterogeneous nucleation established over more than 60 years ago, but the quantitative validity and the key conclusions of the theory have remained unconfirmed. Employing the forward flux sampling method and the coarse-grained water model mW, we explicitly computed the heterogeneous ice nucleation rates in the supercooled water on a graphitic surface at various temperatures. The independently calculated ice nucleation rates were found to fit well according to the classical theory for heterogeneous nucleation. The fitting procedure further yields the estimate of the potency factor which measures the ratio of the heterogeneous nucleation barrier to the homogeneous nucleation barrier. Remarkably, the estimated potency factor agrees quantitatively with the volumetric ratio of the critical nuclei between the heterogeneous and homogeneous nucleation. Our numerical study thus provides a strong support to the ...

  6. 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].

  7. Particle Characterization and Ice Nucleation Efficiency of Field-Collected Aerosol Particles

    Science.gov (United States)

    Wang, B.; Gilles, M. K.; Laskin, A.; Moffet, R.; Nizkorodov, S.; Roedel, T.; Sterckx, L.; Tivanski, A.; Knopf, D. A.

    2011-12-01

    Atmospheric ice formation by heterogeneous nucleation is one of the least understood processes resulting in cirrus and mixed-phase clouds which affect the global radiation budget, the hydrological cycle, and water vapor distribution. In particular, how organic aerosol affect ice nucleation is not well understood. Here we report on heterogeneous ice nucleation from particles collected during the CalNex campaign at the Caltech campus site, Pasadena, on May 19, 2010 at 6am-12pm (A2) and 12pm-6pm (A3) and May 23 at 6am-12pm (B2) and 6pm-12am (B4). The ice nucleation onsets and water uptake were determined as a function of temperature (200-273 K) and relative humidity with respect to ice (RHice). The ice nucleation efficiency was related to the particle chemical composition. Single particle characterization was provided by using 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 (STXM/NEXAFS). The STXM/NEXAFS analysis indicates that the morning sample (A2) constitutes organic particles and organic particles with soot and inorganic inclusions. The afternoon sample (A3) is dominated by organic particles with a potentially higher degree of oxidation associated with soot. The B2 sample shows a higher number fraction of magnesium-containing particle indicative of a marine source and ~93% of the particles contained sulfur besides oxygen and carbon as derived from CCSEM/EDX analysis. The B4 sample lacks the strong marine influence and shows higher organic content. Above 230 K, we observed water uptake followed by condensation freezing at mean RH of 93-100% and 89-95% for A2 and A3, respectively. This indicates that the aged A3 particles are efficient ice nuclei (IN) for condensation freezing. Below 230 K A2 and A3 induced deposition ice nucleation between 125-155% RHice (at mean values of 134-150% RHice). The B2 and B4

  8. Characterization of Ice nucleation Bacteria and their Applications

    OpenAIRE

    ZONOURİ, Sheida Sadat; FATEHİNİA, Milad; NURİTABAR, Safoura; MANUCHEHRİ, Sara

    2015-01-01

    Abstract. Supercooled water can remain in liquid state at the temperatures below zero and needs catalysts for changing from liquid to solid state, and accumulation of water molecules causes nucleation and creates ice embryo. Then, other molecules are attached to this core and will make ice crystals “visible”. These catalysts may be inorganic materials, bacteria and/or fungal spores. In this review article, bacteria such as P. Syringae have been studied in ice nucleation process and their indu...

  9. 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

  10. 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.

  11. Effects of crystallographic properties on the ice nucleation properties of volcanic ash particles

    Science.gov (United States)

    Kulkarni, Gourihar; Nandasiri, Manjula; Zelenyuk, Alla; Beranek, Josef; Madaan, Nitesh; Devaraj, Arun; Shutthanandan, Vaithiyalingam; Thevuthasan, Suntharampillai; Varga, Tamas

    2015-04-01

    Specific chemical and physical properties of volcanic ash particles that could affect their ability to induce ice formation are poorly understood. In this study, the ice nucleating properties of size-selected volcanic ash and mineral dust particles in relation to their surface chemistry and crystalline structure at temperatures ranging from -30 to -38°C were investigated in deposition mode. Ice nucleation efficiency of dust particles was higher compared to ash particles at all temperature and relative humidity conditions. Particle characterization analysis shows that surface elemental composition of ash and dust particles was similar; however, the structural properties of ash samples were different.

  12. Effects Of Crystallographic Properties On The Ice Nucleation Properties Of Volcanic Ash Particles

    Energy Technology Data Exchange (ETDEWEB)

    Kulkarni, Gourihar R.; Nandasiri, Manjula I.; Zelenyuk, Alla; Beranek, Josef; Madaan, Nitesh; Devaraj, Arun; Shutthanandan, V.; Thevuthasan, Suntharampillai; Varga, Tamas

    2015-04-28

    Specific chemical and physical properties of volcanic ash particles that could affect their ability to induce ice formation are poorly understood. In this study, the ice nucleating properties of size-selected volcanic ash and mineral dust particles in relation to their surface chemistry and crystalline structure at temperatures ranging from –30 to –38 °C were investigated in deposition mode. Ice nucleation efficiency of dust particles was higher compared to ash particles at all temperature and relative humidity conditions. Particle characterization analysis shows that surface elemental composition of ash and dust particles was similar; however, the structural properties of ash samples were different.

  13. Immersion freezing of ice nucleation active protein complexes

    Directory of Open Access Journals (Sweden)

    S. Hartmann

    2013-06-01

    Full Text Available Utilising the Leipzig Aerosol Cloud Interaction Simulator (LACIS, the immersion freezing behaviour of droplet ensembles containing monodisperse particles, generated from a Snomax™ solution/suspension, was investigated. Thereto ice fractions were measured in the temperature range between −5 °C to −38 °C. Snomax™ is an industrial product applied for artificial snow production and contains Pseudomonas syringae} bacteria which have long been used as model organism for atmospheric relevant ice nucleation active (INA bacteria. The ice nucleation activity of such bacteria is controlled by INA protein complexes in their outer membrane. In our experiments, ice fractions increased steeply in the temperature range from about −6 °C to about −10 °C and then levelled off at ice fractions smaller than one. The plateau implies that not all examined droplets contained an INA protein complex. Assuming the INA protein complexes to be Poisson distributed over the investigated droplet populations, we developed the CHESS model (stoCHastic modEl of similar and poiSSon distributed ice nuclei which allows for the calculation of ice fractions as function of temperature and time for a given nucleation rate. Matching calculated and measured ice fractions, we determined and parameterised the nucleation rate of INA protein complexes exhibiting class III ice nucleation behaviour. Utilising the CHESS model, together with the determined nucleation rate, we compared predictions from the model to experimental data from the literature and found good agreement. We found that (a the heterogeneous ice nucleation rate expression quantifying the ice nucleation behaviour of the INA protein complex is capable of describing the ice nucleation behaviour observed in various experiments for both, Snomax™ and P. syringae bacteria, (b the ice nucleation rate, and its temperature dependence, seem to be very similar regardless of whether the INA protein complexes inducing ice

  14. Ultrasonic emissions during ice nucleation and propagation in plant xylem.

    Science.gov (United States)

    Charrier, Guillaume; Pramsohler, Manuel; Charra-Vaskou, Katline; Saudreau, Marc; Améglio, Thierry; Neuner, Gilbert; Mayr, Stefan

    2015-08-01

    Ultrasonic acoustic emission analysis enables nondestructive monitoring of damage in dehydrating or freezing plant xylem. We studied acoustic emissions (AE) in freezing stems during ice nucleation and propagation, by combining acoustic and infrared thermography techniques and controlling the ice nucleation point. Ultrasonic activity in freezing samples of Picea abies showed two distinct phases: the first on ice nucleation and propagation (up to 50 AE s(-1) ; reversely proportional to the distance to ice nucleation point), and the second (up to 2.5 AE s(-1) ) after dissipation of the exothermal heat. Identical patterns were observed in other conifer and angiosperm species. The complex AE patterns are explained by the low water potential of ice at the ice-liquid interface, which induced numerous and strong signals. Ice propagation velocities were estimated via AE (during the first phase) and infrared thermography. Acoustic activity ceased before the second phase probably because the exothermal heating and the volume expansion of ice caused decreasing tensions. Results indicate cavitation events at the ice front leading to AE. Ultrasonic emission analysis enabled new insights into the complex process of xylem freezing and might be used to monitor ice propagation in natura.

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

    Energy Technology Data Exchange (ETDEWEB)

    Kulkarni, Gourihar R.; China, Swarup; Liu, Shang; Nandasiri, Manjula I.; Sharma, Noopur; Wilson, Jacqueline M.; Aiken, A. C.; Chand, Duli; Laskin, Alexander; Mazzoleni, Claudio; Pekour, Mikhail S.; Shilling, John E.; Shutthanandan, V.; Zelenyuk, Alla; Zaveri, Rahul A.

    2016-04-16

    The role of atmospheric relevant soot particles that are processed in the atmosphere toward ice nucleation at cirrus cloud condition is poorly understood. In this study, the ice nucleating properties of diesel soot particles subjected to various physical and chemical aging treatments were investigated at temperatures ranging from -40 to -50 °C. We show that bare soot particles nucleate ice in deposition mode, but coating with secondary organics suppresses the heterogeneous ice nucleation potential of soot particles requiring homogeneous freezing threshold conditions. However, the ice nucleation efficiency of soot particles coated with an aqueous organic layer was similar to bare soot particles. Hydration of bare soot particles slightly enhanced the ice nucleation efficiency, and the IN abilities of compact soot particles (roundness = ~ 0.6) were similar to bare lacey soot particles (roundness = ~ 0.4). These results indicate that ice nucleation properties are sensitive to the various aging treatments.

  16. Parameterization of homogeneous ice nucleation for cloud and climate models based on classical nucleation theory

    Directory of Open Access Journals (Sweden)

    V. I. Khvorostyanov

    2012-03-01

    Full Text Available A new analytical parameterization of homogeneous ice nucleation is developed based on extended classical nucleation theory including new equations for the critical radii of the ice germs, free energies and nucleation rates as the functions of the temperature and water saturation ratio simultaneously. By representing these quantities as separable products of the analytical functions of the temperature and supersaturation, analytical solutions are found for the integral-differential supersaturation equation and concentration of nucleated crystals. Parcel model simulations are used to illustrate the general behavior of various nucleation properties under various conditions, for justifications of the further key analytical simplifications, and for verification of the resulting parameterization.

    The final parameterization is based upon the values of the supersaturation that determines the current or maximum concentrations of the nucleated ice crystals. The crystal concentration is analytically expressed as a function of time and can be used for parameterization of homogeneous ice nucleation both in the models with small time steps and for substep parameterization in the models with large time steps. The crystal concentration is expressed analytically via the error functions or elementary functions and depends only on the fundamental atmospheric parameters and parameters of classical nucleation theory. The diffusion and kinetic limits of the new parameterization agree with previous semi-empirical parameterizations.

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

    Directory of Open Access Journals (Sweden)

    T. W. Wilson

    2012-09-01

    Full Text Available Atmospheric secondary organic aerosol (SOA is likely to exist in a semi-solid or glassy state, particularly at low temperatures and humidities. Previously, it has been shown that glassy aqueous citric acid aerosol is able to nucleate ice heterogeneously under conditions relevant to cirrus in the tropical tropopause layer (TTL. In this study we test if glassy aerosol distributions with a range of chemical compositions heterogeneously nucleate ice under cirrus conditions. Three single component aqueous solution aerosols (raffinose, 4-hydroxy-3-methoxy-DL-mandelic acid (HMMA and levoglucosan and one multi component aqueous solution aerosol (raffinose mixed with five dicarboxylic acids and ammonium sulphate were studied in both the liquid and glassy states at a large cloud simulation chamber. The investigated organic compounds have similar functionality to oxidised organic material found in atmospheric aerosol and have estimated temperature/humidity induced glass transition thresholds that fall within the range predicted for atmospheric SOA. A small fraction of aerosol particles of all compositions were found to nucleate ice heterogeneously in the deposition mode at temperatures relevant to the TTL (<200 K. Raffinose and HMMA, which form glasses at higher temperatures, nucleated ice heterogeneously at temperatures as high as 214.6 and 218.5 K respectively. We present the calculated ice active surface site density, ns, of the aerosols tested here and also of glassy citric acid aerosol as a function of relative humidity with respect to ice (RHi. We also propose a parameterisation which can be used to estimate heterogeneous ice nucleation by glassy aerosol for use in cirrus cloud models up to ~220 K. Finally, we show that heterogeneous nucleation by glassy aerosol may compete with ice nucleation on mineral dust particles in mid-latitudes cirrus.

  18. Heterogeneous nucleation of ice on model carbon surfaces

    Science.gov (United States)

    Molinero, V.; Lupi, L.; Hudait, A.

    2014-12-01

    Carbonaceous particles account for 10% of the particulate matter in the atmosphere. The experimental investigation of heterogeneous freezing of water droplets by carbonaceous particles reveals widespread ice freezing temperatures. The origin of the soot and its oxidation and aging modulate its ice nucleation ability, however, it is not known which structural and chemical characteristics of soot account for the variability in ice nucleation efficiency. We find that atomically flat carbon surfaces promote heterogeneous nucleation of ice, while molecularly rough surfaces with the same hydrophobicity do not. We investigate a large set of graphitic surfaces of various dimensions and radii of curvature consistent with those of soot in experiments, and find that variations in nanostructures alone could account for the spread in the freezing temperatures of ice on soot in experiments. A characterization of the nanostructure of soot is needed to predict its ice nucleation efficiency. Atmospheric oxidation and aging of soot modulates its ice nucleation ability. It has been suggested that an increase in the ice nucleation ability of aged soot results from an increase in the hydrophilicity of the surfaces upon oxidation. Oxidation, however, also impacts the nanostructure of soot, making it difficult to assess the separate effects of soot nanostructure and hydrophilicity in experiments. We investigate the effect of changes in hydrophilicity of model graphitic surfaces on the freezing temperature of ice. Our results indicate that the hydrophilicity of the surface is not in general a good predictor of ice nucleation ability. We find a correlation between the ability of a surface to promote nucleation of ice and the layering of liquid water at the surface. The results of this work suggest that ordering of liquid water in contact with the surface plays an important role in the heterogeneous ice nucleation mechanism. References: L. Lupi, A. Hudait and V. Molinero, J. Am. Chem. Soc

  19. Thermodynamic Derivation of the Activation Energy for Ice Nucleation

    Science.gov (United States)

    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

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

    Directory of Open Access Journals (Sweden)

    R. Wagner

    2010-08-01

    Full Text Available The heterogeneous ice nucleation potential of airborne oxalic acid dihydrate and sodium oxalate particles in the deposition and condensation mode has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 244 and 228 K. Previous laboratory studies have highlighted the particular role of oxalic acid dihydrate as the only species amongst a variety of other investigated dicarboxylic acids to be capable of acting as a heterogeneous ice nucleus in both the deposition and immersion mode. We could confirm a high deposition mode ice activity for 0.03 to 0.8 μm sized oxalic acid dihydrate particles that were either formed by nucleation from a gaseous oxalic acid/air mixture or by rapid crystallisation of highly supersaturated aqueous oxalic acid solution droplets. The critical saturation ratio with respect to ice required for deposition nucleation was found to be less than 1.1 and the size-dependent ice-active fraction of the aerosol population was in the range from 0.1 to 22%. In contrast, oxalic acid dihydrate particles that had crystallised from less supersaturated solution droplets and had been allowed to slowly grow in a supersaturated environment from still unfrozen oxalic acid solution droplets over a time period of several hours were found to be much poorer heterogeneous ice nuclei. We speculate that under these conditions a crystal surface structure with less-active sites for the initiation of ice nucleation was generated. Such particles partially proved to be almost ice-inactive in both the deposition and condensation mode. At times, the heterogeneous ice nucleation ability of oxalic acid dihydrate significantly changed when the particles had been processed in preceding cloud droplet activation steps. Such behaviour was also observed for the second investigated species, namely sodium oxalate. Our experiments address the atmospheric scenario

  1. The adsorption of fungal ice-nucleating proteins on mineral dusts: a terrestrial reservoir of atmospheric ice-nucleating particles

    Science.gov (United States)

    O'Sullivan, Daniel; Murray, Benjamin J.; Ross, James F.; Webb, Michael E.

    2016-06-01

    The occurrence of ice-nucleating particles (INPs) in our atmosphere has a profound impact on the properties and lifetime of supercooled clouds. To date, the identities, sources and abundances of particles capable of nucleating ice at relatively low supercoolings (T > -15 °C) remain enigmatic. While biomolecules such as proteins and carbohydrates have been implicated as important high-temperature INPs, the lack of knowledge on the environmental fates of these species makes it difficult to assess their potential atmospheric impacts. Here we show that such nanoscale ice-nucleating proteins from a common soil-borne fungus (Fusarium avenaceum) preferentially bind to and confer their ice-nucleating properties to kaolinite. The ice-nucleating activity of the proteinaceous INPs is unaffected by adsorption to the clay, and once bound the proteins do not readily desorb, retaining much of the activity even after multiple washings with pure water. The atmospheric implications of the finding that biological residues can confer their ice-nucleating ability to dust particles are discussed.

  2. Ice nucleation properties of fine ash particles from the Eyjafjallajökull eruption in April 2010

    Directory of Open Access Journals (Sweden)

    I. Steinke

    2011-12-01

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

  3. Observations on the nucleation of ice VII in compressed water

    Science.gov (United States)

    Stafford, Samuel J. P.; Chapman, David J.; Bland, Simon N.; Eakins, Daniel E.

    2017-01-01

    Water can freeze upon multiple shock compression, but the window material determines the pressure of the phase transition. Several plate impact experiments were conducted with liquid targets on a single-stage gas gun, diagnosed simultaneously using photonic doppler velocimetry (PDV) and high speed imaging through the water. The experiments investigated why silica windows instigate freezing above 2.5 GPa whilst sapphire windows do not until 7 GPa. We find that the nucleation of ice occurs on the surfaces of windows and can be affected by the surface coating suggesting the surface energy of fused silica, likely due to hydroxyl groups, encourages nucleation of ice VII crystallites. Aluminium coatings prevent nucleation and sapphire surfaces do not nucleate until approximately 6.5 GPa. This is believed to be the threshold pressure for the homogeneous nucleation of water.

  4. Feldspar minerals as efficient deposition ice nuclei

    Directory of Open Access Journals (Sweden)

    J. D. Yakobi-Hancock

    2013-06-01

    Full Text Available Mineral dusts are well known to be efficient ice nuclei, where the source of this efficiency has typically been attributed to the presence of clay minerals such as illite and kaolinite. However, the ice nucleating abilities of the more minor mineralogical components have not been as extensively examined. As a result, the deposition ice nucleation abilities of 24 atmospherically-relevant mineral samples have been studied, using a continuous flow diffusion chamber at −40.0 ± 0.3 °C. The same particle size (200 nm and particle preparation procedure were used throughout. The ice nucleation behaviour of the pure minerals is compared to that of complex mixtures, such as Arizona Test Dust (ATD and Mojave Desert Dust (MDD, and to lead iodide, which has been previously proposed for cloud seeding. Lead iodide was the most efficient ice nucleus (IN, requiring a critical relative humidity with respect to ice (RHi of 122.0 ± 2.0% to activate 0.1% of the particles. MDD (RHi 126.3 ± 3.4% and ATD (RHi 129.5 ± 5.1% have lower but comparable activity. From a set of clay minerals (kaolinite, illite, montmorillonite, non-clay minerals (e.g. hematite, magnetite, calcite, cerussite, quartz, and feldspar minerals (orthoclase, plagioclase present in the atmospheric dusts it was found that the feldspar minerals (particularly orthoclase, and not the clays, were the most efficient ice nuclei. Orthoclase and plagioclase were found to have critical RHi values of 127.1 ± 6.3% and 136.2 ± 1.3%, respectively. The presence of feldspars (specifically orthoclase may play a significant role in the IN behaviour of mineral dusts despite their lower percentage in composition relative to clay minerals.

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

    Directory of Open Access Journals (Sweden)

    A. R. Moukahel

    2012-10-01

    Full Text Available 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

  6. 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

  7. Two-Dimensional Nucleation of Ice from Supercooled Water

    Science.gov (United States)

    Seeley, L. H.; Seidler, G. T.

    2001-03-01

    Heterogeneous nucleation is the initial formation of a stable phase from a metastable phase in the presence of a catalyzing surface. This ubiquitous process has consequences ranging from metallurgy to the formation of kidney stones. Heterogeneous nucleation of ice plays a central role in cloud formation, suggesting one possible connection between anthropogenic pollutants and global climate. A key topic in the theory of nucleation is the geometry of the critical nucleus. Standard nucleation theories generally predict a compact critical nucleus with a surface of roughly constant curvature. We report measurements of the temperature dependent nucleation rate of ice from water samples supporting aliphatic alcohol Langmuir films. We use classical nucleation theory to extract thermodynamic parameters from the measured nucleation rates. From these parameters we conclude that both the effective free energy barrier and the molecular kinetics of nucleation are dominated by the physics at the interface. Our results give self-consistent evidence that the geometry of the critical nucleus in this system is essentially two-dimensional.

  8. Ice Nucleation Near the Surfactant-Water Interface

    Science.gov (United States)

    Carlin, Caleb; Cantrell, Will; Taylor, Caroline

    2008-03-01

    Ice nucleation is a fundamental component of the atmospheric mechanisms driving the formation of clouds. Atmospheric nucleation occurs with a variety of compounds and conditions, but understanding the behavior of water is key in all cases. We have used multiscale molecular simulations to study heterogeneous nucleation in clouds, probing the influence of long-chain alcohols on the freezing of water droplets. Ice nucleation occurs at a finite distance from the heterogeneous surface, due to the disruption of the hydrogen bond network in response to the surfactant-water interface. The penetration depth of the disturbance is found to be dependent upon the chain length and surface organization, as well as the acidity of the terminal alcohol group.

  9. 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

  10. The micro-orifice uniform deposit impactor-droplet freezing technique (MOUDI-DFT for measuring concentrations of ice nucleating particles as a function of size: improvements and initial validation

    Directory of Open Access Journals (Sweden)

    R. H. Mason

    2015-02-01

    Full Text Available The micro-orifice uniform deposit impactor-droplet freezing technique (MOUDI-DFT combines particle collection by inertial impaction (via the MOUDI and a microscope-based immersion freezing apparatus (the DFT to measure atmospheric concentrations of ice nucleating particles (INPs as a function of size and temperature. In the first part of this study we improved upon this recently introduced technique. Using optical microscopy, we investigated the non-uniformity of MOUDI aerosol deposits at spatial resolutions of 1, 0.25 mm, and for some stages when necessary 0.10 mm. The results from these measurements show that at a spatial resolution of 1 mm and less, the concentration of particles along the MOUDI aerosol deposit can vary by an order of magnitude or more. Since the total area of a MOUDI aerosol deposit ranges from 425 to 605 mm2 and the area analyzed by the DFT is approximately 1.2 mm2, this non-uniformity needs to be taken into account when using the MOUDI-DFT to determine atmospheric concentrations of INPs. Measurements of the non-uniformity of the MOUDI aerosol deposits were used to select positions on the deposits that had relatively small variations in particle concentration and to build substrate holders for the different MOUDI stages. These substrate holders improve reproducibility by holding the substrate in the same location for each measurement and ensure that DFT analysis is only performed on substrate regions with relatively small variations in particle concentration. In addition, the deposit non-uniformity was used to determine correction factors that take the non-uniformity into account when determining atmospheric concentrations of INPs. In the second part of this study, the MOUDI-DFT utilizing the new substrate holders was compared to the continuous flow diffusion chamber (CFDC technique of Colorado State University. The intercomparison was done using INP concentrations found by the two instruments during ambient measurements of

  11. The micro-orifice uniform deposit impactor-droplet freezing technique (MOUDI-DFT) for measuring concentrations of ice nucleating particles as a function of size: improvements and initial validation

    Science.gov (United States)

    Mason, R. H.; Chou, C.; McCluskey, C. S.; Levin, E. J. T.; Schiller, C. L.; Hill, T. C. J.; Huffman, J. A.; DeMott, P. J.; Bertram, A. K.

    2015-06-01

    The micro-orifice uniform deposit impactor-droplet freezing technique (MOUDI-DFT) combines particle collection by inertial impaction (via the MOUDI) and a microscope-based immersion freezing apparatus (the DFT) to measure atmospheric concentrations of ice nucleating particles (INPs) as a function of size and temperature. In the first part of this study we improved upon this recently introduced technique. Using optical microscopy, we investigated the non-uniformity of MOUDI aerosol deposits at spatial resolutions of 1, 0.25 mm, and for some stages when necessary 0.10 mm. The results from these measurements show that at a spatial resolution of 1 mm and less, the concentration of particles along the MOUDI aerosol deposits can vary by an order of magnitude or more. Since the total area of a MOUDI aerosol deposit ranges from 425 to 605 mm2 and the area analyzed by the DFT is approximately 1.2 mm2, this non-uniformity needs to be taken into account when using the MOUDI-DFT to determine atmospheric concentrations of INPs. Measurements of the non-uniformity of the MOUDI aerosol deposits were used to select positions on the deposits that had relatively small variations in particle concentration and to build substrate holders for the different MOUDI stages. These substrate holders improve reproducibility by holding the substrate in the same location for each measurement and ensure that DFT analysis is only performed on substrate regions with relatively small variations in particle concentration. In addition, the deposit non-uniformity was used to determine correction factors that take the non-uniformity into account when determining atmospheric concentrations of INPs. In the second part of this study, the MOUDI-DFT utilizing the new substrate holders was compared to the continuous flow diffusion chamber (CFDC) technique of Colorado State University. The intercomparison was done using INP concentrations found by the two instruments during ambient measurements of continental

  12. Deposition nucleation viewed as homogeneous or immersion freezing in pores and cavities

    Directory of Open Access Journals (Sweden)

    C. Marcolli

    2013-06-01

    Full Text Available Heterogeneous ice nucleation is an important mechanism for the glaciation of mixed phase clouds and may also be relevant for cloud formation and dehydration at the cirrus cloud level. It is thought to proceed through different mechanisms, namely contact, condensation, immersion and deposition nucleation. Supposedly, deposition nucleation is the only pathway which does not involve liquid water but occurs by direct water vapor deposition on a surface. This study challenges this classical view by putting forward the hypothesis that what is called deposition nucleation is in fact homogeneous or immersion nucleation occurring in pores and cavities that may form between aggregated primary particles and fill with water at relative humidity RHw T=230–235 K in pores with diameters (D of 3.5–4 nm or larger but only gradually at T=210–230 K in pores with D=2.5–3.5 nm. Melting temperatures in pores are depressed by an amount that can be described by the Gibbs–Thomson equation. Water adsorption isotherms of MCM-41 show that pores with D=3.5–4 nm fill with water at RHw = 56–60% in accordance with an inverse Kelvin effect. Water in such pores should freeze homogeneously for T i reaches ice saturation. Ice crystal growth by water vapor deposition from the gas phase is therefore expected to set in as soon as RHw > 100%. Pores with D > 7.5 nm fill with water at RHi > 100% for T T > 235 K if the pore walls contain an active site. Pore analysis of clay minerals shows that kaolinites exhibit pore structures with pore diameters of 20–50 nm. The mesoporosity of illites and montmorillonites is characterized by pores with T = 2–5 nm. The number and size of pores is distinctly increased in acid treated montmorillonites like K10. Many clay minerals and mineral dusts show a strong increase in ice nucleation efficiency when temperature is decreased below 235 K. Such an increase is difficult to explain when ice nucleation is supposed to occur by a

  13. Constraining Climate Forcing of Ice Nucleation with SPartICus/MACPEX Observations

    Science.gov (United States)

    Liu, X.; Zhang, K.; Wang, M.; Comstock, J. M.; Mitchell, D. L.; Mace, G. G.; Jensen, E. J.

    2012-12-01

    Cirrus clouds composed of ice crystals play an important role in modifying the global radiative balance through scattering shortwave (SW) radiation and absorbing and emitting longwave (LW) terrestrial radiation. Cirrus clouds also modulate water vapor in the upper troposphere and lower stratosphere, which is an important greenhouse gas. Although cirrus clouds are an important player in the global climate system, there are still large uncertainties in the understanding of cirrus cloud properties and processes and their treatments in global climate models, due to the scarcity of cirrus measurements and instrument artifacts of in situ ice crystal number measurements. The DOE Atmospheric Radiation Measurement (ARM)'s Small Particles in Cirrus (SPartICus) campaign (http://campaign.arm.gov/sparticus/) and the NASA's Mid-latitude Airborne Cirrus Properties Experiment (MACPEX, http://www.espo.nasa.gov/macpex/) conducted airborne measurements over central North America with special emphasis in the vicinity of the DOE ARM's Southern Great Plains (SGP) site to investigate the properties of mid-latitude cirrus clouds, the processes affecting these properties and their impact on radiation. With a new generation of probes designed to minimize artifacts due to ice shattering, SPartICus and MACPEX provide unprecedented datasets characterizing cirrus microphysical properties and dynamics. In this study we use the SPartICus/MACPEX observations to constrain the parameterizations of formation and growth of ice crystals in the Community Atmospheric Model version 5 (CAM5). This is achieved by comparing modeled ice crystal number concentration, ice water content, updraft velocity and relative humidity in- and outside cirrus, and their covariance with temperature with the statistics from SPartICus/MACPEX observations. Model sensitivity tests are performed with different ice nucleation mechanisms (homogeneous versus heterogeneous nucleation) and different vapor deposition coefficients to

  14. 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

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

    Directory of Open Access Journals (Sweden)

    C. E. Morris

    2013-04-01

    Full Text Available 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

  16. 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

  17. Ice nucleation properties of volcanic ash from Eyjafjallajökull

    Directory of Open Access Journals (Sweden)

    C. R. Hoyle

    2011-09-01

    Full Text Available The ice nucleation ability of volcanic ash particles collected close to the Icelandic volcano Eyjafjallajökull during its eruptions in April and May 2010 is investigated experimentally, in the immersion and deposition modes, and applied to atmospheric conditions by comparison with airborne measurements and microphysical model calculations. The number of ash particles which are active as ice nuclei (IN is strongly temperature dependent, with a very small minority being active in the immersion mode at temperatures of 250–263 K. Average ash particles show only a moderate effect on ice nucleation, by inducing freezing at temperatures between 236 K and 240 K (i.e. approximately 3–4 K higher than temperatures required for homogeneous ice nucleation, measured with the same instrument. By scaling the results to aircraft and lidar measurements of the conditions in the ash plume days down wind of the eruption, and by applying a simple microphysical model, it was found that the IN active in the immersion mode in the range 250–263 K generally occurred in atmospheric number densities at the lower end of those required to have an impact on ice cloud formation. However, 3–4 K above the homogeneous freezing point, immersion mode IN number densities a few days down wind of the eruption were sufficiently high to have a moderate influence on ice cloud formation. The efficiency of IN in the deposition mode was found to be poor except at very cold conditions (<238 K, when they reach an efficiency similar to that of mineral dust with the onset of freezing at 10 % supersaturation with respect to ice, and with the frozen fraction nearing its maximum value at a supersaturation 20 %. In summary, these investigations suggest volcanic ash particles to have only moderate effects on atmospheric ice formation.

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

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    J. M. C. Plane

    2009-11-01

    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 [ns (190 K = 10(3.33×sice+8.16] for the variation in ice-active surface site density (ns: m−2 with ice saturation (sice for Fe2O3 nanoparticles. This was implemented in an aerosol-cloud model to determine a predicted deposition (mass accommodation coefficient for water vapour on ice of 0.1 at temperatures appropriate for the upper atmosphere. Classical nucleation theory was used to determine representative contact angles (θ for the different particle compositions. For the in situ generated Fe2O3 particles, a slight inverse temperature dependence was observed with θ = 10.5° at 182 K, decreasing to 9.0° at 200 K (compared with 10.2° and 11.4°, respectively for the SiO2 and MgO particle samples at the higher temperature.

    These observations indicate that such refractory nanoparticles are relatively efficient materials for the nucleation of ice under the conditions studied in the chamber which correspond to cirrus cloud formation in the upper troposphere. The results also show that Fe2O3 particles do not act as ice nuclei

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

    Directory of Open Access Journals (Sweden)

    R. W. Saunders

    2010-02-01

    Full Text Available Nanoparticles of iron oxide (crystalline and amorphous, silicon oxide and magnesium oxide were investigated for their propensity to nucleate ice over the temperature range 180–250 K, using the AIDA chamber in Karlsruhe, Germany.

    All samples were observed to initiate ice formation via the deposition mode at threshold ice super-saturations (RHithresh ranging from 105% to 140% for temperatures below 220 K. Approximately 10% of amorphous Fe2O3 particles (modal diameter = 30 nm generated in situ from a photochemical aerosol reactor, led to ice nucleation at RHithresh = 140% at an initial chamber temperature of 182 K. Quantitative analysis using a singular hypothesis treatment provided a fitted function [ns(190 K=10(3.33×sice+8.16] for the variation in ice-active surface site density (ns:m−2 with ice saturation (sice for Fe2O3 nanoparticles. This was implemented in an aerosol-cloud model to determine a predicted deposition (mass accommodation coefficient for water vapour on ice of 0.1 at temperatures appropriate for the upper atmosphere. Classical nucleation theory was used to determine representative contact angles (θ for the different particle compositions. For the in situ generated Fe2O3 particles, a slight inverse temperature dependence was observed with θ = 10.5° at 182 K, decreasing to 9.0° at 200 K (compared with 10.2° and 11.4° respectively for the SiO2 and MgO particle samples at the higher temperature.

    These observations indicate that such refractory nanoparticles are relatively efficient materials for the nucleation of ice under the conditions studied in the chamber which correspond to cirrus cloud formation in the upper troposphere. The results also show that Fe2O3 particles do not act as ice

  20. Ice nucleation of ammonia gas exposed montmorillonite mineral dust particles

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    A. Salam

    2007-01-01

    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 within our experimental conditions. The percentages of active ice nuclei were 2 to 9 times higher at 90% RHw and 2 to 13 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 12°C higher than for unexposed montmorillonite particles at 90% RHw and 10°C higher at 100% RHw. In the 25 ppm ammonia exposed montmorillonite experiments, the activation temperature was 7°C warmer than unexposed montmorillonite at 100% RHw. Degassing does not reverse the ice nucleating ability of ammonia exposed montmorillonite mineral dust particles. 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.

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

    Science.gov (United States)

    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

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

    Science.gov (United States)

    Wagner, R.; Möhler, O.; Saathoff, H.; Schnaiter, M.; Skrotzki, J.; Leisner, T.; Wilson, T. W.; Malkin, T. L.; Murray, B. J.

    2012-09-01

    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-vitrified in contact

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

    Directory of Open Access Journals (Sweden)

    B. J. Murray

    2012-04-01

    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 aerosols that have re-vitrified in

  4. 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

  5. State transformations and ice nucleation in glassy or (semi-solid amorphous organic aerosol

    Directory of Open Access Journals (Sweden)

    K. J. Baustian

    2012-10-01

    Full Text Available Glassy or amorphous (semi-solid organic aerosol particles have the potential to serve as surfaces for heterogeneous ice nucleation in cirrus clouds. Raman spectroscopy and optical microscopy have been used in conjunction with a cold stage to examine water uptake and ice nucleation on individual aqueous organic glass particles at atmospherically relevant temperatures (200–273 K. Three organic compounds considered proxies for atmospheric secondary organic aerosol (SOA were used in this investigation: sucrose, citric acid and glucose. Internally mixed particles consisting of each organic species and ammonium sulfate were also investigated.

    Results from water uptake experiments were used to construct glass transition curves and state diagrams for each organic and corresponding mixture. A unique glass transition point on each state diagram, Tg', was used to quantify and compare results from this study to previous works. Values of Tg' determined for aqueous sucrose, glucose and citric acid glasses were 236 K, 230 K and 220 K, respectively. Values of Tg' for internally mixed organic/sulfate particles were always significantly lower; 210 K, 207 K and 215 K for sucrose/sulfate, glucose/sulfate and citric acid/sulfate, respectively.

    All investigated organic species were observed to serve as heterogeneous ice nuclei at tropospheric temperatures. Heterogeneous ice nucleation on pure organic particles occurred at Sice=1.1–1.4 for temperatures between 235 K and 200 K. Particles consisting of 1:1 organic-sulfate mixtures remained liquid over a greater range of conditions but were in some cases also observed to depositionally nucleate ice at temperatures below 202 K (Sice=1.25–1.38.

    Glass transition curves constructed from experimental data were incorporated into the Community Aerosol Radiation Model for Atmospheres (CARMA along with the

  6. Ice nucleating properties of volcanic ash particles from the Eyjafjallajökull volcanic eruption

    Science.gov (United States)

    Kulkarni, G.; Zelenyuk, A.; Beranek, J.

    2011-12-01

    The volcanic ash from the volcanic emissions can significantly contribute to the natural source of aerosols in the atmosphere. In the vicinity and downwind of eruption site, the transported ash might have a stronger impact on the aviation industry, regional air quality, and climate. Despite the environmental significance of ash, our understanding of ash particles reacting with other volcanic plume constituents is rudimentary. In particular, the complex interactions between the water vapor and ash particles under different meteorological conditions that lead to cloud hydrometeors are poorly understood. To improve our understanding, we focus on investigating the ice formation properties of ash particles collected from the recent volcanic eruption. It was observed that the ash particles are less efficient ice nuclei compared to the natural dust particles in the deposition nucleation regime, but have similar efficiencies in the condensation freezing mode. The ice nucleated ash particles are separated from the interstitial particles, and further evaporated to understand the elemental composition, size, shape and morphology of the ice residue using the single particle mass spectrometer. The elemental composition reveals that majority of the elements are also present in the natural dust particles, but subtle differences are observed. This suggests that particle properties play an important role in the ice nucleation process.

  7. Biological residues define the ice nucleation properties of soil dust

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    F. Conen

    2011-06-01

    Full Text Available Soil dust is a major driver of ice nucleation in clouds leading to precipitation. It consists largely of mineral particles with a small fraction of organic matter constituted mainly of remains of micro-organisms that participated in degrading plant debris before their own decay. Some micro-organisms have been shown to be much better ice nuclei than the most efficient soil mineral. Yet, current aerosol schemes in global climate models do not consider a difference between soil dust and mineral dust in terms of ice nucleation activity. Here, we show that particles from the clay and silt size fraction of four different soils naturally associated with 0.7 to 11.8 % organic carbon (w/w can have up to four orders of magnitude more ice nuclei per unit mass active in the immersion freezing mode at −12 °C than montmorillonite, the most efficient pure clay mineral. Most of this activity was lost after heat treatment. Removal of biological residues reduced ice nucleation activity to, or below that of montmorillonite. Desert soils, inherently low in organic content, are a large natural source of dust in the atmosphere. In contrast, agricultural land use is concentrated on fertile soils with much larger organic matter contents than found in deserts. It is currently estimated that the contribution of agricultural soils to the global dust burden is less than 20 %. Yet, these disturbed soils can contribute ice nuclei to the atmosphere of a very different and much more potent kind than mineral dusts.

  8. The measurement and parameterization of ice nucleating particles in different backgrounds of China

    Science.gov (United States)

    Jiang, Hui; Yin, Yan; Wang, Xu; Gao, Renjie; Yuan, Liang; Chen, Kui; Shan, Yunpeng

    2016-11-01

    Investigation of the number concentration of ice nucleating particles (INP) in the deposition nucleation mode during a dust event is reported. The results discussed in this paper are the first continuous INP measurements in Xinjiang, northwest of China, over a period with a strong dust event. The average INP concentration at - 20 °C and 22% of supersaturation with respect to ice during non-dust days is found around 11 particles per liter, but it reached several hundred per liter in a dust event. A close correlation is also found between the INP number concentration with the number concentration of aerosol particles larger than 0.5 μm in diameter measured during a dust event, which means that a higher concentration of larger particles induced higher INP number concentration. Parameterizations were developed based on measurements to represent the variations of INP concentration with temperature, supersaturation, and the number concentration of aerosol particles with size larger than 0.5 μm. It should be the first ever, as we have known so far, to measure ice nuclei and aerosol properties simultaneously in a desert area and to contrast INP concentrations in dust and dust-free days, and could advancing our understanding of the effects of dust particles on ice nucleation.

  9. Ice nucleation of bare and sulfuric acid-coated mineral dust particles and implication for cloud properties

    Science.gov (United States)

    Kulkarni, Gourihar; Sanders, Cassandra; Zhang, Kai; Liu, Xiaohong; Zhao, Chun

    2014-08-01

    Ice nucleation properties of atmospherically relevant dust minerals coated with soluble materials are not yet well understood. We determined ice nucleation ability of bare and sulfuric acid-coated mineral dust particles as a function of temperature (-25 to -35°C) and relative humidity with respect to water (RHw; 75 to 110%) for five different mineral dust types: (1) Arizona test dust, (2) illite, (3) montmorillonite, (4) K-feldspar, and (5) quartz. The particles were dry dispersed and size selected at 200 nm, and we determined the fraction of dust particles nucleating ice at various temperatures and RHw. Under water-subsaturated conditions, compared to bare dust particles, we found that coated particles showed a reduction in their ice nucleation ability. Under water-supersaturated conditions, however, we did not observe a significant coating effect (i.e., the bare and coated dust particles had nearly similar nucleating properties). X-ray diffraction patterns of the coated particles indicated that acid treatment altered the crystalline nature of the surface and caused structural disorder; thus, we concluded that the lack of such structured order reduced the ice nucleation efficiency of the coated particles in deposition ice nucleation mode. In addition, our single column model results show that coated particles significantly modify cloud properties such as ice crystal number concentration and ice water content compared to bare particles in water-subsaturated conditions. However, in water-supersaturated conditions, cloud properties differ only at warmer temperatures. These modeling results imply that future aged dust particle simulations should implement coating parameterizations to accurately predict cloud properties.

  10. Heterogeneous ice nucleation: exploring the transition from stochastic to singular freezing behavior

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    D. Niedermeier

    2011-08-01

    Full Text Available Heterogeneous ice nucleation, a primary pathway for ice formation in the atmosphere, has been described alternately as being stochastic, in direct analogy with homogeneous nucleation, or singular, with ice nuclei initiating freezing at deterministic temperatures. We present an idealized, conceptual model to explore the transition between stochastic and singular ice nucleation. This "soccer ball" model treats particles as being covered with surface sites (patches of finite area characterized by different nucleation barriers, but with each surface site following the stochastic nature of ice embryo formation. The model provides a phenomenological explanation for seemingly contradictory experimental results obtained in our research groups. Even with ice nucleation treated fundamentally as a stochastic process this process can be masked by the heterogeneity of surface properties, as might be typical for realistic atmospheric particle populations. Full evaluation of the model findings will require experiments with well characterized ice nucleating particles and the ability to vary both temperature and waiting time for freezing.

  11. 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

  12. Ice nucleation activity in the widespread soil fungus Mortierella alpina

    Science.gov (United States)

    Fröhlich-Nowoisky, Janine; Hill, Thomas C. J.; Pummer, Bernhard G.; Yordanova, Petya; Franc, Gary D.; Pöschl, Ulrich

    2015-04-01

    Biological residues in soil dust are a potentially strong source of atmospheric ice nucleators (IN). However, the sources and characteristics of biological - in particular, fungal - IN in soil dust have not been characterized. By analysis of the culturable fungi in topsoils, from a range of different land use and ecosystem types in south-east Wyoming, we found ice nucleation active (INA, i.e., inducing ice formation in the probed range of temperature and concentration) fungi to be both widespread and abundant, particularly in soils with recent inputs of decomposable organic matter. For example, in harvested and ploughed sugar beet and potato fields, and in the organic horizon beneath Lodgepole pine forest, their relative abundances and concentrations among the cultivable fungi were 25% (8 x 103 CFU g-1), 17% (4.8 x 103 CFU g-1) and 17% (4 x 103 CFU g-1), respectively. Across all investigated soils, 8% (2.9 x 103 CFU g-1) of fungal isolates were INA. All INA isolates initiated freezing at -5° C to -6° C and all belonged to a single zygomycotic species, Mortierella alpina (Mortierellales, Mortierellomycotina). By contrast, the handful of fungal species so far reported as INA all belong within the Ascomycota or Basidiomycota phyla. Mortierella alpina is known to be saprobic (utilizing non-living organic matter), widespread in soil and present in air and rain. Sequencing of the ITS region and the gene for γ-linolenic elongase revealed four distinct clades, affiliated to different soil types. The IN produced by M. alpina seem to be extracellular proteins of 100-300 kDa in size which are not anchored in the fungal cell wall. Ice nucleating fungal mycelium will ramify topsoils and probably also release cell-free IN into it. If these IN survive decomposition or are adsorbed onto mineral surfaces, these small cell-free IN might contribute to the as yet uncharacterized pool of atmospheric IN released by soils as dusts.

  13. Heterogeneous ice nucleation controlled by the coupling of surface crystallinity and surface hydrophilicity

    CERN Document Server

    Bi, Yuanfei; Li, Tianshu

    2015-01-01

    The microscopic mechanisms controlling heterogeneous ice nucleation are complex and remain poorly understood. Although good ice nucleators are generally believed to match ice lattice and to bind water, counter examples are often identified. Here we show, by advanced molecular simulations, that the heterogeneous nucleation of ice on graphitic surface is controlled by the coupling of surface crystallinity and surface hydrophilicity. Molecular level analysis reveals that the crystalline graphitic lattice with an appropriate hydrophilicity may indeed template ice basal plane by forming a strained ice layer, thus significantly enhancing its ice nucleation efficiency. Remarkably, the templating effect is found to transit from within the first contact layer of water to the second as the hydrophilicity increases, yielding an oscillating distinction between the crystalline and amorphous graphitic surfaces in their ice nucleation efficiencies. Our study sheds new light on the long-standing question of what constitutes ...

  14. Manchester Ice Nucleus Counter (MINC measurements from the 2007 International workshop on Comparing Ice nucleation Measuring Systems (ICIS-2007

    Directory of Open Access Journals (Sweden)

    H. M. Jones

    2010-08-01

    Full Text Available An ice nucleus counter was developed and constructed to enable investigation of potential ice nucleating materials. The Manchester Ice Nucleus Chamber (MINC is a concentric-cylinder continuous flow diffusion chamber (CFDC. A full explanation of the MINC instrument is given here, along with first results and a comparison to an established instrument of similar design (Colorado State University CFDC during sampling of common ice nucleating aerosols at the 2007 International workshop on Comparing Ice nucleation Measuring Systems (ICIS-2007. Both instruments detected the onset of ice nucleation under similar conditions of temperature and supersaturation for several different types of ice nuclei. Comparisons of the ratio of ice nuclei to total aerosol concentrations as a function of relative humidity (RH showed agreement within one order of magnitude. Possible reasons for differences between the two instruments relating to differences in their design are discussed, along with suggestions to future improvements to the current design.

  15. Manchester Ice Nucleus Counter (MINC) measurements from the 2007 International workshop on Comparing Ice nucleation Measuring Systems (ICIS-2007)

    Science.gov (United States)

    Jones, H. M.; Flynn, M. J.; Demott, P. J.; Möhler, O.

    2011-01-01

    An ice nucleus counter was developed and constructed to enable investigation of potential ice nucleating materials. The Manchester Ice Nucleus Chamber (MINC) is a concentric-cylinder continuous flow diffusion chamber (CFDC). A full explanation of the MINC instrument is given here, along with first results and a comparison to an established instrument of similar design (Colorado State University CFDC) during sampling of common ice nucleating aerosols at the 2007 International workshop on Comparing Ice nucleation Measuring Systems (ICIS-2007). MINC and CSU-CFDC detected the onset of ice nucleation under similar conditions of temperature and supersaturation for several different types of ice nuclei. Comparisons of the ratio of ice nuclei to total aerosol concentrations as a function of supersaturation with respect to water (SSw) showed agreement within one order of magnitude. Possible reasons for differences between the two instruments relating to differences in their design are discussed, along with suggestions to future improvements to the current design.

  16. Biological particles capable of triggering ice nucleation in the atmosphere

    Science.gov (United States)

    Felgitsch, Laura; Bichler, Magdalena; Vogel, André; Häusler, Thomas; Grothe, Hinrich

    2016-04-01

    Ice-nucleating particles (INPs) have a huge impact on atmospheric processes, since they can trigger ice cloud formation. In general, ice clouds interfere with the radiation balance of planet Earth effectively at high altitudes. Since ambient matter of biological origin tends to have rather large aerodynamic diameters, it exhibits a fast sinking velocity and can only reach limited altitudes. Therefore, research focused on materials found in higher quantities in the upper atmosphere. However, recent findings indicate that the role of biological INPs has been underestimated in the past. In 2012 Pummer and colleagues found that the INPs from birch pollen can be washed off and constitute of macromolecules in the size-range of a few nanometres. With such a small diameter, they show a much longer life span in the upper atmosphere than expected. Further, Huffman and colleagues showed in 2013 a burst of biological INPs over woodlands triggered by rain events, which matches the finding of Pummer et al. well. Plants originating from the northern timberline experience harsh conditions with night frost even during the warm seasons. To prevent frost damages, those plants developed coping mechanisms. Many plant species, which are domestic in cold weather zones, exhibit ice nucleation activity. Therefore, it is important to examine those plants to understand the scale at which biological INPs can be emitted. For the presented results we focus on two types of samples: Berries and tree pollen. Both belong to plants domestic at the northern timberline. With our results we are able to show that INPs are spread vastly throughout different species. Furthermore, all those INPs show certain similarities to each other, most importantly, all of the found INPs seem to be associated to macromolecules in the nano-particulate size range. We examined the INPs from birch pollen more closely. Results indicate that proteins play a major role. Pummer, B., Bauer, H., Bernardi, J., Bleicher, S

  17. Ice nucleation active particles in continental air samples over Mainz, Germany

    Science.gov (United States)

    Pummer, Bernhard G.; Pöschl, Ulrich; Fröhlich-Nowoisky, Janine

    2016-04-01

    Aerosol particles are of central importance for atmospheric chemistry and physics, climate and public health. Some of these particles possess ice nucleation activity (INA), which is highly relevant for cloud formation and precipitation. In 2010, air filter samples were collected with a high-volume filter sampler separating fine and coarse particles (aerodynamic cut-off diameter 3 μm) in Mainz, Germany. In this study, the INA of the atmospheric particles deposited on these filters was determined. Therefore,they were extracted with ultrapure water, which was then measured in a droplet freezing assay, as described in Fröhlich-Nowoisky et al. (2015). The determined concentration of ice nucleators (INs) was between 0.3 and 2per m³ at 266 K, and between5 and 75 per m³ at 260 K. The INs were further characterized by different treatments, like heating (308 K, 371 K), filtration (0.1 μm, 300 kDa), and digestion with papain (10 mg/ml). We further investigated, which atmospheric conditions (e.g. weather) and distinguished events (e.g. dust storms, volcanic eruptions, and pollen peaks) influenced the number and nature of these INs. Fröhlich-Nowoisky, J., Hill, T. C. J., Pummer, B. G., Yordanova, P., Franc, G. D., and Pöschl, U.: Ice nucleation activity in the widespread soil fungus Mortierella alpina, Biogeosci., 12, 1057-1071, doi:10.5194/bg-12-1057-2015, 2015.

  18. Sources of organic ice nucleating particles in soils

    Science.gov (United States)

    Hill, Tom C. J.; DeMott, Paul J.; Tobo, Yutaka; Fröhlich-Nowoisky, Janine; Moffett, Bruce F.; Franc, Gary D.; Kreidenweis, Sonia M.

    2016-06-01

    Soil organic matter (SOM) may be a significant source of atmospheric ice nucleating particles (INPs), especially of those active > -15 °C. However, due to both a lack of investigations and the complexity of the SOM itself, the identities of these INPs remain unknown. To more comprehensively characterize organic INPs we tested locally representative soils in Wyoming and Colorado for total organic INPs, INPs in the heat-labile fraction, ice nucleating (IN) bacteria, IN fungi, IN fulvic and humic acids, IN plant tissue, and ice nucleation by monolayers of aliphatic alcohols. All soils contained ≈ 106 to ≈ 5 × 107 INPs g-1 dry soil active at -10 °C. Removal of SOM with H2O2 removed ≥ 99 % of INPs active > -18 °C (the limit of testing), while heating of soil suspensions to 105 °C showed that labile INPs increasingly predominated > -12 °C and comprised ≥ 90 % of INPs active > -9 °C. Papain protease, which inactivates IN proteins produced by the fungus Mortierella alpina, common in the region's soils, lowered INPs active at ≥ -11 °C by ≥ 75 % in two arable soils and in sagebrush shrubland soil. By contrast, lysozyme, which digests bacterial cell walls, only reduced INPs active at ≥ -7.5 or ≥ -6 °C, depending on the soil. The known IN bacteria were not detected in any soil, using PCR for the ina gene that codes for the active protein. We directly isolated and photographed two INPs from soil, using repeated cycles of freeze testing and subdivision of droplets of dilute soil suspensions; they were complex and apparently organic entities. Ice nucleation activity was not affected by digestion of Proteinase K-susceptible proteins or the removal of entities composed of fulvic and humic acids, sterols, or aliphatic alcohol monolayers. Organic INPs active colder than -10 to -12 °C were resistant to all investigations other than heat, oxidation with H2O2, and, for some, digestion with papain. They may originate from decomposing plant material, microbial

  19. Ice nucleators, bacterial cells and Pseudomonas syringae in precipitation at Jungfraujoch

    Science.gov (United States)

    Stopelli, Emiliano; Conen, Franz; Guilbaud, Caroline; Zopfi, Jakob; Alewell, Christine; Morris, Cindy E.

    2017-03-01

    Ice nucleation is a means by which the deposition of an airborne microorganism can be accelerated under favourable meteorological conditions. Analysis of 56 snow samples collected at the high-altitude observatory Jungfraujoch (3580 m a.s.l.) revealed an order-of-magnitude-larger dynamic range of ice-nucleating particles active at -8 °C (INPs-8) compared to the total number of bacterial cells (of which on average 60 % was alive). This indicates a shorter atmospheric residence time for INPs-8. Furthermore, concentrations of INPs-8 decreased much faster, with an increasing fraction of water precipitated from the air mass prior to sampling, than the number of total bacterial cells. Nevertheless, at high wind speeds (> 50 km h-1) the ratio of INPs-8 to total bacterial cells largely remained in a range between 10-2 and 10-3, independent of prior precipitation, likely because of recent injections of particles in regions upwind. Based on our field observations, we conclude that ice nucleators travel shorter legs of distance with the atmospheric water cycle than the majority of bacterial cells. A prominent ice-nucleating bacterium, Pseudomonas syringae, has been previously supposed to benefit from this behaviour as a means to spread via the atmosphere and to colonise new host plants. Therefore, we targeted this bacterium with a selective cultivation approach. P. syringae was successfully isolated for the first time at such an altitude in 3 of 13 samples analysed. Colony-forming units of this species constituted a minor fraction (10-4) of the numbers of INPs-8 in these samples. Overall, our findings expand the geographic range of habitats where this bacterium has been found and corroborate theories on its robustness in the atmosphere and its propensity to spread to colonise new habitats.

  20. Potential Sites for Ice Nucleation on Aluminosilicate Clay Minerals and Related Materials.

    Science.gov (United States)

    Freedman, Miriam Arak

    2015-10-01

    Few aerosol particles in clouds nucleate the formation of ice. The surface sites available for nucleus formation, which can include surface defects and functional groups, determine in part the activity of an aerosol particle toward ice formation. Although ice nucleation on particles has been widely studied, exploration of the specific sites at which the initial germ forms has been limited, but is important for predicting the microphysical properties of clouds, which impact climate. This Perspective focuses on what is currently known about surface sites for ice nucleation on aluminosilicate clay minerals, which are commonly found in ice residuals, as well as related materials.

  1. New species of ice nucleating fungi in soil and air

    Science.gov (United States)

    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

  2. Identification and quantification of ice nucleation active microorganisms by digital droplet PCR (ddPCR)

    Science.gov (United States)

    Linden, Martin; Pöschl, Ulrich; Fröhlich-Nowoisky, Janine

    2015-04-01

    Several bioaerosol types, including bacteria, fungi, pollen and lichen, have been identified as sources of biological ice nucleators (IN) which induce ice formation already at temperatures as high as -10 °C or above. Accordingly, they potentially contribute widely to environmental ice nucleation in the atmosphere and are of great interest in the study of natural heterogenous ice nucleation processes. Ice nucleation active microorganisms have been found and studied among bacteria (Proteobacteria) and fungi (phyla Basidiomycota and Ascomycota). The mechanisms enabling the microorganisms to ice nucleation are subject to ongoing research. While it has been demonstrated that whole cells can act as ice nucleators in the case of bacteria due to the presence of specific membrane proteins, cell-free ice nucleation active particles seem to be responsible for this phenomenon in fungi and lichen. The identification and quantification of these ice nucleation active microorganisms and their IN in atmospheric samples is crucial to understand their contribution to the pool of atmospheric IN. This is not a trivial task since the respective microorganisms are often prevalent in lowest concentrations and a variety of states, be it viable cells, spores or cell debris from dead cells. Molecular biology provides tools to identify and quantify ice nucleation active microorganisms independent of their state by detecting genetic markers specific for the organism of interest. Those methods are not without their drawbacks in terms of sample material concentration required or reliable standardization. Digital Droplet Polymerase Chain Reaction (ddPCR) was chosen for our demands as a more elegant, quick and specific method in the investigation of ice nucleation active microorganisms in atmospheric samples. The advantages of ddPCR lie in the simultaneous detection and quantification of genetic markers and their original copy numbers in a sample. This is facilitated by the fractionation of the

  3. Atmospheric aging of dust ice nucleating particles - a combined laboratory and field approach

    Science.gov (United States)

    Boose, Yvonne; Rodríguez, Sergio; García, M. Isabel; Linke, Claudia; Schnaiter, Martin; Zipori, Assaf; Crawford, Ian; Lohmann, Ulrike; Kanji, Zamin A.; Sierau, Berko

    2016-04-01

    We present INP data measured in-situ at two mostly free tropospheric locations: the High Altitude Research Station Jungfraujoch (JFJ) in the Swiss Alps, located at 3580 m above sea level (asl) and the Izaña observatory on Tenerife, off the West African shore (2373 m asl). INP concentrations were measured online with the Portable Ice Nucleation Chamber, PINC, at the Jungfraujoch in the winters of 2012, 2013 and 2014 and at Izaña in the summers of 2013 and 2014. Each measurement period lasted between 2 to 6 weeks. During summer, Izaña is frequently within the Saharan Air Layer and thus often exposed to Saharan dust events. Saharan dust also reaches the Jungfraujoch mainly during spring. For offline ice nucleation analysis in the laboratory under similar thermodynamic conditions, airborne dust was collected a) at Izaña with a cyclone directly from the air and b) collected from the surface of the Aletsch glacier close to the JFJ after deposition. Supporting measurements of aerosol particle size distributions and fluorescence were conducted at both locations, as well as cloud water isotope analysis at the Jungfraujoch and aerosol chemistry at Izaña. For both locations the origin of the INPs was investigated with a focus on dust and biological particles using back trajectories and chemical signature. Results show that dust aerosol is the dominant INP type at both locations at a temperature of 241 K. In addition to Saharan dust, also more local, basaltic dust is found at the Jungfraujoch. Biological particles are not observed to play a role for ice nucleation in clouds during winter at Jungfraujoch but are enriched in INP compared to the total aerosol at Izaña also during dust events. The comparison of the laboratory and the field measurements at Izaña indicates a good reproducibility of the field data by the collected dust samples. Field and laboratory data of the dust samples from both locations show that the dust arriving at JFJ is less ice nucleation active

  4. Ice nucleation from aqueous NaCl droplets with and without marine diatoms

    Directory of Open Access Journals (Sweden)

    P. A. Alpert

    2011-06-01

    Full Text Available Ice formation in the atmosphere by homogeneous and heterogeneous nucleation is one of the least understood processes in cloud microphysics and climate. Here we describe our investigation of the marine environment as a potential source of atmospheric IN by experimentally observing homogeneous ice nucleation from aqueous NaCl droplets and comparing against heterogeneous ice nucleation from aqueous NaCl droplets containing intact and fragmented diatoms. Homogeneous and heterogeneous ice nucleation are studied as a function of temperature and water activity, aw. Additional analyses are presented on the dependence of diatom surface area and aqueous volume on heterogeneous freezing temperatures, ice nucleation rates, ωhet, ice nucleation rate coefficients, Jhet, and differential and cumulative ice nuclei spectra, k(T and K(T, respectively. Homogeneous freezing temperatures and corresponding nucleation rate coefficients are in agreement with the water activity based homogeneous ice nucleation theory within experimental and predictive uncertainties. Our results confirm, as predicted by classical nucleation theory, that a stochastic interpretation can be used to describe the homogeneous ice nucleation process. Heterogeneous ice nucleation initiated by intact and fragmented diatoms can be adequately represented by a modified water activity based ice nucleation theory. A horizontal shift in water activity, Δaw, het = 0.2303, of the ice melting curve can describe median heterogeneous freezing temperatures. Individual freezing temperatures showed no dependence on available diatom surface area and aqueous volume. Determined at median diatom freezing temperatures for aw from 0.8 to 0.99, ωhet~0.11+0.06−0.05 s−1, Jhet~1.0+1.16−0.61×104 cm−2

  5. Ice nucleation of natural desert dust including organics sourced from nine deserts worldwide

    Science.gov (United States)

    Boose, Yvonne; Welti, André; Atkinson, James; Danielczok, Anja; Bingemer, Heinz; Plötze, Michael; Lohmann, Ulrike; Kanji, Zamin A.

    2017-04-01

    The extraordinary high ice nucleation (IN) potential of microcline, a K-feldspar mineral, at temperatures (T) above 248 and up to 271 K has been show recently. However, it is unclear if microcline is also found at the surface of airborne mineral dust particles or if chemical and mechanical aging processes lead to its destruction or shielding and thus reduced IN ability in the atmosphere. It is suggested that instead organic material mixed with inorganic minerals is responsible for cloud glaciation at T ≥ 253 K. We collected airborne Saharan dust at 4 locations at different distances from the desert and 11 samples from the surface of 9 of the major deserts worldwide. We studied immersion IN on these samples between 235 - 263 K using the IMCA-ZINC (immersion mode cooling chamber - Zurich ice nucleation chamber) setup and the FRIDGE (Franfurt Ice Nuclei Deposition Freezing Experiment) instrument run in droplet freezing mode. By correlating the results with the bulk mineralogy of the dust samples, determined by X-ray diffraction analysis, we show that at 253 K, K-feldspar indeed predicts best the IN behavior of the samples. At lower T (238 - 245 K) however, quartz and the total feldspar contents correlate best. Furthermore, microcline is only found in one of the airborne Saharan dust samples (3.9 wt%) while in the others the amount is below the detection limit or completely absent. Relative humidity (RH) scans at constant T = 238, 240 and 242 K were additionally performed with the portable ice nucleation counter, PINC. Above and below water saturation a similar prominent role of quartz is found as in the immersion mode. To investigate the role of organic material on the IN ability, we heated some of the samples at 573 K for 10 h and repeated the RH-scans. Furthermore, we performed thermogravimetric analysis of the dusts. The two tested airborne Saharan samples loose between 2.8 and 7.5 % of their mass at T ≤ 573 K, partly due to water release, partly due to

  6. Impact of controlled ice nucleation on process performance and quality attributes of a lyophilized monoclonal antibody.

    Science.gov (United States)

    Awotwe-Otoo, David; Agarabi, Cyrus; Read, Erik K; Lute, Scott; Brorson, Kurt A; Khan, Mansoor A; Shah, Rakhi B

    2013-06-25

    An efficient and potentially scalable technology was evaluated to control the ice nucleation step of the freezing process for a model monoclonal antibody formulation and the effect on process performance and quality attributes of the final lyophilized product was compared with the conventional shelf ramping method of freezing. Controlled ice nucleation resulted in uniform nucleation at temperatures between -2.3 and -3.2 °C while uncontrolled nucleation resulted in random nucleation at temperatures between -10 and -16.4 °C. The sublimation rate (dm/dt) during primary drying was higher in the controlled nucleation cycle (0.13 g/h/vial) than in the uncontrolled nucleation cycle (0.11 g/h/vial). This was due to the formation of larger ice crystals, leading to lower product resistance (Rp) and 19% reduction in the primary drying for the controlled nucleation cycle. Controlled ice nucleation resulted in lyophilized cakes with more acceptable appearance, no visible collapse or shrinkage and decreased reconstitution times compared with uncontrolled nucleation. There were no observed differences in the particle size, concentration (A280 nm) and presence of aggregates (A410 nm) between the two nucleation cycles when the lyophilized cakes were reconstituted. These were confirmed by SEC and protein A-HPLC analyses which showed similar peak shapes and retention times between the two cycles. However, uncontrolled nucleation resulted in cakes with larger specific surface area (0.90 m(2)/g) than controlled nucleation (0.46 m(2)/g). SEM images of the lyophilized cakes from uncontrolled nucleation revealed a sponge-like morphology with smaller pores while cakes from controlled nucleation cycle revealed plate-like structures with more open and larger pores. While controlled nucleation resulted in a final product with a higher residual moisture content (2.1±0.08%) than uncontrolled nucleation (1.62±0.11%), this was resolved by increasing the secondary drying temperature.

  7. Molecular Simulations of Heterogeneous Ice Nucleation. II. Peeling back the Layers

    Energy Technology Data Exchange (ETDEWEB)

    Cox, Stephen J.; Kathmann, Shawn M.; Slater, B.; Michaelides, Angelos

    2015-05-14

    Coarse grained molecular dynamics simulations are presented in which the sensitivity of the ice nucleation rate to the hydrophilicity of a graphene nanoflake is investigated. We find that an optimal interaction strength for promoting ice nucleation exists, which coincides with that found previously for a face centered cubic (111) surface. We further investigate the role that the layering of interfacial water plays in heterogeneous ice nucleation and demonstrate that the extent of layering is not a good indicator of ice nucleating ability for all surfaces. Our results suggest that to be an efficient ice nucleating agent, a surface should not bind water too strongly if it is able to accommodate high coverages of water.

  8. Interfacial Free Energy as the Key to the Pressure-Induced Deceleration of Ice Nucleation

    Science.gov (United States)

    Espinosa, Jorge R.; Zaragoza, Alberto; Rosales-Pelaez, Pablo; Navarro, Caridad; Valeriani, Chantal; Vega, Carlos; Sanz, Eduardo

    2016-09-01

    The avoidance of water freezing is the holy grail in the cryopreservation of biological samples, food, and organs. Fast cooling rates are used to beat ice nucleation and avoid cell damage. This strategy can be enhanced by applying high pressures to decrease the nucleation rate, but the physics behind this procedure has not been fully understood yet. We perform computer experiments to investigate ice nucleation at high pressures consisting in embedding ice seeds in supercooled water. We find that the slowing down of the nucleation rate is mainly due to an increase of the ice I -water interfacial free energy with pressure. Our work also clarifies the molecular mechanism of ice nucleation for a wide pressure range. This study is not only relevant to cryopreservation, but also to water amorphization and climate change modeling.

  9. Microbial ice nucleators scavenged from the atmosphere during simulated rain events

    Science.gov (United States)

    Hanlon, Regina; Powers, Craig; Failor, Kevin; Monteil, Caroline L.; Vinatzer, Boris A.; Schmale, David G.

    2017-08-01

    Rain and snow collected at ground level have been found to contain biological ice nucleators. These ice nucleators have been proposed to have originated in clouds, where they may have participated in the formation of precipitation via ice phase nucleation. We conducted a series of field experiments to test the hypothesis that at least some of the microbial ice nucleators (prokaryotes and eukaryotes) present in rain may not originate in clouds but instead be scavenged from the lower atmosphere by rainfall. Thirty-three simulated rain events were conducted over four months off the side of the Smart Road Bridge in Blacksburg, VA, USA. In each event, sterile water was dispensed over the side of the bridge and recovered in sterile containers in an open fallow agricultural field below (a distance of ∼55 m). Microbes scavenged from the simulated rain events were cultured and their ice nucleation activity was examined. Putative microbial ice nucleators were cultured from 94% (31/33) of the simulated rain events, and represented 1.5% (121/8331) of the total colonies assayed. Putative ice nucleators were subjected to additional droplet freezing assays, and those confirmed through these repeated assays represented 0.4% (34/8331) of the total. Mean CFUs scavenged by simulated rain ranged from 2 to 267 CFUs/mL. Scavenged ice nucleators belong to a number of taxa including the bacterial genera Pseudomonas, Pantoea, and Xanthomonas, and the fungal genera Fusarium, Humicola, and Mortierella. An ice-nucleating strain of the fungal genus Penicillium was also recovered from a volumetric air sampler at the study site. This work expands our knowledge of the scavenging properties of rainfall, and suggests that at least some ice nucleators in natural precipitation events may have been scrubbed from the atmosphere during rainfall, and thus are not likely to be involved in precipitation.

  10. Nucleation and electrolytic deposition of lead on model carbon electrodes

    Science.gov (United States)

    Cericola, D.; Spahr, M.

    2016-08-01

    There is a general consensus in the lead acid battery industry for the use of carbon additives as a functional component in the negative paste to boost the battery performance with regards to charge acceptance and cycle life especially for upcoming automotive and energy storage applications. Several mechanisms are discussed in the scientific literature and the affinity of the carbon surfaces to lead species seems to play a key role. With a set of experiments on model carbon electrodes we gave evidence to the fact that some carbon materials promote spontaneous nucleation of lead crystals. We propose a mechanism such that the carbon, as soon as in a lead containing environment, immobilizes some lead on its surface. Such immobilized lead acts as nucleation seed for the deposition of lead when a current is passed through the material. It is therefore possible to differentiate and select the carbon materials based on their ability to form nucleation seeds.

  11. High-resolution ice nucleation spectra of sea-ice bacteria: implications for cloud formation and life in frozen environments

    Directory of Open Access Journals (Sweden)

    K. Junge

    2008-05-01

    Full Text Available Even though studies of Arctic ice forming particles suggest that a bacterial or viral source derived from open leads could be important for ice formation in Arctic clouds (Bigg and Leck, 2001, the ice nucleation potential of most polar marine psychrophiles or viruses has not been examined under conditions more closely resembling those in the atmosphere. In this paper, we examined the ice nucleation activity (INA of several representative Arctic and Antarctic sea-ice bacterial isolates and a polar Colwellia phage virus. High-resolution ice nucleation spectra were obtained for droplets containing bacterial cells or virus particles using a free-fall freezing tube technique. The fraction of frozen droplets at a particular droplet temperature was determined by measuring the depolarized light scattering intensity from solution droplets in free-fall. Our experiments revealed that all sea-ice isolates and the virus nucleated ice at temperatures very close to the homogeneous nucleation temperature for the nucleation medium – which for artificial seawater was –42.2±0.3°C. Our results suggest that immersion freezing of these marine psychro-active bacteria and viruses would not be important for heterogeneous ice nucleation processes in polar clouds or to the formation of sea ice. These results also suggested that avoidance of ice formation in close proximity to cell surfaces might be one of the cold-adaptation and survival strategies for sea-ice bacteria. The fact that INA occurs at such low temperature could constitute one factor that explains the persistence of metabolic activities at temperatures far below the freezing point of seawater.

  12. Ice nucleation efficiency of clay minerals in the immersion mode

    Directory of Open Access Journals (Sweden)

    V. Pinti

    2012-07-01

    Full Text Available Emulsion and bulk freezing experiments were performed to investigate immersion ice nucleation on clay minerals in pure water, using various kaolinites, montmorillonites, illites as well as natural dust from the Hoggar Mountains in the Saharan region. Differential scanning calorimeter measurements were performed on three different kaolinites (KGa-1b, KGa-2 and K-SA, two illites (Illite NX and Illite SE and four natural and acid-treated montmorillonites (SWy-2, STx-1b, KSF and K-10. The emulsion experiments provide information on the average freezing behaviour characterized by the average nucleation sites. These experiments revealed one to sometimes two distinct heterogeneous freezing peaks, which suggest the presence of a low number of qualitatively distinct average nucleation site classes. We refer to the peak at the lowest temperature as "standard peak" and to the one occurring in only some clay mineral types at higher temperatures as "special peak". Conversely, freezing in bulk samples is not initiated by the average nucleation sites, but by a very low number of "best sites". The kaolinites and montmorillonites showed quite narrow standard peaks with onset temperatures 238 K<Tonstd<242 K and best sites with averaged median freezing temperature Tmedbest=257 K, but only some featuring a special peak (i.e. KSF, K-10, K-SA and SWy-2 with freezing onsets in the range 240–248 K. The illites showed broad standard peaks with freezing onsets at 244 K Tonstd<246 K and best sites with averaged median freezing temperature Tmedbest=262 K. The large difference between freezing temperatures of standard and best sites shows that characterizing ice nucleation efficiencies of dust particles on the basis of freezing onset temperatures from bulk experiments, as has been done in some atmospheric studies, is not appropriate. Our investigations

  13. Ice nucleation efficiency of AgI: review and new insights

    Science.gov (United States)

    Marcolli, Claudia; Nagare, Baban; Welti, André; Lohmann, Ulrike

    2016-07-01

    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.

  14. High-resolution ice nucleation spectra of sea-ice bacteria: implications for cloud formation and life in frozen environments

    Directory of Open Access Journals (Sweden)

    K. Junge

    2007-11-01

    Full Text Available Even though studies of Arctic ice forming particles suggest that a bacterial or viral source derived from open leads could be important for cloud formation in the Arctic (Bigg and Leck, 2001, the ice nucleation potential of most polar marine psychrophiles or viruses has not been examined under conditions more closely resembling those in the atmosphere. In this paper, we examined the ice nucleation activity (INA of several representative Arctic and Antarctic sea-ice bacterial isolates and a polar Colwellia phage virus. High-resolution ice nucleation spectra were obtained for droplets containing bacterial cells or virus particles using a free-fall freezing tube technique. The fraction of frozen droplets at a particular droplet temperature was determined by measuring the depolarized light scattering intensity from solution droplets in free-fall. Our experiments revealed that all sea-ice isolates and the virus nucleated ice at temperatures very close to the homogeneous nucleation temperature for the nucleation medium – which for artificial seawater was −42.2±0.3°C. Our results indicated that these marine psychro-active bacteria and viruses are not important for heterogeneous ice nucleation processes in sea ice or polar clouds. These results also suggested that avoidance of ice formation in close proximity to cell surfaces might be one of the cold-adaptation and survival strategies for sea-ice bacteria. The fact that INA occurs at such low temperature could constitute one factor that explains the persistence of metabolic activities at temperatures far below the freezing point of seawater.

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

    Directory of Open Access Journals (Sweden)

    C. Budke

    2015-02-01

    Full Text Available A new optical freezing array for the study of heterogeneous ice nucleation in microliter-sized droplets is introduced, tested and applied to the study of immersion freezing in aqueous Snomax® suspensions. In the Bielefeld Ice Nucleation ARraY (BINARY ice nucleation can be studied simultaneously in 36 droplets at temperatures down to −40 °C (233 K and at cooling rates between 0.1 and 10 K min−1. The droplets are separated from each other in individual compartments, thus preventing a Wegener–Bergeron–Findeisen type water vapor transfer between droplets as well as avoiding the seeding of neighboring droplets by formation and surface growth of frost halos. Analysis of freezing and melting occurs via an automated real-time image analysis of the optical brightness of each individual droplet. As an application ice nucleation in water droplets containing Snomax® at concentrations from 1 ng mL−1 to 1 mg mL−1 was investigated. Using different cooling rates, a small time dependence of ice nucleation induced by two different classes of ice nucleators (INs contained in Snomax® was detected and the corresponding heterogeneous ice nucleation rate coefficient was quantified. The observed time dependence is smaller than those of other types of INs reported in the literature, suggesting that the BINARY setup is suitable for quantifying time dependence for most other INs of atmospheric interest, making it a useful tool for future investigations.

  16. 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.

  17. The decisive role of free water in determining homogenous ice nucleation behavior of aqueous solutions.

    Science.gov (United States)

    Wang, Qiang; Zhao, Lishan; Li, Chenxi; Cao, Zexian

    2016-05-26

    It is a challenging issue to quantitatively characterize how the solute and pressure affect the homogeneous ice nucleation in a supercooled solution. By measuring the glass transition behavior of solutions, a universal feature of water-content dependence of glass transition temperature is recognized, which can be used to quantify hydration water in solutions. The amount of free water can then be determined for water-rich solutions, whose mass fraction, Xf, is found to serve as a universal relevant parameter for characterizing the homogeneous ice nucleation temperature, the meting temperature of primary ice, and even the water activity of solutions of electrolytes and smaller organic molecules. Moreover, the effects of hydrated solute and pressure on ice nucleation is comparable, and the pressure, when properly scaled, can be incorporated into the universal parameter Xf. These results help establish the decisive role of free water in determining ice nucleation and other relevant properties of aqueous solutions.

  18. What makes a good descriptor for heterogeneous ice nucleation on OH-patterned surfaces

    Science.gov (United States)

    Pedevilla, Philipp; Fitzner, Martin; Michaelides, Angelos

    2017-09-01

    Freezing of water is arguably one of the most common phase transitions on Earth and almost always happens heterogeneously. Despite its importance, we lack a fundamental understanding of what makes substrates efficient ice nucleators. Here we address this by computing the ice nucleation (IN) ability of numerous model hydroxylated substrates with diverse surface hydroxyl (OH) group arrangements. Overall, for the substrates considered, we find that neither the symmetry of the OH patterns nor the similarity between a substrate and ice correlate well with the IN ability. Instead, we find that the OH density and the substrate-water interaction strength are useful descriptors of a material's IN ability. This insight allows the rationalization of ice nucleation ability across a wide range of materials and can aid the search and design of novel potent ice nucleators in the future.

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

    OpenAIRE

    Budke, C.; T. Koop

    2015-01-01

    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 i...

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

    OpenAIRE

    Budke, C.; T. Koop

    2014-01-01

    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 K min−1 and 10 K min−1. The droplets are separated from e...

  1. Immersion mode ice nucleation measurements with the new Portable Immersion Mode Cooling chAmber (PIMCA)

    Science.gov (United States)

    Kohn, Monika; Lohmann, Ulrike; Welti, André; Kanji, Zamin A.

    2016-05-01

    The new Portable Immersion Mode Cooling chAmber (PIMCA) has been developed for online immersion freezing of single-immersed aerosol particles. PIMCA is a vertical extension of the established Portable Ice Nucleation Chamber (PINC). PIMCA immerses aerosol particles into cloud droplets before they enter PINC. Immersion freezing experiments on cloud droplets with a radius of 5-7 μm at a prescribed supercooled temperature (T) and water saturation can be conducted, while other ice nucleation mechanisms (deposition, condensation, and contact mode) are excluded. Validation experiments on reference aerosol (kaolinite, ammonium sulfate, and ammonium nitrate) showed good agreement with theory and literature. The PIMCA-PINC setup was tested in the field during the Zurich AMBient Immersion freezing Study (ZAMBIS) in spring 2014 in Zurich, Switzerland. Significant concentrations of submicron ambient aerosol triggering immersion freezing at T > 236 K were rare. The mean frozen cloud droplet number concentration was estimated to be 7.22·105 L-1 for T ZAMBIS.

  2. Microbial ice nucleators are scavenged from the atmosphere during artificial rain events

    Science.gov (United States)

    Hanlon, Regina; Powers, Craig; Failor, Kevin; Vinatzer, Boris; Schmale, David

    2016-04-01

    Some microorganisms associated with rain may catalyze the nucleation of ice crystals at significantly warmer temperatures than would normally be required for ice formation, suggesting that they may play an important role in the onset of precipitation. Rain samples collected near the surface of the earth contain an array of microbial ice nucleators, but the little is known about their source(s) and life history. We conducted a series of field experiments to test the hypothesis that microbial ice nucleators are scavenged from the atmosphere by rainfall. Thirty three artificial rain events were conducted over four months (Nov 2014, Dec 2014, April 2015, and June 2015) off the side of the Smart Road Bridge in Blacksburg, VA, USA. In each event, sterile water was dispensed over the side of the bridge and recovered in sterile containers following gravitational settling from the bridge to an open fallow agricultural field below (a distance of ~55m). Microbes scavenged from the artificial rain events were cultured on six different types of agar media (R2A, TSA, CA; +/-cycloheximide), and the ice nucleation activity was examined for colonies cultured from the different media types. Mean CFUs scavenged by artificial rain ranged from 2 to 267 CFUs/mL. Microbial ice nucleators were cultured from 94% (31/33) of the simulated rain events, and represented 1.4% (121/8871) of the total number of colonies assayed. This percentage is similar to the percentage of culturable microbial ice nucleators occurring in about half of the natural rain events studied in Blacksburg, VA. Sequence-assisted identification of the repeatable microbial ice nucleators that were scavenged from the atmosphere showed a number of unique prokaryotic and eukaryotic taxa. This work expands our knowledge of the scavenging properties of rainfall, and suggests that at least some ice nucleators in natural precipitation events may have been scrubbed from the atmosphere during rainfall, and thus are not likely to be

  3. 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.

  4. 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.

  5. Heterogeneous nucleation of ice on anthropogenic organic particles collected in Mexico City

    Energy Technology Data Exchange (ETDEWEB)

    Knopf, D.A.; Wang, B.; Laskin, A.; Moffet, R.C.; Gilles, M.K.

    2010-06-20

    This study reports on heterogeneous ice nucleation activity of predominantly organic (or coated with organic material) anthropogenic particles sampled within and around the polluted environment of Mexico City. The onset of heterogeneous ice nucleation was observed as a function of particle temperature (Tp), relative humidity (RH), nucleation mode, and particle chemical composition which is influenced by photochemical atmospheric aging. Particle analyses included 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 (STXM/NEXAFS). In contrast to most laboratory studies employing proxies of organic aerosol, we show that anthropogenic organic particles collected in Mexico City can potentially induce ice nucleation at experimental conditions relevant to cirrus formation. The results suggest a new precedent for the potential impact of organic particles on ice cloud formation and climate.

  6. Ice nucleation efficiency of clay minerals in the immersion mode

    Directory of Open Access Journals (Sweden)

    V. Pinti

    2012-01-01

    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. DSC (differential scanning calorimeter measurements were performed on the kaolinites KGa-1b and KGa-2 from the Clay Mineral Society and kaolinite from Sigma-Aldrich; the montmorillonites SWy-2 and STx-1b from the Clay Mineral Society and the acid treated montmorillonites KSF and K-10 from Sigma Aldrich; the illites NX and SE from Arginotec. The emulsion experiments provide information on the average freezing behaviour characterized by the average nucleation sites. These experiments revealed one to 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 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 showed quite narrow standard peaks with onset temperatures 239 K < Tonstd < 242 K and best sites with averaged median freezing temperature Tmedbest = 257 K. Only the kaolinite from Sigma Aldrich featured a special peak with freezing onset at 248 K. The illites showed broad standard peaks with freezing onsets at 244 K < Tonstd < 246 K and best sites with averaged median freezing temperature Tmedbest = 262 K. Montmorillonites had standard peaks with onsets 238 K < Tonstd < 240 K and best sites with Tmedbest=257 K. SWy-2, M K10, and KSF featured special peaks with onsets at Tonspcl=247, 240, and 242 K

  7. Suspendable macromolecules are responsible for ice nucleation activity of birch and conifer pollen

    Directory of Open Access Journals (Sweden)

    B. G. Pummer

    2012-03-01

    Full Text Available The ice nucleation of bioaerosols (bacteria, pollen, spores, etc. is a topic of growing interest, since their impact on ice cloud formation and thus on radiative forcing, an important parameter in global climate, is not yet fully understood. Here we show that pollen of different species strongly differ in their ice nucleation behaviour. The average freezing temperatures in laboratory experiments range from 240 to 255 K. As the most efficient nuclei (silver birch, Scots pine and common juniper pollen have a distribution area up to the Northern timberline, their ice nucleation activity might be a cryoprotective mechanism. Far more intriguingly, it has turned out that water, which has been in contact with pollen and then been separated from the bodies, nucleates as good as the pollen grains themselves. The ice nuclei have to be easily-suspendable macromolecules located on the pollen. Once extracted, they can be distributed further through the atmosphere than the heavy pollen grains and so presumably augment the impact of pollen on ice cloud formation even in the upper troposphere. Our experiments lead to the conclusion that pollen ice nuclei, in contrast to bacterial and fungal ice nucleating proteins, are non-proteinaceous compounds.

  8. Manchester Ice Nucleus Counter (MINC measurements from the 2007 International workshop on Comparing Ice nucleation Measuring Systems (ICIS-2007

    Directory of Open Access Journals (Sweden)

    H. M. Jones

    2011-01-01

    Full Text Available An ice nucleus counter was developed and constructed to enable investigation of potential ice nucleating materials. The Manchester Ice Nucleus Chamber (MINC is a concentric-cylinder continuous flow diffusion chamber (CFDC. A full explanation of the MINC instrument is given here, along with first results and a comparison to an established instrument of similar design (Colorado State University CFDC during sampling of common ice nucleating aerosols at the 2007 International workshop on Comparing Ice nucleation Measuring Systems (ICIS-2007. MINC and CSU-CFDC detected the onset of ice nucleation under similar conditions of temperature and supersaturation for several different types of ice nuclei. Comparisons of the ratio of ice nuclei to total aerosol concentrations as a function of supersaturation with respect to water (SSw showed agreement within one order of magnitude. Possible reasons for differences between the two instruments relating to differences in their design are discussed, along with suggestions to future improvements to the current design.

  9. The Many Faces of Heterogeneous Ice Nucleation: Interplay Between Surface Morphology and Hydrophobicity

    CERN Document Server

    Fitzner, Martin; Cox, Stephen J; Michaelides, Angelos

    2016-01-01

    What makes a material a good ice nucleating agent? Despite the importance of heterogeneous ice nucleation to a variety of fields, from cloud science to microbiology, major gaps in our understanding of this ubiquitous process still prevent us from answering this question. In this work, we have examined the ability of generic crystalline substrates to promote ice nucleation as a function of the hydrophobicity and the morphology of the surface. Nucleation rates have been obtained by brute-force molecular dynamics simulations of coarse-grained water on top of different surfaces of a model fcc crystal, varying the water-surface interaction and the surface lattice parameter. It turns out that the lattice mismatch of the surface with respect to ice, customarily regarded as the most important requirement for a good ice nucleating agent, is at most desirable but not a requirement. On the other hand, the balance between the morphology of the surface and its hydrophobicity can significantly alter the ice nucleation rate...

  10. The effects of hygroscopicity on ice nucleation of fossil fuel combustion aerosols in mixed-phase clouds

    Directory of Open Access Journals (Sweden)

    Y. Yun

    2013-04-01

    Full Text Available Fossil fuel black carbon and organic matter (ffBC/OM are often emitted together with sulfate, which coats the surface of these particles and changes their hygroscopicity. Observational studies at cirrus temperatures (≈−40 °C show that the hygroscopicity of soot particles can modulate their ice nucleation ability. Here, we implement a scheme for 3 categories of soot (hydrophobic, hydrophilic and hygroscopic on the basis of laboratory data and specify their ability to act as ice nuclei at mixed-phase temperatures by extrapolating the observations using a published deposition/condensation/immersion freezing parameterization. The new scheme results in significant changes to anthropogenic forcing in mixed-phase clouds. The net forcing in our offline model studies varies from 0.111 to 1.059 W m−2 depending on the ice nucleation capability of hygroscopic soot particles. The total anthropogenic cloud forcing and whole-sky forcing with the new scheme are 0.06 W m−2 and −2.45 W m−2, respectively, but could be more positive (by about 1.17 W m−2 if hygroscopic soot particles are allowed to nucleate ice particles. The change in liquid water path dominates the anthropogenic forcing in mixed-phase clouds.

  11. Advances in Understanding the Role of Aerosols on Ice Clouds from the Fifth International Ice Nucleation (FIN) Workshops

    Science.gov (United States)

    Cziczo, D. J.; Moehler, O.; DeMott, P. J.

    2015-12-01

    The relationship of ambient aerosol particles to the formation of ice-containing clouds is one of the largest uncertainties in understanding climate. This is due to several poorly understood processes including the microphysics of how particles nucleate ice, the number of effective heterogeneous ice nuclei and their atmospheric distribution, the role of anthropogenic activities in producing or changing the behavior of ice forming particles and the interplay between effective heterogeneous ice nuclei and homogeneous ice formation. Our team recently completed a three-part international workshop to improve our understanding of atmospheric ice formation. Termed the Fifth International Ice Nucleation (FIN) Workshops, our motivation was the limited number of measurements and a lack of understanding of how to compare data acquired by different groups. The first activity, termed FIN1, addressed the characterization of ice nucleating particle size, number and chemical composition. FIN2 addressed the determination of ice nucleating particle number density. Groups modeling ice nucleation joined FIN2 to provide insight on measurements critically needed to model atmospheric ice nucleation and to understand the performance of ice chambers. FIN1 and FIN2 took place at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) chamber at the Karlsruhe Institute of Technology. A particular emphasis of FIN1 and FIN2 was the use of 'blind' intercomparisons using a highly characterized, but unknown to the instrument operators, aerosol sample. The third activity, FIN3, took place at the Desert Research Institute's Storm Peak Laboratory (SPL). A high elevation site not subject to local emissions, SPL allowed for a comparison of ice chambers and subsequent analysis of the ice residuals under the challenging conditions of low particle loading, temperature and pressure found in the atmosphere. The presentation focuses on the improvement in understanding how mass spectra from different

  12. Direct Calculation of Ice Homogeneous Nucleation Rate for a Molecular Model of Water

    CERN Document Server

    Haji-Akbari, Amir

    2015-01-01

    Ice formation is ubiquitous in nature, with important consequences in a variety of systems and environments, including biological cells [1], soil [2], aircraft [3], transportation infrastructure [4] and atmospheric clouds [5,6]. 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 [7-9]. For the more realistic molecular models, only indirect estimates have been obtained, e.g.~by assuming the validity of classical nucleation theory [10]. Here, we use a path sampling approach to perform the first direct rate calculation of homogeneous nucleation of ice in a molecular model of water. We use TIP4P/Ice [11], the most accurate among the existing molecular models for studying ice polymorphs. By using a novel topological order parameter for distinguishing different polymorphs, we are able to identify a freezing me...

  13. How important is biological ice nucleation in clouds on a global scale?

    Energy Technology Data Exchange (ETDEWEB)

    Hoose, C; Kristjansson, J E [Department of Geosciences, University of Oslo, Oslo (Norway); Burrows, S M, E-mail: corinna.hoose@kit.edu [Max Planck Institute for Chemistry, Mainz (Germany)

    2010-04-15

    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{sup -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.

  14. Size-resolved measurements of ice nucleating particles at North American and European sites

    Science.gov (United States)

    Mason, R.; Si, M.; Chou, C.; Irish, V.; Dickie, R.; Elizondo, P.; Wong, R.; Brintnell, M.; Elsasser, M.; Lassar, W.; Pierce, K.; Leaitch, W. R.; Macdonald, A. M.; Platt, A.; Desiree, T. S.; Sarda Esteve, R.; Schiller, C. L.; Suski, K. J.; Hill, T. C. J.; Abbatt, J.; Huffman, J. A.; DeMott, P. J.; Bertram, A. K.

    2015-12-01

    Ice nucleating particles (INPs) are a small fraction of the total aerosol population capable of catalyzing ice formation under atmospheric conditions, and may therefore influence the albedo and lifetime of mixed-phase and ice clouds. Compared to ambient measurements of the total number concentration of INPs, relatively little data exists on the size distribution of INPs in the atmosphere. Information on the size of INPs may be useful in source identification, modeling their transport in the atmosphere, and determining the degree to which common INP instrumentation captures the full atmospheric INP population. Measured using the micro-orifice uniform deposit impactor-droplet freezing technique (MOUDI-DFT), we report immersion-mode INP number concentrations as a function of particle size at ground-level sites in North America and Europe, including Arctic, alpine, coastal, marine, agricultural, and suburban environments. On average, more than 91 % of INPs active at -15 °C were found to be supermicron in size and 62 % were in the coarse mode (> 2.5 μm). While these percentages decreased with decreasing freezing temperature, many INPs remained in the supermicron with nearly half of those active at -25 °C belonging to the coarse mode.

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

    Science.gov (United States)

    Wagner, Robert; Kiselev, Alexei; Möhler, Ottmar; Saathoff, Harald; Steinke, Isabelle

    2016-02-01

    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.

  16. 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...

  17. Characterization and recombinant expression of a divergent ice nucleation protein from 'Pseudomonas borealis'.

    Science.gov (United States)

    Wu, Zhongqin; Qin, Lei; Walker, Virginia K

    2009-04-01

    Isolates of 'Pseudomonas borealis' were recovered after ice-affinity selection of summer-collected soils. 'P. borealis' DL7 was further characterized and shown to have ice nucleation activity (INA), a property that allows the crystallization of ice at temperatures close to the melting point, effectively preventing the supercooling of water. INA was optimally detected after culturing at temperatures consistent with psychrophilic growth. The sequence encoding the 'P. borealis' ice nucleation protein (INP) was obtained using both PCR and chromosome walking. When expressed in Escherichia coli, the resulting inaPb recombinants had INA. The 'P. borealis' sequence, dubbed inaPb, is clearly related to previously cloned INP genes, but it shows greater divergence. Sequence analysis suggests that there are two opposite flat surfaces, one relatively hydrophobic that likely serves as an ice template, and the other that could function as a complementary face to facilitate interprotein interaction for ice-step formation.

  18. Refreeze experiments with water droplets containing different types of ice nuclei interpreted by classical nucleation theory

    Science.gov (United States)

    Kaufmann, Lukas; Marcolli, Claudia; Luo, Beiping; Peter, Thomas

    2017-03-01

    Homogeneous nucleation of ice in supercooled water droplets is a stochastic process. In its classical description, the growth of the ice phase requires the emergence of a critical embryo from random fluctuations of water molecules between the water bulk and ice-like clusters, which is associated with overcoming an energy barrier. For heterogeneous ice nucleation on ice-nucleating surfaces both stochastic and deterministic descriptions are in use. Deterministic (singular) descriptions are often favored because the temperature dependence of ice nucleation on a substrate usually dominates the stochastic time dependence, and the ease of representation facilitates the incorporation in climate models. Conversely, classical nucleation theory (CNT) describes heterogeneous ice nucleation as a stochastic process with a reduced energy barrier for the formation of a critical embryo in the presence of an ice-nucleating surface. The energy reduction is conveniently parameterized in terms of a contact angle α between the ice phase immersed in liquid water and the heterogeneous surface. This study investigates various ice-nucleating agents in immersion mode by subjecting them to repeated freezing cycles to elucidate and discriminate the time and temperature dependences of heterogeneous ice nucleation. Freezing rates determined from such refreeze experiments are presented for Hoggar Mountain dust, birch pollen washing water, Arizona test dust (ATD), and also nonadecanol coatings. For the analysis of the experimental data with CNT, we assumed the same active site to be always responsible for freezing. Three different CNT-based parameterizations were used to describe rate coefficients for heterogeneous ice nucleation as a function of temperature, all leading to very similar results: for Hoggar Mountain dust, ATD, and larger nonadecanol-coated water droplets, the experimentally determined increase in freezing rate with decreasing temperature is too shallow to be described properly by

  19. 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

  20. A physically constrained classical description of the homogeneous nucleation of ice in water

    Science.gov (United States)

    Koop, Thomas; Murray, Benjamin J.

    2016-12-01

    Liquid water can persist in a supercooled state to below 238 K in the Earth's atmosphere, a temperature range where homogeneous nucleation becomes increasingly probable. However, the rate of homogeneous ice nucleation in supercooled water is poorly constrained, in part, because supercooled water eludes experimental scrutiny in the region of the homogeneous nucleation regime where it can exist only fleetingly. Here we present a new parameterization of the rate of homogeneous ice nucleation based on classical nucleation theory. In our approach, we constrain the key terms in classical theory, i.e., the diffusion activation energy and the ice-liquid interfacial energy, with physically consistent parameterizations of the pertinent quantities. The diffusion activation energy is related to the translational self-diffusion coefficient of water for which we assess a range of descriptions and conclude that the most physically consistent fit is provided by a power law. The other key term is the interfacial energy between the ice embryo and supercooled water whose temperature dependence we constrain using the Turnbull correlation, which relates the interfacial energy to the difference in enthalpy between the solid and liquid phases. The only adjustable parameter in our model is the absolute value of the interfacial energy at one reference temperature. That value is determined by fitting this classical model to a selection of laboratory homogeneous ice nucleation data sets between 233.6 K and 238.5 K. On extrapolation to temperatures below 233 K, into a range not accessible to standard techniques, we predict that the homogeneous nucleation rate peaks between about 227 and 231 K at a maximum nucleation rate many orders of magnitude lower than previous parameterizations suggest. This extrapolation to temperatures below 233 K is consistent with the most recent measurement of the ice nucleation rate in micrometer-sized droplets at temperatures of 227-232 K on very short time scales

  1. Can secondary nucleation exist in ice banding of freezing colloidal suspensions?

    Science.gov (United States)

    You, Jia-Xue; Wang, Jin-Cheng; Wang, Li-Lin; Wang, Zhi-Jun; Li, Jun-Jie; Lin, Xin

    2016-12-01

    The formation mechanism of ice banding in the system of freezing colloidal suspensions, which is of significance in frost heaving, ice-templating porous materials and biological materials, is still a mystery. Recently, the theory of secondary nucleation and growth of ice has been proposed to explain the emergence of a new ice lens. However, this theory has not been quantitatively examined. Here, we quantitatively measure the initial interfacial undercooling of a new ice lens and the nucleation undercoolings of suspensions. We find that the interfacial undercooling cannot satisfy the nucleation undercooling of ice and hence disprove the secondary nucleation mechanism for ice banding. Project supported by the National Natural Science Foundation of China (Grant Nos. 51371151 and 51571165), the Free Research Fund of State Key Laboratory of Solidification Processing, China (Grant No. 100-QP-2014), the Fund of State Key Laboratory of Solidification Processing in Northwestern Polytechnical University (NWPU), China (Grant No. 13-BZ-2014), and the Fundamental Research Funds for the Central Universities, China (Grant No. 3102015ZY020).

  2. Single ice crystal measurements during nucleation experiments with the depolarization detector IODE

    Directory of Open Access Journals (Sweden)

    M. Nicolet

    2008-12-01

    Full Text Available In order to determine the efficiency of aerosol particles of several types to nucleate ice, an Ice Optical DEpolarization detector (IODE was developed to distinguish between water droplets and ice crystals in ice nucleation chambers. A laser beam polarized linearly (power: 50 mW, wavelength: 407 nm is directed through the chamber. The scattered light intensity from particles is measured at a scattering angle of Θ=175° in both polarization components (parallel and perpendicular. The ratio between the perpendicular intensity over the total one gives the depolarization ratio δ. Single particle detection is possible, using a peak detection algorithm. For high particle concentrations, a real-time signal averaging method can also be run simultaneously. The IODE detector was used in connection with the Zurich ice nucleation chamber during the ICIS 2007 workshop where ice nucleation experiments were performed with several aerosol types. In presence of ice crystals, peaks were detected in both channels, generating depolarization signals. Mean values of δ ranged from 0.24 to 0.37.

  3. Single ice crystal measurements during nucleation experiments with the depolarization detector IODE

    Directory of Open Access Journals (Sweden)

    M. Nicolet

    2010-01-01

    Full Text Available In order to determine the efficiency of different aerosol particles to nucleate ice, an Ice Optical DEpolarization detector (IODE was developed to distinguish between water droplets and ice crystals in ice nucleation chambers. A laser beam polarized linearly (power: 50 mW, wavelength: 407 nm is directed through the chamber. The scattered light intensity from particles is measured at a scattering angle of Θ=175° in both polarization components (parallel and perpendicular. The ratio between the perpendicular intensity over the total one yields the depolarization ratio δ. Single particle detection is possible, using a peak detection algorithm. For high particle concentrations, a real-time signal averaging method can also be run simultaneously.

    The IODE detector was used in connection with the Zurich ice nucleation chamber during the ICIS 2007 workshop where ice nucleation experiments were performed with several aerosol types. In presence of ice crystals, a depolarization ratio could be measured on a particle-by-particle basis. Mean values of δ ranged from 0.24 to 0.37 and agree well with theoretical calculations.

  4. Single ice crystal measurements during nucleation experiments with the depolarization detector IODE

    Science.gov (United States)

    Nicolet, M.; Stetzer, O.; Lüönd, F.; Möhler, O.; Lohmann, U.

    2010-01-01

    In order to determine the efficiency of different aerosol particles to nucleate ice, an Ice Optical DEpolarization detector (IODE) was developed to distinguish between water droplets and ice crystals in ice nucleation chambers. A laser beam polarized linearly (power: 50 mW, wavelength: 407 nm) is directed through the chamber. The scattered light intensity from particles is measured at a scattering angle of Θ=175° in both polarization components (parallel and perpendicular). The ratio between the perpendicular intensity over the total one yields the depolarization ratio δ. Single particle detection is possible, using a peak detection algorithm. For high particle concentrations, a real-time signal averaging method can also be run simultaneously. The IODE detector was used in connection with the Zurich ice nucleation chamber during the ICIS 2007 workshop where ice nucleation experiments were performed with several aerosol types. In presence of ice crystals, a depolarization ratio could be measured on a particle-by-particle basis. Mean values of δ ranged from 0.24 to 0.37 and agree well with theoretical calculations.

  5. Heterogeneous ice nucleation: Exploring the transition from stochastic to singular freezing behavior

    Science.gov (United States)

    Stratmann, F.; Niedermeier, D.; Hartmann, S.; Shaw, R. A.; Clauss, T.; Wex, H.

    2011-12-01

    Heterogeneous ice nucleation directly influences cloud physical processes, precipitation formation, global radiation balances, and therefore Earth's climate (Cantrell and Heymsfield, 2005 and references therein). It is important to understand the heterogeneous freezing process at a fundamental level in order to describe this process in a physically-based way that will behave robustly in weather and climate models. There is longstanding debate as to whether heterogeneous ice nucleation is a stochastic process (e.g., Carte, 1956) or whether it exhibits singular behaviour (e.g., Langham and Mason, 1958). Fundamentally, the stochastic ice nucleation behavior implies ice nucleation being time dependent, while singular behavior is characterized by ice nucleation taking place on specific particle surface sites at a certain temperature and being time independent (Vali and Stansbury, 1966). We addressed this issue using both experimental and theoretical methods. Experiments focused on immersion freezing of Arizona Test Dust (ATD) were carried out using the Leipzig Aerosol Cloud Interaction Simulator (LACIS), a seven meter long laminar flow diffusion chamber. Both, temperature and time dependencies of ATD-particle induced immersion freezing were investigated. It was found, that ATD-particle induced immersion freezing took place over a wide temperature range and exhibited no detectable time dependence within the range investigated. The theoretical investigations were carried out using a Classical Nucleation Theory (CNT) based, i.e., purely stochastic, numerical model. This idealized model treats statistically similar particles as being covered with surface sites (patches of finite area) characterized by different nucleation barriers, but with each surface site following the stochastic nature of ice embryo formation. The model provides a phenomenological explanation for seemingly contradictory experimental results obtained in the past. Based on CNT alone, a population of

  6. 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.

    2017-02-01

    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'.

  7. 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.

  8. Irreversible loss of ice nucleation active sites in mineral dust particles caused by sulphuric acid condensation

    Directory of Open Access Journals (Sweden)

    R. C. Sullivan

    2010-07-01

    Full Text Available During the FROST-2 (FReezing Of duST measurement campaign conducted at the Leipzig Aerosol Cloud Interaction Simulator (LACIS, we investigated changes in the ice nucleation properties of 300 nm Arizona test dust mineral particles following thermochemical processing by varying amounts and combinations of exposure to sulphuric acid vapour, ammonia gas, water vapour, and heat. The processed aerosol's heterogeneous ice nucleation properties were determined in both the water subsaturated and supersaturated humidity regimes at −30 °C and −25 °C using Colorado State University's continuous flow diffusion chamber. The amount of sulphuric acid coating material was estimated by an aerosol mass spectrometer and from CCN-derived hygroscopicity measurements. The condensation of sulphuric acid decreased the dust particles' ice nucleation ability in proportion to the amount of sulphuric acid added. Heating the coated particles in a thermodenuder at 250 °C – intended to evaporate the sulphuric acid coating – reduced their freezing ability even further. We attribute this behaviour to accelerated acid digestion of ice active surface sites by heat. Exposing sulphuric acid coated dust to ammonia gas produced particles with similarly poor freezing potential; however a portion of their ice nucleation ability could be restored after heating in the thermodenuder. In no case did any combination of thermochemical treatments increase the ice nucleation ability of the coated mineral dust particles compared to unprocessed dust. These first measurements of the effect of identical chemical processing of dust particles on their ice nucleation ability in both water subsaturated and mixed-phase supersaturated cloud conditions revealed that ice nucleation was more sensitive to all coating treatments in the water subsaturated regime. The results clearly indicate irreversible impairment of ice nucleation activity in both regimes after condensation of concentrated

  9. Assessment of parameterizations of heterogeneous ice nucleation in cloud and climate models

    Directory of Open Access Journals (Sweden)

    J. A. Curry

    2010-02-01

    Full Text Available Several different types of parameterization of heterogeneous ice nucleation for cloud and climate models have been developed over the past decades, ranging from empirically-derived expressions to parameterizations of ice crystal nucleation rates derived from theory (including the parameterization developed by the authors, hereafter referred to as KC. Parameterizations schemes that address the deliquescence-freezing (DF, which combines the thermodynamically indistinguishable modes of condensation freezing and immersion freezing, are assessed here in the context of thermodynamic constraints, laboratory measurements, and recent field measurements. It is shown that empirical schemes depending only on the ice saturation ratio or only on temperature can produce reasonable crystal concentrations, but ice crystal nucleation is thermodynamically prohibited in certain regions of the temperature-saturation ratio phase space. Some recent empirical parameterizations are shown to have insufficient efficiency, yielding clouds that are almost entire liquid at temperatures as low as −35 °C. A reasonable performance of the KC ice nucleation scheme is demonstrated by comparison with data from several recent field campaigns, laboratory data, climatology of cloud phase-state, and GCM parameterizations. Several mis-applications of the KC parameterization that appeared recently in the literature are described and corrected, by emphasizing that a correct application of the KC scheme with simultaneous dependence on the temperature and saturation ratio requires integration of the individual nucleation rates over the measured size spectrum of the environmental aerosol, and not over the spectrum of ice nuclei equal to the crystal concentration at the exit of an experimental device. Simulation with a spectral bin model and correct application of KC scheme adequately describes ice nucleation via the DF mode and yields crystal concentrations and phase state close to those

  10. Results from the University of Toronto continuous flow diffusion chamber (UT-CFDC at the international workshop for comparing ice nucleation measuring systems (ICIS 2007

    Directory of Open Access Journals (Sweden)

    Z. A. Kanji

    2010-09-01

    Full Text Available The University of Toronto continuous flow diffusion chamber (UT-CFDC was used to study heterogeneous ice nucleation at the International Workshop on Comparing Ice Nucleation Measuring Systems (ICIS 2007 which also represented the 4th ice nucleation workshop, on 14–28 September 2007. One goal of the workshop was to inter-compare different ice nucleation measurement techniques using the same aerosol sample source and preparation method. The aerosol samples included four types of desert mineral dust, graphite soot particles, and live and dead bacterial cells (Snomax®. This paper focuses on the UT-CFDC results, with a comparison to techniques of established heritage including the Colorado State CFDC and the AIDA expansion chamber. Good agreement was found between the different instruments with a few specific differences attributed to the variation in how onset of ice formation is defined between the instruments. It was found that when efficiency of ice formation is based on the lowest onset relative humidity, Snomax® particles were most efficient followed by the desert dusts and then soot. For all aerosols, deposition mode freezing was only observed for T < 245 K except for the dead bacteria where freezing occurred below water saturation as warm as 263 K.

  11. Results from the University of Toronto continuous flow diffusion chamber (UT-CFDC) at the international workshop for comparing ice nucleation measuring systems (ICIS 2007)

    Science.gov (United States)

    Kanji, Z. A.; Demott, P. J.; Möhler, O.; Abbatt, J. P. D.

    2010-09-01

    The University of Toronto continuous flow diffusion chamber (UT-CFDC) was used to study heterogeneous ice nucleation at the International Workshop on Comparing Ice Nucleation Measuring Systems (ICIS 2007) which also represented the 4th ice nucleation workshop, on 14-28 September 2007. One goal of the workshop was to inter-compare different ice nucleation measurement techniques using the same aerosol sample source and preparation method. The aerosol samples included four types of desert mineral dust, graphite soot particles, and live and dead bacterial cells (Snomax®). This paper focuses on the UT-CFDC results, with a comparison to techniques of established heritage including the Colorado State CFDC and the AIDA expansion chamber. Good agreement was found between the different instruments with a few specific differences attributed to the variation in how onset of ice formation is defined between the instruments. It was found that when efficiency of ice formation is based on the lowest onset relative humidity, Snomax® particles were most efficient followed by the desert dusts and then soot. For all aerosols, deposition mode freezing was only observed for T < 245 K except for the dead bacteria where freezing occurred below water saturation as warm as 263 K.

  12. Role of ice nucleation and antifreeze activities in pathogenesis and growth of snow molds.

    Science.gov (United States)

    Snider, C S; Hsiang, T; Zhao, G; Griffith, M

    2000-04-01

    ABSTRACT We examined the ability of snow molds to grow at temperatures from -5 to 30 degrees C and to influence the growth of ice through assays for ice nucleation and antifreeze activities. Isolates of Coprinus psychromorbidus (low temperature basidiomycete variant), Microdochium nivale, Typhula phacorrhiza, T. ishikariensis, T. incarnata, and T. canadensis all grew at -5 degrees C, whereas Sclerotinia borealis and S. homoeocarpa did not grow at temperatures below 4 degrees C. The highest threshold ice nucleation temperature was -7 degrees C. Because snow molds are most damaging to their hosts at temperatures above this, our results imply that the pathogenesis of these fungi is not dependent on ice nucleation activity to cause freeze-wounding of host plants. All snow molds that grew at subzero temperatures also exhibited antifreeze activity in the growth medium and in the soluble and insoluble hyphal fractions, with the exception of M. nivale and one isolate of T. canadensis. The lack of high ice nucleation activity combined with the presence of antifreeze activity in all fungal fractions indicates that snow molds can moderate their environment to inhibit or modify intra- and extracellular ice formation, which helps explain their ability to grow at subzero temperatures under snow cover.

  13. Ice nucleation by soil dusts: relative importance of mineral dust and biogenic components

    Directory of Open Access Journals (Sweden)

    D. O'Sullivan

    2013-08-01

    Full Text Available Agricultural dust emissions have been estimated to contribute around 20% to the global dust burden. In contrast to dusts from arid source regions, the ice-nucleating abilities of which have been relatively well studied, soil dusts from fertile sources often contain a substantial fraction of organic matter. Using an experimental methodology which is sensitive to a wide range of ice nucleation efficiencies, we have characterised the immersion mode ice-nucleating activities of dusts extracted from fertile soils collected at four locations around England. By controlling droplet sizes, which ranged in volume from 10−12 to 10−6 L, we have been able to determine the ice nucleation behaviour of soil dust particles at temperatures ranging from 267 K (−6 °C down to the homogeneous limit of freezing at about 237 K (−36 °C. At temperatures above 258 K (−15 °C we find that the ice-nucleating activity of soil dusts is diminished by heat treatment or digestion with hydrogen peroxide, suggesting that the ice nuclei stem from biogenic components in the soil. However, below 258 K, we find that the ice active site densities tend towards those expected from the mineral components in the soils, suggesting that the inorganic fraction of soil dusts, in particular the K-feldspar fraction, becomes increasingly important in the initiation of the ice phase at lower temperatures. We conclude that although only a relatively minor contributor to the global atmospheric dust burden, the enhanced IN activities of dusts generated from agricultural activities may play an important role in cloud glaciation, particularly at temperatures above 258 K.

  14. Assessment of some parameterizations of heterogeneous ice nucleation in cloud and climate models

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    J. A. Curry

    2012-01-01

    Full Text Available Several different types of parameterization of heterogeneous ice nucleation for cloud and climate models have been developed over the past decades, ranging from empirically-derived expressions to parameterizations of ice crystal nucleation rates derived from theory, including the parameterization developed by the authors that includes simultaneous dependence on the temperature and saturation ratio, hereafter referred to as KC. Parameterizations schemes that address the deliquescence-heterogeneous-freezing (DHetF, which combines the modes of condensation freezing and immersion freezing, are assessed here in the context of thermodynamic constraints, laboratory measurements, and recent field measurements. It is shown that empirical schemes depending only on the ice saturation ratio or only on temperature can produce reasonable crystal concentrations, but ice crystal nucleation is thermodynamically prohibited in certain regions of the temperature-saturation ratio phase space. Some recent empirical parameterizations yield clouds that are almost entire liquid at temperatures as low as −35 °C in contrast to cloud climatology. Reasonable performance of the KC ice nucleation scheme is demonstrated by comparison with numerous data from several recent field campaigns, laboratory data, climatology of cloud phase-state. Several mis-applications of the KC parameterization that appeared recently in the literature are described and corrected. It is emphasized here that a correct application of the KC scheme requires integration of the individual nucleation rates over the measured size spectrum of ice nuclei that represent a fraction or several fractions of the environmental aerosol with specific ice nucleation properties. The concentration in these fractions can be substantially smaller than that of the total aerosol, but greater than the crystal concentration measured by an experimental device. Simulations with temperature-dependent active site area or with

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

    Science.gov (United States)

    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.

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

    Science.gov (United States)

    Wagner, R.; Kiselev, A.; Möhler, O.; Saathoff, H.; Steinke, I.

    2015-10-01

    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. Already 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. 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.

  17. Ice nucleation and cloud microphysical properties in tropical tropopause layer cirrus

    Directory of Open Access Journals (Sweden)

    E. J. Jensen

    2009-10-01

    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. Possible implications of the observed cloud microphysical properties for ice sedimentation, dehydration, and cloud persistence are also discussed.

  18. Ice nucleation and cloud microphysical properties in tropical tropopause layer cirrus

    Directory of Open Access Journals (Sweden)

    E. J. Jensen

    2010-02-01

    Full Text Available In past modeling studies, it has generally been assumed that the predominant mechanism for nucleation of ice in the uppermost troposphere is homogeneous freezing of aqueous aerosols. However, recent in situ and remote-sensing measurements of the properties of cirrus clouds at very low temperatures in the tropical tropopause layer (TTL are broadly inconsistent with theoretial predictions based on the homogeneous freezing assumption. The nearly ubiquitous occurence of gravity waves in the TTL makes the predictions from homogeneous nucleation theory particularly difficult to reconcile with measurements. These measured properties include ice number concentrations, which are much lower than theory predicts; ice crystal size distributions, which are much broader than theory predicts; and cloud extinctions, which are much lower than theory predicts. Although other explanations are possible, one way to limit ice concentrations is to have on the order of 50 L−1 effective ice nuclei (IN that could nucleate ice at relatively low supersaturations. We suggest that ammonium sulfate particles, which would be dry much of the time in the cold TTL, are a potential IN candidate for TTL cirrus. However, this mechanism remains to be fully quantified for the size distribution of ammonium sulfate (possibly internally mixed with organics actually present in the upper troposphere. Possible implications of the observed cloud microphysical properties for ice sedimentation, dehydration, and cloud persistence are also discussed.

  19. Re-evaluating the Frankfurt isothermal static diffusion chamber for ice nucleation

    Directory of Open Access Journals (Sweden)

    J. Schrod

    2015-12-01

    Full Text Available Recently significant advances have been made in the collection, detection, and characterization of ice nucleating particles (INP. Ice nuclei are particles that facilitate the heterogeneous formation of ice within the atmospheric aerosol by lowering the free energy barrier to spontaneous nucleation and growth of ice from atmospheric water and/or vapor. The Frankfurt isostatic diffusion chamber (FRIDGE is an INP collection and offline detection system that has become widely deployed and shows additional potential for ambient measurements. Since its initial development FRIDGE has gone through several iterations and improvements. Here we describe improvements that have been made in the collection and analysis techniques. We detail the uncertainties inherent in the measurement method, and suggest a systematic method of error analysis for FRIDGE measurements. Thus what is presented herein should serve as a foundation for the dissemination of all current and future measurements using FRIDGE instrumentation.

  20. Thermodynamics of homogeneous nucleation of ice particles in the polar summer mesosphere

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    A. Y. Zasetsky

    2008-07-01

    Full Text Available We present the hypothesis of homogeneous nucleation of ice nano-particles in the polar summer mesosphere. The nucleation of condensed phase is traced back to the first step on the formation pathway, which is assumed to be the transition of water vapor to amorphous cluster. Amorphous clusters then freeze into water ice, likely metastable cubic ice, when they reach the critical size. The estimates based on the equilibrium thermodynamics give the critical size (radius of amorphous water clusters as about 1.0 nm. The same estimates for the final transition step, that is the transformation of cubic to hexagonal ice, give the critical size of about 15 nm at typical upper mesospheric conditions during the polar summer (temperature T=150 K, water vapor density ρvapor=109 cm−3.

  1. Immersion mode heterogeneous ice nucleation by an illite rich powder representative of atmospheric mineral dust

    Directory of Open Access Journals (Sweden)

    S. L. Broadley

    2011-08-01

    Full Text Available Atmospheric dust rich in illite is transported globally from arid regions and may impact cloud properties through the nucleation of ice. We present measurements of ice nucleation in water droplets containing known quantities of an illite rich powder under atmospherically relevant conditions. The illite rich powder used here, NX illite, has a similar mineralogical composition to atmospheric mineral dust sampled in remote locations, i.e. dust which has been subject to long range transport, cloud processing and sedimentation. Arizona Test Dust has a significantly different mineralogical composition and we suggest that NX illite is a better surrogate of natural atmospheric dust. Heterogeneous nucleation by NX illite was observed, using optical microscopy, to occur dominantly between 246 K and the homogeneous freezing limit and higher freezing temperatures were observed with larger surface areas of NX illite present within the droplets. It is shown that there is strong particle to particle variability in terms of ice nucleating ability with a few particles dominating ice nucleation at high surface areas. In fact, this work suggests that the bulk of atmospheric mineral dust particles are less efficient at nucleating ice than assumed in parameterisation currently used in models. For droplets containing ≤2 × 10−6 cm2 of NX illite, freezing temperatures did not noticeably change when the cooling rate was varied by an order of magnitude. The data obtained during cooling experiments (with surface areas ≤2 × 10−6 cm2 is shown to be inconsistent with the single component stochastic model, but is well described by the singular model (ns(236.2 K ≤ T ≤ 247.5 K = exp(6.53043 × 104 − 8.2153088 × 102 T + 3.446885376 T 2 − 4.822268 × 10−3 T3. However, droplets continued to freeze when the temperature

  2. A Continuous Flow Diffusion Chamber Study of Sea Salt Particles Acting as Cloud Seeds: Deliquescence, Ice Nucleation and Sublimation

    Science.gov (United States)

    Kong, X.; Wolf, M. J.; Garimella, S.; Roesch, M.; Cziczo, D. J.

    2016-12-01

    Sea Salt Aerosols (SSA) are abundant in the atmosphere, and important to the Earth's chemistry and energy budget. However, the roles of sea salts in the context of cloud formation are still poorly understood, which is partially due to the complexity of the water-salt phase diagram. At ambient temperatures, even well below 0°C, SSA deliquesces at sub-water saturated conditions. Since the ratio of the partial pressure over ice versus super-cooled water continuously declines with decreasing temperatures, it is interesting to consider if SSA continues to deliquesce under a super-saturated condition of ice, or if particles act as depositional ice nuclei when a critical supersaturation is reached. Some recent studies suggest hydrated NaCl and simulated sea salt might deliquesce between -35°C to -44°C, and below that deposition freezing becomes possible. Deliquesced droplets can subsequently freeze via the immersion or homogenous freezing mode, depending on if the deliquescence processes is complete. After the droplets or ice particles are formed, it is also interesting to consider how the different processes influence physical properties after evaporation or sublimation. This data is important for climate modeling that includes bromine burst observed in Antarctica, which is hypothesized to be relevant to the sublimation of blowing snow particles. In this study we use a SPectrometer for Ice Nuclei (SPIN; DMT, Inc., Boulder, CO) to perform experiments over a wide range of temperature and RH conditions to quantify deliquescence, droplet formation and ice nucleation. The formation of droplets and ice particles is detected by an advanced Optical Particle Counter (OPC) and the liquid/solid phases are distinguished by a machine learning method based on laser scattering and polarization data. Using an atomizer, four different sea salt samples are generated: pure NaCl and MgCl2 solutions, synthetic seawater, and natural seawater. Downstream of the SPIN chamber, a Pumped

  3. Raman Spectra and Nucleation Rates of Sulfuric Acid and Ammonium Sulfate Aerosols Supercooled with Respect to Ice

    Science.gov (United States)

    Knopf, D. A.; Koop, T.; Weers, U. G.; Krieger, U. K.; Peter, T.

    2001-12-01

    Sulfuric acid and ammonium sulfate aerosol particles can serve as ice condensation nuclei for the formation of upper tropospheric cirrus clouds. These clouds influence the global radiation budget by scattering of short wavelength (solar) radiation as well as by absorbing long wavelength (terrestrial) radiation. Knowledge of the thermodynamics and the nucleation rates of aerosols is fundamental for the understanding of formation processes of cirrus clouds. Here, we present a new investigation tool to observe phase transitions of aerosols supercooled with respect to ice. Confocal Raman microscopy is used to determine the phase changes and the morphology of the particles. Raman spectroscopy is employed to distinguish and to characterize the different phases inside the frozen particles. Single droplets with a diameter of typically 20-120 μ m are deposited on a hydrophobically coated Herasil-plate that is covered by a spacer and another plate. Since the gas phase volume of the cell is small compared to the liquid droplet volume the composition of the droplets remains fixed during temperature changes. The temperature of the droplets can be varied between 150-350~K. We present the first Raman spectra of aqueous H2SO4/H2O and (NH4)2SO4/H2O droplets for several concentrations and temperatures to the homogeneous ice nucleation limits. The analysis of the speciation of the components inside the droplets (e.g. sulfate vs. bisulfate ions) is compared to results from thermodynamic models. Evaluation of the freezing data gives upper limits for ice nucleation rates of droplets as a function of sulfuric acid or ammonium sulfate concentration.

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

    Science.gov (United States)

    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. PMID:28056077

  5. 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

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

    Directory of Open Access Journals (Sweden)

    G. Kulkarni

    2009-01-01

    Full Text Available A new Thermal Gradient ice nucleation Diffusion Chamber (TGDC capable of investigating ice nucleation efficiency of atmospherically important aerosols, termed Ice Nuclei (IN, has been designed, constructed and validated. The TGDC can produce a range of supersaturations with respect to ice (SSi over the temperature range of −10 to −34°C for sufficiently long time needed to observe the ice nucleation by the aerosol particles. The novel aspect of this new TGDC is that the chamber is run in static mode with aerosol particles supported on a Teflon substrate, which can be raised and lowered in a controlled way through the SSi profile within the chamber, and nucleation events are directly observed using digital photography. The TGDC consists of two ice coated plates to which a thermal gradient is applied to produce the range of SSi. The design of the TGDC gives the ability to understand time-related ice nucleation event information and to perform experiments at different temperatures and SSi conditions for different IN without changing the thermal gradient within the TGDC. The temperature and SSi conditions of the experimental system are validated by observing (NH42SO4 deliquescence and the results are in good agreement with the literature data. First results are presented of the onset ice nucleation for mineral dust sampled from the Saharan Desert, including images of nucleation and statistical distributions of onset ice nucleation SSi as a function of temperature. This paper illustrates how useful this new TGDC is for process level studies of ice nucleation and more experimental investigations are needed to better quantify the role of ice formation in the atmosphere.

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

    Directory of Open Access Journals (Sweden)

    J. B. McQuaid

    2009-06-01

    Full Text Available A new Thermal Gradient ice nucleation Diffusion Chamber (TGDC capable of investigating ice nucleation efficiency of atmospherically important aerosols, termed Ice Nuclei (IN, has been designed, constructed and validated. The TGDC can produce a range of supersaturations with respect to ice (SSi over the temperature range of −10 to −34°C for sufficiently long time needed to observe the ice nucleation by the particles. The novel aspect of this new TGDC is that the chamber is run in static mode with aerosol particles supported on a Teflon substrate, which can be raised and lowered in a controlled way through the SSi profile within the chamber, and nucleation events are directly observed using digital photography. The TGDC consists of two ice coated plates to which a thermal gradient is applied to produce the range of SSi. The design of the TGDC gives the ability to understand time-related ice nucleation event information and to perform experiments at different temperatures and SSi conditions for different IN without changing the thermal gradient within the TGDC. The temperature and SSi conditions of the experimental system are validated by observing (NH42SO4 deliquescence and the results are in good agreement with the literature data. First results are presented of the onset ice nucleation for mineral dust sampled from the Saharan Desert, including images of nucleation and statistical distributions of onset ice nucleation SSi as a function of temperature. This paper illustrates how useful this new TGDC is for process level studies of ice nucleation and more experimental investigations are needed to better quantify the role of ice formation in the atmosphere.

  8. 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...

  9. Probing the Biomimetic Ice Nucleation Inhibition Activity of Poly(vinyl alcohol) and Comparison to Synthetic and Biological Polymers.

    Science.gov (United States)

    Congdon, Thomas; Dean, Bethany T; Kasperczak-Wright, James; Biggs, Caroline I; Notman, Rebecca; Gibson, Matthew I

    2015-09-14

    Nature has evolved many elegant solutions to enable life to flourish at low temperatures by either allowing (tolerance) or preventing (avoidance) ice formation. These processes are typically controlled by ice nucleating proteins or antifreeze proteins, which act to either promote nucleation, prevent nucleation or inhibit ice growth depending on the specific need, respectively. These proteins can be expensive and their mechanisms of action are not understood, limiting their translation, especially into biomedical cryopreservation applications. Here well-defined poly(vinyl alcohol), synthesized by RAFT/MADIX polymerization, is investigated for its ice nucleation inhibition (INI) activity, in contrast to its established ice growth inhibitory properties and compared to other synthetic polymers. It is shown that ice nucleation inhibition activity of PVA has a strong molecular weight dependence; polymers with a degree of polymerization below 200 being an effective inhibitor at just 1 mg.mL(-1). Other synthetic and natural polymers, both with and without hydroxyl-functional side chains, showed negligible activity, highlighting the unique ice/water interacting properties of PVA. These findings both aid our understanding of ice nucleation but demonstrate the potential of engineering synthetic polymers as new biomimetics to control ice formation/growth processes.

  10. 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).

  11. Immersion mode heterogeneous ice nucleation by an illite rich powder representative of atmospheric mineral dust

    Directory of Open Access Journals (Sweden)

    S. L. Broadley

    2012-01-01

    Full Text Available Atmospheric dust rich in illite is transported globally from arid regions and impacts cloud properties through the nucleation of ice. We present measurements of ice nucleation in water droplets containing known quantities of an illite rich powder under atmospherically relevant conditions. The illite rich powder used here, NX illite, has a similar mineralogical composition to atmospheric mineral dust sampled in remote locations, i.e. dust which has been subject to long range transport, cloud processing and sedimentation. Arizona Test Dust, which is used in other ice nucleation studies as a model atmospheric dust, has a significantly different mineralogical composition and we suggest that NX illite is a better surrogate of natural atmospheric dust.

    Using optical microscopy, heterogeneous nucleation in the immersion mode by NX illite was observed to occur dominantly between 246 K and the homogeneous freezing limit. In general, higher freezing temperatures were observed when larger surface areas of NX illite were present within the drops. Homogenous nucleation was observed to occur in droplets containing low surface areas of NX illite. We show that NX illite exhibits strong particle to particle variability in terms of ice nucleating ability, with ~1 in 105 particles dominating ice nucleation when high surface areas were present. In fact, this work suggests that the bulk of atmospheric mineral dust particles may be less efficient at nucleating ice than assumed in current model parameterisations.

    For droplets containing ≤2 × 10−6 cm2 of NX illite, freezing temperatures did not noticeably change when the cooling rate was varied by an order of magnitude. The data obtained during cooling experiments (surface area ≤2 × 10−6 cm2 is shown to be inconsistent with the single component stochastic model, but is well described by the singular model (ns(236

  12. 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.

  13. Ice nucleation efficiency of natural dust samples in the immersion mode

    Science.gov (United States)

    Kaufmann, Lukas; Marcolli, Claudia; Hofer, Julian; Pinti, Valeria; Hoyle, Christopher R.; Peter, Thomas

    2016-09-01

    A total of 12 natural surface dust samples, which were surface-collected on four continents, most of them in dust source regions, were investigated with respect to their ice nucleation activity. Dust collection sites were distributed across Africa, South America, the Middle East, and Antarctica. Mineralogical composition has been determined by means of X-ray diffraction. All samples proved to be mixtures of minerals, with major contributions from quartz, calcite, clay minerals, K-feldspars, and (Na, Ca)-feldspars. Reference samples of these minerals were investigated with the same methods as the natural dust samples. Furthermore, Arizona test dust (ATD) was re-evaluated as a benchmark. Immersion freezing of emulsion and bulk samples was investigated by differential scanning calorimetry. For emulsion measurements, water droplets with a size distribution peaking at about 2 µm, containing different amounts of dust between 0.5 and 50 wt % were cooled until all droplets were frozen. These measurements characterize the average freezing behaviour of particles, as they are sensitive to the average active sites present in a dust sample. In addition, bulk measurements were conducted with one single 2 mg droplet consisting of a 5 wt % aqueous suspension of the dusts/minerals. These measurements allow the investigation of the best ice-nucleating particles/sites available in a dust sample. All natural dusts, except for the Antarctica and ATD samples, froze in a remarkably narrow temperature range with the heterogeneously frozen fraction reaching 10 % between 244 and 250 K, 25 % between 242 and 246 K, and 50 % between 239 and 244 K. Bulk freezing occurred between 255 and 265 K. In contrast to the natural dusts, the reference minerals revealed ice nucleation temperatures with 2-3 times larger scatter. Calcite, dolomite, dolostone, and muscovite can be considered ice nucleation inactive. For microcline samples, a 50 % heterogeneously frozen fraction occurred above 245 K for all

  14. Immersion freezing in concentrated solution droplets for a variety of ice nucleating particles

    Science.gov (United States)

    Wex, Heike; Kohn, Monika; Grawe, Sarah; Hartmann, Susan; Hellner, Lisa; Herenz, Paul; Welti, Andre; Lohmann, Ulrike; Kanji, Zamin; Stratmann, Frank

    2016-04-01

    The measurement campaign LINC (Leipzig Ice Nucleation counter Comparison) was conducted in September 2015, during which ice nucleation measurements as obtained with the following instruments were compared: - LACIS (Leipzig Aerosol Cloud Interaction Simulator, see e.g. Wex et al., 2014) - PIMCA-PINC (Portable Immersion Mode Cooling Chamber together with PINC) - PINC (Portable Ice Nucleation Chamber, Chou et al., 2011) - SPIN (SPectrometer for Ice Nuclei, Droplet Measurement Technologies) While LACIS and PIMCA-PINC measured immersion freezing, PINC and SPIN varied the super-saturation during the measurements and collected data also for relative humidities below 100% RHw. A suite of different types of ice nucleating particles were examined, where particles were generated from suspensions, subsequently dried and size selected. For the following samples, data for all four instruments are available: K-feldspar, K-feldspar treated with nitric acid, Fluka-kaolinite and birch pollen. Immersion freezing measurements by LACIS and PIMCA-PINC were in excellent agreement. Respective parameterizations from these measurement were used to model the ice nucleation behavior below water vapor saturation, assuming that the process can be described as immersion freezing in concentrated solutions. This is equivalent to simply including a concentration dependent freezing point depression in the immersion freezing parameterization, as introduced for coated kaolinite particles in Wex et al. (2014). Overall, measurements performed below water vapor saturation were reproduced by the model, and it will be discussed in detail, why deviations were observed in some cases. Acknowledgement: Part of this work was funded by the DFG Research Unit FOR 1525 INUIT, grant WE 4722/1-2. Literature: Chou, C., O. Stetzer, E. Weingartner, Z. Juranyi, Z. A. Kanji, and U. Lohmann (2011), Ice nuclei properties within a Saharan dust event at the Jungfraujoch in the Swiss Alps, Atmos. Chem. Phys., 11(10), 4725

  15. Construction of ice nucleation active Enterobacter cloacae for control of insect pests

    Institute of Scientific and Technical Information of China (English)

    2003-01-01

    Ice nucleation active (INA) bacteria are the most potent heterogeneous ice nuclei in nature, which have become an important biological resource for diverse applications. Many researches have proved that INA bacteria can raise the supercooling points (SCPs) of insect pests, then reduce their cold hardiness. However, INA bacteria's inefficient colonization on the surface or in the guts of insects, and the high incidence of frost injury induced by their release hampered the application of INA bacteria in controlling insect pests in agricultural fields. In this study, we constructed a recombinant plasmid mob-Tn5-iceA with the ability of broad-host-range conjugal mobilization and integration of the ina gene of iceA into chromosomal DNA of many gram-negative bacteria by Tn5 transposition. In addition, Ent. cloacae strains stably carrying iceA and expressing high ice nucleation activity (INA), even in the absence of antibiotic pressure, were constructed through conjugal mobilization and Tn5 transposition. Ent. cloacae strains have been reported to be able to efficiently colonize in the guts of insects, but have weak plant epiphytic ability. Therefore, these transgenic Ent. cloacae may be promising candidates for control of insect pests in agricultural fields.

  16. a Design of Experiment Study of the Nucleation of Chemical Vapor Deposited Diamond Films.

    Science.gov (United States)

    Tang, Chi

    1995-01-01

    Because of its property, diamond has a unique role in the semiconductor and tool industry. As diamond synthesis technology advances, more and more applications are emerging. However, in order to take advantage of its exceptional property, reliable control of nucleation and growth must be accomplished. In this study, the author systematically studies the nucleation process in chemical vapor deposition (CVD) of diamonds. Among many important intricacies concerning diamond nucleation on foreign surfaces, this study addresses the following issues: the role of ultrasonic pre-treatment in CVD; the correlation between hot filament chemical vapor deposition (HFCVD) and microwave assisted chemical vapor deposition (MACVD) control parameters and the nucleation processes; the role of biasing substrates on the nucleation density in MACVD; the correlation between parameters of biasing substrates and the nucleation density; the reliable control of nucleation in CVD diamond synthesis. To achieve the goal of this research, a multi -purpose deposition system was built enabling the author to eliminate unnecessary variables in the deposition process. To ensure the accuracy of the nucleation effects of parameters investigated, great effort was made to calibrate measurement instruments so that noise or fluctuations in the experiments were minimized. The implementation of design of experiments (DOE), a systematic investigating technique, vastly improved the efficiency of this study over the less sophisticated empirical approach. In addition, DOE allowed the author to quantitatively estimate the effects of control parameters. Finally, diamond deposition was confirmed by Scanning Electron microscope, Micro Raman Scattering and Rutherford Backscattering. This research has successfully implemented DOE in estimating the effects of diamond nucleation quantitatively. The mechanism of ultrasonic pre-treatment is explained, and its effects are ascribed to seeding. The effects of primary CVD

  17. Contribution of feldspar and marine organic aerosols to global ice nucleating particle concentrations

    Science.gov (United States)

    Vergara-Temprado, Jesús; Murray, Benjamin J.; Wilson, Theodore W.; O'Sullivan, Daniel; Browse, Jo; Pringle, Kirsty J.; Ardon-Dryer, Karin; Bertram, Allan K.; Burrows, Susannah M.; Ceburnis, Darius; DeMott, Paul J.; Mason, Ryan H.; O'Dowd, Colin D.; Rinaldi, Matteo; Carslaw, Ken S.

    2017-03-01

    Ice-nucleating particles (INPs) are known to affect the amount of ice in mixed-phase clouds, thereby influencing many of their properties. The atmospheric INP concentration changes by orders of magnitude from terrestrial to marine environments, which typically contain much lower concentrations. Many modelling studies use parameterizations for heterogeneous ice nucleation and cloud ice processes that do not account for this difference because they were developed based on INP measurements made predominantly in terrestrial environments without considering the aerosol composition. Errors in the assumed INP concentration will influence the simulated amount of ice in mixed-phase clouds, leading to errors in top-of-atmosphere radiative flux and ultimately the climate sensitivity of the model. Here we develop a global model of INP concentrations relevant for mixed-phase clouds based on laboratory and field measurements of ice nucleation by K-feldspar (an ice-active component of desert dust) and marine organic aerosols (from sea spray). The simulated global distribution of INP concentrations based on these two species agrees much better with currently available ambient measurements than when INP concentrations are assumed to depend only on temperature or particle size. Underestimation of INP concentrations in some terrestrial locations may be due to the neglect of INPs from other terrestrial sources. Our model indicates that, on a monthly average basis, desert dusts dominate the contribution to the INP population over much of the world, but marine organics become increasingly important over remote oceans and they dominate over the Southern Ocean. However, day-to-day variability is important. Because desert dust aerosol tends to be sporadic, marine organic aerosols dominate the INP population on many days per month over much of the mid- and high-latitude Northern Hemisphere. This study advances our understanding of which aerosol species need to be included in order to

  18. Contribution of feldspar and marine organic aerosols to global ice nucleating particle concentrations

    Energy Technology Data Exchange (ETDEWEB)

    Vergara-Temprado, Jesús; Murray, Benjamin J.; Wilson, Theodore W.; O& amp; apos; Sullivan, Daniel; Browse, Jo; Pringle, Kirsty J.; Ardon-Dryer, Karin; Bertram, Allan K.; Burrows, Susannah M.; Ceburnis, Darius; DeMott, Paul J.; Mason, Ryan H.; O& amp; apos; Dowd, Colin D.; Rinaldi, Matteo; Carslaw, Ken S.

    2017-01-01

    Ice-nucleating particles (INPs) are known to affect the amount of ice in mixed-phase clouds, thereby influencing many of their properties. The atmospheric INP concentration changes by orders of magnitude from terrestrial to marine environments, which typically contain much lower concentrations. Many modelling studies use parameterizations for heterogeneous ice nucleation and cloud ice processes that do not account for this difference because they were developed based on INP measurements made predominantly in terrestrial environments without considering the aerosol composition. Errors in the assumed INP concentration will influence the simulated amount of ice in mixed-phase clouds, leading to errors in top-of-atmosphere radiative flux and ultimately the climate sensitivity of the model. Here we develop a global model of INP concentrations relevant for mixed-phase clouds based on laboratory and field measurements of ice nucleation by K-feldspar (an ice-active component of desert dust) and marine organic aerosols (from sea spray). The simulated global distribution of INP concentrations based on these two species agrees much better with currently available ambient measurements than when INP concentrations are assumed to depend only on temperature or particle size. Underestimation of INP concentrations in some terrestrial locations may be due to the neglect of INPs from other terrestrial sources. Our model indicates that, on a monthly average basis, desert dusts dominate the contribution to the INP population over much of the world, but marine organics become increasingly important over remote oceans and they dominate over the Southern Ocean. However, day-to-day variability is important. Because desert dust aerosol tends to be sporadic, marine organic aerosols dominate the INP population on many days per month over much of the mid- and high-latitude Northern Hemisphere. This study advances our understanding of which aerosol species need to be included in order to

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

    Directory of Open Access Journals (Sweden)

    O. Möhler

    2008-04-01

    Full Text Available The ice nucleation activities of five different Pseudomonas syringae, Pseudomonas viridiflava and Erwinia herbicola bacterial species and of SnomaxTM were investigated in the temperature range between −5 and −15°C. Water suspensions of these bacteria were directly spray into the cloud chamber of the AIDA facility of Forschungszentrum Karlsruhe at a temperature of −5.7°. At this temperature, about 1% of the SnomaxTM cells induced freezing of the spray droplets before they evaporated in the cloud chamber. The other suspensions of living cells didn't induce any measurable ice concentration during spray formation at −5.7°. The remaining aerosol was exposed to typical cloud activation conditions in subsequent experiments with expansion cooling to about −11°C. During these experiments, the bacterial cells first acted as cloud condensation nuclei to form cloud droplets and then eventually acted as ice nuclei to freeze the droplets. 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 INA fraction of the order of 10−4. The ice nucleation efficiency of SnomaxTM cells was much larger with an INA fraction of 0.2 at temperatures around −8°C.

  20. 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.

  1. 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.

  2. High saturated fatty acids proportion in Escherichia coli enhances the activity of ice-nucleation protein from Pantoea ananatis.

    Science.gov (United States)

    Yu, Feifei; Liu, Xiping; Tao, Yong; Zhu, Kun

    2013-08-01

    The ice-nucleation protein (INP) from Pantoea ananatis was expressed in Escherichia coli. INP expression increased the freezing point of the E. coli culture by a few degrees. Deletion of FabH, an important enzyme in fatty acid biosynthesis, significantly inhibited the ice-nucleation activity. Increased unsaturated fatty acids in the fabH mutant cells decreased the ice-nucleation activity. Adding exogenous saturated fatty acids increased both E. coli fatty acid saturation and the ice-nucleation activity. In contrast, adding unsaturated fatty acids exhibited the opposite effects. Furthermore, an E. coli MG1655-fadR strain with high saturated fatty acids content was constructed, in which the INP activity was enhanced by about 17% compared with its activity in the wild-type MG1655 strain.

  3. 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.

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

    Directory of Open Access Journals (Sweden)

    O. Möhler

    2008-10-01

    Full Text Available The ice nucleation activities of five different Pseudomonas syringae, Pseudomonas viridiflava and Erwinia herbicola bacterial species and of Snomax™ were investigated in the temperature range between −5 and −15°C. Water suspensions of these bacteria were directly sprayed into the cloud chamber of the AIDA facility of Forschungszentrum Karlsruhe at a temperature of −5.7°C. At this temperature, about 1% of the Snomax™ cells induced immersion freezing of the spray droplets before the droplets evaporated in the cloud chamber. The living cells didn't induce any detectable immersion freezing in the spray droplets at −5.7°C. After evaporation of the spray droplets the bacterial cells remained as aerosol particles in the cloud chamber and were exposed to typical cloud formation conditions in experiments with expansion cooling to about −11°C. During these experiments, the bacterial cells first acted as cloud condensation nuclei to form cloud droplets. Then, only a minor fraction of the cells acted as heterogeneous ice nuclei either in the condensation or the immersion mode. The results indicate that the bacteria investigated in the present study are mainly ice active in the temperature range between −7 and −11°C with an ice nucleation (IN active fraction of the order of 10−4. In agreement to previous literature results, the ice nucleation efficiency of Snomax™ cells was much larger with an IN active fraction of 0.2 at temperatures around −8°C.

  5. Novel dimeric β-helical model of an ice nucleation protein with bridged active sites

    Directory of Open Access Journals (Sweden)

    Walker Virginia K

    2011-09-01

    Full Text Available Abstract Background Ice nucleation proteins (INPs allow water to freeze at high subzero temperatures. Due to their large size (>120 kDa, membrane association, and tendency to aggregate, an experimentally-determined tertiary structure of an INP has yet to be reported. How they function at the molecular level therefore remains unknown. Results Here we have predicted a novel β-helical fold for the INP produced by the bacterium Pseudomonas borealis. The protein uses internal serine and glutamine ladders for stabilization and is predicted to dimerize via the burying of a solvent-exposed tyrosine ladder to make an intimate hydrophobic contact along the dimerization interface. The manner in which PbINP dimerizes also allows for its multimerization, which could explain the aggregation-dependence of INP activity. Both sides of the PbINP structure have tandem arrays of amino acids that can organize waters into the ice-like clathrate structures seen on antifreeze proteins. Conclusions Dimerization dramatically increases the 'ice-active' surface area of the protein by doubling its width, increasing its length, and presenting identical ice-forming surfaces on both sides of the protein. We suggest that this allows sufficient anchored clathrate waters to align on the INP surface to nucleate freezing. As PbINP is highly similar to all known bacterial INPs, we predict its fold and mechanism of action will apply to these other INPs.

  6. Microbial ice-nucleators in cloud water at the puy de Dôme (France)

    Science.gov (United States)

    Joly, Muriel; Amato, Pierre; Deguillaume, Laurent; Attard, Eleonore; Sancelme, Martine; Monier, Marie; Morris, Cindy E.; Delort, Anne-Marie

    2013-04-01

    Ice nucleation active (INA) biological particles, in particular microorganisms, were studied in cloud water. Twelve cloud samples were collected over a period of 16 months from the puy de Dôme summit (1465 m, France) using sterile cloud droplet impactors. The samples were characterized through biological (cultures, cell counts) and physico-chemical measurements (pH, ion concentrations, carbon content…), and biological ice nuclei were investigated by droplet-freezing assays from -3°C to -13°C. The concentration of total INA particles within this temperature range typically varied from ~1 to ~100 per mL of cloud water; the concentrations of biological IN were several orders of magnitude higher than the values previously reported for precipitations. At -12°C, at least 76% of the IN were biological in origin, i.e. they were inactivated by heating at 95°C, and at temperatures above -8°C only biological material could induce ice. By culture, 44 Pseudomonas-like strains of bacteria were isolated from cloud water samples; 16% of them were found INA at the temperature of -8°C and they were identified as Pseudomonas syringae, Xanthomonas sp. and Pseudoxanthomonas sp.. Two strains induced freezing at as warm as -2°C, positioning them among the most active ice nucleators described so far. We estimated that, in average, 0.18% and more than 1% of the bacterial cells present in clouds (~104 mL-1) are INA at the temperatures of -8°C and -12°C, respectively. References: Attard E. et al. (2012) Effects of atmospheric conditions on ice nucleation activity of Pseudomonas. Atmospheric Chemistry and Physics Discussion 12, 9491-9516. Joly M. et al. Ice nucleation activity of bacteria isolated from cloud water, accepted in Atmospheric Environment. Vaïtilingom M. et al. (2012) Long-term features of cloud microbiology at the Puy de Dôme (France). Atmospheric Environment 56, 88-100.

  7. 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.

  8. Laboratory investigations of mixed organic/inorganic particles: Ice nucleation and optical hygroscopic growth

    Science.gov (United States)

    Beaver, Melinda R.

    The interactions of ambient aerosol particles with the atmosphere influence global climate and local visibility. Many of these atmospheric interactions are determined by the chemical composition of the aerosol particles. Ice nucleation in the upper troposphere is influenced and modified by the presence of anthropogenic aerosol particles. Also, interactions between particles and solar radiation are influenced by hygroscopic growth upon humidification. This thesis contains laboratory investigations into the role organic compounds play in ice nucleation and optical hygroscopic growth. Using an aerosol flow tube apparatus, we have studied the effects of aliphatic aldehydes (C3 to C10) and ketones (C 3 and C9) on ice nucleation in sulfuric acid aerosols. No acid-catalyzed reactions were observed under these conditions, and physical uptake was responsible for the organic content of the sulfuric acid aerosols. 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. Light extinction by atmospheric particles is strongly dependent on the size, chemical composition, and water content of the aerosol. Since light extinction by particles directly impacts climate and visibility, measurements of

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

    Science.gov (United States)

    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

  10. Ice nucleation activity in Pantoea ananatis obtained from maize white spot lesions

    Directory of Open Access Journals (Sweden)

    Aline Vanessa Sauer

    2014-09-01

    Full Text Available Maize white spot lesions caused by Pantoea ananatis has contributed substantially to yield reduction of maize crops in many countries, including Brazil. The initial symptoms of the disease include water-soaked lesions on the leaves, which later become necrotic and straw-colored. Basic knowledge regarding the biology and the infection mechanisms of this pathogen is lacking. In this study, 15 P. ananatis isolates obtained from maize white spot lesions were examined for their ice nucleation activity (INA. The INAs of individual bacterial isolates was determined by tube nucleation tests. Bacterial isolates were grown on tryptic soy broth medium and an aliquot of 0.1 mL of culture was added to test tubes containing 1 mL of sterile distilled water. The tubes were packed in an ice bath, which had a temperature below –10°C, for approximately 2 min. Instantaneous formation of ice in the tube revealed a positive INA phenotype of the isolate. Only 9 of the 15 studied isolates showed the INA+ phenotype. Pathogenicity tests were performed using whole plants and detached leaves. Symptoms were reproduced in both tests, but only for the inoculations using INA+ isolates. Electron microscopy allowed visualization of protein vesicles under outer cell wall of isolates characterized as INA+.

  11. 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

  12. The effects of mineral dust particles, aerosol regeneration and ice nucleation parameterizations on clouds and precipitation

    Directory of Open Access Journals (Sweden)

    A. Teller

    2012-03-01

    Full Text Available This study focuses on the effects of aerosol particles on the formation of convective clouds and precipitation in the Eastern Mediterranean sea with a special emphasis on the role of mineral dust particles in these processes. We used a new detailed numerical cloud microphysics scheme that has been implemented in the Weather Research and Forecast (WRF model in order to study aerosol-cloud interaction in 3-D configuration based on realistic meteorological data. Using a number of case studies we tested the contribution of mineral dust particles and different ice nucleation parameterizations to precipitation development. In this study we also investigated the importance of recycled (regenerated aerosols that had been released to the atmosphere following the evaporation of cloud droplets.

    The results showed that increased aerosol concentration due to the presence of mineral dust enhanced the formation of ice crystals. The dynamic evolution of the cloud system sets the time periods and regions in which heavy or light precipitation occurred in the domain. The precipitation rate, the time and duration of precipitation were affected by the aerosol properties only at small area scales (with areas of about 20 km2. Changes of the ice nucleation scheme from ice supersaturation dependent parameterization to a recent approach of aerosol concentration and temperature dependent parameterization modified the ice crystals concentrations but did not affect the total precipitation in the domain. Aerosol regeneration modified the concentration of cloud droplets at cloud base by dynamic recirculation of the aerosols but also had only a minor effect on precipitation.

    The major conclusion from this study is that the effect of mineral dust particles on clouds and total precipitation is limited by the properties of the atmospheric dynamics and the only effect of aerosol on precipitation may come from significant increase in the concentration

  13. Heterogeneous Ice Nucleation During Ozonolysis of Organic Thin Films on Aqueous Solution Droplets

    Science.gov (United States)

    Wicks, G.; Cantrell, W.

    2005-12-01

    The mechanism by which ice is created affects cloud properties and processes. Although homogeneous ice nucleation is reasonably well understood, both experimentally and theoretically, heterogeneous ice nucleation is not. Since deep convection in the tropics lofts organic materials high into the atmosphere, it is important to achieve an understanding of heterogeneous nucleation by these materials and how it affects cirrus cloud formation. Sources of atmospheric organic compounds include combustion, biomass burning, emissions from vegetation, and sea spray which contains organic material from the ocean's surface. Fatty acids such as stearic acid and oleic acid are common organic constituents. The reaction of oleic acid with atmospheric ozone has recently become a model for understanding how atmospheric oxidation processes affect organic particles. Over the past six years, more than twenty publications have described reactive uptake coefficients, primary products, secondary reactions, mechanisms, and other aspects of this oxidation. With this background information in mind, we built an ozonolysis apparatus in tandem with a solution drop freezer to study the freezing point of 10-microliter, 0.25 M sodium chloride solution droplets coated with thin layers of 18-carbon fatty acids or alcohols. We determined the freezing points before and after ozonolysis for solution droplets coated with stearic acid, oleic acid, cis-13-octadecenoic acid, oleyl alcohol, and 1-octadecanol. During the experiments, temperature cycling was controlled by a computer-driven temperature controller. Results showed little change in mean freezing temperature before and after ozonolysis for all of the organic compounds studied except oleyl alcohol. The lack of a significant temperature change for oleic acid may be good news for atmospheric modelers since the well-studied reaction of ozone with oleic acid is known to give a complex mixture of products.

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

    Directory of Open Access Journals (Sweden)

    H. E. Ahern

    2006-10-01

    Full Text Available 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.

  15. 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.

  16. Controlling nucleation of monolayer WSe2 during metal-organic chemical vapor deposition growth

    Science.gov (United States)

    Eichfeld, Sarah M.; Oliveros Colon, Víctor; Nie, Yifan; Cho, Kyeongjae; Robinson, Joshua A.

    2016-06-01

    Tungsten diselenide (WSe2) is a semiconducting, two-dimensional (2D) material that has gained interest in the device community recently due to its electronic properties. The synthesis of atomically thin WSe2, however, is still in its infancy. In this work we elucidate the requirements for large selenium/tungsten precursor ratios and explain the effect of nucleation temperature on the synthesis of WSe2 via metal-organic chemical vapor deposition (MOCVD). The introduction of a nucleation-step prior to growth demonstrates that increasing nucleation temperature leads to a transition from a Volmer-Weber to Frank-van der Merwe growth mode. Additionally, the nucleation step prior to growth leads to an improvement of WSe2 layer coverage on the substrate. Finally, we note that the development of this two-step technique may allow for improved control and quality of 2D layers grown via CVD and MOCVD processes.

  17. Characterization of airborne ice-nucleation-active bacteria and bacterial fragments

    Science.gov (United States)

    Šantl-Temkiv, Tina; Sahyoun, Maher; Finster, Kai; Hartmann, Susan; Augustin-Bauditz, Stefanie; Stratmann, Frank; Wex, Heike; Clauss, Tina; Nielsen, Niels Woetmann; Sørensen, Jens Havskov; Korsholm, Ulrik Smith; Wick, Lukas Y.; Karlson, Ulrich Gosewinkel

    2015-05-01

    Some bacteria have the unique capacity of synthesising ice-nucleation-active (INA) proteins and exposing them at their outer membrane surface. As INA bacteria enter the atmosphere, they may impact the formation of clouds and precipitation. We studied members of airborne bacterial communities for their capacity to catalyse ice formation and we report on the excretion of INA proteins by airborne Pseudomonas sp. We also observed for the first time that INA biological fragments outer membrane vesicles and found that two isolates could do so. However, only very few INA vesicles were released per INA cell. Thus, the source of the submicron INA proteinaceous particles that we detected in the atmosphere remains to be elucidated.

  18. 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.

  19. 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.

  20. The effect of ultrasonic pre-treatment on nucleation density of chemical vapor deposition diamond

    Science.gov (United States)

    Tang, Chi; Ingram, David C.

    1995-11-01

    Using statistical design of experiments, the effect of ultrasonic pre-treatment on the nucleation density of diamond was studied. The parameters investigated included ultrasonic excitation power, concentration of diamond powder in water, duration of ultrasonic excitation, and duration of cleaning with water after ultrasonic excitation. Diamond films were deposited on silicon (100) substrates using microwave assisted plasma chemical vapor deposition. The nucleation density varied from 106 nuclei/cm2 to 109 nuclei/cm2. The results illustrated that the dominant effect in ultrasonic pre-treatment was seeding. Moreover, scratches caused by the seeds during the treatment enabled more seeds to be retained on the surface. Based on these results, an optimized ultrasonic pretreatment has been developed. The new procedure yields a uniform nucleation density of 109 nuclei/cm2 on silicon (100) substrates.

  1. Chemical and physical transformations of aluminosilicate clay minerals due to acid treatment and consequences for heterogeneous ice nucleation.

    Science.gov (United States)

    Sihvonen, Sarah K; Schill, Gregory P; Lyktey, Nicholas A; Veghte, Daniel P; Tolbert, Margaret A; Freedman, Miriam Arak

    2014-09-25

    Mineral dust aerosol is one of the largest contributors to global ice nuclei, but physical and chemical processing of dust during atmospheric transport can alter its ice nucleation activity. In particular, several recent studies have noted that sulfuric and nitric acids inhibit heterogeneous ice nucleation in the regime below liquid water saturation in aluminosilicate clay minerals. We have exposed kaolinite, KGa-1b and KGa-2, and montmorillonite, STx-1b and SWy-2, to aqueous sulfuric and nitric acid to determine the physical and chemical changes that are responsible for the observed deactivation. To characterize the changes to the samples upon acid treatment, we use X-ray diffraction, transmission electron microscopy, and inductively coupled plasma-atomic emission spectroscopy. We find that the reaction of kaolinite and montmorillonite with aqueous sulfuric acid results in the formation of hydrated aluminum sulfate. In addition, sulfuric and nitric acids induce large structural changes in montmorillonite. We additionally report the supersaturation with respect to ice required for the onset of ice nucleation for these acid-treated species. On the basis of lattice spacing arguments, we explain how the chemical and physical changes observed upon acid treatment could lead to the observed reduction in ice nucleation activity.

  2. Characterization of the ice nucleation activity of an airborne Penicillium species

    Science.gov (United States)

    Yordanova, Petya; Hill, Thomas C. J.; Pummer, Bernhard G.; Franc, Gary D.; Pöschl, Ulrich; Fröhlich-Nowoisky, Janine

    2016-04-01

    Microorganisms are ubiquitous both on and above the Earth. Several bacterial and fungal spe-cies are the focus of atmospheric studies due to their ability to trigger ice formation at high subzero temperatures. Thus, they have potential to modify cloud albedo, lifetime and precipita-tion, and ultimately the hydrological cycle. Several fungal strains have already been identified as possessing ice nucleation (IN) activity, and recent studies have shown that IN active fungi are present in the cultivable community of air and soil samples [1, 2]. However, the abundance, diversity, and sources of fungal ice nuclei in the atmosphere are still poorly characterized. In this study, fungal colonies obtained from air samples were screened for IN activity in the droplet-freezing assay described in Fröhlich-Nowoisky et al., 2015 [2]. Out of 128 tested iso-lates, two were found to catalyze ice formation at temperatures up to -4°C. By DNA analysis, both isolates were classified as Penicillium spp. The freezing activity of both was further char-acterized after different filtration, heat, and enzymatic treatments in the temperature range from -4°C to -15°C. Preliminary results show that a proteinaceous compound is responsible for the IN activity. Furthermore, ongoing experiments indicate that the activity is associated only with the hyphae. [1] Huffman, et al. (2013): Atmos. Chem. Phys., 13, 6151-6164. [2] Fröhlich-Nowoisky et al. (2015): Biogeosciences, 12: 1057-1071.

  3. 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.

  4. Gas hydrate fast nucleation from melting ice and quiescent growth along vertical heat transfer tube

    Institute of Scientific and Technical Information of China (English)

    XIE; Yingming; GUO; Kaihua; LIANG; Deqing; FAN; Shuanshi

    2005-01-01

    During the observation of HCFC141b gas hydrate growth processes outside a vertical heat transfer tube, two exciting phenomena were found: fast nucleation of gas hydrate from melting ice, and the spontaneous permeation of water into the guest phases along the surface of heat transfer tube to form gas hydrate continuously. These two phenomena were explained with Zhou & Sloan's hypothesis and the theory of surface free energy respectively, and a novel method of gas hydrate formation was presented--gas hydrate fast nucleation from melting ice and quiescent growth along heat transfer tube. There is no mechanic stirring in this method, the formed gas hydrates are compact, the ratio of unreacted interstitial water is little, which overcome the drawback of high energy cost and high ratio of unreacted interstitial water among the formed gas hydrates in the system with mechanic stirring. This finding will benefit the gas hydrate application technologies such as natural gas storage technology or cool storage technology with gas hydrate.

  5. 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.

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

    Science.gov (United States)

    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

  7. Probing ice clouds by broadband mid-infrared extinction spectroscopy: case studies from ice nucleation experiments in the AIDA aerosol and cloud chamber

    Directory of Open Access Journals (Sweden)

    R. Wagner

    2006-01-01

    Full Text Available Series of infrared extinction spectra of ice crystals were recorded in the 6000–800 cm−1 wavenumber regime during expansion cooling experiments in the large aerosol and cloud chamber AIDA of Forschungszentrum Karlsruhe. Either supercooled sulphuric acid solution droplets or dry mineral dust particles were added as seed aerosols to initiate ice formation after having established ice supersaturated conditions inside the chamber. The various ice nucleation runs were conducted at temperatures between 237 and 195 K, leading to median sizes of the nucleated ice particles of 1–15 µm. The measured infrared spectra were fitted with reference spectra from T-matrix calculations to retrieve the number concentration as well as the number size distribution of the generated ice clouds. The precise evaluation of the time-dependent ice particle number concentrations, i.e., the rates of new ice particle formation, is of particular importance to quantitatively analyse the ice nucleation experiments in terms of nucleation rates and ice activation spectra. The ice particles were modelled as finite circular cylinders with aspect ratios ranging from 0.5 to 3.0. Benefiting from the comprehensive diagnostic tools for the characterisation of ice clouds which are available at the AIDA facility, the infrared retrieval results with regard to the ice particle number concentration could be compared to independent measurements with various optical particle counters. This provided a unique chance to quantitatively assess potential errors or solution ambiguities in the retrieval procedure which mainly originate from the difficulty to find an appropriate shape representation for the aspherical particle habits of the ice crystals. Based on these inter-comparisons, we demonstrate that there is no standard retrieval approach which can be routinely applied to all different experimental scenarios. In particular, the concept to account for the asphericity of the ice crystals

  8. Investigating the discrepancy between wet-suspension and dry-dispersion derived ice nucleation efficiency of mineral particles

    Directory of Open Access Journals (Sweden)

    C. Emersic

    2015-01-01

    Full Text Available Cloud chamber investigations into ice nucleation by mineral particles were compared with results from cold stage droplet freezing experiments. Kaolinite, NX-illite, and K-feldspar were examined and K-feldspar was revealed to be the most ice active mineral particle sample, in agreement with recent cold stage studies. The ice nucleation efficiencies, as quantified using the ice active site density method, were found to be in agreement with previous studies for the lower temperatures; however, at higher temperatures the efficiency was consistently higher than those inferred from cold stage experiments. Numerical process modelling of cloud formation during the experiments, using the cold-stage-derived parameterisations to initiate the ice phase, revealed the cold-stage-derived parameterisations to consistently under predict the number of ice crystals relative to that observed. We suggest the reason for the underestimation of ice in the model is that the slope of the cold-stage-derived ice active site density vs temperature curves are too steep, which results in an underestimation of the number of ice crystals at higher temperatures during the expansion. These ice crystals suppress further freezing due to the Bergeron-Findeison process. Application of a coagulation model to the size distribution of mineral particles present in the suspensions as used in the cold-stage-derived parameterisations revealed that it is likely that the mineral particles coagulate in suspension, which either removes the particles from the drops by sedimentation or reduces the total particle surface area available for ice nucleation to take place. This is confirmed with measurements of colloidal suspensions. The implication is that the mineral particles may be more important than previously thought at high temperatures.

  9. Closure between ice-nucleating particle and ice crystal number concentrations in ice clouds embedded in Saharan dust: Lidar observation during the BACCHUS Cyprus 2015 campaign

    Science.gov (United States)

    Mamouri, Rodanthi-Elisavet; Ansmann, Albert; Bühl, Johannes; Engelmann, Ronny; Baars, Holger; Nisantzi, Argyro; Hadjimitsis, Diofantos; Atkinson, James; Kanji, Zamin; Vrekoussis, Michalis; Sciare, Jean; Mihalopoulos, Nikos

    2016-04-01

    For the first time, we compare ice-nucleating particle number concentration (INPC) derived from polarization lidar (Mamouri and Ansmann, 2015) with ice crystal number concentrations (ICNC) in ice cloud layers embedded in the observed Saharan dust layers (at heights above 6 km and corresponding temperatures from -20 to -40°C). ICNC is estimated from the respective cirrus extinction profiles obtained with the same polarization lidar in combination with Doppler lidar measurements of the ice crystal sedimentation speed from which the mean size of the crystals can be estimated. Good agreement between INPC and ICNC was obtained for two case studies of the BACCHUS Cyprus 2015 field campaign with focus on INPC profiling. The campaign was organized by the Cyprus Institute, Nicosia, where a lidar was deployed. Additionaly, observations of AERONET and EALINET Lidar stations during the BACCHUS Cyprus 2015 field campaign, performed by Cyprus University of Technology in Limassol. Both, INPC and ICNC were found in the range from 10-50 1/L. Lidar-derived INPC values were also compared with in-situ INPC measurements (Horizontal Ice Nucleation Chamber, HINC, ETH Zurich, deployed at Agia Marina, at 500 m a.s.l., 30 km west of the lidar site). Reasonable and partly good agreement (during dust events) was found between the two retrievals. The findings of these closure studies corroborate the applicability of available INPC parameterization schemes (DeMott et al., 2010, 2015) implemented in the lidar retrieval scheme, and more generally INPC profiling by using active remote sensing (at ground and in space with CALIPSO and EarthCARE lidars).

  10. Size-resolved measurements of ice-nucleating particles at six locations in North America and one in Europe

    Science.gov (United States)

    Mason, R. H.; Si, M.; Chou, C.; Irish, V. E.; Dickie, R.; Elizondo, P.; Wong, R.; Brintnell, M.; Elsasser, M.; Lassar, W. M.; Pierce, K. M.; Leaitch, W. R.; MacDonald, A. M.; Platt, A.; Toom-Sauntry, D.; Sarda-Estève, R.; Schiller, C. L.; Suski, K. J.; Hill, T. C. J.; Abbatt, J. P. D.; Huffman, J. A.; DeMott, P. J.; Bertram, A. K.

    2016-02-01

    Detailed information on the size of ice-nucleating particles (INPs) may be useful in source identification, modeling their transport in the atmosphere to improve climate predictions, and determining how effectively or ineffectively instrumentation used for quantifying INPs in the atmosphere captures the full INP population. In this study we report immersion-mode INP number concentrations as a function of size at six ground sites in North America and one in Europe using the micro-orifice uniform-deposit impactor droplet freezing technique (MOUDI-DFT), which combines particle size-segregation by inertial impaction and a microscope-based immersion freezing apparatus. The lowest INP number concentrations were observed at Arctic and alpine locations and the highest at suburban and agricultural locations, consistent with previous studies of INP concentrations in similar environments. We found that 91 ± 9, 79 ± 17, and 63 ± 21 % of INPs had an aerodynamic diameter > 1 µm at ice activation temperatures of -15, -20, and -25 °C, respectively, when averaging over all sampling locations. In addition, 62 ± 20, 55 ± 18, and 42 ± 17 % of INPs were in the coarse mode (> 2.5 µm) at ice activation temperatures of -15, -20, and -25 °C, respectively, when averaging over all sampling locations. These results are consistent with six out of the nine studies in the literature that have focused on the size distribution of INPs in the atmosphere. Taken together, these findings strongly suggest that supermicron and coarse-mode aerosol particles are a significant component of the INP population in many different ground-level environments. Further size-resolved studies of INPs as a function of altitude are required since the size distribution of INPs may be different at high altitudes due to size-dependent removal processes of atmospheric particles.

  11. Impact of Ice Nucleation Parameterization on CAM5 Simulated Arctic Clouds and Radiation: A Sensitivity Study

    Science.gov (United States)

    Xie, S.; Liu, X.; Zhao, C.; Zhang, Y.

    2012-12-01

    Sensitivity of Arctic clouds and radiation in the Community Atmospheric Model version 5 (CAM5) to ice nucleation parameterization is examined by testing a new and more physically based ice nucleation scheme that links the variation of ice nuclei (IN) number concentration to aerosol properties. The CAM5 default scheme parameterizes the IN number concentration simply as a function of ice supersaturation. The new scheme has led to a significant reduction in simulated IN number concentrations at all latitudes while changes in cloud and cloud properties are mainly seen in high latitudes and middle latitude storm tracks. In the Arctic region, there is a noticeable increase in mid- and high-level clouds and a decrease in low-level clouds. The smaller IN concentrations results in a considerable increase of cloud liquid water path and decrease of ice water path, which are likely related to the increase of optically intermediate and thick low- and middle-top clouds and the decrease of optically thin and intermediate high clouds, respectively. Overall, there is an increase of cloud optical depth of Arctic clouds, which leads to a stronger shortwave, longwave, and net cloud radiative forcing (cooling) at the top of the atmosphere. The comparison with satellite data indicates that the new scheme has slightly improved optically thin low cloud simulation, but produced too many optically thick middle and high clouds. A further comparison with Arctic ground-based measurements shows that the new scheme has led to a clearly better simulation of clouds and their properties, which helps reduce model errors in surface radiation. Uncertainties in these observations are discussed. Work at LLNL was performed under the auspices of the U. S. Department of Energy (DOE), Office of Science, Office of Biological and Environmental Research by Lawrence Livermore National Laboratory under contract No. DE-AC52-07NA27344. The Pacific Northwest National Laboratory (PNNL) is operated for the DOE by

  12. Application of an Online-Coupled Regional Climate Model, WRF-CAM5, over East Asia for Examination of Ice Nucleation Schemes: Part II. Sensitivity to Heterogeneous Ice Nucleation Parameterizations and Dust Emissions

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Yang; Chen, Ying; Fan, Jiwen; Leung, Lai-Yung

    2015-09-01

    Aerosol particles can affect cloud microphysical properties by serving as ice nuclei (IN). Large uncertainties exist in the ice nucleation parameterizations (INPs) used in current climate models. In this Part II paper, to examine the sensitivity of the model predictions to different heterogeneous INPs, WRF-CAM5 simulation using the INP of Niemand et al. (N12) [1] is conducted over East Asia for two full years, 2006 and 2011, and compared with simulation using the INP of Meyers et al. (M92) [2], which is the original INP used in CAM5. M92 calculates the nucleated ice particle concentration as a function of ice supersaturation, while N12 represents the nucleated ice particle concentration as a function of temperature and the number concentrations and surface areas of dust particles. Compared to M92, the WRF-CAM5 simulation with N12 produces significantly higher nucleated ice crystal number concentrations (ICNCs) in the northern domain where dust sources are located, leading to significantly higher cloud ice number and mass concentrations and ice water path, but the opposite is true in the southern domain where temperatures and moistures play a more important role in ice formation. Overall, the simulation with N12 gives lower downward shortwave radiation but higher downward longwave radiation, cloud liquid water path, cloud droplet number concentrations, and cloud optical depth. The increase in cloud optical depth and the decrease in downward solar flux result in a stronger shortwave and longwave cloud forcing, and decreases temperature at 2-m and precipitation. Changes in temperature and radiation lower surface concentrations of OH, O3, SO42-, and PM2.5, but increase surface concentrations of CO, NO2, and SO2 over most of the domain. By acting as cloud condensation nuclei (CCN) and IN, dust particles have different impacts on cloud water and ice number concentrations, radiation, and temperature at 2-m and

  13. Influence of Sweet Crude Oil on Nucleation and Corrosion Resistance of Calcareous Deposits

    Science.gov (United States)

    Hoseinieh, S. M.; Shahrabi, T.; Ramezanzadeh, B.; Farrokhi Rad, M.

    2016-11-01

    The influence of sweet crude oil on calcareous scale deposition under cathodic protection of carbon steel in artificial seawater was investigated using chronoamperometry, electrochemical impedance spectroscopy, scanning electron microscope/energy-dispersive spectroscopy, x-ray diffraction and Raman spectroscopy. In the presence of crude oil, calcareous deposit formation is influenced in terms of both kinetic and nucleation mostly in high volume concentrations. It is indicated that the CaCO3 deposition is hindered by absorption of active surface compounds present in oil on to the surface mainly due to strong covalent bonding of aromatic compounds.

  14. 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

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

    Directory of Open Access Journals (Sweden)

    C. M. Archuleta

    2005-01-01

    Full Text Available This study examines the potential role of some types of mineral dust and mineral dust with sulfuric acid coatings as heterogeneous ice nuclei at cirrus temperatures. Commercially-available nanoscale powder samples of aluminum oxide, alumina-silicate and iron oxide were used as surrogates for atmospheric mineral dust particles, with and without multilayer coverage of sulfuric acid. A sample of Asian dust aerosol particles was also studied. Measurements of ice nucleation were made using a continuous-flow ice-thermal diffusion chamber (CFDC operated to expose size-selected aerosol particles to temperatures between -45 and -60°C and a range of relative humidity above ice-saturated conditions. Pure metal oxide particles supported heterogeneous ice nucleation at lower relative humidities than those required to homogeneously freeze sulfuric acid solution particles at sizes larger than about 50 nm. The ice nucleation behavior of the same metal oxides coated with sulfuric acid indicate heterogeneous freezing at lower relative humidities than those calculated for homogeneous freezing of the diluted particle coatings. The effect of soluble coatings on the ice activation relative humidity varied with the respective uncoated core particle types, but for all types the heterogeneous freezing rates increased with particle size for the same thermodynamic conditions. For a selected size of 200 nm, the natural mineral dust particles were the most effective ice nuclei tested, supporting heterogeneous ice formation at an ice relative humidity of approximately 135%, irrespective of temperature. Modified homogeneous freezing parameterizations and theoretical formulations are shown to have application to the description of heterogeneous freezing of mineral dust-like particles with soluble coatings.

  16. Nucleation and growth of chemically vapor deposited tungsten on various substrate materials: A review

    Energy Technology Data Exchange (ETDEWEB)

    Broadbent, E.K.

    1987-11-01

    W films produced by chemical-vapor deposition (CVD), typically via reduction of WF/sub 6/, are being used for numerous applications in very large scale integrated circuit technology. Blanket and selectively deposited films require nucleation and growth on a specific underlayer material: Si, metal, or metal silicide. The compatibility of CVD W with various underlayers is reviewed for the device applications of contact/via fill, diffusion barrier, metal interconnect, and source/drain coating. Nucleation of W directly on single crystal Si can sometimes produce tunnel-defect structures at the edges or along the entire interface of the deposit. Sputtered Mo and W, and to some extent TiW and TiN, have been shown to be suitable nucleation layers for CVD W, yielding a fluorine-free interface with low-electrical contact resistance. A sputtered W/Ti adhesion bilayer is demonstrated for a blanket W deposition+etchback process. CoSi/sub 2/ appears an appropriate choice where CVD W and salicide technologies are combined.

  17. Nucleation and growth of single layer graphene on electrodeposited Cu by cold wall chemical vapor deposition

    Science.gov (United States)

    Das, Shantanu; Drucker, Jeff

    2017-03-01

    The nucleation density and average size of graphene crystallites grown using cold wall chemical vapor deposition (CVD) on 4 μm thick Cu films electrodeposited on W substrates can be tuned by varying growth parameters. Growth at a fixed substrate temperature of 1000 °C and total pressure of 700 Torr using Ar, H2 and CH4 mixtures enabled the contribution of total flow rate, CH4:H2 ratio and dilution of the CH4/H2 mixture by Ar to be identified. The largest variation in nucleation density was obtained by varying the CH4:H2 ratio. The observed morphological changes are analogous to those that would be expected if the deposition rate were varied at fixed substrate temperature for physical deposition using thermal evaporation. The graphene crystallite boundary morphology progresses from irregular/jagged through convex hexagonal to regular hexagonal as the effective C deposition rate decreases. This observation suggests that edge diffusion of C atoms along the crystallite boundaries, in addition to H2 etching, may contribute to shape evolution of the graphene crystallites. These results demonstrate that graphene grown using cold wall CVD follows a nucleation and growth mechanism similar to hot wall CVD. As a consequence, the vast knowledge base relevant to hot wall CVD may be exploited for graphene synthesis by the industrially preferable cold wall method.

  18. Ice nucleation and its effect on the atmospheric transport of fungal spores from the classes Agaricomycetes, Ustilaginomycetes, and Eurotiomycetes

    Science.gov (United States)

    Haga, D. I.; Burrows, S. M.; Iannone, R.; Wheeler, M. J.; Mason, R.; Chen, J.; Polishchuk, E. A.; Pöschl, U.; Bertram, A. K.

    2014-02-01

    Ice nucleation on fungal spores may affect the frequency and properties of ice and mixed-phase clouds. We studied the ice nucleation properties of 12 different species of fungal spores chosen from three classes: Agaricomycetes, Ustilaginomycetes, and Eurotiomycetes. Agaricomycetes include many types of mushroom species and are cosmopolitan. Ustilaginomycetes are agricultural pathogens and have caused widespread damage to crops. Eurotiomycetes are found on all types of decaying material and include important human allergens. We focused on these classes since they are thought to be abundant in the atmosphere and because there is very little information on the ice nucleation ability of these classes of spores in the literature. All of the fungal spores investigated were found to cause freezing of water droplets at temperatures warmer than homogeneous freezing. The cumulative number of ice nuclei per spore was 0.001 at temperatures between -19 °C and -29 °C, 0.01 between -25.5 °C and -31 °C, and 0.1 between -26 °C and -36 °C. On average, the order of ice nucleating ability for these spores is Ustilaginomycetes > Agaricomycetes ≃ Eurotiomycetes. We show that at temperatures below -20 °C, all of the fungal spores studied here are less efficient ice nuclei compared to Asian mineral dust on a per surface area basis. We used our new freezing results together with data in the literature to compare the freezing temperatures of spores from the phyla Basidiomycota and Ascomycota, which together make up 98% of known fungal species found on Earth. The data show that within both phyla (Ascomycota and Basidiomycota) there is a wide range of freezing properties, and also that the variation within a phylum is greater than the variation between the average freezing properties of the phyla. Using a global chemistry-climate transport model, we investigated whether ice nucleation on the studied spores, followed by precipitation, can influence the atmospheric transport and

  19. Clues that decaying leaves enrich Arctic air with ice nucleating particles

    Science.gov (United States)

    Conen, Franz; Stopelli, Emiliano; Zimmermann, Lukas

    2016-03-01

    Decaying leaves from Arctic regions have previously been reported to produce large numbers of ice nucleating particles (IN). Their atmospheric relevance is unclear. Our initial observations at a coastal mountain observatory in northern Norway reveal a tripling in concentrations of IN active at -15 °C (IN-15) in oceanic air after about one day of passage over land (from 1.7 and 4.9 IN-15 m-3, to 9.6 and 12.2 IN-15 m-3). Analysis of leaf litter collected near the observatory supports the earlier report of numerous IN associated with leaf litter on the ground (2 ṡ 102 IN-15 μg-1 litter particles decaying leaves are a strong emission source of IN to the Arctic boundary layer.

  20. Impacts from ice-nucleating bacteria on deep convection: implications for the biosphere-atmosphere interaction in climate change

    Directory of Open Access Journals (Sweden)

    V. T. J. Phillips

    2008-03-01

    Full Text Available A cloud modeling framework is described to simulate ice nucleation by biogenic aerosol particles, as represented by airborne ice-nucleation active (INA bacteria. It includes the empirical parameterization of heterogeneous ice nucleation. The formation of cloud liquid by soluble material coated on such insoluble aerosols is represented and determines their partial removal from deep convective clouds by accretion onto precipitation.

    Preliminary simulations are performed for a case of deep convection over Oklahoma. If present at high enough concentrations, as might occur in proximity to land sources, INA bacteria are found to influence significantly: – (1 the average numbers and sizes of crystals in the clouds; (2 the horizontal cloud coverage in the free troposphere; and (3 precipitation and incident solar insolation at the surface, which influence rates of bacterial growth. At lower concentrations, the corresponding responses of cloud fields appear much lower or are ambiguous.

    In nature, the growth rates of INA bacteria on leaves prior to emission into the atmosphere are known to be highly dependent on temperature, precipitation and plant species. Consequently, the open question emerges of whether emissions of such ice-nucleating biogenic particles can then be modified by their own effects on clouds and atmospheric conditions, forming a weak feedback in climate or microclimate systems.

  1. Surface Display of Domain Ⅲ of Japanese Encephalitis Virus E Protein on Salmonella Typhimurium by Using an Ice Nucleation Protein

    Institute of Scientific and Technical Information of China (English)

    Jian-lin Dou; Tao Jing; Jing-jing Fan; Zhi-ming Yuan

    2011-01-01

    A bacterial cell surface display technique based on an ice nucleation protein has been employed for the development of live vaccine against viral infection.Due to its ubiquitous ability to invade host cells,Salmonella typhimurium might be a good candidate for displaying viral antigens.We demonstrated the surface display of domain III of Japanese encephalitis virus E protein and the enhanced green fluorescent protein on S.typhimurium BRD509 using the ice nucleation protein.The effects of the motif in the ice nucleation protein on the effective display of integral protein were also investigated.The results showed that display motifs in the protein can target integral foreign protein on the surface of S.typhimurium BRD509.Moreover,recombinant strains with surface displayed viral proteins retained their invasiveness,suggesting that the recombinant S.typhimurium can be used as live vaccine vector for eliciting complete immunogenicity.The data may yield better understanding of the mechanism by which ice nucleation protein displays foreign proteins in the Salmonella strain.

  2. Sea ice dynamics influence halogen deposition to Svalbard

    Directory of Open Access Journals (Sweden)

    A. Spolaor

    2013-03-01

    Full Text Available Sea ice is an important parameter in the climate system and its changes impact upon the polar albedo and the atmospheric and oceanic circulation. Iodine (I and bromine (Br have been measured in a shallow ice core drilled at the summit of the Holtedahlfonna glacier (Northwest Spitsbergen, Svalbard. Changing I concentrations can be linked to the spring 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 spring sea ice coincides with enlargement of the open ocean surface which enhances marine primary production and consequent I emission. The observed Br enrichment can be explained by greater Br emissions during the Br explosion that have been observed to occur 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.

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

    Directory of Open Access Journals (Sweden)

    P. Amato

    2015-02-01

    Full Text Available 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 lacks 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 per m2 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.

  4. Quantification of summertime water ice deposition on the Martian north polar ice cap

    CERN Document Server

    Brown, Adrian J; Becerra, Patricio; Byrne, Shane

    2015-01-01

    We use observations from the Compact Reconnaissance Imaging Spectrometer for Mars (CRISM) of the north polar cap during late summer for two Martian years, to monitor the complete summer cycle of albedo and water ice grain size in order to place quantitative limits of the amount of water ice deposited in late summer. We establish here for the first time the complete spring to summer cycle of water ice grain sizes on the north polar cap. The apparent grain sizes grow until Ls=132, when they appear to shrink again, until they are obscured at the end of summer by the north polar hood. Under the assumption that the shrinking of grain sizes is due to the deposition of find grained ice, we quantify the amount of water ice deposited per Martian boreal summer, and estimate the amount of water ice that must be transported equatorward. Interestingly, we find that the relative amount of water ice deposited in the north cap during boreal summer (0.7-7 microns) is roughly equivalent to the average amount of water ice depos...

  5. Local order parameters for use in driving homogeneous ice nucleation with all-atom models of water.

    Science.gov (United States)

    Reinhardt, Aleks; Doye, Jonathan P K; Noya, Eva G; Vega, Carlos

    2012-11-21

    We present a local order parameter based on the standard Steinhardt-Ten Wolde approach that is capable both of tracking and of driving homogeneous ice nucleation in simulations of all-atom models of water. We demonstrate that it is capable of forcing the growth of ice nuclei in supercooled liquid water simulated using the TIP4P/2005 model using over-biassed umbrella sampling Monte Carlo simulations. However, even with such an order parameter, the dynamics of ice growth in deeply supercooled liquid water in all-atom models of water are shown to be very slow, and so the computation of free energy landscapes and nucleation rates remains extremely challenging.

  6. 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.

  7. Sea ice dynamics influence halogen deposition to Svalbard

    Directory of Open Access Journals (Sweden)

    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.

  8. 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

  9. An ice age recorded in the polar deposits of Mars.

    Science.gov (United States)

    Smith, Isaac B; Putzig, Nathaniel E; Holt, John W; Phillips, Roger J

    2016-05-27

    Layered ice deposits at the poles of Mars record a detailed history of accumulation and erosion related to climate processes. Radar investigations measure these layers and provide evidence for climate changes such as ice advance and retreat. We present a detailed analysis of observational data showing that ~87,000 cubic kilometers of ice have accumulated at the poles since the end of the last ice age ~370,000 years ago; this volume is equivalent to a global layer of ~60 centimeters. The majority of the material accumulated at the north pole. These results provide both a means to understand the accumulation history of the polar deposits as related to orbital Milankovitch cycles and constraints for better determination of Mars' past and future climates.

  10. An ice age recorded in the polar deposits of Mars

    Science.gov (United States)

    Smith, Isaac B.; Putzig, Nathaniel E.; Holt, John W.; Phillips, Roger J.

    2016-05-01

    Layered ice deposits at the poles of Mars record a detailed history of accumulation and erosion related to climate processes. Radar investigations measure these layers and provide evidence for climate changes such as ice advance and retreat. We present a detailed analysis of observational data showing that ~87,000 cubic kilometers of ice have accumulated at the poles since the end of the last ice age ~370,000 years ago; this volume is equivalent to a global layer of ~60 centimeters. The majority of the material accumulated at the north pole. These results provide both a means to understand the accumulation history of the polar deposits as related to orbital Milankovitch cycles and constraints for better determination of Mars’ past and future climates.

  11. Ice nucleation of ice thermal storage air-condition%冰蓄冷空调蓄冰成核

    Institute of Scientific and Technical Information of China (English)

    章学来; 孟祥来; 赵群志; 李春蕾

    2014-01-01

    Experiment on different depth of water tank supercooling degree was carried out. The results show that the supercooling degree of the upper water in ice storage tank is higher. In order to reduce the supercooling degree of the water and energy consumption of the chiller, different nucleation additives are tested and it is found that adding nano-copper oxide can reduce the supercooling degree and improve the ice storage efficiency. Appropriate mass fraction of copper oxide nanoparticles is obtained under a certain quality dispersant. When the ice-making temperature is-5℃,0.10% mass fraction copper oxide suspension is at the top. Supercooling degree of water is also associated with the temperature difference of heat transfer medium. The higher the difference in temperature is, the smaller the supercooling degree.%在对内融冰式蓄冰槽内不同水层的水进行过冷度测试中发现上层水的过冷度较大。为了降低水的过冷度和冷水机组能耗,通过实验的方法对不同的成核添加剂进行筛选测试,结果显示纳米氧化铜不但在降低过冷度方面效果显著,而且提高了蓄冰效率。最后获取了一定质量分散剂下最佳纳米氧化铜的质量分数,即在-5℃的制冰温度下,质量分数为0.10%的氧化铜悬浊液为最佳配比。在实验过程中发现水的过冷度还与换热介质的传热温差有关,温差越大过冷度越小。

  12. Laboratory studies with cloud-derived Bacterial Cells acting as Ice Nuclei in the Immersion and Deposition Mode

    Science.gov (United States)

    Oehm, C.; Chou, C.; Amato, P.; Attard, E.; Delort, A.-M.; Morris, C.; Kiselev, A.; Stetzer, O.; Möhler, O.; Leisner, T.

    2012-04-01

    Atmospheric aerosol particles play an important role in cloud microphysics. Aerosols of biological origin are a subgroup, and some of them are able to act as heterogeneous ice nuclei and thus influence cloud life cycles and the climate. Some bacteria species have been found to act as ice nuclei at relatively high temperatures up to -2 degree Celsius and are therefore of particular importance as "high temperature" ice nuclei. Recently, ice nucleation experiments with bacterial cells from different sources were performed at the aerosol and cloud simulation chamber AIDA at the Karlsruhe Institute of Technology. At the AIDA facility, microphysical cloud processes can be simulated and investigated in laboratory at realistic atmospheric cloud conditions. Different ice nucleation active (INA) bacteria strains were isolated from cloud water, glacier melt water and phyllosphere and examined in AIDA experiments. The living cells were suspended in nanopure or artificial cloud water and injected into the cloud chamber through a dispersion nozzle. The injected droplets evaporated in the chamber and the bacterial cells were transformed into the aerosol phase. After the spraying, the cloud formation was started by expansion cooling. Experiments were performed in the temperature range from -2 down to -20 degree Celsius. Detailed measurements of the number concentration and size distribution of the aerosol particles as well as of the droplets and ice particles were carried out during the AIDA experiments. A minor fraction of the bacteria cells was observed to act as ice nuclei in the immersion nucleation mode at higher temperatures as well as in the deposition nucleation mode at lower temperatures. The ice activity started at -6 degree Celsius. The most efficient INA bacteria species were Pseudomonas syringae 32b74 and Pseudomonas fluorescens Antarctica1. The ice active number fraction with respect to the cells varied from 0,01 to 0,1, and it does not change at different

  13. Pre-ordering of interfacial water in the pathway of heterogeneous ice nucleation does not lead to a two-step crystallization mechanism

    Science.gov (United States)

    Lupi, Laura; Peters, Baron; Molinero, Valeria

    2016-12-01

    According to Classical Nucleation Theory (CNT), the transition from liquid to crystal occurs in a single activated step with a transition state controlled by the size of the crystal embryo. This picture has been challenged in the last two decades by several reports of two-step crystallization processes in which the liquid first produces pre-ordered or dense domains, within which the crystal nucleates in a second step. Pre-ordering preceding crystal nucleation has been recently reported in simulations of ice crystallization, raising the question of whether the mechanism of ice nucleation involves two steps. In this paper, we investigate the heterogeneous nucleation of ice on carbon surfaces. We use molecular simulations with efficient coarse-grained models combined with rare event sampling methods and free energy calculations to elucidate the role of pre-ordering of liquid water at the carbon surface in the reaction coordinate for heterogeneous nucleation. We find that ice nucleation proceeds through a classical mechanism, with a single barrier between liquid and crystal. The reaction coordinate that determines the crossing of the nucleation barrier is the size of the crystal nucleus, as predicted by CNT. Wetting of the critical ice nuclei within pre-ordered domains decreases the nucleation barrier, increasing the nucleation rates. The preferential pathway for crystallization involves the early creation of pre-ordered domains that are the birthplace of the ice crystallites but do not represent a minimum in the free energy pathway from liquid to ice. We conclude that a preferential pathway through an intermediate-order precursor does not necessarily result in a two-step mechanism.

  14. Prokaryotic expression of iceA gene from ice nucleation active bacteria Erwinia ananas 110 and analysis of ice nucleation activity%冰核细菌Erwinia ananas 110冰核基因iceA的原核表达及冰核活性分析

    Institute of Scientific and Technical Information of China (English)

    姚润贤; 袁哲明

    2013-01-01

    To obtain recombinant strain with high ice nucleation activity,iceA gene were amplified by PCR from ice nucleation active bacteria Erwinia ananas 110 and cloned into vector pMD19-T which was transformed into E.coli DH5α.The recombinant clones were screened by single and double digestion before sequenced.From the positive recombinant strain,iceA gene was subcloned into prokaryotic expression vector pET-23a(+),resulting in recombinant plasmid pET-23a(+)-ice which was transformed into E.coli BL21(DE3)pLysS and induced by IPTG.SDS-PAGE indicated that ice nucleation active protein was expressed as inclusion bodies with molecular weight of about 180 000.Ice nucleation activity test showed there was no difference in ice nucleation activity under-5,4,-3,and-2 ℃ between recombinant E.coli BL21(DE3)pLysS and wild ice nucleation active bacteria Erwinia ananas 110.%为获得具有高冰核活性的基因工程菌,从冰核细菌Erwinia ananas 110扩增冰核基因iceA,将其克隆到pMD 19-T载体上,转化大肠杆菌DH5α,单、双酶切鉴定并测序;阳性克隆目的片段亚克隆到表达载体pET-23a(+)上,转化大肠杆菌DH5αt,单、双酶切鉴定重组质粒;阳性重组质粒转化大肠杆菌BL21(DE3)pLysS,并经IPTG诱导表达.SDS-PAGE电泳检测表明,冰核基因iceA能够并以包涵体形式表达,相对分子质量约为180 000.冰核活性测定结果表明,重组菌BL21 (DE3)pLysS/pET-ice的冰核活性与野生冰核细菌Erwinia ananas 110在-5、-4、-3、-2℃下无明显差别.

  15. Ice-nucleating particles in Canadian Arctic sea-surface microlayer and bulk seawater

    Science.gov (United States)

    Irish, Victoria E.; Elizondo, Pablo; Chen, Jessie; Chou, Cédric; Charette, Joannie; Lizotte, Martine; Ladino, Luis A.; Wilson, Theodore W.; Gosselin, Michel; Murray, Benjamin J.; Polishchuk, Elena; Abbatt, Jonathan P. D.; Miller, Lisa A.; Bertram, Allan K.

    2017-09-01

    The sea-surface microlayer and bulk seawater can contain ice-nucleating particles (INPs) and these INPs can be emitted into the atmosphere. Our current understanding of the properties, concentrations, and spatial and temporal distributions of INPs in the microlayer and bulk seawater is limited. In this study we investigate the concentrations and properties of INPs in microlayer and bulk seawater samples collected in the Canadian Arctic during the summer of 2014. INPs were ubiquitous in the microlayer and bulk seawater with freezing temperatures in the immersion mode as high as -14 °C. A strong negative correlation (R = -0. 7, p = 0. 02) was observed between salinity and freezing temperatures (after correction for freezing depression by the salts). One possible explanation is that INPs were associated with melting sea ice. Heat and filtration treatments of the samples show that the INPs were likely heat-labile biological materials with sizes between 0.02 and 0.2 µm in diameter, consistent with previous measurements off the coast of North America and near Greenland in the Arctic. The concentrations of INPs in the microlayer and bulk seawater were consistent with previous measurements at several other locations off the coast of North America. However, our average microlayer concentration was lower than previous observations made near Greenland in the Arctic. This difference could not be explained by chlorophyll a concentrations derived from satellite measurements. In addition, previous studies found significant INP enrichment in the microlayer, relative to bulk seawater, which we did not observe in this study. While further studies are needed to understand these differences, we confirm that there is a source of INP in the microlayer and bulk seawater in the Canadian Arctic that may be important for atmospheric INP concentrations.

  16. The ice nucleation ability of one of the most abundant types of fungal spores found in the atmosphere

    Directory of Open Access Journals (Sweden)

    R. Iannone

    2011-02-01

    Full Text Available Recent atmospheric measurements show that biological particles are a potentially important class of ice nuclei. Types of biological particles that may be good ice nuclei include bacteria, pollen and fungal spores. We studied the ice nucleation properties of water droplets containing fungal spores from the genus Cladosporium, one of the most abundant types of spores found in the atmosphere. For water droplets containing a Cladosporium spore surface area of ~217 μm2 (equivalent to ~5 spores with average diameters of 3.2 μm , 1% of the droplets froze by −28.5 °C and 10% froze by –30.1 °C. However, there was a strong dependence on freezing temperature with the spore surface area of Cladosporium within a given droplet. Mean freezing temperatures for droplets containing 1–5 spores are expected to be approximately −35.1 ± 2.3 °C (1σ S. D.. Atmospheric ice nucleation on spores of Cladosporium sp., or other spores with similar surface properties, thus do not appear to explain recent atmospheric measurements showing that biological particles participate as atmospheric ice nuclei. The poor ice nucleation ability of Cladosporium sp. may be attributed to the surface which is coated with hydrophobins (a class of hydrophobic proteins that appear to be widespread in filamentous fungi. Given the ubiquity of hydrophobins on spore surfaces, the current study may be applicable to many fungal species of atmospheric importance.

  17. Thin film deposition of diamond using normal paraffins as source of diamond nucleation centers

    Energy Technology Data Exchange (ETDEWEB)

    Ershova, A., E-mail: ershovaangelina@mail.ru [Nano-Technology Laboratory, Triangle Inc., 01079 (Ukraine); Eizenbraun, A. [Nano-Technology Laboratory, Triangle Inc., 01079 (Ukraine)

    2012-11-15

    Highlights: ► Paraffin compounds are diamond nucleation sources. ► Thermoconductivity of Cu–DTF device is higher than such conductivity of Cu. ► DTF growth in HFCVD reactor is not linear function of time. -- Abstract: We propose a process for diamond thin film (DTF) deposition using normal paraffins (nP) as source of diamond nucleation centers. We deposited micro-crystalline diamond thin films (MCDTF) on a Cu substrate using Hot Filament CVD (HFCVD) and Passive Pt/Pd Surface Catalysis (PPt/PdSC) methods. Beeswax and a 1:1 mixture of normal paraffins of the general formula CH{sub 3}(CH{sub 2}){sub n}CH{sub 3} with n = 22 and 26 were tested as nP starting material. The films obtained were characterized by scanning electronic microscopy (SEM), Raman scattering temperature dependent spectroscopy and X-ray diffraction (XRD) methods, all of which confirmed that the deposited material is MCDTF.

  18. Multispectral comparison of water ice deposits observed on cometary nuclei

    Science.gov (United States)

    Oklay Vincent, Nilda; Sunshine, Jessica M.; Pajola, Maurizio; Pommerol, Antoine; Vincent, Jean-Baptiste; Sierks, Holger; OSIRIS Team

    2016-10-01

    Cometary missions Deep Impact, EPOXI and Rosetta investigated the nuclei of comets 9P/Tempel 1, 103P/Hartley 2 and 67P/Churyumov-Gerasimenko respectively. Each of these three missions was equipped with multispectral cameras, allowing imaging at various wavelengths from NUV to NIR. In this spectral range, water ice-rich features display bluer spectral slopes than the average surface and some have very flat spectra. Features enriched in water ice are bright in the monochromatic images and are blue in the RGB color composites generated by using images taken in NUV, visible and NIR wavelentghs. Using these properties, water ice-rich features were detected on the nuclei of comets 9P [1], 103P [2] and 67P [3] via multispectral imaging cameras. Moreover, there were visual detections of jets and outbursts associated to some of these water ice-rich features when the right observing conditions were fulfilled [4, 5].We analyzed multispectral properties of different types of water ice-rich features [3] observed via OSIRIS NAC on comet 67P in the wavelength range of 260 nm to 1000 nm and then compared with those observed on comets 9P and 103P. Our multispectral analysis shows that the water ice deposits observed on comet 9P are very similar to the large bright blue clusters observed on comet 67P, while the large water ice deposit observed on comet 103P is similar to the large isolated water ice-rich features observed on comet 67P. The ice-rich deposits on comet 103P are the bluest of any comet, which indicates that the deposits on 103P contain more water ice than the ones observed on comets 9P and 67P [6].[1] Sunshine et al 2006, Science[2] Sunshine et al 2011, LPSC[3] Pommerol et al 2015, A&A[4] Oklay et al 2016, A&A[5] Vincent et al 2016, A&A[6] Oklay et al 2016, submitted

  19. Key factors for causing poplar Ice Nucleation Active bacterial canker and its control techniques

    Institute of Scientific and Technical Information of China (English)

    2001-01-01

    The isolation, culture and the active determination of poplar ice nucleation active (INA) bacteria and the inoculation tests in laboratory and field were conducted, and the varieties, distribution and number of poplar INA bacteria and its pathogenicity and freezing injury property were determined. The study results showed that the INA bacteria widely spread on poplar in Northeast China and caused the frozen injury for poplar under the frost condition in Spring or Autumn, which was the key factor to induce INA bacterial canker. Through evaluation and investigation of different poplar varieties and inoculation tests, fine disease-resistant varieties and strains of poplar suitable for Northeast China were selected. Further tests for strong seedling showed that burying cuttings in sand and covering with plastic film could effectively avoid the frostbite, frozen and drought damage, reduce INA bacteria infection, and promote poplar growth. INA bacterial canker was detected early by highly specialized antiserums of INA bacteria and the agglutinated test of ring-shaped boundary surface. The inducers such as streptomycin, phenylmercuric acetae, salicylic acid and heat-killed bacteria to immerse cuttings, have obvious induced disease-resistant effect. Before poplar sprouted in early spring, through spraying the solution of frostbite agent, the control effect also was obvious.

  20. 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.

  1. Heterogeneous ice nucleation on phase-separated organic-sulfate particles: effect of liquid vs. glassy coatings

    OpenAIRE

    G. P. Schill; Tolbert, M. A.

    2013-01-01

    Atmospheric ice nucleation on aerosol particles relevant to cirrus clouds remains one of the least understood processes in the atmosphere. Upper tropospheric aerosols as well as sub-visible cirrus residues are known to be enhanced in both sulfates and organics. The hygroscopic phase transitions of organic-sulfate particles can have an impact on both the cirrus cloud formation mechanism and resulting cloud microphysical properties. In addition to deliquescence and efflorescen...

  2. Lidar observations of ice-nucleating particle (INPC) and ice crystal number (ICNC) concentrations: height-resolved INPC-ICNC closure studies in mixed-phase altocumulus layers

    Science.gov (United States)

    Ansmann, Albert; Bühl, Johannes; Mamouri, Rodanthi-Elisavet; Engelmann, Ronny; Seifert, Patric; Nisantzi, Argyro; Hadjimitsis, Diofantos; Sciare, Jean

    2017-04-01

    During the six-week Cyprus-2015 field campaign in March and April 2015, conducted in the framework of the BACCHUS project (Impact of Biogenic versus Anthropogenic emissions on Clouds and Climate: towards a Holistic UnderStanding, collaborative project of the seventh EU framework programme, ENV.2013.6.1-2), we observed the evolution of extended liquid-water altocumulus fields with subsequent heterogeneous ice formation. The altocumulus layers developed in aged Saharan dust layers between 3.5 km (-20°C) and 7.5 km height (-35°C cloud top temperature). We observed such altocumulus developments on 12 days. By applying our recently developed polarization-lidar method we estimated the ice-nucleating particle concentration (INPC, immersion freezing) at cloud level (before the clouds developed and after their dissolution). Simultaneously performed Doppler lidar observations of the terminal velocities of falling ice crystals in virga below the shallow altocumulus layers allowed us to estimate the ice crystal number concentration (ICNC) of the falling ice crystals. In this retrieval, a realistic ice crystal size distribution has to be assumed. In addition, the volume extinction coefficient of the ice crystals has to be known (to obtain the total ice crystal concentration), and is obtained from the polarization lidar observations by using classical backscatter or Raman lidar retrieval methods. We assume that all ice crystals, which nucleated in the 300-500 m thick altocumulus layers, grow fast (according to the literature to about 100 µm size within 1 minute) and immediately fall out of the main shallow cloud layer so that the derived ICNC values provide us with the number of nucleated ice crystals as a function of cloud top temperature and given INP conditions. Based on this unique observational approach we investigated, to our knowledge for the first time, the consistency between the INPC and ICNC in mixed-phase clouds. We found reasonable agreement between INPC

  3. Spatial and temporal distributions of ice nucleating particles during the Atmospheric Radiation Measurement (ARM) Cloud Aerosol Precipitation Experiment (ACAPEX)

    Science.gov (United States)

    Levin, E. J.; DeMott, P. J.; Suski, K. J.; Boose, Y.; Hill, T. C. J.; McCluskey, C. S.; Schill, G. P.; Duncan, D.; Al-Mashat, H.; Prather, K. A.; Sedlacek, A. J., III; Tomlinson, J. M.; Mei, F.; Hubbe, J. M.; Pekour, M. S.; Leung, L. R.; Kreidenweis, S. M.

    2016-12-01

    California is currently under drought conditions and changes in precipitation due to future climate change scenarios are uncertain. Thus, understanding the controlling factors for precipitation in this region, and having the capability to accurately model these scenarios, is important. A crucial area in understanding precipitation is in the interplay between atmospheric moisture and aerosols. Specifically, ice nucleation in clouds is an important process controlling precipitation formation. A major component of CA's yearly precipitation comes from wintertime atmospheric river (AR) events which were the focus of the 2015 Atmospheric Radiation Measurement (ARM) Cloud Aerosol Precipitation Experiment (ACAPEX) and CalWater 2 campaigns. These two campaigns provided sampling platforms on four aircraft, including the ARM Aerial Facility G-1, as well as the NOAA Ron Brown research vessel and at a ground station at Bodega Bay, CA. Measurements of ice nucleating particles (INPs) were made with the Colorado State University (CSU) Continuous Flow Diffusion Chamber (CFDC) aboard the G-1 and at Bodega Bay, and using aerosol filter collections on these platforms as well as the Ron Brown for post-processing via immersion freezing in the CSU Ice Spectrometer. Aerosol composition was measured aboard the G-1 with the Aerosol Time-of-Flight Mass Spectrometer (ATOFMS). Both the CFDC and ATOFMS sampled off of an isokinetic inlet when flying in clear air and a counter-flow virtual impactor in clouds to capture ice crystal and cloud droplet residuals. In this presentation we present ice nucleating particle concentrations before, during and after an AR event from air, ground and ocean-based measurements. We also examine INP concentration variability in orographic clouds and in clear air at altitude along the Sierra Nevada range, in the marine boundary layer and through the Central Valley, and relate these INP measurements to other aerosol physical and chemical properties.

  4. 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.

  5. Ambient in-situ immersion freezing measurements - findings from the ZAMBIS 2014 field campaign for three ice nucleation techniques

    Science.gov (United States)

    Kohn, Monika; Atkinson, James D.; Lohmann, Ulrike; Kanji, Zamin A.

    2015-04-01

    To estimate the influence of clouds on the Earth's radiation budget, it is crucial to understand cloud formation processes in the atmosphere. A key process, which significantly affects cloud microphysical properties and the initiation of precipitation thus contributing to the hydrological cycle, is the prevailing type of ice nucleation mechanism. In mixed-phase clouds immersion freezing is the dominant ice crystal forming mechanism, whereby ice nucleating particles (INP) first act as cloud condensation nuclei (CCN) and are activated to cloud droplets followed by freezing upon supercooling. There are a number of experimental methods and techniques to investigate the ice nucleating ability in the immersion mode, however most techniques are offline for field sampling or only suitable for laboratory measurements. In-situ atmospheric studies are needed to understand the ice formation processes of 'real world' particles. Laboratory experiments simulate conditions of atmospheric processes like ageing or coating but are still idealized. Our method is able to measure ambient in-situ immersion freezing on single immersed aerosol particles. The instrumental setup consists of the recently developed portable immersion mode cooling chamber (PIMCA) as a vertical extension to the portable ice nucleation chamber (PINC, [1]), where the frozen fraction of activated aerosol particles are detected by the ice optical depolarization detector (IODE, [2]). Two additional immersion freezing techniques based on a droplet freezing array [3,4] are used to sample ambient aerosol particles either in a suspension (fraction larger ~0.6 μm) or on PM10-filters to compare different ice nucleation techniques. Here, we present ambient in-situ measurements at an urban forest site in Zurich, Switzerland held during the Zurich ambient immersion freezing study (ZAMBIS) in spring 2014. We investigated the ice nucleating ability of natural atmospheric aerosol with the PIMCA/PINC immersion freezing setup as

  6. A nucleation and growth model of silicon nanoparticles produced by pulsed laser deposition via Monte Carlo simulation

    Science.gov (United States)

    Wang, Yinglong; Qin, Aili; Chu, Lizhi; Deng, Zechao; Ding, Xuecheng; Guan, Li

    2017-02-01

    We simulated the nucleation and growth of Si nanoparticles produced by pulse laser deposition using Monte Carlo method at the molecular (microscopic) level. In the model, the mechanism and thermodynamic conditions of nucleation and growth of Si nanoparticles were described. In a real physical scale of target-substrate configuration, the model was used to analyze the average size distribution of Si nanoparticles in argon ambient gas and the calculated results are in agreement with the experimental results.

  7. Effect of lactic acid on nucleation morphology and surface roughness of electroless Ni–P deposition in nanoscale

    Indian Academy of Sciences (India)

    A Babanejhad; M Hashemi; Y Rahmatallahpur; Sh A Nozad

    2012-08-01

    The present work aims to study effect of lactic acid concentration as complexing agent on surface roughness and nucleation morphology of electroless N–P deposition. Scanning electron microscopy (SEM) and atomic force microscopy (AFM) have been used to study nucleation morphology and surface roughness of deposition. Deposition process started at some initial priority growing centres independently distributed on the substrate. We found that the morphology and surface roughness of deposition strongly depends on the complexing agent concentration. Morphology of initial deposited centres with no concentration of lactic acid was in coniform structure. By increasing the complexing agent concentration, the structure of initial growing centres changed from coniform to nodular shape and the surface roughness of depositions decreased.

  8. 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.

  9. 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.

  10. Species of Ice Nucleation Active Bacteria on the Apricot and the Relationship Between Their Activity and Flower Frost

    Institute of Scientific and Technical Information of China (English)

    SUN Fu-Zai; ZHAO Ting-chang; YANG Jian-min; CAO Xiao-yu; TANG Chao-rong; MENG Qing-rui

    2001-01-01

    During 1996- 1997, sixty samples were collected from apricot in Hebei Province, from which nineteen ice nucleation active bacterial strains were isolated. Nine stains were identified as Pseudomonas syringae pv. syringae by bacteriological determination, while the others were Erwinia uredovora. Assay of ice nucleation activity (INA) showed the activity of the Pseudomonas strains was higher than that of the Erwinia.According to the number of bacterial cells required to produce one ice nucleus active at - 3℃, four stains was classified as strong ones, three as medium-strong, the remainder as weak. In general, the INA of these strains were regarded as medium-strong. Under stress of Iow temperatures, treatment of INA bacteria can greatly raised relative electric conductivity of petals and permeability of cell membrane. The treated petals showed symptoms of serious frost at - 3 - - 4℃ and had supercooling points of 2 - 3℃ higher than controls. Our results demon strated that INA bacteria are one major factor to incite frost damage to apricot flowers. We may reduce frost injury to apricot during flowering phage through control of INA bacteria.

  11. Ice nucleation, shape, and composition of aerosol particles in one of the most polluted cities in the world: Ulaanbaatar, Mongolia

    Science.gov (United States)

    Hasenkopf, Christa A.; Veghte, Daniel P.; Schill, Gregory P.; Lodoysamba, Sereeter; Freedman, Miriam Arak; Tolbert, Margaret A.

    2016-08-01

    Air pollution is attributable to 7 million deaths per year, or one out of every eight deaths globally. In particular, high concentrations of particulate matter (PM), a major air pollutant, have significant impacts on health and regional climate in urban centers. Many of the most polluted places, largely in developing countries, go severely understudied. Additionally, high particulate matter levels can have an impact on the microphysical properties of clouds, impacting precipitation and regional climate. Semi-arid regions can be especially affected by small changes in precipitation. Here we characterize the physical and chemical properties of PM in one of the most PM-polluted cities in the world: Ulaanbaatar, Mongolia, a semi-arid region in central Asia. Twice monthly aerosol samples were collected over 10 months from a central location and analyzed for composition and ice nucleation activity. Almost all particles collected were inhalable, consisting primarily of mineral dust, soot, and sulfate-organic. In winter, all classes of PM increase in concentration, with increased sulfur concentrations, and the particles are less active towards heterogeneous ice nucleation. In addition, concurrent monthly average PM10, SO2, NOx, and O3 levels and meteorological data at a nearby location are reported and made publicly available. These measurements provide an unprecedented seasonal characterization of the size, shape, chemical structure, and ice nucleating activity of PM data from Ulaanbaatar. This 10-month field study, exploring a variety of aerosol properties in Ulaanbaatar, Mongolia, is one of very few such studies conducted in the region or in such a highly polluted environment. The results of this study may inform work done in other similarly situated and polluted cities in Asia and elsewhere.

  12. 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.

  13. Externally applied electric fields up to 1.6 × 10(5) V/m do not affect the homogeneous nucleation of ice in supercooled water.

    Science.gov (United States)

    Stan, Claudiu A; Tang, Sindy K Y; Bishop, Kyle J M; Whitesides, George M

    2011-02-10

    The freezing of water can initiate at electrically conducting electrodes kept at a high electric potential or at charged electrically insulating surfaces. The microscopic mechanisms of these phenomena are unknown, but they must involve interactions between water molecules and electric fields. This paper investigates the effect of uniform electric fields on the homogeneous nucleation of ice in supercooled water. Electric fields were applied across drops of water immersed in a perfluorinated liquid using a parallel-plate capacitor; the drops traveled in a microchannel and were supercooled until they froze due to the homogeneous nucleation of ice. The distribution of freezing temperatures of drops depended on the rate of nucleation of ice, and the sensitivity of measurements allowed detection of changes by a factor of 1.5 in the rate of nucleation. Sinusoidal alternation of the electric field at frequencies from 3 to 100 kHz prevented free ions present in water from screening the electric field in the bulk of drops. Uniform electric fields in water with amplitudes up to (1.6 ± 0.4) × 10(5) V/m neither enhanced nor suppressed the homogeneous nucleation of ice. Estimations based on thermodynamic models suggest that fields in the range of 10(7)-10(8) V/m might cause an observable increase in the rate of nucleation.

  14. Ice nucleating particles at a coastal marine boundary layer site: correlations with aerosol type and meteorological conditions

    Science.gov (United States)

    Mason, R. H.; Si, M.; Li, J.; Chou, C.; Dickie, R.; Toom-Sauntry, D.; Pöhlker, C.; Yakobi-Hancock, J. D.; Ladino, L. A.; Jones, K.; Leaitch, W. R.; Schiller, C. L.; Abbatt, J. P. D.; Huffman, J. A.; Bertram, A. K.

    2015-11-01

    Information on what aerosol particle types are the major sources of ice nucleating particles (INPs) in the atmosphere is needed for climate predictions. To determine which aerosol particles are the major sources of immersion-mode INPs at a coastal site in Western Canada, we investigated correlations between INP number concentrations and both concentrations of different atmospheric particles and meteorological conditions. We show that INP number concentrations are strongly correlated with the number concentrations of fluorescent bioparticles between -15 and -25 °C, and that the size distribution of INPs is most consistent with the size distribution of fluorescent bioparticles. We conclude that biological particles were likely the major source of ice nuclei at freezing temperatures between -15 and -25 °C at this site for the time period studied. At -30 °C, INP number concentrations are also well correlated with number concentrations of the total aerosol particles ≥ 0.5 μm, suggesting that non-biological particles may have an important contribution to the population of INPs active at this temperature. As we found that black carbon particles were unlikely to be a major source of ice nuclei during this study, these non-biological INPs may include mineral dust. Furthermore, correlations involving chemical tracers of marine aerosols and marine biological activity, sodium and methanesulfonic acid, indicate that the majority of INPs measured at the coastal site likely originated from terrestrial rather than marine sources. Finally, six existing empirical parameterizations of ice nucleation were tested to determine if they accurately predict the measured INP number concentrations. We found that none of the parameterizations selected are capable of predicting INP number concentrations with high accuracy over the entire temperature range investigated. This finding illustrates that additional measurements are needed to improve parameterizations of INPs and their

  15. 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.

  16. 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,).

  17. Size-resolved measurements of ice nucleating particles at six locations in North America and one in Europe

    Science.gov (United States)

    Mason, R. H.; Si, M.; Chou, C.; Irish, V. E.; Dickie, R.; Elizondo, P.; Wong, R.; Brintnell, M.; Elsasser, M.; Lassar, W. M.; Pierce, K. M.; Leaitch, W. R.; MacDonald, A. M.; Platt, A.; Toom-Sauntry, D.; Sarda-Estève, R.; Schiller, C. L.; Suski, K. J.; Hill, T. C. J.; Abbatt, J. P. D.; Huffman, J. A.; DeMott, P. J.; Bertram, A. K.

    2015-07-01

    Detailed information on the size of ice nucleating particles (INPs) may be useful in source identification, modeling their transport in the atmosphere to improve climate predictions, and determining how effectively or ineffectively instrumentation used for quantifying INPs in the atmosphere captures the full INP population. In this study we report immersion-mode INP number concentrations as a function of size at six ground sites in North America and one in Europe. The lowest INP number concentrations were observed at Arctic and alpine locations and the highest at suburban and agricultural locations, consistent with previous studies of INP concentrations in similar environments. We found that 91, 79, and 63 % of INPs had an aerodynamic diameter > 1 μm at ice activation temperatures of -15, -20, and -25 °C, respectively, when averaging over all sampling locations. In addition, 62, 55, and 42 % of INPs were in the coarse mode (> 2.5 μm) at ice activation temperatures of -15, -20, and -25 °C, respectively, when averaging over all sampling locations. These results are consistent with six out of the seven studies in the literature that have focused on the size distribution of INPs in the atmosphere. Taken together, these findings strongly suggest that supermicron and coarse mode aerosol particles are a significant component of the ice nuclei population in many different ground-level environments. Further size-resolved studies of INPs as a function of altitude are required.

  18. Ice sublimation and rheology - Implications for the Martian polar layered deposits

    Science.gov (United States)

    Hofstadter, Mark D.; Murray, Bruce C.

    1990-01-01

    If the sublimation and creep of water ice are important processes in the Martian polar layered deposits, ice-rich scenario formation and evolution schemes must invoke a mechanism for the inhibition of sublimation, such as a dust layer derived from the residue of the sublimating deposits. This layer could be of the order of 1 m in thickness. If the deposits are ice-rich, flows of more than 1 km should have occurred. It is noted that the dust particles in question may be cemented by such ice that may be present, but that impurities may also have served to cement dust particles together even in the absence of ice.

  19. How thick are Mercury's polar water ice deposits?

    CERN Document Server

    Eke, Vincent R; Teodoro, Luıs F A

    2016-01-01

    An estimate is made of the thickness of the radar-bright deposits in craters near to the north pole of Mercury. To construct an objective set of craters for this measurement, an automated crater finding algorithm is developed and applied to a digital elevation model based on data from the Mercury Laser Altimeter on board the MESSENGER spacecraft. This produces a catalogue of 663 craters with diameters exceeding 4 km, northwards of latitude +55 degrees. A subset of 12 larger, well-sampled and fresh polar craters are selected to search for correlations between topography and radar same-sense backscatter cross-section. It is found that the typical excess height associated with the radar-bright regions within these fresh polar craters is (50+/-35)m. This puts an approximate upper limit on the total polar water ice deposits on Mercury of 3e15 kg.

  20. How thick are Mercury's polar water ice deposits?

    Science.gov (United States)

    Eke, Vincent R.; Lawrence, David J.; Teodoro, Luís F. A.

    2017-03-01

    An estimate is made of the thickness of the radar-bright deposits in craters near to Mercury's north pole. To construct an objective set of craters for this measurement, an automated crater finding algorithm is developed and applied to a digital elevation model based on data from the Mercury Laser Altimeter onboard the MESSENGER spacecraft. This produces a catalogue of 663 craters with diameters exceeding 4 km, northwards of latitude +55∘ . A subset of 12 larger, well-sampled and fresh polar craters are selected to search for correlations between topography and radar same-sense backscatter cross-section. It is found that the typical excess height associated with the radar-bright regions within these fresh polar craters is (50 ± 35) m. This puts an approximate upper limit on the total polar water ice deposits on Mercury of ∼ 3 × 1015 kg.

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

    Science.gov (United States)

    Stopelli, Emiliano; Conen, Franz; Morris, Cindy E.; Herrmann, Erik; Henne, Stephan; Steinbacher, Martin; Alewell, Christine

    2016-07-01

    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.

  2. Multiscale approaches for simulation of nucleation, growth, and additive chemistry during electrochemical deposition of thin metal films

    Science.gov (United States)

    Stephens, Ryan Mark

    Molecularly engineered deposition processes require computational algorithms that efficiently capture phenomena present at widely varying length and time scales. In this work, the island dynamics method was applied to simulation of kinetically-limited metal nucleation and growth by electrodeposition in the presence of additives. The model included additive kinetics, surface diffusion of adatoms, nucleation, and growth. The model was demonstrated for copper deposition in acid sulfate electrolyte containing [bis(3-sulfopropyl)disulfide], polyethylene glycol, and chloride. Simulation results were compared with kinetic Monte Carlo (KMC) calculations and found to be within 1% for fractional coverage values, and within 10% for nucleation density. The computational time was more than 10X faster than comparable KMC simulations over the range studied. The island dynamics algorithm was applied to the electrodeposition of a metal onto a substrate initially configured with an array of hemispherical seed clusters. It was found that the presence of chloride in the model additive system caused high densities of nuclei on the substrate surrounding the initial seed clusters, which led to the formation of a continuous thin metal film. Simulations carried out under low-chloride conditions resulted in the growth only of the initial seed clusters, without significant nucleation or thin film formation. Additional phenomena were explored by linking the molecular scale island dynamics algorithm to a continuum model that described the migration and diffusion in the diffusion layer near the electrode surface. The multiscale linkage allowed simulation of nucleation, growth, and additive chemistry under mass transport limited conditions, including the formation of nucleation exclusion zones surrounding growing nuclei. A two-step approach was used to calculate the spatial distribution of nucleation events on an electrode undergoing deposition by electrolysis under the influence of mass

  3. In Situ Conductance Analysis of Zinc Oxide Nucleation and Coalescence during Atomic Layer Deposition on Metal Oxides and Polymers.

    Science.gov (United States)

    Sweet, William J; Parsons, Gregory N

    2015-07-07

    Real time in situ conductance is collected continuously during atomic layer deposition (ALD) of zinc oxide films, and trends are used to study ALD nucleation on polypropylene, nylon-6, SiO2, TiO2, and Al2O3 substrates. The detailed conductance change during the ALD cycle is ascribed to changes in surface band bending upon precursor/reactant exposure. Conductive pathways form earlier on the inorganic surfaces than on the polymers, with Al2O3 substrates showing more rapid nucleation than SiO2 or TiO2, consistent with the expected density of nucleation sites (e.g., hydroxyl groups) on these different materials. The measured conductance is ohmic, and both two- and four-electrode configurations show the same data trends. Detailed analysis of conductivity at deposition temperatures between 100 and 175 °C shows faster conductivity decay at higher temperature during the water purge step, ascribed to thermally activated water desorption kinetics. Analysis of real-time conductivity during ALD of other material systems could provide further insight into key aspects of film nucleation and nuclei coalescence.

  4. Glaciochemical investigations on the subterranean ice deposit of Vukušić Ice Cave, Velebit Mountain, Croatia

    Science.gov (United States)

    Kern, Z.; Fórizs, I.; Horvatinčić, N.; Széles, É.; Bočić, N.; Nagy, B.

    2010-09-01

    The 3H activity, 18O/16O and 2H/1H ratio and concentration of 33 metals and metalloids have been analysed on ice core samples from the perennial subterranean cave ice deposit of Vukušić Ice Cave, Velebit Mt. The tritium data suggested that the ice deposition at 2-2.4 m depth is build from precipitation fallen ~45 years before sampling and the uppermost ice layer could be estimated between early 1970s and early 1980s or between ~1954 and 1960. Both the fluctuation range of stable water isotopes and the derived isotopic waterline of the ice agree reasonably well with the corresponding data of the local precipitation. This fact predicts that the potential of Vukušić Ice Cave's ice deposit is superior for paleoclimatological studies to the nearby Ledena Pit. Principal component analysis helped to select three groups of elements. The Ca-Mg governed group (PC1) encompasses the bedrock related components; hence the fluctuation of these elements might reflect the past intensities of the dissolution process of the adjacent epikarst. The Zn governed group (PC2) preserves probably an atmospheric deposition signal and related to the emission of regional non-ferrous metallurgy. PC3 is governed by Al and Fe. This probably carries the distal, non-karstic crustal signal hence might be related to the past atmospheric circulation (i.e. wind direction and speed).

  5. Ice Nucleation of Fungal Spores from the Classes Agaricomycetes, Ustilaginomycetes, and Eurotiomycetes, and the effect on the Atmospheric Transport of these Spores

    Energy Technology Data Exchange (ETDEWEB)

    Haga, D. I.; Burrows, Susannah M.; Iannone, R.; Wheeler, M. J.; Mason, R.; Chen, J.; Polishchuk, E. A.; Poschl, U.; Bertram, Allan K.

    2014-08-26

    Ice nucleation on fungal spores may affect the frequency and properties of ice and mixed-phase clouds. We studied the ice nucleation properties of 12 different species of fungal spores chosen from three classes: Agaricomycetes, Ustilagomycetes, and Eurotiomycetes. Agaricomycetes include many types of mushroom species and are cosmopolitan all over the globe. Ustilagomycetes are agricultural pathogens and have caused widespread damage to crops. Eurotiomycetes are found on all types of decaying material and include important human allergens. We focused on these classes since they are thought to be abundant in the atmosphere and because there is very little information on the ice nucleation ability of these classes of spores in the literature. All of the fungal spores investigated were found to cause freezing of water droplets at temperatures warmer than homogeneous freezing. The cumulative number of ice nuclei per spore was 0.001 at temperatures between -19 °C and -29 °C, 0.01 between -25.5 °C and -31 °C, and 0.1 between -26 °C and -36 °C. On average, the order of ice nucleating ability for these spores is Ustilagomycetes > Agaricomycetes ≅ Eurotiomycetes. We show that at temperatures below -20 °C, all of the fungal spores studied here are less efficient ice nuclei compared to Asian mineral dust on a per surface area basis. We used our new freezing results together with data in the literature to compare the freezing temperatures of spores from the phyla Basidiomycota and Ascomycota, which together make up 98 % of known fungal species found on Earth. The data show that within both phyla (Ascomycota and Basidiomycota) there is a wide range of freezing properties, and also that the variation within a phylum is greater than the variation between the average freezing properties of the phyla. Using a global chemistry-climate transport model, we investigated whether ice nucleation on the studied spores, followed by precipitation, can influence the atmospheric

  6. Frost-related dieback of willows. Comparison of epiphytically and endophytically isolated bacteria from different Salix clones, with emphasis on ice nucleation activity, pathogenic properties and seasonal variation

    Energy Technology Data Exchange (ETDEWEB)

    Cambours, M.A.; Nejad, P.; Ramstedt, M. [Swedish University of Agricultural Sciences, Uppsala (Sweden). Plant Pathology and Biocontrol Unit; Granhall, U. [Swedish University of Agricultural Sciences, Uppsala (Sweden). Department of Microbiology

    2005-01-01

    Swedish Salix plantation for biomass production have been suffering severe dieback during the past 10 years, possibly due to the combination of frost and bacterial disease. As opposed to summer and winter, spring and autumn are periods when epiphytic populations of ice nucleation active (INA) bacteria are generally high. The culturable bacterial floras from stems of diseased plant of four Salix viminalis clones were compared in spring and autumn. Both epiphytic and endophytic bacteria were isolated (i.e. from plant surface and from tissues beneath the bark, respectively), characterised and tested for ice nucleating activity and pathogenicity. Some strains were also identified with BIOLOG and 16S rRNA. Endophytically isolated communities were generally more stable than epiphytes, both in number of isolates and type of bacteria. More types were found in autumn than in spring the same year, although the total number of strains isolated was rather constant. In contrast, more strains (and a higher percentage of the total community) expressed ice nucleating activity in spring than in autumn. The overall number of pathogenic strains remained stable but their proportion among the community tested on plants increased. A close relationship was observed between the dieback rates in the field and the percentage of pathogenic strains found in the different clones. The dominating bacterial type isolated, Sphingomonas spp., also contained the highest percentage of ice nucleation active pathogenic strains. (author)

  7. 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.

  8. Characterization of the inaA gene and expression of ice nucleation phenotype in Pantoea ananatis isolates from Maize White Spot disease.

    Science.gov (United States)

    Miller, A M; Figueiredo, J E F; Linde, G A; Colauto, N B; Paccola-Meirelles, L D

    2016-03-04

    Maize White Spot (MWS), a foliar disease caused by Pantoea ananatis, could cause up to 60% yield loss. Some strains of P. ananatis harboring the ice nucleation gene inaA catalyze the formation of ice nuclei, causing tissue damage at temperatures slightly below freezing. Little is known about the relationship between the presence of the ina gene in this maize pathogen and its expression during the phenomenon of ice nucleus formation. Here, we attempted to verify the presence of the inaA gene and the expression of phenotype in vitro. The identity of the isolates and the presence of the inaA gene were determined by P. ananatis species-specific primers. The expression of the inaA gene was assessed in vitro by the visualization of ice-crystal formation in water at subzero temperatures. A total of ninety P. ananatis isolates from MWS lesions were characterized. The presence of the inaA gene was confirmed by gel electrophoresis of the 350-400-bp PCR products. The inaA primers did not lead to DNA fragment amplification in three isolates. The ice nucleation phenotype was expressed in 83.34% of the isolates carrying the inaA gene. Our study showed that the ice nucleation in P. ananatis isolated from MWS lesions was dependent on the presence of a functional ina gene in the genome. We also found evidence indicating that some P. ananatis strains have a mutated form of the inaA gene, producing a non-functional ice nucleation protein. This is the first report on inaA gene characterization in P. ananatis isolates from Maize White Spot.

  9. Determination of the ice-nucleating ability of Fusarium caucascium microconidia

    Science.gov (United States)

    Mason, Ryan H.; Bertram, Allan K.

    2013-05-01

    Recent studies have indicated that biological particles may be an important class of ice nuclei on regional scales. Quantitative measurements on the immersion ice-activity of spores of the common genus Fusarium have been performed. Droplets containing an average of approximately five Fusarium caucasicum microconidia were found to have a median freezing temperature of -33.6°C. The activity spectrum revealed that 0.1% and 1% of spores are active at -29.1°C and -30.7°C, respectively.

  10. 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

    2014-07-31

    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. Published by Oxford University Press on behalf of the Annals of Botany Company.

  11. Ice nucleation properties of rust and bunt fungal spores and their transport to high altitudes, where they can cause heterogeneous freezing

    Science.gov (United States)

    Haga, D. I.; Iannone, R.; Wheeler, M. J.; Mason, R.; Polishchuk, E. A.; Fetch, T.; van der Kamp, B. J.; McKendry, I. G.; Bertram, A. K.

    2013-07-01

    Rust and bunt spores that act as ice nuclei (IN) could change the formation characteristics and properties of ice-containing clouds. In addition, ice nucleation on rust and bunt spores, followed by precipitation, may be an important removal mechanism of these spores from the atmosphere. Using an optical microscope, we studied the ice nucleation properties of spores from four rust species (Puccinia graminis, Puccinia triticina, Puccinia allii, and Endocronartium harknesssii) and two bunt species (Tilletia laevis and Tilletia tritici) immersed in water droplets. We show that the cumulative number of IN per spore is 5 × 10-3, 0.01, and 0.10 at temperatures of roughly -24°C, -25°C, and -28°C, respectively. Using a particle dispersion model, we also investigated if these rust and bunt spores will reach high altitudes in the atmosphere where they can cause heterogeneous freezing. Simulations suggest that after 3 days and during periods of high spore production, between 6 and 9% of 15 µm particles released over agricultural regions in Kansas (U.S.), North Dakota (U.S.), Saskatchewan (Canada), and Manitoba (Canada) can reach at least 6 km in altitude. An altitude of 6 km corresponds to a temperature of roughly -25°C for the sites chosen. The combined results suggest that (a) ice nucleation by these fungal spores could play a role in the removal of these particles from the atmosphere and (b) ice nucleation by these rust and bunt spores are unlikely to compete with mineral dust on a global and annual scale at an altitude of approximately 6 km.

  12. Molecular biological basis of ice-nucleating of ice-nucleation active bacteria and its application in food freezing%冰核活性细菌成冰的分子生物学基础及其在食品冷冻中的应用

    Institute of Scientific and Technical Information of China (English)

    徐荣荣; 邓开野; 丁力行

    2012-01-01

    The molecular biological basis of ice-nucleating of ice-nucleation active bacteria, its application in food freezing and the relative safety problem were reviewed. Research directions of the application of ice-nucleation active micro-organism in food freezing were put forward in this review.%对冰核活性细菌成冰的分子生物学基础、在食品冷冻中的应用及其安全性问题进行了综述,并对冰核活性微生物在食品冷冻中的应用前景进行了展望.

  13. Effects of cloud condensation nuclei and ice nucleating particles on precipitation processes and supercooled liquid in mixed-phase orographic clouds

    Energy Technology Data Exchange (ETDEWEB)

    Fan, Jiwen; Leung, L. Ruby; Rosenfeld, Daniel; DeMott, Paul J.

    2017-01-01

    How orographic mixed-phase clouds respond to the change in cloud condensation nuclei (CCN) and ice nucleating particles (INPs) are highly uncertain. The main snow production mechanism in warm and cold mixed-phase orographic clouds (referred to as WMOCs and CMOCs, respectively, distinguished here as those having cloud tops warmer and colder than -20°C) could be very different. We quantify the CCN and INP impacts on supercooled water content, cloud phases, and precipitation for a WMOC case and a CMOC case, with sensitivity tests using the same CCN and INP concentrations between the WMOC and CMOC cases. It was found that deposition plays a more important role than riming for forming snow in the CMOC case, while the role of riming is dominant in the WMOC case. As expected, adding CCN suppresses precipitation, especially in WMOCs and low INPs. However, this reverses strongly for CCN of 1000 cm-3 and larger. We found a new mechanism through which CCN can invigorate mixed-phase clouds over the Sierra Nevada and drastically intensify snow precipitation when CCN concentrations are high (1000 cm-3 or higher). In this situation, more widespread shallow clouds with a greater amount of cloud water form in the Central Valley and foothills west of the mountain range. The increased latent heat release associated with the formation of these clouds strengthens the local transport of moisture to the windward slope, invigorating mixed-phase clouds over the mountains, and thereby producing higher amounts of snow precipitation. Under all CCN conditions, increasing the INPs leads to decreased riming and mixed-phase fraction in the CMOC as a result of liquid-limited conditions, but has the opposite effects in the WMOC as a result of ice-limited conditions. However, precipitation in both cases is increased by increasing INPs due to an increase in deposition for the CMOC but enhanced riming and deposition in the WMOC. Increasing the INPs dramatically reduces

  14. Surface modification of mineral dust particles by sulphuric acid processing: implications for ice nucleation abilities

    OpenAIRE

    P. Reitz; C. Spindler; T. F. Mentel; Poulain, L.; H. Wex; K. Mildenberger; D. Niedermeier; Hartmann, S.; T. Clauss; F. Stratmann; R. C. Sullivan; Demott, P. J.; Petters, M. D.; Sierau, B.; Schneider, J.

    2011-01-01

    The ability of coated mineral dust particles to act as ice nuclei (IN) was investigated at LACIS (Leipzig Aerosol Cloud Interaction Simulator) during the FROST1- and FROST2-campaigns (Freezing of dust). Sulphuric acid was condensed on the particles which afterwards were optionally humidified, treated with ammonia vapour and/or heat. By means of aerosol mass spectrometry we found evidence that processing of mineral dust particles with su...

  15. Ice nucleation by fungal spores from the classes Agaricomycetes, Ustilaginomycetes, and Eurotiomycetes, and the effect on the atmospheric transport of these spores

    Science.gov (United States)

    Haga, D. I.; Burrows, S. M.; Iannone, R.; Wheeler, M. J.; Mason, R. H.; Chen, J.; Polishchuk, E. A.; Pöschl, U.; Bertram, A. K.

    2014-08-01

    We studied the ice nucleation properties of 12 different species of fungal spores chosen from three classes: Agaricomycetes, Ustilaginomycetes, and Eurotiomycetes. Agaricomycetes include many types of mushroom species and are widely distributed over the globe. Ustilaginomycetes are agricultural pathogens and have caused widespread damage to crops. Eurotiomycetes are found on all types of decaying material and include important human allergens. We focused on these classes because they are thought to be abundant in the atmosphere and because there is very little information on the ice nucleation ability of these classes of spores in the literature. All of the fungal spores investigated contained some fraction of spores that serve as ice nuclei at temperatures warmer than homogeneous freezing. The cumulative number of ice nuclei per spore was 0.001 at temperatures between -19 °C and -29 °C, 0.01 between -25.5 °C and -31 °C, and 0.1 between -26 °C and -31.5 °C. On average, the order of ice nucleating ability for these spores is Ustilaginomycetes > Agaricomycetes ≃ Eurotiomycetes. The freezing data also suggests that, at temperatures ranging from -20 °C to -25 °C, all of the fungal spores studied here are less efficient ice nuclei compared to Asian mineral dust on a per surface area basis. We used our new freezing results together with data in the literature to compare the freezing temperatures of spores from the phyla Basidiomycota and Ascomycota, which together make up 98% of known fungal species found on Earth. The data show that within both phyla (Ascomycota and Basidiomycota), there is a wide range of freezing properties, and also that the variation within a phylum is greater than the variation between the average freezing properties of the phyla. Using a global chemistry-climate transport model, we investigated whether ice nucleation on the studied spores, followed by precipitation, can influence the transport and global distributions of these spores in

  16. Glaciochemical investigations on the subterranean ice deposit of Vukušić Ice Cave, Velebit Mountain, Croatia

    Directory of Open Access Journals (Sweden)

    Z. Kern

    2010-09-01

    Full Text Available The 3H activity, 18O/16O and 2H/1H ratio and concentration of 33 metals and metalloids have been analysed on ice core samples from the perennial subterranean cave ice deposit of Vukušić Ice Cave, Velebit Mt. The tritium data suggested that the ice deposition at 2–2.4 m depth is build from precipitation fallen ~45 years before sampling and the uppermost ice layer could be estimated between early 1970s and early 1980s or between ~1954 and 1960. Both the fluctuation range of stable water isotopes and the derived isotopic waterline of the ice agree reasonably well with the corresponding data of the local precipitation. This fact predicts that the potential of Vukušić Ice Cave's ice deposit is superior for paleoclimatological studies to the nearby Ledena Pit. Principal component analysis helped to select three groups of elements. The Ca-Mg governed group (PC1 encompasses the bedrock related components; hence the fluctuation of these elements might reflect the past intensities of the dissolution process of the adjacent epikarst. The Zn governed group (PC2 preserves probably an atmospheric deposition signal and related to the emission of regional non-ferrous metallurgy. PC3 is governed by Al and Fe. This probably carries the distal, non-karstic crustal signal hence might be related to the past atmospheric circulation (i.e. wind direction and speed.

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

    Directory of Open Access Journals (Sweden)

    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.

  18. Modeling the cell-type dependence of diffusion-limited intracellular ice nucleation and growth during both vitrification and slow freezing

    Science.gov (United States)

    Yang, Geer; Zhang, Aili; Xu, Lisa X.; He, Xiaoming

    2009-06-01

    In this study, a set of models for predicting the diffusion-limited ice nucleation and growth inside biological cells were established. Both the heterogeneous and homogeneous nucleation mechanisms were considered in the models. Molecular mobility including viscosity and mutual diffusion coefficient of aqueous cryoprotectant (i.e., glycerol here) solutions was estimated using models derived from the free volume theory for glass transition, which makes it possible to predict the two most important physical properties (i.e., viscosity and mutual diffusion coefficient) over wide ranges of temperature and concentration as encountered in cryopreservation. After being verified using experimental data, the models were used to predict the critical cooling rate (defined as the cooling rate required so that the crystallized volume is less than 0.1% of the cell volume) as a function of the initial glycerol concentration in a number of cell types with different sizes. For slowing freezing, it was found that the required critical cooling rate is cell-type dependent with influences from cell size and the ice nucleation and water transport parameters. In general, the critical cooling rate does not change significantly with the initial glycerol concentration used and tends to be higher for smaller cells. For vitrification, the required critical cooling rate does change significantly with the initial glycerol concentration used and tends to decrease with the decrease in cell size. However, the required critical cooling rate can be similar for cells with very different sizes. It was further found that the thermodynamic and kinetic parameters for intracellular ice formation associated with different cells rather than the cell size per se significantly affect the critical cooling rates required for vitrification. For all cell types, it was found that homogeneous nucleation dominates at ultrafast cooling rates and/or high glycerol concentrations, whereas heterogeneous nucleation becomes

  19. The test freezing temperature of C2-C6 dicarboxylic acid: The important indicator for ice nucleation processes

    Institute of Scientific and Technical Information of China (English)

    DU Rui; P. A. ARIYA

    2008-01-01

    The importance of organic compounds as significant constituents of atmospheric aerosols, and cloud condensation nuclei (CCN), as well as players influencing the tropospheric oxidation and atmospheric energy budget, have been increasingly recognized. Low molecular weight dicarboxylic acids (LMW-DCAs) are significant identified portions of atmospheric condensed matter including aerosols, fog and clouds. Besides the photochemical transformation of DCA, the implication of organic matter in ice nucleation processes has been considered. In this study, we investigated the freezing temperature of pure and mixed (C2-C6) DCA solutions in ultra-pure water and tap water solution droplets using a freezing nucleus counter at different pH, and in different water ionic conditions. The mean freezing temperature of different mixture of LMW-DCA in ultra-pure and tap water solution droplets ranged from -24.1±2.8 to-21.3±3.9℃ and -10.2±2.2 to -9.5±2.2℃, respectively. The mean freezing temperature of the control (ultra-pure and tap) water droplets (-22.6±3.5℃, 11.2±2.4℃) was also measured. The results, and their implications in atmospheric chemistry and physics of the atmosphere will be discussed.

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

    Energy Technology Data Exchange (ETDEWEB)

    Seidel, Thomas E., E-mail: zoomtotom@gmail.com [Seitek50, Palm Coast, Florida 32135 (United States); Goldberg, Alexander; Halls, Mat D. [Schrödinger, Inc., San Diego, California 92122 (United States); Current, Michael I. [Current Scientific, San Jose, California 95124 (United States)

    2016-01-15

    Simulations for the nucleation and growth of phosphorus films were carried out using density functional theory. The surface was represented by a Si{sub 9}H{sub 12} truncated cluster surface model with 2 × 1-reconstructured (100) Si-OH terminations for the initial reaction sites. Chemistries included phosphorous halides (PF{sub 3}, PCl{sub 3}, and PBr{sub 3}) and disilane (Si{sub 2}H{sub 6}). Atomic layer deposition (ALD) reaction sequences were illustrated with three-dimensional molecular models using sequential PF{sub 3} and Si{sub 2}H{sub 6} reactions and featuring SiFH{sub 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.

  1. A comparative study of K-rich and Na/Ca-rich feldspar ice-nucleating particles in a nanoliter droplet freezing assay

    Science.gov (United States)

    Peckhaus, Andreas; Kiselev, Alexei; Hiron, Thibault; Ebert, Martin; Leisner, Thomas

    2016-09-01

    A recently designed droplet freezing assay was used to study the freezing of up to 1500 identical 0.2 nL water droplets containing suspensions of one Na/Ca-rich feldspar and three K-rich and one Na/Ca-rich feldspar particles. Three types of experiments have been conducted: cooling ramp, isothermal freezing at a constant temperature, and freeze-thaw cycles. The observed freezing behavior has been interpreted with the help of a model based on the classical nucleation theory (soccer ball model (SBM); Niedermeier et al., 2015). By applying the model to the different freezing experiments conducted with the same ice-nucleating material, the unique sets of model parameters for specific feldspar suspensions could be derived. The SBM was shown to adequately describe the observed cooling rate dependence, the ice-nucleating active sites (INAS) surface density ns(T) in a wide temperature range, and the shift of the freezing curves towards lower temperature with dilution. Moreover, the SBM was capable of reproducing the variation of INAS surface density ns(T) with concentration of ice-nucleating particles in the suspension droplets and correctly predicting the leveling-off of ns(T) at low temperature. The freeze-thaw experiments have clearly shown that the heterogeneous freezing induced even by very active ice-nucleating species still possesses a stochastic nature, with the degree of randomness increasing towards homogeneous nucleation. A population of the high-temperature INAS has been identified in one of the K-rich feldspar samples. The freezing of 0.8 wt % suspension droplets of this particular feldspar was observed already at -5 °C. These high-temperature active sites could be deactivated by treating the sample with hydrogen peroxide but survived heating up to 90 °C. Given a high mass concentration of these high-temperature active sites (2.9 × 108 g-1) and a very low value of contact angle (0.56 rad) the possibility of biological contamination of the sample was

  2. Separation and sampling of ice nucleation chamber generated ice particles by means of the counterflow virtual impactor technique for the characterization of ambient ice nuclei.

    Science.gov (United States)

    Schenk, Ludwig; Mertes, Stephan; Kästner, Udo; Schmidt, Susan; Schneider, Johannes; Frank, Fabian; Nillius, Björn; Worringen, Annette; Kandler, Konrad; Ebert, Martin; Stratmann, Frank

    2014-05-01

    In 2011, the German research foundation (DFG) research group called Ice Nuclei Research Unit (INUIT (FOR 1525, project STR 453/7-1) was established with the objective to achieve a better understanding concerning heterogeneous ice formation. The presented work is part of INUIT and aims for a better microphysical and chemical characterization of atmospheric aerosol particles that have the potential to act as ice nuclei (IN). For this purpose a counterflow virtual impactor (Kulkarni et al., 2011) system (IN-PCVI) was developed and characterized in order to separate and collect ice particles generated in the Fast Ice Nucleus Chamber (FINCH; Bundke et al., 2008) and to release their IN for further analysis. Here the IN-PCVI was used for the inertial separation of the IN counter produced ice particles from smaller drops and interstitial particles. This is realized by a counterflow that matches the FINCH output flow inside the IN-PCVI. The choice of these flows determines the aerodynamic cut-off diameter. The collected ice particles are transferred into the IN-PCVI sample flow where they are completely evaporated in a particle-free and dry carrier air. In this way, the aerosol particles detected as IN by the IN counter can be extracted and distributed to several particle sensors. This coupled setup FINCH, IN-PCVI and aerosol instrumentation was deployed during the INUIT-JFJ joint measurement field campaign at the research station Jungfraujoch (3580m asl). Downstream of the IN-PCVI, the Aircraft-based Laser Ablation Aerosol Mass Spectrometer (ALABAMA; Brands et al., 2011) was attached for the chemical analysis of the atmospheric IN. Also, number concentration and size distribution of IN were measured online (TROPOS) and IN impactor samples for electron microscopy (TU Darmstadt) were taken. Therefore the IN-PCVI was operated with different flow settings than known from literature (Kulkarni et al., 2011), which required a further characterisation of its cut

  3. Preservation of ancient ice at Pavonis and Arsia Mons: Tropical mountain glacier deposits on Mars

    Science.gov (United States)

    Head, James W.; Weiss, David K.

    2014-11-01

    Large tropical mountain glacier (TMG) deposits on the northwest flanks of the Tharsis Montes and Olympus Mons volcanoes are interpreted to be the record of ancient climates characteristic of Mars several hundred million years ago when planetary spin-axis obliquity was ~45°. During this era, polar volatiles (predominantly H2O) were mobilized and transferred equatorward, undergoing adiabatic cooling on the Tharsis volcano flanks, and precipitating snow and ice to form cold-based tropical mountain glaciers up to several kilometers in thickness. Subsequent climate change resulted in retreat, sublimation and collapse of the tropical mountain glaciers, leaving the three typical facies observed today: (1) concentric ridges, the ridged facies, interpreted as drop moraines; (2) knobby facies, interpreted as debris-dominated sublimation residue; and (3) the smooth facies, interpreted as remnant alpine glacial deposits. Ring-mold craters (RMCs) are distinctive features formed by impacts into debris-covered ice. We describe a set of relatively fresh ring-mold craters superposed on the Arsia and Pavonis Mons TMG deposits; we interpret these to indicate that the impact events penetrated a veneer of sublimation lag and excavated buried remnant glacial ice, despite the lack of detection of buried ice by orbital radar instruments. The diameter distribution of the RMCs suggest that the remnant ice lies at a depth of at least 16 m. The TMG deposit ages suggest that these ice deposits date from a period in the range of 125-220 million years before the present; the remnant ice may thus preserve records of the ancient atmospheric gas content and microbiota, as is common in terrestrial glacial ice. Preservation of this ice and the lack of any associated fluvial features suggest that the post-glacial climate has been cold, and related surface temperatures have not been sufficient to bring the buried deposits to the melting point of water.

  4. 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

  5. Comparative measurements of ambient atmospheric concentrations of ice nucleating particles using multiple immersion freezing methods and a continuous flow diffusion chamber

    Science.gov (United States)

    DeMott, Paul J.; Hill, Thomas C. J.; Petters, Markus D.; Bertram, Allan K.; Tobo, Yutaka; Mason, Ryan H.; Suski, Kaitlyn J.; McCluskey, Christina S.; Levin, Ezra J. T.; Schill, Gregory P.; Boose, Yvonne; Rauker, Anne Marie; Miller, Anna J.; Zaragoza, Jake; Rocci, Katherine; Rothfuss, Nicholas E.; Taylor, Hans P.; Hader, John D.; Chou, Cedric; Huffman, J. Alex; Pöschl, Ulrich; Prenni, Anthony J.; Kreidenweis, Sonia M.

    2017-09-01

    A number of new measurement methods for ice nucleating particles (INPs) have been introduced in recent years, and it is important to address how these methods compare. Laboratory comparisons of instruments sampling major INP types are common, but few comparisons have occurred for ambient aerosol measurements exploring the utility, consistency and complementarity of different methods to cover the large dynamic range of INP concentrations that exists in the atmosphere. In this study, we assess the comparability of four offline immersion freezing measurement methods (Colorado State University ice spectrometer, IS; North Carolina State University cold stage, CS; National Institute for Polar Research Cryogenic Refrigerator Applied to Freezing Test, CRAFT; University of British Columbia micro-orifice uniform deposit impactor-droplet freezing technique, MOUDI-DFT) and an online method (continuous flow diffusion chamber, CFDC) used in a manner deemed to promote/maximize immersion freezing, for the detection of INPs in ambient aerosols at different locations and in different sampling scenarios. We also investigated the comparability of different aerosol collection methods used with offline immersion freezing instruments. Excellent agreement between all methods could be obtained for several cases of co-sampling with perfect temporal overlap. Even for sampling periods that were not fully equivalent, the deviations between atmospheric INP number concentrations measured with different methods were mostly less than 1 order of magnitude. In some cases, however, the deviations were larger and not explicable without sampling and measurement artifacts. Overall, the immersion freezing methods seem to effectively capture INPs that activate as single particles in the modestly supercooled temperature regime (> -20 °C), although more comparisons are needed in this temperature regime that is difficult to access with online methods. Relative to the CFDC method, three immersion freezing

  6. Characteristics of atmospheric ice nucleating particles associated with biomass burning in the US: Prescribed burns and wildfires

    Science.gov (United States)

    McCluskey, Christina S.

    Insufficient knowledge regarding the sources and number concentrations of atmospheric ice nucleating particles (INP) leads to large uncertainties in understanding the interaction of aerosols with cloud processes, such as cloud life time and precipitation rates. This study utilizes measurements of INP from a diverse set of biomass burning events to better understand INP associated with biomass burning in the U.S. Prescribed burns in Georgia and Colorado, two Colorado wildfires and two laboratory burns were monitored for INP number concentrations. The relationship between nINP and total particle number concentrations, evident within prescribed burning plumes, was degraded within aged smoke plumes from the wildfires, limiting the utility of this relationship for comparing laboratory and field data. Larger particles, represented by n500nm, are less vulnerable to plume processing and have previously been evaluated for their relation to nINP. Our measurements indicated that for a given n500nm, nINP associated with the wildfires were nearly an order of magnitude higher than nINP found in prescribed fire emissions. Reasons for the differences between INP characteristics in these emissions were explored, including variations in combustion efficiency, fuel type, transport time and environmental conditions. Combustion efficiency and fuel type were eliminated as controlling factors by comparing samples with contrasting combustion efficiencies and fuel types. Transport time was eliminated because the expected impact would be to reduce n500nm, thus resulting in the opposite effect from the observed change. Bulk aerosol chemical composition analyses support the potential role of elevated soil dust particle concentrations during the fires, contributing to the population of INP, but the bulk analyses do not target INP composition directly. It is hypothesized that both hardwood burning and soil lofting are responsible for the elevated production of INP in the Colorado wildfires in

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

    CERN Document Server

    Brown, Adrian J; 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 s...

  8. Dust ice nuclei effects on cirrus clouds

    Directory of Open Access Journals (Sweden)

    M. Kuebbeler

    2013-04-01

    Full Text Available In order to study aerosol-cloud interactions in cirrus clouds we apply a new multiple-mode ice microphysical scheme to the general circulation model ECHAM5-HAM. The multiple-mode ice microphysical scheme allows to analyse the competition between homogeneous freezing of solution droplets, deposition nucleation of pure dust particles, immersion freezing of coated dust particles and pre-existing ice. We base the freezing efficiencies of coated and pure dust particles on most recent laboratory data. The effect of pre-existing ice, which was neglected in previous ice nucleation parameterizations, is to deplete water vapour by depositional growth and thus prevent homogeneous and heterogeneous freezing from occurring. In a first step, we extensively tested the model and validated the results against in-situ measurements from various aircraft campaigns. The results compare well with observations; properties like ice crystal size and number concentration as well as supersaturation are predicted within the observational spread. We find that heterogeneous nucleation on mineral dust particles and the consideration of pre-existing ice in the nucleation process may lead to significant effects: globally, ice crystal number and mass are reduced by 10% and 5%, whereas the ice crystals size is increased by 3%. The reductions in ice crystal number are most pronounced in the tropics and mid-latitudes on the Northern Hemisphere. While changes in the microphysical and radiative properties of cirrus clouds in the tropics are mostly driven by considering pre-existing ice, changes in the northern hemispheric mid-latitudes mainly result from heterogeneous nucleation. The so called negative Twomey-effect in cirrus clouds is represented in ECHAM5-HAM. The net change in the radiation budget is −0.94 W m−2, implying that both, heterogeneous nucleation on dust and pre-existing ice have the potential to modulate cirrus properties in climate simulations and thus should be

  9. Nucleation and Oriented Textured Growth of Diamond Films on Si(100) via Electron Emission in Ho.t Filament Chemical Vapor Deposition

    Institute of Scientific and Technical Information of China (English)

    2000-01-01

    Oriented textured diamond films were obtained on Si(100) substrate via electron emission in hot filament chemical vapor deposition (HFCVD). A dc bias voltage relative to the filament was applied to the tungsten electrode between the substrate and the filament. The nucleation and subsequent growth of diamond films were characterized by scanning electron microscopy and Raman spectroscopy. The experimental results showed that the electron emission from the diamond coating on the electrode played a critical role during the nucleation.The maximum value of nucleation density was up to 1011 cm-2 on pristine Si surface at emission current of 250 mA. The effect of the electron emission on the reactive gas composition was analyzed by in situ infrared absorption, indicating that the concentration of CH3 and C2H2 near the substrate surface was extremely increased. This may be responsible for the enhanced nucleation by electron emission.

  10. Fabrication of Nanolaminates with Ultrathin Nanolayers Using Atomic Layer Deposition: Nucleation & Growth Issues

    Science.gov (United States)

    2009-02-01

    microscopy ( FE -SEM). • Construction of new experimental apparatus based on ALD reactor, glovebox and physical vapor deposition (PVD) chamber all...left the research group, Shih-Hui continued the barrier research and also made the FE -SEM measurements of film cracking resulting from compressive...Colorado, September 21, 2007. 25. "Atomic Layer Deposition: Fundamentals and Applications" (Invited Short Course), Sociedad Mexicana de Ciencia y

  11. Linking sulfate and phyllosilicate formation at Mawrth Vallis: Weathering in ancient low-latitude ice deposits

    Science.gov (United States)

    Niles, P. B.; Michalski, J.

    2009-12-01

    A currently outstanding question in martian geology is the mechanism by which large and numerous deposits of sulfate-rich and phyllosilicate-rich sedimentary rocks were generated. Hypotheses proposed to explain the origin of layered, sulfate-rich sediments at Meridiani Planum include: a) alteration by acidic fluids in a shallow and intermittently wet groundwater/playa/sebkha system, b) alteration of volcanic ash-flows by acidic sulfur-rich gases, c) reworking of sulfate-rich material by impact base surge, and d) acidic weathering within massive low-latitude ice deposits. We favor the ice-weathering model because this scenario can best explain the geologic and geochemical observations made from orbit and the surface. In addition, this model is in accord with an emerging picture of Mars in which ice-related processes have driven many aspects of sedimentation through time. The ice weathering model may also be relevant for understanding the origin of phyllosilicate deposits located beneath the sulfate-rich deposits at Meridiani Planum as well as at Mawrth Vallis. The Mawrth Vallis phyllosilicate deposits have several special characteristics: they are laterally extensive - occurring within stratigraphic windows over >~2*106 km2, and the mineralogical stratigraphy is the same everywhere that they are observed (Al-phyllosilicates overlying Fe/Mg-phyllosilicates). These observations can only be explained by a process that operated on a large spatial scale, just as with the sulfate deposits at Meridiani. However, if there were in fact massive ice deposits at low latitudes as called for in the Meridiani ice-weathering model, basal melting of these deposits may have driven a large regional groundwater system. Groundwater derived from extensive basal melting would likely have been alkaline due to increased water-rock interaction and increased dilution of the acid present in the ice deposit. Thus, the mineralogical stratigraphy could be explained by this alkaline groundwater

  12. The Metastable Persistence of Vapor-Deposited Amorphous Ice at Anomalously High Temperatures

    Science.gov (United States)

    Blake, David F.; Jenniskens, Peter; DeVincenzi, Donald L. (Technical Monitor)

    1995-01-01

    Studies of the gas release, vaporization behavior and infrared (IR) spectral properties of amorphous and crystalline water ice have direct application to cometary and planetary outgassing phenomena and contribute to an understanding of the physical properties of astrophysical ices. Several investigators report anomalous phenomena related to the warming of vapor-deposited astrophysical ice analogs. However gas release, ice volatilization and IR spectral features are secondary or tertiary manifestations of ice structure or morphology. These observations are useful in mimicking the bulk physical and chemical phenomena taking place in cometary and other extraterrestrial ices but do not directly reveal the structural changes which are their root cause. The phenomenological interpretation of spectral and gas release data is probably the cause of somewhat contradictory explanations invoked to account for differences in water ice behavior in similar temperature regimes. It is the microstructure, micromorphology and microchemical heterogeneity of astrophysical ices which must be characterized if the mechanisms underlying the observed phenomena are to be understood. We have been using a modified Transmission Electron Microscope to characterize the structure of vapor-deposited astrophysical ice analogs as a function of their deposition, temperature history and composition. For the present experiments, pure water vapor is deposited at high vacuum onto a 15 K amorphous carbon film inside an Hitachi H-500H TEM. The resulting ice film (approx. 0.05 micrometers thick) is warmed at the rate of 1 K per minute and diffraction patterns are collected at 1 K intervals. These patterns are converted into radial intensity distributions which are calibrated using patterns of crystalline gold deposited on a small part of the carbon substrate. The small intensity contributed by the amorphous substrate is removed by background subtraction. The proportions of amorphous and crystalline material

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

    Directory of Open Access Journals (Sweden)

    S. Unterstrasser

    2010-02-01

    Full Text Available Simulations of contrail-to-cirrus transition were performed with an LES model. In Part 1 the impact of relative humidity, temperature and vertical wind shear was explored in a detailed parametric study. Here, we study atmospheric parameters like stratification and depth of the supersaturated layer and processes which may affect the contrail evolution. We consider contrails in various radiation scenarios herein defined by the season, time of day and the presence of lower-level cloudiness which controls the radiance incident on the contrail layer. Under suitable conditions, controlled by the radiation scenario and stratification, radiative heating lifts the contrail-cirrus and prolongs its lifetime. The potential of contrail-driven secondary nucleation is investigated. We consider homogeneous nucleation and heterogeneous nucleation of preactivated soot cores released from sublimated contrail ice crystals. In our model the contrail dynamics triggered by radiative heating does not suffice to force homogeneous freezing of ambient liquid aerosol particles. Furthermore, our model results suggest that heterogeneous nucleation of preactivated soot cores is unimportant. Contrail evolution is not controlled by the depth of the supersaturated layer as long as it exceeds roughly 500 m. Deep fallstreaks however need thicker layers. A variation of the initial ice crystal number is effective during the whole evolution of a contrail. A cut of the soot particle emission by two orders of magnitude can reduce the contrail timescale by one hour and the optical thickness by a factor of 5. Hence future engines with lower soot particle emissions could potentially lead to a reduction of the climate impact of aviation.

  14. Importance of Chemical Composition of Ice Nuclei on the Formation of Arctic Ice Clouds

    Science.gov (United States)

    Keita, Setigui Aboubacar; Girard, Eric

    2016-09-01

    Ice clouds play an important role in the Arctic weather and climate system but interactions between aerosols, clouds and radiation remain poorly understood. Consequently, it is essential to fully understand their properties and especially their formation process. Extensive measurements from ground-based sites and satellite remote sensing reveal the existence of two Types of Ice Clouds (TICs) in the Arctic during the polar night and early spring. TICs-1 are composed by non-precipitating small (radar-unseen) ice crystals of less than 30 μm in diameter. The second type, TICs-2, are detected by radar and are characterized by a low concentration of large precipitating ice crystals ice crystals (>30 μm). To explain these differences, we hypothesized that TIC-2 formation is linked to the acidification of aerosols, which inhibits the ice nucleating properties of ice nuclei (IN). As a result, the IN concentration is reduced in these regions, resulting to a lower concentration of larger ice crystals. Water vapor available for deposition being the same, these crystals reach a larger size. Current weather and climate models cannot simulate these different types of ice clouds. This problem is partly due to the parameterizations implemented for ice nucleation. Over the past 10 years, several parameterizations of homogeneous and heterogeneous ice nucleation on IN of different chemical compositions have been developed. These parameterizations are based on two approaches: stochastic (that is nucleation is a probabilistic process, which is time dependent) and singular (that is nucleation occurs at fixed conditions of temperature and humidity and time-independent). The best approach remains unclear. This research aims to better understand the formation process of Arctic TICs using recently developed ice nucleation parameterizations. For this purpose, we have implemented these ice nucleation parameterizations into the Limited Area version of the Global Multiscale Environmental Model

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

    Energy Technology Data Exchange (ETDEWEB)

    Hiranuma, Naruki; Augustin-Bauditz, Stefanie; Bingemer, Heinz; Budke, Carsten; Curtius, J.; Danielczok, Anja; Diehl, K.; Dreischmeier, Katharina; Ebert, Martin; Frank, F.; Hoffmann, Nadine; Kandler, Kondrad; Kiselev, Alexei; Koop, Thomas; Leisner, Thomas; Mohler, Ottmar; Nillius, Bjorn; Peckhaus, Andreas; Rose, Diana; Weinbruch, Stephan; Wex, Heike; Boose, Yvonne; DeMott, Paul J.; Hader, John D.; Hill, Thomas; Kanji, Zamin; Kulkarni, Gourihar R.; Levin, Ezra; McCluskey, Christina; Murakami, Masataka; Murray, Benjamin J.; Niedermeier, Dennis; Petters, Markus D.; O' Sullivan, Daniel; Saito, Atsushi; Schill, Gregory; Tajiri, Takuya; Tolbert, Margaret A.; Welti, Andre; Whale, Thomas; Wright, Timothy; Yamashita, Katsuya

    2015-01-01

    Immersion freezing is the most relevant heterogeneous ice nucleation mechanism 3 through which ice crystals are formed in mixed-phase clouds. In recent years, an increasing 4 number of laboratory experiments utilizing a variety of instruments have examined immersion 5 freezing activity of atmospherically relevant ice nucleating particles (INPs). However, an 6 inter-comparison of these laboratory results is a difficult task because investigators have used 7 different ice nucleation (IN) measurement methods to produce these results. A remaining 8 challenge is to explore the sensitivity and accuracy of these techniques and to understand how 9 the IN results are potentially influenced or biased by experimental parameters associated with 10 these techniques. 11 Within the framework of INUIT (Ice Nucleation research UnIT), we distributed an 12 illite rich sample (illite NX) as a representative surrogate for atmospheric mineral dust 13 particles to investigators to perform immersion freezing experiments using different IN 14 measurement methods and to obtain IN data as a function of particle concentration, 15 temperature (T), cooling rate and nucleation time. Seventeen measurement methods were 16 involved in the data inter-comparison. Experiments with seven instruments started with the 17 test sample pre-suspended in water before cooling, while ten other instruments employed 18 water vapor condensation onto dry-dispersed particles followed by immersion freezing. The 19 resulting comprehensive immersion freezing dataset was evaluated using the ice nucleation 20 active surface-site density (ns) to develop a representative ns(T) spectrum that spans a wide 21 temperature range (-37 °C < T < -11 °C) and covers nine orders of magnitude in ns. 22 Our inter-comparison results revealed a discrepancy between suspension and dry-23 dispersed particle measurements for this mineral dust. While the agreement was good below ~-24 26 °C, the ice nucleation activity, expressed in ns, was

  16. Nucleation mechanism and microstructural assessment of SnO2 nanowires prepared by pulsed laser deposition

    Science.gov (United States)

    Chen, Z. W.; Lai, J. K. L.; Shek, C. H.

    2005-10-01

    Tin dioxide, SnO2, nanowires have been successfully synthesized by a pulsed laser deposition process based on a sintered cassiterite SnO2 target, being deposited on Si (100) substrates at room temperature. Transmission electron microscopy shows that nanowires are structurally perfect and uniform, and diameters range from 10 nm to 30 nm, and lengths of several hundreds nanometers to a few micrometers. X-ray diffraction and energy dispersive X-ray spectroscopy analysis indicate that the nanowires have the same crystal structure and chemical composition found in the tetragonal rutile form of SnO2. Selected area electron diffraction and high-resolution transmission electron microscopy reveal that the nanowires grow along the [110] growth direction. In addition to the fundamental Raman scattering peaks, the other two Raman scattering peaks are also observed. We discussed the possible reasons for the appearance of Raman scattering peaks at 518.7 and 701.8 cm-1. The growth process of the SnO2 nanowires is suggested to follow a vapor solid mechanism.

  17. A Wunda-full world? Carbon dioxide ice deposits on Umbriel and other Uranian moons

    Science.gov (United States)

    Sori, Michael M.; Bapst, Jonathan; Bramson, Ali M.; Byrne, Shane; Landis, Margaret E.

    2017-07-01

    Carbon dioxide has been detected on the trailing hemispheres of several Uranian satellites, but the exact nature and distribution of the molecules remain unknown. One such satellite, Umbriel, has a prominent high albedo annulus-shaped feature within the 131-km-diameter impact crater Wunda. We hypothesize that this feature is a solid deposit of CO2 ice. We combine thermal and ballistic transport modeling to study the evolution of CO2 molecules on the surface of Umbriel, a high-obliquity (∼98°) body. Considering processes such as sublimation and Jeans escape, we find that CO2 ice migrates to low latitudes on geologically short (100s-1000 s of years) timescales. Crater morphology and location create a local cold trap inside Wunda, and the slopes of crater walls and a central peak explain the deposit's annular shape. The high albedo and thermal inertia of CO2 ice relative to regolith allows deposits 15-m-thick or greater to be stable over the age of the solar system. We conclude that Wunda, located at low latitude (7.9° S) and near the center of the trailing hemisphere where CO2 detections are strongest, likely contains a solid CO2 ice deposit. We discuss prospects for similar CO2 ice deposits on crater floors on the other major Uranian moons, and predict that they are present on Ariel, Titania, and possibly Oberon (but not Miranda or smaller satellites). Such deposits have likely not been observed due to the limited nature of Voyager 2 image coverage.

  18. 冰核细菌Pseudomonas syringae是否可以影响大气的冰核核化过程%Do ice nucleation active bacteria effect on ice nucleation in the real atmosphere: Pseudomonas syringae

    Institute of Scientific and Technical Information of China (English)

    王亚玲; 杜睿; 梁宗敏; 周宇光

    2012-01-01

    In recent years, numerous investigations have highlighted the importance of bioaerosols in the atmosphere as effective cloud condensation nuclei (CCN) or ice nuclei (IN) during atmospheric physics and chemistry processes. Culturable strains of the ice nuclei active (INA) bacteria Pseudomonas syringae have been isolated from cloud water samples. This has led to an increase in research on bioaerosols associated with climatic effects. Such research is important because of the impacts that bacteria have in certain atmospheric cloud physical processes, especially in precipitation processes. This paper reports freezing temperatures, measured via Vali's even drops freezing method, of water droplets containing representative strains of three commonly recognized INA bacterial genera. These strains are Pseudomonas fluorescens, Erwinia uredovora, Xanthomonas campestris, Pseudomonas syringae pv. Panici and Pseudomonas syringae pv. Lachrymans. Results show that the first four bacteria strains do not have expected IN activity - freezing temperatures were -20.3±2.3℃, -21.8±2.3℃, -20.8±3.4℃, -19.9±3.3℃, respectively, when the concentration of the bacterial suspension was 108 cells/mL (OD600=0.25). These are not significantly different from the freezing temperature of ultrapure water droplets, -20.8±2.7℃. However, a higher freezing temperature of -5.0±0.8℃ was observed from measurement of P. Syringae pv. Lachrymans (psl-10) contained in water droplets with the same bacterial suspension concentration. Additionally, average freezing temperatures of the water droplets are correlated with bacterial concentration. With a concentration lower than 105 cells/mL, droplet freezing temperature decreased significantly, and was even close to that of ultrapure water when the concentration was less than 104 cells/mL. This seems to indicate there was no IN activity for bacteria at such a low concentration. Based on the results, a question is raised that should be verified in the

  19. Impact ejecta-induced melting of surface ice deposits on Mars

    Science.gov (United States)

    Weiss, David K.; Head, James W.

    2016-12-01

    Fluvial features present around impact craters on Mars can offer insight into the ancient martian climate and its relationship to the impact cratering process. The widespread spatial and temporal distribution of surface ice on Mars suggests that the interaction between impact cratering and surface ice could have been a relatively frequent occurrence. We explore the thermal and melting effects on regional surface ice sheets in this case, where an impact event occurs in regional surface ice deposits overlying a regolith/bedrock target. We provide an estimate for the post-impact temperature of martian ejecta as a function of crater diameter, and conduct thermal modeling to assess the degree to which contact melting of hot ejecta superposed on surface ice deposits can produce meltwater and carve fluvial features. We also evaluate whether fluvial features could form as a result of basal melting of the ice deposits in response to the thermal insulation provided by the overlying impact ejecta. Contact melting is predicted to occur immediately following ejecta emplacement over the course of hundreds of years to tens of kyr. Basal melting initiates when the 273 K isotherm rises through the crust and reaches the base of the ice sheet ∼0.1 to ∼1 Myr following the impact. We assess the range of crater diameters predicted to produce contact and basal melting of surface ice sheets, as well as the melt fluxes, volumes, timescales, predicted locations of melting (relative to the crater), and the associated hydraulic and hydrologic consequences. We find that the heat flux and surface temperature conditions required to produce contact melting are met throughout martian history, whereas the heat flux and surface temperature conditions to produce basal melting are met only under currently understood ancient martian thermal conditions. For an impact into a regional ice sheet, the contact and basal melting mechanisms are predicted to generate melt volumes between ∼10-1 and 105 km3

  20. Nucleation and initial growth of atomic layer deposited titanium oxide determined by spectroscopic ellipsometry and the effect of pretreatment by surface barrier discharge

    Energy Technology Data Exchange (ETDEWEB)

    Cameron, David C., E-mail: dccameron@mail.muni.cz [R& D Centre for Low-Cost Plasma and Nanotechnology Surface Modification, Masaryk University, Kotlářská 267/2, 611 37 Brno (Czech Republic); Krumpolec, Richard, E-mail: richard.krumpolec@fmph.uniba.sk [Department of Experimental Physics, Faculty of Mathematics, Physics and Informatics, Comenius University, Mlynská dolina, 842 4 Bratislava (Slovakia); Ivanova, Tatiana V., E-mail: tatiana.ivanova@lut.fi [ASTRaL team, Laboratory of Green Chemistry, Lappeenranta University of Technology, Sammonkatu 12, 50130 Mikkeli (Finland); Homola, Tomáš, E-mail: tomas.homola@mail.muni.cz [R& D Centre for Low-Cost Plasma and Nanotechnology Surface Modification, Masaryk University, Kotlářská 267/2, 611 37 Brno (Czech Republic); Černák, Mirko, E-mail: cernak@physics.muni.cz [R& D Centre for Low-Cost Plasma and Nanotechnology Surface Modification, Masaryk University, Kotlářská 267/2, 611 37 Brno (Czech Republic)

    2015-08-01

    Highlights: • Spectroscopic ellipsometry shows initial nucleation and growth process in atomic layer deposited titanium dioxide. • Quantum confinement effects were used to measure evolution of crystallite size. • Crystallite surface density can be extracted from ellipsometric surface roughness data and crystallite size. • Pretreatment of silicon substrates by diffuse coplanar surface barrier discharge has only minor effects on titanium dioxide film nucleation and growth. - Abstract: This paper reports on the use of spectroscopic ellipsometry to characterise the initial nucleation stage of the atomic layer deposition of the anatase phase of titanium dioxide on silicon substrates. Careful control and analysis of the ellipsometric measurements enables the determination of the evolution of crystallite diameter and surface density in the nucleation stage before a continuous film is formed. This growth behaviour is in line with atomic force microscopy measurements of the crystallite size. The crystallite diameter is a linear function of the number of ALD cycles with a slope of approximately 1.7 Å cycle{sup −1} which is equivalent to a layer growth rate of 0.85 Å cycle{sup −1} consistent with a ripening process which increases the crystallite size while reducing their density. The crystallite density decreases from ∼3 × 10{sup 17} m{sup −3} in the initial nucleation stages to ∼3 × 10{sup 15} m{sup −3} before the film becomes continuous. The effect of exposing the substrate to a diffuse coplanar surface barrier discharge in an air atmosphere before deposition was measured and only small differences were found: the plasma treated samples were slightly rougher in the initial stages and required a greater number of cycles to form a continuous film (∼80) compared to the untreated films (∼50). A thicker layer of native oxide was found after plasma treatment.

  1. Generalisation of Levine's prediction for the distribution of freezing temperatures of droplets: a general singular model for ice nucleation

    Directory of Open Access Journals (Sweden)

    R. P. Sear

    2013-04-01

    Full Text Available Models without an explicit time dependence, called singular models, are widely used for fitting the distribution of temperatures at which water droplets freeze. In 1950 Levine developed the original singular model. His key assumption was that each droplet contained many nucleation sites, and that freezing occurred due to the nucleation site with the highest freezing temperature. The fact that freezing occurs due to the maximum value out of large number of nucleation temperatures, means that we can apply the results of what is called extreme-value statistics. This is the statistics of the extreme, i.e., maximum or minimum, value of a large number of random variables. Here we use the results of extreme-value statistics to show that we can generalise Levine's model to produce the most general singular model possible. We show that when a singular model is a good approximation, the distribution of freezing temperatures should always be given by what is called the generalised extreme-value distribution. In addition, we also show that the distribution of freezing temperatures for droplets of one size, can be used to make predictions for the scaling of the median nucleation temperature with droplet size, and vice versa.

  2. Generalisation of Levine's prediction for the distribution of freezing temperatures of droplets: a general singular model for ice nucleation

    Directory of Open Access Journals (Sweden)

    R. P. Sear

    2013-07-01

    Full Text Available Models without an explicit time dependence, called singular models, are widely used for fitting the distribution of temperatures at which water droplets freeze. In 1950 Levine developed the original singular model. His key assumption was that each droplet contained many nucleation sites, and that freezing occurred due to the nucleation site with the highest freezing temperature. The fact that freezing occurs due to the maximum value out of a large number of nucleation temperatures, means that we can apply the results of what is called extreme-value statistics. This is the statistics of the extreme, i.e. maximum or minimum, value of a large number of random variables. Here we use the results of extreme-value statistics to show that we can generalise Levine's model to produce the most general singular model possible. We show that when a singular model is a good approximation, the distribution of freezing temperatures should always be given by what is called the generalised extreme-value distribution. In addition, we also show that the distribution of freezing temperatures for droplets of one size, can be used to make predictions for the scaling of the median nucleation temperature with droplet size, and vice versa.

  3. 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.

  4. 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.

  5. Surface Water-Ice Deposits in the Northern Shadowed Regions of Ceres

    Science.gov (United States)

    Platz, T.; Nathues, A.; Schorghofer, N.; Preusker, F.; Mazarico, E.; Schroeder, S. E.; Byrne, S.; Kneissl, T.; Schmedemann, N.; Combe, J.-P.; Schaefer, M.; Thangjam, G. S.; Hoffmann, M.; Gutierrez-Marques, P.; Landis, M. E.; Dietrich, W.; Ripken, J.; Matz, K. D.; Russell, C. T.

    2016-01-01

    Ceres, a dwarf planet located in the main asteroid belt, has a low bulk density, and models predict that a substantial amount of water ice is present in its mantle and outer shell. The Herschel telescope and the Dawn spacecraft have observed the release of water vapor from Ceres, and exposed water ice has been detected by Dawn on its surface at mid-latitudes. Water molecules from endogenic and exogenic sources can also be cold-trapped in permanent shadows at high latitudes, as happens on the Moon and Mercury. Here we present the first image-based survey of Ceres's northern permanent shadows and report the discovery of bright deposits in cold traps. We identify a minimum of 634 permanently shadowed craters. Bright deposits are detected on the floors of just 10 of these craters in multiscattered light. We spectroscopically identify one of the bright deposits as water ice. This detection strengthens the evidence that permanently shadowed areas have preserved water ice on airless planetary bodies.

  6. Post-depositional migration and preservation of methanesulfonic acid (MSA) in polar ice cores

    Science.gov (United States)

    Osman, M.; Marchal, O.; Guo, W.; Das, S. B.; Evans, M. J.

    2015-12-01

    Methanesulfonic acid (MSA; CH3SO3-) in ice cores is a unique, high-resolution proxy of regional sea ice behavior, marine primary productivity, and synoptic climatology. Significant uncertainties remain, however, in both our understanding of the production and transfer of MSA to the ice sheet, as well as its preservation over time, compromising the paleoclimatological utility of the proxy. Here we apply a numerical modeling approach to quantitatively investigate the post-depositional processes affecting MSA migration and preservation within the firn and ice column, building on recent observational and theoretical studies. Our model allows us to evaluate the timing and magnitude of the vertical movement of MSA in response to varying influences, including the competing effects of 1) concentration gradients of sea-salts typically deposited asynchronously to MSA, 2) snow accumulation and densification rates, and 3) in situ temperature gradients. We first test the model against a recently collected ice core from a high accumulation site in coastal West Antarctica, where monthly-resolved MSA records show an abrupt shift from a summer-to-winter maximum in MSA at ~23m depth (ρ ≈ 650 kg/m3), near the firn-ice transition. We find our model to be a robust predictor of the observed migrational features in this record, capturing both (i) the abrupt shift in summer-to-winter maximal concentrations of MSA (steady state ≈ 3.2 yrs), and (ii) the depression of the seasonal amplitude at depth. Further, our modeling results suggest post-depositional effects can lead to substantial interannual alteration of the MSA signal, contrary to previous assumptions that MSA migration is confined within annual layers at high accumulation sites. Using a broad range of polar MSA records and their associated, site-specific environmental conditions, we will evaluate the fidelity of subannual to interannual variability of MSA records and systematically determine the factors conducive to its

  7. Evaluating the Age of Buried Ice in Antarctica Using Ashfall Deposits: New Insights from Deposit Morphology, Grain Shape, and LA-ICP-MS Trace-Element Geochemistry

    Science.gov (United States)

    Lewis, A. R.; Marchant, D. R.

    2003-12-01

    Dating of buried ice in the western Dry Valleys region relies on 40Ar/39Ar analysis of ashfall deposits within sublimation tills that rest directly on stagnant glacier ice. The oldest ice so dated is >8.1 Ma. The fundamental assumption is that dated ashes are in-situ and have not been transported from surface deposits elsewhere in the Dry Valleys region. Given that the surface of sublimation tills shows well-developed patterned ground, the presumption of ground stability and long-term preservation of in-situ ashfall is questioned. As a test of ground stability, we examined ash-deposit morphology, grain shape, and glass-shard trace-element geochemistry from several ashfall deposits used to provide limiting ages on buried ice and tills in the western Dry Valleys. Detailed field analyses show that ashfall that collects in sublimation tills over buried ice occurs in one of three morphologic settings: surface troughs that delineate sand-wedge polygons, void spaces in gravel-and-cobble lags that overlie active sand wedges, and 1 to 2-cm-wide thermal contraction cracks. Post-depositional sublimation of underlying ice may distort initial deposit morphology through uneven surface lowering. Microscopic analyses of concentrated ashfall deposits that lack detrital sand grains show highly angular glass shards that preserve delicate hair-like spires and thin bubble-wall vesicles. Grain edges are sharp with no chipped, fractured, or pitted surfaces. In contrast, ash deposits containing detrital sand grains show subangular to subrounded shard morphologies with concave fractures and pits on grain edges, all of which are suggestive of abrasion during transport. In such deposits, grains preserving delicate bubble walls and hair-like spires are conspicuously absent. Laser ablation-inductively coupled plasma-mass spectrometry shows that glass shards within each ashfall deposit have uniform trace-element geochemical signatures. If ashfall were eroded and transported after initial

  8. Nucleation and growth of hydroxyapatite on arc-deposited TiO{sub 2} surfaces studied by quartz crystal microbalance with dissipation

    Energy Technology Data Exchange (ETDEWEB)

    Lilja, Mirjam [Division for Nanotechnology and Functional Materials, Department of Engineering Sciences, The Ångström Laboratory, Uppsala University, Box 534, 75121 Uppsala (Sweden); Sandvik Coromant Sverige AB, Lerkrogsvägen 19, 12680 Stockholm (Sweden); Butt, Umer [Sandvik Coromant Sverige AB, Lerkrogsvägen 19, 12680 Stockholm (Sweden); Berzelii Centre EXSELENT on Porous Materials and Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, 114 18 Stockholm (Sweden); Shen, Zhijian [Berzelii Centre EXSELENT on Porous Materials and Department of Materials and Environmental Chemistry, Arrhenius Laboratory, Stockholm University, 114 18 Stockholm (Sweden); Bjöörn, Dorota, E-mail: dorota.bjoorn@sandvik.com [Sandvik Coromant Sverige AB, Lerkrogsvägen 19, 12680 Stockholm (Sweden)

    2013-11-01

    Understanding of nucleation and growth kinetics of biomimetically deposited hydroxyapatite (HA) on crystalline TiO{sub 2} surfaces is important with respect to the application and performance of HA as functional implant coatings. Arc-evaporation was used to deposit TiO{sub 2} coatings dominated by anatase phase, rutile phase or their mixtures. Subsequent formation of HA from phosphate buffered saline solution (PBS) was investigated in real-time using in situ quartz crystal microbalance with dissipation technique (QCM-D). Scanning electron microscopy (SEM) and X-ray diffraction (XRD) were employed to characterize the presence, morphology and crystal structure of TiO{sub 2} coatings and the formed HA. Increasing temperature of the PBS, increasing flow rate and applying a higher ion concentration in solution were found to accelerate HA nucleation process and hence affect growth kinetics. Lower PBS temperature resulted in the formation of HA coatings with flake-like morphology and increasing HA porosity. All TiO{sub 2} coatings under study enabled HA formation at body temperature, while in contrast Ti reference surfaces only supported HA nucleation and growth at elevated temperatures. QCM-D technique is a powerful tool for studying the impact of process parameters during biomimetic coating deposition on coating structure evolution in real time and provides valuable information for understanding, optimizing as well as tailoring the biomimetic HA growth processes.

  9. Generalisation of Levine's prediction for the distribution of freezing temperatures of droplets: A general singular model for ice nucleation

    CERN Document Server

    Sear, Richard P

    2013-01-01

    Models without an explicit time dependence, called singular models, are widely used for fitting the distribution of temperatures at which water droplets freeze. In 1950 Levine developed the original singular model. His key assumption was that each droplet contained many nucleation sites, and that freezing occurred due to the nucleation site with the highest freezing temperature. The fact that freezing occurs due to the maximum value out of large number of nucleation temperatures, means that we can apply the results of what is called extreme-value statistics. This is the statistics of the extreme, i.e., maximum or minimum, value of a large number of random variables. Here we use the results of extreme-value statistics to show that we can generalise Levine's model to produce the most general singular model possible. We show that when a singular model is a good approximation, the distribution of freezing temperatures should always be given by what is called the generalised extreme-value distribution. In addition...

  10. 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.; hide

    2017-01-01

    Black carbon (BC) concentrations observed in 22 snowpits sampled in the northwest sector of the Greenland ice sheet in April 2014 have allowed us to identify a strong and widespread BC aerosol deposition event, which was dated to have accumulated in the pits from two snow storms between 27 July and 2 August 2013. This event comprises a significant portion (57 on average across all pits) of total BC deposition over 10 months (July 2013 to April 2014). Here we link this deposition event to forest fires burning in Canada during summer 2013 using modeling and remote sensing tools. Aerosols were detected by both the Cloud-Aerosol Lidar with Orthogonal Polarization (on board CALIPSO) and Moderate Resolution Imaging Spectroradiometer (Aqua) instruments during transport between Canada and Greenland. We use high-resolution regional chemical transport modeling (WRF-Chem) combined with high-resolution fire emissions (FINNv1.5) to study aerosol emissions, transport, and deposition during this event. The model captures the timing of the BC deposition event and shows that fires in Canada were the main source of deposited BC. However, the model underpredicts BC deposition compared to measurements at all sites by a factor of 2100. Underprediction of modeled BC deposition originates from uncertainties in fire emissions and model treatment of wet removal of aerosols. Improvements in model descriptions of precipitation scavenging and emissions from wildfires are needed to correctly predict deposition, which is critical for determining the climate impacts of aerosols that originate from fires.

  11. 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.

  12. Post-depositional migration and signal reconstruction of methanesulfonic acid (MSA) in polar ice cores

    Science.gov (United States)

    Osman, Matthew; Das, Sarah B.; Marchal, Olivier; Evans, Matthew J.

    2017-04-01

    Methanesulfonic acid (MSA; CH3SO3H) in polar ice cores is a unique proxy of marine primary productivity, synoptic atmospheric transport, and regional sea ice behavior. However, MSA can be unstable within the ice column, leading to uncertainties surrounding the integrity of its paleoclimatic signal. Here, we use ice core records coupled with forward and inverse numerical models to investigate the post-depositional processes affecting the migration of MSA within the firn and ice column, and attempt to reconstruct the original signal in the ice column. The forward model, detailing the vertical diffusive transport of soluble impurities through supercooled liquid pathways, allows us to systematically assess the contribution of varying influences on the post-depositional migration of MSA. Our results show that two site-specific variables in particular, i) snow accumulation rate, and ii) seasonal concentration gradients of Na+(typically the highest concentration sea salt), may be sufficient to reasonably predict the timing and magnitude of MSA migration within the ice column. However, at present the temporal accuracy of the forward MSA migration model remains limited by inadequate constraints on the diffusion coefficient of MSA, DMS-. Specifically, we find that previous estimates of DMS-are unable to reproduce, within significant uncertainty, the progressive phase alignment of the MSA and Na+signals observed in real Antarctic ice cores. To attempt to correct for the effects of post-depositional migration, we combine recent high-resolution West Antarctic MSA data using sequential methods from optimal control theory (a Kalman filter and a related fixed-interval smoother) to reconstruct and provide uncertainty estimates on the original, pre-migrated MSA profile. We find that although the reconstructed MSA profile provides a reasonable estimate of the original MSA signal, the large uncertainties associated with this reconstructed signal cannot be objectively discriminated

  13. 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...... at 355 nm at a fluence of 2.5-12 J/cm(2). Even at this high fluence, Fourier transform infrared spectroscopy (FTIR) indicates a chemical structure of the deposit close to that of the un-irradiated PEG. Matrix assisted laser desorption and ionization (MALDI) and gel permeation chromatography (GPC) show...... that the mass distribution of the deposited PEG is similar to that of the starting material. Optical pictures of the films show particle structures of PEG of a size up to 5-10 mu m. The deposition rate measured with a quartz crystal microbalance is typically of the order of 1 ng/ (cm(2) shot). (c) 2005 Elsevier...

  14. An improved ice cloud formation parameterization in the EMAC model

    Science.gov (United States)

    Bacer, Sara; Pozzer, Andrea; Karydis, Vlassis; Tsimpidi, Alexandra; Tost, Holger; Sullivan, Sylvia; Nenes, Athanasios; Barahona, Donifan; Lelieveld, Jos

    2017-04-01

    Cirrus clouds cover about 30% of the Earth's surface and are an important modulator of the radiative energy budget of the atmosphere. Despite their importance in the global climate system, there are still large uncertainties in understanding the microphysical properties and interactions with aerosols. Ice crystal formation is quite complex and a variety of mechanisms exists for ice nucleation, depending on aerosol characteristics and environmental conditions. Ice crystals can be formed via homogeneous nucleation or heterogeneous nucleation of ice-nucleating particles in different ways (contact, immersion, condensation, deposition). We have implemented the computationally efficient cirrus cloud formation parameterization by Barahona and Nenes (2009) into the EMAC (ECHAM5/MESSy Atmospheric Chemistry) model in order to improve the representation of ice clouds and aerosol-cloud interactions. The parameterization computes the ice crystal number concentration from precursor aerosols and ice-nucleating particles accounting for the competition between homogeneous and heterogeneous nucleation and among different freezing modes. Our work shows the differences and the improvements obtained after the implementation with respect to the previous version of EMAC.

  15. Minimalist model of ice microphysics in mixed-phase stratiform clouds

    Science.gov (United States)

    Yang, F.; Ovchinnikov, M.; Shaw, R. A.

    2013-12-01

    The question of whether persistent ice crystal precipitation from supercooled layer clouds can be explained by time-dependent, stochastic ice nucleation is explored using an approximate, analytical model and a large-eddy simulation (LES) cloud model. The updraft velocity in the cloud defines an accumulation zone, where small ice particles cannot fall out until they are large enough, which will increase the residence time of ice particles in the cloud. Ice particles reach a quasi-steady state between growth by vapor deposition and fall speed at cloud base. The analytical model predicts that ice water content (wi) has a 2.5 power-law relationship with ice number concentration (ni). wi and ni from a LES cloud model with stochastic ice nucleation confirm the 2.5 power-law relationship, and initial indications of the scaling law are observed in data from the Indirect and Semi-Direct Aerosol Campaign. The prefactor of the power law is proportional to the ice nucleation rate and therefore provides a quantitative link to observations of ice microphysical properties. Ice water content (wi) and ice number concentration (ni) relationship from LES. a and c: Accumulation zone region; b and d: Selective accumulation zone region. Black lines in c and d are best fitted 2.5 slope lines. Colors in Figures a and b represent updraft velocity, while colors in c and d represent altitude. The cloud base and top are at about 600 m and 800 m, respectively. Ice water content (wi) and ice number concentration (ni) relationship for two ice nucleation rates. Blue points are from LES with low ice nucleation rate and red points with high ice nucleation rate. Solid and dashed lines are best fitted 2.5 slope lines.

  16. Atomic Layer Deposition of Titanium Oxide on Single-Layer Graphene: An Atomic-Scale Study toward Understanding Nucleation and Growth

    Science.gov (United States)

    2017-01-01

    Controlled synthesis of a hybrid nanomaterial based on titanium oxide and single-layer graphene (SLG) using atomic layer deposition (ALD) is reported here. The morphology and crystallinity of the oxide layer on SLG can be tuned mainly with the deposition temperature, achieving either a uniform amorphous layer at 60 °C or ∼2 nm individual nanocrystals on the SLG at 200 °C after only 20 ALD cycles. A continuous and uniform amorphous layer formed on the SLG after 180 cycles at 60 °C can be converted to a polycrystalline layer containing domains of anatase TiO2 after a postdeposition annealing at 400 °C under vacuum. Using aberration-corrected transmission electron microscopy (AC-TEM), characterization of the structure and chemistry was performed on an atomic scale and provided insight into understanding the nucleation and growth. AC-TEM imaging and electron energy loss spectroscopy revealed that rocksalt TiO nanocrystals were occasionally formed at the early stage of nucleation after only 20 ALD cycles. Understanding and controlling nucleation and growth of the hybrid nanomaterial are crucial to achieving novel properties and enhanced performance for a wide range of applications that exploit the synergetic functionalities of the ensemble.

  17. Severnaya Zemlya, Arctic Russia: a nucleation area for Kara Sea ice sheets during the Middle to Late Quaternary

    NARCIS (Netherlands)

    Moller, P.; Lubinski, D.J.; Ingolfsson, O.; Forman, S.L.; Seidenkrantz, M.S.; Bolshiyanov, D.Y.; Lokrantz, H.; Antonov, O.; Pavlov, M.; Ljung, K.; Zeeberg, J.J.; Andreev, A.

    2006-01-01

    Quaternary glacial stratigraphy and relative sea-level changes reveal at least four expansions of the Kara Sea ice sheet over the Severnaya Zemlya Archipelago at 79°N in the Russian Arctic, as indicated from tills interbedded with marine sediments, exposed in stratigraphic superposition, and from

  18. Severnaya Zemlya, arctic Russia: a nucleation area for Kara Sea ice sheets during the Middle to Late Quaternary

    DEFF Research Database (Denmark)

    Möller, Per; Lubinski, David J.; Ingólfsson, Ólafur

    2006-01-01

    Quaternary glacial stratigraphy and relative sea-level changes reveal at least four expansions of the Kara Sea ice sheet over the Severnaya Zemlya Archipelago at 79°N in the Russian Arctic, as indicated from tills interbedded with marine sediments, exposed in stratigraphic superposition, and from...

  19. Severnaya Zemlya, Arctic Russia: a nucleation area for Kara Sea ice sheets during the Middle to Late Quaternary

    NARCIS (Netherlands)

    Moller, P.; Lubinski, D.J.; Ingolfsson, O.; Forman, S.L.; Seidenkrantz, M.S.; Bolshiyanov, D.Y.; Lokrantz, H.; Antonov, O.; Pavlov, M.; Ljung, K.; Zeeberg, J.J.; Andreev, A.

    2006-01-01

    Quaternary glacial stratigraphy and relative sea-level changes reveal at least four expansions of the Kara Sea ice sheet over the Severnaya Zemlya Archipelago at 79°N in the Russian Arctic, as indicated from tills interbedded with marine sediments, exposed in stratigraphic superposition, and from ra

  20. Application of linear polarized light for the discrimination of frozen and liquid droplets in ice nucleation experiments

    Directory of Open Access Journals (Sweden)

    T. Clauss

    2012-08-01

    Full Text Available We report on the development and test results of the new optical particle counter TOPS-Ice (Thermostabilized Optical Particle Spectrometer for the detection of Ice particles. The instrument uses measurements of the depolarized component of light scattered by single particles into the near-forward direction (42.5° ± 12.7° to distinguish between spherical and non-spherical particles. This approach allows the differentiation between liquid water droplets (spherical and ice particles (non-spherical having similar volume equivalent sizes and therefore can be used to determine the fraction of frozen droplets in a typical immersion freezing experiment. We show that the numerical simulation of the light scattering on non-spherical particles (ellipsoids in random orientation with account for the actual scattering geometry used in the instrument supports the validity of the approach, even though the cross polarized component of the light scattered by spherical droplets is not vanishing in this scattering angle. For the separation of the ice particle mode from the liquid droplet mode, we use the width of the pulse detected in the depolarization channel instead of the pulse height. Exploiting the intrinsic relationship between pulse height and pulse width for Gaussian pulses allows us to calculate the fraction of frozen droplets even if the liquid droplet mode dominates the particle ensemble. We present test results obtained with TOPS-Ice in the immersion freezing experiments at the laminar diffusion chamber LACIS (Leipzig Aerosol Cloud Interaction Simulator and demonstrate the excellent agreement with the data obtained in the same experiment with a different optical instrument. Finally, the advantages of using the cross-polarized light measurements for the differentiation of liquid and frozen droplets in the realistic immersion freezing experiments are discussed.

  1. Application of linear polarized light for the discrimination of frozen and liquid droplets in ice nucleation experiments

    Directory of Open Access Journals (Sweden)

    T. Clauss

    2013-04-01

    Full Text Available We report on the development and test results of the new optical particle counter TOPS-Ice (Thermo-stabilized Optical Particle Spectrometer for the detection of Ice. The instrument uses measurements of the cross-polarized scattered light by single particles into the near-forward direction (42.5° ± 12.7° to distinguish between spherical and non-spherical particles. This approach allows the differentiation between liquid water droplets (spherical and ice particles (non-spherical having similar volume-equivalent sizes and therefore can be used to determine the fraction of frozen droplets in a typical immersion freezing experiment. We show that the numerical simulation of the light scattered on non-spherical particles (spheroids in random orientation considering the actual scattering geometry used in the instrument supports the validity of the approach, even though the cross-polarized component of the light scattered by spherical droplets does not vanish in this scattering angle. For the separation of the ice particle mode from the liquid droplet mode, we use the width of the pulse detected in the depolarization channel instead of the pulse height. Exploiting the intrinsic relationship between pulse height and pulse width for Gaussian pulses allows us to calculate the fraction of frozen droplets even if the liquid droplet mode dominates the particle ensemble. We present test results obtained with TOPS-Ice in the immersion freezing experiments at the laminar diffusion chamber LACIS (Leipzig Aerosol Cloud Interaction Simulator and demonstrate the excellent agreement with the data obtained in similar experiments with a different optical instrument. Finally, the advantages of using the cross-polarized light measurements for the differentiation of liquid and frozen droplets in the realistic immersion freezing experiments are discussed.

  2. Dynamical Conditions of Ice Supersaturation and Ice Nucleation in Convective Systems: A Comparative Analysis Between in Situ Aircraft Observations and WRF Simulations

    Science.gov (United States)

    D’Alessandro, John J.; Diao, Minghui; Wu, Chenglai; Liu, Xiaohong; Chen, Ming; Morrison, Hugh; Eidhammer, Trude; Jensen, Jorgen B.; Bansemer, Aaron; Zondlo, Mark A.; hide

    2017-01-01

    Occurrence frequency and dynamical conditions of ice supersaturation (ISS, where relative humidity with respect to ice (RHi) greater than 100%) are examined in the upper troposphere around convective activity. Comparisons are conducted between in situ airborne observations and the Weather Research and Forecasting model simulations using four double-moment microphysical schemes at temperatures less than or or equal to -40degdegC. All four schemes capture both clear-sky and in-cloud ISS conditions. However, the clear-sky (in-cloud) ISS conditions are completely (significantly) limited to the RHi thresholds of the Cooper parameterization. In all of the simulations, ISS occurrence frequencies are higher by approximately 3-4 orders of magnitude at higher updraft speeds (greater than 1 m s(exp -1) than those at the lower updraft speeds when ice water content (IWC) greater than 0.01 gm(exp -3), while observations show smaller differences up to approximately 1-2 orders of magnitude. The simulated ISS also occurs less frequently at weaker updrafts and downdrafts than observed. These results indicate that the simulations have a greater dependence on stronger updrafts to maintain/generate ISS at higher IWC. At lower IWC (less than or equal or 0.01 gm(exp -3), simulations unexpectedly show lower ISS frequencies at stronger updrafts. Overall, the Thompson aerosol-aware scheme has the closest magnitudes and frequencies of ISS greater than 20% to the observations, and the modified Morrison has the closest correlations between ISS frequencies and vertical velocity at higher IWC and number density. The Cooper parameterization often generates excessive ice crystals and therefore suppresses the frequency and magnitude of ISS, indicating that it should be initiated at higher ISS (e.g.,lees than or equal to 25%).

  3. Remnant buried ice in the equatorial regions of Mars: Morphological indicators associated with the Arsia Mons tropical mountain glacier deposits

    Science.gov (United States)

    Scanlon, Kathleen E.; Head, James W.; Marchant, David R.

    2015-06-01

    The fan-shaped deposit (FSD) on the western and northwestern flanks of Arsia Mons is the remnant of tropical mountain glaciers, deposited several tens to hundreds of millions of years ago during periods of high spin-axis obliquity. Previous workers have argued that the Smooth Facies in the FSD contains a core of ancient glacial ice. Here, we find evidence that additional glacial ice remains preserved within several other landforms in the Smooth Facies and Ridged Facies. These include landforms that we interpret as kame and kettle topography on the basis of their distribution, size, and morphologies ranging progressively from knobs to degraded knobs to pits. We argue that some moraines in the Ridged Facies are ice-cored on the basis of their interactions with lava flows and the axial troughs at the crests of some moraines. We also argue that dunes with axial troughs, found in and surrounding the FSD, are the remnants of sediment-covered snow dunes formed by reworking of snow or glacial ice, and that the axial troughs form as tension cracks in the sediment and deepen by sublimation of the underlying ice. Long-term preservation of water ice in equatorial environments is assisted by a meters- to decameters-thick debris cover (lag) formed from sublimation of dirty ice, as well as burial beneath volcanic tephra and aeolian deposits. This ancient ice could contain preserved biosignatures, provide information on Martian climate and atmospheric history, and serve as a resource for human exploration.

  4. Deglaciated areas of Kilimanjaro as a source of volcanic trace elements deposited on the ice cap during the late Holocene

    Science.gov (United States)

    Gabrielli, P.; Hardy, D. R.; Kehrwald, N.; Davis, M.; Cozzi, G.; Turetta, C.; Barbante, C.; Thompson, L. G.

    2014-06-01

    Ice fields on Kilimanjaro (5895 m a.s.l., Tanzania) are retreating and 85% of the ice cover has been lost since 1912. The degree to which this recession is exceptional during the Holocene is uncertain, as age control of the entire ice stratigraphy exists only for the very shallow and very bottom ice of the Northern Ice Field. This empirical evidence suggests that the Kilimanjaro ice cover may be a persistent Holocene feature, while a model based on maximum possible extent and a constant shrinkage rate of the summit glaciers suggests a cyclic decay time on the order of one to two centuries. Today the mass balance of these ice fields is negative and no persistent ice accumulation zones are observed over multiannual scales. The expanding deglaciated area within the Kilimanjaro caldera should act as an increasingly larger and productive source of volcanic-origin aeolian dust that is quickly deposited onto the surface of the adjacent ice fields, particularly in the seasonal absence of caldera snow cover. Variations in the local dust influx may directly influence albedo and the energy balance of these ice fields. Investigating the characteristics of insoluble material entrapped in the ice remnants of Kilimanjaro can thus provide insights into the extent of ice and/or continuity of the summit snow cover through time. Here we report the trace element composition linked to the insoluble particles entrapped in Holocene Kilimanjaro ice in the context of the current understanding of the past ice accumulation processes (including solid precipitations and ablation) contributing to build the horizontal caldera ice fields. For this purpose we analysed an ice core drilled to bedrock from the Northern Ice Field thought to span the late Holocene (2200 BC-1950 AD). The ultra low trace element concentrations recorded in this Kilimanjaro core are consistent with a generally low volcanic dust source availability (i.e. limited exposure of the deglaciated area in the caldera) and fairly

  5. 果汁冷冻浓缩中生物冰核的成冰作用及初步应用%Bacterial ice nucleation and its applications in the freeze concentration of fruit juice

    Institute of Scientific and Technical Information of China (English)

    何松; 胡卓炎; 孙福在; 赵廷昌; 钟士清

    2001-01-01

    介绍了冰核细菌促进成冰的机制,并结合国外有关报道和我们的研究结果,论述了冰核细菌在食品冷冻浓缩中导致冰晶形成的结构、冷冻效率、应用前的预处理及食用级冰核细菌在果汁中的应用情况,最后展望了未来的研究方向。%Freeze concentration of foods using ice-nucleation active bacteria was reviewed, including the ice formation mechanism, freezing texture, freezing efficiency, preliminary treatments of this bacterium before it was applied, and applications of food-gradeice-nucleation active bacteria in freeze concentration of fruit juice.

  6. Application of Ice-nucleation Active Bacteria in Freeze Concentration of Foods%冰核活性细菌及其在食品冻结浓缩中的应用

    Institute of Scientific and Technical Information of China (English)

    胡卓炎; 何松; 孙福在; 赵廷昌; 钟士清

    2001-01-01

    Freeze concentration of foods using ice-nucleation active bacteria was reviewed. It indicated that bacterial ice nuclei can not only increase the freezing point, but also shorten the freezing time of the treated foods. Furthermore, larger ice crystals can be made during the freezing. It suggested that this bacteria should be applied to freeze concentration of foods to obtain a concentrated product for efficient freezing and retaining its original flavor. This paper reviewed the ice-made mechanism, preliminary treatments, freezing efficiency, freezing texture and applications of ice-nucleation active bacteria in freeze concentration of foods. Finally, it looked ahead the prospects of this technique in the future.%介绍冰核细菌的成冰机制、预处理工艺及在食品中的冷冻效率、冰晶形成结构与应用方面的最新进展,最后展望未来的发展趋势。

  7. 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.

  8. Short review on Controlled Nucleation

    Directory of Open Access Journals (Sweden)

    Gupta Anuj

    2012-09-01

    Full Text Available Freeze-drying (also known as lyophilization or cryodesiccation is a dehydration process mainly used to preserve for perishable material and this method make the material more convenient for transport. Freezedrying works by freezing the material and then reducing the surrounding pressure and giving sufficient heat to allow the frozen water into the material to sublime directly from the solid phase to gas phase. Sublimation is the transition of a substance from the solid to the vapor state, without first passing through an intermediate liquid phase. A method to achieve controlled ice nucleation during the freeze-drying process using an ice fog, vial treatment, ultrasound, additives and electro freezing technique was demonstrated in an earlier report. And by the potential of a high electric field was utilized to induce ice nucleus formation in aqueous solutions. Using this technique it was possible to reduce the primary drying time during lyophilization. [1] Many technical issues surrounding the freeze-drying process have been addressed over the past several decades. Better understanding of critical formulation characteristics and cycle conditions. There are two types of technique for nucleation 1 Uncontrolled Nucleation, 2 Controlled Nucleation. The objectives of the present study simply introduce controlled Nucleation is the rapid ice nucleation in freeze drying technique. [2

  9. Impact of dust deposition on the albedo of Vatnajökull ice cap, Iceland

    Science.gov (United States)

    Wittmann, Monika; Dorothea Groot Zwaaftink, Christine; Steffensen Schmidt, Louise; Guðmundsson, Sverrir; Pálsson, Finnur; Arnalds, Olafur; Björnsson, Helgi; Thorsteinsson, Throstur; Stohl, Andreas

    2017-03-01

    Deposition of small amounts of airborne dust on glaciers causes positive radiative forcing and enhanced melting due to the reduction of surface albedo. To study the effects of dust deposition on the mass balance of Brúarjökull, an outlet glacier of the largest ice cap in Iceland, Vatnajökull, a study of dust deposition events in the year 2012 was carried out. The dust-mobilisation module FLEXDUST was used to calculate spatio-temporally resolved dust emissions from Iceland and the dispersion model FLEXPART was used to simulate atmospheric dust dispersion and deposition. We used albedo measurements at two automatic weather stations on Brúarjökull to evaluate the dust impacts. Both stations are situated in the accumulation area of the glacier, but the lower station is close to the equilibrium line. For this site ( ˜ 1210 m a.s.l.), the dispersion model produced 10 major dust deposition events and a total annual deposition of 20.5 g m-2. At the station located higher on the glacier ( ˜ 1525 m a.s.l.), the model produced nine dust events, with one single event causing ˜ 5 g m-2 of dust deposition and a total deposition of ˜ 10 g m-2 yr-1. The main dust source was found to be the Dyngjusandur floodplain north of Vatnajökull; northerly winds prevailed 80 % of the time at the lower station when dust events occurred. In all of the simulated dust events, a corresponding albedo drop was observed at the weather stations. The influence of the dust on the albedo was estimated using the regional climate model HIRHAM5 to simulate the albedo of a clean glacier surface without dust. By comparing the measured albedo to the modelled albedo, we determine the influence of dust events on the snow albedo and the surface energy balance. We estimate that the dust deposition caused an additional 1.1 m w.e. (water equivalent) of snowmelt (or 42 % of the 2.8 m w.e. total melt) compared to a hypothetical clean glacier surface at the lower station, and 0.6 m w.e. more melt (or 38 % of

  10. Atmospheric Mercury Depositional Chronology Reconstructed from Lake Sediments and Ice Core in the Himalayas and Tibetan Plateau.

    Science.gov (United States)

    Kang, Shichang; Huang, Jie; Wang, Feiyue; Zhang, Qianggong; Zhang, Yulan; Li, Chaoliu; Wang, Long; Chen, Pengfei; Sharma, Chhatra Mani; Li, Qing; Sillanpää, Mika; Hou, Juzhi; Xu, Baiqing; Guo, Junming

    2016-03-15

    Alpine lake sediments and glacier ice cores retrieved from high mountain regions can provide long-term records of atmospheric deposition of anthropogenic contaminants such as mercury (Hg). In this study, eight lake sediment cores and one glacier ice core were collected from high elevations across the Himalaya-Tibet region to investigate the chronology of atmospheric Hg deposition. Consistent with modeling results, the sediment core records showed higher Hg accumulation rates in the southern slopes of the Himalayas than those in the northern slopes in the recent decades (post-World War II). Despite much lower Hg accumulation rates obtained from the glacier ice core, the temporal trend in the Hg accumulation rates matched very well with that observed from the sediment cores. The combination of the lake sediments and glacier ice core allowed us to reconstruct the longest, high-resolution atmospheric Hg deposition chronology in High Asia. The chronology showed that the Hg deposition rate was low between the 1500s and early 1800, rising at the onset of the Industrial Revolution, followed by a dramatic increase after World War II. The increasing trend continues to the present-day in most of the records, reflecting the continuous increase in anthropogenic Hg emissions from South Asia.

  11. A New Horizontal Gradient, Continuous Flow, Ice Thermal Diffusion Chamber and Detailed Observation of Condensation-Freezing and Deposition Nucleations.

    Science.gov (United States)

    1980-06-01

    active nuclei. 2.1.2 Expansion chambers Expansion chambers were originally used in nuclear physics to trace cosmic rays (Sears and Zemansky , 1962) and... Zemansky , 1962: University Physics, Addison- Wesley Publishing Co., Inc., Reading, Mass., p 909. Sinclair, D., and G. S. Hoopes, 1975: A continuous flow

  12. Comment on evidence for surface-initiated homogenous nucleation

    Directory of Open Access Journals (Sweden)

    J. E. Kay

    2003-01-01

    Full Text Available We investigate theoretical, laboratory, and atmospheric evidence for a recently proposed hypothesis: homogenous ice nucleation occurs at the surface, not in the volume, of supercooled water drops. Using existing thermodynamic arguments, laboratory experiments, and atmospheric data, we conclude that ice embryo formation at the surface cannot be confirmed or disregarded. Ice nucleation rates measured as a function of drop size in an air ambient could help distinguish between volume and surface nucleation rates.

  13. Formation of Jarosite in the Marwrth Vallis Region of Mars by Weathering Within Paleo-Ice Deposits

    Science.gov (United States)

    Michalski, J. R.; Niles, Paul B.

    2011-01-01

    Here we report new detections of jarosite in the Mawrth Vallis region of Mars. These newly recognized deposits expand the known occurrences of sulfates [1-2] in the region and further expand the already considerable geologic-mineralogic diversity of the Mawrth Vallis area [3-6]. The occurrence of sulfates such as jarosite in geologic contact with thick deposits of phyllosilicates in the Mawrth Vallis area is a relatively rare case on Mars where the enigmatic transition from an early phyllosilicateforming era to a younger sulfate-forming era [7] can be explored. We propose an ice-weathering model which can potentially explain the formation of jarosite-silicakaolinite within acidic ice deposits.

  14. Molecular Characterization of an Ice Nucleation Protein Variant (InaQ from Pseudomonas syringae and the Analysis of Its Transmembrane Transport Activity in Escherichia coli

    Directory of Open Access Journals (Sweden)

    Qianqian Li, Qi Yan, Jinsi Chen, Yan He, Jing Wang, Hongxing Zhang, Ziniu Yu, Lin Li

    2012-01-01

    Full Text Available The ice nucleation protein (INP of Pseudomonas syringae has gained scientific interest not only because of its pathogenicity of foliar necroses but also for its wide range of potential applications, such as in snow making, frozen food preparation, and surface-display system development. However, studies on the transport activity of INP remain lacking. In the present study, a newly identified INP-gene variant, inaQ, from a P. syringae MB03 strain was cloned. Its structural domains, signal sequences, and the hydrophilicity or hydrophobicity of each domain, were then characterized. The deduced amino acid sequence of InaQ shares similar protein domains with three P. syringae INPs, namely, InaK, InaZ, and InaV, which were identified as an N-terminal domain, a central repeating domain, and a C-terminal domain. The expression of the full-length InaQ and of various truncated variants was induced in Escherichia coli to analyze their transmembrane transport and surface-binding activities, while using the green fluorescence protein (GFP as the fusion partner. With two transmembrane segments and a weak secretion signal, the N-terminal domain (InaQ-N alone was found to be responsible for the transport process as well as for the binding to the outer membrane, whereas the C-terminal region was nonfunctional in protein transport. Increased membrane transport and surface-binding capacities were induced by a low isopropyl-β-D-thiogalactoside concentration (0.1 mmol/l but not by culture temperatures (15 ºC to 37 ºC. Furthermore, by constructing the GFP-fused proteins with a single InaQ-N, as well as two and three tandemly aligned InaQ-N molecules, the transport and membrane-binding activities of these proteins were compared using Western blot analysis, immmunofluorescence microscopy, and assays of the GFP specific fluorescence intensity of subcellular fractions and flow cytometry, which showed that the increase of InaQ-N repeats resulted in a coordinated

  15. Molecular characterization of an ice nucleation protein variant (inaQ) from Pseudomonas syringae and the analysis of its transmembrane transport activity in Escherichia coli.

    Science.gov (United States)

    Li, Qianqian; Yan, Qi; Chen, Jinsi; He, Yan; Wang, Jing; Zhang, Hongxing; Yu, Ziniu; Li, Lin

    2012-01-01

    The ice nucleation protein (INP) of Pseudomonas syringae has gained scientific interest not only because of its pathogenicity of foliar necroses but also for its wide range of potential applications, such as in snow making, frozen food preparation, and surface-display system development. However, studies on the transport activity of INP remain lacking. In the present study, a newly identified INP-gene variant, inaQ, from a P. syringae MB03 strain was cloned. Its structural domains, signal sequences, and the hydrophilicity or hydrophobicity of each domain, were then characterized. The deduced amino acid sequence of InaQ shares similar protein domains with three P. syringae INPs, namely, InaK, InaZ, and InaV, which were identified as an N-terminal domain, a central repeating domain, and a C-terminal domain. The expression of the full-length InaQ and of various truncated variants was induced in Escherichia coli to analyze their transmembrane transport and surface-binding activities, while using the green fluorescence protein (GFP) as the fusion partner. With two transmembrane segments and a weak secretion signal, the N-terminal domain (InaQ-N) alone was found to be responsible for the transport process as well as for the binding to the outer membrane, whereas the C-terminal region was nonfunctional in protein transport. Increased membrane transport and surface-binding capacities were induced by a low isopropyl-β-D-thiogalactoside concentration (0.1 mmol/l) but not by culture temperatures (15 ºC to 37 ºC). Furthermore, by constructing the GFP-fused proteins with a single InaQ-N, as well as two and three tandemly aligned InaQ-N molecules, the transport and membrane-binding activities of these proteins were compared using Western blot analysis, immmunofluorescence microscopy, and assays of the GFP specific fluorescence intensity of subcellular fractions and flow cytometry, which showed that the increase of InaQ-N repeats resulted in a coordinated increase of the

  16. Nucleation mechanism and microstructural assessment of SnO{sub 2} nanowires prepared by pulsed laser deposition

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Z.W. [Department of Physics and Materials Science, City University of Hong Kong, Tat Chee Avenue, Kowloon Tong, Hong Kong (China)]. E-mail: cnzwchen@yahoo.com.cn; Lai, J.K.L. [Department of Physics and Materials Science, City University of Hong Kong, Tat Chee Avenue, Kowloon Tong, Hong Kong (China); Shek, C.H. [Department of Physics and Materials Science, City University of Hong Kong, Tat Chee Avenue, Kowloon Tong, Hong Kong (China)

    2005-10-03

    Tin dioxide, SnO{sub 2}, nanowires have been successfully synthesized by a pulsed laser deposition process based on a sintered cassiterite SnO{sub 2} target, being deposited on Si (100) substrates at room temperature. Transmission electron microscopy shows that nanowires are structurally perfect and uniform, and diameters range from 10 nm to 30 nm, and lengths of several hundreds nanometers to a few micrometers. X-ray diffraction and energy dispersive X-ray spectroscopy analysis indicate that the nanowires have the same crystal structure and chemical composition found in the tetragonal rutile form of SnO{sub 2}. Selected area electron diffraction and high-resolution transmission electron microscopy reveal that the nanowires grow along the [110] growth direction. In addition to the fundamental Raman scattering peaks, the other two Raman scattering peaks are also observed. We discussed the possible reasons for the appearance of Raman scattering peaks at 518.7 and 701.8 cm{sup -1}. The growth process of the SnO{sub 2} nanowires is suggested to follow a vapor-solid mechanism.

  17. The Subsurface Ice Probe (SIPR): A Low-Power Thermal Probe for the Martian Polar Layered Deposits

    Science.gov (United States)

    Cardell, G.; Hecht, M. H.; Carsey, F. D.; Engelhardt, H.; Fisher, D.; Terrell, C.; Thompson, J.

    2004-01-01

    The distinctive layering visible in images from Mars Global Surveyor of the Martian polar caps, and particularly in the north polar cap, indicates that the stratigraphy of these polar layered deposits may hold a record of Martian climate history covering millions of years. On Earth, ice sheets are cored to retrieve a pristine record of the physical and chemical properties of the ice at depth, and then studied in exacting detail in the laboratory. On the Martian north polar cap, coring is probably not a practical method for implementation in an autonomous lander. As an alternative, thermal probes that drill by melting into the ice are feasible for autonomous operation, and are capable of reasonable approximations to the scientific investigations performed on terrestrial cores, while removing meltwater to the surface for analysis. The Subsurface Ice Probe (SIPR) is such a probe under development at JPL. To explore the dominant climate cycles, it is postulated that tens of meters of depth should be profiled, as this corresponds to the vertical separation of the major layers visible in the MOC images [1]. Optical and spectroscopic analysis of the layers, presumably demarcated by embedded dust and possibly by changes in the ice properties, would contribute to the construction of a chronology. Meltwater analysis may be used to determine the soluble chemistry of the embedded dust, and to monitor gradients of atmospheric gases, particularly hydrogen and oxygen, and isotopic variations that reflect atmospheric conditions at the time the layer was deposited. Thermal measurements can be used to determine the geothermal gradient and the bulk mechanical properties of the ice.

  18. Bacterial Ice Crystal Controlling Proteins

    Directory of Open Access Journals (Sweden)

    Janet S. H. Lorv

    2014-01-01

    Full Text Available 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.

  19. Changes in black carbon deposition to Antarctica from two high-resolution ice core records, 1850–2000 AD

    Directory of Open Access Journals (Sweden)

    M. M. Bisiaux

    2012-05-01

    Full Text Available Refractory black carbon aerosols (rBC emitted by biomass burning (fires and fossil fuel combustion, affect global climate and atmospheric chemistry. In the Southern Hemisphere (SH, rBC is transported in the atmosphere from low- and mid-latitudes to Antarctica and deposited to the polar ice sheet preserving a history of emissions and atmospheric transport. Here, we present two high-resolution Antarctic rBC ice core records drilled from the West Antarctic Ice Sheet divide and Law Dome on the periphery of the East Antarctic ice sheet. Separated by ~3500 km, the records span calendar years 1850–2001 and reflect the rBC distribution over the Indian and Pacific ocean sectors of the Southern Ocean. Concentrations of rBC in the ice cores displayed significant variability at annual to decadal time scales, notably in ENSO-QBO and AAO frequency bands. The delay observed between rBC and ENSO variability suggested that ENSO does not directly affect rBC transport, but rather continental hydrology, subsequent fire regimes, and aerosol emissions. From 1850 to 1950, the two ice core records were uncorrelated but were highly correlated from 1950 to 2002 (cross-correlation coefficient at annual resolution: r = 0.54, p < 0.01 due to a common decrease in rBC variability. The decrease in ice-core rBC from the 1950s to late 1980s displays similarities with inventories of SH rBC grass fires and biofuel emissions, which show reduced emission estimates over that period.

  20. Control of the nucleation and quality of graphene grown by low-pressure chemical vapor deposition with acetylene

    Energy Technology Data Exchange (ETDEWEB)

    Yang, Meng, E-mail: youmou@rift.mech.tohoku.ac.jp [Department of Nanomechanics, Graduate School of Engineering, Tohoku University, Sendai 980-8579 (Japan); Sasaki, Shinichirou [Department of Nanomechanics, Graduate School of Engineering, Tohoku University, Sendai 980-8579 (Japan); Suzuki, Ken; Miura, Hideo [Fracture and Reliability Research Institute, Tohoku University, Sendai 980-8579 (Japan)

    2016-03-15

    Graphical abstract: - Highlights: • For the first time, we succeeded in the LPCVD growth of monolayer graphene using acetylene as the precursor gas. • The growth rate is very high when acetylene is used as the source gas. Our process has exhibited the potential to shorten the growth time of CVD graphene. • We found that the domain size, defects density, layer number and the sheet resistance of graphene can be changed by changing the acetylene flow rates. • We found that it is also possible to form bilayer graphene using acetylene. However, further study are necessary to reduce the defects density. - Abstract: Although many studies have reported the chemical vapor deposition (CVD) growth of large-area monolayer graphene from methane, synthesis of graphene using acetylene as the source gas has not been fully explored. In this study, the low-pressure CVD (LPCVD) growth of graphene from acetylene was systematically investigated. We succeeded in regulating the domain size, defects density, layer number and the sheet resistance of graphene by changing the acetylene flow rates. Scanning electron microscopy and Raman spectroscopy were employed to confirm the layer number, uniformity and quality of the graphene films. It is found that a low flow rate of acetylene (0.28 sccm) is required to form high-quality monolayer graphene in our system. On the other hand, the high acetylene flow rate (7 sccm) will induce the growth of the bilayer graphene domains with high defects density. On the basis of selected area electron diffraction (SAED) pattern, the as-grown monolayer graphene domains were analyzed to be polycrystal. We also discussed the relation between the sheet resistacne and defects density in graphene. Our results provide great insights into the understanding of the CVD growth of monolayer and bilayer graphene from acetylene.

  1. 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....

  2. Characteristics of Dust Deposition at High Elevation Sites in Caucasus Over the Past 190 years Recorded in Ice Cores.

    Science.gov (United States)

    Kutuzov, Stanislav; Ginot, Patrick; Mikhaenko, Vladimir; Krupskaya, Victoria; Legrand, Michel; Preunkert, Suzanne; Polukhov, Alexey; Khairedinova, Alexandra

    2017-04-01

    The nature and extent of both radiative and geochemical impacts of mineral dust on snow pack and glaciers depend on physical and chemical properties of dust particles and its deposition rates. Ice cores can provide information about amount of dust particles in the atmosphere and its characteristic and also give insights on strengths of the dust sources and its changes in the past. A series of shallow ice cores have been obtained in Caucasus mountains, Russia in 2004 - 2015. A 182 meter ice core has been recovered at the Western Plateau of Mt. Elbrus (5115 m a.s.l.) in 2009. The ice cores have been dated using stable isotopes, NH4+ and succinic acid data with the seasonal resolution. Samples were analysed for chemistry, concentrations of dust and black carbon, and particle size distributions. Dust mineralogy was assessed by XRD. Individual dust particles were analysed using SEM. Dust particle number concentration was measured using the Markus Klotz GmbH (Abakus) implemented into the CFA system. Abakus data were calibrated with Coulter Counter multisizer 4. Back trajectory cluster analysis was used to assess main dust source areas. It was shown that Caucasus region experiencing influx of mineral dust from the Sahara and deserts of the Middle East. Mineralogy of dust particles of desert origin was significantly different from the local debris material and contained large proportion of calcite and clay minerals (kaolinite, illite, palygorskite) associated with material of desert origin. Annual dust flux in the Caucasus Mountains was estimated as 300 µg/cm2 a-1. Particle size distribution depends on individual characteristics of dust deposition event and also on the elevation of the drilling site. The contribution of desert dust deposition was estimated as 35-40 % of the total dust flux. Average annual Ca2+ concentration over the period from 1824 to 2013 was of 150 ppb while some of the strong dust deposition events led to the Ca2+ concentrations reaching 4400 ppb. An

  3. A nucleation and growth model of vertically-oriented carbon nanofibers or nanotubes by plasma-enhanced catalytic chemical vapor deposition.

    Science.gov (United States)

    Cojocaru, C S; Senger, A; Le Normand, F

    2006-05-01

    Carbon nanofibers are grown by direct current and hot filaments-activated catalytic chemical vapor deposition while varying the power of the hot filaments. Observations of these carbon nanofibers vertically oriented on a SiO2 (8 nm thick)/Si(100) substrate covered with Co nanoparticles (10-15 nm particle size) by Scanning Electron and Transmission Electron Microscopies show the presence of a graphitic "nest" either on the surface of the substrate or at the end of the specific nanofiber that does not encapsulate the catalytic particle. Strictly in our conditions, the activation by hot filaments is required to grow nanofibers with a C2H2 - H2 gas mixture, as large amounts of amorphous carbon cover the surface of the substrate without using hot filaments. From these observations as well as data of the literature, it is proposed that the nucleation of carbon nanofibers occurs through a complex process involving several steps: carbon concentration gradient starting from the catalytic carbon decomposition and diffusion from the surface of the catalytic nanoparticles exposed to the activated gas and promoted by energetic ionic species of the gas phase; subsequent graphitic condensation of a "nest" at the interface of the Co particle and substrate. The large concentration of highly reactive hydrogen radicals mainly provided by activation with hot filaments precludes further spreading out of this interfacial carbon nest over the entire surface of the substrate and thus selectively orientates the growth towards the condensation of graphene over facets that are perpendicular to the surface. Carbon nanofibers can then be grown within the well-known Vapor-Liquid-Solid process. Thus the effect of energetic ions and highly reactive neutrals like atomic hydrogen in the preferential etching of carbon on the edge of graphene shells and on the broadening of the carbon nanofiber is underlined.

  4. Active sites in heterogeneous ice nucleation—the example of K-rich feldspars

    Science.gov (United States)

    Kiselev, Alexei; Bachmann, Felix; Pedevilla, Philipp; Cox, Stephen J.; Michaelides, Angelos; Gerthsen, Dagmar; Leisner, Thomas

    2017-01-01

    Ice formation on aerosol particles is a process of crucial importance to Earth’s climate and the environmental sciences, but it is not understood at the molecular level. This is partly because the nature of active sites, local surface features where ice growth commences, is still unclear. Here we report direct electron-microscopic observations of deposition growth of aligned ice crystals on feldspar, an atmospherically important component of mineral dust. Our molecular-scale computer simulations indicate that this alignment arises from the preferential nucleation of prismatic crystal planes of ice on high-energy (100) surface planes of feldspar. The microscopic patches of (100) surface, exposed at surface defects such as steps, cracks, and cavities, are thought to be responsible for the high ice nucleation efficacy of potassium (K)-feldspar particles.

  5. Gullies and Lobate Deposits as Geomorphological Evidence for Impact-induced Transient Water Flow and Localized, Buried Ice-bearing Deposits on Vesta.

    Science.gov (United States)

    Scully, J. E. C.; Russell, C. T.; Yin, A.; Jaumann, R.; Carey, E. M.; McSween, H. Y., Jr.; Castillo, J. C.; Raymond, C. A.; Reddy, V.; Le Corre, L.

    2014-12-01

    Vesta, the second most massive asteroid, has long been perceived as anhydrous. However, recent studies suggesting the localized presence of hydrated minerals and past sub-surface water have challenged this perception (e.g. Sarafian et al., 2013; De Sanctis et al., 2012; Prettyman et al., 2012; McCord et al. 2012; Reddy et al. 2012; Treiman et al, 2004). Herein we show evidence that transient water flowed on the surface, in a debris-flow-like process, and left distinctive geomorphologic features. Based on analysis of ~20 m/ pixel images obtained by Dawn, we identify a class of locally occurring, interconnected and curvilinear systems of gullies in the walls of young (< 100s Ma) impact craters, ending in lobate deposits near the crater floors. As curvilinear systems only occur within impact craters, we propose that they formed by a particulate-dominated transient flow of water (≤ 26 minutes) that was released from buried ice-bearing deposits by impact-induced heating. Our interpretation is in accordance with the occurrence of pitted terrain on lobate deposits and crater floors. Pitted terrain is interpreted to result from the degassing of volatiles (Denevi et al., 2012). We also identify linear gully systems, which are morphologically distinct from the curvilinear systems, and are interpreted to form by dry flow of material. Craters containing curvilinear systems are clustered in two regions of Vesta's surface, whereas linear systems are evenly distributed. This indicates that the proposed buried ice-bearing deposits are likely localized in extent. Together with the newly expanded understanding of the distribution and behavior of water in the asteroid belt (e.g. Küppers et al., 2014; Hsieh & Jewitt, 2006), our results support the new paradigm that there is a continuum of small bodies in the solar system with many intermediate states of hydration. The varied hydrologic processes that occur within this new paradigm suggest the evolution of our solar system is more

  6. Historical and Future Black Carbon Deposition on the Three Ice Caps: Ice Core Measurements and Model Simulations from 1850 to 2100

    Science.gov (United States)

    Bauer, Susanne E.; Bausch, Alexandra; Nazarenko, Larissa; Tsigaridis, Kostas; Xu, Baiqing; Edwards. Ross; Bisiaux, Marion; McConnell, Joe

    2013-01-01

    Ice core measurements in conjunction with climate model simulations are of tremendous value when examining anthropogenic and natural aerosol loads and their role in past and future climates. Refractory black carbon (BC) records from the Arctic, the Antarctic, and the Himalayas are analyzed using three transient climate simulations performed with the Goddard Institute for Space Studies ModelE. Simulations differ in aerosol schemes (bulk aerosols vs. aerosol microphysics) and ocean couplings (fully coupled vs. prescribed ocean). Regional analyses for past (1850-2005) and future (2005-2100) carbonaceous aerosol simulations focus on the Antarctic, Greenland, and the Himalayas. Measurements from locations in the Antarctic show clean conditions with no detectable trend over the past 150 years. Historical atmospheric deposition of BC and sulfur in Greenland shows strong trends and is primarily influenced by emissions from early twentieth century agricultural and domestic practices. Models fail to reproduce observations of a sharp eightfold BC increase in Greenland at the beginning of the twentieth century that could be due to the only threefold increase in the North American emission inventory. BC deposition in Greenland is about 10 times greater than in Antarctica and 10 times less than in Tibet. The Himalayas show the most complicated transport patterns, due to the complex terrain and dynamical regimes of this region. Projections of future climate based on the four CMIP5 Representative Concentration Pathways indicate further dramatic advances of pollution to the Tibetan Plateau along with decreasing BC deposition fluxes in Greenland and the Antarctic.

  7. 超声场中声压与空化对冰晶分裂的影响%The Effect of Acoustic Pressure and Cavitation on the Secondary Nucleation of Ice

    Institute of Scientific and Technical Information of China (English)

    余德洋; 刘宝林; 王伯春

    2011-01-01

    In order to clarify the mechanism of secondary nucleation of iceinduced by ultrasound, experiments on ice crystals in degassed sucrose solutions and untreated solutions have been carried out using a novel ultrasonic cold stage device. For each experiment, the ultrasonic waves operated at a power output of 120W. The results show that the ice dendrite crystals growing in a sucrose solution can be broken up into smaller fragments when ultrasound was applied for 2 s, but the pre-existing ice dendrite crystals in a degassed sucrose solution are still unbroken when ultrasound was applied for 6 s. These findings confirm that cavitation induced by ultrasound is a major factor for the fragmentation of ice crystals.%为了探讨超声波强化冰晶二次成核的机理,利用自行研制的超声波冷却实验台,研究了超声波对未脱气蔗糖稀溶液和脱气蔗糖稀溶液中树枝状冰晶体的影响.实验结果表明:未脱气蔗糖稀溶液中的树枝状冰晶体受超声波辐射2s后已发生分裂,而脱气溶液中的树枝状冰晶体受功率相同的超声波辐射6s后却仍未分裂.说明超声场中冰晶发生分裂的主要原因是空化效应,而不是超声波在溶液中传播所引起的声压.

  8. SHARAD detection and characterization of subsurface water ice deposits in Utopia Planitia, Mars

    Science.gov (United States)

    Stuurman, C. M.; Osinski, G. R.; Holt, J. W.; Levy, J. S.; Brothers, T. C.; Kerrigan, M.; Campbell, B. A.

    2016-09-01

    Morphological analyses of Utopia Planitia, Mars, have led to the hypothesis that the region contains a substantial amount of near-surface ice. This paper tests this hypothesis using ground-penetrating radar techniques. We have identified an expansive radar reflective region spanning approximately 375,000 km2 in SHAllow RADar (SHARAD) data over western Utopia Planitia. The SHARAD reflective regions coincides with high densities of scalloped depressions and polygonal terrain. The reflectors are associated with layered mesas ˜80-170 m thick. We find a value of 2.8 ± 0.8 for the dielectric constant of the material overlying the reflectors. This work finds that the dielectric constant is consistent with a mixture of ice, air, and dust, containing a water ice volume up to 14,300 km3 in this unit.

  9. Application of an Online-Coupled Regional Climate Model, WRF-CAM5, over East Asia for Examination of Ice Nucleation Schemes: Part I. Comprehensive Model Evaluation and Trend Analysis for 2006 and 2011

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Ying; Zhang, Yang; Fan, Jiwen; Leung, Lai-Yung; Zhang, Qiang; He, Kebin

    2015-08-18

    Online-coupled climate and chemistry models are necessary to realistically represent the interactions between climate variables and chemical species and accurately simulate aerosol direct and indirect effects on cloud, precipitation, and radiation. In this Part I of a two-part paper, simulations from the Weather Research and Forecasting model coupled with the physics package of Community Atmosphere Model (WRF-CAM5) are conducted with the default heterogeneous ice nucleation parameterization over East Asia for two full years: 2006 and 2011. A comprehensive model evaluation is performed using satellite and surface observations. The model shows an overall acceptable performance for major meteorological variables at the surface and in the boundary layer, as well as column variables (e.g., precipitation, cloud fraction, precipitating water vapor, downward longwave and shortwave radiation). Moderate to large biases exist for cloud condensation nuclei over oceanic areas, cloud variables (e.g., cloud droplet number concentration, cloud liquid and ice water paths, cloud optical depth, longwave and shortwave cloud forcing). These biases indicate a need to improve the model treatments for cloud processes, especially cloud droplets and ice nucleation, as well as to reduce uncertainty in the satellite retrievals. The model simulates well the column abundances of chemical species except for column SO2 but relatively poor for surface concentrations of several species such as CO, NO2, SO2, PM2.5, and PM10. Several reasons could contribute to the underestimation of major chemical species in East Asia including underestimations of anthropogenic emissions and natural dust emissions, uncertainties in the spatial and vertical distributions of the anthropogenic emissions, as well as biases in meteorological, radiative, and cloud predictions. Despite moderate to large biases in the chemical predictions, the model performance is generally consistent with

  10. Application of an Online-Coupled Regional Climate Model, WRF-CAM5, over East Asia for Examination of Ice Nucleation Schemes: Part I. Comprehensive Model Evaluation and Trend Analysis for 2006 and 2011

    Directory of Open Access Journals (Sweden)

    Ying Chen

    2015-08-01

    Full Text Available Online-coupled climate and chemistry models are necessary to realistically represent the interactions between climate variables and chemical species and accurately simulate aerosol direct and indirect effects on cloud, precipitation, and radiation. In this Part I of a two-part paper, simulations from the Weather Research and Forecasting model coupled with the physics package of Community Atmosphere Model (WRF-CAM5 are conducted with the default heterogeneous ice nucleation parameterization over East Asia for two full years: 2006 and 2011. A comprehensive model evaluation is performed using satellite and surface observations. The model shows an overall acceptable performance for major meteorological variables at the surface and in the boundary layer, as well as column variables (e.g., precipitation, cloud fraction, precipitating water vapor, downward longwave and shortwave radiation. Moderate to large biases exist for cloud condensation nuclei over oceanic areas, cloud variables (e.g., cloud droplet number concentration, cloud liquid and ice water paths, cloud optical depth, longwave and shortwave cloud forcing. These biases indicate a need to improve the model treatments for cloud processes, especially cloud droplets and ice nucleation, as well as to reduce uncertainty in the satellite retrievals. The model simulates well the column abundances of chemical species except for column SO2 but relatively poor for surface concentrations of several species such as CO, NO2, SO2, PM2.5, and PM10. Several reasons could contribute to the underestimation of major chemical species in East Asia including underestimations of anthropogenic emissions and natural dust emissions, uncertainties in the spatial and vertical distributions of the anthropogenic emissions, as well as biases in meteorological, radiative, and cloud predictions. Despite moderate to large biases in the chemical predictions, the model performance is generally consistent with or even better

  11. Quantifying black carbon deposition over the Greenland ice sheet from forest fires in Canada

    Energy Technology Data Exchange (ETDEWEB)

    Thomas, J. L.; Polashenski, Christopher M.; Soja, Amber J.; Marelle, L.; Casey, Kimberly A.; Choi, Hyundeok; Raut, Jean-Christophe; Wiedinmyer, Christine; Emmons, L.; Fast, Jerome D.; Pelon, J.; Law, K. S.; Flanner, M. G.; Dibb, Jack E.

    2017-06-19

    We identify an important Black Carbon (BC) aerosol deposition event that was observed in snow stratigraphy and dated to between 27 July 2013 – 2 August 2013. This event comprises a significant portion (∼60%) of total deposition over a 10 month period (July 2013 – April 2014). Here we link this event to forest fires burning in Canada during summer 2013 using modeling and remote sensing tools. Aerosols were detected by both the CALIOP and MODIS instruments during transport between Canada and Greenland, confirming that this event involved emissions from forest fires in Canada. We use high-resolution regional chemical transport mod-eling (WRF-Chem) combined with high-resolution fire emissions (FINNv1.5) to study aerosol emissions, transport, and deposition during this event. The model accurately captures the timing of the BC deposition event and shows that the major contribution to deposition during this event is emissions originating from fires in Canada. However, the model under-predicts aerosol deposition compared to measurements at all sites by a factor of 2–100. Under-prediction of modeled BC deposition originates from uncertainties in fire emissions combined with uncertainties in aerosol scavenging by clouds. This study suggests that it is possible to describe the transport of an exceptional smoke event on regional and continental scales. Improvements in model descriptions of precipitation scavenging and emissions from wildfires are needed to correctly predict deposition, which is critical for determining the climate impacts of aerosols that originate from fires.

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

    Directory of Open Access Journals (Sweden)

    H. Wex

    2014-06-01

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

  13. Dislocation nucleation in heteroepitaxial semiconducting films

    Energy Technology Data Exchange (ETDEWEB)

    Pichaud, B.; Burle, N.; Texier, M.; Alfonso, C.; Gailhanou, M.; Thibault-Penisson, J. [IM2NP UMR6242 CNRS, Aix-Marseille University, Marseille (France); Fontaine, C. [LAAS CNRS, Toulouse (France); Vdovin, V.I. [Institute for Chemical Problems of Microelectronics, Moscow (Russian Federation)

    2009-08-15

    The nucleation of dislocation in semiconductors is still a matter of debate and especially in heteroepitaxial films. To understand this nucleation process the classical models of dislocation nucleation are presented and criticized. Two main points are then developed: emission of dislocations from surface steps and the role of point defects agglomeration on dislocation nucleation. Recent atomic simulation of half loops emission from surface steps and experimental evidences of anisotropic relaxation of GaInAs films deposited on vicinal (111)GaAs substrates strongly support surface steps as preferential sites for nucleation. In low temperature buffer layer structures (SiGe/Si) an original dislocation structure is observed which corresponds to the dislocation emission in different glide systems by a unique nucleation centre. (copyright 2009 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  14. 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

  15. Factors influencing ice formation and growth in simulations of a mixed-phase wave cloud

    Directory of Open Access Journals (Sweden)

    C. Dearden

    2012-10-01

    Full Text Available In this paper, numerical simulations of an orographically induced wave cloud sampled in-situ during the ICE-L (Ice in Clouds Experiment - Layer clouds field campaign are performed and compared directly against the available observations along various straight and level flight paths. The simulations are based on a detailed mixed-phase bin microphysics model embedded within a 1-D column framework with the latest parameterizations for heterogeneous ice nucleation and an adaptive treatment of ice crystal growth based on the evolution of crystal habit. The study focuses on the second of two clouds sampled on 16th November 2007, the in-situ data from which exhibits some interesting and more complex microphysics than other flights from the campaign. The model is used to demonstrate the importance of both heterogeneous and homogeneous nucleation in explaining the in-situ observations of ice crystal concentration and habit, and how the ability to isolate the influence of both nucleation mechanisms helps when quantifying active IN concentrations. The aspect ratio and density of the simulated ice crystals is shown to evolve in a manner consistent with the in-situ observations along the flight track, particularly during the transition from the mixed-phase region of the cloud to the ice tail dominated by homogeneous nucleation. Some additional model runs are also performed to explore how changes in IN concentration and the value of the deposition coefficient for ice affect the competition between heterogeneous and homogeneous ice formation in the wave cloud, where the Factorial Method is used to isolate and quantify the effect of such non-linear interactions. The findings from this analysis show that the effect on homogeneous freezing rates is small, suggesting that any competition between the microphysical variables is largely overshadowed by the strong dynamical forcing of the cloud in the early stages of ice formation.

  16. Modeling and Thermal Performance Evaluation of Porous Curd Layers in Sub-Cooled Boiling Region of PWRs and Effects of Sub-Cooled Nucleate Boiling on Anomalous Porous Crud Deposition on Fuel Pin Surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Barclay Jones

    2005-06-27

    A significant number of current PWRs around the world are experiencing anomalous crud deposition in the sub-cooled region of the core, resulting in an axial power shift or Axial Offset Anomaly (AOA), a condition that continues to elude prediction of occurrence and thermal/neutronic performance. This creates an operational difficulty of not being able to accurately determine power safety margin. In some cases this condition has required power ''down rating'' by as much as thirty percent and the concomitant considerable loss of revenue for the utility. This study examines two aspects of the issue: thermal performance of crud layer and effect of sub-cooled nucleate boiling on the solute concentration and its influence on initiation of crud deposition/formation on fuel pin surface.

  17. An ice-contact rhythmite (turbidite) succession deposited during the November 1996 catastrophic outburst flood (jökulhlaup), Skeiðarárjökull, Iceland

    Science.gov (United States)

    Russell, Andrew J.; Knudsen, Óskar

    1999-08-01

    This paper presents new evidence of coarse-grained deposition from a turbulent suspension within a low-energy `slack-water' location during a recent well-documented, volcanically related, high-magnitude glacier outburst flood or jökulhlaup, Skeiðarárjökull, Iceland. This study uses established spatial and temporal constraints on processes observed during the November 1996 jökulhlaup to interpret resultant flood sediments. Coarse-grained sediments were deposited within flood slack-water conditions from suspension load by repeated turbulent flow pulses with durations of seconds-minutes. Depositional processes are thought to be analogous to turbidity currents. A minimum thickness of 15 m of rhythmites record suspended sediment dynamics at a conduit mouth during the late rising and early falling stages of the jökulhlaup. The morphology and sedimentology of deposits in a large ice-walled chamber are consistent with previous models proposed for bar deposition during cataclysmic floods. Flood flows within subglacial conduits and ice-walled open channels were sufficiently powerful to carry material up to boulder size in suspension. Macro-turbulent flows carried huge quantities of suspended sediment to high levels within the main outlet channel. High-frequency, short-duration flow pulses entering a complex ice-walled channel geometry generated highly unsteady and non-uniform flows capable of both erosional and depositional work. This study lends support to the deposition of multiple rhythmites per flood under main flow slack-water conditions. Identification of high-magnitude jökulhlaups in the ice-marginal sedimentary record will depend on the identification and correct interpretation of feeder channel and slack-water turbidite sediments. The results described here may also have application to rhythmic deposits formed by large turbulent flows in other environmental settings.

  18. Dynamics of homogeneous nucleation

    DEFF Research Database (Denmark)

    Toxværd, Søren

    2015-01-01

    The classical nucleation theory for homogeneous nucleation is formulated as a theory for a density fluctuation in a supersaturated gas at a given temperature. But molecular dynamics simulations reveal that it is small cold clusters which initiates the nucleation. The temperature in the nucleating...

  19. Laser-induced ion emission during polymer deposition from a flash-frozen water ice matrix

    DEFF Research Database (Denmark)

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

    2004-01-01

    Flash-frozen water solutions of 1% weight PEG (polyethylene glycol) at -50 degreesC were used as targets at a laser wavelength of 355 nm for polymer deposition with Matrix-Assisted Pulsed Laser Evaporation (MAPLE). For medium laser fluences the transfer of PEG material to the substrate was accomp......Flash-frozen water solutions of 1% weight PEG (polyethylene glycol) at -50 degreesC were used as targets at a laser wavelength of 355 nm for polymer deposition with Matrix-Assisted Pulsed Laser Evaporation (MAPLE). For medium laser fluences the transfer of PEG material to the substrate...... Elsevier B.V. All rights reserved....

  20. Characterisation of three regimes of collapsing Arctic ice complex deposits on the SE Laptev Sea coast using biomarkers and dual carbon isotopes

    NARCIS (Netherlands)

    Sanchez-Garcia, Laura; Vonk, Jorien; Charkin, Alexander; Kosmach, Denis; Dudarev, Oleg; Semiletov, Igor; Gustafsson, Örjan

    2014-01-01

    Arctic amplification of climate warming is intensifying the thaw and coastal erosion of the widespread and carbon-rich Siberian Ice Complex Deposits (ICD). Despite the potential for altering long-term carbon dynamics in the Arctic, the susceptibility of organic carbon (OC) to degradation as the ICD

  1. Emerging investigator series: a 14-year depositional ice record of perfluoroalkyl substances in the High Arctic.

    Science.gov (United States)

    MacInnis, John J; French, Katherine; Muir, Derek C G; Spencer, Christine; Criscitiello, Alison; De Silva, Amila O; Young, Cora J

    2017-01-25

    To improve understanding of long-range transport of perfluoroalkyl substances to the High Arctic, samples were collected from a snow pit on the Devon Ice Cap in spring 2008. Snow was analyzed for perfluoroalkyl acids (PFAAs), including perfluoroalkyl carboxylic acids (PFCAs) and perfluoroalkyl sulfonic acids (PFSAs), as well as perfluorooctane sulfonamide (FOSA). PFAAs were detected in all samples dated from 1993 to 2007. PFAA fluxes ranged from <1 to hundreds of ng per m(2) per year. Flux ratios of even-odd PFCA homologues were mostly between 0.5 and 2, corresponding to molar ratios expected from atmospheric oxidation of fluorotelomer compounds. Concentrations of perfluorobutanoic acid (PFBA) were much higher than other PFCAs, suggesting PFBA loading on the Devon Ice Cap is influenced by additional sources, such as the oxidation of heat transfer fluids. All PFCA fluxes increased with time, while PFSA fluxes generally decreased with time. No correlations were observed between PFAAs and the marine aerosol tracer, sodium. Perfluoro-4-ethylcyclohexanesulfonate (PFECHS) was detected for the first time in an atmospherically - derived sample, and its presence may be attributed to aircraft hydraulic system leakage. Observations of PFAAs from these samples provide further evidence that atmospheric oxidation of volatile precursors is an important source of PFAAs to the Arctic environment.

  2. Current use and legacy pesticide deposition to ice caps on Svalbard, Norway

    NARCIS (Netherlands)

    Ruggirello, Rachel M.; Hermanson, Mark H.; Isaksson, Elisabeth; Teixeira, Camilla; Forsstrom, Sanja; Muir, Derek C. G.; Pohjola, Veijo; van de Wal, Roderik; Meijer, Harro A. J.

    2010-01-01

    Transport and deposition of current use (CUP) and legacy pesticides (LP) and residual products to the Arctic have been documented in abiotic matrices. These observations show that some "low-persistence" pesticides with high OH center dot reaction rates are stable enough to accumulate in a polar envi

  3. Current use and legacy pesticide deposition to ice caps on Svalbard, Norway

    NARCIS (Netherlands)

    Ruggirello, R. M.; Hermanson, M.H.; Isaksson, E.; Teixeira, C.; Forsström, S.; Muir, D.C.G.; Pohjola, V.; van de Wal, R.S.W.; Meijer, H.A.J.

    2010-01-01

    Transport and deposition of current use (CUP) and legacy pesticides (LP) and residual products to the Arctic have been documented in abiotic matrices. These observations show that some “low-persistence” pesticides with high OH· reaction rates are stable enough to accumulate in a polar environment. I

  4. Deposition history of brominated flame retardant compounds in an ice core from Holtedahlfonna, Svalbard, Norway

    NARCIS (Netherlands)

    Hermanson, M.H.; Isaksson, E.; Forsström, S.; Teixeira, C.; Muir, D.C.G.; Pohjola, V.A.; van de Wal, R.S.W.

    2010-01-01

    Brominated flame retardants (BFRs) have been found in Arctic wildlife, lake sediment, and air. To identify the atmospheric BFR deposition history on Svalbard, Norway, we analyzed 19 BFRs, including hexabromocyclododecane (HBCD), 1,2-bis(2,4,6-tribromophenoxy)ethane (BTBPE), decabromodiphenyl ethane

  5. An Overview of the Studies on Black Carbon and Mineral Dust Deposition in Snow and Ice Cores in East Asia

    Institute of Scientific and Technical Information of China (English)

    WANG Xin; XU Baiqing; MING Jing

    2014-01-01

    Black carbon (BC) is the most eff ective insoluble light-absorbing particulate (ILAP), which can strongly absorb solar radiation at visible wavelengths. Once BC is deposited in snow via dry or wet process, even a small amount of BC could signifi cantly decrease snow albedo, enhance absorption of solar radiation, accelerate snow melting, and cause climate feedback. BC is considered the second most important component next to CO2 in terms of global warming. Similarly, mineral dust (MD) is another type of ILAP. So far, little attention has been paid to quantitative measurements of BC and MD deposition on snow surface in the midlatitudes of East Asia, especially over northern China. In this paper, we focus on reviewing several experiments performed for collecting and measuring scavenging BC and MD in the high Asian glaciers over the mountain range (such as the Himalayas) and in seasonal snow over northern China. Results from the surveyed literature indicate that the absorption of ILAP in seasonal snow is dominated by MD in the Qilian Mountains and by local soil dust in the Inner Mongolian region close to dust sources. The detection of BC in snow and ice cores using modern techniques has a large bias and uncertainty when the snow sample is mixed with MD. Evidence also indicates that the reduction of snow albedo by BC and MD perturbations can signifi cantly increase the net surface solar radiation, cause surface air temperature to rise, reduce snow accumulation, and accelerate snow melting.

  6. Influence of Aerosol Chemical Composition on Heterogeneous Ice Formation under Mid-Upper Troposphere Conditions

    Science.gov (United States)

    Kanji, Z. A.; Niemand, M.; Saathoff, H.; Möhler, O.; Chou, C.; Abbatt, J.; Stetzer, O.

    2011-12-01

    Aerosols are involved in cooling/warming the atmosphere directly via interaction with incoming solar radiation (aerosol direct effect), or via their ability to act as cloud condensation or ice nuclei (IN) and thus play a role in cloud formation (indirect effect). In particular, the physical properties of aerosols such as size and solubility and chemical composition can influence their behavior and fate in the atmosphere. Ice nucleation taking place via IN is termed as heterogeneous ice nucleation and can take place with via deposition (ice forming on IN directly from the vapor phase), condensation/immersion (freezing via formation of the liquid phase on IN) or condensation (IN colliding with supercooled liquid drops). This presentation shows how the chemical composition and surface area of various tropospherically relevant aerosols influence conditions of temperature (T) and relative humidity (RH) required for heterogeneous ice formation conditions in the mid-upper troposphere regime (253 - 220K)? Motivation for this comes first from, the importance of being able to predict ice formation accurately so as to understand the hydrological cycle since the ice is the primary initiator of precipitation forming clouds. Second, the tropospheric budget of water vapour, an especially active greenhouse gas is strongly influenced by ice nucleation and growth. Third, ice surfaces in the atmosphere act as heterogeneous surfaces for chemical reactions of trace gases (e.g., SO2, O3, NOx and therefore being able to accurately estimate ice formation rates and quantify ice surface concentrations will allow a more accurate calculation of trace gas budgets in the troposphere. Ice nucleation measurements were conducted using a self-developed continuous flow diffusion chamber and static chamber. A number of tropospherically relevant particulates with naturally-varying and laboratory-modified surface chemistry/structure were investigated for their ice formation efficiency based on highest

  7. Natural and anthropogenic variations in atmospheric mercury deposition during the Holocene near Quelccaya Ice Cap, Peru

    Science.gov (United States)

    Beal, Samuel A.; Kelly, Meredith A.; Stroup, Justin S.; Jackson, Brian P.; Lowell, Thomas V.; Tapia, Pedro M.

    2014-04-01

    Mercury (Hg) is a toxic metal that is transported globally through the atmosphere. Emissions of Hg from mineral reservoirs and recycling between soil/biomass, oceans, and the atmosphere are fundamental to the global Hg cycle, yet past emissions from anthropogenic and natural sources are not fully constrained. We use a sediment core from Yanacocha, a headwater lake in southeastern Peru, to study the anthropogenic and natural controls on atmospheric Hg deposition during the Holocene. From 12.3 to 3.5 ka, Hg fluxes in the record are relatively constant (mean ± 1σ: 1.4 ± 0.6 µg m-2 a-1). Past Hg deposition does not correlate with changes in regional temperature and precipitation or with most large volcanic events that occurred regionally (~300-400 km from Yanacocha) and globally. In 1450 B.C. (3.4 ka), Hg fluxes abruptly increased and reached the Holocene-maximum flux (6.7 µg m-2 a-1) in 1200 B.C., concurrent with a ~100 year peak in Fe and chalcophile metals (As, Ag, Tl) and the presence of framboidal pyrite. Continuously elevated Hg fluxes from 1200 to 500 B.C. suggest a protracted mining-dust source near Yanacocha that is identical in timing to documented pre-Incan cinnabar mining in central Peru. During Incan and Colonial time (A.D. 1450-1650), Hg deposition remains elevated relative to background levels but lower relative to other Hg records from sediment cores in central Peru, indicating a limited spatial extent of preindustrial Hg emissions. Hg fluxes from A.D. 1980 to 2011 (4.0 ± 1.0 µg m-2 a-1) are 3.0 ± 1.5 times greater than preanthropogenic fluxes.

  8. Comparison of areas in shadow from imaging and altimetry in the north polar region of Mercury and implications for polar ice deposits

    Science.gov (United States)

    Deutsch, Ariel N.; Chabot, Nancy L.; Mazarico, Erwan; Ernst, Carolyn M.; Head, James W.; Neumann, Gregory A.; Solomon, Sean C.

    2016-12-01

    Earth-based radar observations and results from the MESSENGER mission have provided strong evidence that permanently shadowed regions near Mercury's poles host deposits of water ice. MESSENGER's complete orbital image and topographic datasets enable Mercury's surface to be observed and modeled under an extensive range of illumination conditions. The shadowed regions of Mercury's north polar region from 65°N to 90°N were mapped by analyzing Mercury Dual Imaging System (MDIS) images and by modeling illumination with Mercury Laser Altimeter (MLA) topographic data. The two independent methods produced strong agreement in identifying shadowed areas. All large radar-bright deposits, those hosted within impact craters ≥6 km in diameter, collocate with regions of shadow identified by both methods. However, only ∼46% of the persistently shadowed areas determined from images and ∼43% of the permanently shadowed areas derived from altimetry host radar-bright materials. Some sizable regions of shadow that do not host radar-bright deposits experience thermal conditions similar to those that do. The shadowed craters that lack radar-bright materials show a relation with longitude that is not related to the thermal environment, suggesting that the Earth-based radar observations of these locations may have been limited by viewing geometry, but it is also possible that water ice in these locations is insulated by anomalously thick lag deposits or that these shadowed regions do not host water ice.

  9. A semianalytical algorithm for quantitatively estimating sediment and atmospheric deposition flux from MODIS-derived sea ice albedo in the Bohai Sea, China

    Science.gov (United States)

    Xu, Zhantang; Hu, Shuibo; Wang, Guifen; Zhao, Jun; Yang, Yuezhong; Cao, Wenxi; Lu, Peng

    2016-05-01

    Quantitative estimates of particulate matter [PM) concentration in sea ice using remote sensing data is helpful for studies of sediment transport and atmospheric dust deposition flux. In this study, the difference between the measured dirty and estimated clean albedo of sea ice was calculated and a relationship between the albedo difference and PM concentration was found using field and laboratory measurements. A semianalytical algorithm for estimating PM concentration in sea ice was established. The algorithm was then applied to MODIS data over the Bohai Sea, China. Comparisons between MODIS derived and in situ measured PM concentration showed good agreement, with a mean absolute percentage difference of 31.2%. From 2005 to 2010, the MODIS-derived annual average PM concentration was approximately 0.025 g/L at the beginning of January. After a month of atmospheric dust deposition, it increased to 0.038 g/L. Atmospheric dust deposition flux was estimated to be 2.50 t/km2/month, similar to 2.20 t/km2/month reported in a previous study. The result was compared with on-site measurements at a nearby ground station. The ground station was close to industrial and residential areas, where larger dust depositions occurred than in the sea, but although there were discrepancies between the absolute magnitudes of the two data sets, they demonstrated similar trends.

  10. Atmospheric chemistry of mercury in Antarctica and the role of cryptogams to assess deposition patterns in coastal ice-free areas.

    Science.gov (United States)

    Bargagli, R

    2016-11-01

    Mercury in the Antarctic troposphere has a distinct chemistry and challenging long-term measurements are needed for a better understanding of the atmospheric Hg reactions with oxidants and the exchanges of the various mercury forms among air-snow-sea and biota. Antarctic mosses and lichens are reliable biomonitors of airborne metals and in short time they can give useful information about Hg deposition patterns. Data summarized in this review show that although atmospheric Hg concentrations in the Southern Hemisphere are lower than those in the Northern Hemisphere, Antarctic cryptogams accumulate Hg at levels in the same range or higher than those observed for related cryptogam species in the Arctic, suggesting an enhanced deposition of bioavailable Hg in Antarctic coastal ice-free areas. In agreement with the newest findings in the literature, the Hg bioaccumulation in mosses and lichens from a nunatak particularly exposed to strong katabatic winds can be taken as evidence for a Hg contribution to coastal ecosystems by air masses from the Antarctic plateau. Human activities on the continent are mostly concentrated in coastal ice-free areas, and the deposition in these areas of Hg from the marine environment, the plateau and anthropogenic sources raises concern. The use of Antarctic cryptogams as biomonitors will be very useful to map Hg deposition patterns in costal ice-free areas and will contribute to a better understanding of Hg cycling in Antarctica and its environmental fate in terrestrial ecosystems.

  11. Ice Formation on Kaolinite: Insights from Molecular Dynamics Simulations

    CERN Document Server

    Sosso, Gabriele C; Zen, Andrea; Pedevilla, Philipp; Michaelides, Angelos

    2016-01-01

    The formation of ice affects many aspects of our everyday life as well as technologies such as cryotherapy and cryopreservation. Foreign substances almost always aid water freezing through heterogeneous ice nucleation, but the molecular details of this process remain largely unknown. In fact, insight into the microscopic mechanism of ice formation on different substrates is difficult to obtain even via state-of-the-art experimental techniques. At the same time, atomistic simulations of heterogeneous ice nucleation frequently face extraordinary challenges due to the complexity of the water-substrate interaction and the long timescales that characterize nucleation events. Here, we have investigated several aspects of molecular dynamics simulations of heterogeneous ice nucleation considering as a prototypical ice nucleating material the clay mineral kaolinite, which is of relevance in atmospheric science. We show via seeded molecular dynamics simulations that ice nucleation on the hydroxylated (001) face of kaol...

  12. CO2 ice structure and density under Martian atmospheric conditions

    Science.gov (United States)

    Mangan, T. P.; Salzmann, C. G.; Plane, J. M. C.; Murray, B. J.

    2017-09-01

    Clouds composed of CO2 ice form throughout the Martian atmosphere. In the mesosphere, CO2 ice clouds are thought to form via heterogeneous ice nucleation on nanoparticles of meteoric origin at temperatures often below 100 K. Lower altitude CO2 ice clouds in the wintertime polar regions form up to around 145 K and lead to the build-up of the polar ice caps. However, the crystal structure and related fundamental properties of CO2 ice under Martian conditions are poorly characterised. Here we present X-ray diffraction (XRD) measurements of CO2 ice, grown via deposition from the vapour phase under temperature and pressure conditions analogous to the Martian mesosphere. A crystalline cubic structure was determined, consistent with the low-pressure polymorph (CO2-I, space group Pa-3 (No. 205)). CO2 deposited at temperatures of 80-130 K and pressures of 0.01-1 mbar was consistent with dry ice and previous literature measurements, thus removing the possibility of a more complicated phase diagram for CO2 in this region. At 80 K, a lattice parameter of 5.578 ± 0.002 Å, cell volume of 173.554 ± 0.19 Å3 and density of 1.684 ± 0.002 g cm-3 was determined. Using these measurements, we determined the thermal expansion of CO2 across 80-130 K that allowed for a fit of CO2 ice density measurements across a larger temperature range (80-195 K) when combined with literature data (CO2 density = 1.72391 - 2.53 × 10-4T - 2.87 × 10-6 T2). Temperature-dependent CO2 density values are used to estimate sedimentation velocities and heterogeneous ice nucleation rates, showing an increase in nucleation rate of up to a factor of 1000 when compared to commonly used literature values. This temperature-dependent equation of state is therefore suggested for use in future studies of Martian mesospheric CO2 clouds. Finally, we discuss the possible shapes of crystals of CO2 ice in the Martian atmosphere and show that a range of shapes including cubes and octahedra as well as a combination of the

  13. Ice cores from Arctic sub-polar glaciers : Chronology and post-depositional processes deduced from radioactivity measurements

    NARCIS (Netherlands)

    Pinglot, J.F.; Vaikmae, R.A.; Kamiyama, K.; Igarashi, M.; Fritsche, D.; Wilhalms, F.; Koerner, R.; Henderson, L.; Isaksson, E.; Winther, J.G.; van de Wal, R.S.W.; Fournier, M; Bouisset, P.; Meijer, H.A.J.

    2003-01-01

    The response of Arctic ice masses to climate change is studied using ice cores containing information on past climatic and environmental features. Interpretation of this information requires accurate chronological data. Absolute dating of ice cores from sub-polar Arctic glaciers is possible using

  14. Ice cores from Arctic sub-polar glaciers : Chronology and post-depositional processes deduced from radioactivity measurements

    NARCIS (Netherlands)

    Pinglot, J.F.; Vaikmae, R.A.; Kamiyama, K.; Igarashi, M.; Fritsche, D.; Wilhalms, F.; Koerner, R.; Henderson, L.; Isaksson, E.; Winther, J.G.; van de Wal, R.S.W.; Fournier, M; Bouisset, P.; Meijer, H.A.J.

    2003-01-01

    The response of Arctic ice masses to climate change is studied using ice cores containing information on past climatic and environmental features. Interpretation of this information requires accurate chronological data. Absolute dating of ice cores from sub-polar Arctic glaciers is possible using we

  15. Ice cores from Arctic sub-polar glaciers : Chronology and post-depositional processes deduced from radioactivity measurements

    NARCIS (Netherlands)

    Pinglot, J.F.; Vaikmae, R.A.; Kamiyama, K.; Igarashi, M.; Fritsche, D.; Wilhalms, F.; Koerner, R.; Henderson, L.; Isaksson, E.; Winther, J.G.; van de Wal, R.S.W.; Fournier, M; Bouisset, P.; Meijer, H.A.J.

    2003-01-01

    The response of Arctic ice masses to climate change is studied using ice cores containing information on past climatic and environmental features. Interpretation of this information requires accurate chronological data. Absolute dating of ice cores from sub-polar Arctic glaciers is possible using we

  16. Seismic architecture and sedimentology of a major grounding zone system deposited by the Bjørnøyrenna Ice Stream during Late Weichselian deglaciation

    Science.gov (United States)

    Rüther, Denise Christina; Mattingsdal, Rune; Andreassen, Karin; Forwick, Matthias; Husum, Katrine

    2011-09-01

    A 280 km wide sediment wedge in outer Bjørnøyrenna (Bear Island Trough), south-western Barents Sea, has been investigated using 2D and 3D seismic data, sediment gravity cores, as well as regional swath and large scale bathymetry data. The bathymetry data indicate a division into an up to 35 m high frontal wedge with large depressions, and an upstream part characterized by mega scale glacial lineations (MSGL). From seismic sections increasing erosion is demonstrated for the upstream part, coinciding with the location of MSGL. Whether the latter are depositional features postdating an extensive erosional event or formed by erosion remains inconclusive. Based on the distinct morphology and internal structures, we infer that the system was deposited during a rapid readvance whereby the ice front pushed and bulldozed predominantly soft, diluted proglacial sediments. Analyses in the eastern part of the sediment system reveal the existence of imbricated thrust sheets in the frontal part of the wedge. This is suggested to imply upstream erosion of sedimentary rock and incorporation of thrusted blocks into the moraine, forming a composite ridge locally. We argue that observed large scale depressions are dead-ice features in the marine environment. It is envisioned that intense englacial thrusting may have developed into a decollement as the cold glacier snout got overrun by ice masses from the interior, thereby enabling the inclusion of slabs of ice in the push moraine mass. Radiocarbon dates indicate that the sediment wedge was deposited around 17,090 cal yrs BP (14,530 14C yrs BP) and that the ice front probably remained stable until 16,580 cal yrs BP (13,835 14C yrs BP).

  17. Multidisciplinary study of sediments deposited in the Ross Sea (Antarctica) during the last 50 ka: information on changes of ice extent during the glacial-interglacial transition

    Science.gov (United States)

    Del Carlo, Paola; Baneschi, Ilaria; Bertagnini, Antonella; Boschi, Chiara; Cascella, Antonio; Colizza, Ester; Di Roberto, Alessio; Di Vincenzo, Gianfranco; Finocchiaro, Furio; Landi, Patrizia; Lirer, Fabrizio; Pompilio, Massimo; Sagnotti, Leonardo; Sangiorgi, Francesca; Sprovieri, Mario; Wrinkler, Aldo

    2013-04-01

    In the Ross Sea (Antarctica), sedimentation is controlled by the dynamics of the ice shelves, fluctuations of the ice sheets extensions (Eastern and Western) and volcanic activity from several volcanic complex of the Victoria Land. Marine sediments consisting of alternated glacigenic, biogenic and volcanic deposits can be interpreted in terms of changes in paleoclimate and paleoenvironment conditions. In this project we present a multidisciplinary study (comprising tephrostratigraphy, petrology, paleomagnetism, rock magnetism, TIC/TOC geochemistry, Ar/Ar dating, palinology and integrated biostratigraphy of forams and calcareous nannoplankton) of the sediments recovered in selected cores from Ross Sea during 1999 and 2000 cruises and stored in the Italian archive at Museo Nazionale dell'Antartide (Trieste). Results provide new data on local and/or global changes of paleoclimate and paleoenvironmental conditions over the past 50 Ka. Furthermore, the study of the recovered volcanic deposits adds new information about the poorly known, recent volcanic activity in the Victoria Land area.

  18. Results from the University of Toronto continuous flow diffusion chamber at ICIS 2007: instrument intercomparison and ice onsets for different aerosol types

    Directory of Open Access Journals (Sweden)

    Z. A. Kanji

    2011-01-01

    Full Text Available The University of Toronto continuous flow diffusion chamber (UT-CFDC was used to study heterogeneous ice nucleation at the International Workshop on Comparing Ice Nucleation Measuring Systems (ICIS 2007 which also represented the 4-th ice nucleation workshop, on 14–28 September 2007. One goal of the workshop was to inter-compare different ice nucleation measurement techniques using the same aerosol sample source and preparation method. The aerosol samples included four types of desert mineral dust, graphite soot particles, and live and dead bacterial cells (Snomax®. This paper focuses on the UT-CFDC results, with a comparison to techniques of established heritage including the Colorado State CFDC and the AIDA expansion chamber. Good agreement was found between the different instruments with a few specific differences, especially at low temperatures, perhaps due to the variation in how onset of ice formation is defined between the instruments and the different inherent residence times. It was found that when efficiency of ice formation is based on the lowest onset relative humidity, Snomax® particles were most efficient followed by the desert dusts and then soot. For all aerosols, deposition mode freezing was only observed for T<45 K except for the dead bacteria where freezing occurred below water saturation as warm as 263 K.

  19. Results from the University of Toronto continuous flow diffusion chamber at ICIS 2007: instrument intercomparison and ice onsets for different aerosol types

    Science.gov (United States)

    Kanji, Z. A.; Demott, P. J.; Möhler, O.; Abbatt, J. P. D.

    2011-01-01

    The University of Toronto continuous flow diffusion chamber (UT-CFDC) was used to study heterogeneous ice nucleation at the International Workshop on Comparing Ice Nucleation Measuring Systems (ICIS 2007) which also represented the 4-th ice nucleation workshop, on 14-28 September 2007. One goal of the workshop was to inter-compare different ice nucleation measurement techniques using the same aerosol sample source and preparation method. The aerosol samples included four types of desert mineral dust, graphite soot particles, and live and dead bacterial cells (Snomax®). This paper focuses on the UT-CFDC results, with a comparison to techniques of established heritage including the Colorado State CFDC and the AIDA expansion chamber. Good agreement was found between the different instruments with a few specific differences, especially at low temperatures, perhaps due to the variation in how onset of ice formation is defined between the instruments and the different inherent residence times. It was found that when efficiency of ice formation is based on the lowest onset relative humidity, Snomax® particles were most efficient followed by the desert dusts and then soot. For all aerosols, deposition mode freezing was only observed for T<45 K except for the dead bacteria where freezing occurred below water saturation as warm as 263 K.

  20. 150 kyr History of Arctic Black Carbon Deposition Recorded by Paired Ice Core and Sediment Core Records from Lake El'gygytgyn and NEEM

    Science.gov (United States)

    Chellman, N.; McConnell, J. R.; Heyvaert, A.; Brigham-Grette, J.; Melles, M.; Wennrich, V.; Svensson, A.

    2016-12-01

    Black carbon (BC) is a proxy for biomass burning and industrial combustion that has recently been recognized to have a major forcing on Earth's climate. The radiative effect of BC is most pronounced when BC is deposited onto highly reflective surfaces such as ice and snow and is estimated to have the third largest climate forcing after carbon dioxide and methane. Thus, quantifying BC in the climate system is crucial for modeling and understanding Earth's fire history and radiative budget. Here we present two long-term records of Northern Hemisphere BC deposition extending back 150 kyr. The first record, from the NEEM ice core, shows that BC deposition in Greenland is related to Northern Hemisphere climate and temperature proxies. The second record was obtained from a sediment core from Lake El'gygytgyn using a new method for BC measurements in lake sediments. The link between BC, insolation, and other climate proxies at these distant sites suggests a direct link between fire and climate that has been recorded in two distinct depositional environments. These two records capture both the local and regional BC signals that reflect fire emissions from different source regions and provide insight as to how climate affects BC deposition and, in turn, fire regime.

  1. Detailed cloud resolving model simulations of the impacts of Saharan air layer dust on tropical deep convection – Part 1: Dust acts as ice nuclei

    Directory of Open Access Journals (Sweden)

    W. Gong

    2010-05-01

    Full Text Available Observational studies suggest that the Saharan Air Layer (SAL, an elevated layer (850–500 hPa of Saharan air and mineral dust, has strong impacts on the microphysical as well as dynamical properties of tropical deep convective cloud systems along its track. In this case study, numerical simulations using a two-dimensional Detailed Cloud Resolving Model (DCRM were carried out to investigate the dust-cloud interactions in the tropical deep convection, focusing on the dust role as Ice Nuclei (IN.

    The simulations showed that mineral dust considerably enhanced heterogeneous nucleation and freezing at temperatures warmer than −40 °C, resulting in more ice hydrometeors number concentration and reduced precipitating size of ice particles. Because of the lower in the saturation over ice as well as more droplet freezing, total latent heating increased, and consequently the updraft velocity was stronger.

    On the other hand, the increased ice deposition consumed more water vapor at middle troposphere, which induces a competition for water vapor between heterogeneous and homogeneous freezing and nucleation. As a result, dust suppressed the homogeneous droplet freezing and nucleation due to the heterogeneous droplet freezing and the weakened transport of water vapor at lower stratosphere, respectively. These effects led to decreased number concentration of ice cloud particles in the upper troposphere, and consequently lowered the cloud top height during the stratus precipitating stage.

    Acting as IN, mineral dust also influenced precipitation in deep convection. It initiated earlier the collection because dust-related heterogeneous nucleation and freezing at middle troposphere occur earlier than homogeneous nucleation at higher altitudes. Nevertheless, the convective precipitation was suppressed by reduced collection of large graupel particles and insufficient fallout related to decreased sizes of precipitating ice hydrometeors

  2. Dynamics of homogeneous nucleation

    DEFF Research Database (Denmark)

    Toxværd, Søren

    2015-01-01

    The classical nucleation theory for homogeneous nucleation is formulated as a theory for a density fluctuation in a supersaturated gas at a given temperature. But molecular dynamics simulations reveal that it is small cold clusters which initiates the nucleation. The temperature in the nucleating...... clusters fluctuates, but the mean temperature remains below the temperature in the supersaturated gas until they reach the critical nucleation size. The critical nuclei have, however, a temperature equal to the supersaturated gas. The kinetics of homogeneous nucleation is not only caused by a grow...... or shrink by accretion or evaporation of monomers only but also by an exponentially declining change in cluster size per time step equal to the cluster distribution in the supersaturated gas....

  3. The structural properties of uncompressed crystalline monolayers of alcohols CnH2n+1OH(n=13-31) on water and their role as ice nucleators

    DEFF Research Database (Denmark)

    Majewski, J.; Popovitz-Biro, R.; Bouwman, W.G.;

    1995-01-01

    to 13. The relative amount of two dimensional (2-D crystalline material formed fell drastically; shorter crystalline coherence lengths were also observed. For n = 31-18 the molecules are arranged in a rectangular cell (a approximate to 5 Angstrom, b increases from ca. 7.4 to ca. 8.2 Angstrom) with plane...... symmetry p1g1. For n vertical in the b direction; the tilt angle...... length, lattice dimensions, chain orientation, and molecular motion, may be correlated with the ice-nucleating efficiency of these alcohol monolayers as a function of n....

  4. Roosevelt Island Climate Evolution Project (RICE): A 65 Kyr ice core record of black carbon aerosol deposition to the Ross Ice Shelf, West Antarctica.

    Science.gov (United States)

    Edwards, Ross; Bertler, Nancy; Tuohy, Andrea; Neff, Peter; Proemse, Bernedette; Feiteng, Wang; Goodwin, Ian; Hogan, Chad

    2015-04-01

    Emitted by fires, black carbon aerosols (rBC) perturb the atmosphere's physical and chemical properties and are climatically active. Sedimentary charcoal and other paleo-fire records suggest that rBC emissions have varied significantly in the past due to human activity and climate variability. However, few paleo rBC records exist to constrain reconstructions of the past rBC atmospheric distribution and its climate interaction. As part of the international Roosevelt Island Climate Evolution (RICE) project, we have developed an Antarctic rBC ice core record spanning the past ~65 Kyr. The RICE deep ice core was drilled from the Roosevelt Island ice dome in West Antarctica from 2011 to 2013. The high depth resolution (~ 1 cm) record was developed using a single particle intracavity laser-induced incandescence soot photometer (SP2) coupled to an ice core melter system. The rBC record displays sub-annual variability consistent with both austral dry-season and summer biomass burning. The record exhibits significant decadal to millennial-scale variability consistent with known changes in climate. Glacial rBC concentrations were much lower than Holocene concentrations with the exception of several periods of abrupt increases in rBC. The transition from glacial to interglacial rBC concentrations occurred over a much longer time relative to other ice core climate proxies such as water isotopes and suggests . The protracted increase in rBC during the transition may reflected Southern hemisphere ecosystem / fire regime changes in response to hydroclimate and human activity.

  5. Perturbation and melting of snow and ice by the 13 November 1985 eruption of Nevado del Ruiz, Colombia, and consequent mobilization, flow and deposition of lahars

    Science.gov (United States)

    Pierson, T.C.; Janda, R.J.; Thouret, J.-C.; Borrero, C.A.

    1990-01-01

    A complex sequence of pyroclastic flows and surges erupted by Nevado del Ruiz volcano on 13 November 1985 interacted with snow and ice on the summit ice cap to trigger catastrophic lahars (volcanic debris flows), which killed more than 23,000 people living at or beyond the base of the volcano. The rapid transfer of heat from the hot eruptive products to about 10 km2 of the snowpack, combined with seismic shaking, produced large volumes of meltwater that flowed downslope, liquefied some of the new volcanic deposits, and generated avalanches of saturated snow, ice and rock debris within minutes of the 21:08 (local time) eruption. About 2 ?? 107 m3 of water was discharged into the upper reaches of the Molinos, Nereidas, Guali, Azufrado and Lagunillas valleys, where rapid entrainment of valley-fill sediment transformed the dilute flows and avalanches to debris flows. Computed mean velocities of the lahars at peak flow ranged up to 17 m s-1. Flows were rapid in the steep, narrow upper canyons and slowed with distance away from the volcano as flow depth and channel slope diminished. Computed peak discharges ranged up to 48,000 m3 s-1 and were greatest in reaches 10 to 20 km downstream from the summit. A total of about 9 ?? 107 m3 of lahar slurry was transported to depositional areas up to 104 km from the source area. Initial volumes of individual lahars increased up to 4 times with distance away from the summit. The sedimentology and stratigraphy of the lahar deposits provide compelling evidence that: (1) multiple initial meltwater pulses tended to coalesce into single flood waves; (2) lahars remained fully developed debris flows until they reached confluences with major rivers; and (3) debris-flow slurry composition and rheology varied to produce gradationally density-stratified flows. Key lessons and reminders from the 1985 Nevado del Ruiz volcanic eruption are: (1) catastrophic lahars can be generated on ice- and snow-capped volcanoes by relatively small eruptions; (2

  6. Formation of the Martian Polar Layered Terrains: Quantifying Polar Water Ice and Dust Surface Deposition during Current and Past Orbital Epochs with the NASA Ames GCM

    Science.gov (United States)

    Emmett, Jeremy; Murphy, Jim

    2016-10-01

    Structural and compositional variability in the layering sequences comprising Mars' polar layered terrains (PLT's) is likely explained by orbital-forced climatic variations in the sedimentary cycles of water ice and dust from which they formed [1]. The PLT's therefore contain a direct, extensive record of the recent climate history of Mars encoded in their structure and stratigraphy, but deciphering this record requires understanding the depositional history of their dust and water ice constituents. 3D Mars atmosphere modeling enables direct simulation of atmospheric dynamics, aerosol transport and quantification of surface accumulation for a range of past and present orbital configurations. By quantifying the net yearly polar deposition rates of water ice and dust under Mars' current and past orbital configurations characteristic of the last several millions of years, and integrating these into the present with a time-stepping model, the formation history of the north and south PLT's will be investigated, further constraining their age and composition, and, if reproducible, revealing the processes responsible for prominent features and stratigraphy observed within the deposits. Simulating the formation of the deposits by quantifying net deposition rates during past orbital epochs and integrating these into the present, effectively 'rebuilding' the terrains, could aid in understanding deeper stratigraphic trends, correlating between geographically-separated deposits, explaining the presence and shapes of large-scale polar features, and correlating stratigraphy with geological time. Quantification of the magnitude and geographical distribution of surface aerosol accumulation will build on the work of previous GCM-based investigations [3]. Construction and analysis of hypothetical stratigraphic sequences in the PLT's will draw from previous climate-controlled stratigraphy methodologies [2,4], but will utilize GCM-derived net deposition rates to model orbital

  7. Changes in Black Carbon Deposition to Antarctica from Two Ice Core Records, A.D. 1850-2000

    Science.gov (United States)

    Bisiaux, Marion M.; Edward, Ross; McConnell, Joseph R.; Curran, Mark A. J.; VanOmmen, Tas D.; Smith, Andrew M.; Neumann, Thomas A.; Pasteris, Daniel R.; Penner, Joyce E.; Taylor, Kendrick

    2012-01-01

    Continuous flow analysis was based on a steady sample flow and in-line detection of BC and other chemical substances as described in McConnell et al. (2007). In the cold room, previously cut one meter ice core sticks of 3x3cm, are melted continuously on a heated melter head specifically designed to eliminate contamination from the atmosphere or by the external parts of the ice. The melted ice from the most inner part of the ice stick is continuously pumped by a peristaltic pump and carried to a clean lab by Teflon lines. The recorded signal is continuous, integrating a sample volume of about 0.05 mL, for which the temporal resolution depends on the speed of melting, ice density and snow accumulation rate at the ice core drilling site. For annual accumulation derived from the WAIS and Law Dome ice cores, we assumed 3.1 cm water equivalent uncertainty in each year's accumulation from short scale spatial variability (glaciological noise) which was determined from several measurements of annual accumulation in multiple parallel ice cores notably from the WAIS Divide ice core site (Banta et al., 2008) and from South Pole site (McConnell et al., 1997; McConnell et al., 2000). Refractory black carbon (rBC) concentrations were determined using the same method as in (Bisiaux et al., 2011) and adapted to continuous flow measurements as described by (McConnell et al., 2007). The technique uses a single particle intracavity laser induced incandescence photometer (SP2, Droplet Measurement Technologies, Boulder, Colorado) coupled to an ultrasonic nebulizer/desolvation (CETAC UT5000) Flow Injection Analysis (FIA). All analyses, sample preparation etc, were performed in a class 100 cleanroom using anti contamination "clean techniques". The samples were not acidified.

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

    Directory of Open Access Journals (Sweden)

    I. Crawford

    2011-09-01

    Full Text Available The ice nucleation efficiency of propane flame soot particles with and without a sulphuric acid coating was investigated using the aerosol and cloud chamber facility AIDA (Aerosol Interaction and Dynamics in the Atmosphere. The test soot for cloud formation simulations was produced using a propane flame Combustion Aerosol Standard generator (CAST, Jing-CAST Technologies. The organic carbon content (OC of the test soot was altered in a reproducible fashion by changing the fuel/air mixture of the generator. The soot content of ice nuclei was subsequently investigated using a combination of a pumped counterflow virtual impactor (PCVI to separate and evaporate the ice crystals, and a DMT single particle soot photometer (SP2 to examine the mixing state of the BC containing ice residuals.

    Ice nucleation was found to be most efficient for uncoated soot of low organic carbon content (~5 % organic carbon content where deposition freezing occurred at an ice saturation ratio Sice ~ 1.22 at a temperature T = 226.6 K with 25 % of the test soot becoming active as ice nuclei. Propane flame soot of higher organic carbon content (~30 % and ~70 % organic carbon content showed significantly lower ice nucleation efficiency (an activated fraction of the order of a few percent in the experiments than the low organic carbon content soot, with water saturation being required for freezing to occur. Ice nucleation occurred over the range Sice = 1.22–1.70, and T = 223.2–226.6 K. Analysis of the SP2 data showed that the 5 % organic carbon content soot had an undetectable OC coating whereas the 30 % organic carbon content soot had a thicker or less volatile OC coating.

    The application of a sulphuric acid coating to the flame soot shifted the threshold of the onset of freezing towards that of the homogeneous freezing of sulphuric acid; for the minimum OC flame soot this inhibited nucleation since the

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

    Directory of Open Access Journals (Sweden)

    I. Crawford

    2011-04-01

    Full Text Available The ice nucleation efficiency of propane flame soot particles with and without a sulphuric acid coating was investigated using the aerosol and cloud chamber facility AIDA (Aerosol Interaction and Dynamics in the Atmosphere. The test soot for cloud formation simulations was produced using a propane flame Combustion Aerosol Standard generator (CAST, Jing-CAST Technologies. The organic carbon content (OC of the test soot was altered in a reproducible fashion by changing the fuel/air mixture of the generator. The soot content of ice nuclei was subsequently investigated using a combination of a pumped counterflow virtual impactor (PCVI to separate and evaporate the ice crystals, and a DMT single particle soot photometer (SP2 to examine the mixing state of the BC containing ice residuals.

    Ice nucleation was found to be most efficient for uncoated soot of low organic carbon content (~5% organic carbon content where deposition freezing occurred at an ice saturation ratio Sice~1.22 at a temperature T = 226.6 K with 25% of the test soot becoming active as ice nuclei. Propane flame soot of higher organic carbon content (~30% and ~70% organic carbon content showed significantly lower ice nucleation efficiency (an activated fraction of the order of a few percent in the experiments than the low organic carbon content soot, with water saturation being required for freezing to occur. Ice nucleation occurred over the range Sice = 1.22–1.70, and T = 223.2–226.6 K. Analysis of the SP2 data showed that the 5% organic carbon content soot had an undetectable OC coating whereas the 30% organic carbon content soot had a thicker or less volatile OC coating.

    The application of a sulphuric acid coating to the flame soot shifted the threshold of the onset of freezing towards that of the homogeneous freezing of sulphuric acid; for the minimum OC flame soot this inhibited nucleation since the onset of

  10. NUCLEATION STUDIES OF GOLD ON CARBON ELECTRODES

    Directory of Open Access Journals (Sweden)

    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.

  11. Atomic Layer Deposition of Hafnium(IV) Oxide on Graphene Oxide: Probing Interfacial Chemistry and Nucleation by using X-ray Absorption and Photoelectron Spectroscopies.

    Science.gov (United States)

    Alivio, Theodore E G; De Jesus, Luis R; Dennis, Robert V; Jia, Ye; Jaye, Cherno; Fischer, Daniel A; Singisetti, Uttam; Banerjee, Sarbajit

    2015-07-27

    Interfacing graphene with metal oxides is of considerable technological importance for modulating carrier density through electrostatic gating as well as for the design of earth-abundant electrocatalysts. Herein, we probe the early stages of the atomic layer deposition (ALD) of HfO2 on graphene oxide using a combination of C and O K-edge near-edge X-ray absorption fine structure spectroscopies and X-ray photoelectron spectroscopy. Dosing with water is observed to promote defunctionalization of graphene oxide as a result of the reaction between water and hydroxyl/epoxide species, which yields carbonyl groups that further react with migratory epoxide species to release CO2 . The carboxylates formed by the reaction of carbonyl and epoxide species facilitate binding of Hf precursors to graphene oxide surfaces. The ALD process is accompanied by recovery of the π-conjugated framework of graphene. The delineation of binding modes provides a means to rationally assemble 2D heterostructures. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  12. Nucleation and Crystallization in nucleated Polymers

    Science.gov (United States)

    Schick, Christoph; Zhuravlev, Evgeny; Wurm, Andreas

    2012-02-01

    Crystallization is commonly considered as nucleation followed by a growth process. Here we apply the recently developed technique, differential fast scanning calorimetry (DFSC), for a unique, new look at the crystal growth of poly(epsilon-caprolactone) (PCL) and PCL carbon nanotube composites from 185 K, below the glass transition temperature, to 330 K, close to the equilibrium melting temperature. The DFSC allows temperature control of the sample and determination of its heat capacity during temperature treatments by employing cooling and heating rates from 50 to 50,000 K/s. First, the crystal nucleation and overall crystallization half times were determined simultaneously in the range of temperatures where crystallization of PCL occurs. After attempting to analyze the experiments with the classical nucleation and growth model a new methodology is described, which addresses the specific problems of crystallization of flexible linear macromolecules. The structures seem to range from having practically unmeasurable latent heats of ordering (nuclei) to being clearly-recognizable, ordered species with rather sharp disordering endotherms at temperatures from the glass transition to equilibrium melting (increasingly perfect and larger crystals). The mechanisms and kinetics of growth (if any) involve a detailed understanding of the interaction with the surrounding rigid amorphous fraction (RAF) in dependence of crystal size and perfection. E. Zhuravlev, J.W.P. Schmelzer, B. Wunderlich and C. Schick, Kinetics of nucleation and crystallization in poly(epsilon-caprolactone) (PCL), Polymer 52 (2011) 1983-1997.

  13. Stacking disorder in ice I.

    Science.gov (United States)

    Malkin, Tamsin L; Murray, Benjamin J; Salzmann, Christoph G; Molinero, Valeria; Pickering, Steven J; Whale, Thomas F

    2015-01-07

    Traditionally, ice I was considered to exist in two well-defined crystalline forms at ambient pressure: stable hexagonal ice (ice Ih) and metastable cubic ice (ice Ic). However, it is becoming increasingly evident that what has been called cubic ice in the past does not have a structure consistent with the cubic crystal system. Instead, it is a stacking-disordered material containing cubic sequences interlaced with hexagonal sequences, which is termed stacking-disordered ice (ice Isd). In this article, we summarise previous work on ice with stacking disorder including ice that was called cubic ice in the past. We also present new experimental data which shows that ice which crystallises after heterogeneous nucleation in water droplets containing solid inclusions also contains stacking disorder even at freezing temperatures of around -15 °C. This supports the results from molecular simulations, that the structure of ice that crystallises initially from supercooled water is always stacking-disordered and that this metastable ice can transform to the stable hexagonal phase subject to the kinetics of recrystallization. We also show that stacking disorder in ice which forms from water droplets is quantitatively distinct from ice made via other routes. The emerging picture of ice I is that of a very complex material which frequently contains stacking disorder and this stacking disorder can vary in complexity depending on the route of formation and thermal history.

  14. Nucleation in food colloids

    Science.gov (United States)

    Povey, Malcolm J. W.

    2016-12-01

    Nucleation in food colloids has been studied in detail using ultrasound spectroscopy. Our data show that classical nucleation theory (CNT) remains a sound basis from which to understand nucleation in food colloids and analogous model systems using n-alkanes. Various interpretations and modifications of CNT are discussed with regard to their relevance to food colloids. Much of the evidence presented is based on the ultrasound velocity spectrometry measurements which has many advantages for the study of nucleating systems compared to light scattering and NMR due to its sensitivity at low solid contents and its ability to measure true solid contents in the nucleation and early crystal growth stages. Ultrasound attenuation spectroscopy also responds to critical fluctuations in the induction region. We show, however, that a periodic pressure fluctuation such as a quasi-continuous (as opposed to a pulse comprising only a few pressure cycles) ultrasound field can alter the nucleation process, even at very low acoustic intensity. Thus care must be taken when using ultrasound techniques that the measurements do not alter the studied processes. Quasi-continuous ultrasound fields may enhance or suppress nucleation and the criteria to determine such effects are derived. The conclusions of this paper are relevant to colloidal systems in foods, pharmaceuticals, agro-chemicals, cosmetics, and personal products.

  15. Nonequilibrium thermodynamics of nucleation

    Energy Technology Data Exchange (ETDEWEB)

    Schweizer, M., E-mail: marco.schweizer@math.ethz.ch [ETH Zurich, Department of Materials, Polymer Physics, Vladimir-Prelog-Weg 2, 8093 Zurich (Switzerland); Sagis, L. M. C., E-mail: leonard.sagis@wur.nl [ETH Zurich, Department of Materials, Polymer Physics, Vladimir-Prelog-Weg 2, 8093 Zurich (Switzerland); Food Physics Group, Wageningen University, Bornse Weilanden, 6708 WG Wageningen (Netherlands)

    2014-12-14

    We present a novel approach to nucleation processes based on the GENERIC framework (general equation for the nonequilibrium reversible-irreversible coupling). Solely based on the GENERIC structure of time-evolution equations and thermodynamic consistency arguments of exchange processes between a metastable phase and a nucleating phase, we derive the fundamental dynamics for this phenomenon, based on continuous Fokker-Planck equations. We are readily able to treat non-isothermal nucleation even when the nucleating cores cannot be attributed intensive thermodynamic properties. In addition, we capture the dynamics of the time-dependent metastable phase being continuously expelled from the nucleating phase, and keep rigorous track of the volume corrections to the dynamics. Within our framework the definition of a thermodynamic nuclei temperature is manifest. For the special case of nucleation of a gas phase towards its vapor-liquid coexistence, we illustrate that our approach is capable of reproducing recent literature results obtained by more microscopic considerations for the suppression of the nucleation rate due to nonisothermal effects.

  16. 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

  17. Surface effects in nucleation

    CERN Document Server

    Alekseechkin, Nikolay V

    2016-01-01

    The classical nucleation theory (CNT) concept of a nucleus as a fragment of the bulk new phase fails for nanosized nuclei. An extension of CNT taking into account the properties of the transition region between coexisting bulk phases is proposed. For this purpose, the finite-thickness layer method which is an alternative to the Gibbs one is used; the transition region is considered as a separate (surface) phase. An equation for the nucleation work is derived which is basic for the multivariable theory of nucleation.

  18. Implications of the ISOCLOUD campaigns at the AIDA Cloud Chamber for ice growth in cold cirrus

    Science.gov (United States)

    Lamb, Kara; Clouser, Benjamin; Sarkozy, Laszlo; Wagner, Steven; Ebert, Volker; Kerstel, Erik; Saathoff, Harald; Möhler, Ottmar; Moyer, Elisabeth

    2015-04-01

    In-situ water vapor measurements in the upper troposphere and lower stratosphere (UTLS) have routinely observed anomalous supersaturations on the order of 10-20particles when temperatures were below 200 K, raising questions about the physics of how ice forms at cold temperatures in the atmosphere1,2,3,4. The ISOCLOUD campaigns in 2012-2013 at the AIDA Aerosol and Cloud Chamber sought to investigate ice growth at cold temperatures by simulating cirrus clouds at temperatures and pressures characteristic of the upper troposphere. Experiments tested both homogeneous nucleation of sulfate aerosols and heterogeneous nucleation with various ice nuclei, including mineral dust and organic aerosols with and without nitric acid coatings. Optical instruments, both in-situ (TDLAS) and extractive (TDLAS and OFCEAS), measured ice particle number density, water vapor, total water, and water vapor isotopic concentrations, with multiple instruments measuring water. In a series of cirrus formation experiments, we observed no evidence of anomalous saturation vapor pressure and no evidence of ice growth inhibition at low temperatures for the parameter space tested during the ISOCLOUD campaigns. That is, we see no evidence for temperature dependence in the deposition coefficient. In these experiments we determined the deposition coefficient from bulk parameters of the gas (vapor concentration and ice number density). The ISOCLOUD experiments were particularly suited to deposition coefficient measurements since they involved lower pressures and often lower temperatures than previous similar campaigns, producing lower error bars.5 These results can aid in the interpretation of data from aircraft campaigns in the UTLS by solidifying our understanding of the microphysics of ice formation at cold temperatures. [1] Gao, R. et al., Science, 303, no. 6567, 516-520, (2004). [2] Jensen, E. et al., Atmos. Chem. Phys., 5, 851-862, (2005). [3] Peter, T. et al., Science, 314, no. 5804, 1399

  19. Surface Bubble Nucleation Stability

    NARCIS (Netherlands)

    Seddon, James Richard Thorley; Kooij, Ernst S.; Poelsema, Bene; Zandvliet, Henricus J.W.; Lohse, Detlef

    2011-01-01

    Recent research has revealed several different techniques for nanoscopic gas nucleation on submerged surfaces, with findings seemingly in contradiction with each other. In response to this, we have systematically investigated the occurrence of surface nanobubbles on a hydrophobized silicon substrate

  20. Characterization of the Micro-Orifice Uniform Deposit Impactor-droplet freezing technique (MOUDI-DFT) for size-resolved quantitative measurements of ice nuclei

    Science.gov (United States)

    Mason, Ryan; Si, Meng; Li, Jixiao; Huffman, J. Alex; McCluskey, Christina; Levin, Ezra; Irish, Victoria; Chou, Cédric; Hill, Thomas; Ladino, Luis; Yakobi, Jacqueline; Schiller, Corinne; Abbatt, Jon; DeMott, Paul; Bertram, Allan

    2014-05-01

    Ice formation within a cloud system can significantly modify its lifetime and radiative forcing. Many current instruments for measuring atmospheric concentrations of ice nuclei (IN) are not capable of providing size-resolved information. Such knowledge is useful in identifying the sources of IN and predicting their transport in the atmosphere. Furthermore, those that use size-discrimination to identify IN typically exclude particles with an aerodynamic diameter greater than 2.5 μm from analysis. Several studies have indicated this may be an important size regime for IN, particularly with those activating at warmer temperatures. The recently developed Micro-Orifice Uniform Deposit Impactor-droplet freezing technique (MOUDI-DFT) addresses these limitations through combining sample collection by a model of cascade impactor with an established immersion freezing apparatus. Here we present a characterization of the MOUDI-DFT and the development of a modified technique which address experimental uncertainties arising from sample deposit inhomogeneity and the droplet freezing method. An intercomparison with a continuous-flow diffusion chamber (CFDC) was performed. We also show preliminary results from a campaign undertaken in a remote coastal region of western Canada. Correlations between atmospheric IN concentrations and the abundance of suspended submicron and supermicron particles, biological aerosols, carbonaceous aerosols, and prevailing meteorological conditions were investigated.

  1. On the usage of classical nucleation theory in quantification of the impact of bacterial INP on weather and climate

    Science.gov (United States)

    Sahyoun, Maher; Wex, Heike; Gosewinkel, Ulrich; Šantl-Temkiv, Tina; Nielsen, Niels W.; Finster, Kai; Sørensen, Jens H.; Stratmann, Frank; Korsholm, Ulrik S.

    2016-08-01

    Bacterial ice-nucleating particles (INP) are present in the atmosphere and efficient in heterogeneous ice-nucleation at temperatures up to -2 °C in mixed-phase clouds. However, due to their low emission rates, their climatic impact was considered insignificant in previous modeling studies. In view of uncertainties about the actual atmospheric emission rates and concentrations of bacterial INP, it is important to re-investigate the threshold fraction of cloud droplets containing bacterial INP for a pronounced effect on ice-nucleation, by using a suitable parameterization that describes the ice-nucleation process by bacterial INP properly. Therefore, we compared two heterogeneous ice-nucleation rate parameterizations, denoted CH08 and HOO10 herein, both of which are based on classical-nucleation-theory and measurements, and use similar equations, but different parameters, to an empirical parameterization, denoted HAR13 herein, which considers implicitly the number of bacterial INP. All parameterizations were used to calculate the ice-nucleation probability offline. HAR13 and HOO10 were implemented and tested in a one-dimensional version of a weather-forecast-model in two meteorological cases. Ice-nucleation-probabilities based on HAR13 and CH08 were similar, in spite of their different derivation, and were higher than those based on HOO10. This study shows the importance of the method of parameterization and of the input variable, number of bacterial INP, for accurately assessing their role in meteorological and climatic processes.

  2. Size dependence of volume and surface nucleation rates for homogeneous freezing of supercooled water droplets

    Directory of Open Access Journals (Sweden)

    T. Kuhn

    2009-10-01

    Full Text Available We investigated the relative roles of volume and surface nucleation in the freezing of water droplets. Nucleation experiments were carried out in a cryogenic laminar aerosol flow tube using supercooled liquid water aerosols with radii between about 1 and 3 μ m. Temperature- and size-dependent values of volume- and surface-based homogeneous nucleation rate between 234.8 and 236.2 K are derived with help of a microphysical model from aerosol compositions and size distributions based on infrared extinction measurements in the aerosol flow tube. The results show that the contribution from nucleation at the droplet surface increases with decreasing droplet radius and dominates over nucleation in the bulk droplet volume for droplets with radii smaller than approximately 5 μm. This is interpreted in terms of a lowered free energy of ice germ formation in the surface-based process and has implications for the parameterization of homogeneous ice nucleation in numerical models.

  3. Atmospheric depositions of black carbon, inorganic pollutants and mineral dust from the Ortles, Eastern European Alps ice cores during the last 3000 years

    Science.gov (United States)

    Bertò, Michele; Barbante, Carlo; Gabrielli, Paolo; Gabrieli, Jacopo; Spolaor, Andrea; Dreossi, Giuliano; Laj, Paolo; Zanatta, Marco; Stenni, Barbara

    2017-04-01

    Reconstructions of the atmospheric content of black carbon, heavy metals and mineral dust covering millennial time scales are rare, particularly in the European region. Evaluating the human impact on the environment through mining and