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

2014 ◽  
Vol 7 (9) ◽  
pp. 9137-9172 ◽  
Author(s):  
C. Budke ◽  
T. Koop

Abstract. A new optical freezing array for the study of heterogeneous ice nucleation in microliter-sized droplets is introduced, tested and applied to the study of immersion freezing in aqueous Snomax® suspensions. In the Bielefeld Ice Nucleation ARraY (BINARY) ice nucleation can be studied simultaneously in 36 droplets at temperatures down to −40 °C (233 K) and at cooling rates between 0.1 K min−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 minute time dependence of ice nucleation induced by Class A and Class C ice nucleators contained in Snomax® was detected. For the Class A IN a very strong increase of the heterogeneous ice nucleation rate coefficient with decreasing temperature of λ ≡ −dln(jhet)/dT = 8.7 K−1 was observed emphasizing the capability of the BINARY device. This value is larger than those of other types of IN reported in the literature, suggesting that the BINARY setup is suitable for quantifying time dependence for most other IN of atmospheric interest, making it a useful tool for future investigations.

2015 ◽  
Vol 8 (2) ◽  
pp. 689-703 ◽  
Author(s):  
C. Budke ◽  
T. Koop

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


2021 ◽  
Author(s):  
Jonas Jakobsson ◽  
Vaughan Phillips ◽  
Thomas Bjerring-Kristensen

Abstract. The time dependence of ice-nucleating particle (INP) activity is known to exist, yet for simplicity it is often omitted in atmospheric models as an approximation. Hitherto only limited experimental work has been done to quantify this time dependency, for which published data are especially scarce regarding ambient aerosol samples and longer time scales. In this study, the time dependence of INP activity is quantified experimentally for ambient environmental samples. The experimental approach includes a series of hybrid experiments with alternating constant cooling and isothermal experiments using a recently developed cold-stage setup called the Lund University Cold-Stage (LUCS). This approach of observing ambient aerosol samples provides the optimum realism for representing their time dependence in any model. Six ambient aerosol samples were collected representing aerosol conditions likely influenced by these types of INPs: marine, mineral dust, continental pristine, continental polluted, combustion-related and rural continental aerosol. Active INP concentrations were seen to be augmented by about 40 % to 100 % (or 70 % to 200 %), depending on the sample, over 2 (or 10) hours. This degree of time dependence observed was comparable to that seen in previous published works. Our observations show that the minority of active ice nuclei (IN) with strong time dependency on hourly time scales display only weak time dependence on short time scales of a few minutes. A general tendency was observed for the natural time scale of the freezing to dilate increasingly with time. The fractional freezing rate was observed to steadily declines exponentially with the order of magnitude (logarithm) of the time since the start of isothermal conditions. A representation of time dependence for incorporation into schemes of heterogeneous ice nucleation that currently omit time dependence is proposed.


2020 ◽  
Author(s):  
Hinrich Grothe ◽  
Teresa M. Seifried ◽  
Paul Bieber ◽  
Laura Felgitsch

<p>Several biological particles are able to trigger heterogeneous ice nucleation at subzero temperatures above -38°C. Many plants species such as winter rye [1], certain berries [2], pines and birches [3, 4] are known to contain biological ice-nucleating particles (BINPs) or rather ice-nucleating macromolecules (INMs). However, the influence of these BINPs on atmospheric processes including cloud glaciation and precipitation formation, as well as transport mechanisms of BINPs from the land surface into the atmosphere remain uncertain. If those INMs are easily available on the surfaces of a plant, they could be washed down by heavy rain events and could add an important new source for BINPs in the atmosphere, which has not received enough attention in the past.</p><p>In this study, we have focused on alpine trees, which form INMs extractable from their surfaces. We examined ice nucleation activity of samples from different birches (Betula pendula) and pines (Pinus sylvestris) growing in the Alps in Austria, Europe. Filtered aqueous extracts of leaves, needles, bark and wood were analyzed in the laboratory in terms of heterogeneous ice nucleation using VODCA (Vienna Optical Droplet Crystallization Analyzer), a cryo-microscope  for  emulsion  samples.  All plant tissues contained INMs in the submicron size range. Furthermore, we conducted a field experiment, in which we investigated the possibility of INMs to be released from the surface of the trees into the atmosphere during rain showers.</p><p>[1] Brush, R.A., M. Griffith, and A. Mlynarz, Characterization and Quantification of Intrinsic Ice Nucleators in Winter Rye (Secale cereale) Leaves. Plant Physiol, 1994. <strong>104</strong>(2): p. 725-735.</p><p>[2] Felgitsch, L., et al., Heterogeneous Freezing of Liquid Suspensions Including Juices and Extracts from Berries and Leaves from Perennial Plants. Atmosphere, 2019. <strong>10</strong>(1): p. 1-22.</p><p> [3] Pomeroy, M.K., D. Siminovitch, and F. Wightman, Seasonal biochemical changes in the living bark and needles of red pine (Pinus resinosa) in relation to adaptation to freezing. Canadian Journal of Botany, 1970. <strong>48</strong>(5): p. 953-967.</p><p>[4] Felgitsch, L., et al., Birch leaves and branches as a source of ice-nucleating macromolecules. Atmospheric Chemistry and Physics, 2018. <strong>18</strong>(21): p. 16063-16079.</p><p>[5] Pummer, B.G., et al., Ice nucleation by water-soluble macromolecules. Atmospheric Chemistry and Physics, 2015. <strong>15</strong>(8): p. 4077-4091.</p>


2007 ◽  
Vol 7 (19) ◽  
pp. 5081-5091 ◽  
Author(s):  
C. Marcolli ◽  
S. Gedamke ◽  
T. Peter ◽  
B. Zobrist

Abstract. A differential scanning calorimeter (DSC) was used to explore heterogeneous ice nucleation of emulsified aqueous suspensions of two Arizona test dust (ATD) samples with particle diameters of nominally 0–3 and 0–7 μm, respectively. Aqueous suspensions with ATD concentrations of 0.01–20 wt% have been investigated. The DSC thermograms exhibit a homogeneous and a heterogeneous freezing peak whose intensity ratios vary with the ATD concentration in the aqueous suspensions. Homogeneous freezing temperatures are in good agreement with recent measurements by other techniques. Depending on ATD concentration, heterogeneous ice nucleation occurred at temperatures as high as 256 K or down to the onset of homogeneous ice nucleation (237 K). For ATD-induced ice formation Classical Nucleation Theory (CNT) offers a suitable framework to parameterize nucleation rates as a function of temperature, experimentally determined ATD size, and emulsion droplet volume distributions. The latter two quantities serve to estimate the total heterogeneous surface area present in a droplet, whereas the suitability of an individual heterogeneous site to trigger nucleation is described by the compatibility function (or contact angle) in CNT. The intensity ratio of homogeneous to heterogeneous freezing peaks is in good agreement with the assumption that the ATD particles are randomly distributed amongst the emulsion droplets. The observed dependence of the heterogeneous freezing temperatures on ATD concentrations cannot be described by assuming a constant contact angle for all ATD particles, but requires the ice nucleation efficiency of ATD particles to be (log)normally distributed amongst the particles. Best quantitative agreement is reached when explicitly assuming that high-compatibility sites are rare and that therefore larger particles have on average more and better active sites than smaller ones. This analysis suggests that a particle has to have a diameter of at least 0.1 μm to exhibit on average one active site.


2018 ◽  
Vol 18 (20) ◽  
pp. 15437-15450 ◽  
Author(s):  
Matthias Hummel ◽  
Corinna Hoose ◽  
Bernhard Pummer ◽  
Caroline Schaupp ◽  
Janine Fröhlich-Nowoisky ◽  
...  

Abstract. Primary ice formation, which is an important process for mixed-phase clouds with an impact on their lifetime, radiative balance, and hence the climate, strongly depends on the availability of ice-nucleating particles (INPs). Supercooled droplets within these clouds remain liquid until an INP immersed in or colliding with the droplet reaches its activation temperature. Only a few aerosol particles are acting as INPs and the freezing efficiency varies among them. Thus, the fraction of supercooled water in the cloud depends on the specific properties and concentrations of the INPs. Primary biological aerosol particles (PBAPs) have been identified as very efficient INPs at high subzero temperatures, but their very low atmospheric concentrations make it difficult to quantify their impact on clouds. Here we use the regional atmospheric model COSMO–ART to simulate the heterogeneous ice nucleation by PBAPs during a 1-week case study on a domain covering Europe. We focus on three highly ice-nucleation-active PBAP species, Pseudomonas syringae bacteria cells and spores from the fungi Cladosporium sp. and Mortierella alpina. PBAP emissions are parameterized in order to represent the entirety of bacteria and fungal spores in the atmosphere. Thus, only parts of the simulated PBAPs are assumed to act as INPs. The ice nucleation parameterizations are specific for the three selected species and are based on a deterministic approach. The PBAP concentrations simulated in this study are within the range of previously reported results from other modeling studies and atmospheric measurements. Two regimes of PBAP INP concentrations are identified: a temperature-limited and a PBAP-limited regime, which occur at temperatures above and below a maximal concentration at around −10 ∘C, respectively. In an ensemble of control and disturbed simulations, the change in the average ice crystal concentration by biological INPs is not statistically significant, suggesting that PBAPs have no significant influence on the average state of the cloud ice phase. However, if the cloud top temperature is below −15 ∘C, PBAP can influence the cloud ice phase and produce ice crystals in the absence of other INPs. Nevertheless, the number of produced ice crystals is very low and it has no influence on the modeled number of cloud droplets and hence the cloud structure.


2008 ◽  
Vol 5 (6) ◽  
pp. 373 ◽  
Author(s):  
Roya Mortazavi ◽  
Christopher T. Hayes ◽  
Parisa A. Ariya

Environmental context. Biological ice nucleators have been found to freeze water at very warm temperatures. The potential of bio-aerosols to greatly influence cloud chemistry and microphysics is becoming increasingly apparent, yet detailed knowledge of their actual role in atmospheric processes is lacking. The formation of ice in the atmosphere has significant local, regional and global influence, ranging from precipitation to cloud nucleation and thus climate. Ice nucleation tests on bacteria isolated from snow and laboratory-grown bacteria, in comparison with those of known organic and inorganic aerosols, shed light on this issue. Abstract. Ice nucleation experiments on bacteria isolated from snow as well as grown in the laboratory, in comparison with those of known organic and inorganic aerosols, examined the importance of bio-aerosols on cloud processes. Snow samples were collected from urban and suburban sites in the greater Montreal region in Canada (45°28′N, 73°45′W). Among many snow bacterial isolates, eight types of bacterial species, none belonging to known effective ice nucleators such as Pseudomonas or Erwinia genera, were identified to show an intermediate range of ice nucleation activity (–12.9 ± 1.3°C to –17.5 ± 2.8°C). Comparable results were also obtained for molten snow samples and inorganic suspensions (kaolin and montmorillonite) of buffered water solutions. The presence of organic molecules (oxalic, malonic and succinic acids) had minimal effect (<2°C) on ice nucleation. Considering experimental limitations, and drawing from observation in snow samples of a variety of bacterial populations with variable ice-nucleation ability, a shift in airborne-species population may significantly alter glaciation processes in clouds.


2016 ◽  
Vol 16 (10) ◽  
pp. 6495-6509 ◽  
Author(s):  
Karoliina Ignatius ◽  
Thomas B. Kristensen ◽  
Emma Järvinen ◽  
Leonid Nichman ◽  
Claudia Fuchs ◽  
...  

Abstract. 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.


2021 ◽  
Author(s):  
Ralph Schwidetzky ◽  
Max Lukas ◽  
Anna T. Kunert ◽  
Ulrich Pöschl ◽  
Janine Fröhlich-Nowoisky ◽  
...  

&lt;p&gt;Bacterial ice-nucleating proteins (INPs) promote heterogeneous ice nucleation better than any known material. On the molecular scale, bacterial INPs are believed to function by organizing water into ice&amp;#8209;like patterns to enable the formation of embryonic crystals. However, the details of their working mechanism remains largely elusive. Here, we report the results of comprehensive evaluations of environmentally relevant effects such as changes in pH, the presence of ions and temperature on the activity, three-dimensional structure and hydration shell of bacterial ice nucleators using ice affinity purification, high-throughput ice nucleation assays and surface-specific sum-frequency generation spectroscopy.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;[1] Lukas, Max, et al. &quot;Electrostatic Interactions Control the Functionality of Bacterial Ice Nucleators.&quot; Journal of the American Chemical Society 142.15 (2020): 6842-6846.&lt;/p&gt;&lt;p&gt;[2] Lukas, Max, et al. &quot;Interfacial Water Ordering Is Insufficient to Explain Ice-Nucleating Protein Activity.&quot; The Journal of Physical Chemistry Letters 12 (2020): 218-223.&lt;/p&gt;


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