Ice in Clouds Experiment–Layer Clouds. Part II: Testing Characteristics of Heterogeneous Ice Formation in Lee Wave Clouds

2012 ◽  
Vol 69 (3) ◽  
pp. 1066-1079 ◽  
Author(s):  
P. R. Field ◽  
A. J. Heymsfield ◽  
B. J. Shipway ◽  
P. J. DeMott ◽  
K. A. Pratt ◽  
...  

Abstract Heterogeneous ice nucleation is a source of uncertainty in models that represent ice clouds. The primary goal of the Ice in Clouds Experiment–Layer Clouds (ICE-L) field campaign was to determine if a link can be demonstrated between ice concentrations and the physical and chemical characteristics of the ambient aerosol. This study combines a 1D kinematic framework with lee wave cloud observations to infer ice nuclei (IN) concentrations that were compared to IN observations from the same flights. About 30 cloud penetrations from six flights were modeled. The temperature range of the observations was −16° to −32°C. Of the three simplified ice nucleation representations tested (deposition, evaporation freezing, and condensation/immersion droplet freezing), condensation/immersion freezing reproduced the lee wave cloud observations best. IN concentrations derived from the modeling ranged from 0.1 to 13 L−1 compared to 0.4 to 6 L−1 from an IN counter. A better correlation was found between temperature and the ratio of IN concentration to the concentration of large aerosol (>500 nm) than between IN concentration and the large aerosol concentration or temperature alone.

2010 ◽  
Vol 67 (8) ◽  
pp. 2483-2503 ◽  
Author(s):  
Corinna Hoose ◽  
Jón Egill Kristjánsson ◽  
Jen-Ping Chen ◽  
Anupam Hazra

Abstract An ice nucleation parameterization based on classical nucleation theory, with aerosol-specific parameters derived from experiments, has been implemented into a global climate model—the Community Atmosphere Model (CAM)-Oslo. The parameterization treats immersion, contact, and deposition nucleation by mineral dust, soot, bacteria, fungal spores, and pollen in mixed-phase clouds at temperatures between 0° and −38°C. Immersion freezing is considered for insoluble particles that are activated to cloud droplets, and deposition and contact nucleation are only allowed for uncoated, unactivated aerosols. Immersion freezing by mineral dust is found to be the dominant ice formation process, followed by immersion and contact freezing by soot. The simulated biological aerosol contribution to global atmospheric ice formation is marginal, even with high estimates of their ice nucleation activity, because the number concentration of ice nucleation active biological particles in the atmosphere is low compared to other ice nucleating aerosols. Because of the dominance of mineral dust, the simulated ice nuclei concentrations at temperatures below −20°C are found to correlate with coarse-mode aerosol particle concentrations. The ice nuclei (IN) concentrations in the model agree well overall with in situ continuous flow diffusion chamber measurements. At individual locations, the model exhibits a stronger temperature dependence on IN concentrations than what is observed. The simulated IN composition (77% mineral dust, 23% soot, and 10−5% biological particles) lies in the range of observed ice nuclei and ice crystal residue compositions.


2016 ◽  
Author(s):  
Claudia Marcolli ◽  
Baban Nagare ◽  
André Welti ◽  
Ulrike Lohmann

Abstract. AgI is one of the best investigated ice nuclei. It has relevance for the atmosphere since it is used for glaciogenic cloud seeding. Theoretical and experimental studies over the last sixty years provide a complex picture of silver iodide as ice nucleating agent with conflicting and inconsistent results. This review compares experimental ice nucleation studies in order to analyse the factors that influence the ice nucleation ability of AgI. We have performed experiments to compare contact and immersion freezing by AgI. This is one of three papers that describe and analyse contact and immersion freezing experiments with AgI. In Nagare et al. (Nagare, B., Marcolli, C., Stetzer, O., and Lohmann, U.: Comparison of measured and calculated collision efficiencies at low temperatures, Atmos. Chem. Phys., 15, 13759–13776, doi:10.5194/acp-15-13759-2015, 2015) collision efficiencies based on contact freezing experiments with AgI are determined and compared with theoretical formulations. In a companion paper, contact freezing experiments are compared with immersion freezing experiments conducted with AgI, kaolinite, and ATD as ice nuclei. 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. Ice nucleation by particles with surfaces exposed to air, depends on water adsorption. AgI surfaces seem to be most efficient as ice nuclei when they are exposed to relative humidity at or even above water saturation. For AgI particles that are totally immersed in water, the freezing temperature increases with increasing AgI surface area. Higher threshold freezing temperature 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 of ice nucleation in cloud chambers with short residence times.


2015 ◽  
Vol 15 (13) ◽  
pp. 7523-7536 ◽  
Author(s):  
G. P. Schill ◽  
K. Genareau ◽  
M. A. Tolbert

Abstract. 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.


2013 ◽  
Vol 13 (19) ◽  
pp. 9801-9818 ◽  
Author(s):  
P. Spichtinger ◽  
M. Krämer

Abstract. The occurrence of high, persistent ice supersaturation inside and outside cold cirrus in the tropical tropopause layer (TTL) remains an enigma that is intensely debated as the "ice supersaturation puzzle". However, it was recently confirmed that observed supersaturations are consistent with very low ice crystal concentrations, which is incompatible with the idea that homogeneous freezing is the major method of ice formation in the TTL. Thus, the tropical tropopause "ice supersaturation puzzle" has become an "ice nucleation puzzle". To explain the low ice crystal concentrations, a number of mainly heterogeneous freezing methods have been proposed. Here, we reproduce in situ measurements of frequencies of occurrence of ice crystal concentrations by extensive model simulations, driven by the special dynamic conditions in the TTL, namely the superposition of slow large-scale updraughts with high-frequency short waves. From the simulations, it follows that the full range of observed ice crystal concentrations can be explained when the model results are composed from scenarios with consecutive heterogeneous and homogeneous ice formation and scenarios with pure homogeneous ice formation occurring in very slow (< 1 cm s−1) and faster (> 1 cm s−1) large-scale updraughts, respectively. This statistical analysis shows that about 80% of TTL cirrus can be explained by "classical" homogeneous ice nucleation, while the remaining 20% stem from heterogeneous and homogeneous freezing occurring within the same environment. The mechanism limiting ice crystal production via homogeneous freezing in an environment full of gravity waves is the shortness of the gravity waves, which stalls freezing events before a higher ice crystal concentration can be formed.


2012 ◽  
Vol 12 (18) ◽  
pp. 8589-8610 ◽  
Author(s):  
R. Wagner ◽  
O. Möhler ◽  
H. Saathoff ◽  
M. Schnaiter ◽  
J. Skrotzki ◽  
...  

Abstract. 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 with the ice crystals during the preceding homogeneous freezing cycle exhibit pre-activation: they may retain small ice embryos in pores, have footprints on their surface which match the ice lattice, or simply have a much greater surface area or different surface microstructure compared to the unprocessed glassy aerosol particles. Pre-activation must be considered for the correct interpretation of experimental results on the heterogeneous ice nucleation ability of glassy aerosol particles and may provide a mechanism of producing a population of extremely efficient ice nuclei in the upper troposphere.


2013 ◽  
Vol 13 (11) ◽  
pp. 5751-5766 ◽  
Author(s):  
S. Hartmann ◽  
S. Augustin ◽  
T. Clauss ◽  
H. Wex ◽  
T. Šantl-Temkiv ◽  
...  

Abstract. 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 nucleation are attached to the outer membrane of intact bacteria or membrane fragments, (c) the temperature range in which heterogeneous droplet freezing occurs, and the fraction of droplets being able to freeze, both depend on the actual number of INA protein complexes present in the droplet ensemble, and (d) possible artifacts suspected to occur in connection with the drop freezing method, i.e., the method frequently used by biologist for quantifying ice nucleation behaviour, are of minor importance, at least for substances such as P. syringae, which induce freezing at comparably high temperatures. The last statement implies that for single ice nucleation entities such as INA protein complexes, it is the number of entities present in the droplet population, and the entities' nucleation rate, which control the freezing behaviour of the droplet population. Quantities such as ice active surface site density are not suitable in this context. The results obtained in this study allow a different perspective on the quantification of the immersion freezing behaviour of bacterial ice nucleation.


2011 ◽  
Vol 11 (8) ◽  
pp. 23139-23167 ◽  
Author(s):  
M. E. Wise ◽  
K. J. Baustian ◽  
T. Koop ◽  
M. A. Freedman ◽  
E. J. Jensen ◽  
...  

Abstract. Sea-salt aerosol particles (SSA) are ubiquitous in the marine boundary layer and over coastal areas. Therefore SSA have ability to directly and indirectly affect the Earth's radiation balance. The influence SSA have on climate is related to their water uptake and ice nucleation characteristics. In this study, optical microscopy coupled with Raman spectroscopy was used to detect the formation of an NaCl hydrate that could form under atmospheric conditions. NaCl(s) particles deliquesced at the well established value of 75.7 ± 2.5 % RH. NaCl(aq) particles effloresced to a mixture of hydrated and non-hydrated particles at temperatures between 236 and 252 K. The aqueous particles effloresced into the non-hydrated form at temperatures warmer than 252 K. At temperatures colder than 236 K all particles effloresced into the hydrated form. The deliquescence relative humidities (DRH) of hydrated NaCl(s) particles ranged from 76.6 to 93.2 % RH. Based on the measured DRH and efflorescence relative humidities (ERH), we estimate crystalline NaCl particles could be in the hydrated form 40–80 % of the time in the troposphere. Additionally, the ice nucleating abilities of NaCl(s) and hydrated NaCl(s) were determined at temperatures ranging from 221 to 238 K. NaCl(s) particles depositionally nucleated ice at an average Sice value of 1.11 ± 0.07. Hydrated NaCl(s) particles depositionally nucleated ice at an average Sice value of 1.02 ± 0.04. When a mixture of hydrated and anhydrous NaCl(s) particles was present in the same sample, ice preferentially nucleated on the hydrated particles 100 % of the time. While both types of particles are efficient ice nuclei, hydrated NaCl(s) particles are better ice nuclei than NaCl(s) particles.


2011 ◽  
Vol 11 (6) ◽  
pp. 17665-17698 ◽  
Author(s):  
I. Steinke ◽  
O. Möhler ◽  
A. Kiselev ◽  
M. Niemand ◽  
H. Saathoff ◽  
...  

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


2020 ◽  
Author(s):  
Anna J. Miller ◽  
Killian P. Brennan ◽  
Claudia Mignani ◽  
Jörg Wieder ◽  
Assaf Zipori ◽  
...  

Abstract. Aerosol-cloud interactions, including the ice nucleation of supercooled liquid water droplets caused by ice nucleating particles (INPs) and macromolecules (INMs), are a source of uncertainty in predicting future climate. Because of INPs' and INMs' spatial and temporal heterogeneity in source, number, and composition, predicting their concentration and distribution is a challenge, requiring apt analytical instrumentation. Here, we present the development of our drop Freezing Ice Nucleation Counter (FINC), a droplet freezing technique (DFT), for the quantification of INP and INM concentrations in the immersion freezing mode. FINC's design builds upon previous DFTs and uses an ethanol bath to cool sample aliquots while detecting freezing using a camera. Specifically, FINC uses 288 sample wells of 5–60 µL volume, has a limit of detection of −25.37 &amp;pm; 0.15 ˚C with 5 µL, and has an instrument temperature uncertainty of &amp;pm; 0.5 ˚C. We further conducted freezing control experiments to quantify the non-homogeneous behavior of our developed DFT, including the consideration of eight different sources of contamination. As part of the validation of FINC, an intercomparison campaign was conducted using an NX-illite suspension and an ambient aerosol sample with two other drop-freezing instruments: ETH's DRoplet Ice Nuclei Counter Zurich (DRINCZ) and University of Basel’s LED-based ice nucleation detection apparatus (LINDA). We also tabulated an exhaustive list of peer-reviewed DFTs, to which we added our characterized and validated FINC. In addition, we propose herein the use of a water-soluble biopolymer, lignin, as a suitable ice nucleating standard. An ideal INM standard should be inexpensive, accessible, reproducible, unaffected by sample preparation, and consistent across techniques. First, we show that commercial lignin has a consistent ice nucleating activity across product batches. Second, we demonstrate that aqueous lignin solutions exhibit good solution stability over time. Third, we compare its freezing temperature across different drop-freezing instruments, including on DRINCZ, LINDA, and on the Weizmann Institute's Supercooled Droplets Observation on a Microarray (WISDOM) and determine an empirical fit parameter for future drop freezing validations. With these findings, we aim to show that lignin can be used as a good immersion freezing standard in future technique intercomparisons in the field of atmospheric ice nucleation.


2009 ◽  
Vol 9 (5) ◽  
pp. 20949-20977 ◽  
Author(s):  
K. J. Baustian ◽  
M. E. Wise ◽  
M. A. Tolbert

Abstract. Heterogeneous ice nucleation on solid ammonium sulfate and solid amorphous 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 occurred preferentially on just a few ammonium sulfate and glutaric acid particles in each sample. For freezing temperatures between 214 K and 235 K average ice saturation ratios of S=1.10±0.07 for solid ammonium sulfate and S=1.39±0.16 for solid amorphous glutaric acid particles were determined. Experiments with externally mixed particles further show that ammonium sulfate is a more potent ice nucleus that 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 aerosol particles are available for ice formation. This pathway for ice formation may be particularly significant near the tropopause region where sulfates are abundant and other species known to be good ice nuclei are depleted.


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