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

2005 ◽  
Vol 5 (3) ◽  
pp. 3391-3436 ◽  
Author(s):  
C. M. Archuleta ◽  
P. J. DeMott ◽  
S. M. Kreidenweis
Keyword(s):  
Sulfuric Acid ◽  
Relative Humidity ◽  
Mineral Dust ◽  
Aerosol Particles ◽  
Diffusion Chamber ◽  
Ice Nucleation ◽  
Dust Particles ◽  
Nucleation Behavior ◽  
Ice Nuclei ◽  
Homogeneous Freezing

Abstract. 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.

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

2005 ◽  
Vol 5 (10) ◽  
pp. 2617-2634 ◽  
Author(s):  
C. M. Archuleta ◽  
P. J. DeMott ◽  
S. M. Kreidenweis
Keyword(s):  
Sulfuric Acid ◽  
Relative Humidity ◽  
Mineral Dust ◽  
Aerosol Particles ◽  
Diffusion Chamber ◽  
Ice Nucleation ◽  
Dust Particles ◽  
Nucleation Behavior ◽  
Ice Nuclei ◽  
Homogeneous Freezing

Abstract. 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.

scholarly journals Ice nucleation of ammonia gas exposed montmorillonite mineral dust particles

2007 ◽  
Vol 7 (14) ◽  
pp. 3923-3931 ◽  
Author(s):  
A. Salam ◽  
U. Lohmann ◽  
G. Lesins
Keyword(s):  
Room Temperature ◽  
Mineral Dust ◽  
Diffusion Chamber ◽  
Ice Nucleation ◽  
Dust Particles ◽  
Experimental Conditions ◽  
Activation Temperature ◽  
Ammonia Gas ◽  
Ice Nuclei ◽  
Gas Exposure

Abstract. The ice nucleation characteristics of montmorillonite mineral dust aerosols with and without exposure to ammonia gas were measured at different atmospheric temperatures and relative humidities with a continuous flow diffusion chamber. The montmorillonite particles were exposed to pure (100%) and diluted ammonia gas (25 ppm) at room temperature in a stainless steel chamber. There was no significant change in the mineral dust particle size distribution due to the ammonia gas exposure. 100% pure ammonia gas exposure enhanced the ice nucleating fraction of montmorillonite mineral dust particles 3 to 8 times at 90% relative humidity with respect to water (RHw) and 5 to 8 times at 100% RHw for 120 min exposure time compared to unexposed montmorillonite within our experimental conditions. The percentages of active ice nuclei were 2 to 8 times higher at 90% RHw and 2 to 7 times higher at 100% RHw in 25 ppm ammonia exposed montmorillonite compared to unexposed montmorillonite. All montmorillonite particles are more efficient as ice nuclei with increasing relative humidities and decreasing temperatures. The activation temperature of montmorillonite exposed to 100% pure ammonia was 15°C higher than for unexposed montmorillonite particles at 90% RHw. In the 25 ppm ammonia exposed montmorillonite experiments, the activation temperature was 10°C warmer than unexposed montmorillonite at 90% RHw. Degassing does not reverse the ice nucleating ability of ammonia exposed montmorillonite mineral dust particles suggesting that the ammonia is chemically bound to the montmorillonite particle. This is the first experimental evidence that ammonia gas exposed montmorillonite mineral dust particles can enhance its activation as ice nuclei and that the activation can occur at temperatures warmer than –10°C where natural atmospheric ice nuclei are very scarce.

scholarly journals Ice nucleation of ammonia gas exposed montmorillonite mineral dust particles

2007 ◽  
Vol 7 (1) ◽  
pp. 383-403
Author(s):  
A. Salam ◽  
U. Lohmann ◽  
G. Lesins
Keyword(s):  
Room Temperature ◽  
Mineral Dust ◽  
Diffusion Chamber ◽  
Ice Nucleation ◽  
Dust Particles ◽  
Experimental Conditions ◽  
Activation Temperature ◽  
Ammonia Gas ◽  
Ice Nuclei ◽  
Gas Exposure

Abstract. 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.

scholarly journals Heterogeneous ice nucleation on dust particles sourced from nine deserts worldwide – Part 2: Deposition nucleation and condensation freezing

2019 ◽  
Vol 19 (2) ◽  
pp. 1059-1076 ◽  
Author(s):  
Yvonne Boose ◽  
Philipp Baloh ◽  
Michael Plötze ◽  
Johannes Ofner ◽  
Hinrich Grothe ◽  
...  
Keyword(s):  
Active Sites ◽  
Mineral Dust ◽  
Atmospheric Transport ◽  
Chemical Imaging ◽  
Ice Nucleation ◽  
Dust Particles ◽  
Full Potential ◽  
Nucleation Behavior ◽  
Crystal Water ◽  
Desert Dust

Abstract. Mineral dust particles from deserts are amongst the most common ice nucleating particles in the atmosphere. The mineralogy of desert dust differs depending on the source region and can further fractionate during the dust emission processes. Mineralogy to a large extent explains the ice nucleation behavior of desert aerosol, but not entirely. Apart from pure mineral dust, desert aerosol particles often exhibit a coating or are mixed with small amounts of biological material. Aging on the ground or during atmospheric transport can deactivate nucleation sites, thus strong ice nucleating minerals may not exhibit their full potential. In the partner paper of this work, it was shown that mineralogy determines most but not all of the ice nucleation behavior in the immersion mode found for desert dust. In this study, the influence of semi-volatile organic compounds and the presence of crystal water on the ice nucleation behavior of desert aerosol is investigated. This work focuses on the deposition and condensation ice nucleation modes at temperatures between 238 and 242 K of 18 dust samples sourced from nine deserts worldwide. Chemical imaging of the particles' surface is used to determine the cause of the observed differences in ice nucleation. It is found that, while the ice nucleation ability of the majority of the dust samples is dominated by their quartz and feldspar content, in one carbonaceous sample it is mostly caused by organic matter, potentially cellulose and/or proteins. In contrast, the ice nucleation ability of an airborne Saharan sample is found to be diminished, likely by semi-volatile species covering ice nucleation active sites of the minerals. This study shows that in addition to mineralogy, other factors such as organics and crystal water content can alter the ice nucleation behavior of desert aerosol during atmospheric transport in various ways.

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

2012 ◽  
Vol 12 (18) ◽  
pp. 8589-8610 ◽  
Author(s):  
R. Wagner ◽  
O. Möhler ◽  
H. Saathoff ◽  
M. Schnaiter ◽  
J. Skrotzki ◽  
...  
Keyword(s):  
Glass Transition ◽  
Aerosol Particles ◽  
Ice Nucleation ◽  
Ice Formation ◽  
Transition Temperatures ◽  
Glass Transition Temperatures ◽  
Ice Cloud ◽  
Ice Nuclei ◽  
Freezing Cycle ◽  
Homogeneous Freezing

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.

scholarly journals Influence of particle size on the ice nucleating ability of mineral dusts

2009 ◽  
Vol 9 (18) ◽  
pp. 6705-6715 ◽  
Author(s):  
A. Welti ◽  
F. Lüönd ◽  
O. Stetzer ◽  
U. Lohmann
Keyword(s):  
Particle Size ◽  
Size Dependence ◽  
Water Saturation ◽  
Mineral Dust ◽  
Ice Nucleation ◽  
Dust Particles ◽  
Ice Nuclei ◽  
Mineral Dusts ◽  
Measured Activation ◽  
Formation Efficiency

Abstract. The recently developed Zurich Ice Nucleation Chamber (ZINC) was used to explore ice nucleation of size-selected mineral dust particles at temperatures between −20°C and −55°C. Four different mineral dust species have been tested: montmorillonite, kaolinite, illite and Arizona test dust (ATD). The selected particle diameters are 100 nm, 200 nm, 400 nm and 800 nm. Relative humidities with respect to ice (RHi) required to activate 1% of the dust particles as ice nuclei (IN) are reported as a function of temperature. An explicit size dependence of the ice formation efficiency has been observed for all dust types. 800 nm particles required the lowest RHi to activate. Deposition nucleation below water saturation was found only below −30°C or −35°C dependent on particle size. Minimum RHi for 1% activation were 105% for illite, kaolinite and montmorillonite at −40°C, respectively 110% for ATD at −45°C. In addition, a possible parameterisation for the measured activation spectra is proposed, which could be used in modeling studies.

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

2014 ◽  
Vol 14 (11) ◽  
pp. 5529-5546 ◽  
Author(s):  
H. Wex ◽  
P. J. DeMott ◽  
Y. Tobo ◽  
S. Hartmann ◽  
M. Rösch ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Succinic Acid ◽  
Freezing Point ◽  
Active Surface ◽  
Diffusion Chamber ◽  
Ice Nucleation ◽  
Rate Coefficients ◽  
Ice Nuclei ◽  
Ability To Act ◽  
Immersion Freezing

Abstract. 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 for the CMS kaolinite particles was comparable to jhet derived for Fluka kaolinite particles coated with sulfuric acid. This is suggestive for the Fluka kaolinite possessing a type of ice-nucleating surface feature which is not present on the CMS kaolinite, and which can be destroyed by reaction with sulfuric acid. This might be potassium feldspar.

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

2014 ◽  
Vol 119 (16) ◽  
pp. 9993-10011 ◽  
Author(s):  
Gourihar Kulkarni ◽  
Cassandra Sanders ◽  
Kai Zhang ◽  
Xiaohong Liu ◽  
Chun Zhao
Keyword(s):  
Sulfuric Acid ◽  
Mineral Dust ◽  
Ice Nucleation ◽  
Dust Particles ◽  
Cloud Properties

scholarly journals Laboratory-generated mixtures of mineral dust particles with biological substances: characterization of the particle mixing state and immersion freezing behavior

2016 ◽  
Vol 16 (9) ◽  
pp. 5531-5543 ◽  
Author(s):  
Stefanie Augustin-Bauditz ◽  
Heike Wex ◽  
Cyrielle Denjean ◽  
Susan Hartmann ◽  
Johannes Schneider ◽  
...  
Keyword(s):  
Biological Material ◽  
Mineral Dust ◽  
Research Unit ◽  
Ice Nucleation ◽  
Freezing Behavior ◽  
Dust Particles ◽  
Mixing State ◽  
Nucleation Behavior ◽  
Immersion Freezing

Abstract. Biological particles such as bacteria, fungal spores or pollen are known to be efficient ice nucleating particles. Their ability to nucleate ice is due to ice nucleation active macromolecules (INMs). It has been suggested that these INMs maintain their nucleating ability even when they are separated from their original carriers. This opens the possibility of an accumulation of such INMs in soils, resulting in an internal mixture of mineral dust and INMs. If particles from such soils which contain biological INMs are then dispersed into the atmosphere due to wind erosion or agricultural processes, they could induce ice nucleation at temperatures typical for biological substances, i.e., above −20 up to almost 0 °C, while they might be characterized as mineral dust particles due to a possibly low content of biological material. We conducted a study within the research unit INUIT (Ice Nucleation research UnIT), where we investigated the ice nucleation behavior of mineral dust particles internally mixed with INM. Specifically, we mixed a pure mineral dust sample (illite-NX) with ice active biological material (birch pollen washing water) and quantified the immersion freezing behavior of the resulting particles utilizing the Leipzig Aerosol Cloud Interaction Simulator (LACIS). A very important topic concerning the investigations presented here as well as for atmospheric application is the characterization of the mixing state of aerosol particles. In the present study we used different methods like single-particle aerosol mass spectrometry, Scanning Electron Microscopy (SEM), Energy Dispersive X-ray analysis (EDX), and a Volatility–Hygroscopicity Tandem Differential Mobility Analyser (VH-TDMA) to investigate the mixing state of our generated aerosol. Not all applied methods performed similarly well in detecting small amounts of biological material on the mineral dust particles. Measuring the hygroscopicity/volatility of the mixed particles with the VH-TDMA was the most sensitive method. We found that internally mixed particles, containing ice active biological material, follow the ice nucleation behavior observed for the pure biological particles. We verified this by modeling the freezing behavior of the mixed particles with the Soccerball model (SBM). It can be concluded that a single INM located on a mineral dust particle determines the freezing behavior of that particle with the result that freezing occurs at temperatures at which pure mineral dust particles are not yet ice active.

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