Laboratory Studies of Deposition Mode Heterogeneous Ice Nucleation: Effect of Ice Nuclei Composition, Size and Surface Area PDF Download
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Languages : en
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PhD.
Author: Zaminhussein Abdulali Kanji
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ISBN: 9780494609897
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Languages : en
Pages : 490
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The indirect aerosol effect contributes to major uncertainties in determining the radiation budget of the earth. A large uncertainty is due to the formation of ice clouds onto natural or anthropogenic aerosols. Field studies have shown that mineral type particles are often associated with ice crystals in the mid-upper troposphere and given the long residence time in the atmosphere of dust particles (∼2 weeks in the absence of precipitation), their contribution to ice formation processes is not fully defined.It was concluded that there is no single value for the onset of ice formation in the atmosphere via deposition freezing. The associated contact angles show that there is a distribution of active sites on IN and that not all active sites have the same affinity for initiation of ice formation even within the same aerosol type. This work provides evidence that deposition mode nucleation can be an alternate pathway to homogeneous nucleation when mineral aerosols are present in the troposphere since the high T-low RH conditions required for deposition mode nucleation are more easily encountered in the atmosphere than the low T-high RH required for homogeneous nucleation.In order to probe ice formation onto natural mineral dust in a setting where it could be suspended as aerosol, a new continuous flow diffusion chamber (CFDC) was built. This allowed investigations of the effects of total aerosol surface area and particle size. The CFDC was also used in an international inter-comparison of ice nucleation instrumentation to compare efficiencies of soot, biological aerosol (bacteria) and samples of natural desert dusts from different regions of the world. The laboratory observations were parameterized using nucleation rates (Jhet) and contact angles (theta) as described by classical nucleation theory.For both this experimental technique and a static one developed during the candidate's Masters degree, mineral dust particulate proved to be the most efficient ice nuclei (IN) activating at RH with respect to ice (RH i) as low as 105% at T=233 K. The efficiency varied with particle size and aerosol surface area (SA). Large particles or higher SA activated at lower RHi than small particles or lower SA. The static chamber was sensitive to the first ice event out of a large SA and therefore gave true onset RHi, which was lower than the onset defined by the CFDC studies, which was not sensitive to a single ice event. In addition the static chamber used a broader size range of particulate matter, including super micron particles while the CFDC particles sizes were restricted to below 0.5 microm. Soot and organic coated dust particles were inefficient IN compared to pure dust. Soot aerosols showed some efficiency at T
Author: Zaminhussein Abdulali Kanji
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ISBN: 9780494163191
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Languages : en
Pages : 168
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Laboratory studies are described whereby the heterogeneous ice nucleating ability of various dust samples was studied for particles mounted on a hydrophobic cold stage. Ice formation is observed using digital photography. The relative humidity with respect to ice (RHIce) and temperature conditions of the flow system are validated by observing (NH4)2SO 4 deliquescence. Four types of solid mineral samples, including authentic Saharan dust, and commercial samples of alumina, silica and montmorillonite, were investigated in the deposition freezing mode. The size of the dust particles ranged from 0.5 to 5 microns, and the temperature range was from 263 to 218 K. With roughly 104 particles present on the cold stage, the onset for ice formation was observed at low relative humidities, between 102 and 108% RHIce, for all samples and temperatures. This indicates that deposition mode nucleation is an efficient mode of ice formation, particularly under the cold temperatures prevalent in the cirrus regime. By contrast, ice deposition onto n-hexane soot particles was not nearly so efficient. Nucleation rates prevalent in the experiment are calculated as a function of relative humidity from a suite of experiments conducted with Saharan dust where the dependence of the onset RHIce as a function of the total dust surface area was measured.
Author: Katherine Marak
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Languages : en
Pages : 0
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Aerosol particles can facilitate heterogenous ice formation in the troposphere and stratosphere by acting as ice nuclei, modulating cloud formation/dissipation, precipitation, and their microphysical properties. Heterogeneous ice nucleation is driven by ice embryo formation on the particle surface, which can be influenced by features of the surface such as crystallinity, surface structure, lattice structure, defects, and functional groups. Probing for deeper understanding of what surface features have the greatest impact on heterogeneous freezing is significant and can be done with synthetic and modified materials. To characterize the effect of crystallinity, pores, and surface functional groups towards ice nucleation, samples of comparable silica systems, specifically, quartz, ordered and non-ordered porous amorphous silica samples with a range of pore sizes (2-11 nm), and non-porous functionalized silica spheres were used as models for mineral dust aerosol particles (Chapter 2). The results suggest that crystallinity has a larger effect than porosity on ice nucleation activity, as all of the porous silica samples investigated had lower onset freezing temperatures and lower ice nucleation activities than quartz. Our findings also suggest that pores alone are not sufficient to serve as effective active sites, and need some additional chemical or physical property, like crystallinity, to nucleate ice in immersion mode freezing. The addition of a low density of organic functional groups to non-porous samples showed little enhancement compared to the inherent nucleation activity of silica with native surface hydroxyl groups. The density of functional groups investigated in this work suggests that a different arrangement of surface groups may be needed for enhanced immersion mode ice nucleation activity. In summary, crystallinity dictates the ice nucleation activity of silica samples rather than porosity or low-density surface functional groups. Silver and gold nanoparticles with thiol ligands of different functionalities (alkane, carboxylic acid and alcohol) were investigated for immersion ice nucleation activities (Chapter 3). The alcohol ligand nanoparticles of both silver and gold had significantly higher activities than the alkane thiol ligand, with a 4.5 oC and 10.7 oC difference in median freezing temperature respectively. Silver nanoparticles capped with thiol alcohol ligands were also tested for aggregation and oxidative stability. The silver nanoparticles are oxidatively stable for at least 2 years. We have also shown that aggregates of nanoparticles have likely caused the activity for all of the silver and gold samples, as ice nucleation activity strongly diminished when large aggregates (>200 nm) were filtered from solution. Investigating the ice nucleation activity of synthetic ZSM-5 samples with varying Si:Al helps to clarify ice nucleation activity of natural mineral dust samples, which are often aluminosilicate based materials (Chapter 4). Additionally, ammonium is a very common cation in the atmosphere, and its effects on ice nucleation activity are still being studied. Ice nucleation temperature increases with increasing Al content. Additionally, when ammonium is the cation that is strongly adsorbed to the surface and in pores, initial freezing temperatures are reduced by up to 6 oC. Seeing a drastic decrease in ice nucleation activity in the presence of ammonium, suggests that the cation can interact with the surface to block active sites. In addition to ice nucleation, dust samples can affect human health. The goal of Chapter 5 is to present risk assessments for trace element concentrations in PM10 dusts from simulated road material and township roads with/without oil and gas produced water brine (O&GPWB) treatment. PM10 trace metal quantification was conducted by Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and compared to values from EDS analysis on PM2.5. Among adults, PM10 inhalation lifetime cancer risks (CRinh range: 2.39E+01 to 7.73E+01) and hazard quotients for As, Ni and Pb exposure were elevated for O&GPWB, SFSR and RRA. Cumulative Pb dose for the O&GPWB-treated roads was 71 ng/kg by age 21, compared with 37 ng/kg for non-treated roads. Our results may be consistent with elevated blood lead (Pb) concentrations above state averages in this rural O&G producing region.
Author: Alessia Nicosia
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Languages : en
Pages : 0
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Heterogeneous ice nucleation is one element inside the overall complexity of the Earth's atmosphere, however, it has a profound impact on our representation of cloud properties: this process affects the optical thickness and lifetime of mixed-phase clouds and cirrus clouds, and it is responsible for a significant proportion of precipitations formed globally. Heterogeneous ice nucleation is related to the presence of specific aerosol particles, named ice nuclei particles (INP), with the unique ability of lowering the energy barrier required for the formation of ice crystals, especially where cloud's temperatures are >-38 °C. In the last decades, significant advancements have been made to the fundamental understanding of ice nucleation, however the lack of knowledge on the cloud ice phase still contributes to major uncertainties in climate model prediction of radiative forcing. This is partly due to limited observational data quantifying INP distributions and properties all over the world, especially in remote locations. In the first part of this thesis, field observations of ice nucleating particles have been performed at the Italian Climate Observatory “O. Vittori” on Mountain Cimone (2165 m above sea level), in the spring 2014 and autumn 2015, within the Bacchus and Air Sea Lab projects. For the first time we report the results of offline INP measurements, performed at a high altitude site within the Mediterranean basin. In the period 19-29 May 2014, a parallel campaign took place at the low-altitude station San Pietro Capofiume, a rural site in the Po Valley. The two campaigns were concerned, for a few days, by a Saharan Dust transport Event, which was recorded simultaneously at the high and the low-level station. We investigated the ambient number concentration of INP under condensation freezing activation mechanism (at -18 °C and above water saturation). In the second part of this thesis, we present the observations that were performed during the Arctic campaign Parcs-Maca, in the period of transition among the polar night and the polar day. We could characterise for the first time the ice nucleating and physical/chemical properties of the Arctic Primary Marine Aerosol, in a laboratory-controlled generation approach, that was combined to a mesocosm experiment. The aim of the mesocosm experiment was to adopt a multidisciplinary approach to study the effect of marine pollution on marine emissions. We found a moderate but significant decrease of the ice nuclei concentration in the polluted seawater (with respect to the control seawater) recorded in the freezing range between -8.5 and -19 °C and activated through immersion-freezing. Within the seaspray our measurements have indicated a relation among INP active at warm temperature (above -15 °C through immersion-freezing) and a calcium enrichment detected in PM1 filters (and followed by an apparent Chloride depletion). On the basis of our observations, and the results reported from other studies, a few suggestions on the nature of these marine ice nuclei have been suggested. In summary, the measurements made for this thesis provide new information on the concentrations of ice nuclei in ambient aerosol particles in remote regions (a high-altitude observatory in the central Mediterranean region) and in relation to a specific source (the Arctic sea spray).
Author: Thibault Hiron
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Category : Impact
Languages : en
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Author: Sarah Sihvonen
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Languages : en
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Aerosol particles impact the climate by serving as the seeds to form water droplets and ice to form clouds. However, these aerosol-cloud interactions are the least understood aspect of our understanding of the climate system. Mineral dust aerosol is the largest global source of ice nucleating particles. During atmospheric transport, mineral dust can be exposed to sulfuric acid, which has been shown to decrease the ice nucleation activity of these particles. Many explanations for this observation, such as chemical changes to the surface or product formation that blocks active sites, have been suggested. Our research focused on building a molecular picture of these surfaces to understand why sulfuric acid exposure reduces the ice nucleation activity of clay minerals such as kaolinite. We performed studies using X-ray diffraction and solid state NMR that investigate the changes that clay minerals undergo as a result of acid exposure. We are the first to show that the formation of a product on the surface of kaolinite was responsible for the decreased ice nucleation activity, not surface changes to the mineral itself. We continued to study aerosol-cloud interactions by using parcel models that explore the impact of ice growth surface kinetics on the competition between heterogeneous and homogeneous ice nucleation in clouds. We found that impaired growth of ice favors homogeneous freezing. The parcel models will be expanded to include our work on clay minerals to explore the impact of chemical aging of ice nuclei on overall cloud properties. We also studied the effect of acidic-processing on coal fly ash samples. Coal fly ash has been found to have a similar atmospheric impact as mineral dust, but is studied to a lesser extent. Like mineral dust, coal fly ash can serve as a source of bioavailable iron to phytoplankton in nutrient limited regions of the ocean. Fly ash has also been found to serve as an ice nucleating material. We performed aqueous sulfuric acid-treatment on fly ash samples representative of the types produced in the United States. We found that a soluble salt, gypsum (hydrated calcium sulfate), formed on three out of four samples. The most iron rich sample did not react with sulfuric acid. However, acidic-processing was shown to increase the amount of soluble iron which has implications for the biogeochemical cycle. These results also demonstrate that further work investigating these fly ash systems is warranted. In addition to our work on ice nucleation, we constructed a photoacoustic spectrometer to measure the absorbance of aerosol particles to study the optical properties of atmospheric aerosol. These measurements will aid in understanding the interactions of aerosol particles with light and the radiative balance of the planet.
Author: Bingbing Wang
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Category : Aerosols
Languages : en
Pages : 320
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Abstract : Ice particles in atmospheric clouds play an important role in determining cloud lifetime, precipitation and radiation. It is therefore important to understand the whole life cycle of ice particles in the atmosphere, e.g., where they come from (nucleation), how they evolve (growth), and where they go (precipitation). Ice nucleation is the crucial step for ice formation, and in this study, we will mainly focus on ice nucleation in the lab and its effect on mixed-phase stratiform clouds. In the first half of this study, we investigate the relevance of moving contact lines (i.e., the region where three or more phases meet) on the phenomenon of contact nucleation. High speed video is used to investigate heterogeneous ice nucleation in supercooled droplets resting on cold substrates under two different dynamic conditions: droplet electrowetting and droplet vibration. Results show that contact-line motion is not a sufficient condition to trigger ice nucleation, while locally curved contact lines that can result from contact-line motion are strongly related to ice nucleation. We propose that pressure perturbations due to locally curved contact lines can strongly enhance the ice nucleation rate, which gives another interpretation for the mechanism for contact nucleation. Corresponding theoretical results provide a quantitative connection between pressure perturbations and temperature, providing a useful tool for ice nucleation calculations in atmospheric models. In this second half of the study, we build a minimalist model for long lifetime mixed-phase stratiform clouds based on stochastic ice nucleation. Our result shows that there is a non-linear relationship between ice water contact and ice number concentration in the mixed-phase cloud, as long as the volume ice nucleation rate is constant. This statistical property may help identify the source of ice nuclei in mixed-phase clouds. In addition, results from Lagrangian ice particle tracking in time dependent fields show that long lifetime ice particles exist in mixed-phase stratiform clouds. We find that small ice particle can be trapped in eddy-like structures. Whether ice particles grow or sublimate depends on the thermodynamic field in the trapping region. This dynamic-thermodynamic coupling effect on the lifetime of ice particles might explain the fast phase-partition change observed in the mixed phase cloud.
Author: Michael James Wheeler
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Languages : en
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