Author: Daniel Veghte
Publisher:
ISBN:
Category :
Languages : en
Pages :
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Book Description
Major factors that affect climate change depend on gas and particulate phase components in the atmosphere. Gas phase species have been studied in great detail and are well understood, causing a warming effect on the atmosphere. The less understood major contributing factor in the atmosphere are aerosol particles, which range in size from nanometers up to microns. Aerosol particles can directly scatter and absorb light and also have secondary effects such as acting as a surface for gas phase reactions to occur or seed particles for cloud formation. Aerosol particles can cause health problems ranging from serious cardiovascular to respiratory effects. All Climate and health effects of aerosol particles are dependent on particle composition, morphology, concentration, and size. Since a large variety of particulate types exist in the atmosphere, we have focused on understanding the effect of mineral dust composition and morphology. Mineral dust is important because it is the second largest emission by mass. In order to study the optical properties of aerosol particles, we built a cavity ring-down spectrometer and developed methods to interpret the excinction cross section results for particles with a varied shape. We have studied the major components of mineral dust that include calcium carbonate, hematite, quartz, aluminosilicate clay minerals, and feldspars, along with a heterogeneous dust sample. We have found that non-absorbing species that have surface roughness and an aspect ratio close to one (such as calcite, quartz and feldspar) can be treated as spheres. Aerosol particles that are absorbing (hematite) that have an aspect ratio near one with a roughened surface need to be treated with more complex models; otherwise the extinction cross section will be underrepresented. For aerosol particles that are non-absorbing but have a high aspect ratio (aluminosilicate clay minerals), additional modeling parameters are also needed that will account for shape and orientation. We have used Arizona Test Dust to determine if the models we have developed can be used to model the optical properties of a heterogeneous mixture. We have shown that the extinction cross section of the Arizona Test Dust can be modeled as long as individual components are treated independently and significant error would be introduces if all species were treated as spheres.Organic aerosol particles are chemically complex species that originate from primary or secondary emissions. We have described mixed organic/ammonium sulfate particles in the submicron regime using TEM to understand phase separation. When the organic component has a high aqueous solubility, all particles exhibit a homogeneous morphology while at low aqueous solubility all particles exhibit a phase separated structure. Intermediate solubility organics show a size dependent morphology. For pimelic and succinic acid, small particles (under approximately 200 nm) have a homogeneous structure while the larger particles exhibit phase separated structures. We have studied samples collected in Ulaanbaatar, Mongolia to better understand the types of particles and the effect of aging on these particles in an urban environment. The majority of the particles are soot, small spheres, or mineral dust. When we compared the monthly particle composition, we saw that there was an increased aging of the particles during the winter months due to pollution and a lower boundary layer leading to reduced atmospheric mixing. By understanding the particle composition present in areas and modeling the optical properties of individual particle types, better models can be created to give insight into aerosol particles affects on the atmosphere.
Author: Joshua Haines
Publisher:
ISBN:
Category :
Languages : en
Pages :
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Book Description
The morphology of aerosol particles influences the reactions that occur during atmospheric aging, as well as altering their contributions to the direct and indirect effects. In order to study the morphology of aerosol particles coated with organic compounds, we have condensed palmitic acid onto ammonium sulfate, quartz, and kaolinite particles with a coating oven. Using transmission electron microscopy, we have determined that the coated particles consist of a core particle with palmitic acid non-uniformly surrounding this core. This particle morphology matches atmospherically relevant particles. However, to our knowledge, particles with this morphology have not been created through the use of a coating oven. The optical properties of the coated particles are characterized through cavity ring-down spectroscopy and compared to Mie scattering calculations. For thick coatings, Mie scattering theory is effective at predicting the extinction cross section of the observed particles. We discuss the atmospheric relevance of the observed particles and their impact on climate-aerosol interactions.
Author: Kristin Di Monte
Publisher:
ISBN:
Category :
Languages : en
Pages : 0
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Book Description
Light extinction by atmospheric aerosol particles and their interactions with water are heavily dependent on their chemical composition, morphology, and mixing state. Both properties are crucial for determining the impact aerosol particles have on our climate. Since light extinction directly impacts visibility as well as climate, measurements of the extinction at varying relative humidities (RH) are needed in order to improve climate models. In this work we have measured the relative humidity dependence of aerosol light extinction and water uptake at 643 nm for particles of varying ammonium sulfate/organic compositions. Internal as well as external mixtures of levoglucosan, sucrose, and adipic acid with ammonium sulfate are investigated using cavity ring-down spectroscopy (CRDS). Optical growth factor (fRH) and hygroscopicity parameters ([kappa]) are reported for each aerosol system.
Author: Richard K Chang
Publisher: World Scientific
ISBN: 9814571296
Category : Science
Languages : en
Pages : 360
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Book Description
This volume is a collection of review articles by scientists who have pioneered many of the recent advances in studies of the optical effects of small particles. The book begins with a review of the multitude of sharp dielectric resonances which exist in all optical spectra as a result of particle size and shape. Latest advances in absorption and fluorescence spectroscopy of a single particle and/or an ensemble of particles are also discussed, as well as advances in the energy transfer mechanisms for molecules embedded in the particle. The effects of laser-induced heating on a single particle are reviewed in terms of the hydrodynamics and thermodynamics of the liquid droplet and its ambient gas surrounding. The limits of applying bulk optical constants to small particles which lie between the bulk substance and the quantum-sized substance are also presented.
Author: Ryan Christopher Moffet
Publisher:
ISBN:
Category :
Languages : en
Pages : 340
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Book Description
Knowledge of aerosol physical, chemical, optical properties is essential for judging the effect that particulates have on human health, climate and visibility. The aerosol time-of-flight mass spectrometer (ATOFMS) is capable of measuring, in real-time, the size and chemical composition of atmospheric aerosols. This was exemplified by the recent deployments of the ATOFMS to Mexico City and Riverside. The ATOFMS provided rapid information about the major particle types present in the atmosphere. Industrial sources of particles, such as fine mode particles containing lead, zinc and chloride were detected in Mexico City. The rapid time response of the ATOFMS was also exploited to characterize a coarse particle concentrator used in human health effects studies. The ATOFMS showed the ability to detect changes in particle composition with a time resolution of 15 min during short 2 hour human exposure studies.
Author:
Publisher:
ISBN:
Category :
Languages : en
Pages : 348
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Book Description
Author: Muhammad Altaf
Publisher:
ISBN:
Category :
Languages : en
Pages :
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Book Description
The Earths atmosphere is composed of a wide variety of gas phase species and particulate matter that have a large impact on our climate. Though our understanding of the climate system has improved significantly over the past few decades, the impact of aerosol particles remains uncertain. Aerosol particles can affect climate through the absorption and scattering of radiation (aerosol direct effect) and by serving as cloud condensation nuclei (aerosol indirect effect). It is known that aerosol particles cause a net cooling effect on the planet, but the magnitude of cooling is unclear and remains under investigation. A large part of this uncertainty is due to an incomplete understanding of the complex physical and chemical properties of aerosol particles such as composition, morphology, and phase state.In this dissertation, we focus on investigating the role of particle size and composition in determining morphology. We have discovered that for some organic aerosol systems, particle morphology depends on size, where small particles are homogeneous and large particles are phase separated. To explore the origins of this size dependent behavior, we have worked with a model organic aerosol system, poly(ethylene glycol)-400 mixed with ammonium sulfate. We have used cryogenic-transmission electron microscopy to probe the effect of phase separation mechanism on particle morphology by varying the organic aerosol composition. Our results suggest that a size dependent morphology occurs due to an activated process, where the presence or absence of an activation barrier to phase separation controls the resulting morphology.We have also explored the kinetics and thermodynamics of the phase separation process that results in a size dependent morphology by varying the experimental drying rates. Drying rates that span over four orders of magnitude were investigated. We have observed that at the fastest drying rates, the size of the transition region where both phase separated and homogeneous morphologies exist is on the order of ~100 nm. At the slowest drying rates, the transition region shifts to smaller diameters and the width narrows to ~3 nm. Our results suggest that a size dependent morphology persists to the slowest drying rates. Thus, we conclude that an underlying thermodynamic effect results in this size dependent behavior, rather than solely a kinetic phenomenon.To determine the atmospheric implications of a size dependent morphology, we have used a cloud condensation nuclei counter to probe the effect of a homogeneous vs. a phase separated morphology on cloud condensation nuclei (CCN) activity. We have found that the activation diameters differ for particles which have the same composition, but varying morphology. Since aerosol optical properties are a sensitive measure of particle structure, we have studied the morphology-resolved optical properties of organic aerosol using cavity ring-down spectroscopy. Our spectroscopy data indicate that the optical properties of core-shell and partially engulfed particles are approximately equal, but different than the prediction for homogeneous particles. By accurately parametrizing aerosol particle morphology, optical properties, and CCN activity we will be able to better predict heterogeneous chemistry in the atmosphere, in addition to the aerosol direct and aerosol indirect effects which play a critical role in constraining climate forcing.
Author: Huaxin Xue
Publisher:
ISBN:
Category :
Languages : en
Pages :
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Book Description
Soot aerosols are well known to be atmospheric constituents, but the hydrophobic nature of fresh soot likely prohibits them from encouraging cloud development. Soot aged through contact with oxygenated organic compounds may become hydrophilic enough to promote water uptake. In this study, the tandem differential mobility analyzer (TDMA) and differential mobility analyzer-aerosol particle mass analyzer (DMA-APM) were employed to measure the changes in morphology and hygroscopicity of soot aerosol particles upon coating with succinic and glutaric acids. The effective densities, fractal dimensions and dynamic shape factors of fresh and coated soot aerosol particles have been determined. Significant size-dependent increases of soot particle mobility diameter, mass, and effective density ([rho]eff) were observed upon coating of aggregates with succinic acid. These properties were restored back to their initial states once the acid was removed by heating, suggesting no restructuring of the soot core had occurred. Coating of soot with glutaric acid, on the other hand, leads to a strong size shrinking with a diameter growth factor ~0.60, even after the acid has been removed by heating suggesting the strong restructuring of the soot agglomerate. The additional 90% RH cycle can evidently enhance the restructuring process. The extinction and scattering properties at 532 nm of soot particles internally mixed with dicarboxylic acids were investigated experimentally using a cavity ring-down spectrometer and an integrating nephelometer, respectively, and the absorption is derived as the difference between extinction and scattering. It was found that the organic coatings significantly affect the optical and microphysical properties of the soot aggregates. The size-dependent amplification factors of light scattering were as much as 3.8 and 1.7 with glutaric and succinic acids coatings, respectively. Additional measurements with soot particles that are first coated with glutaric acid and then heated to remove the coating show that both scattering and absorption are enhanced by irreversible restructuring of soot aggregates to more compact globules. These results reveal the microphysical state of soot aerosol with incomplete restructuring in the atmosphere, and advance the treatment of atmospheric aged soot aerosol in the Mie theory shell-and-core model.
Author: Eric P. Shettle
Publisher:
ISBN:
Category : Aerosols
Languages : en
Pages : 100
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Book Description
Aerosol models have been developed for the lower atmosphere. These models are representative of conditions found in rural, urban, and maritime air masses. The changes in the aerosol properties with variations in the relative humidity are discussed. To describe the aerosol optical properties in the extreme of 100 percent relative humidity, several fog models are presented. For each model the coefficients for extinction, scattering, and absorption, the angular scattering distribution, and other optical parameters have been computed for wavelengths between 0.2 and 40 microns. These aerosol models are presented together with a review of their experimental basis. The optical properties of these models are discussed and some comparisons of the model with experimental measurements are presented.
Author: Alexander A. Kokhanovsky
Publisher: Springer Science & Business Media
ISBN: 3540499091
Category : Science
Languages : en
Pages : 154
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Book Description
This new text offers experienced students a comprehensive review of available techniques for the remote sensing of aerosols. These small particles influence both atmospheric visibility and the thermodynamics of the atmosphere. They are also of great importance in any consideration of climate change problems. Aerosols may also be responsible for the loss of harvests, human health problems and ecological disasters. Thus, this detailed study of aerosol properties on a global scale could not be more timely.
