Modeling Aerosol - Water Interactions in Subsaturated and Supersaturated Environments

Modeling Aerosol - Water Interactions in Subsaturated and Supersaturated Environments PDF Author: Christos Fountoukis
Publisher:
ISBN:
Category : Aerosols
Languages : en
Pages :

Get Book Here

Book Description
The current dissertation is motivated by the need for an improved understanding of aerosol -- water interactions both in subsaturated and supersaturated atmospheric conditions with a strong emphasis on air pollution and climate change modeling. A cloud droplet formation parameterization was developed to i) predict droplet formation from a lognormal representation of aerosol size distribution and composition, and, ii) include a size-dependant mass transfer coefficient for the growth of water droplets which explicitly accounts for the impact of organics on droplet growth kinetics. The parameterization unravels most of the physics of droplet formation and is in remarkable agreement with detailed numerical parcel model simulations, even for low values of the accommodation coefficient. The parameterization offers a much needed rigorous and computationally inexpensive framework for directly linking complex chemical effects on aerosol activation in global climate models. The new aerosol activation parameterization was also tested against observations from highly polluted clouds (within the vicinity of power plant plumes). Remarkable closure was achieved (much less than the 20% measurement uncertainty). The error in predicted cloud droplet concentration was mostly sensitive to updraft velocity. Optimal closure is obtained if the water vapor uptake coefficient is equal to 0.06. These findings can serve as much needed constraints in modeling of aerosol-cloud interactions in the North America. Aerosol -- water interactions in ambient relative humidities less than 100% were studied using a thermodynamic equilibrium model for inorganic aerosol and a three dimensional air quality model. We developed a new thermodynamic equilibrium model, ISORROPIA-II, which predicts the partitioning of semi-volatiles and the phase state of K+/Ca2+/Mg2+/NH4+/Na+/SO42-/NO3-/Cl-/H2O aerosols. A comprehensive evaluation of its performance was conducted against the thermodynamic module SCAPE2 over a wide range of atmospherically relevant conditions. Based on its computational rigor and performance, ISORROPIA-II appears to be a highly attractive alternative for use in large scale air quality and atmospheric transport models. The new equilibrium model was also used to thermodynamically characterize aerosols measured at a highly polluted area. In the ammonia-rich environment of Mexico City, nitrate and chloride primarily partition in the aerosol phase with a 20-min equilibrium timescale; PM2.5 is insensitive to changes in ammonia but is to acidic semivolatile species. When RH is below 50%, predictions improve substantially if the aerosol follows a deliquescent behavior. The impact of including crustal species (Ca2+, K+, M2+) in equilibrium calculations within a three dimensional air quality model was also studied. A significant change in aerosol water ( -19.8%) and ammonium ( -27.5%) concentrations was predicted when crustals are explicitly included in the calculations even though they contributed, on average, only a few percent of the total PM2.5 mass, highlighting the need for comprehensive thermodynamic calculations in the presence of dust.

Modeling Aerosol - Water Interactions in Subsaturated and Supersaturated Environments

Modeling Aerosol - Water Interactions in Subsaturated and Supersaturated Environments PDF Author: Christos Fountoukis
Publisher:
ISBN:
Category : Aerosols
Languages : en
Pages :

Get Book Here

Book Description
The current dissertation is motivated by the need for an improved understanding of aerosol -- water interactions both in subsaturated and supersaturated atmospheric conditions with a strong emphasis on air pollution and climate change modeling. A cloud droplet formation parameterization was developed to i) predict droplet formation from a lognormal representation of aerosol size distribution and composition, and, ii) include a size-dependant mass transfer coefficient for the growth of water droplets which explicitly accounts for the impact of organics on droplet growth kinetics. The parameterization unravels most of the physics of droplet formation and is in remarkable agreement with detailed numerical parcel model simulations, even for low values of the accommodation coefficient. The parameterization offers a much needed rigorous and computationally inexpensive framework for directly linking complex chemical effects on aerosol activation in global climate models. The new aerosol activation parameterization was also tested against observations from highly polluted clouds (within the vicinity of power plant plumes). Remarkable closure was achieved (much less than the 20% measurement uncertainty). The error in predicted cloud droplet concentration was mostly sensitive to updraft velocity. Optimal closure is obtained if the water vapor uptake coefficient is equal to 0.06. These findings can serve as much needed constraints in modeling of aerosol-cloud interactions in the North America. Aerosol -- water interactions in ambient relative humidities less than 100% were studied using a thermodynamic equilibrium model for inorganic aerosol and a three dimensional air quality model. We developed a new thermodynamic equilibrium model, ISORROPIA-II, which predicts the partitioning of semi-volatiles and the phase state of K+/Ca2+/Mg2+/NH4+/Na+/SO42-/NO3-/Cl-/H2O aerosols. A comprehensive evaluation of its performance was conducted against the thermodynamic module SCAPE2 over a wide range of atmospherically relevant conditions. Based on its computational rigor and performance, ISORROPIA-II appears to be a highly attractive alternative for use in large scale air quality and atmospheric transport models. The new equilibrium model was also used to thermodynamically characterize aerosols measured at a highly polluted area. In the ammonia-rich environment of Mexico City, nitrate and chloride primarily partition in the aerosol phase with a 20-min equilibrium timescale; PM2.5 is insensitive to changes in ammonia but is to acidic semivolatile species. When RH is below 50%, predictions improve substantially if the aerosol follows a deliquescent behavior. The impact of including crustal species (Ca2+, K+, M2+) in equilibrium calculations within a three dimensional air quality model was also studied. A significant change in aerosol water ( -19.8%) and ammonium ( -27.5%) concentrations was predicted when crustals are explicitly included in the calculations even though they contributed, on average, only a few percent of the total PM2.5 mass, highlighting the need for comprehensive thermodynamic calculations in the presence of dust.

Aerosol-Cloud-Climate Interactions

Aerosol-Cloud-Climate Interactions PDF Author: Peter V. Hobbs
Publisher: Academic Press
ISBN: 0080959962
Category : Science
Languages : en
Pages : 259

Get Book Here

Book Description
Aerosol and clouds play important roles in determining the earth's climate, in ways that we are only beginning to comprehend. In conjunction with molecular scattering from gases, aerosol and clouds determine in part what fraction of solar radiation reaches the earth's surface, and what fraction of the longwave radiation from the earth escapes to space. This book provides an overview of the latest research on atmospheric aerosol and clouds and their effects on global climate. Subjects reviewed include the direct and indirect effects of aerosol on climate, the radiative properties of clouds and their effects on the Earth's radiation balance, the incorporation of cloud effects in numerical weather prediction models, and stratospheric aerosol and clouds.

Modeling Atmospheric Chemistry

Modeling Atmospheric Chemistry PDF Author: Rolf Sander
Publisher:
ISBN:
Category : Aerosols
Languages : en
Pages : 31

Get Book Here

Book Description
For detailed modeling of atmospheric chemistry it is necessary to consider aqueous-phase reactions in cloud droplets and deliquesced aerosol particles. Often, the gas-phase concentration is in equilibrium with the aqueous phase. Then Henrys law can be used to describe the distribution between the phases provided that the Henry's law coefficient is known. In some cases, thermodynamic equilibrium will not be reached and it is necessary to use kinetic expressions of the rates involved. These rates depend on diffusion constants, accommodation coefficients, Henry's law coefficients, particle size distributions, and several other parameters. This review describes how these processes can be treated in computer modeling and how the necessary data can be obtained. Even though it is written primarily for use in modeling atmospheric chemistry, some parts will also be useful for waste water and pesticide control and in other areas where the distribution of chemicals between the aqueous and the gas phase is important.

Dissertation Abstracts International

Dissertation Abstracts International PDF Author:
Publisher:
ISBN:
Category : Dissertations, Academic
Languages : en
Pages : 980

Get Book Here

Book Description


Aerosol-Cloud Interactions from Urban, Regional, to Global Scales

Aerosol-Cloud Interactions from Urban, Regional, to Global Scales PDF Author: Yuan Wang
Publisher:
ISBN: 9783662471760
Category :
Languages : en
Pages :

Get Book Here

Book Description
The studies in this dissertation aim at advancing our scientific understandings about physical processes involved in the aerosol-cloud-precipitation interaction and quantitatively assessing the impacts of aerosols on the cloud systems with diverse scales over the globe on the basis of the observational data analysis and various modeling studies. As recognized in the Fifth Assessment Report by the Inter-government Panel on Climate Change, the magnitude of radiative forcing by atmospheric aerosols is highly uncertain, representing the largest uncertainty in projections of future climate by anthropogenic activities. By using a newly implemented cloud microphysical scheme in the cloud-resolving model, the thesis assesses aerosol-cloud interaction for distinct weather systems, ranging from individual cumulus to mesoscale convective systems. This thesis also introduces a novel hierarchical modeling approach that solves a long outstanding mismatch between simulations by regional weather models and global climate models in the climate modeling community. More importantly, the thesis provides key scientific solutions to several challenging questions in climate science, including the global impacts of the Asian pollution. As scientists wrestle with the complexities of climate change in response to varied anthropogenic forcings, perhaps no problem is more challenging than the understanding of the impacts of atmospheric aerosols from air pollution on clouds and the global circulation.

Microphysics of Clouds and Precipitation

Microphysics of Clouds and Precipitation PDF Author: H.R. Pruppacher
Publisher: Springer Science & Business Media
ISBN: 0306481006
Category : Science
Languages : en
Pages : 975

Get Book Here

Book Description
Cloud physics has achieved such a voluminous literature over the past few decades that a significant quantitative study of the entire field would prove unwieldy. This book concentrates on one major aspect: cloud microphysics, which involves the processes that lead to the formation of individual cloud and precipitation particles. Common practice has shown that one may distinguish among the following addi tional major aspects: cloud dynamics, which is concerned with the physics respon sible for the macroscopic features of clouds; cloud electricity, which deals with the electrical structure of clouds and the electrification processes of cloud and precipi tation particles; and cloud optics and radar meteorology, which describe the effects of electromagnetic waves interacting with clouds and precipitation. Another field intimately related to cloud physics is atmospheric chemistry, which involves the chemical composition ofthe atmosphere and the life cycle and characteristics of its gaseous and particulate constituents. In view of the natural interdependence of the various aspects of cloud physics, the subject of microphysics cannot be discussed very meaningfully out of context. Therefore, we have found it necessary to touch briefly upon a few simple and basic concepts of cloud dynamics and thermodynamics, and to provide an account of the major characteristics of atmospheric aerosol particles. We have also included a separate chapter on some of the effects of electric fields and charges on the precipitation-forming processes.

Characterizing Water-soluble Organic Aerosol and Their Effects on Cloud Droplet Formation: Interactions of Carbonaceous Matter with Water Vapor

Characterizing Water-soluble Organic Aerosol and Their Effects on Cloud Droplet Formation: Interactions of Carbonaceous Matter with Water Vapor PDF Author: Akua Asabea Asa-Awuku
Publisher:
ISBN:
Category : Aerosols
Languages : en
Pages :

Get Book Here

Book Description
Aerosols have significant impacts on earth's climate and hydrological cycle. They can directly reflect the amount of incoming solar radiation into space; by acting as cloud condensation nuclei (CCN), they can indirectly impact climate by affecting cloud albedo. Our current assessment of the interactions of aerosols and clouds is uncertain and parameters used to estimate cloud droplet formation in global climate models are not well constrained.Organic aerosols attribute much of the uncertainty in these estimates and are known to affect the ability of aerosol to form cloud droplets (CCN Activity) by i) providing solute, thus reducing the equilibrium water vapor pressure of the droplet and ii) acting as surfactants capable of depressing surface tension, and potentially, growth kinetics. My thesis dissertation investigates various organic aerosol species (e.g., marine, urban, biomass burning, Humic-like Substances). An emphasis is placed on the water soluble components and secondary organic aerosols (SOA). In addition the sampled organic aerosols are acquired via different media; directly from in-situ ambient studies (TEXAQS 2006) environmental chamber experiments, regenerated from filters, and cloud water samples. Novel experimental methods and analyses to determine surface tension, molar volumes, and droplet growth rates are presented from nominal volumes of sample. These key parameters for cloud droplet formation incorporated into climate models will constrain aerosol-cloud interactions and provide a more accurate assessment for climate prediction.

Introduction to Aerosol Modelling

Introduction to Aerosol Modelling PDF Author: David L. Topping
Publisher: John Wiley & Sons
ISBN: 1119625653
Category : Science
Languages : en
Pages : 372

Get Book Here

Book Description
INTRODUCTION TO AEROSOL MODELLING Introduction to Aerosol Modelling: From Theory to Code An aerosol particle is defined as a solid or liquid particle suspended in a carrier gas. Whilst we often treat scientific challenges in a siloed way, aerosol particles are of interest across many disciplines. For example, atmospheric aerosol particles are key determinants of air quality and climate change. Knowledge of aerosol physics and generation mechanisms is key to efficient fuel delivery and drug delivery to the lungs. Likewise, various manufacturing processes require optimal generation, delivery and removal of aerosol particles in a range of conditions. There is a natural tendency for the aerosol scientist to therefore work at the interface of the traditional academic subjects of physics, chemistry, biology, mathematics and computing. The impacts that aerosol particles have are linked to their evolving chemical and physical characteristics. Likewise, the chemical and physical characteristic of aerosol particles reflect their sources and subsequent processes they have been subject to. Computational models are not only essential for constructing evidence-based understanding of important aerosol processes, but also to predict change and impact. Whilst existing textbooks provide an overview of theoretical frameworks on which aerosol models are based, there is a significant gap in reference material that provide training in translating theory into code. The purpose of this book is to provide readers with exactly that. In following the content provided in this book, you will be able to reproduce models of key processes that can either be used in isolation or brought together to construct a demonstrator 0D box-model of a coupled gaseous-particulate system. You may be reading this book as an undergraduate, postgraduate, seasoned researcher in the private/public sector or as someone who wishes to better understand the pathways to aerosol model development. Wherever you position yourself, it is hoped that the tools you will learn through this book will provide you with the basis to develop your own platforms and to ensure the next generation of aerosol modellers are equipped with foundational skills to address future challenges in aerosol science.

The Interaction of Water and Aerosols in the Marine Boundary Layer: A Study of Selected Processes Impacting Radiative Transfer and Cloudiness

The Interaction of Water and Aerosols in the Marine Boundary Layer: A Study of Selected Processes Impacting Radiative Transfer and Cloudiness PDF Author:
Publisher:
ISBN:
Category :
Languages : en
Pages : 8

Get Book Here

Book Description
The overarching, log term goal of the study is to explore the profound effect of aerosol-water interaction both on radiation propagation in, and the thermodynamic structure of, the marine boundary layer. Specific goals are: 1) compile a climatology of aerosol hygroscopicity for use in the NAAPS and COAMPS models, and, further, to develop a model parameterization of hygroscopicity based on aerosol size and composition for such models, 2) explore the relative impacts of cross-inversion mixing and sub-cloud aerosol on cloud thickness and cloud base height, 3) quantify and parameterize the impact of precipitation scavenging on below cloud radiative transfer and cloud liquid water path. The sampling platform utilized is the CIRPAS Twin Otter research aircraft and the venue is the littoral environment off the California coast, representative of areas with high shipping densities.

Experimental and Modeling Studies of Interactions of Marine Aerosols and Clouds

Experimental and Modeling Studies of Interactions of Marine Aerosols and Clouds PDF Author:
Publisher:
ISBN:
Category :
Languages : en
Pages : 8

Get Book Here

Book Description
The primary goals of this research were to address the following key questions regarding marine aerosol/ cloud interactions: (1) What factors control the abundance and vertical distribution of aerosol in the marine boundary layer? (2) How do these factors affect the formation and lifetime of marine clouds? These questions have been addressed through a combination of modeling and experimental approaches, as described below. The goal of the modeling component was to produce a model description of aerosol evolution and aerosol / cloud interaction that can be applied to a variety of marine boundary layer scenarios. The specific objective of this component was to develop a model for prediction of the effects of aerosol characteristics on cloud formation and evolution, and, in turn, the effects of cloud processes on the marine aerosol. The models built in this project can be used to study the role of aerosol in cloud modification, including ship tracks and indirect climate effects. The goals of the experimental component were to develop new measurement techniques aimed at elucidating some important aerosol / cloud interactions, and to adapt and use these techniques in field work involving characterization of marine aerosol. A particular objective was the development of techniques for determination of size dependent particle properties with high time resolution.