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The Influence of Complex Meteorology and Surface Heterogeneity on Oxidation in the Troposphere.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	The Influence of Complex Meteorology and Surface Heterogeneity on Oxidation in the Troposphere./
作者:	Vermeuel, Michael P.
出版者:	Ann Arbor : ProQuest Dissertations & Theses, : 2021,
面頁冊數:	451 p.
附註:	Source: Dissertations Abstracts International, Volume: 82-10, Section: B.
Contained By:	Dissertations Abstracts International82-10B.
標題:	Atmospheric chemistry. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=28318994
ISBN:	9798597065342

The Influence of Complex Meteorology and Surface Heterogeneity on Oxidation in the Troposphere.
Vermeuel, Michael P.

The Influence of Complex Meteorology and Surface Heterogeneity on Oxidation in the Troposphere. - Ann Arbor : ProQuest Dissertations & Theses, 2021 - 451 p.

Source: Dissertations Abstracts International, Volume: 82-10, Section: B.

Thesis (Ph.D.)--The University of Wisconsin - Madison, 2021.

This item must not be sold to any third party vendors.

The planetary boundary layer (PBL) constitutes the lowest portion of the troposphere and is therefore subject to a direct surface-atmosphere influence due to its proximity to the Earth surface. The landscape of a particular region can have a unique influence on the PBL due to its contribution of chemical inputs through surface emissions, control on turbulent mixing that drives vertical transport and surface-atmosphere exchange, and through the presence of physical surfaces that may provide reversible or irreversible routes of loss. These coupled surface-atmosphere processes are important to understand since they control atmospheric composition and allow us to make accurate predictions of the effects of atmospheric chemistry on regional air quality and global climate. A compound that is of particular importance to understand in the PBL is the ambient oxidant ozone (O3), due to its influence on air quality and climate. O3 is the product of catalytic cycling of hydrogen oxides (HOx = OH + HO2) and nitrogen oxides (NOx = NO + NO2), with its production nonlinearly dependent on volatile organic compounds (VOCs) and NOx, both of which have biogenic and anthropogenic sources. Tropospheric O3 is a pollutant that is harmful to human health and plant productivity and can control atmospheric composition through the oxidative removal of reactive traces gases. It impacts climate by acting as a greenhouse gas and participating in particulate production, both of which contribute to the earth's radiation budget. Surface level O3 also delivers ecological damage which impacts the earth's carbon and water cycles due to irreversible damage to plants. As landscapes become increasingly more complex due to changes in land use, increased urbanization, or from ecological impacts of climate change it is important to have a more comprehensive knowledge of the many surface processes that can control the atmosphere in diverse environments as well as the resulting chemical mechanisms that ultimately regulate the composition of the atmosphere.This thesis presents work that performed direct and unique observations of O3 and other critical atmospheric species in complex landscapes and used those observations, along with remote sensing, ground monitor, and assimilated data products, as constraints in atmospheric chemical models to close the knowledge gap on the diverse chemical and physical processes that control ambient oxidation in the troposphere. Chapter 1 presents the sensitivity of enhanced O3 production to the concentrations of NOx and VOC on a high O3 day as observed during lake breeze circulation along the mixed urban/rural coastline of Lake Michigan. A box model constrained by anthropogenic and biogenic emissions, observed meteorology, and parameterized land-type dependent loss processes was evaluated using in-situ measurements of O3 precursors and oxidation products at a ground site that intercepted a plume originating from the Chicago-Gary area. Chapter 2 builds upon the analysis in Chapter 1, extending to more days with plumes that originate in different source regions and advect along diverse paths along the Lake Michigan area. Chapter 3 presents the first observations of simultaneous fluxes of O3 and formic acid (HCOOH), a biogenic VOC (BVOC) ozonolysis product, at a highly mixed forest in Northern WI in the summer of 2019. A model was constructed that used surface-type dependent parameterizations of processes contributing to forest-atmosphere exchange of O3 and it was determined that a large fraction of O3 downward flux in the mixed forest was due to the oxidation of BVOC within the forest canopy. Chapter 4 briefly describes observations of BVOC at the same site in the following summer. Chapter 5 presents the first ground level fluxes and concentrations of a newly-discovered marine dimethyl sulfide reservoir, hydroperoxymethyl thioformate (HPMTF) at an urban coastal site in La Jolla, CA. The subsequent box model-driven analysis shows that HPMTF is irreversibly removed from the PBL by particle surfaces and low-level clouds. Chapter 6 and 7 describe instrumental and theoretical characterizations of a novel, highly sensitive method for detecting VOC. As a whole, this thesis describes novel tools and methods for making and interpreting unique observations of chemical species involved in atmospheric oxidation, while providing knowledge on the processes that control atmospheric chemistry over diverse and complex landscapes.

ISBN: 9798597065342Subjects--Topical Terms:

544140
Atmospheric chemistry.
Subjects--Index Terms:

Planetary Boundary Layer

The Influence of Complex Meteorology and Surface Heterogeneity on Oxidation in the Troposphere.
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500 $a Source: Dissertations Abstracts International, Volume: 82-10, Section: B.
500 $a Advisor: Bertram, Timothy H.
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506 $a This item must not be sold to any third party vendors.
506 $a This item must not be sold to any third party vendors.
520 $a The planetary boundary layer (PBL) constitutes the lowest portion of the troposphere and is therefore subject to a direct surface-atmosphere influence due to its proximity to the Earth surface. The landscape of a particular region can have a unique influence on the PBL due to its contribution of chemical inputs through surface emissions, control on turbulent mixing that drives vertical transport and surface-atmosphere exchange, and through the presence of physical surfaces that may provide reversible or irreversible routes of loss. These coupled surface-atmosphere processes are important to understand since they control atmospheric composition and allow us to make accurate predictions of the effects of atmospheric chemistry on regional air quality and global climate. A compound that is of particular importance to understand in the PBL is the ambient oxidant ozone (O3), due to its influence on air quality and climate. O3 is the product of catalytic cycling of hydrogen oxides (HOx = OH + HO2) and nitrogen oxides (NOx = NO + NO2), with its production nonlinearly dependent on volatile organic compounds (VOCs) and NOx, both of which have biogenic and anthropogenic sources. Tropospheric O3 is a pollutant that is harmful to human health and plant productivity and can control atmospheric composition through the oxidative removal of reactive traces gases. It impacts climate by acting as a greenhouse gas and participating in particulate production, both of which contribute to the earth's radiation budget. Surface level O3 also delivers ecological damage which impacts the earth's carbon and water cycles due to irreversible damage to plants. As landscapes become increasingly more complex due to changes in land use, increased urbanization, or from ecological impacts of climate change it is important to have a more comprehensive knowledge of the many surface processes that can control the atmosphere in diverse environments as well as the resulting chemical mechanisms that ultimately regulate the composition of the atmosphere.This thesis presents work that performed direct and unique observations of O3 and other critical atmospheric species in complex landscapes and used those observations, along with remote sensing, ground monitor, and assimilated data products, as constraints in atmospheric chemical models to close the knowledge gap on the diverse chemical and physical processes that control ambient oxidation in the troposphere. Chapter 1 presents the sensitivity of enhanced O3 production to the concentrations of NOx and VOC on a high O3 day as observed during lake breeze circulation along the mixed urban/rural coastline of Lake Michigan. A box model constrained by anthropogenic and biogenic emissions, observed meteorology, and parameterized land-type dependent loss processes was evaluated using in-situ measurements of O3 precursors and oxidation products at a ground site that intercepted a plume originating from the Chicago-Gary area. Chapter 2 builds upon the analysis in Chapter 1, extending to more days with plumes that originate in different source regions and advect along diverse paths along the Lake Michigan area. Chapter 3 presents the first observations of simultaneous fluxes of O3 and formic acid (HCOOH), a biogenic VOC (BVOC) ozonolysis product, at a highly mixed forest in Northern WI in the summer of 2019. A model was constructed that used surface-type dependent parameterizations of processes contributing to forest-atmosphere exchange of O3 and it was determined that a large fraction of O3 downward flux in the mixed forest was due to the oxidation of BVOC within the forest canopy. Chapter 4 briefly describes observations of BVOC at the same site in the following summer. Chapter 5 presents the first ground level fluxes and concentrations of a newly-discovered marine dimethyl sulfide reservoir, hydroperoxymethyl thioformate (HPMTF) at an urban coastal site in La Jolla, CA. The subsequent box model-driven analysis shows that HPMTF is irreversibly removed from the PBL by particle surfaces and low-level clouds. Chapter 6 and 7 describe instrumental and theoretical characterizations of a novel, highly sensitive method for detecting VOC. As a whole, this thesis describes novel tools and methods for making and interpreting unique observations of chemical species involved in atmospheric oxidation, while providing knowledge on the processes that control atmospheric chemistry over diverse and complex landscapes.
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650 4 $a Atmospheric chemistry. $3 544140
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653 $a Complex meteorology
653 $a Troposphere
653 $a Surface-atmosphere processes
653 $a Lake Michigan
690 $a 0371
710 2 $a The University of Wisconsin - Madison. $b Chemistry. $3 2049906
773 0 $t Dissertations Abstracts International $g 82-10B.
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791 $a Ph.D.
792 $a 2021
793 $a English
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