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Toward Better Characterization of th...

Rothfuss, Nicholas Ernest.

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Toward Better Characterization of the Viscosity of Organic Aerosol.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Toward Better Characterization of the Viscosity of Organic Aerosol./
Author:	Rothfuss, Nicholas Ernest.
Published:	Ann Arbor : ProQuest Dissertations & Theses, : 2019,
Description:	486 p.
Notes:	Source: Dissertations Abstracts International, Volume: 80-09, Section: A.
Contained By:	Dissertations Abstracts International80-09A.
Subject:	Atmospheric chemistry. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=13850602

Toward Better Characterization of the Viscosity of Organic Aerosol.
Rothfuss, Nicholas Ernest.

Toward Better Characterization of the Viscosity of Organic Aerosol. - Ann Arbor : ProQuest Dissertations & Theses, 2019 - 486 p.

Source: Dissertations Abstracts International, Volume: 80-09, Section: A.

Thesis (Ph.D.)--North Carolina State University, 2019.

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

Atmospheric aerosol is central to various processes of meteorological or climatological concern and is a pollutant of significant concern for human health. Much of the particulate matter present in the atmosphere is composed of organic compounds. Organic aerosol (OA) can be liquid-like, semi-solid, or have mechanical properties similar to a glass, a difference of approximately 15 orders of magnitude in measured viscosities. Modelling studies suggest that highly viscous OA will be common in the middle and upper troposphere and in drier and colder regions of the lower troposphere. At near-glassy viscosities, bulk diffusion within the particle may be sufficiently inhibited as to render assumptions of rapid equilibration between the particle and its ambient environment during processes such as hygroscopic growth invalid, and thus serve as a potential source of error in cloud and climate models. Viscous outer shells may shield reactive species in the particle bulk from reaction with ambient oxidant species or inhibit evaporation of volatile species initially present within the bulk, dramatically increasing the atmospheric lifespan of such compounds and thus can provide a long-range transport mechanism for toxic or carcinogenic substances such as polycyclic aromatic hydrocarbons. Finally, highly viscous OA particles may serve as ice nuclei, altering pathways of cirrus cloud formation and concomitant radiative effects. Accordingly, there is scientific merit in quantifying OA viscosity and characterizing the processes that drive it and are modulated by it. Full understanding will require development of new instrumental methods and robust numerical models. This dissertation works towards closing this gap. This dissertation comprises six chapters on the topic of OA viscosity. A review of relevant literature on topics relating to OA viscosity is provided as an introductory chapter. Chapter 2 investigates how different functional groups modulate viscosity and/or glass transition temperature of atmospherically relevant compounds, based upon data collated from literature. Chapter 3 demonstrates a method for probing the viscosity of nanoscale aerosol by using measurements of apparent electrical mobility diameter to assess the morphology of dimerized particles subject to a brief period of conditioning. Chapter 4 presents a phase diagram model for binary aqueous aerosol, using sucrose as the representative system. This model combines the Gordon-Taylor equation for representing the humidity-dependence of glass transition temperature, a modified Vogel-Fulcher- Tammann equation for representing the temperature-dependence of viscosity, and a mass-based water activity parameterization, with model parameters derived using viscosity measurements made with the experimental method of Chapter 3. Chapter 5 characterizes and defines minimum experimental parameters for the experimental method of Chapter 3. Finally, Chapter 6 investigates the relationship between initial particle viscosity and condensational growth kinetics for a number of aqueous carbohydrate systems commonly used as OA proxies, using a combination of electrodynamic balance-based laboratory measurements and a gas diffusional growth model.Subjects--Topical Terms:

544140
Atmospheric chemistry.

Toward Better Characterization of the Viscosity of Organic Aerosol.
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300 $a 486 p.
500 $a Source: Dissertations Abstracts International, Volume: 80-09, Section: A.
500 $a Publisher info.: Dissertation/Thesis.
500 $a Advisor: Ziemann, Paul;Zhang, Yang;Grieshop, Andrew;Petters, Markus.
502 $a Thesis (Ph.D.)--North Carolina State University, 2019.
506 $a This item must not be sold to any third party vendors.
520 $a Atmospheric aerosol is central to various processes of meteorological or climatological concern and is a pollutant of significant concern for human health. Much of the particulate matter present in the atmosphere is composed of organic compounds. Organic aerosol (OA) can be liquid-like, semi-solid, or have mechanical properties similar to a glass, a difference of approximately 15 orders of magnitude in measured viscosities. Modelling studies suggest that highly viscous OA will be common in the middle and upper troposphere and in drier and colder regions of the lower troposphere. At near-glassy viscosities, bulk diffusion within the particle may be sufficiently inhibited as to render assumptions of rapid equilibration between the particle and its ambient environment during processes such as hygroscopic growth invalid, and thus serve as a potential source of error in cloud and climate models. Viscous outer shells may shield reactive species in the particle bulk from reaction with ambient oxidant species or inhibit evaporation of volatile species initially present within the bulk, dramatically increasing the atmospheric lifespan of such compounds and thus can provide a long-range transport mechanism for toxic or carcinogenic substances such as polycyclic aromatic hydrocarbons. Finally, highly viscous OA particles may serve as ice nuclei, altering pathways of cirrus cloud formation and concomitant radiative effects. Accordingly, there is scientific merit in quantifying OA viscosity and characterizing the processes that drive it and are modulated by it. Full understanding will require development of new instrumental methods and robust numerical models. This dissertation works towards closing this gap. This dissertation comprises six chapters on the topic of OA viscosity. A review of relevant literature on topics relating to OA viscosity is provided as an introductory chapter. Chapter 2 investigates how different functional groups modulate viscosity and/or glass transition temperature of atmospherically relevant compounds, based upon data collated from literature. Chapter 3 demonstrates a method for probing the viscosity of nanoscale aerosol by using measurements of apparent electrical mobility diameter to assess the morphology of dimerized particles subject to a brief period of conditioning. Chapter 4 presents a phase diagram model for binary aqueous aerosol, using sucrose as the representative system. This model combines the Gordon-Taylor equation for representing the humidity-dependence of glass transition temperature, a modified Vogel-Fulcher- Tammann equation for representing the temperature-dependence of viscosity, and a mass-based water activity parameterization, with model parameters derived using viscosity measurements made with the experimental method of Chapter 3. Chapter 5 characterizes and defines minimum experimental parameters for the experimental method of Chapter 3. Finally, Chapter 6 investigates the relationship between initial particle viscosity and condensational growth kinetics for a number of aqueous carbohydrate systems commonly used as OA proxies, using a combination of electrodynamic balance-based laboratory measurements and a gas diffusional growth model.
590 $a School code: 0155.
650 4 $a Atmospheric chemistry. $3 544140
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710 2 $a North Carolina State University. $3 1018772
773 0 $t Dissertations Abstracts International $g 80-09A.
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791 $a Ph.D.
792 $a 2019
793 $a English
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=13850602