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Insights into the molecular level composition, sources, and formation mechanisms of dissolved organic matter in aerolsols and precipitation

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TypeOfResource
Text
TitleInfo (ID = T-1)
Title
Insights into the molecular level composition, sources, and formation mechanisms of dissolved organic matter in aerolsols and precipitation
Identifier
ETD_1616
Identifier (type = hdl)
http://hdl.rutgers.edu/1782.2/rucore10001600001.ETD.000051125
Language
LanguageTerm (authority = ISO639-2)
eng
Genre (authority = marcgt)
theses
Subject (ID = SBJ-1)
Name (authority = LC-NAF)
Subject (ID = SBJ-1); (authority = RUETD)
Topic
Oceanography
Subject (ID = SBJ-1); (authority = ETD-LCSH)
Topic
Atmospheric aerosols
Subject (ID = SBJ-1); (authority = ETD-LCSH)
Topic
Atmospheric chemistry
Subject (ID = SBJ-1); (authority = ETD-LCSH)
Topic
Precipitation (Meteorology)
Subject (ID = SBJ-1); (authority = ETD-LCSH)
Abstract
Atmospheric aerosols scatter and absorb light influencing the global radiation budget and climate, and are associated with adverse effects on human health. Precipitation is an important removal mechanism for atmospheric dissolved organic matter (DOM), and a potentially important input for receiving ecosystems. However, the sources, formation, and composition of atmospheric DOM in aerosols and precipitation are not well understood. This dissertation investigates the composition and formation mechanisms of secondary organic aerosol (SOA) formed through cloud processing reactions, elucidates the composition and sources of DOM in rainwater, and provides links connecting the two.
Photochemical batch aqueous-phase reactions of organics with both biogenic and anthropogenic sources (i.e., methylglyoxal, pyruvic acid) and OH radical were performed to simulate cloud processing. The composition of products formed through cloud processing experiments and rainwater collected in New Jersey, USA was investigated using a combination of electrospray ionization mass spectrometry techniques, including ultra-high resolution Fourier transform ion cyclotron resonance mass spectrometry.
This dissertation has resulted in the first evidence that oligomers form through cloud processing reactions, the first detailed chemical mechanism of aqueous phase oligomerization, the first identification of oligomers, organosulfates, and nitrooxy organosulfates in precipitation, and the first molecular level chemical characterization of organic nitrogen in precipitation. The formation of oligomers in SOA helps to explain the presence of large multifunctional compounds and humic like substances (HULIS) that dominate particulate organic mass. Oligomers have low vapor pressures and remain in the particle phase after cloud evaporation, enhancing SOA. The chemical properties of the oligomers suggest that they are less hygroscopic than the monomeric reaction products (i.e., organic acids). Their elemental ratios are consistent with the hypothesis that oligomers are a large contributor to aged organic aerosol mass. The majority of the compounds identified in rainwater samples by advanced mass spectrometry appear to be products of atmospheric reactions, including known contributors to SOA formed from gas phase, aerosol phase, and in-cloud reactions in the atmosphere. The similarities between the complex organic matter in rainwater and SOA suggest that the large uncharacterized component of SOA is the main contributor to the large uncharacterized component of rainwater DOM.
PhysicalDescription
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electronic resource
Extent
xii, 163 p. : ill.
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application/pdf
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Note (type = degree)
Ph.D.
Note (type = bibliography)
Includes bibliographical references (p. 116-133)
Note (type = statement of responsibility)
by Katye Elisabeth Altieri
Name (ID = NAME-1); (type = personal)
NamePart (type = family)
Altieri
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Katye Elisabeth
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1982
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author
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Katye Elisabeth Altieri
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Seitzinger
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Sybil
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chair
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Advisory Committee
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Sybil P Seitzinger
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Turpin
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Barbara
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internal member
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Advisory Committee
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Barbara J Turpin
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Falkowski
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Paul
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Advisory Committee
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Paul G Falkowski
Name (ID = NAME-5); (type = personal)
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Reinfelder
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John
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internal member
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Advisory Committee
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John Reinfelder
Name (ID = NAME-6); (type = personal)
NamePart (type = family)
Jickells
NamePart (type = given)
Tim
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outside member
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Advisory Committee
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Tim Jickells
Name (ID = NAME-1); (type = corporate)
NamePart
Rutgers University
Role
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degree grantor
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NamePart
Graduate School - New Brunswick
Role
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school
OriginInfo
DateCreated (point = ); (qualifier = exact)
2009
DateOther (qualifier = exact); (type = degree)
2009-05
Place
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xx
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TitleInfo
Title
Rutgers University Electronic Theses and Dissertations
Identifier (type = RULIB)
ETD
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TitleInfo
Title
Graduate School - New Brunswick Electronic Theses and Dissertations
Identifier (type = local)
rucore19991600001
Location
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NjNbRU
Identifier (type = doi)
doi:10.7282/T3N016RQ
Genre (authority = ExL-Esploro)
ETD doctoral
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The author owns the copyright to this work.
Copyright
Status
Copyright protected
Availability
Status
Open
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Detail
Non-exclusive ETD license
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Author Agreement License
Detail
I hereby grant to the Rutgers University Libraries and to my school the non-exclusive right to archive, reproduce and distribute my thesis or dissertation, in whole or in part, and/or my abstract, in whole or in part, in and from an electronic format, subject to the release date subsequently stipulated in this submittal form and approved by my school. I represent and stipulate that the thesis or dissertation and its abstract are my original work, that they do not infringe or violate any rights of others, and that I make these grants as the sole owner of the rights to my thesis or dissertation and its abstract. I represent that I have obtained written permissions, when necessary, from the owner(s) of each third party copyrighted matter to be included in my thesis or dissertation and will supply copies of such upon request by my school. I acknowledge that RU ETD and my school will not distribute my thesis or dissertation or its abstract if, in their reasonable judgment, they believe all such rights have not been secured. I acknowledge that I retain ownership rights to the copyright of my work. I also retain the right to use all or part of this thesis or dissertation in future works, such as articles or books.
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