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    Photodissociation and quantum yield determination of peroxyacetyl nitrate

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    Author
    Angerhofer, Mark Ernest
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    URI
    http://hdl.handle.net/11122/6241
    Abstract
    Peroxyacetyl nitrate (PAN) is an important atmospheric species due to its role in global transport of reactive nitrogen oxides, NOx (= ·NO₂ + ·NO). Peroxyacetyl nitrate is formed by reactions involving hydrocarbons and ·NO₂ in polluted regions and can be transported into the Arctic. To understand the role of PAN as a transporter of NOx to the Arctic, we need to quantify its decomposition pathways which include: thermal decomposition, photolysis, and reaction with the hydroxyl radical (·OH). In colder regions, such as the Arctic, the most rapid decomposition pathway is photolysis. Several photolytic pathways are possible for PAN. We photolyzed PAN in the laboratory using a frequency-doubled tunable dye laser. A highly sensitive technique called cavity ring-down spectroscopy (CRDS) probed the ·NO₃ produced in the photolysis reaction and we quantified the quantum yield for production of ·NO₃. The quantum yield is the fraction of photoexcited molecules that decompose to a certain chemical product. We determined that the quantum yield of ·NO₃ at 289 nm is 0.30 [plus/minus] 0.08. These results are discussed in context of previous work on PAN photolysis and in terms of a mechanistic model.
    Description
    Thesis (M.S.) University of Alaska Fairbanks, 2003
    Table of Contents
    Ch. 1. Atmospheric chemistry of peroxyacetyl nitrate -- ch. 2. Synthesis and photochemical properties of PAN and N₂O₅ -- ch. 3. Experimental and system design -- ch. 4. Calculations -- ch. 5. Results -- ch. 6. Discussion and conclusion -- References.
    Date
    2003-08
    Type
    Thesis
    Collections
    Chemistry and Biochemistry

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