Mechanistic Insights from the 15N-Site Preference of Nitrous Oxide utilizing High Resolution Near-Infrared cw Cavity Ringdown Spectroscopy and Density Functional Theory Calculations
Year: 2012
Type: dissertation
Abstract: The 15N-site preference, the ratio between the single 15N-substituted nitrous oxide isotopomers 14N15N16O and 15N14N16O, is discussed as an important proxy for formation and decomposition pathways of N2O in environmental sciences. In this thesis, different aspects concerning determination and significance of this parameter have been investigated. Based on a novel ultrasensitive, high resolution cw cavity ringdown spectrometer, an approach to determine this parameter spectroscopically has been followed. Furthermore, the detailed formation mechanism of N2O from HNO dimerization has been assessed theoretically based on DFT calculations. Finally, influences of the possible intermediate structures during N2O formation and parallels to site preferences found for diverse biochemical formation pathways are discussed.
Author: Carsten Fehling
Language: English
Subfield: Spectroscopy
Field: Chemistry
Domain: Physical Sciences
Open Access status: green
Funder: Deutsche Forschungsgemeinschaft
OpenAlex ID: W2593497979