Title
The gas-phase structure of the asymmetric, trans-dinitrogen tetroxide (N2O4), formed by dimerization of nitrogen dioxide (NO2), from rotational spectroscopy and ab initio quantum chemistry
Contributors
Creator: Marshall, Mark D. (Amherst College. Department of Chemistry)
Creator: Leung, Helen O. (Amherst College. Department of Chemistry)
Creator: Seifert, Nathan A. (University of Virginia. Department of Chemistry)
Creator: Zaleski, Daniel P. (University of Virginia. Department of Chemistry)
Creator: Fehnel, Robert (University of Virginia. Department of Chemistry)
Creator: Goswami, Mausumi (University of Virginia. Department of Chemistry)
Creator: Pate, Brooks Hart (University of Virginia. Department of Chemistry)
Creator: Lehmann, Kevin Keith (University of Virginia. Department of Chemistry and Physics)
Creator: Stanton, John (John F.) (University of Florida. Department of Chemistry and Quantum Theory Project)
Creator: Leung, Helen O. (Amherst College. Department of Chemistry)
Creator: Seifert, Nathan A. (University of Virginia. Department of Chemistry)
Creator: Zaleski, Daniel P. (University of Virginia. Department of Chemistry)
Creator: Fehnel, Robert (University of Virginia. Department of Chemistry)
Creator: Goswami, Mausumi (University of Virginia. Department of Chemistry)
Creator: Pate, Brooks Hart (University of Virginia. Department of Chemistry)
Creator: Lehmann, Kevin Keith (University of Virginia. Department of Chemistry and Physics)
Creator: Stanton, John (John F.) (University of Florida. Department of Chemistry and Quantum Theory Project)
Genre
Publication Information
Author's Final Version
Date Issued
2017-04-04
Note
Final published version appeared in Journal of Chemical Physics.
Abstract
We report the first experimental gas-phase observation of an asymmetric, trans N2O4 formed by the dimerization of NO2. In additional to the dominant 14N2 6O4 species, rotational transitions have been observed for all species with single 15N and 18O substitutions, as well as several multiply substituted isotopologues. These transitions were used to determine a complete substitution structure as well as an r0 structure from the fitted zero-point averaged rotational constants. The determined structure is found to be that of an ON—O-NO2 linkage with the shared oxygen atom closer to the NO2 than the NO (1.42 vs 1.61 Å). The structure is found to be nearly planar with a trans O-N-O-N linkage. From the spectra of the 14N15NO4 species, we were able to determine the nuclear quadrupole coupling constants for each specific nitrogen atom. The equilibrium structure determined by ab initio quantum chemistry calculations is in excellent agreement with the experimentally determined structure. No spectral evidence of the predicted asymmetric, cis N2O4 was found in the spectra.
Subjects
Identifier (DOI)
10.1063/1.4979182
Language
English
Files referenced in this Digital Object
- Download Leung_2017_thegas-phasestructure.pdf
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