Distribution and fate of selected oxygenated organic species in the troposphere and lower stratosphere over the Atlantic

H. Singh, Y. Chen, A. Tabazadeh, Y. Fukui, I. Bey, R. Yantosca, D. Jacob, F. Arnold, K. Wohlfrom, E. Atlas, F. Flocke, D. Blake, N. Blake, B. Heikes, J. Snow, R. Talbot, G. Gregory, G. Sachse, S. Vay, Y. Kondo

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223 Scopus citations

Abstract

A large number of oxygenated organic chemicals (peroxyacyl nitrates, alkyl nitrates, acetone, formaldehyde, methanol, methylhydroperoxide, acetic acid and formic acid) were measured during the 1997 Subsonic Assessment (SASS) Ozone and Nitrogen Oxide Experiment (SONEX) airborne field campaign over the Atlantic. In this paper, we present a first picture of the distribution of these oxygenated organic chemicals (Ox-organic) in the troposphere and the lower stratosphere, and assess their source and sink relationships. In both the troposphere and the lower stratosphere, the total atmospheric abundance of these oxygenated species (ΣOx-organic) nearly equals that of total nonmethane hydrocarbons (ΣNMHC), which have been traditionally measured. A sizable fraction of the reactive nitrogen (10-30%) is present in its oxygenated organic form. The organic reactive nitrogen fraction is dominated by peroxyacetyl nitrate (PAN), with alkyl nitrates and peroxypropionyl nitrate (PPN) accounting for <5% of total NOy. Comparison of observations with the predictions of the Harvard three-dimensional global model suggests that in many key areas (e.g., formaldehyde and peroxides) substantial differences between measurements and theory are present and must be resolved. In the case of CH3OH, there appears to be a large mismatch between atmospheric concentrations and estimated sources, indicating the presence of major unknown removal processes. Instrument intercomparisons as well as disagreements between observations and model predictions are used to identify needed improvements in key areas. The atmospheric chemistry and sources of this group of chemicals is poorly understood even though their fate is intricately linked with upper tropospheric NOx and HOx cycles.

Original languageEnglish (US)
Article number1999JD900779
Pages (from-to)3795-3805
Number of pages11
JournalJournal of Geophysical Research Atmospheres
Volume105
Issue numberD3
DOIs
StatePublished - Feb 16 2000

ASJC Scopus subject areas

  • Geophysics
  • Forestry
  • Oceanography
  • Aquatic Science
  • Ecology
  • Water Science and Technology
  • Soil Science
  • Geochemistry and Petrology
  • Earth-Surface Processes
  • Atmospheric Science
  • Earth and Planetary Sciences (miscellaneous)
  • Space and Planetary Science
  • Palaeontology

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    Singh, H., Chen, Y., Tabazadeh, A., Fukui, Y., Bey, I., Yantosca, R., Jacob, D., Arnold, F., Wohlfrom, K., Atlas, E., Flocke, F., Blake, D., Blake, N., Heikes, B., Snow, J., Talbot, R., Gregory, G., Sachse, G., Vay, S., & Kondo, Y. (2000). Distribution and fate of selected oxygenated organic species in the troposphere and lower stratosphere over the Atlantic. Journal of Geophysical Research Atmospheres, 105(D3), 3795-3805. [1999JD900779]. https://doi.org/10.1029/1999JD900779