Temporal and latitudinal distributions of stratospheric N2O isotopomers

Sakae Toyoda, Naohiro Yoshida, Taichiro Urabe, Yusuke Nakayama, Takeshi Suzuki, Kazuhide Tsuji, Kazuhiko Shibuya, Shuji Aoki, Takakiyo Nakazawa, Shigeyuki Ishidoya, Kentaro Ishijima, Satoshi Sugawara, Toshinobu Machida, Gen Hashida, Shinji Morimoto, Hideyuki Honda

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Abstract

Temporal and latitudinal variations of vertical profiles of N2O isotopomers were observed in the stratosphere over Japan (39°N, 142°E), Sweden (68°N, 20°E), and Antarctica (69°N, 40°E) during the period between 1990 and 2001. Samples were collected with a balloon-borne cryogenic sampler and analyzed by mass spectrometry in the laboratory. Observed enrichment factors for heavier isotopomers (15N14N16O2, 14N15N16O, and 14N14N18O) relative to 14N14N16O were nearly constant in the lower stratosphere (less than ∼22 km) but increased at higher altitudes (∼22-35 km) while showing seasonal and latitudinal differences. Enrichment factors during the photolysis and photo-oxidation of N2O were also obtained in laboratory experiments and compared with those observed. We found that in the higher-altitude region (1) fractionation of the isotopomers is mainly determined by photolysis, but is also affected by physical processes, (2 subsidence of air masses in the winter polar vortex induces the intrusion of an upper stratospheric air mass depleted in N2O, and (3) decay of the vortex in the local spring leads to rapid horizontal advection of midlatitude air masses. At lower altitudes, isotopomer ratios are determined by photolysis, photo-oxidation, and the mixing of air masses within the stratosphere or between the stratosphere and the troposphere. Secular trend of isotopomer profiles was not detectable over Japan during 11 years. Assuming that the lower stratospheric air over midlatitudes is exchanged with the troposphere, isotopomer ratios of the N2O "back-flux" from the stratosphere were estimated. These values can be used in the isotopomeric mass balance model to constrain the global N2O budget.

Original languageEnglish
Pages (from-to)D08308 1-15
JournalJournal of Geophysical Research D: Atmospheres
Volume109
Issue number8
DOIs
Publication statusPublished - 2004 Apr 27

Keywords

  • Isotopic fractionation
  • Isotopomers
  • Nitrous oxide (NO)
  • Stable isotopes
  • Stratosphere
  • Temporal and latitudinal distributions

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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    Toyoda, S., Yoshida, N., Urabe, T., Nakayama, Y., Suzuki, T., Tsuji, K., Shibuya, K., Aoki, S., Nakazawa, T., Ishidoya, S., Ishijima, K., Sugawara, S., Machida, T., Hashida, G., Morimoto, S., & Honda, H. (2004). Temporal and latitudinal distributions of stratospheric N2O isotopomers. Journal of Geophysical Research D: Atmospheres, 109(8), D08308 1-15. https://doi.org/10.1029/2003JD004316