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

被引:226
作者
Singh, H [1 ]
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
机构
[1] NASA, Ames Res Ctr, Moffett Field, CA 94035 USA
[2] Max Planck Inst Kernphys, D-69029 Heidelberg, Germany
[3] Natl Ctr Atmospher Res, Boulder, CO 80307 USA
[4] Harvard Univ, Cambridge, MA 02138 USA
[5] Univ Calif Irvine, Irvine, CA 92697 USA
[6] NASA, Langley Res Ctr, Hampton, VA 23681 USA
[7] Univ Rhode Isl, Ctr Atmospher Chem Studies, Narragansett, RI 02882 USA
[8] Nagoya Univ, Aichi 4428507, Japan
[9] Univ New Hampshire, Durham, NH 03824 USA
关键词
D O I
10.1029/1999JD900779
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
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 (Sigma Ox-organic) nearly equals that of total nonmethane hydrocarbons (Sigma NMHC), 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.
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页码:3795 / 3805
页数:11
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