ǂa ǂglobal budget and source attribution
E. V. Fischer (Author), D. J. Jacob (Author), R. M. Yantosca (Author), M. P. Sulprizio (Author), D. B. Millet (Author), Jiandong Mao (Author), F. Paulot (Author), H. B. Singh (Author), A. Roiger (Author), Katja Džepina (Author)

Abstract

Peroxyacetyl nitrate (PAN) formed in the atmospheric oxidation of non-methane volatile organic compounds (NMVOCs) is the principal tropospheric reservoir for nitrogen oxide radicals (NOx = NO + NO2). PAN enables the transport and release of NOx to the remote troposphere with major implications for the global distributions of ozone and OH, the main tropospheric oxidants. Simulation of PAN is a challenge for global models because of the dependence of PAN on vertical transport as well as complex and uncertain NMVOC sources and chemistry. Here we use an improved representation of NMVOCs in a global 3-D chemical transport model (GEOS-Chem) and show that it can simulate PAN observations from aircraft campaigns worldwide. The immediate carbonyl precursors for PAN formation include acetaldehyde (44 % of the global source), methylglyoxal (30 %), acetone (7 %), and a suite of other isoprene and terpene oxidation products (19 %). A diversity of NMVOC emissions is responsible for PAN formation globally including isoprene (37 %) and alkanes (14 %). Anthropogenic sources are dominant in the extratropical Northern Hemisphere outside the growing season. Open fires appear to play little role except at high northern latitudes in spring, although results are very sensitive to plume chemistry and plume rise. Lightning NOx is the dominant contributor to the observed PAN maximum in the free troposphere over the South Atlantic.

Keywords

peroxyacetyl nitrate;non-methane volatile organic compounds;global 3-D chemical transport model;GEOS-chem;

Data

Language: English
Year of publishing:
Typology: 1.01 - Original Scientific Article
Organization: UNG - University of Nova Gorica
UDC: 54
COBISS: 59043331 Link will open in a new window
ISSN: 1680-7316
Views: 1544
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Other data

URN: URN:SI:UNG
Pages: str. 2679-2698
Volume: ǂVol. ǂ14
Issue: ǂiss. ǂ5
Chronology: 2014
DOI: 10.5194/acp-14-2679-2014
ID: 12757736
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