Can a "state of the art" chemistry transport model simulate Amazonian tropospheric chemistry?

被引:35
作者
Barkley, Michael P. [1 ]
Palmer, Paul I. [2 ]
Ganzeveld, Laurens [3 ]
Arneth, Almut [4 ,12 ]
Hagberg, Daniel [4 ]
Karl, Thomas [7 ]
Guenther, Alex [7 ]
Paulot, Fabien [9 ]
Wennberg, Paul O. [9 ,14 ]
Mao, Jingqiu [8 ]
Kurosu, Thomas P. [5 ]
Chance, Kelly [5 ]
Mueller, J. -F. [6 ]
De Smedt, Isabelle [6 ]
Van Roozendael, Michel [6 ]
Chen, Dan [13 ]
Wang, Yuxuan [10 ]
Yantosca, Robert M. [11 ]
机构
[1] Univ Leicester, Dept Phys & Astron, EOS Grp, Leicester LE1 7RH, Leics, England
[2] Univ Edinburgh, Sch Geosci, Edinburgh EH9 3JW, Midlothian, Scotland
[3] Univ Wageningen & Res Ctr, Dept Environm Sci, NL-6708 PB Wageningen, Netherlands
[4] Lund Univ, Geobiosphere Sci Ctr, Dept Phys Geog & Ecosyst Anal, SE-22362 Lund, Sweden
[5] Harvard Smithsonian Ctr Astrophys, Atom & Mol Phys Div, Cambridge, MA 02138 USA
[6] Belgian Inst Space Aeron, B-1180 Brussels, Belgium
[7] Natl Ctr Atmospher Res, Boulder, CO 80307 USA
[8] Princeton Univ, Geophys Fluid Dynam Lab, Princeton, NJ 08628 USA
[9] CALTECH, Div Engn & Appl Sci, Pasadena, CA 91125 USA
[10] Tsinghua Univ, Minist Educ Key Lab Earth Syst Modeling, Ctr Earth Syst Sci, Inst Global Change Studies, Beijing 100084, Peoples R China
[11] Harvard Univ, Div Engn & Appl Sci, Cambridge, MA 02138 USA
[12] Karlsruhe Inst Technol, Inst Meteorol & Climate Res, Karlsruhe, Germany
[13] Tsinghua Univ, Dept Environm Sci & Engn, Beijing 100084, Peoples R China
[14] CALTECH, Div Geol & Planetary Sci, Pasadena, CA 91125 USA
基金
瑞典研究理事会; 英国自然环境研究理事会;
关键词
TROPICAL RAIN-FOREST; VOLATILE ORGANIC-COMPOUNDS; MASTER CHEMICAL MECHANISM; FIRE EMISSIONS EXPERIMENT; PLANETARY BOUNDARY-LAYER; MCM V3 PART; ISOPRENE EMISSIONS; ATMOSPHERIC CHEMISTRY; NONMETHANE HYDROCARBONS; UNITED-STATES;
D O I
10.1029/2011JD015893
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
We present an evaluation of a nested high-resolution Goddard Earth Observing System (GEOS)-Chem chemistry transport model simulation of tropospheric chemistry over tropical South America. The model has been constrained with two isoprene emission inventories: (1) the canopy-scale Model of Emissions of Gases and Aerosols from Nature (MEGAN) and (2) a leaf-scale algorithm coupled to the Lund-Potsdam-Jena General Ecosystem Simulator (LPJ-GUESS) dynamic vegetation model, and the model has been run using two different chemical mechanisms that contain alternative treatments of isoprene photo-oxidation. Large differences of up to 100 Tg C yr (1) exist between the isoprene emissions predicted by each inventory, with MEGAN emissions generally higher. Based on our simulations we estimate that tropical South America (30-85 degrees W, 14 degrees N-25 degrees S) contributes about 15-35% of total global isoprene emissions. We have quantified the model sensitivity to changes in isoprene emissions, chemistry, boundary layer mixing, and soil NOx emissions using ground-based and airborne observations. We find GEOS-Chem has difficulty reproducing several observed chemical species; typically hydroxyl concentrations are underestimated, whilst mixing ratios of isoprene and its oxidation products are overestimated. The magnitude of model formaldehyde (HCHO) columns are most sensitive to the choice of chemical mechanism and isoprene emission inventory. We find GEOS-Chem exhibits a significant positive bias (10-100%) when compared with HCHO columns from the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) and Ozone Monitoring Instrument (OMI) for the study year 2006. Simulations that use the more detailed chemical mechanism and/or lowest isoprene emissions provide the best agreement to the satellite data, since they result in lower-HCHO columns.
引用
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页数:28
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