globalchange  > 影响、适应和脆弱性
DOI: 10.1002/jgrd.50817
Ozone and organic nitrates over the eastern United States: Sensitivity to isoprene chemistry
Author: Mao J.; Paulot F.; Jacob D.J.; Cohen R.C.; Crounse J.D.; Wennberg P.O.; Keller C.A.; Hudman R.C.; Barkley M.P.; Horowitz L.W.
Source Publication: Journal of Geophysical Research Atmospheres
ISSN: 21698996
Publishing Year: 2013
Volume: 118, Issue:19
pages begin: 11256
pages end: 11268
Language: 英语
Keyword: isoprene chemistry ; nighttime chemistry ; nitrogen export ; organic nitrates ; ozone ; photooxidation
Scopus Keyword: Atmospheric chemistry ; Boundary layers ; Computer simulation ; Isomerization ; Isoprene ; Nitrates ; Nitrogen oxides ; Oxidation ; Photooxidation ; Atmospheric research ; Chemical transport models ; International consortium ; Isomerization channels ; Nitrogen export ; Organic nitrates ; Oxidation mechanisms ; Transport and transformation ; Ozone ; atmospheric modeling ; atmospheric pollution ; boundary layer ; carbon monoxide ; emission ; isoprene ; nitrate ; nitrogen oxides ; oxidation ; ozone ; radical ; sensitivity analysis ; United States
English Abstract: We implement a new isoprene oxidation mechanism in a global 3-D chemical transport model (GEOS-Chem). Model results are evaluated with observations for ozone, isoprene oxidation products, and related species from the International Consortium for Atmospheric Research on Transport and Transformation aircraft campaign over the eastern United States in summer 2004. The model achieves an unbiased simulation of ozone in the boundary layer and the free troposphere, reflecting canceling effects from recent model updates for isoprene chemistry, bromine chemistry, and HO2 loss to aerosols. Simulation of the ozone-CO correlation is improved relative to previous versions of the model, and this is attributed to a lower and reversible yield of isoprene nitrates, increasing the ozone production efficiency per unit of nitrogen oxides (NO x ≡ NO + NO2). The model successfully reproduces the observed concentrations of organic nitrates (ΣANs) and their correlations with HCHO and ozone. ΣANs in the model is principally composed of secondary isoprene nitrates, including a major contribution from nighttime isoprene oxidation. The correlations of ΣANs with HCHO and ozone then provide sensitive tests of isoprene chemistry and argue in particular against a fast isomerization channel for isoprene peroxy radicals. ΣANs can provide an important reservoir for exporting NOx from the U.S. boundary layer. We find that the dependence of surface ozone on isoprene emission is positive throughout the U.S., even if NOx emissions are reduced by a factor of 4. Previous models showed negative dependences that we attribute to erroneous titration of OH by isoprene. Key Points The model achieves an unbiased simulation of ozone over eastern US The model reproduces ΣANs and their correlations with HCHO and ozone ΣANs can provide an important reservoir for exporting NOx ©2013. American Geophysical Union. All Rights Reserved.
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被引频次[WOS]:124   [查看WOS记录]     [查看WOS中相关记录]
Document Type: 期刊论文
Appears in Collections:影响、适应和脆弱性

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Affiliation: Program in Atmospheric and Oceanic Sciences, Princeton University, NOAA/GFDL, 201 Forrestal Road, Princeton, NJ 08540, United States; Geophysical Fluid Dynamics Laboratory, National Oceanic and Atmospheric Administration, Princeton NJ, United States; School of Engineering and Applied Sciences, Harvard University, Cambridge MA, United States; Department of Chemistry, University of California, Berkeley CA, United States; Division of Engineering and Applied Science, Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena CA, United States; Environmental Protection Agency Region IX, San Francisco CA, United States; EOS Group, Department of Physics and Astronomy, University of Leicester, Leicester, United Kingdom

Recommended Citation:
Mao J.,Paulot F.,Jacob D.J.,et al. Ozone and organic nitrates over the eastern United States: Sensitivity to isoprene chemistry[J]. Journal of Geophysical Research Atmospheres,2013-01-01,118(19)
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