globalchange  > 影响、适应和脆弱性
DOI: 10.1002/2017JD026781
New insights into the column CH2O/NO2 ratio as an indicator of near-surface ozone sensitivity
Author: Schroeder J.R.; Crawford J.H.; Fried A.; Walega J.; Weinheimer A.; Wisthaler A.; Müller M.; Mikoviny T.; Chen G.; Shook M.; Blake D.R.; Tonnesen G.S.
Source Publication: Journal of Geophysical Research: Atmospheres
Publishing Year: 2017
Volume: 122, Issue:16
pages begin: 8885
pages end: 8907
Language: 英语
Keyword: air quality ; DISCOVER-AQ ; formaldehyde ; NO2 ; ozone sensitivity ; remote sensing
English Abstract: Satellite-based measurements of the column CH2O/NO2 ratio have previously been used to estimate near-surface ozone (O3) sensitivity (i.e., NOx or VOC limited), and the forthcoming launch of air quality-focused geostationary satellites provides a catalyst for reevaluating the ability of satellite-measured CH2O/NO2 to be used in this manner. In this study, we use a 0-D photochemical box model to evaluate O3 sensitivity and find that the relative rate of radical termination from radical-radical interactions to radical-NOx interactions (referred to as LROx/LNOx) provides a good indicator of maximum O3 production along NOx ridgelines. Using airborne measurements from NASA's Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relative to Air Quality (DISCOVER-AQ) deployments in Colorado, Maryland, and Houston, we show that in situ measurements of CH2O/NO2 can be used to indicate O3 sensitivity, but there is an important “transition/ambiguous” range whereby CH2O/NO2 fails to categorize O3 sensitivity, and the range and span of this transition/ambiguous range varies regionally. Then, we apply these findings to aircraft-derived column density measurements from DISCOVER-AQ and find that inhomogeneities in vertical mixing in the lower troposphere further degrades the ability of column CH2O/NO2 to indicate near-surface O3 sensitivity (i.e., the transition/ambiguous range is much larger than indicated by in situ data alone), and we hypothesize that the global transition/ambiguous range is sufficiently large to make the column CH2O/NO2 ratio unuseful for classifying near-surface O3 sensitivity. Lastly, we present a case study from DISCOVER-AQ-Houston that suggests that O3 sensitivity on exceedance days may be substantially different than on nonexceedance days (which may be observable from space) and explore the diurnal evolution of O3 sensitivity, O3 production, and the column CH2O/NO2 ratio. The results of these studies suggest that although satellite measurements of CH2O/NO2 alone may not be sufficient for accurately classifying near-surface O3 sensitivity, new techniques offered by geostationary platforms may nonetheless provide methods for using space-based measurements to develop O3 mitigation strategies. ©2017. American Geophysical Union. All Rights Reserved.
Funding Project: "The authors would like to thank Glenn Diskin for providing measurements of CO and CH4 and all members of the DISCOVER-AQ science team for executing this field project. All data used in this work can be downloaded from PTR-MS measurements during DISCOVER-AQ were supported by the Austrian Ministry for Transport, Innovation, and Technology through the Austrian Space Applications Program (ASAP) of the Austrian Research Promotion Agency (FFG). Jason Schroeder and Tomas Mikoviny were partially supported by an appointment with the NASA Postdoctoral Program at NASA Langley Research Center, administered by Oak Ridge Associated Universities and Universities Space Research Association through contracts with NASA. Armin Wisthaler and Markus Müller received support from the Visiting Scientist Program of the National Institute of Aerospace (NIA). The authors would also like to thank Bryan Duncan, Brian Heikes, Luke Valin, and Heather Simon for useful comments that improved the quality of this paper.
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Document Type: 期刊论文
Appears in Collections:影响、适应和脆弱性

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Affiliation: NASA Langley Research Center, Hampton, VA, United States; NASA Postdoctoral Program, NASA Langley Research Center, Hampton, VA, United States; Institute of Arctic and Alpine Research, University of Colorado Boulder, Boulder, CO, United States; National Center for Atmospheric Research, Boulder, CO, United States; Institute of Ion Physics and Applied Physics, University of Innsbruck, Innsbruck, Austria; Department of Chemistry, University of Oslo, Oslo, Norway; Department of Chemistry, University of California, Irvine, CA, United States; US Environmental Protection Agency, Denver, CO, United States

Recommended Citation:
Schroeder J.R.,Crawford J.H.,Fried A.,et al. New insights into the column CH2O/NO2 ratio as an indicator of near-surface ozone sensitivity[J]. Journal of Geophysical Research: Atmospheres,2017-01-01,122(16)
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