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Towards a Satellite Formaldehyde – in situ Hybrid Estimate for Organic Aerosol AbundanceOrganic aerosol (OA) is one of the main components of the global particulate burden and intimately links natural and anthropogenic emissions with air quality and climate. It is challenging to accurately represent OA in global models. Direct quantification of global OA abundance is not possible with current remote sensing technology; however, it may be possible to exploit correlations of OA with remotely observable quantities to infer OA spatiotemporal distributions. In particular, formaldehyde (HCHO) and OA share common sources via both primary emissions and secondary production from oxidation of volatile organic compounds (VOCs). Here, we examine OA–HCHO correlations using data from summertime airborne campaigns investigating biogenic (NASA SEAC4RS and DC3), biomass burning (NASA SEAC4RS), and anthropogenic conditions (NOAA CalNex and NASA KORUS-AQ). In situ OA correlates well with HCHO (r=0.59–0.97), and the slope and intercept of this relationship depend on the chemical regime. For biogenic and anthropogenic regions, the OA–HCHO slopes are higher in low NOx conditions, because HCHO yields are lower and aerosol yields are likely higher. The OA–HCHO slope of wildfires is over 9 times higher than that for biogenic and anthropogenic sources. The OA–HCHO slope is higher for highly polluted anthropogenic sources (e.g., KORUS-AQ) than less polluted (e.g., CalNex) anthropogenic sources. Near-surface OAs over the continental US are estimated by combining the observed in situ relationships with HCHO column retrievals from NASA's Ozone Monitoring Instrument (OMI). HCHO vertical profiles used in OA estimates are from climatology a priori profiles in the OMI HCHO retrieval or output of specific period from a newer version of GEOS-Chem. Our OA estimates compare well with US EPA IMPROVE data obtained over summer months (e.g., slope =0.60–0.62, r=0.56 for August 2013), with correlation performance comparable to intensively validated GEOS-Chem (e.g., slope =0.57, r=0.56) with IMPROVE OA and superior to the satellite-derived total aerosol extinction (r=0.41) with IMPROVE OA. This indicates that OA estimates are not very sensitive to these HCHO vertical profiles and that a priori profiles from OMI HCHO retrieval have a similar performance to that of the newer model version in estimating OA. Improving the detection limit of satellite HCHO and expanding in situ airborne HCHO and OA coverage in future missions will improve the quality and spatiotemporal coverage of our OA estimates, potentially enabling constraints on global OA distribution.
Document ID
20190025719
Acquisition Source
Goddard Space Flight Center
Document Type
Reprint (Version printed in journal)
Authors
Liao, Jin
(NASA Goddard Space Flight Center Greenbelt, MD, United States)
Hanisco, Thomas F.
(NASA Goddard Space Flight Center Greenbelt, MD, United States)
Wolfe, Glenn M.
(NASA Goddard Space Flight Center Greenbelt, MD, United States)
Clair, Jason St.
(NASA Goddard Space Flight Center Greenbelt, MD, United States)
Jimenez, Jose L.
(Colorado Univ. Boulder, CO, United States)
Campuzano-Jost, Pedro
(Colorado Univ. Boulder, CO, United States)
Nault, Benjamin A.
(Colorado Univ. Boulder, CO, United States)
Fried, Alan
(Colorado Univ. Boulder, CO, United States)
Marais, Eloise A.
(University of Birmingham Birmingham, United Kingdom)
Abad, Gonzalo Gonzalez
(Harvard-Smithsonian Center for Astrophysics Cambridge, MA, United States)
Chance, Kelly
(Harvard-Smithsonian Center for Astrophysics Cambridge, MA, United States)
Jethva, Hiren T.
(NASA Goddard Space Flight Center Greenbelt, MD, United States)
Ryerson, Thomas B.
(National Oceanic and Atmospheric Administration (NOAA) Boulder, CO, United States)
Warneke, Carsten
(National Oceanic and Atmospheric Administration (NOAA) Boulder, CO, United States)
Wisthaler, Armin
(University of Oslo Oslo, Norway)
Date Acquired
June 5, 2019
Publication Date
March 4, 2019
Publication Information
Publication: Atmospheric Chemistry and Physics
Publisher: European Geosciences Union
Volume: 19
Issue: 5
ISSN: 1680-7316
e-ISSN: 1680-7324
Subject Category
Geosciences (General)
Report/Patent Number
GSFC-E-DAA-TN68210
Funding Number(s)
CONTRACT_GRANT: 80NSSC18K0630
CONTRACT_GRANT: NNH10ZDA001N
CONTRACT_GRANT: NNX15AT96G
CONTRACT_GRANT: NNG11HP16A
CONTRACT_GRANT: NNH15ZDA001N
Distribution Limits
Public
Copyright
Use by or on behalf of the US Gov. Permitted.
Keywords
anthropogenic emissions
spatiotemporal
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