An observation-based, reduced-form model for oxidation in the remote marine troposphere

Author:

Baublitz Colleen B.12ORCID,Fiore Arlene M.12ORCID,Ludwig Sarah M.12ORCID,Nicely Julie M.34ORCID,Wolfe Glenn M.4ORCID,Murray Lee T.5ORCID,Commane Róisín12ORCID,Prather Michael J.6ORCID,Anderson Daniel C.47ORCID,Correa Gustavo2ORCID,Duncan Bryan N.4,Follette-Cook Melanie48,Westervelt Daniel M.29ORCID,Bourgeois Ilann1011ORCID,Brune William H.12ORCID,Bui T. Paul13,DiGangi Joshua P.14ORCID,Diskin Glenn S.14ORCID,Hall Samuel R.15ORCID,McKain Kathryn1016ORCID,Miller David O.12ORCID,Peischl Jeff1011ORCID,Thames Alexander B.12,Thompson Chelsea R.1011,Ullmann Kirk15ORCID,Wofsy Steven C.17

Affiliation:

1. Department of Earth and Environmental Sciences, Columbia University, New York, NY 10027

2. Division of Ocean and Climate Physics, Lamont-Doherty Earth Observatory of Columbia University, Palisades, NY 10964

3. Earth System Science Interdisciplinary Center, University of Maryland, College Park, MD 20740

4. Atmospheric Chemistry and Dynamics Laboratory, National Aeronautics and Space Administration Goddard Space Flight Center, Greenbelt, MD 20771

5. Department of Earth and Environmental Sciences, University of Rochester, Rochester, NY 14627

6. Department of Earth System Science, University of California, Irvine, CA 92697

7. Goddard Earth Sciences Technology and Research II, University of Maryland Baltimore County, Baltimore, MD 21250

8. Goddard Earth Sciences Technology and Research II, Morgan State University, Baltimore, MD 21251

9. National Aeronautics and Space Administration Goddard Institute for Space Studies, New York, NY 10025

10. Cooperative Institute for Research in Environmental Sciences, University of Colorado Boulder, Boulder, CO 80309

11. National Oceanic and Atmospheric Administration Chemical Sciences Laboratory, Boulder, CO 80305

12. Department of Meteorology and Atmospheric Science, Pennsylvania State University, University Park, PA 16802

13. Atmospheric Science Branch, National Aeronautics and Space Administration Ames Research Center, Moffett Field, CA 94035

14. National Aeronautics and Space Administration Langley Research Center, Hampton, VA 23666

15. Atmospheric Chemistry Observations & Modeling Laboratory, National Center for Atmospheric Research, Boulder, CO 80307

16. National Oceanic and Atmospheric Administration Global Monitoring Laboratory, Boulder, CO 80305

17. Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA 02138

Abstract

The hydroxyl radical (OH) fuels atmospheric chemical cycling as the main sink for methane and a driver of the formation and loss of many air pollutants, but direct OH observations are sparse. We develop and evaluate an observation-based proxy for short-term, spatial variations in OH (Proxy OH ) in the remote marine troposphere using comprehensive measurements from the NASA Atmospheric Tomography (ATom) airborne campaign. Proxy OH is a reduced form of the OH steady-state equation representing the dominant OH production and loss pathways in the remote marine troposphere, according to box model simulations of OH constrained with ATom observations. Proxy OH comprises only eight variables that are generally observed by routine ground- or satellite-based instruments. Proxy OH scales linearly with in situ [OH] spatial variations along the ATom flight tracks (median r 2 = 0.90, interquartile range = 0.80 to 0.94 across 2-km altitude by 20° latitudinal regions). We deconstruct spatial variations in Proxy OH as a first-order approximation of the sensitivity of OH variations to individual terms. Two terms modulate within-region Proxy OH variations—water vapor (H 2 O) and, to a lesser extent, nitric oxide (NO). This implies that a limited set of observations could offer an avenue for observation-based mapping of OH spatial variations over much of the remote marine troposphere. Both H 2 O and NO are expected to change with climate, while NO also varies strongly with human activities. We also illustrate the utility of Proxy OH as a process-based approach for evaluating intermodel differences in remote marine tropospheric OH.

Funder

NASA | Earth Sciences Division

DOC | NOAA | Climate Program Office

Publisher

Proceedings of the National Academy of Sciences

Subject

Multidisciplinary

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