Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements – corrected

Creators: Guo, Hao¹; Flynn, Clare M.²; Prather, Michael J.¹; Strode, Sarah A.³; Steenrod, Stephen D.³; Emmons, Louisa⁴; Lacey, Forrest^{4, 5}; Lamarque, Jean-Francois⁴; Fiore, Arlene M.⁶; Correa, Gus⁶; Murray, Lee T.⁷; Wolfe, Glenn M.^{3, 8}; St. Clair, Jason M.^{3, 8}; Kim, Michelle⁹; Crounse, John¹⁰; Diskin, Glenn¹⁰; DiGangi, Joshua¹⁰; Daube, Bruce C.¹¹; Commane, Roisin¹¹; McKain, Kathryn^{12, 13}; Peischl, Jeff¹³; Ryerson, Thomas B.^{12, 13}; Thompson, Chelsea¹²; Hanisco, Thomas F.³; Blake, Donald¹; Blake, Nicola J.¹; Apel, Eric C.⁴; Hornbrook, Rebecca S.⁴; Elkins, James W.¹³; Hintsa, Eric J.^{12, 13}; Moore, Fred L.^{12, 13}; Wofsy, Steven C.¹¹

1. University of California, Irvine
2. Stockholm University
3. Goddard Space Flight Center
4. National Center for Atmospheric Research
5. University of Colorado Boulder
6. Lamont-Doherty Earth Observatory
7. University of Rochester
8. University of Maryland, Baltimore County
9. California Institute of Technology
10. Langley Research Center
11. Harvard University
12. Cooperative Institute for Research in Environmental Sciences
13. Earth System Research Laboratory

Abstract

The NASA Atmospheric Tomography (ATom) mission built a photochemical climatology of air parcels based on in situ measurements with the NASA DC-8 aircraft along objectively planned profiling transects through the middle of the Pacific and Atlantic oceans. In this paper we present and analyze a data set of 10 s (2 km) merged and gap-filled observations of the key reactive species driving the chemical budgets of O₃ and CH₄ (O₃, CH₄, CO, H₂O, HCHO, H₂O₂, CH₃OOH, C₂H₆, higher alkanes, alkenes, aromatics, NO_x, HNO₃, HNO₄, peroxyacetyl nitrate, and other organic nitrates), consisting of 146 494 distinct air parcels from ATom deployments 1 through 4. Six models calculated the O₃ and CH₄ photochemical tendencies from this modeling data stream for ATom 1. We find that 80 %–90 % of the total reactivity lies in the top 50 % of the parcels and 25 %–35 % in the top 10 %, supporting previous model-only studies that tropospheric chemistry is driven by a fraction of all the air. Surprisingly, the probability densities of species and reactivities averaged on a model scale (100 km) differ only slightly from the 2 km ATom 10 s data, indicating that much of the heterogeneity in tropospheric chemistry can be captured with current global chemistry models. Comparing the ATom reactivities over the tropical oceans with climatological statistics from six global chemistry models, we find generally good agreement with the reactivity rates for O₃ and CH₄. Models distinctly underestimate O₃ production below 2 km relative to the mid-troposphere, and this can be traced to lower NO_x levels than observed. Attaching photochemical reactivities to measurements of chemical species allows for a richer, yet more constrained-to-what-matters, set of metrics for model evaluation.

This paper presents a corrected version of the paper published under the same authors and title (sans “corrected”) as https://doi.org/10.5194/acp-21-13729-2021.

Copyright and License

Errata

Editorial note: the authors discovered several major mistakes or decision errors in their analysis of the NASA Atmospheric Tomography (ATom) data presented in [the previous] paper. The changes were sufficiently extensive so that the executive editors decided to ask the authors for a completely new paper and to retract the 2021 paper. The errors that were corrected are described in the preface of the corrected paper [available in this record], which is published as follows:

Guo, H., Flynn, C. M., Prather, M. J., Strode, S. A., Steenrod, S. D., Emmons, L., Lacey, F., Lamarque, J.-F., Fiore, A. M., Correa, G., Murray, L. T., Wolfe, G. M., St. Clair, J. M., Kim, M., Crounse, J., Diskin, G., DiGangi, J., Daube, B. C., Commane, R., McKain, K., Peischl, J., Ryerson, T. B., Thompson, C., Hanisco, T. F., Blake, D., Blake, N. J., Apel, E. C., Hornbrook, R. S., Elkins, J. W., Hintsa, E. J., Moore, F. L., and Wofsy, S. C.: Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements – corrected, Atmos. Chem. Phys., 23, 99–117, https://doi.org/10.5194/acp-23-99-2023, 2023.

The main conclusions of the study are unchanged except those regarding production of ozone, but most of the numbers and many of the figures changed slightly. Readers should refer to the corrected paper.

Ken Carslaw (chief-executive editor)

Acknowledgement

The authors are indebted to the entire ATom Science Team including the managers, pilots and crew, who made this mission possible. Many other scientists not on the author list enabled the measurements and model results used here. The authors thank Xin Zhu for maintaining and updating the UCI chemistry transport model used here. We are grateful for the efforts of the two anonymous reviewers and the editor, Ken Carslaw, for their help in organizing this awkward paper.

Funding

The Atmospheric Tomography Mission (ATom) was supported by the National Aeronautics and Space Administration's Earth System Science Pathfinder Venture-Class Science Investigations: Earth Venture Suborbital-2. Primary funding of the preparation of this paper at UC Irvine was through NASA (grant nos. NNX15AG57A and 80NSSC21K1454).

Data Availability

The MDS-2b and RDS*-2b data for ATom 1, 2, 3, and 4 are presented here as core ATom deliverables and are posted temporarily on the NASA ESPO ATom website (https://espo.nasa.gov/atom/content/ATom, last access: 1 July 2022; Science team of the NASA Atmospheric Tomography Mission, 2021) and permanently on Dryad|UCI (https://doi.org/10.7280/D1B12H; Prather, 2022). This publication marks the public release of the reactivity calculations for ATom 2, 3, and 4, but we have not yet analyzed these data, and thus users should be aware and report any anomalous features to the lead authors via haog2@uci.edu and mprather@uci.edu. Details of the ATom mission and data sets are found on the NASA mission website (https://espo.nasa.gov/atom/content/ATom) and in the final archive at Oak Ridge National Laboratory (ORNL; https://daac.ornl.gov/ATOM/guides/ATom_merge.html, last access: 12 December 2022; https://doi.org/10.3334/ORNLDAAC/1581, Wofsy et al., 2018). The MATLAB scripts and data sets used in the analysis here are posted on Dryad (https://doi.org/10.7280/D1Q699; Guo, 2021).

Supplemental Material

The supplement related to this article is available online at: https://doi.org/10.5194/acp-23-99-2023-supplement.

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