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





Citation of Original Publication

Guo, H., et al. "Heterogeneity and chemical reactivity of the remote troposphere defined by aircraft measurements – corrected" Atmos. Chem. Phys. 23 (04 Jan 2023): 99–117, https://doi.org/10.5194/acp-23-99-2023, 2023.


This work was written as part of one of the author's official duties as an Employee of the United States Government and is therefore a work of the United States Government. In accordance with 17 U.S.C. 105, no copyright protection is available for such works under U.S. Law.
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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, NOx, 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 NOx 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.