Synthesizing evidence for the external cycling of NOx in high- to low-NOx atmospheres

Chunxiang Ye (), Xianliang Zhou, Yingjie Zhang, Youfeng Wang, Jianshu Wang, Chong Zhang, Robert Woodward-Massey, Christopher Cantrell, Roy L. Mauldin, Teresa Campos, Rebecca S. Hornbrook, John Ortega, Eric C. Apel, Julie Haggerty, Samuel Hall, Kirk Ullmann, Andrew Weinheimer, Jochen Stutz, Thomas Karl, James N. Smith, Alex Guenther and Shaojie Song
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Chunxiang Ye: College of Environmental Sciences and Engineering, Peking University
Xianliang Zhou: Wadsworth Center, New York State Department of Health
Yingjie Zhang: College of Environmental Sciences and Engineering, Peking University
Youfeng Wang: College of Environmental Sciences and Engineering, Peking University
Jianshu Wang: College of Environmental Sciences and Engineering, Peking University
Chong Zhang: College of Environmental Sciences and Engineering, Peking University
Robert Woodward-Massey: College of Environmental Sciences and Engineering, Peking University
Christopher Cantrell: Université Paris-est Créteil, LISA (Laboratoire Interuniversitaire des Systèmes Atmosphériques)
Roy L. Mauldin: Carnegie Mellon University
Teresa Campos: National Center for Atmospheric Research
Rebecca S. Hornbrook: National Center for Atmospheric Research
John Ortega: National Center for Atmospheric Research
Eric C. Apel: National Center for Atmospheric Research
Julie Haggerty: National Center for Atmospheric Research
Samuel Hall: National Center for Atmospheric Research
Kirk Ullmann: National Center for Atmospheric Research
Andrew Weinheimer: National Center for Atmospheric Research
Jochen Stutz: University of California
Thomas Karl: University of Innsbruck
James N. Smith: University of California
Alex Guenther: University of California
Shaojie Song: College of Environmental Science and Engineering, Nankai University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract External cycling regenerating nitrogen oxides (NOx ≡ NO + NO2) from their oxidative reservoir, NOz, is proposed to reshape the temporal–spatial distribution of NOx and consequently hydroxyl radical (OH), the most important oxidant in the atmosphere. Here we verify the in situ external cycling of NOx in various environments with nitrous acid (HONO) as an intermediate based on synthesized field evidence collected onboard aircraft platform at daytime. External cycling helps to reconcile stubborn underestimation on observed ratios of HONO/NO2 and NO2/NOz by current chemical model schemes and rationalize atypical diurnal concentration profiles of HONO and NO2 lacking noontime valleys specially observed in low-NOx atmospheres. Perturbation on the budget of HONO and NOx by external cycling is also found to increase as NOx concentration decreases. Consequently, model underestimation of OH observations by up to 41% in low NOx atmospheres is attributed to the omission of external cycling in models.

Date: 2023
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DOI: 10.1038/s41467-023-43866-z

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