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

Author

Listed:
  • Chunxiang Ye

    (College of Environmental Sciences and Engineering, Peking University)

  • Xianliang Zhou

    (Wadsworth Center, New York State Department of Health
    State University of New York)

  • Yingjie Zhang

    (College of Environmental Sciences and Engineering, Peking University
    Beijing Forestry 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
    University of Leeds)

  • Christopher Cantrell

    (Université Paris-est Créteil, LISA (Laboratoire Interuniversitaire des Systèmes Atmosphériques))

  • Roy L. Mauldin

    (Carnegie Mellon University
    Carnegie Mellon University
    University of Colorado Boulder)

  • 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)

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.

Suggested Citation

  • 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, 2023. "Synthesizing evidence for the external cycling of NOx in high- to low-NOx atmospheres," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-43866-z
    DOI: 10.1038/s41467-023-43866-z
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    References listed on IDEAS

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    1. J. Lelieveld & T. M. Butler & J. N. Crowley & T. J. Dillon & H. Fischer & L. Ganzeveld & H. Harder & M. G. Lawrence & M. Martinez & D. Taraborrelli & J. Williams, 2008. "Atmospheric oxidation capacity sustained by a tropical forest," Nature, Nature, vol. 452(7188), pages 737-740, April.
    2. M. Ammann & M. Kalberer & D. T. Jost & L. Tobler & E. Rössler & D. Piguet & H. W. Gäggeler & U. Baltensperger, 1998. "Heterogeneous production of nitrous acid on soot in polluted air masses," Nature, Nature, vol. 395(6698), pages 157-160, September.
    3. Chunxiang Ye & Xianliang Zhou & Dennis Pu & Jochen Stutz & James Festa & Max Spolaor & Catalina Tsai & Christopher Cantrell & Roy L. Mauldin & Teresa Campos & Andrew Weinheimer & Rebecca S. Hornbrook , 2016. "Rapid cycling of reactive nitrogen in the marine boundary layer," Nature, Nature, vol. 532(7600), pages 489-491, April.
    4. Konrad Stemmler & Markus Ammann & Chantal Donders & Jörg Kleffmann & Christian George, 2006. "Photosensitized reduction of nitrogen dioxide on humic acid as a source of nitrous acid," Nature, Nature, vol. 440(7081), pages 195-198, March.
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