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

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Title: Synthesizing evidence for the external cycling of NOx in high- to low-NOx atmospheres
Authors: 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, Shaojie Song
Source: Nature Communications, Vol 14, Iss 1, Pp 1-10 (2023)
Publisher Information: Nature Portfolio, 2023.
Publication Year: 2023
Collection: LCC:Science
Subject Terms: Science
More Details: 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.
Document Type: article
File Description: electronic resource
Language: English
ISSN: 2041-1723
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DOI: 10.1038/s41467-023-43866-z
Access URL: https://doaj.org/article/dc8026c53c4f45c198b40e6742d8522e
Accession Number: edsdoj.8026c53c4f45c198b40e6742d8522e
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  Data: 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.
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