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; Shaojie Song

doi:10.1038/s41467-023-43866-z

Synthesizing evidence for the external cycling of NO_x in high- to low-NO_x 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, Shaojie Song

Peking University
Wadsworth Center for Laboratories and Research
SUNY Albany
Beijing Forestry University
University of Leeds
Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA) - UMR 7583
Carnegie Mellon University
University of Colorado Boulder
National Center for Atmospheric Research
University of California at Los Angeles
University of Innsbruck
University of California at Irvine
Nankai University

Research output: Contribution to journal › Article › peer-review

32 Scopus citations

Abstract

External cycling regenerating nitrogen oxides (NO_x ≡ NO + NO₂) from their oxidative reservoir, NO_z, is proposed to reshape the temporal–spatial distribution of NO_x and consequently hydroxyl radical (OH), the most important oxidant in the atmosphere. Here we verify the in situ external cycling of NO_x 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/NO_z by current chemical model schemes and rationalize atypical diurnal concentration profiles of HONO and NO₂ lacking noontime valleys specially observed in low-NO_x atmospheres. Perturbation on the budget of HONO and NO_x by external cycling is also found to increase as NO_x concentration decreases. Consequently, model underestimation of OH observations by up to 41% in low NO_x atmospheres is attributed to the omission of external cycling in models.

Original language	English
Article number	7995
Journal	Nature Communications
Volume	14
Issue number	1
DOIs	https://doi.org/10.1038/s41467-023-43866-z
State	Published - Dec 2023
Externally published	Yes

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Ye, C., Zhou, X., Zhang, Y., Wang, Y., Wang, J., Zhang, C., Woodward-Massey, R., Cantrell, C., Mauldin, R. L., Campos, T., Hornbrook, R. S., Ortega, J., Apel, E. C., Haggerty, J., Hall, S., Ullmann, K., Weinheimer, A., Stutz, J., Karl, T., ... Song, S. (2023). Synthesizing evidence for the external cycling of NO_x in high- to low-NO_x atmospheres. Nature Communications, 14(1), Article 7995. https://doi.org/10.1038/s41467-023-43866-z

@article{06d046d95b61438093675829c074eb26,

title = "Synthesizing evidence for the external cycling of NOx in high- to low-NOx atmospheres",

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.",

author = "Chunxiang Ye and Xianliang Zhou and Yingjie Zhang and Youfeng Wang and Jianshu Wang and Chong Zhang and Robert Woodward-Massey and Christopher Cantrell and Mauldin, \{Roy L.\} and Teresa Campos and Hornbrook, \{Rebecca S.\} and John Ortega and Apel, \{Eric C.\} and Julie Haggerty and Samuel Hall and Kirk Ullmann and Andrew Weinheimer and Jochen Stutz and Thomas Karl and Smith, \{James N.\} and Alex Guenther and Shaojie Song",

note = "Publisher Copyright: {\textcopyright} 2023, The Author(s).",

year = "2023",

month = dec,

doi = "10.1038/s41467-023-43866-z",

language = "English",

volume = "14",

journal = "Nature Communications",

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Ye, C, Zhou, X, Zhang, Y, Wang, Y, Wang, J, Zhang, C, Woodward-Massey, R, Cantrell, C, Mauldin, RL, Campos, T , Hornbrook, RS, Ortega, J, Apel, EC , Haggerty, J , Hall, S , Ullmann, K, Weinheimer, A, Stutz, J, Karl, T, Smith, JN, Guenther, A & Song, S 2023, 'Synthesizing evidence for the external cycling of NO_x in high- to low-NO_x atmospheres', Nature Communications, vol. 14, no. 1, 7995. https://doi.org/10.1038/s41467-023-43866-z

TY - JOUR

T1 - Synthesizing evidence for the external cycling of NOx in high- to low-NOx atmospheres

AU - Ye, Chunxiang

AU - Zhou, Xianliang

AU - Zhang, Yingjie

AU - Wang, Youfeng

AU - Wang, Jianshu

AU - Zhang, Chong

AU - Woodward-Massey, Robert

AU - Cantrell, Christopher

AU - Mauldin, Roy L.

AU - Campos, Teresa

AU - Hornbrook, Rebecca S.

AU - Ortega, John

AU - Apel, Eric C.

AU - Haggerty, Julie

AU - Hall, Samuel

AU - Ullmann, Kirk

AU - Weinheimer, Andrew

AU - Stutz, Jochen

AU - Karl, Thomas

AU - Smith, James N.

AU - Guenther, Alex

AU - Song, Shaojie

PY - 2023/12

Y1 - 2023/12

N2 - 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.

AB - 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.

UR - https://www.scopus.com/pages/publications/85178380462

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DO - 10.1038/s41467-023-43866-z

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AN - SCOPUS:85178380462

SN - 2041-1723

VL - 14

JO - Nature Communications

JF - Nature Communications

IS - 1

M1 - 7995

ER -

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

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