Atmospheric Acetaldehyde: Importance of Air-Sea Exchange and a Missing Source in the Remote Troposphere

Siyuan Wang; Rebecca S. Hornbrook; Alan Hills; Louisa K. Emmons; Simone Tilmes; Jean François Lamarque; Jose L. Jimenez; Pedro Campuzano-Jost; Benjamin A. Nault; John D. Crounse; Paul O. Wennberg; Michelle Kim; Hannah Allen; Thomas B. Ryerson; Chelsea R. Thompson; Jeff Peischl; Fred Moore; David Nance; Brad Hall; James Elkins; David Tanner; L. Gregory Huey; Samuel R. Hall; Kirk Ullmann; John J. Orlando; Geoff S. Tyndall; Frank M. Flocke; Eric Ray; Thomas F. Hanisco; Glenn M. Wolfe; Jason St. Clair; Róisín Commane; Bruce Daube; Barbara Barletta; Donald R. Blake; Bernadett Weinzierl; Maximilian Dollner; Andrew Conley; Francis Vitt; Steven C. Wofsy; Daniel D. Riemer; Eric C. Apel

doi:10.1029/2019GL082034

Atmospheric Acetaldehyde: Importance of Air-Sea Exchange and a Missing Source in the Remote Troposphere

Siyuan Wang
, Rebecca S. Hornbrook
, Alan Hills
, Louisa K. Emmons
, Simone Tilmes
, Jean François Lamarque
, Jose L. Jimenez
, Pedro Campuzano-Jost
, Benjamin A. Nault
, John D. Crounse
, Paul O. Wennberg
, Michelle Kim
, Hannah Allen
, Thomas B. Ryerson
, Chelsea R. Thompson
, Jeff Peischl
, Fred Moore
, David Nance
, Brad Hall
, James Elkins

David Tanner, L. Gregory Huey, Samuel R. Hall, Kirk Ullmann, John J. Orlando, Geoff S. Tyndall, Frank M. Flocke, Eric Ray, Thomas F. Hanisco, Glenn M. Wolfe, Jason St. Clair, Róisín Commane, Bruce Daube, Barbara Barletta, Donald R. Blake, Bernadett Weinzierl, Maximilian Dollner, Andrew Conley, Francis Vitt, Steven C. Wofsy, Daniel D. Riemer, Eric C. Apel

Atmospheric Chemistry Observations & Modeling Lab

National Center for Atmospheric Research
University of Colorado Boulder
California Institute of Technology Division of Engineering and Applied Science
National Oceanic and Atmospheric Administration
Georgia Institute of Technology
NASA Goddard Space Flight Center
University of Maryland, College Park
Harvard University
Columbia University
University of California at Irvine
University of Vienna
Environmental Inc.

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

57 Scopus citations

Abstract

We report airborne measurements of acetaldehyde (CH₃CHO) during the first and second deployments of the National Aeronautics and Space Administration Atmospheric Tomography Mission (ATom). The budget of CH₃CHO is examined using the Community Atmospheric Model with chemistry (CAM-chem), with a newly developed online air-sea exchange module. The upper limit of the global ocean net emission of CH₃CHO is estimated to be 34 Tg/a (42 Tg/a if considering bubble-mediated transfer), and the ocean impacts on tropospheric CH₃CHO are mostly confined to the marine boundary layer. Our analysis suggests that there is an unaccounted CH₃CHO source in the remote troposphere and that organic aerosols can only provide a fraction of this missing source. We propose that peroxyacetic acid is an ideal indicator of the rapid CH₃CHO production in the remote troposphere. The higher-than-expected CH₃CHO measurements represent a missing sink of hydroxyl radicals (and halogen radical) in current chemistry-climate models.

Original language	English
Pages (from-to)	5601-5613
Number of pages	13
Journal	Geophysical Research Letters
Volume	46
Issue number	10
DOIs	https://doi.org/10.1029/2019GL082034
State	Published - May 28 2019

Keywords

acetaldehyde
air-sea exchange
chemistry climate model
ocean biogeochemistry
oxidative capacity

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10.1029/2019GL082034

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Wang, S., Hornbrook, R. S., Hills, A., Emmons, L. K., Tilmes, S., Lamarque, J. F., Jimenez, J. L., Campuzano-Jost, P., Nault, B. A., Crounse, J. D., Wennberg, P. O., Kim, M., Allen, H., Ryerson, T. B., Thompson, C. R., Peischl, J., Moore, F., Nance, D., Hall, B., ... Apel, E. C. (2019). Atmospheric Acetaldehyde: Importance of Air-Sea Exchange and a Missing Source in the Remote Troposphere. Geophysical Research Letters, 46(10), 5601-5613. https://doi.org/10.1029/2019GL082034

@article{3772a0b1a5db47d9ab6e875ce2578e57,

title = "Atmospheric Acetaldehyde: Importance of Air-Sea Exchange and a Missing Source in the Remote Troposphere",

abstract = "We report airborne measurements of acetaldehyde (CH3CHO) during the first and second deployments of the National Aeronautics and Space Administration Atmospheric Tomography Mission (ATom). The budget of CH3CHO is examined using the Community Atmospheric Model with chemistry (CAM-chem), with a newly developed online air-sea exchange module. The upper limit of the global ocean net emission of CH3CHO is estimated to be 34 Tg/a (42 Tg/a if considering bubble-mediated transfer), and the ocean impacts on tropospheric CH3CHO are mostly confined to the marine boundary layer. Our analysis suggests that there is an unaccounted CH3CHO source in the remote troposphere and that organic aerosols can only provide a fraction of this missing source. We propose that peroxyacetic acid is an ideal indicator of the rapid CH3CHO production in the remote troposphere. The higher-than-expected CH3CHO measurements represent a missing sink of hydroxyl radicals (and halogen radical) in current chemistry-climate models.",

keywords = "acetaldehyde, air-sea exchange, chemistry climate model, ocean biogeochemistry, oxidative capacity",

author = "Siyuan Wang and Hornbrook, \{Rebecca S.\} and Alan Hills and Emmons, \{Louisa K.\} and Simone Tilmes and Lamarque, \{Jean Fran{\c c}ois\} and Jimenez, \{Jose L.\} and Pedro Campuzano-Jost and Nault, \{Benjamin A.\} and Crounse, \{John D.\} and Wennberg, \{Paul O.\} and Michelle Kim and Hannah Allen and Ryerson, \{Thomas B.\} and Thompson, \{Chelsea R.\} and Jeff Peischl and Fred Moore and David Nance and Brad Hall and James Elkins and David Tanner and Huey, \{L. Gregory\} and Hall, \{Samuel R.\} and Kirk Ullmann and Orlando, \{John J.\} and Tyndall, \{Geoff S.\} and Flocke, \{Frank M.\} and Eric Ray and Hanisco, \{Thomas F.\} and Wolfe, \{Glenn M.\} and \{St. Clair\}, Jason and R{\'o}is{\'i}n Commane and Bruce Daube and Barbara Barletta and Blake, \{Donald R.\} and Bernadett Weinzierl and Maximilian Dollner and Andrew Conley and Francis Vitt and Wofsy, \{Steven C.\} and Riemer, \{Daniel D.\} and Apel, \{Eric C.\}",

year = "2019",

month = may,

day = "28",

doi = "10.1029/2019GL082034",

language = "English",

volume = "46",

pages = "5601--5613",

journal = "Geophysical Research Letters",

issn = "0094-8276",

publisher = "John Wiley and Sons Inc.",

number = "10",

}

Wang, S, Hornbrook, RS , Hills, A , Emmons, LK , Tilmes, S, Lamarque, JF, Jimenez, JL, Campuzano-Jost, P, Nault, BA, Crounse, JD, Wennberg, PO, Kim, M, Allen, H, Ryerson, TB, Thompson, CR, Peischl, J, Moore, F, Nance, D, Hall, B, Elkins, J, Tanner, D, Huey, LG, Hall, SR , Ullmann, K, Orlando, JJ, Tyndall, GS, Flocke, FM, Ray, E, Hanisco, TF, Wolfe, GM, St. Clair, J, Commane, R, Daube, B, Barletta, B, Blake, DR, Weinzierl, B, Dollner, M, Conley, A, Vitt, F, Wofsy, SC, Riemer, DD & Apel, EC 2019, 'Atmospheric Acetaldehyde: Importance of Air-Sea Exchange and a Missing Source in the Remote Troposphere', Geophysical Research Letters, vol. 46, no. 10, pp. 5601-5613. https://doi.org/10.1029/2019GL082034

TY - JOUR

T1 - Atmospheric Acetaldehyde

T2 - Importance of Air-Sea Exchange and a Missing Source in the Remote Troposphere

AU - Wang, Siyuan

AU - Hornbrook, Rebecca S.

AU - Hills, Alan

AU - Emmons, Louisa K.

AU - Tilmes, Simone

AU - Lamarque, Jean François

AU - Jimenez, Jose L.

AU - Campuzano-Jost, Pedro

AU - Nault, Benjamin A.

AU - Crounse, John D.

AU - Wennberg, Paul O.

AU - Kim, Michelle

AU - Allen, Hannah

AU - Ryerson, Thomas B.

AU - Thompson, Chelsea R.

AU - Peischl, Jeff

AU - Moore, Fred

AU - Nance, David

AU - Hall, Brad

AU - Elkins, James

AU - Tanner, David

AU - Huey, L. Gregory

AU - Hall, Samuel R.

AU - Ullmann, Kirk

AU - Orlando, John J.

AU - Tyndall, Geoff S.

AU - Flocke, Frank M.

AU - Ray, Eric

AU - Hanisco, Thomas F.

AU - Wolfe, Glenn M.

AU - St. Clair, Jason

AU - Commane, Róisín

AU - Daube, Bruce

AU - Barletta, Barbara

AU - Blake, Donald R.

AU - Weinzierl, Bernadett

AU - Dollner, Maximilian

AU - Conley, Andrew

AU - Vitt, Francis

AU - Wofsy, Steven C.

AU - Riemer, Daniel D.

AU - Apel, Eric C.

PY - 2019/5/28

Y1 - 2019/5/28

N2 - We report airborne measurements of acetaldehyde (CH3CHO) during the first and second deployments of the National Aeronautics and Space Administration Atmospheric Tomography Mission (ATom). The budget of CH3CHO is examined using the Community Atmospheric Model with chemistry (CAM-chem), with a newly developed online air-sea exchange module. The upper limit of the global ocean net emission of CH3CHO is estimated to be 34 Tg/a (42 Tg/a if considering bubble-mediated transfer), and the ocean impacts on tropospheric CH3CHO are mostly confined to the marine boundary layer. Our analysis suggests that there is an unaccounted CH3CHO source in the remote troposphere and that organic aerosols can only provide a fraction of this missing source. We propose that peroxyacetic acid is an ideal indicator of the rapid CH3CHO production in the remote troposphere. The higher-than-expected CH3CHO measurements represent a missing sink of hydroxyl radicals (and halogen radical) in current chemistry-climate models.

AB - We report airborne measurements of acetaldehyde (CH3CHO) during the first and second deployments of the National Aeronautics and Space Administration Atmospheric Tomography Mission (ATom). The budget of CH3CHO is examined using the Community Atmospheric Model with chemistry (CAM-chem), with a newly developed online air-sea exchange module. The upper limit of the global ocean net emission of CH3CHO is estimated to be 34 Tg/a (42 Tg/a if considering bubble-mediated transfer), and the ocean impacts on tropospheric CH3CHO are mostly confined to the marine boundary layer. Our analysis suggests that there is an unaccounted CH3CHO source in the remote troposphere and that organic aerosols can only provide a fraction of this missing source. We propose that peroxyacetic acid is an ideal indicator of the rapid CH3CHO production in the remote troposphere. The higher-than-expected CH3CHO measurements represent a missing sink of hydroxyl radicals (and halogen radical) in current chemistry-climate models.

KW - acetaldehyde

KW - air-sea exchange

KW - chemistry climate model

KW - ocean biogeochemistry

KW - oxidative capacity

UR - https://www.scopus.com/pages/publications/85067597815

U2 - 10.1029/2019GL082034

DO - 10.1029/2019GL082034

M3 - Article

AN - SCOPUS:85067597815

SN - 0094-8276

VL - 46

SP - 5601

EP - 5613

JO - Geophysical Research Letters

JF - Geophysical Research Letters

IS - 10

ER -

Atmospheric Acetaldehyde: Importance of Air-Sea Exchange and a Missing Source in the Remote Troposphere

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Keywords

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