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Formaldehyde in the Tropical Western Pacific: Chemical Sources and Sinks, Convective Transport, and Representation in CAM-Chem and the CCMI Models

Anderson, Daniel C. and Nicely, Julie M. and Wolfe, Glenn M. and Hanisco, Thomas F. and Salawitch, Ross J. and Canty, Timothy P. and Dickerson, Russell R. and Apel, Eric C. and Baidar, Sunil and Bannan, Thomas J. and Blake, Nicola J. and Chen, Dexian and Dix, Barbara and Fernandez, Rafael P. and Hall, Samuel R. and Hornbrook, Rebecca S. and Huey, L. Gregory and Josse, Beatrice and Jöckel, Patrick and Kinnison, Douglas E. and Koenig, Theodore K. and Le Breton, Michael and Marécal, Virginie and Morgenstern, Olaf and Oman, Luke D. and Pan, Laura L. and Percival, Carl and Plummer, David and Revell, Laura E. and Rozanov, Eugene and Saiz-Lopez, Alfonso and Stenke, Andrea and Sudo, Kengo and Tilmes, Simone and Ullmann, Kirk and Volkamer, Rainer and Weinheimer, Andrew J. and Zeng, Guang (2017) Formaldehyde in the Tropical Western Pacific: Chemical Sources and Sinks, Convective Transport, and Representation in CAM-Chem and the CCMI Models. Journal of Geophysical Research: Atmospheres, pp. 1-26. Wiley. DOI: 10.1002/2016JD026121 ISSN 0148-0227

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Official URL: http://dx.doi.org/10.1002/2016JD026121

Abstract

Formaldehyde (HCHO) directly affects the atmospheric oxidative capacity through its effects on HOx. In remote marine environments, such as the tropical western Pacific (TWP), it is particularly important to understand the processes controlling the abundance of HCHO because model output from these regions is used to correct satellite retrievals of HCHO. Here we have used observations from the Convective Transport of Active Species in the Tropics (CONTRAST) field campaign, conducted during January and February 2014, to evaluate our understanding of the processes controlling the distribution of HCHO in the TWP as well as its representation in chemical transport/climate models. Observed HCHO mixing ratios varied from ~500 parts per trillion by volume (pptv) near the surface to ~75 pptv in the upper troposphere. Recent convective transport of near surface HCHO and its precursors, acetaldehyde and possibly methyl hydroperoxide, increased upper tropospheric HCHO mixing ratios by ~33% (22 pptv); this air contained roughly 60% less NO than more aged air. Output from the CAM-Chem chemistry transport model (2014 meteorology) as well as nine chemistry climate models from the Chemistry-Climate Model Initiative (free-running meteorology) are found to uniformly underestimate HCHO columns derived from in situ observations by between 4 and 50%. This underestimate of HCHO likely results from a near factor of two underestimate of NO in most models, which strongly suggests errors in NOx emissions inventories and/or in the model chemical mechanisms. Likewise, the lack of oceanic acetaldehyde emissions and potential errors in the model acetaldehyde chemistry lead to additional underestimates in modeled HCHO of up to 75 pptv (~15%) in the lower troposphere.

Item URL in elib:https://elib.dlr.de/115372/
Document Type:Article
Additional Information:2016JD026121
Title:Formaldehyde in the Tropical Western Pacific: Chemical Sources and Sinks, Convective Transport, and Representation in CAM-Chem and the CCMI Models
Authors:
AuthorsInstitution or Email of AuthorsAuthors ORCID iD
Anderson, Daniel C.Univ. Maryland, College Park, MD, USAUNSPECIFIED
Nicely, Julie M.NASA Goddard, Green Belt, MD, USAUNSPECIFIED
Wolfe, Glenn M.NASA Goddard, Green Belt, MD, USAUNSPECIFIED
Hanisco, Thomas F.NASA Goddard, Green Belt, MD, USAUNSPECIFIED
Salawitch, Ross J.Univ. Maryland, College Park, MD, USAUNSPECIFIED
Canty, Timothy P.Univ. Maryland, College Park, MD, USAUNSPECIFIED
Dickerson, Russell R.Univ. Maryland, College Park, MD, USAUNSPECIFIED
Apel, Eric C.NCAR, Boulder, CO, USAUNSPECIFIED
Baidar, SunilUniv. Colorado, Boulder, CO, USAUNSPECIFIED
Bannan, Thomas J.Univ. Manchester, UKUNSPECIFIED
Blake, Nicola J.Univ. California, Irvine, CA, USAUNSPECIFIED
Chen, DexianGeorgia Inst. of Technology, Atlanta, GA, USAUNSPECIFIED
Dix, BarbaraUniv. Colorado, Boulder, CO, USAUNSPECIFIED
Fernandez, Rafael P.CSIC, Madrid, SpanienUNSPECIFIED
Hall, Samuel R.NCAR, Boulder, CO, USAUNSPECIFIED
Hornbrook, Rebecca S.NCAR, Boulder, CO, USAUNSPECIFIED
Huey, L. GregoryGeorgia Inst. of Technology, Atlanta, GA, USAUNSPECIFIED
Josse, BeatriceCNRM, Toulouse, FrankreichUNSPECIFIED
Jöckel, PatrickDLR, IPAhttps://orcid.org/0000-0002-8964-1394
Kinnison, Douglas E.NCAR, Boulder, CO, USAUNSPECIFIED
Koenig, Theodore K.Univ. Colorado, Boulder, CO, USAUNSPECIFIED
Le Breton, MichaelUniv. Göteborg, SchwedenUNSPECIFIED
Marécal, VirginieCNRM, Toulouse, FrankreichUNSPECIFIED
Morgenstern, OlafNIWA, Wellington, NeuseelandUNSPECIFIED
Oman, Luke D.NASA Goddard, Green Belt, MD, USAUNSPECIFIED
Pan, Laura L.NCAR, Boulder, CO, USAUNSPECIFIED
Percival, CarlUniv. Manchester, UKUNSPECIFIED
Plummer, DavidEnv. Canada, Victoria, BC, KanadaUNSPECIFIED
Revell, Laura E.ETH Zürich, SchweizUNSPECIFIED
Rozanov, EugeneETH Zürich, SchweizUNSPECIFIED
Saiz-Lopez, AlfonsoCSIC, Madrid, SpanienUNSPECIFIED
Stenke, AndreaETH Zürich, SchweizUNSPECIFIED
Sudo, KengoNagoya Univ., JapanUNSPECIFIED
Tilmes, SimoneNCAR, Boulder, CO, USAUNSPECIFIED
Ullmann, KirkNCAR, Boulder, CO, USAUNSPECIFIED
Volkamer, RainerUniv. Colorado, Boulder, CO, USAUNSPECIFIED
Weinheimer, Andrew J.NCAR, Boulder, CO, USAUNSPECIFIED
Zeng, GuangNIWA, Wellington, NeuseelandUNSPECIFIED
Date:3 October 2017
Journal or Publication Title:Journal of Geophysical Research: Atmospheres
Refereed publication:Yes
Open Access:Yes
Gold Open Access:No
In SCOPUS:Yes
In ISI Web of Science:Yes
DOI :10.1002/2016JD026121
Page Range:pp. 1-26
Publisher:Wiley
ISSN:0148-0227
Status:Published
Keywords:Troposphere: composition and chemistry, Troposphere: constituent transport and chemistry, Formaldehyde, CONTRAST, CCMI, NOx, Acetaldehyde, Convective transport, EMAC, Modular Earth Submodel System
HGF - Research field:Aeronautics, Space and Transport
HGF - Program:Space
HGF - Program Themes:Earth Observation
DLR - Research area:Raumfahrt
DLR - Program:R EO - Erdbeobachtung
DLR - Research theme (Project):R - Vorhaben Atmosphären- und Klimaforschung, R - Project Climatic relevance of atmospheric tracer gases, aerosols and clouds, V - Verkehrsentwicklung und Umwelt II (old)
Location: Oberpfaffenhofen
Institutes and Institutions:Institute of Atmospheric Physics > Earth System Modelling
Deposited By: Jöckel, Dr. Patrick
Deposited On:16 Nov 2017 12:08
Last Modified:31 Jul 2019 20:12

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