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

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dc.contributor.authorAnderson, Daniel C.
dc.contributor.authorNicely, Julie M.
dc.contributor.authorWolfe, Glenn M.
dc.contributor.authorHanisco, Thomas F.
dc.contributor.authorSalawitch, Ross J.
dc.contributor.authorCanty, Timothy P.
dc.contributor.authorDickerson, Russell R.
dc.contributor.authorApel, Eric C.
dc.contributor.authorBaidar, Sunil
dc.contributor.authorBannan, Thomas J.
dc.contributor.authorBlake, Nicola J.
dc.contributor.authorChen, Dexian
dc.contributor.authorDix, Barbara
dc.contributor.authorFernandez, Rafael P.
dc.contributor.authorHall, Samuel R.
dc.contributor.authorHornbrook, Rebecca S.
dc.contributor.authorHuey, L. Gregory
dc.contributor.authorJosse, Beatrice
dc.contributor.authorJöckel, Patrick
dc.contributor.authorKinnison, Douglas E.
dc.contributor.authorKoenig, Theodore K.
dc.contributor.authorBreton, Michael Le
dc.contributor.authorMarécal, Virginie
dc.contributor.authorMorgenstern, Olaf
dc.contributor.authorOman, Luke D.
dc.contributor.authorPan, Laura L.
dc.contributor.authorPercival, Carl
dc.contributor.authorPlummer, David
dc.contributor.authorRevell, Laura E.
dc.contributor.authorRozanov, Eugene
dc.contributor.authorSaiz‐Lopez, Alfonso
dc.contributor.authorStenke, Andrea
dc.contributor.authorSudo, Kengo
dc.contributor.authorTilmes, Simone
dc.contributor.authorUllmann, Kirk
dc.contributor.authorVolkamer, Rainer
dc.contributor.authorWeinheimer, Andrew J.
dc.contributor.authorZeng, Guang
dc.date.accessioned2020-09-21T16:03:53Z
dc.date.available2020-09-21T16:03:53Z
dc.date.issued2017-10-06
dc.description.abstractFormaldehyde (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.en_US
dc.description.sponsorshipWe would like to thank H. Fischer forinsight into the role of MHP, theCONTRAST field team for help with fieldoperations, and the pilots and crews ofthe CAST BAe-146 and CONTRASTGulfstream V aircrafts for their dedicationand professionalism. CAST was fundedby the Natural Environment ResearchCouncil; CONTRAST was funded by theNational Science Foundation (grantNSF-AGS-1261740). A number of theU.S.-based investigators also benefittedfrom the support of NASA. Workconducted at the University of Marylandwas supported, in part, by the NASAModeling and Analysis Program underNNH12ZDA001N-MAP. G. M. W., D. C. A.,and T. F. H. received supported from theNASA Upper Atmospheric ResearchProgram under NNH12ZDA001N-UACO.J. M. N. was supported by an appoint-ment to the NASA Postdoctoral Programat the NASA Goddard Space FlightCenter, administered by UniversitiesSpace Research Association undercontract with NASA. We would like toacknowledge high-performancecomputing support from Yellowston e(ark:/85065/d7wd3xhc) provided byNCAR’s Computational and InformationSystems Laboratory. NCAR is sponsoredby the National Science Foundation. CONTRAST data are publicly available forall researchers and can be obtained athttp://data.eol.ucar.edu/master_list/?project = CONTRAST. The CAM-Chemmodel simulations are available uponrequest to the lead author(dca54@drexel.edu). CCMI output for allmodels except CESM1-WACCM isavailable at badc.nerc.ac.uk;CESM1-WACCM output is available atwww.earthsystemgrid.org. Weacknowledge the joint WCRPSPARC/IGAC Chemistry-Climate ModelInitiative (CCMI) for organizing andcoordinating the model data analysisactivity and the British Atmospheric DataCentre (BADC) for collecting andarchiving the CCMI model output. O. M.acknowledges funding by the RoyalSociety of New Zealand (grant12-NIW-006). The authors wish toacknowledge the contribution of NeSIhigh-performance computing facilitiesto the results of this research. NewZealand’s national facilities are providedby the NZ eScience Infrastructure andfunded jointly by NeSI’s collaboratorinstitutions and through the Ministry ofBusiness, Innovation & Employment’sResearch Infrastructure programme: URLhttps://www.nesi.org.nz. The EMACsimulations have been performed at theGerman Climate Computing Centre(DKRZ) through support from the Bundesministerium für Bildung undForschung (BMBF). DKRZ and itsscientific steering committee areen_US
dc.description.urihttps://agupubs.onlinelibrary.wiley.com/doi/full/10.1002/2016JD026121en_US
dc.format.extent26 pagesen_US
dc.genrejournal articlesen_US
dc.identifierdoi:10.13016/m2lpkj-qdky
dc.identifier.citationAnderson, D. C., Nicely, J. M., Wolfe, G. M.,Hanisco, T. F., Salawitch, R. J., Canty, T. P. et al., (2017). Formaldehyde in thetropical western Paci fic: Chemicalsources and sinks, convective transport,and representation in CAM-Chem andthe CCMI models. Journal of GeophysicalResearch: Atmospheres, 122,11,201–11,226, doi: https://doi.org/10.1002/2016JD026121en_US
dc.identifier.urihttps://doi.org/10.1002/2016JD026121
dc.identifier.urihttp://hdl.handle.net/11603/19696
dc.language.isoen_USen_US
dc.publisherAGU Pubicationen_US
dc.relation.isAvailableAtThe University of Maryland, Baltimore County (UMBC)
dc.relation.ispartofUMBC Joint Center for Earth Systems Technology
dc.relation.ispartofUMBC Physics Department
dc.relation.ispartofUMBC Faculty Collection
dc.rightsThis item is likely protected under Title 17 of the U.S. Copyright Law. Unless on a Creative Commons license, for uses protected by Copyright Law, contact the copyright holder or the author.
dc.rightsPublic Domain Mark 1.0*
dc.rightsThis work was written as part of one of the author's official duties as an Employee of the United States Government and is therefore a work of the United States Government. In accordance with 17 U.S.C. 105, no copyright protection is available for such works under U.S. Law.
dc.rights.urihttp://creativecommons.org/publicdomain/mark/1.0/*
dc.titleFormaldehyde in the Tropical Western Pacific: Chemical Sources and Sinks, Convective Transport, and Representation in CAM‐Chem and the CCMI Modelsen_US
dc.typeTexten_US

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