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Importance of secondary sources in the atmospheric budgets of formic and acetic acids

Paulot, F. and Wunch, D. and Crounse, J. D. and Toon, G. C. and Miller, D. B. and DeCarlo, P. F. and Vigouroux, C. and Deutscher, N. M. and González-Abad, G. and Notholt, J. and Warneke, T. and Hannigan, J. W. and Warneke, C. and de Gouw, J. A. and Dunlea, E. J. and De Mazière, M. and Griffith, D. W. T. and Bernath, P. and Jimenez, J. L. and Wennberg, P. O. (2011) Importance of secondary sources in the atmospheric budgets of formic and acetic acids. Atmospheric Chemistry and Physics, 11 (5). pp. 1989-2013. ISSN 1680-7316. https://resolver.caltech.edu/CaltechAUTHORS:20140716-074539855

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Abstract

We present a detailed budget of formic and acetic acids, two of the most abundant trace gases in the atmosphere. Our bottom-up estimate of the global source of formic and acetic acids are ~1200 and ~1400 Gmol yr^(−1), dominated by photochemical oxidation of biogenic volatile organic compounds, in particular isoprene. Their sinks are dominated by wet and dry deposition. We use the GEOS-Chem chemical transport model to evaluate this budget against an extensive suite of measurements from ground, ship and satellite-based Fourier transform spectrometers, as well as from several aircraft campaigns over North America. The model captures the seasonality of formic and acetic acids well but generally underestimates their concentration, particularly in the Northern midlatitudes. We infer that the source of both carboxylic acids may be up to 50% greater than our estimate and report evidence for a long-lived missing secondary source of carboxylic acids that may be associated with the aging of organic aerosols. Vertical profiles of formic acid in the upper troposphere support a negative temperature dependence of the reaction between formic acid and the hydroxyl radical as suggested by several theoretical studies.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.5194/acp-11-1989-2011DOIArticle
http://www.atmos-chem-phys.net/11/1989/2011/acp-11-1989-2011.htmlPublisherArticle
ORCID:
AuthorORCID
Wunch, D.0000-0002-4924-0377
Crounse, J. D.0000-0001-5443-729X
Jimenez, J. L.0000-0001-6203-1847
Wennberg, P. O.0000-0002-6126-3854
Additional Information:© 2011 Author(s). Published by Copernicus Publications on behalf of the European Geosciences Union. This work is distributed under the Creative Commons Attribution 3.0 License. Received: 18 September 2010. Published in Atmos. Chem. Phys. Discuss.: 20 October 2010. Revised: 23 February 2011. Accepted: 25 February 2011. Published: 4 March 2011. The authors thank two anonymous referees and T. Stavrakou for their constructive comments. FP is supported by a NASA Earth and Space Science fellowship. GGA is supported by the Wild Fund and the National Center for Earth Observation (NCEO). DBM acknowledges support from NASA under Grant NNX10AG65G. The National Center for Atmospheric Research is supported by the National Science Foundation. The NCAR FTS observation program at Thule (GR) is supported under contract by the National Aeronautics and Space Administration (NASA). This work is also supported by the NSF Office of Polar Programs (OPP). PFD, EJD and JLJ were supported by NASA NNX08AD39G and NOAA NA08OAR4310565. The authors wish to thank the Danish Meteorological Institute for support at the Thule site. JN acknowledges funding by the grant from the Deutsche Forschungsgemeinschaft (DFG) NO 404/14-1. NMD and DWTG acknowledge support from the Australian Department of Innovation, Industry, Science and Research, Internation Science Linkage under Grant CG130014. CV and MDM acknowledge the PRODEX project SECPEA and the project AGACC from the Belgian Science Policy Office (contracts SD/AT/O1A and SD/AT/01B) for supporting the FTIR experiment at La Réunion. Part of this work was performed at the Jet Propulsion Laboratory, California Institute of Technology, under contract with NASA. The ACE mission is supported primarily by the Canadian Space Agency. Some support was also provided by the UK Natural Environment Research Council (NERC), through the National Centre for Earth Observation (NCEO). Measurements of FA and AA during the INTEX-B and Milagro missions were supported by NASA under Grant NNG06GB32B. The authors are grateful to Stephen Arnold and Dominick Spracklen for providing the marine isoprene fluxes, and to Sheryl Akagi and Robert Yokelson for providing updated biomass burning and biofuel emission factors. The numerical simulations for this research were performed on Caltech’s Division of Geological and Planetary Sciences Dell cluster. Edited by: J. P. D. Abbatt.
Funders:
Funding AgencyGrant Number
NASA Earth and Space Science FellowshipUNSPECIFIED
Wild Fund and National Center for Earth Observation (NCEO)UNSPECIFIED
NASANNX10AG65G
NSFUNSPECIFIED
NASANNX08AD39G
National Oceanic and Atmospheric Administration (NOAA)NA08OAR4310565
Deutsche Forschungsgemeinschaft (DFG)404/14-1
Department of Innovation, Industry, Science and Research (Australia)CG130014
Belgian Science Policy Office (BELSPO)SD/AT/O1A
Belgian Science Policy Office (BELSPO)SD/AT/01B
NASA/JPL/CaltechUNSPECIFIED
Canadian Space Agency (CSA)UNSPECIFIED
Natural Environment Research Council (NERC)UNSPECIFIED
National Centre for Earth Observation (NCEO)UNSPECIFIED
NASANNG06GB32B
Issue or Number:5
Record Number:CaltechAUTHORS:20140716-074539855
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20140716-074539855
Official Citation:Paulot, F., Wunch, D., Crounse, J. D., Toon, G. C., Millet, D. B., DeCarlo, P. F., Vigouroux, C., Deutscher, N. M., González Abad, G., Notholt, J., Warneke, T., Hannigan, J. W., Warneke, C., de Gouw, J. A., Dunlea, E. J., De Mazière, M., Griffith, D. W. T., Bernath, P., Jimenez, J. L., and Wennberg, P. O.: Importance of secondary sources in the atmospheric budgets of formic and acetic acids, Atmos. Chem. Phys., 11, 1989-2013, doi:10.5194/acp-11-1989-2011, 2011.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:47252
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:16 Jul 2014 16:21
Last Modified:03 Oct 2019 06:51

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