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

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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 ∼1400Gmolyr −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.

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                Author and article information

                Journal
                101214388
                38670
                Atmos Chem Phys
                Atmos Chem Phys
                Atmospheric chemistry and physics
                1680-7316
                1680-7324
                4 March 2021
                4 February 2011
                March 2011
                22 March 2021
                : 11
                : 5
                : 1989-2013
                Affiliations
                [1 ]Division of Engineering and Applied Sciences, California Institute of Technology, Pasadena, California, USA
                [2 ]Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California, USA
                [3 ]Jet Propulsion Laboratory, California Institute of Technology, Pasadena, California, USA
                [4 ]University of Minnesota, Department of Soil, Water and Climate, St. Paul, Minnesota, USA
                [5 ]Department of Atmospheric and Oceanic Sciences, University of Colorado, Boulder, Colorado, USA
                [6 ]Belgian Institute for Space Aeronomy, Brussels, Belgium
                [7 ]School of Chemistry, University of Wollongong, Wollongong, Australia
                [8 ]Department of Chemistry, University of York, York, UK
                [9 ]Institute of Environmental Physics, Bremen, Germany
                [10 ]National Center for Atmospheric Research, Boulder, Colorado, USA
                [11 ]Earth System Research Laboratory, Chemical Sciences Division, NOAA, Boulder, Colorado, USA
                [12 ]Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, Colorado, USA
                [13 ]Department of Chemistry and Biochemistry, University of Colorado, Boulder, Colorado, USA
                Author notes
                [*]

                now at: AAAS Science and Technology Policy Fellow hosted at the US EPA, Washington, DC, USA

                [**]

                now at: Institute of Environmental Physics, Bremen, Germany

                Correspondence to: F. Paulot, ( paulot@ 123456caltech.edu )
                Article
                NASAPA1669546
                10.5194/acp-11-1989-2011
                7983864
                33758586
                889b4c14-50f7-4e90-9819-e888a4efecd6

                CC Attribution 3.0 License.

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