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    Bidirectional Ecosystem–Atmosphere Fluxes of Volatile Organic Compounds Across the Mass Spectrum: How Many Matter?
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    • Dylan B. Millet*
      Dylan B. Millet
      University of Minnesota, Saint Paul, Minnesota 55108, United States
      *E-mail: [email protected]
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      Orcidhttp://orcid.org/0000-0003-3076-125X
    • Hariprasad D. Alwe
      Hariprasad D. Alwe
      University of Minnesota, Saint Paul, Minnesota 55108, United States
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    • Xin Chen
      Xin Chen
      University of Minnesota, Saint Paul, Minnesota 55108, United States
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    • Malte Julian Deventer
      Malte Julian Deventer
      University of Minnesota, Saint Paul, Minnesota 55108, United States
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    • Timothy J. Griffis
      Timothy J. Griffis
      University of Minnesota, Saint Paul, Minnesota 55108, United States
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    • Rupert Holzinger
      Rupert Holzinger
      Utrecht University, Utrecht 3584 CC, The Netherlands
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    • Steven B. Bertman
      Steven B. Bertman
      Western Michigan University, Kalamazoo, Michigan 49008, United States
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    • Pamela S. Rickly
      Pamela S. Rickly
      Indiana University, Bloomington, Indiana 47405, United States
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    • Philip S. Stevens
      Philip S. Stevens
      Indiana University, Bloomington, Indiana 47405, United States
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      Orcidhttp://orcid.org/0000-0001-9899-4215
    • Thierry Léonardis
      Thierry Léonardis
      IMT Lille Douai, Univ. Lille, SAGE - Département Sciences de l’Atmosphère et Génie de l’Environnement, 59000 Lille, France
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    • Nadine Locoge
      Nadine Locoge
      IMT Lille Douai, Univ. Lille, SAGE - Département Sciences de l’Atmosphère et Génie de l’Environnement, 59000 Lille, France
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    • Sébastien Dusanter
      Sébastien Dusanter
      IMT Lille Douai, Univ. Lille, SAGE - Département Sciences de l’Atmosphère et Génie de l’Environnement, 59000 Lille, France
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    • Geoffrey S. Tyndall
      Geoffrey S. Tyndall
      National Center for Atmospheric Research, Boulder, Colorado 80305, United States
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    • Sergio L. Alvarez
      Sergio L. Alvarez
      University of Houston, Houston, Texas 77004, United States
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    • Matthew H. Erickson
      Matthew H. Erickson
      University of Houston, Houston, Texas 77004, United States
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    • James H. Flynn
      James H. Flynn
      University of Houston, Houston, Texas 77004, United States
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    ACS Earth and Space Chemistry

    Cite this: ACS Earth Space Chem. 2018, 2, 8, 764–777
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    https://doi.org/10.1021/acsearthspacechem.8b00061
    Published June 14, 2018
    Copyright © 2018 American Chemical Society
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    Abstract

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    Terrestrial ecosystems are simultaneously the largest source and a major sink of volatile organic compounds (VOCs) to the global atmosphere, and these two-way fluxes are an important source of uncertainty in current models. Here, we apply high-resolution mass spectrometry (proton transfer reaction-quadrupole interface time-of-flight; PTR-QiTOF) to measure ecosystem–atmosphere VOC fluxes across the entire detected mass range (m/z 0–335) over a mixed temperate forest and use the results to test how well a state-of-science chemical transport model (GEOS-Chem CTM) is able to represent the observed reactive carbon exchange. We show that ambient humidity fluctuations can give rise to spurious VOC fluxes with PTR-based techniques and present a method to screen for such effects. After doing so, 377 of the 636 detected ions exhibited detectable gross fluxes during the study, implying a large number of species with active ecosystem–atmosphere exchange. We introduce the reactivity flux as a measure of how Earth–atmosphere fluxes influence ambient OH reactivity and show that the upward total VOC (∑VOC) carbon and reactivity fluxes are carried by a far smaller number of species than the downward fluxes. The model underpredicts the ∑VOC carbon and reactivity fluxes by 40–60% on average. However, the observed net fluxes are dominated (90% on a carbon basis, 95% on a reactivity basis) by known VOCs explicitly included in the CTM. As a result, the largest CTM uncertainties in simulating VOC carbon and reactivity exchange for this environment are associated with known rather than unrepresented species. This conclusion pertains to the set of species detectable by PTR-TOF techniques, which likely represents the majority in terms of carbon mass and OH reactivity, but not necessarily in terms of aerosol formation potential. In the case of oxygenated VOCs, the model severely underpredicts the gross fluxes and the net exchange. Here, unrepresented VOCs play a larger role, accounting for ∼30% of the carbon flux and ∼50% of the reactivity flux. The resulting CTM biases, however, are still smaller than those that arise from uncertainties for known and represented compounds.

    Copyright © 2018 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsearthspacechem.8b00061.

    • Table S1, parameters for compressed VOC standards; Figure S1, workflow for assigning molecular formulas; Figure S2, comparison of above-canopy and canopy storage fluxes; Figures S3 and S4, spectral analysis for example m/z ratios; Figure S5, diel cycle of isoprene and monoterpene fluxes; Figure S6, OH reactivity comparison (PDF)

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    ACS Earth and Space Chemistry

    Cite this: ACS Earth Space Chem. 2018, 2, 8, 764–777
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsearthspacechem.8b00061
    Published June 14, 2018
    Copyright © 2018 American Chemical Society
    Request reuse permissions

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