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Rapid deposition of oxidized biogenic compounds to a temperate forest

Nguyen, Tran B. and Crounse, John D. and Teng, Alex P. and St. Clair, Jason M. and Paulot, Fabien and Wolfe, Glenn M. and Wennberg, Paul O. (2015) Rapid deposition of oxidized biogenic compounds to a temperate forest. Proceedings of the National Academy of Sciences of the United States of America, 112 (5). E392-E401. ISSN 0027-8424. PMCID PMC4321284. https://resolver.caltech.edu/CaltechAUTHORS:20141222-144149377

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Abstract

We report fluxes and dry deposition velocities for 16 atmospheric compounds above a southeastern United States forest, including: hydrogen peroxide (H_2O_2), nitric acid (HNO_3), hydrogen cyanide (HCN), hydroxymethyl hydroperoxide, peroxyacetic acid, organic hydroxy nitrates, and other multifunctional species derived from the oxidation of isoprene and monoterpenes. The data suggest that dry deposition is the dominant daytime sink for small, saturated oxygenates. Greater than 6 wt %C emitted as isoprene by the forest was returned by dry deposition of its oxidized products. Peroxides account for a large fraction of the oxidant flux, possibly eclipsing ozone in more pristine regions. The measured organic nitrates comprise a sizable portion (15%) of the oxidized nitrogen input into the canopy, with HNO_3 making up the balance. We observe that water-soluble compounds (e.g., strong acids and hydroperoxides) deposit with low surface resistance whereas compounds with moderate solubility (e.g., organic nitrates and hydroxycarbonyls) or poor solubility (e.g., HCN) exhibited reduced uptake at the surface of plants. To first order, the relative deposition velocities of water-soluble compounds are constrained by their molecular diffusivity. From resistance modeling, we infer a substantial emission flux of formic acid at the canopy level (∼1 nmol m^(−2)⋅s^(−1)). GEOS−Chem, a widely used atmospheric chemical transport model, currently underestimates dry deposition for most molecules studied in this work. Reconciling GEOS−Chem deposition velocities with observations resulted in up to a 45% decrease in the simulated surface concentration of trace gases.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1073/pnas.1418702112 DOIArticle
http://www.pnas.org/content/112/5/E392.abstractPublisherArticle
http://www.pnas.org/lookup/suppl/doi:10.1073/pnas.1418702112/-/DCSupplementalPublisherSupporting Information
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC4321284/PubMed CentralArticle
ORCID:
AuthorORCID
Crounse, John D.0000-0001-5443-729X
St. Clair, Jason M.0000-0002-9367-5749
Paulot, Fabien0000-0001-7534-4922
Wolfe, Glenn M.0000-0001-6586-4043
Wennberg, Paul O.0000-0002-6126-3854
Additional Information:Copyright © 2015 National Academy of Sciences. Freely available online through the PNAS open access option. Edited by Mark H. Thiemens, University of California, San Diego, La Jolla, CA, and approved December 22, 2014 (received for review September 28, 2014) Published online before print January 20, 2015 We thank the organizers and committee members of the SOAS campaign: A. G. Carlton, A. H. Goldstein, J. L. Jimenez, R. W. Pinder, J. de Gouw, B. J. Turpin, and A. B. Guenther. We acknowledge C. J. Groff at Purdue University for his help with leaf area index measurements and tree surveys. We thank D. J. Jacob and the Atmospheric Chemistry Modeling Group at Harvard University for making GEOS−Chem available for this work. Meteorological data used in the GEOS−Chem simulations were provided by the Global Modeling and Assimilation Office at NASA Goddard Space Flight Center. We acknowledge funding from the National Science Foundation (NSF) under Grant AGS-1240604 and NSF Postdoctoral Research Fellowship program Award AGS-1331360. Financial and logistical support for SOAS was provided by the NSF, the Earth Observing Laboratory at the National Center for Atmospheric Research (operated by NSF), the personnel at Atmospheric Research and Analysis, and the Electric Power Research Institute. Author contributions: P.O.W. designed research; T.B.N., J.D.C., A.P.T., J.M.S.C., F.P., and G.M.W. performed research; J.D.C. contributed new reagents/analytic tools; T.B.N. analyzed data; and T.B.N. and P.O.W. wrote the paper. The authors declare no conflict of interest. This article is a PNAS Direct Submission. This article contains supporting information online at www.pnas.org/lookup/suppl/doi:10.1073/pnas.1418702112/-/DCSupplemental.
Funders:
Funding AgencyGrant Number
NSFAGS-1240604
NSF Postdoctoral FellowshipAGS-1331360
National Center for Atmospheric Research (NCAR)UNSPECIFIED
Electric Power Research Institute (EPRI)UNSPECIFIED
Subject Keywords:biosphere−atmosphere exchange | isoprene | dry deposition | OVOCs | fluxes
Issue or Number:5
PubMed Central ID:PMC4321284
Record Number:CaltechAUTHORS:20141222-144149377
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20141222-144149377
Official Citation:Tran B. Nguyen, John D. Crounse, Alex P. Teng, Jason M. St. Clair, Fabien Paulot, Glenn M. Wolfe, and Paul O. Wennberg Rapid deposition of oxidized biogenic compounds to a temperate forest PNAS 2015 112 (5) E392-E401; published ahead of print January 20, 2015, doi:10.1073/pnas.1418702112
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:53113
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:20 Jan 2015 17:51
Last Modified:09 Mar 2020 13:19

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