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Title: High upward fluxes of formic acid from a boreal forest canopy

Abstract

Eddy covariance fluxes of formic acid, HCOOH, were measured over a boreal forest canopy in spring/summer 2014. The HCOOH fluxes were bidirectional but mostly upward during daytime, in contrast to studies elsewhere that reported mostly downward fluxes. Downward flux episodes were explained well by modeled dry deposition rates. The sum of net observed flux and modeled dry deposition yields an upward “gross flux” of HCOOH, which could not be quantitatively explained by literature estimates of direct vegetative/soil emissions nor by efficient chemical production from other volatile organic compounds, suggesting missing or greatly underestimated HCOOH sources in the boreal ecosystem. Here, we implemented a vegetative HCOOH source into the GEOS-Chem chemical transport model to match our derived gross flux and evaluated the updated model against airborne and spaceborne observations. Model biases in the boundary layer were substantially reduced based on this revised treatment, but biases in the free troposphere remain unexplained.

Authors:
 [1];  [2];  [3];  [4];  [5];  [6];  [6];  [6]; ORCiD logo [7];  [2];  [6];  [2]
  1. Univ. of Washington, Seattle, WA (United States). Dept. of Atmospheric Sciences; Univ. of Helsinki (Finland). Dept. of Physics
  2. Univ. of Washington, Seattle, WA (United States). Dept. of Atmospheric Sciences
  3. Estonian Univ. of Life Sciences, Tartu (Estonia). Dept. of Plant Physiology; Univ. of Helsinki (Finland). Dept. of Forest Sciences
  4. Univ. of Minnesota, Minneapolis, MN (United States). Dept. of Soil, Water, and Climate
  5. Univ. of Washington, Seattle, WA (United States). Dept. of Chemistry
  6. Univ. of Helsinki (Finland). Dept. of Physics
  7. NASA Goddard Space Flight Center (GSFC), Greenbelt, MD (United States). Atmospheric Chemistry and Dynamics Lab.; Univ. of Maryland, Baltimore, MD (United States). Joint Center for Earth Systems Technology
Publication Date:
Research Org.:
Univ. of Washington, Seattle, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC); European Commission (EU); National Science Foundation (NSF)
OSTI Identifier:
1392635
Alternate Identifier(s):
OSTI ID: 1402387
Grant/Contract Number:
SC0011791; SC0006867
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Geophysical Research Letters
Additional Journal Information:
Journal Volume: 43; Journal Issue: 17; Journal ID: ISSN 0094-8276
Publisher:
American Geophysical Union
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; formic acid; eddy covariance fluxes; chemical ionization mass spectrometry; boreal forest; biogenic emissions

Citation Formats

Schobesberger, Siegfried, Lopez-Hilfiker, Felipe D., Taipale, Ditte, Millet, Dylan B., D'Ambro, Emma L., Rantala, Pekka, Mammarella, Ivan, Zhou, Putian, Wolfe, Glenn M., Lee, Ben H., Boy, Michael, and Thornton, Joel A. High upward fluxes of formic acid from a boreal forest canopy. United States: N. p., 2016. Web. doi:10.1002/2016GL069599.
Schobesberger, Siegfried, Lopez-Hilfiker, Felipe D., Taipale, Ditte, Millet, Dylan B., D'Ambro, Emma L., Rantala, Pekka, Mammarella, Ivan, Zhou, Putian, Wolfe, Glenn M., Lee, Ben H., Boy, Michael, & Thornton, Joel A. High upward fluxes of formic acid from a boreal forest canopy. United States. doi:10.1002/2016GL069599.
Schobesberger, Siegfried, Lopez-Hilfiker, Felipe D., Taipale, Ditte, Millet, Dylan B., D'Ambro, Emma L., Rantala, Pekka, Mammarella, Ivan, Zhou, Putian, Wolfe, Glenn M., Lee, Ben H., Boy, Michael, and Thornton, Joel A. Sun . "High upward fluxes of formic acid from a boreal forest canopy". United States. doi:10.1002/2016GL069599. https://www.osti.gov/servlets/purl/1392635.
@article{osti_1392635,
title = {High upward fluxes of formic acid from a boreal forest canopy},
author = {Schobesberger, Siegfried and Lopez-Hilfiker, Felipe D. and Taipale, Ditte and Millet, Dylan B. and D'Ambro, Emma L. and Rantala, Pekka and Mammarella, Ivan and Zhou, Putian and Wolfe, Glenn M. and Lee, Ben H. and Boy, Michael and Thornton, Joel A.},
abstractNote = {Eddy covariance fluxes of formic acid, HCOOH, were measured over a boreal forest canopy in spring/summer 2014. The HCOOH fluxes were bidirectional but mostly upward during daytime, in contrast to studies elsewhere that reported mostly downward fluxes. Downward flux episodes were explained well by modeled dry deposition rates. The sum of net observed flux and modeled dry deposition yields an upward “gross flux” of HCOOH, which could not be quantitatively explained by literature estimates of direct vegetative/soil emissions nor by efficient chemical production from other volatile organic compounds, suggesting missing or greatly underestimated HCOOH sources in the boreal ecosystem. Here, we implemented a vegetative HCOOH source into the GEOS-Chem chemical transport model to match our derived gross flux and evaluated the updated model against airborne and spaceborne observations. Model biases in the boundary layer were substantially reduced based on this revised treatment, but biases in the free troposphere remain unexplained.},
doi = {10.1002/2016GL069599},
journal = {Geophysical Research Letters},
number = 17,
volume = 43,
place = {United States},
year = {Sun Aug 14 00:00:00 EDT 2016},
month = {Sun Aug 14 00:00:00 EDT 2016}
}

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