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Title: Ambient observations of dimers from terpene oxidation in the gas phase: Implications for new particle formation and growth: Ambient Observations of Gas-Phase Dimers

Abstract

Here, we present ambient observations of dimeric monoterpene oxidation products (C 16–20H yO 6–9) in gas and particle phases in the boreal forest in Finland in spring 2013 and 2014, detected with a chemical ionization mass spectrometer with a filter inlet for gases and aerosols employing acetate and iodide as reagent ions. These are among the first online dual-phase observations of such dimers in the atmosphere. Estimated saturation concentrations of 10 -15 to 10 -6 µg m -3 (based on observed thermal desorptions and group-contribution methods) and measured gas-phase concentrations of 10 -3 to 10 -2 µg m -3 (~10 6–10 7 molecules cm -3) corroborate a gas-phase formation mechanism. Regular new particle formation (NPF) events allowed insights into the potential role dimers may play for atmospheric NPF and growth. The observationally constrained Model for Acid-Base chemistry in NAnoparticle Growth indicates a contribution of ~5% to early stage particle growth from the ~60 gaseous dimer compounds.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3];  [3];  [4]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [6];  [3]; ORCiD logo [7]; ORCiD logo [6];  [8];  [9];  [6];  [6]; ORCiD logo [7]
  1. Karlsruhe Inst. of Technology (KIT) (Germany). Inst. of Meteorology and Climate Research; Univ. of Washington, Seattle, WA (United States). Dept.of Atmospheric Sciences
  2. Univ. of Washington, Seattle, WA (United States). Dept.of Atmospheric Sciences; Paul Scherrer Inst. (PSI), Villigen (Switzerland). Lab. of Atmospheric Chemistry
  3. Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics
  4. Univ. of Gothenburg (Sweden). Dept. of Chemistry and Molecular Biology
  5. Univ. of Washington, Seattle, WA (United States). Dept.of Chemistry
  6. Univ. of Helsinki (Finland). Dept. of Physics
  7. Univ. of Washington, Seattle, WA (United States). Dept.of Atmospheric Sciences
  8. Univ. of Helsinki (Finland). Dept. of Physics; Univ. of Colorado, Boulder, CO (United States). Dept. of Atmospheric and Oceanic Sciences
  9. Finnish Meteorological Inst. (FMI), Helsinki (Finland)
Publication Date:
Research Org.:
Univ. of Washington, Seattle, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1390598
Grant/Contract Number:
SC0011791
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Geophysical Research Letters
Additional Journal Information:
Journal Volume: 44; Journal Issue: 6; Journal ID: ISSN 0094-8276
Publisher:
American Geophysical Union
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; dimeric monoterpene oxidation dimers

Citation Formats

Mohr, Claudia, Lopez-Hilfiker, Felipe D., Yli-Juuti, Taina, Heitto, Arto, Lutz, Anna, Hallquist, Mattias, D'Ambro, Emma L., Rissanen, Matti P., Hao, Liqing, Schobesberger, Siegfried, Kulmala, Markku, Mauldin, Roy L., Makkonen, Ulla, Sipilä, Mikko, Petäjä, Tuukka, and Thornton, Joel A. Ambient observations of dimers from terpene oxidation in the gas phase: Implications for new particle formation and growth: Ambient Observations of Gas-Phase Dimers. United States: N. p., 2017. Web. doi:10.1002/2017GL072718.
Mohr, Claudia, Lopez-Hilfiker, Felipe D., Yli-Juuti, Taina, Heitto, Arto, Lutz, Anna, Hallquist, Mattias, D'Ambro, Emma L., Rissanen, Matti P., Hao, Liqing, Schobesberger, Siegfried, Kulmala, Markku, Mauldin, Roy L., Makkonen, Ulla, Sipilä, Mikko, Petäjä, Tuukka, & Thornton, Joel A. Ambient observations of dimers from terpene oxidation in the gas phase: Implications for new particle formation and growth: Ambient Observations of Gas-Phase Dimers. United States. doi:10.1002/2017GL072718.
Mohr, Claudia, Lopez-Hilfiker, Felipe D., Yli-Juuti, Taina, Heitto, Arto, Lutz, Anna, Hallquist, Mattias, D'Ambro, Emma L., Rissanen, Matti P., Hao, Liqing, Schobesberger, Siegfried, Kulmala, Markku, Mauldin, Roy L., Makkonen, Ulla, Sipilä, Mikko, Petäjä, Tuukka, and Thornton, Joel A. Tue . "Ambient observations of dimers from terpene oxidation in the gas phase: Implications for new particle formation and growth: Ambient Observations of Gas-Phase Dimers". United States. doi:10.1002/2017GL072718. https://www.osti.gov/servlets/purl/1390598.
@article{osti_1390598,
title = {Ambient observations of dimers from terpene oxidation in the gas phase: Implications for new particle formation and growth: Ambient Observations of Gas-Phase Dimers},
author = {Mohr, Claudia and Lopez-Hilfiker, Felipe D. and Yli-Juuti, Taina and Heitto, Arto and Lutz, Anna and Hallquist, Mattias and D'Ambro, Emma L. and Rissanen, Matti P. and Hao, Liqing and Schobesberger, Siegfried and Kulmala, Markku and Mauldin, Roy L. and Makkonen, Ulla and Sipilä, Mikko and Petäjä, Tuukka and Thornton, Joel A.},
abstractNote = {Here, we present ambient observations of dimeric monoterpene oxidation products (C16–20HyO6–9) in gas and particle phases in the boreal forest in Finland in spring 2013 and 2014, detected with a chemical ionization mass spectrometer with a filter inlet for gases and aerosols employing acetate and iodide as reagent ions. These are among the first online dual-phase observations of such dimers in the atmosphere. Estimated saturation concentrations of 10-15 to 10-6 µg m-3 (based on observed thermal desorptions and group-contribution methods) and measured gas-phase concentrations of 10-3 to 10-2 µg m-3 (~106–107 molecules cm-3) corroborate a gas-phase formation mechanism. Regular new particle formation (NPF) events allowed insights into the potential role dimers may play for atmospheric NPF and growth. The observationally constrained Model for Acid-Base chemistry in NAnoparticle Growth indicates a contribution of ~5% to early stage particle growth from the ~60 gaseous dimer compounds.},
doi = {10.1002/2017GL072718},
journal = {Geophysical Research Letters},
number = 6,
volume = 44,
place = {United States},
year = {Tue Mar 28 00:00:00 EDT 2017},
month = {Tue Mar 28 00:00:00 EDT 2017}
}

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