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Ambient observations of dimers from terpene oxidation in the gas phase: Implications for new particle formation and growth

Journal article
Authors C. Mohr
F. D. Lopez-Hilfiker
T. Yli-Juuti
A. Heitto
Anna Lutz
Mattias Hallquist
E. L. D'Ambro
M. P. Rissanen
L. Q. Hao
S. Schobesberger
M. Kulmala
R. L. Mauldin
U. Makkonen
M. Sipila
T. Petaja
J. A. Thornton
Published in Geophysical Research Letters
Volume 44
Issue 6
Pages 2958-2966
ISSN 0094-8276
Publication year 2017
Published at Department of Chemistry and Molecular Biology
Pages 2958-2966
Language en
Links dx.doi.org/10.1002/2017GL072718
https://gup.ub.gu.se/file/206885
Keywords dimers, CIMS, new particle formation, monoterpene oxidation, boreal forest, SECONDARY ORGANIC AEROSOL, IONIZATION MASS-SPECTROMETRY, ALPHA-PINENE, OZONOLYSIS, OXIDIZED RO2 RADICALS, BOREAL-FOREST, VAPOR-PRESSURES, ATMOSPHERIC AEROSOLS, OLIGOMER FORMATION, SOUTHERN OXIDANT, PEROXY-RADICALS
Subject categories Climate Research, Organic Chemistry, Physical Chemistry, Analytical Chemistry, Chemical Sciences, Meteorology and Atmospheric Sciences, Geophysics

Abstract

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)mu gm(-3) (based on observed thermal desorptions and group-contribution methods) and measured gas-phase concentrations of 10(-3) to 10(-2)mu gm(-3) (similar to 10(6)-10(7)moleculescm(-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 similar to 5% to early stage particle growth from the similar to 60 gaseous dimer compounds. Plain Language Summary Atmospheric aerosol particles influence climate and air quality. We present new insights into how emissions of volatile organic compounds from trees are transformed in the atmosphere to contribute to the formation and growth of aerosol particles. We detected for the first time over a forest, a group of organic molecules, known to grow particles, in the gas phase at levels far higher than expected. Previous measurements had only measured them in the particles. This finding provides guidance on how models of aerosol formation and growth should describe their appearance and fate in the atmosphere.

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