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

Claudia Mohr, Felipe D. Lopez-Hilfiker, Taina Yli-Juuti, Arto Heitto, Anna Lutz, Mattias Hallquist, Emma L. D'Ambro, Matti P. Rissanen, Liqing Hao, Siegfried Schobesberger, Markku Kulmala, Roy L. Mauldin III, Ulla Makkonen, Mikko Sipilä, Tuukka Petäjä, Joel A. Thornton

Research output: Contribution to journalArticleScientificpeer-review

80 Citations (Scopus)

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 50 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.
Original languageEnglish
Pages (from-to)2958-2966
Number of pages9
JournalGeophysical Research Letters
Volume44
Issue number6
DOIs
Publication statusPublished - 1 Mar 2017
Publication typeA1 Journal article-refereed

Keywords

  • 114 Physical sciences
  • PEROXY-RADICALS
  • SECONDARY ORGANIC AEROSOL
  • OLIGOMER FORMATION
  • 1172 Environmental sciences
  • dimers
  • VAPOR-PRESSURES
  • boreal forest
  • new particle formation
  • IONIZATION MASS-SPECTROMETRY
  • BOREAL-FOREST
  • ALPHA-PINENE OZONOLYSIS
  • ATMOSPHERIC AEROSOLS
  • CIMS
  • monoterpene oxidation
  • OXIDIZED RO2 RADICALS
  • SOUTHERN OXIDANT

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