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Discussion papers | Copyright
https://doi.org/10.5194/acp-2018-538
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 09 Aug 2018

Research article | 09 Aug 2018

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This discussion paper is a preprint. It is a manuscript under review for the journal Atmospheric Chemistry and Physics (ACP).

Combined effects of boundary layer dynamics and atmospheric chemistry on aerosol composition during new particle formation periods

Liqing Hao1, Olga Garmash2, Mikael Ehn2, Pasi Miettinen1, Paola Massoli3, Santtu Mikkonen1, Tuija Jokinen2, Pontus Roldin4, Pasi Aalto2, Taina Yli-Juuti1, Jorma Joutsensaari1, Tuukka Petäjä2, Markku Kulmala2, Kari E. J. Lehtinen1,5, Douglas R. Worsnop1,2,3, and Annele Virtanen1 Liqing Hao et al.
  • 1Department of Applied Physics, University of Eastern Finland, Kuopio, Finland
  • 2Department of Physics, University of Helsinki, P.O. 64, Finland
  • 3Aerodyne Research Inc., Billerica, MA 08121-3976, USA
  • 4Division of Nuclear Physics, Department of Physics, Lund University, P. O. Box 118, SE-221 00, Lund, Sweden
  • 5Finnish Meteorological Institute, Kuopio, Finland

Abstract. Characterizing aerosol chemical composition in response to meteorological changes and atmospheric chemistry is important to gain insights into new particle formation mechanisms. A BAECC (Biogenic Aerosols-Effects on Clouds and Climate) campaign was conducted during the spring 2014 at SMEAR II station (Station for Measuring Forest Ecosystem-Aerosol Relations) in Finland. The particles were characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). A PBL (planetary boundary layer) dilution model was developed to assist interpreting the measurement results. Right before nucleation events, the mass concentrations of organic and sulfate aerosol species were both decreased rapidly along with the growth of PBL heights. However, the mass fraction of sulfate aerosol of the total aerosol mass was increased, in contrast to a decrease for the organic mass fraction. Meanwhile, an increase of LVOOA (low-volatility oxygenated organic aerosol) mass fraction of the total organic mass was observed, in distinct comparison to a reduction of SVOOA (semi-volatile OOA) mass fraction. Our results demonstrate that, at the beginning of nucleation events, the observed sulfate aerosol mass was mainly driven by vertical turbulent mixing of sulfate-rich aerosols between the residual layer and the newly formed boundary layer, while the condensation of sulfuric acid played a minor role in interpreting the measured sulfate mass concentration. For the measured organic aerosols, their temporal profiles were mainly driven by dilution from PBL development, organic aerosol mixing in different boundary layers and/or condensation of organic vapors, but accurate measurements of organic vapor concentrations and characterization on the spatial aerosol chemical composition are required. In general, the observed aerosol particles by AMS are subjected to joint effects of PBL dilution, atmospheric chemistry and aerosol mixing in different boundary layers. During aerosol growth periods in the night time, the mass concentrations of organic aerosols and organic nitrate aerosols were both increased. The increase of SVOOA mass correlated well with the calculated increase of condensed HOMs (highly oxygenated organic molecules) mass. To our knowledge, our results are the first atmospheric observations showing a connection between increase in SVOOA and condensed HOMs during the night time.

Liqing Hao et al.
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Short summary
An aerosol mass spectrometer was used to characterize aerosol chemical composition during new particle formation periods. The time profiles of mass concentrations and chemical composition of observed aerosol particles are subjected to joint effects of boundary layer dilution, atmospheric chemistry and aerosol mixing in different boundary layers. During the night time, the increase of organic aerosol mass correlated well with the increase of condensed highly oxygenated organic molecules mass.
An aerosol mass spectrometer was used to characterize aerosol chemical composition during new...
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