Articles | Volume 12, issue 16
Atmos. Chem. Phys., 12, 7517–7529, 2012
Atmos. Chem. Phys., 12, 7517–7529, 2012

Research article 17 Aug 2012

Research article | 17 Aug 2012

Humidity-dependent phase state of SOA particles from biogenic and anthropogenic precursors

E. Saukko1, A. T. Lambe2,3, P. Massoli3, T. Koop4, J. P. Wright2, D. R. Croasdale2, D. A. Pedernera4,*, T. B. Onasch2,3, A. Laaksonen5,6, P. Davidovits2, D. R. Worsnop3,7, and A. Virtanen1,6 E. Saukko et al.
  • 1Department of Physics, Tampere University of Technology, Tampere, Finland
  • 2Chemistry Department, Boston College, Chestnut Hill, MA, USA
  • 3Aerodyne Research Inc., Billerica, MA, USA
  • 4Faculty of Chemistry, Bielefeld University, Bielefeld, Germany
  • 5Finnish Meteorological Institute, Helsinki, Finland
  • 6Department of Applied Physics, University of Eastern Finland, Kuopio, Finland
  • 7Division of Atmospheric Sciences, Department of Physics, University of Helsinki, Helsinki, Finland
  • *now at: Faculty of Mathematics, Astronomy and Physics, National University of Córdoba, Córdoba, Argentina

Abstract. The physical phase state (solid, semi-solid, or liquid) of secondary organic aerosol (SOA) particles has important implications for a number of atmospheric processes. We report the phase state of SOA particles spanning a wide range of oxygen to carbon ratios (O / C), used here as a surrogate for SOA oxidation level, produced in a flow tube reactor by photo-oxidation of various atmospherically relevant surrogate anthropogenic and biogenic volatile organic compounds (VOCs). The phase state of laboratory-generated SOA was determined by the particle bounce behavior after inertial impaction on a polished steel substrate. The measured bounce fraction was evaluated as a function of relative humidity and SOA oxidation level (O / C) measured by an Aerodyne high resolution time of flight aerosol mass spectrometer (HR-ToF AMS).

The main findings of the study are: (1) biogenic and anthropogenic SOA particles are found to be amorphous solid or semi-solid based on the measured bounced fraction (BF), which was typically higher than 0.6 on a 0 to 1 scale. A decrease in the BF is observed for most systems after the SOA is exposed to relative humidity of at least 80% RH, corresponding to a RH at impaction of 55%. (2) Long-chain alkanes have a low BF (indicating a "liquid-like", less viscous phase) particles at low oxidation levels (BF < 0.2 ± 0.05 for O / C = 0.1). However, BF increases substantially upon increasing oxidation. (3) Increasing the concentration of sulphuric acid (H2SO4) in solid SOA particles (here tested for longifolene SOA) causes a decrease in BF levels. (4) In the majority of cases the bounce behavior of the various SOA systems did not show correlation with the particle O / C. Rather, the molar mass of the gas-phase VOC precursor showed a positive correlation with the resistance to the RH-induced phase change of the formed SOA particles.

Final-revised paper