Atmospheric Chemistry and Physics, vol. 11, issue 22 (2011) pp. 11477-11496
The evolution of secondary organic aerosols (SOA) during (photo-)chemical aging processes was investigated in a smog chamber. Fresh SOA from ozonolysis of 10 to 40 ppb alpha-pinene was formed followed by aging with OH radicals. The particles' volatility and hygroscopicity (expressed as volume fraction remaining (VFR) and hygroscopicity parameter kappa) were measured in parallel with a volatility and hygroscopicity tandem differential mobility analyzer (V/H-TDMA). An aerosol mass spectrometer (AMS) was used for the chemical characterization of the aerosol. These measurements were used as sensitive parameters to reveal the mechanisms possibly responsible for the changes in the SOA composition during aging. A change of VFR and/or kappa during processing of atmospheric aerosols may occur either by addition of SOA mass (by condensation) or by a change of SOA composition leading to different aerosol properties. The latter may occur either by heterogeneous reactions on the surface of the SOA particles, by condensed phase reactions like oligomerization or by an evaporation - gas-phase oxidation - recondensation cycle. The condensation mechanism showed to be dominant when there is a substantial change in the aerosol mass by addition of new molecules to the aerosol phase with time. Experiments could be divided into four periods based on the temporal evolution (qualitative changes) of VFR, kappa and organic mass: O-3 induced condensation, ripening, and OH induced chemical aging first with substantial mass gain and then without significant mass gain.
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