1Department of Chemistry, University of York, Heslington, York, YO10 5DD, UK
2National Centre for Atmospheric Science (NCAS), School of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, M13 9PL, UK
3Centre for Atmospheric Science, School of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester, M13 9PL, UK
4Atmospheric Chemistry Group, Department of Chemistry, University of Leicester, Leicester, LE1 7RH, UK
*now at: Laboratoire de Météorologie Physique, Blaise Pascal Univ., Clermont-Ferrand, 63000, France
Received: 13 Oct 2010 – Discussion started: 27 Oct 2010
Abstract. The use of β-caryophyllene secondary organic aerosol particles as seeds for smog chamber simulations has been investigated. A series of experiments were carried out in the Manchester photochemical chamber as part of the Aerosol Coupling in the Earth System (ACES) project to study the effect of seed particles on the formation of secondary organic aerosol (SOA) from limonene photo-oxidation. Rather than use a conventional seed aerosol containing ammonium sulfate or diesel particles, a method was developed to use in-situ chamber generated seed particles from β-caryophyllene photo-oxidation, which were then diluted to a desired mass loading (in this case 4–13 μg m−3). Limonene was then introduced into the chamber and oxidised, with the formation of SOA seen as a growth in the size of oxidised organic seed particles from 150 to 325 nm mean diameter. The effect of the partitioning of limonene oxidation products onto the seed aerosol was assessed using aerosol mass spectrometry during the experiment and the percentage of m/z 44, an indicator of degree of oxidation, increased from around 5 to 8 %. The hygroscopicity of the aerosol also changed, with the growth factor for 200 nm particles increasing from less than 1.05 to 1.25 at 90 % RH. The detailed chemical composition of the limonene SOA could be extracted from the complex β-caryophyllene matrix using two-dimensional gas chromatography (GC × GC) and liquid chromatography coupled to mass spectrometry. High resolution Fourier Transform Ion Cyclotron Resonance Mass Spectrometry (FTICR-MS) was used to determine exact molecular formulae of the seed and the limonene modified aerosol. The average O:C ratio was seen to increase from 0.32 to 0.37 after limonene oxidation products had condensed onto the organic seed.
Revised: 28 Mar 2011 – Accepted: 18 Apr 2011 – Published: 23 Jun 2011
Hamilton, J. F., Rami Alfarra, M., Wyche, K. P., Ward, M. W., Lewis, A. C., McFiggans, G. B., Good, N., Monks, P. S., Carr, T., White, I. R., and Purvis, R. M.: Investigating the use of secondary organic aerosol as seed particles in simulation chamber experiments, Atmos. Chem. Phys., 11, 5917-5929, doi:10.5194/acp-11-5917-2011, 2011.