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The role of VOC oxidation products in continental new particle formation

Ari LaaksonenFinnish Meteorological Institute, POB 503, 00101 Helsinki, FinlandMarkku KulmalaUniversity of Helsinki, Department of Physical Sciences, Helsinki, FinlandColin O’DowdNational University of Ireland, Galway, Department of Physics, IrelandJorma JoutsensaariUniversity of Kuopio, Department of Physics, POB 1627, 70211 Kuopio, FinlandP. VaattovaaraUniversity of Kuopio, Department of Physics, POB 1627, 70211 Kuopio, FinlandSanttu MikkonenUniversity of Kuopio, Department of Physics, POB 1627, 70211 Kuopio, FinlandK. E. J. LehtinenFinnish Meteorological Institute, POB 503, 00101 Helsinki, FinlandLarisa SogachevaUniversity of Helsinki, Department of Physical Sciences, Helsinki, FinlandMiikka Dal MasoUniversity of Helsinki, Department of Physical Sciences, Helsinki, FinlandTuula AaltoUniversity of Helsinki, Department of Physical Sciences, Helsinki, FinlandTuukka PetäjäUniversity of Helsinki, Department of Physical Sciences, Helsinki, FinlandAndrey SogachevUniversity of Helsinki, Department of Physical Sciences, Helsinki, FinlandYoung Jun YoonNational University of Ireland, Galway, Department of Physics, IrelandHeikki LihavainenFinnish Meteorological Institute, POB 503, 00101 Helsinki, FinlandE. D. NilssonStockholm Univ., Dept. of Applied Environmental Science (ITM), Atmospheric Science Unit, 10691, Stockholm, SwedenM. C. FacchiniIstituto di Scienze dell'Atmosfera e del Clima – CNR, Italy Via Gobetti 101, 40 129 Bologna ,ItalyF. CavalliIstituto di Scienze dell'Atmosfera e del Clima – CNR, Italy Via Gobetti 101, 40 129 Bologna ,ItalyS. FuzziIstituto di Scienze dell'Atmosfera e del Clima – CNR, Italy Via Gobetti 101, 40 129 Bologna ,ItalyThorsten HoffmannJohannes Gutenberg-University of Mainz, 55128, Mainz, GermanyFrances H. ArnoldMax-Planck-Institute for Nuclear Physics, Heidelberg, GermanyM. HankeMax-Planck-Institute for Nuclear Physics, Heidelberg, GermanyKarine SellegriMax-Planck-Institute for Nuclear Physics, Heidelberg, GermanyB. UmannMax-Planck-Institute for Nuclear Physics, Heidelberg, GermanyW. JunkermannHugh CoeSchool of Atmospheric and Environmental Science, University of Manchester, PO Box 88, Manchester, M60 1QD, UKJ. D. AllanSchool of Atmospheric and Environmental Science, University of Manchester, PO Box 88, Manchester, M60 1QD, UKM. Rami AlfarraSchool of Atmospheric and Environmental Science, University of Manchester, PO Box 88, Manchester, M60 1QD, UKDouglas R. WorsnopAerodyne Research Inc., 45 Manning Road, Billerica, Ma 01821-3976, USAMarja‐Liisa RiekkolaUniversity of Helsinki, Department of Chemistry, Helsinki, FinlandTuulia HyötyläinenUniversity of Helsinki, Department of Chemistry, Helsinki, FinlandY. ViisanenFinnish Meteorological Institute, POB 503, 00101 Helsinki, Finland
2008en
ABI

Аннотация

Abstract. Aerosol physical and chemical properties and trace gas concentrations were measured during the QUEST field campaign in March–April 2003, in Hyytiälä, Finland. Our aim was to understand the role of oxidation products of VOC's such as mono- and sesquiterpenes in atmospheric nucleation events. Particle chemical compositions were measured using the Aerodyne Aerosol Mass Spectrometer, and chemical compositions of aerosol samples collected with low-pressure impactors and a high volume sampler were analysed using a number of techniques. The results indicate that during and after new particle formation, all particles larger than 50 nm in diameter contained similar organic substances that are likely to be mono- and sesquiterpene oxidation products. The oxidation products identified in the high volume samples were shown to be mostly aldehydes. In order to study the composition of particles in the 10–50 nm range, we made use of Tandem Differential Mobility Analyzer results. We found that during nucleation events, both 10 and 50 nm particle growth factors due to uptake of ethanol vapour correlate strongly with gas-phase monoterpene oxidation product (MTOP) concentrations, indicating that the organic constituents of particles smaller than 50 nm in diameter are at least partly similar to those of larger particles. We furthermore showed that particle growth rates during the nucleation events are correlated with the gas-phase MTOP concentrations. This indicates that VOC oxidation products may have a key role in determining the spatial and temporal features of the nucleation events. This conclusion was supported by our aircraft measurements of new 3–10 nm particle concentrations, which showed that the nucleation event on 28 March 2003, started at the ground layer, i.e. near the VOC source, and evolved together with the mixed layer. Furthermore, no new particle formation was detected upwind away from the forest, above the frozen Gulf of Bothnia.

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