The role of VOC oxidation products in continental new particle formation

被引:144
作者
Laaksonen, A. [1 ]
Kulmala, M. [2 ]
O'Dowd, C. D. [3 ]
Joutsensaari, J. [1 ]
Vaattovaara, P. [1 ]
Mikkonen, S. [1 ]
Lehtinen, K. E. J. [1 ,4 ]
Sogacheva, L. [2 ]
Dal Maso, M. [2 ]
Aalto, P.
Petaja, T. [2 ]
Sogachev, A. [2 ]
Yoon, Y. J. [3 ]
Lihavainen, H. [4 ]
Nilsson, D. [5 ]
Facchini, M. C. [6 ]
Cavalli, F. [6 ]
Fuzzi, S. [6 ]
Hoffmann, T. [7 ]
Arnold, F. [8 ]
Hanke, M. [8 ]
Sellegri, K. [8 ]
Umann, B. [8 ]
Junkermann, W. [9 ]
Coe, H. [10 ]
Allan, J. D. [10 ]
Alfarra, M. R. [10 ]
Worsnop, D. R. [11 ]
Riekkola, M. -L. [12 ]
Hyotylainen, T. [12 ]
Viisanen, Y. [4 ]
机构
[1] Univ Kuopio, Dept Phys, FIN-70211 Kuopio, Finland
[2] Univ Helsinki, Dept Phys Sci, Helsinki, Finland
[3] Natl Univ Irelan, Dept Phys, Dublin, Ireland
[4] Finnish Meteorol Inst, FIN-00101 Helsinki, Finland
[5] Stockholm Univ, Dept Appl Environm Sci, Atmospher Sci Unit, S-10691 Stockholm, Sweden
[6] CNR, Ist Sci Atmosfera & Clima, I-40129 Bologna, Italy
[7] Johannes Gutenberg Univ Mainz, D-55128 Mainz, Germany
[8] Max Planck Inst Nucl Phys, D-69117 Heidelberg, Germany
[9] IMK IFU, Ins Meteorol & Climate Res, Forschungszentrum Karlsruhe, Garmisch Partenkirchen, Germany
[10] Univ Manchester, Sch Atmospher & Environm Sci, Manchester M60 1QD, Lancs, England
[11] Aerodyne Res Inc, Billerica, MA 01821 USA
[12] Univ Helsinki, Dept Chem, SF-00100 Helsinki, Finland
关键词
D O I
10.5194/acp-8-2657-2008
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Aerosol physical and chemical properties and trace gas concentrations were measured during the QUEST field campaign in March-April 2003, in Hyytiala, 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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收藏
页码:2657 / 2665
页数:9
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