Atmospheric sulphuric acid and aerosol formation:: implications from atmospheric measurements for nucleation and early growth mechanisms

被引:327
作者
Sihto, S. -L.
Kulmala, M.
Kerminen, V. -M.
Dal Maso, M.
Petaja, T.
Riipinen, I.
Korhonen, H.
Arnold, F.
Janson, R.
Boy, M.
Laaksonen, A.
Lehtinen, K. E. J.
机构
[1] Univ Helsinki, Dept Phys Sci, FIN-00014 Helsinki, Finland
[2] Finnish Meteorol Inst, FIN-00101 Helsinki, Finland
[3] MPIK, Atmospher Phys Div, D-69029 Heidelberg, Germany
[4] Univ Stockholm, Dept Appl Environm Sci, Air Pollut Lab, S-10691 Stockholm, Sweden
[5] Univ Kuopio, Dept Appl Phys, FIN-70211 Kuopio, Finland
[6] Finnish Meteorol Inst, Kuopio 70211, Finland
[7] Univ Kuopio, Dept Appl Phys, Kuopio 70211, Finland
关键词
D O I
10.5194/acp-6-4079-2006
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
We have investigated the formation and early growth of atmospheric secondary aerosol particles building on atmospheric measurements. The measurements were part of the QUEST 2 campaign which took place in spring 2003 in Hyytiala ( Finland). During the campaign numerous aerosol particle formation events occurred of which 15 were accompanied by gaseous sulphuric acid measurements. Our detailed analysis of these 15 events is focussed on nucleation and early growth ( to a diameter of 3 nm) of fresh particles. It revealed that new particle formation seems to be a function of the gaseous sulphuric acid concentration to the power from one to two when the time delay between the sulphuric acid and particle number concentration is taken into account. From the time delay the growth rates of freshly nucleated particles from 1 nm to 3 nm were determined. The mean growth rate was 1.2 nm/h and it was clearly correlated with the gaseous sulphuric acid concentration. We tested two nucleation mechanisms - recently proposed cluster activation and kinetic type nucleation - as possible candidates to explain the observed dependences, and determined experimental nucleation coefficients. We found that some events are dominated by the activation mechanism and some by the kinetic mechanism. Inferred coefficients for the two nucleation mechanisms are the same order of magnitude as chemical reaction coefficients in the gas phase and they correlate with the product of gaseous sulphuric acid and ammonia concentrations. This indicates that besides gaseous sulphuric acid also ammonia has a role in nucleation.
引用
收藏
页码:4079 / 4091
页数:13
相关论文
共 47 条
[1]   Rapid formation of sulfuric acid particles at near-atmospheric conditions [J].
Berndt, T ;
Böge, O ;
Stratmann, F ;
Heintzenberg, J ;
Kulmala, M .
SCIENCE, 2005, 307 (5710) :698-700
[2]   The Hohenpeissenberg aerosol formation experiment (HAFEX):: a long-term study including size-resolved aerosol, H2SO4, OH, and monoterpenes measurements [J].
Birmili, W ;
Berresheim, H ;
Plass-Dülmer, C ;
Elste, T ;
Gilge, S ;
Wiedensohler, A ;
Uhrner, U .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2003, 3 :361-376
[3]  
Birmili W, 1998, J AEROSOL SCI, V29, pS1015, DOI DOI 10.1016/S0021-8502(98)90690-5
[4]   Sulphuric acid closure and contribution to nucleation mode particle growth [J].
Boy, M ;
Kulmala, M ;
Ruuskanen, TM ;
Pihlatie, M ;
Reissell, A ;
Aalto, PP ;
Keronen, P ;
Dal Maso, M ;
Hellen, H ;
Hakola, H ;
Jansson, R ;
Hanke, M ;
Arnold, F .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2005, 5 :863-878
[5]   Light scattering by fine particles during the Pittsburgh Air Quality Study: measurements and modeling [J].
Cabada, JC ;
Khlystov, A ;
Wittig, AE ;
Pilinis, C ;
Pandis, SN .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2004, 109 (D16) :D16S031-13
[6]  
Dal Maso M, 2005, BOREAL ENVIRON RES, V10, P323
[7]   Ultrafine (nanometre) particle mediated lung injury [J].
Donaldson, K ;
Li, XY ;
MacNee, W .
JOURNAL OF AEROSOL SCIENCE, 1998, 29 (5-6) :553-560
[8]   Measurements of Mexico City nanoparticle size distributions:: Observations of new particle formation and growth -: art. no. L10102 [J].
Dunn, MJ ;
Jiménez, JL ;
Baumgardner, D ;
Castro, T ;
McMurry, PH ;
Smith, JN .
GEOPHYSICAL RESEARCH LETTERS, 2004, 31 (10) :L101021-4
[9]   The contribution of sulphuric acid to atmospheric particle formation and growth: a comparison between boundary layers in Northern and Central Europe [J].
Fiedler, V ;
Dal Maso, M ;
Boy, M ;
Aufmhoff, H ;
Hoffmann, J ;
Schuck, T ;
Birmili, W ;
Hanke, M ;
Uecker, J ;
Arnold, F ;
Kulmala, M .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2005, 5 :1773-1785
[10]   Atmospheric peroxy radicals:: ROXMAS, a new mass-spectrometric methodology for speciated measurements of HO2 and ΣRO2 and first results [J].
Hanke, M ;
Uecker, J ;
Reiner, T ;
Arnold, F .
INTERNATIONAL JOURNAL OF MASS SPECTROMETRY, 2002, 213 (2-3) :91-99