Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation

被引：988

作者：

Kirkby, Jasper ^{[7
]}

Curtius, Joachim ^{[1
]}

Almeida, Joao ^{[1
,2
,3
]}

Dunne, Eimear ^{[4
]}

Duplissy, Jonathan ^{[5
,6
,7
]}

Ehrhart, Sebastian ^{[1
]}

Franchin, Alessandro ^{[5
]}

Gagne, Stephanie ^{[5
,6
]}

Ickes, Luisa ^{[1
]}

Kuerten, Andreas ^{[1
]}

Kupc, Agnieszka ^{[8
]}

Metzger, Axel ^{[9
,10
]}

Riccobono, Francesco ^{[11
]}

Rondo, Linda ^{[1
]}

Schobesberger, Siegfried ^{[5
]}

Tsagkogeorgas, Georgios ^{[12
]}

Wimmer, Daniela ^{[1
]}

Amorim, Antonio ^{[2
,3
]}

Bianchi, Federico ^{[11
,13
]}

Breitenlechner, Martin ^{[9
,10
]}

David, Andre ^{[7
]}

Dommen, Josef ^{[11
]}

Downard, Andrew ^{[14
]}

Ehn, Mikael ^{[5
]}

Flagan, Richard C. ^{[14
]}

Haider, Stefan ^{[7
]}

Hansel, Armin ^{[9
,10
]}

Hauser, Daniel ^{[9
,10
]}

Jud, Werner ^{[9
,10
]}

Junninen, Heikki ^{[5
]}

Kreissl, Fabian ^{[1
]}

Kvashin, Alexander ^{[15
]}

Laaksonen, Ari ^{[16
]}

Lehtipalo, Katrianne ^{[5
]}

Lima, Jorge ^{[2
,3
]}

Lovejoy, Edward R. ^{[17
]}

Makhmutov, Vladimir ^{[15
]}

Mathot, Serge ^{[7
]}

Mikkila, Jyri ^{[5
]}

Minginette, Pierre ^{[7
]}

Mogo, Sandra ^{[2
,3
]}

Nieminen, Tuomo ^{[5
]}

Onnela, Antti ^{[7
]}

Pereira, Paulo ^{[2
,3
]}

Petaja, Tuukka ^{[5
]}

Schnitzhofer, Ralf ^{[9
,10
]}

Seinfeld, John H. ^{[14
]}

Sipila, Mikko ^{[5
,6
]}

Stozhkov, Yuri ^{[15
]}

Stratmann, Frank ^{[12
]}

机构：

[1] Goethe Univ Frankfurt, Inst Atmospher & Environm Sci, D-60438 Frankfurt, Germany

[2] Univ Lisbon, SIM, P-1749016 Lisbon, Portugal

[3] Univ Beira Interior, P-1749016 Lisbon, Portugal

[4] Univ Leeds, Sch Earth & Environm, Leeds LS2 9JT, W Yorkshire, England

[5] Univ Helsinki, Dept Phys, FI-00014 Helsinki, Finland

[6] Univ Helsinki, Helsinki Inst Phys, FI-00014 Helsinki, Finland

[7] CERN, CH-1211 Geneva, Switzerland

[8] Univ Vienna, Fac Phys, A-1090 Vienna, Austria

[9] Univ Innsbruck, Inst Ion & Appl Phys, A-6020 Innsbruck, Austria

[10] Ionicon Analyt GmbH, A-6020 Innsbruck, Austria

[11] Paul Scherrer Inst, Lab Atmospher Chem, CH-5232 Villigen, Switzerland

[12] Leibniz Inst Tropospher Res, D-04318 Leipzig, Germany

[13] Univ Milan, Dept Inorgan Metallorgan & Analyt Chem, I-20133 Milan, Italy

[14] CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA

[15] PN Lebedev Phys Inst, Solar & Cosm Ray Res Lab, Moscow 119991, Russia

[16] Univ Eastern Finland, FI-70211 Kuopio, Finland

[17] NOAA, Earth Syst Res Lab, Boulder, CO 80305 USA

[18] Finnish Meteorol Inst, FI-00101 Helsinki, Finland

[19] Aerodyne Res Inc, Billerica, MA 01821 USA

来源：

NATURE | 2011年 / 476卷 / 7361期

基金：

芬兰科学院; 奥地利科学基金会; 瑞士国家科学基金会; 俄罗斯基础研究基金会;

关键词：

ION-INDUCED NUCLEATION; PARTICLE FORMATION; MASS-SPECTROMETER; UPPER TROPOSPHERE; NANOPARTICLES; H2SO4; WATER; H2O;

D O I：

10.1038/nature10343

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Atmospheric aerosols exert an important influence on climate(1) through their effects on stratiform cloud albedo and lifetime(2) and the invigoration of convective storms(3). Model calculations suggest that almost half of the global cloud condensation nuclei in the atmospheric boundary layer may originate from the nucleation of aerosols from trace condensable vapours(4), although the sensitivity of the number of cloud condensation nuclei to changes of nucleation rate may be small(5,6). Despite extensive research, fundamental questions remain about the nucleation rate of sulphuric acid particles and the mechanisms responsible, including the roles of galactic cosmic rays and other chemical species such as ammonia(7). Here we present the first results from the CLOUD experiment at CERN. We find that atmospherically relevant ammonia mixing ratios of 100 parts per trillion by volume, or less, increase the nucleation rate of sulphuric acid particles more than 100-1,000-fold. Time-resolved molecular measurements reveal that nucleation proceeds by a base-stabilization mechanism involving the stepwise accretion of ammonia molecules. Ions increase the nucleation rate by an additional factor of between two and more than ten at ground-level galactic-cosmic-ray intensities, provided that the nucleation rate lies below the limiting ion-pair production rate. We find that ion-induced binary nucleation of H2SO4-H2O can occur in the midtroposphere but is negligible in the boundary layer. However, even with the large enhancements in rate due to ammonia and ions, atmospheric concentrations of ammonia and sulphuric acid are insufficient to account for observed boundary-layer nucleation.

引用

页码：429 / U77

页数：7

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