Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere

被引：756

作者：

Almeida, Joao ^{[1
,2
]}

Schobesberger, Siegfried ^{[3
]}

Kuerten, Andreas ^{[1
]}

Ortega, Ismael K. ^{[3
]}

Kupiainen-Maatta, Oona ^{[3
]}

Praplan, Arnaud P. ^{[4
]}

Adamov, Alexey ^{[3
]}

Amorim, Antonio ^{[5
,6
]}

Bianchi, Federico ^{[4
]}

Breitenlechner, Martin ^{[7
,8
]}

David, Andre ^{[2
]}

Dommen, Josef ^{[4
]}

Donahue, Neil M. ^{[9
]}

Downard, Andrew ^{[10
]}

Dunne, Eimear ^{[11
]}

Duplissy, Jonathan ^{[3
]}

Ehrhart, Sebastian ^{[1
]}

Flagan, Richard C. ^{[10
]}

Franchin, Alessandro ^{[3
]}

Guida, Roberto ^{[2
]}

Hakala, Jani ^{[3
]}

Hansel, Armin ^{[7
,8
]}

Heinritzi, Martin ^{[7
,8
]}

Henschel, Henning ^{[3
]}

Jokinen, Tuija ^{[3
]}

Junninen, Heikki ^{[3
]}

Kajos, Maija ^{[3
]}

Kangasluoma, Juha ^{[3
]}

Keskinen, Helmi ^{[12
]}

Kupc, Agnieszka ^{[13
]}

Kurten, Theo ^{[14
]}

Kvashin, Alexander N. ^{[15
]}

Laaksonen, Ari ^{[12
,16
]}

Lehtipalo, Katrianne ^{[3
]}

Leiminger, Markus ^{[1
]}

Leppa, Johannes ^{[16
]}

Loukonen, Ville ^{[3
]}

Makhmutov, Vladimir ^{[15
]}

Mathot, Serge ^{[2
]}

McGrath, Matthew J. ^{[17
]}

Nieminen, Tuomo ^{[3
,18
]}

Olenius, Tinja ^{[3
]}

Onnela, Antti ^{[2
]}

Petaja, Tuukka ^{[3
]}

Riccobono, Francesco ^{[4
]}

Riipinen, Ilona ^{[19
]}

Rissanen, Matti ^{[3
]}

Rondo, Linda ^{[1
]}

Ruuskanen, Taina ^{[3
]}

Santos, Filipe D. ^{[5
,6
]}

机构：

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

[2] CERN, CH-1211 Geneva, Switzerland

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

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

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

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

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

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

[9] Carnegie Mellon Univ, Ctr Atmospher Particle Studies, Pittsburgh, PA 15213 USA

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

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

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

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

[14] Univ Helsinki, Dept Chem, FI-00014 Helsinki, Finland

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

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

[17] Kyoto Univ, Grad Sch Sci, Dept Biophys, Kyoto 6068502, Japan

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

[19] Univ Stockholm, Dept Appl Environm Sci, SE-10961 Stockholm, Sweden

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

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

来源：

NATURE | 2013年 / 502卷 / 7471期

基金：

俄罗斯基础研究基金会; 美国国家科学基金会; 瑞士国家科学基金会; 芬兰科学院; 瑞典研究理事会; 奥地利科学基金会;

关键词：

MASS-SPECTROMETER; FORMATION EVENTS; AEROSOL; DIMETHYLAMINE; AMMONIA; WATER;

D O I：

10.1038/nature12663

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：

Nucleation of aerosol particles from trace atmospheric vapours is thought to provide up to half of global cloud condensation nuclei(1). Aerosols can cause a net cooling of climate by scattering sunlight and by leading to smaller but more numerous cloud droplets, which makes clouds brighter and extends their lifetimes(2). Atmospheric aerosols derived from human activities are thought to have compensated for a large fraction of the warming caused by greenhouse gases(2). However, despite its importance for climate, atmospheric nucleation is poorly understood. Recently, it has been shown that sulphuric acid and ammonia cannot explain particle formation rates observed in the lower atmosphere(3). It is thought that amines may enhance nucleation(4-16), but until now there has been no direct evidence for amine ternary nucleation under atmospheric conditions. Here we use the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN and find that dimethylamine above three parts per trillion by volume can enhance particle formation rates more than 1,000-fold compared with ammonia, sufficient to account for the particle formation rates observed in the atmosphere. Molecular analysis of the clusters reveals that the faster nucleation is explained by a base-stabilization mechanism involving acid-amine pairs, which strongly decrease evaporation. The ion-induced contribution is generally small, reflecting the high stability of sulphuric acid-dimethylamine clusters and indicating that galactic cosmic rays exert only a small influence on their formation, except at low overall formation rates. Our experimental measurements are well reproduced by a dynamical model based on quantum chemical calculations of binding energies of molecular clusters, without any fitted parameters. These results show that, in regions of the atmosphere near amine sources, both amines and sulphur dioxide should be considered when assessing the impact of anthropogenic activities on particle formation.

引用

页码：359 / +

页数：11

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