Oxidation Products of Biogenic Emissions Contribute to Nucleation of Atmospheric Particles

被引：422

作者：

Riccobono, Francesco ^{[1
]}

Schobesberger, Siegfried ^{[2
]}

Scott, Catherine E. ^{[3
]}

Dommen, Josef ^{[1
]}

Ortega, Ismael K. ^{[2
]}

Rondo, Linda ^{[4
]}

Almeida, Joao ^{[4
]}

Amorim, Antonio ^{[5
,6
]}

Bianchi, Federico ^{[1
]}

Breitenlechner, Martin ^{[7
,8
]}

David, Andre ^{[9
]}

Downard, Andrew ^{[10
]}

Dunne, Eimear M. ^{[3
]}

Duplissy, Jonathan ^{[2
,14
]}

Ehrhart, Sebastian ^{[4
]}

Flagan, Richard C. ^{[10
]}

Franchin, Alessandro ^{[2
]}

Hansel, Armin ^{[7
,8
]}

Junninen, Heikki ^{[2
]}

Kajos, Maija ^{[2
]}

Keskinen, Helmi ^{[11
]}

Kupc, Agnieszka ^{[12
]}

Kuerten, Andreas ^{[4
]}

Kvashin, Alexander N. ^{[13
]}

Laaksonen, Ari ^{[11
]}

Lehtipalo, Katrianne ^{[2
]}

Makhmutov, Vladimir ^{[13
]}

Mathot, Serge ^{[9
]}

Nieminen, Tuomo ^{[2
,14
]}

Onnela, Antti ^{[9
]}

Petaja, Tuukka ^{[2
]}

Praplan, Arnaud P. ^{[1
]}

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

Schallhart, Simon ^{[2
]}

Seinfeld, John H. ^{[10
]}

Sipila, Mikko ^{[2
,14
]}

Spracklen, Dominick V. ^{[3
]}

Stozhkov, Yuri ^{[13
]}

Stratmann, Frank ^{[15
]}

Tome, Antonio ^{[5
,6
]}

Tsagkogeorgas, Georgios ^{[15
]}

Vaattovaara, Petri ^{[11
]}

Viisanen, Yrjo ^{[16
]}

Vrtala, Aron ^{[12
]}

Wagner, Paul E. ^{[12
]}

Weingartner, Ernest ^{[1
]}

Wex, Heike ^{[15
]}

Wimmer, Daniela ^{[4
]}

Carslaw, Kenneth S. ^{[3
]}

Curtius, Joachim ^{[4
]}

机构：

[1] Paul Scherrer Inst, Lab Atmospher Chem, Villigen, Switzerland

[2] Univ Helsinki, Dept Phys, Helsinki, Finland

[3] Univ Leeds, Sch Earth & Environm, Leeds, W Yorkshire, England

[4] Goethe Univ Frankfurt, Inst Atmospher & Environm Sci, D-60054 Frankfurt, Germany

[5] Univ Lisbon, Lab Syst Instrumentat & Modeling Sci & Technol Sp, P-1699 Lisbon, Portugal

[6] Univ Beira Interior, Lisbon, Portugal

[7] Ionicon Analyt GmbH, Innsbruck, Austria

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

[9] CERN European Org Nucl Res, Geneva, Switzerland

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

[11] Univ Eastern Finland, Kuopio, Finland

[12] Univ Vienna, Fac Phys, Vienna, Austria

[13] PN Lebedev Phys Inst, Solar & Cosm Ray Res Lab, Moscow 117924, Russia

[14] Univ Helsinki, Helsinki Inst Phys, Helsinki, Finland

[15] Leibniz Inst Tropospher Res, Leipzig, Germany

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

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

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

来源：

SCIENCE | 2014年 / 344卷 / 6185期

基金：

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

关键词：

SULFURIC-ACID; AEROSOL MICROPHYSICS; ORGANIC-COMPOUNDS; GROWTH-RATES; GLOBAL-MODEL; H2SO4; SIZE; NANOPARTICLES; UNCERTAINTY; MAGNITUDE;

D O I：

10.1126/science.1243527

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 new-particle formation affects climate and is one of the least understood atmospheric aerosol processes. The complexity and variability of the atmosphere has hindered elucidation of the fundamental mechanism of new-particle formation from gaseous precursors. We show, in experiments performed with the CLOUD (Cosmics Leaving Outdoor Droplets) chamber at CERN, that sulfuric acid and oxidized organic vapors at atmospheric concentrations reproduce particle nucleation rates observed in the lower atmosphere. The experiments reveal a nucleation mechanism involving the formation of clusters containing sulfuric acid and oxidized organic molecules from the very first step. Inclusion of this mechanism in a global aerosol model yields a photochemically and biologically driven seasonal cycle of particle concentrations in the continental boundary layer, in good agreement with observations.

引用

页码：717 / 721

页数：5

共 39 条

[1] Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere [J].

Almeida, Joao ;

Schobesberger, Siegfried ;

Kuerten, Andreas ;

Ortega, Ismael K. ;

Kupiainen-Maatta, Oona ;

Praplan, Arnaud P. ;

Adamov, Alexey ;

Amorim, Antonio ;

Bianchi, Federico ;

Breitenlechner, Martin ;

David, Andre ;

Dommen, Josef ;

Donahue, Neil M. ;

Downard, Andrew ;

Dunne, Eimear ;

Duplissy, Jonathan ;

Ehrhart, Sebastian ;

Flagan, Richard C. ;

Franchin, Alessandro ;

Guida, Roberto ;

Hakala, Jani ;

Hansel, Armin ;

Heinritzi, Martin ;

Henschel, Henning ;

Jokinen, Tuija ;

Junninen, Heikki ;

Kajos, Maija ;

Kangasluoma, Juha ;

Keskinen, Helmi ;

Kupc, Agnieszka ;

Kurten, Theo ;

Kvashin, Alexander N. ;

Laaksonen, Ari ;

Lehtipalo, Katrianne ;

Leiminger, Markus ;

Leppa, Johannes ;

Loukonen, Ville ;

Makhmutov, Vladimir ;

Mathot, Serge ;

McGrath, Matthew J. ;

Nieminen, Tuomo ;

Olenius, Tinja ;

Onnela, Antti ;

Petaja, Tuukka ;

Riccobono, Francesco ;

Riipinen, Ilona ;

Rissanen, Matti ;

Rondo, Linda ;

Ruuskanen, Taina ;

Santos, Filipe D. .

NATURE, 2013, 502 (7471) :359-+

[2] Laboratory studies of particle nucleation:: Initial results for H2SO4, H2O, and NH3 vapors [J].

Ball, SM ;

Hanson, DR ;

Eisele, FL ;

McMurry, PH .

JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1999, 104 (D19) :23709-23718

[3] The magnitude and sources of uncertainty in global aerosol [J].

Carslaw, Kenneth S. ;

Lee, Lindsay A. ;

Reddington, Carly L. ;

Mann, Graham W. ;

Pringle, Kirsty J. .

FARADAY DISCUSSIONS, 2013, 165 :495-512

[4] Acid-base chemical reaction model for nucleation rates in the polluted atmospheric boundary layer [J].

Chen, Modi ;

Titcombe, Mari ;

Jiang, Jingkun ;

Jen, Coty ;

Kuang, Chongai ;

Fischer, Marc L. ;

Eisele, Fred L. ;

Siepmann, J. Ilja ;

Hanson, David R. ;

Zhao, Jun ;

McMurry, Peter H. .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2012, 109 (46) :18713-18718

[5] Composition and temporal behavior of ambient ions in the boreal forest [J].

Ehn, M. ;

Junninen, H. ;

Petaja, T. ;

Kurten, T. ;

Kerminen, V. -M. ;

Schobesberger, S. ;

Manninen, H. E. ;

Ortega, I. K. ;

Vehkamaki, H. ;

Kulmala, M. ;

Worsnop, D. R. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (17) :8513-8530

[6] Influence of aerosol lifetime on the interpretation of nucleation experiments with respect to the first nucleation theorem [J].

Ehrhart, S. ;

Curtius, J. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2013, 13 (22) :11465-11471

[7] Negative atmospheric ions and their potential role in ion-induced nucleation [J].

Eisele, FL ;

Lovejoy, ER ;

Kosciuch, E ;

Moore, KF ;

Mauldin, RL ;

Smith, JN ;

McMurry, PH ;

Iida, K .

JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2006, 111 (D4)

[8] A GLOBAL-MODEL OF NATURAL VOLATILE ORGANIC-COMPOUND EMISSIONS [J].

GUENTHER, A ;

HEWITT, CN ;

ERICKSON, D ;

FALL, R ;

GERON, C ;

GRAEDEL, T ;

HARLEY, P ;

KLINGER, L ;

LERDAU, M ;

MCKAY, WA ;

PIERCE, T ;

SCHOLES, B ;

STEINBRECHER, R ;

TALLAMRAJU, R ;

TAYLOR, J ;

ZIMMERMAN, P .

JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1995, 100 (D5) :8873-8892

[9] In situ measurements of volatile organic compounds in a boreal forest [J].

Hakola, H. ;

Hellen, H. ;

Hemmila, M. ;

Rinne, J. ;

Kulmala, M. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2012, 12 (23) :11665-11678

[10] Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation [J].

Kirkby, Jasper ;

Curtius, Joachim ;

Almeida, Joao ;

Dunne, Eimear ;

Duplissy, Jonathan ;

Ehrhart, Sebastian ;

Franchin, Alessandro ;

Gagne, Stephanie ;

Ickes, Luisa ;

Kuerten, Andreas ;

Kupc, Agnieszka ;

Metzger, Axel ;

Riccobono, Francesco ;

Rondo, Linda ;

Schobesberger, Siegfried ;

Tsagkogeorgas, Georgios ;

Wimmer, Daniela ;

Amorim, Antonio ;

Bianchi, Federico ;

Breitenlechner, Martin ;

David, Andre ;

Dommen, Josef ;

Downard, Andrew ;

Ehn, Mikael ;

Flagan, Richard C. ;

Haider, Stefan ;

Hansel, Armin ;

Hauser, Daniel ;

Jud, Werner ;

Junninen, Heikki ;

Kreissl, Fabian ;

Kvashin, Alexander ;

Laaksonen, Ari ;

Lehtipalo, Katrianne ;

Lima, Jorge ;

Lovejoy, Edward R. ;

Makhmutov, Vladimir ;

Mathot, Serge ;

Mikkila, Jyri ;

Minginette, Pierre ;

Mogo, Sandra ;

Nieminen, Tuomo ;

Onnela, Antti ;

Pereira, Paulo ;

Petaja, Tuukka ;

Schnitzhofer, Ralf ;

Seinfeld, John H. ;

Sipila, Mikko ;

Stozhkov, Yuri ;

Stratmann, Frank .

NATURE, 2011, 476 (7361) :429-U77

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