Effect of ions on sulfuric acid-water binary particle formation: 2. Experimental data and comparison with QC-normalized classical nucleation theory

被引：82

作者：

Duplissy, J. ^{[1
,2
]}

Merikanto, J. ^{[3
]}

Franchin, A. ^{[2
]}

Tsagkogeorgas, G. ^{[4
]}

Kangasluoma, J. ^{[2
]}

Wimmer, D. ^{[2
,5
]}

Vuollekoski, H. ^{[2
]}

Schobesberger, S. ^{[2
,6
]}

Lehtipalo, K. ^{[2
]}

Flagan, R. C. ^{[7
]}

Brus, D. ^{[3
]}

Donahue, N. M. ^{[8
]}

Vehkamaki, H. ^{[2
]}

Almeida, J. ^{[5
,9
]}

Amorim, A. ^{[10
,11
]}

Barmet, P. ^{[12
,13
]}

Bianchi, F. ^{[12
,14
]}

Breitenlechner, M. ^{[15
]}

Dunne, E. M. ^{[16
,17
]}

Guida, R. ^{[9
]}

Henschel, H. ^{[2
]}

Junninen, H. ^{[2
]}

Kirkby, J. ^{[5
,9
]}

Kuerten, A. ^{[5
]}

Kupc, A. ^{[18
]}

Maattanen, A. ^{[19
,20
,21
]}

Makhmutov, V. ^{[22
]}

Mathot, S. ^{[9
]}

Nieminen, T. ^{[1
]}

Onnela, A. ^{[9
]}

Praplan, A. P. ^{[2
]}

Riccobono, F. ^{[12
]}

Rondo, L. ^{[5
]}

Steiner, G. ^{[2
,15
,18
]}

Tome, A. ^{[10
,11
]}

Walther, H. ^{[12
]}

Baltensperger, U. ^{[12
]}

Carslaw, K. S.

Dommen, J.

Hansel, A. ^{[15
,23
]}

Petaja, T. ^{[2
]}

Sipila, M. ^{[2
]}

Stratmann, F. ^{[4
]}

Vrtala, A. ^{[18
]}

Wagner, P. E. ^{[18
]}

Worsnop, D. R. ^{[2
,24
]}

Curtius, J. ^{[5
]}

Kulmala, M. ^{[2
]}

机构：

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

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

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

[4] Leibniz Inst Tropospher Res, Leipzig, Germany

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

[6] Univ Washington, Dept Atmospher Sci, Seattle, WA 98195 USA

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

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

[9] CERN, PH Dept, Geneva, Switzerland

[10] FCU Lisboa, CENTRA SIM, Covilha, Portugal

[11] U Beira Interior, Covilha, Portugal

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

[13] Canton Aargau, Dept Construct Traff & Environm, Canton, Switzerland

[14] ETH, Inst Atmospher & Climate Sci, Zurich, Switzerland

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

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

[17] Finnish Meteorol Inst, Atmospher Res Ctr Eastern Finland, Kuopio, Finland

[18] Univ Vienna, Aerosol Phys & Environm Phys, Vienna, Austria

[19] Univ Versailles St Quentin, Guyancourt, France

[20] Univ Paris 06, Sorbonne Univ, Guyancourt, France

[21] CNRS INSU, LATMOS IPSL, Guyancourt, France

[22] PN Lebedev Phys Inst, Solar & Cosm Ray Res Lab, Leninsky Prospect 53, Moscow 117924, Russia

[23] Ionicon Analyt GmbH, Innsbruck, Austria

[24] Aerodyne Res Inc, Billerica, MA USA

来源：

JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES | 2016年 / 121卷 / 04期

基金：

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

关键词：

binary particle formation; ion-induced nucleation; sulfuric acid; classical nucleation theory; IONIZATION MASS-SPECTROMETER; HOMOGENEOUS NUCLEATION; HYDRATE FORMATION; AEROSOL FORMATION; VAPOR-PRESSURE; OXIDATION-PRODUCTS; EXPERIMENTAL SETUP; H2SO4; PRODUCTION; MODE PARTICLES; GROWTH-RATES;

D O I：

10.1002/2015JD023539

中图分类号：

P4 [大气科学（气象学）];

学科分类号：

0706 ; 070601 ;

摘要：

We report comprehensive, demonstrably contaminant-free measurements of binary particle formation rates by sulfuric acid and water for neutral and ion-induced pathways conducted in the European Organization for Nuclear Research Cosmics Leaving Outdoor Droplets chamber. The recently developed Atmospheric Pressure interface-time of flight-mass spectrometer was used to detect contaminants in charged clusters and to identify runs free of any contaminants. Four parameters were varied to cover ambient conditions: sulfuric acid concentration (10(5) to 10(9)molcm(-3)), relative humidity (11% to 58%), temperature (207K to 299K), and total ion concentration (0 to 6800ionscm(-3)). Formation rates were directly measured with novel instruments at sizes close to the critical cluster size (mobility size of 1.3nm to 3.2nm). We compare our results with predictions from Classical Nucleation Theory normalized by Quantum Chemical calculation (QC-normalized CNT), which is described in a companion paper. The formation rates predicted by the QC-normalized CNT were extended from critical cluster sizes to measured sizes using the UHMA2 sectional particle microphysics model. Our results show, for the first time, good agreement between predicted and measured particle formation rates for the binary (neutral and ion-induced) sulfuric acid-water system. Formation rates increase with RH, sulfuric acid, and ion concentrations and decrease with temperature at fixed RH and sulfuric acid concentration. Under atmospheric conditions, neutral particle formation dominates at low temperatures, while ion-induced particle formation dominates at higher temperatures. The good agreement between the theory and our comprehensive data set gives confidence in using the QC-normalized CNT as a powerful tool to study neutral and ion-induced binary particle formation in atmospheric modeling.

引用

页码：1752 / 1775

页数：24

共 108 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] ON THE VAPOR-PRESSURE OF SULFURIC-ACID [J].

AYERS, GP ;

GILLETT, RW ;

GRAS, JL .

GEOPHYSICAL RESEARCH LETTERS, 1980, 7 (06) :433-436

[3] 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

[4] Ternary homogeneous nucleation of H2SO4, NH3, and H2O under conditions relevant to the lower troposphere [J].

Benson, D. R. ;

Yu, J. H. ;

Markovich, A. ;

Lee, S. -H. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2011, 11 (10) :4755-4766

[5] Laboratory-measured nucleation rates of sulfuric acid and water binary homogeneous nucleation from the SO2+OHreaction [J].

Benson, David R. ;

Young, Li-Hao ;

Kameel, F. Rifkha ;

Lee, Shan-Hu .

GEOPHYSICAL RESEARCH LETTERS, 2008, 35 (11)

[6] 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

[7] Enhancement of atmospheric H2SO4/H2O nucleation: organic oxidation products versus amines [J].

Berndt, T. ;

Sipila, M. ;

Stratmann, F. ;

Petaja, T. ;

Vanhanen, J. ;

Mikkila, J. ;

Patokoski, J. ;

Taipale, R. ;

Mauldin, R. L., III ;

Kulmala, M. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2014, 14 (02) :751-764

[8] Chemical ionization mass spectrometer for long-term measurements of atmospheric OH and H2SO4 [J].

Berresheim, H ;

Elste, T ;

Plass-Dülmer, C ;

Eisele, FL ;

Tanner, DJ .

INTERNATIONAL JOURNAL OF MASS SPECTROMETRY, 2000, 202 (1-3) :91-109

[9] On-line determination of ammonia at low pptv mixing ratios in the CLOUD chamber [J].

Bianchi, F. ;

Dommen, J. ;

Mathot, S. ;

Baltensperger, U. .

ATMOSPHERIC MEASUREMENT TECHNIQUES, 2012, 5 (07) :1719-1725

[10] Insight into Acid-Base Nucleation Experiments by Comparison of the Chemical Composition of Positive, Negative, and Neutral Clusters [J].

Bianchi, Federico ;

Praplan, Arnaud P. ;

Sarnela, Nina ;

Dommen, Josef ;

Kuerten, Andreas ;

Ortega, Ismael K. ;

Schobesberger, Siegfried ;

Junninen, Heikki ;

Simon, Mario ;

Troestl, Jasmin ;

Jokinen, Tuija ;

Sipila, Mikko ;

Adamov, Alexey ;

Amorim, Antonio ;

Almeida, Joao ;

Breitenlechner, Martin ;

Duplissy, Jonathan ;

Ehrhart, Sebastian ;

Flagan, Richard C. ;

Franchin, Alessandro ;

Hakala, Jani ;

Hansel, Armin ;

Heinritzi, Martin ;

Kangasluoma, Juha ;

Keskinen, Helmi ;

Kim, Jaeseok ;

Kirkby, Jasper ;

Laaksonen, Ari ;

Lawler, Michael J. ;

Lehtipalo, Katrianne ;

Leiminger, Markus ;

Makhmutov, Vladimir ;

Mathot, Serge ;

Onnela, Antti ;

Petaja, Tuukka ;

Riccobono, Francesco ;

Rissanen, Matti P. ;

Rondo, Linda ;

Tome, Antonio ;

Virtanen, Annele ;

Viisanen, Yrjo ;

Williamson, Christina ;

Wimmer, Daniela ;

Winkler, Paul M. ;

Ye, Penglin ;

Curtius, Joachim ;

Kulmala, Markku ;

Worsnop, Douglas R. ;

Donahue, Neil M. ;

Baltensperger, Urs .

ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2014, 48 (23) :13675-13684

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