Atmospheric sulphuric acid and neutral cluster measurements using CI-APi-TOF

被引：366

作者：

Jokinen, T. ^{[1
]}

Sipila, M. ^{[1
]}

Junninen, H. ^{[1
]}

Ehn, M. ^{[2
]}

Lonn, G. ^{[1
]}

Hakala, J. ^{[1
]}

Petaja, T. ^{[1
]}

Mauldin, R. L., III ^{[1
,3
]}

Kulmala, M. ^{[1
]}

Worsnop, D. R. ^{[1
,4
,5
,6
]}

机构：

[1] Univ Helsinki, Dept Phys, FIN-00014 Helsinki, Finland

[2] Forschungszentrum Julich, Inst Energy & Climate Res, D-52425 Julich, Germany

[3] Univ Colorado, Inst Arctic & Alpine Res, Boulder, CO 80309 USA

[4] Univ Eastern Finland, Kuopio 70211, Finland

[5] Finnish Meteorol Inst, Helsinki 00880, Finland

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

来源：

ATMOSPHERIC CHEMISTRY AND PHYSICS | 2012年 / 12卷 / 09期

基金：

欧洲研究理事会; 芬兰科学院;

关键词：

PRENUCLEATION MOLECULAR CLUSTERS; GALACTIC COSMIC-RAYS; PARTICLE FORMATION; NUCLEATION MECHANISMS; ELECTRICAL MOBILITY; H2SO4; SIZE; SPECTROMETER; MASS; AMMONIA;

D O I：

10.5194/acp-12-4117-2012

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

The first ambient measurements using nitrate ion based Chemical Ionization with the Atmospheric Pressure interface Time-Of-Flight mass spectrometer (CI-APi-TOF) for sulphuric acid and neutral cluster detection are presented. We have found CI-APi-TOF a highly stable and sensitive tool for molecular sulphuric acid detection. The lowest limit of detection for sulphuric acid was determined to be 3.6 x 10(4) molecules cm(-3) for 15 min averaging. Signals from sulphuric acid clusters up to tetramer containing ammonia were also obtained but these were found to result from naturally charged clusters formed by ion induced clustering in the atmosphere during nucleation. Opposite to earlier studies with cluster mass spectrometers, we had no indication of neutral clusters. The reason is either less efficient charging of clusters in comparison to molecular sulphuric acid, or the low concentration of neutral clusters at our measurement site during these particular nucleation events. We show that utilizing high resolution mass spectrometry is crucial in separating the weak sulfuric acid cluster signal from other compounds.

引用

页码：4117 / 4125

页数：9

共 31 条

[1] Physical characterization of aerosol particles during nucleation events [J].

Aalto, P ;

Hämeri, K ;

Becker, E ;

Weber, R ;

Salm, J ;

Mäkelä, JM ;

Hoell, C ;

O'Dowd, CD ;

Karlsson, H ;

Hansson, HC ;

Väkevä, M ;

Koponen, IK ;

Buzorius, G ;

Kulmala, M .

TELLUS SERIES B-CHEMICAL AND PHYSICAL METEOROLOGY, 2001, 53 (04) :344-358

[2] Results of the first air ion spectrometer calibration and intercomparison workshop [J].

Asmi, E. ;

Sipila, M. ;

Manninen, H. E. ;

Vanhanen, J. ;

Lehtipalo, K. ;

Gagne, S. ;

Neitola, K. ;

Mirme, A. ;

Mirme, S. ;

Tamm, E. ;

Uin, J. ;

Komsaare, K. ;

Attoui, M. ;

Kulmala, M. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (01) :141-154

[3] 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

[4] Laboratory study on new particle formation from the reaction OH + SO2: influence of experimental conditions, H2O vapour, NH3 and the amine tert-butylamine on the overall process [J].

Berndt, T. ;

Stratmann, F. ;

Sipilae, M. ;

Vanhanen, J. ;

Petaja, T. ;

Mikkila, J. ;

Gruener, A. ;

Spindler, G. ;

Mauldin, R. Lee, III ;

Curtius, J. ;

Kulmala, M. ;

Heintzenberg, J. .

ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (15) :7101-7116

[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] MEASUREMENT OF THE GAS-PHASE CONCENTRATION OF H2SO4 AND METHANE SULFONIC-ACID AND ESTIMATES OF H2SO4 PRODUCTION AND LOSS IN THE ATMOSPHERE [J].

EISELE, FL ;

TANNER, DJ .

JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 1993, 98 (D5) :9001-9010

[7] First measurement of prenucleation molecular clusters [J].

Eisele, FL ;

Hanson, DR .

JOURNAL OF PHYSICAL CHEMISTRY A, 2000, 104 (04) :830-836

[8] Measurement of the thermodynamics of the hydrated dimer and trimer of sulfuric acid [J].

Hanson, D. R. ;

Lovejoy, E. R. .

JOURNAL OF PHYSICAL CHEMISTRY A, 2006, 110 (31) :9525-9528

[9] Measurement of prenucleation molecular clusters in the NH3, H2SO4, H2O system -: art. no. 4158 [J].

Hanson, DR ;

Eisele, FL .

JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2002, 107 (D12)

[10] Effect of Working Fluid on Sub-2 nm Particle Detection with a Laminar Flow Ultrafine Condensation Particle Counter [J].

Iida, Kenjiro ;

Stolzenburg, Mark R. ;

McMurry, Peter H. .

AEROSOL SCIENCE AND TECHNOLOGY, 2009, 43 (01) :81-96

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