Aerosol hygroscopicity and CCN activation kinetics in a boreal forest environment during the 2007 EUCAARI campaign

被引:79
作者
Cerully, K. M. [1 ]
Raatikainen, T. [2 ,3 ]
Lance, S. [4 ,5 ]
Tkacik, D. [6 ]
Tiitta, P. [7 ,8 ]
Petaja, T. [9 ]
Ehn, M. [9 ]
Kulmala, M. [9 ]
Worsnop, D. R. [3 ,7 ,9 ,10 ]
Laaksonen, A. [3 ,7 ]
Smith, J. N. [7 ]
Nenes, A. [1 ,2 ,11 ]
机构
[1] Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA
[2] Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA
[3] Finnish Meteorol Inst, FIN-00101 Helsinki, Finland
[4] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA
[5] NOAA, Earth Syst Res Lab, Boulder, CO USA
[6] Carnegie Mellon Univ, Ctr Atmospher Particle Studies, Pittsburgh, PA 15213 USA
[7] Univ Eastern Finland, Dept Appl Phys, Kuopio, Finland
[8] North West Univ, Atmospher Chem Res Grp, Potchefstroom, South Africa
[9] Univ Helsinki, Dept Phys, Helsinki, Finland
[10] Aerodyne Res Inc, Billerica, MA 01821 USA
[11] Fdn Res & Technol Hellas, Inst Chem Engn & High Temp Chem Proc, Patras, Greece
基金
芬兰科学院;
关键词
CLOUD CONDENSATION NUCLEI; SIZE-RESOLVED MEASUREMENTS; DROPLET GROWTH-KINETICS; MASS-SPECTROMETER; ORGANIC AEROSOL; SINGLE-COMPONENT; PARTICLE GROWTH; SULFURIC-ACID; DISTRIBUTIONS; NUCLEATION;
D O I
10.5194/acp-11-12369-2011
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Measurements of size-resolved cloud condensation nuclei (CCN) concentrations, subsaturated hygroscopic growth, size distribution, and chemical composition were collected from March through May, 2007, in the remote Boreal forests of Hyytiala, Finland, as part of the European Integrated project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) campaign. Hygroscopicity parameter, kappa, distributions were derived independently from Continuous Flow-Streamwise Thermal Gradient CCN Chamber (CFSTGC) and Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) measurements. CFSTGC-derived kappa values for 40, 60, and 80 nm particles range mostly between 0.10 and 0.40 with an average characteristic of highly oxidized organics of 0.20 +/- 0.10, indicating that organics play a dominant role for this environment. HTDMA-derived kappa were generally 30% lower. Diurnal trends of kappa show a minimum at sunrise and a maximum in the late afternoon; this trend covaries with inorganic mass fraction and the m/z 44 organic mass fraction given by a quadrupole aerosol mass spectrometer, further illustrating the importance of organics in aerosol hygroscopicity. The chemical dispersion inferred from the observed kappa distributions indicates that while 60 and 80 nm dispersion increases around midday, 40 nm dispersion remains constant. Additionally, 80 nm particles show a markedly higher level of chemical dispersion than both 40 and 60 nm particles. An analysis of droplet activation kinetics for the sizes considered indicates that most of the CCN activate as rapidly as (NH4)(2)SO4 calibration aerosol.
引用
收藏
页码:12369 / 12386
页数:18
相关论文
共 86 条
[1]  
Aalto Pasi, 2000, Boreal Environment Research, V5, P349
[2]   O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry [J].
Aiken, Allison C. ;
Decarlo, Peter F. ;
Kroll, Jesse H. ;
Worsnop, Douglas R. ;
Huffman, J. Alex ;
Docherty, Kenneth S. ;
Ulbrich, Ingrid M. ;
Mohr, Claudia ;
Kimmel, Joel R. ;
Sueper, Donna ;
Sun, Yele ;
Zhang, Qi ;
Trimborn, Achim ;
Northway, Megan ;
Ziemann, Paul J. ;
Canagaratna, Manjula R. ;
Onasch, Timothy B. ;
Alfarra, M. Rami ;
Prevot, Andre S. H. ;
Dommen, Josef ;
Duplissy, Jonathan ;
Metzger, Axel ;
Baltensperger, Urs ;
Jimenez, Jose L. .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2008, 42 (12) :4478-4485
[3]   Characterization of urban and rural organic particulate in the lower Fraser valley using two aerodyne aerosol mass spectrometers [J].
Alfarra, MR ;
Coe, H ;
Allan, JD ;
Bower, KN ;
Boudries, H ;
Canagaratna, MR ;
Jimenez, JL ;
Jayne, JT ;
Garforth, AA ;
Li, SM ;
Worsnop, DR .
ATMOSPHERIC ENVIRONMENT, 2004, 38 (34) :5745-5758
[4]   Quantitative sampling using an Aerodyne aerosol mass spectrometer - 1. Techniques of data interpretation and error analysis [J].
Allan, JD ;
Jimenez, JL ;
Williams, PI ;
Alfarra, MR ;
Bower, KN ;
Jayne, JT ;
Coe, H ;
Worsnop, DR .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2003, 108 (D3)
[5]   Size and composition measurements of background aerosol and new particle growth in a Finnish forest during QUEST 2 using an Aerodyne Aerosol Mass Spectrometer [J].
Allan, JD ;
Alfarra, MR ;
Bower, KN ;
Coe, H ;
Jayne, JT ;
Worsnop, DR ;
Aalto, PP ;
Kulmala, M ;
Hyötyläinen, T ;
Cavalli, F ;
Laaksonen, A .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2006, 6 :315-327
[6]   A generalised method for the extraction of chemically resolved mass spectra from aerodyne aerosol mass spectrometer data [J].
Allan, JD ;
Delia, AE ;
Coe, H ;
Bower, KN ;
Alfarra, MR ;
Jimenez, JL ;
Middlebrook, AM ;
Drewnick, F ;
Onasch, TB ;
Canagaratna, MR ;
Jayne, JT ;
Worsnop, DR .
JOURNAL OF AEROSOL SCIENCE, 2004, 35 (07) :909-922
[7]   Aerosol-cloud-precipitation interactions. Part 1. The nature and sources of cloud-active aerosols [J].
Andreae, M. O. ;
Rosenfeld, D. .
EARTH-SCIENCE REVIEWS, 2008, 89 (1-2) :13-41
[8]   Water-soluble SOA from Alkene ozonolysis: composition and droplet activation kinetics inferences from analysis of CCN activity [J].
Asa-Awuku, A. ;
Nenes, A. ;
Gao, S. ;
Flagan, R. C. ;
Seinfeld, J. H. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2010, 10 (04) :1585-1597
[9]   Relating CCN activity, volatility, and droplet growth kinetics of β-caryophyllene secondary organic aerosol [J].
Asa-Awuku, A. ;
Engelhart, G. J. ;
Lee, B. H. ;
Pandis, S. N. ;
Nenes, A. .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2009, 9 (03) :795-812
[10]   Airborne cloud condensation nuclei measurements during the 2006 Texas Air Quality Study [J].
Asa-Awuku, Akua ;
Moore, Richard H. ;
Nenes, Athanasios ;
Bahreini, Roya ;
Holloway, John S. ;
Brock, Charles A. ;
Middlebrook, Ann M. ;
Ryerson, Thomas B. ;
Jimenez, Jose L. ;
DeCarlo, Peter F. ;
Hecobian, Arsineh ;
Weber, Rodney J. ;
Stickel, Robert ;
Tanner, Dave J. ;
Huey, Lewis G. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2011, 116