Relating CCN activity, volatility, and droplet growth kinetics of β-caryophyllene secondary organic aerosol

被引:127
作者
Asa-Awuku, A. [1 ]
Engelhart, G. J. [2 ]
Lee, B. H. [2 ]
Pandis, S. N. [2 ,3 ]
Nenes, A. [1 ,4 ]
机构
[1] Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA
[2] Carnegie Mellon Univ, Dept Chem Engn, Pittsburgh, PA 15213 USA
[3] Univ Patras, Dept Chem Engn, Patras, Greece
[4] Georgia Inst Technol, Sch Earth & Atmospher Sci, Atlanta, GA 30332 USA
基金
美国国家科学基金会;
关键词
CLOUD CONDENSATION NUCLEI; ATMOSPHERIC PARTICLES; ALPHA-PINENE; BIOGENIC HYDROCARBONS; TERPENE OZONOLYSIS; SURFACE-TENSION; CRITICAL SUPERSATURATION; SINGLE-COMPONENT; SOLUBLE ORGANICS; EMISSION RATES;
D O I
10.5194/acp-9-795-2009
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
This study investigates the droplet formation characteristics of secondary organic aerosol (SOA) formed during the ozonolysis of sesquiterpene beta-caryophyllene (with and without hydroxyl radicals present). Emphasis is placed on understanding the role of semi-volatile material on Cloud Condensation Nucleus (CCN) activity and droplet growth kinetics. Aging of beta-caryophyllene SOA significantly affects all CCN-relevant properties measured throughout the experiments. Using a thermodenuder and two CCN instruments, we find that CCN activity is a strong function of temperature (activation diameter at similar to 0.6% supersaturation: 100 +/- 10 nm at 20 degrees C and 130 +/- 10 nm at 35 degrees C), suggesting that the hygroscopic fraction of the SOA is volatile. The water-soluble organic carbon (WSOC) is extracted from the SOA and characterized with K Kohler Theory Analysis (KTA); the results suggest that the WSOC is composed of low molecular weight (<200 g mol(-1)) slightly surface-active material that constitute 5-15% of the SOA mass. These properties are similar to the water-soluble fraction of monoterpene SOA, suggesting that predictive understanding of SOA CCN activity requires knowledge of the WSOC fraction but not its exact speciation. Droplet growth kinetics of the CCN are found to be strongly anticorrelated with WSOC fraction, suggesting that the insoluble material in the SOA forms a kinetic barrier that delays droplet growth. Overall, volatilization effects can increase activation diameters by 30%, and depress droplet growth rate by a factor of two; these results may have important implications for the droplet formation characteristics of SOA, and the atmospheric relevance of CCN measurements carried out at temperatures different from ambient.
引用
收藏
页码:795 / 812
页数:18
相关论文
共 98 条
[31]   Estimate of global atmospheric organic aerosol from oxidation of biogenic hydrocarbons [J].
Griffin, RJ ;
Cocker, DR ;
Seinfeld, JH ;
Dabdub, D .
GEOPHYSICAL RESEARCH LETTERS, 1999, 26 (17) :2721-2724
[32]   ATMOSPHERIC OXIDATION OF BIOGENIC HYDROCARBONS - REACTION OF OZONE WITH BETA-PINENE, D-LIMONENE AND TRANS-CARYOPHYLLENE [J].
GROSJEAN, D ;
WILLIAMS, EL ;
GROSJEAN, E ;
ANDINO, JM ;
SEINFELD, JH .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1993, 27 (13) :2754-2758
[33]   Natural emissions of non-methane volatile organic compounds; carbon monoxide, and oxides of nitrogen from North America [J].
Guenther, A ;
Geron, C ;
Pierce, T ;
Lamb, B ;
Harley, P ;
Fall, R .
ATMOSPHERIC ENVIRONMENT, 2000, 34 (12-14) :2205-2230
[34]   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
[35]   Biogenic hydrocarbon emissions and landcover/climate change in a subtropical savanna [J].
Guenther, A ;
Archer, S ;
Greenberg, J ;
Harley, P ;
Helmig, D ;
Klinger, L ;
Vierling, L ;
Wildermuth, M ;
Zimmerman, P ;
Zitzer, S .
PHYSICS AND CHEMISTRY OF THE EARTH PART B-HYDROLOGY OCEANS AND ATMOSPHERE, 1999, 24 (06) :659-667
[36]   Temperature and light dependence of β-caryophyllene emission rates -: art. no. 4801 [J].
Hansen, U ;
Seufert, G .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2003, 108 (D24)
[37]   Cloud condensation nuclei activation of monoterpene and sesquiterpene secondary organic aerosol [J].
Hartz, KEH ;
Rosenorn, T ;
Ferchak, SR ;
Raymond, TM ;
Bilde, M ;
Donahue, NM ;
Pandis, SN .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2005, 110 (D14) :1-8
[38]   Sesquiterpene emissions from pine trees - Identifications, emission rates and flux estimates for the contiguous United States [J].
Helmig, Detlev ;
Ortega, John ;
Duhl, Tiffany ;
Tanner, David ;
Guenther, Alex ;
Harley, Peter ;
Wiedinmyer, Christine ;
Milford, Jana ;
Sakulyanontvittaya, Tanarit .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2007, 41 (05) :1545-1553
[39]   Cloud droplet activation and surface tension of mixtures of slightly soluble organics and inorganic salt [J].
Henning, S ;
Rosenorn, T ;
D'Anna, B ;
Gola, AA ;
Svenningsson, B ;
Bilde, M .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2005, 5 :575-582
[40]  
HOFFMANN T, 1995, FRESEN J ANAL CHEM, V351, P41