Organic condensation: a vital link connecting aerosol formation to cloud condensation nuclei (CCN) concentrations

被引:302
作者
Riipinen, I. [1 ,2 ]
Pierce, J. R. [3 ]
Yli-Juuti, T. [2 ]
Nieminen, T. [2 ]
Hakkinen, S. [2 ]
Ehn, M. [2 ]
Junninen, H. [2 ]
Lehtipalo, K. [2 ]
Petaja, T. [2 ]
Slowik, J. [4 ]
Chang, R. [4 ]
Shantz, N. C. [5 ]
Abbatt, J. [4 ]
Leaitch, W. R. [5 ]
Kerminen, V. -M. [2 ,6 ]
Worsnop, D. R. [2 ,7 ]
Pandis, S. N. [1 ,8 ]
Donahue, N. M. [1 ]
Kulmala, M. [2 ]
机构
[1] Carnegie Mellon Univ, Ctr Atmospher Particle Studies CAPS, Pittsburgh, PA 15213 USA
[2] Univ Helsinki, Dept Phys, Helsinki 00014, Finland
[3] Dalhousie Univ, Dept Phys & Atmospher Sci, Halifax, NS B3H 3J5, Canada
[4] Univ Toronto, Dept Chem, Toronto, ON M5S 3H6, Canada
[5] Environm Canada, Sci & Technol Branch, Toronto, ON M3H 5T4, Canada
[6] Finnish Meteorol Inst, Helsinki 00880, Finland
[7] Aerodyne Res Inc, Billerica, MA 01821 USA
[8] Hellas FORTH, Fdn Res & Technol, Inst Chem Engn & High Temp Proc ICE HT, Patras 26504, Greece
基金
美国国家科学基金会; 芬兰科学院;
关键词
COUNTER BATTERY CPCB; SULFURIC-ACID; ATMOSPHERIC PARTICLES; ASSIMILATED METEOROLOGY; SIZE DISTRIBUTION; MODEL DESCRIPTION; LIGHT-SCATTERING; GROWTH-RATES; NUCLEATION; AIR;
D O I
10.5194/acp-11-3865-2011
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Atmospheric aerosol particles influence global climate as well as impair air quality through their effects on atmospheric visibility and human health. Ultrafine (< 100 nm) particles often dominate aerosol numbers, and nucleation of atmospheric vapors is an important source of these particles. To have climatic relevance, however, the freshly nucleated particles need to grow in size. We combine observations from two continental sites (Egbert, Canada and Hyytiala, Finland) to show that condensation of organic vapors is a crucial factor governing the lifetimes and climatic importance of the smallest atmospheric particles. We model the observed ultrafine aerosol growth with a simplified scheme approximating the condensing species as a mixture of effectively non-volatile and semi-volatile species, demonstrate that state-of-the-art organic gas-particle partitioning models fail to reproduce the observations, and propose a modeling approach that is consistent with the measurements. We find that roughly half of the mass of the condensing mass needs to be distributed proportional to the aerosol surface area (thus implying that the condensation is governed by gas-phase concentration rather than the equilibrium vapour pressure) to explain the observed aerosol growth. We demonstrate the large sensitivity of predicted number concentrations of cloud condensation nuclei (CCN) to these interactions between organic vapors and the smallest atmospheric nanoparticles highlighting the need for representing this process in global climate models.
引用
收藏
页码:3865 / 3878
页数:14
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