Evidence for the role of organics in aerosol particle formation under atmospheric conditions

被引:327
作者
Metzger, Axel [1 ]
Verheggen, Bart [2 ]
Dommen, Josef [1 ]
Duplissy, Jonathan [1 ]
Prevot, Andre S. H. [1 ]
Weingartner, Ernest [1 ]
Riipinen, Ilona [3 ]
Kulmala, Markku [3 ]
Spracklen, Dominick V. [4 ]
Carslaw, Kenneth S. [4 ]
Baltensperger, Urs [1 ]
机构
[1] Paul Scherrer Inst, Lab Atmospher Chem, CH-5232 Villigen, Switzerland
[2] Energy Res Ctr Netherlands, Dept Air Qual & Climate Change, NL-1755 ZG Petten, Netherlands
[3] Univ Helsinki, Dept Phys, Helsinki 00014, Finland
[4] Univ Leeds, Inst Climate & Atmospher Sci, Sch Earth & Environm, Leeds LS2 9JT, W Yorkshire, England
基金
英国自然环境研究理事会; 瑞士国家科学基金会;
关键词
aerosol particles; atmospheric nucleation; new particle formation; sulfuric acid; SULFURIC-ACID; GROWTH-RATES; NUCLEATION EVENTS; BOREAL FOREST; SIZE; QUEST; MODEL;
D O I
10.1073/pnas.0911330107
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
New particle formation in the atmosphere is an important parameter in governing the radiative forcing of atmospheric aerosols. However, detailed nucleation mechanisms remain ambiguous, as laboratory data have so far not been successful in explaining atmospheric nucleation. We investigated the formation of new particles in a smog chamber simulating the photochemical formation of H2SO4 and organic condensable species. Nucleation occurs at H2SO4 concentrations similar to those found in the ambient atmosphere during nucleation events. The measured particle formation rates are proportional to the product of the concentrations of H2SO4 and an organic molecule. This suggests that only one H2SO4 molecule and one organic molecule are involved in the rate-limiting step of the observed nucleation process. Parameterizing this process in a global aerosol model results in substantially better agreement with ambient observations compared to control runs.
引用
收藏
页码:6646 / 6651
页数:6
相关论文
共 27 条
[1]   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)
[2]   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
[3]   How biogenic terpenes govern the correlation between sulfuric acid concentrations and new particle formation [J].
Bonn, B. ;
Kulmala, M. ;
Riipinen, I. ;
Sihto, S. -L. ;
Ruuskanen, T. M. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2008, 113 (D12)
[4]   Nucleation of atmospheric aerosol particles [J].
Curtius, Joachim .
COMPTES RENDUS PHYSIQUE, 2006, 7 (9-10) :1027-1045
[5]   Structure, variability and persistence of the submicrometre marine aerosol [J].
Heintzenberg, J ;
Birmili, W ;
Wiedensohler, A ;
Nowak, A ;
Tuch, T .
TELLUS SERIES B-CHEMICAL AND PHYSICAL METEOROLOGY, 2004, 56 (04) :357-367
[6]   Analytical formulae connecting the "real" and the "apparent" nucleation rate and the nuclei number concentration for atmospheric nucleation events [J].
Kerminen, VM ;
Kulmala, M .
JOURNAL OF AEROSOL SCIENCE, 2002, 33 (04) :609-622
[7]   Dependence of nucleation rates on sulfuric acid vapor concentration in diverse atmospheric locations [J].
Kuang, C. ;
McMurry, P. H. ;
McCormick, A. V. ;
Eisele, F. L. .
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2008, 113 (D10)
[8]   On the formation, growth and composition of nucleation mode particles [J].
Kulmala, M ;
Dal Maso, M ;
Mäkelä, JM ;
Pirjola, L ;
Väkevä, M ;
Aalto, P ;
Miikkulainen, P ;
Hämeri, K ;
O'Dowd, CD .
TELLUS SERIES B-CHEMICAL AND PHYSICAL METEOROLOGY, 2001, 53 (04) :479-490
[9]   Cluster activation theory as an explanation of the linear dependence between formation rate of 3nm particles and sulphuric acid concentration [J].
Kulmala, M ;
Lehtinen, KEJ ;
Laaksonen, A .
ATMOSPHERIC CHEMISTRY AND PHYSICS, 2006, 6 :787-793
[10]   Formation and growth rates of ultrafine atmospheric particles:: a review of observations [J].
Kulmala, M ;
Vehkamäki, H ;
Petäjä, T ;
Dal Maso, M ;
Lauri, A ;
Kerminen, VM ;
Birmili, W ;
McMurry, PH .
JOURNAL OF AEROSOL SCIENCE, 2004, 35 (02) :143-176