New particle formation in the free troposphere: A question of chemistry and timing

被引:366
作者
Bianchi, F. [1 ,2 ,3 ]
Trostl, J. [1 ]
Junninen, H. [3 ]
Frege, C. [1 ]
Henne, S. [4 ]
Hoyle, C. R. [1 ,5 ]
Molteni, U. [1 ]
Herrmann, E. [1 ]
Adamov, A. [3 ]
Bukowiecki, N. [1 ]
Chen, X. [3 ]
Duplissy, J. [3 ,6 ]
Gysel, M. [1 ]
Hutterli, M. [7 ]
Kangasluoma, J. [3 ]
Kontkanen, J. [3 ]
Kuerten, A. [8 ]
Manninen, H. E. [3 ]
Muench, S. [8 ]
Perakyla, O. [3 ]
Petaja, T. [3 ]
Rondo, L. [8 ]
Williamson, C. [8 ,10 ]
Weingartner, E. [1 ,11 ]
Curtius, J. [8 ]
Worsnop, D. R. [3 ,9 ]
Kulmala, M. [3 ]
Dommen, J. [1 ]
Baltensperger, U. [1 ]
机构
[1] Paul Scherrer Inst, Lab Atmospher Chem, CH-5232 Villigen, Switzerland
[2] ETH, Inst Atmospher & Climate Sci, CH-8092 Zurich, Switzerland
[3] Univ Helsinki, Dept Phys, Helsinki 00014, Finland
[4] Empa, Swiss Fed Labs Mat Sci & Technol, CH-8600 Dubendorf, Switzerland
[5] Inst Snow & Avalanche Res SLF, WSL Swiss Fed Inst Forest Snow & Landscape Res, CH-7260 Davos, Switzerland
[6] Univ Helsinki, Helsinki Inst Phys, FIN-00014 Helsinki, Finland
[7] Tofwerk, CH-3600 Thun, Switzerland
[8] Goethe Univ Frankfurt, Inst Atmospher & Environm Sci, D-60438 Frankfurt, Germany
[9] Aerodyne Res, Billerica, MA 01821 USA
[10] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA
[11] Univ Appl Sci FHNW, Inst Aerosol & Sensor Technol, CH-5210 Windisch, Switzerland
基金
瑞士国家科学基金会; 欧洲研究理事会; 芬兰科学院;
关键词
SULFURIC-ACID; M A.S.L; NUCLEATION; GROWTH; JUNGFRAUJOCH; OZONOLYSIS; PRODUCTS; SIZE;
D O I
10.1126/science.aad5456
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 (NPF) is the source of over half of the atmosphere's cloud condensation nuclei, thus influencing cloud properties and Earth's energy balance. Unlike in the planetary boundary layer, few observations of NPF in the free troposphere exist. We provide observational evidence that at high altitudes, NPF occurs mainly through condensation of highly oxygenated molecules (HOMs), in addition to taking place through sulfuric acid-ammonia nucleation. Neutral nucleation is more than 10 times faster than ion-induced nucleation, and growth rates are size-dependent. NPF is restricted to a time window of 1 to 2 days after contact of the air masses with the planetary boundary layer; this is related to the time needed for oxidation of organic compounds to form HOMs. These findings require improved NPF parameterization in atmospheric models.
引用
收藏
页码:1109 / 1112
页数:4
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