期刊
ATMOSPHERIC CHEMISTRY AND PHYSICS
卷 17, 期 24, 页码 15181-15197出版社
COPERNICUS GESELLSCHAFT MBH
DOI: 10.5194/acp-17-15181-2017
关键词
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资金
- European Organization for Nuclear Research (CERN)
- EC Seventh Framework Programme [316662, 227463, 616075, 335478, 257360, 600377]
- EC Horizon (Marie Sklodowska-Curie Individual Fellowships Nano-CAVa) [656994]
- EC Horizon (Marie Sklodowska-Curie Individual Fellowship starting grant COALA) [638703]
- German Federal Ministry of Education and Research [01LK1222A, 01LK0902A]
- Russian Foundation for Basic Research [08-02-91006-CERN, 12-02-91522-CERN]
- US Department of Energy [DE-SC0014469]
- Swiss National Science Foundation [206620_141278, 200020_135307, 200021_140663, 206021_144947/1]
- Austrian Science Fund [J3198-N21, L593, P19546]
- Portuguese Foundation for Science and Technology [CERN/FP/116387/2010]
- Swedish Research Council [2011-5120]
- US National Science Foundation [AGS1136479, AGS1447056, AGC1439551, CHE1012293]
- Natural Environment Research Council [NE/J024252/1, NE/K015966/1]
- Royal Society (Wolfson Merit Award)
- Dreyfus Award [EP-11-117]
- European Funds for Regional Economic Development (Labex-Cappa grant) [ANR-11LABX-0005-01]
- Nessling Foundation
- Finnish Funding Agency for Technology and Innovation
- Vaisala Foundation
- Caltech Environmental Science and Engineering grant (Davidow Foundation)
- French National Research Agency, Nord-Pas de Calais
- Academy of Finland [299574, 1118615, 135054, 133872, 251427, 139656, 139995, 141451, 137749, 141217, 138951]
- Presidium of the Russian Academy of Sciences
- U.S. Department of Energy (DOE) [DE-SC0014469] Funding Source: U.S. Department of Energy (DOE)
- NERC [NE/K015966/1] Funding Source: UKRI
- Swiss National Science Foundation (SNF) [206620_141278, 206021_144947, 200021_140663] Funding Source: Swiss National Science Foundation (SNF)
- Natural Environment Research Council [NE/K015966/1, NE/J024252/1] Funding Source: researchfish
- Div Atmospheric & Geospace Sciences
- Directorate For Geosciences [1439551, 1447056] Funding Source: National Science Foundation
- Marie Curie Actions (MSCA) [656994] Funding Source: Marie Curie Actions (MSCA)
- European Research Council (ERC) [257360] Funding Source: European Research Council (ERC)
- Academy of Finland (AKA) [138951, 138951] Funding Source: Academy of Finland (AKA)
The formation of secondary particles in the atmosphere accounts for more than half of global cloud condensation nuclei. Experiments at the CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber have underlined the importance of ions for new particle formation, but quantifying their effect in the atmosphere remains challenging. By using a novel instrument setup consisting of two nanoparticle counters, one of them equipped with an ion filter, we were able to further investigate the ion-related mechanisms of new particle formation. In autumn 2015, we carried out experiments at CLOUD on four systems of different chemical compositions involving monoterpenes, sulfuric acid, nitrogen oxides, and ammonia. We measured the influence of ions on the nucleation rates under precisely controlled and atmospherically relevant conditions. Our results indicate that ions enhance the nucleation process when the charge is necessary to stabilize newly formed clusters, i.e., in conditions in which neutral clusters are unstable. For charged clusters that were formed by ion-induced nucleation, we were able to measure, for the first time, their progressive neutralization due to recombination with oppositely charged ions. A large fraction of the clusters carried a charge at 1.5 nm diameter. However, depending on particle growth rates and ion concentrations, charged clusters were largely neutralized by ion-ion recombination before they grew to 2.5 nm. At this size, more than 90% of particles were neutral. In other words, particles may originate from ion-induced nucleation, although they are neutral upon detection at diameters larger than 2.5 nm. Observations at Hyytiala, Finland, showed lower ion concentrations and a lower contribution of ion-induced nucleation than measured at CLOUD under similar conditions. Although this can be partly explained by the observation that ion-induced fractions decrease towards lower ion concentrations, further investigations are needed to resolve the origin of the discrepancy.
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