| 1. |
- Almeida, Joao, et al.
(författare)
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Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere
- 2013
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Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 502:7471, s. 359-
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Tidskriftsartikel (refereegranskat)abstract
- Nucleation of aerosol particles from trace atmospheric vapours is thought to provide up to half of global cloud condensation nuclei(1). Aerosols can cause a net cooling of climate by scattering sunlight and by leading to smaller but more numerous cloud droplets, which makes clouds brighter and extends their lifetimes(2). Atmospheric aerosols derived from human activities are thought to have compensated for a large fraction of the warming caused by greenhouse gases(2). However, despite its importance for climate, atmospheric nucleation is poorly understood. Recently, it has been shown that sulphuric acid and ammonia cannot explain particle formation rates observed in the lower atmosphere(3). It is thought that amines may enhance nucleation(4-16), but until now there has been no direct evidence for amine ternary nucleation under atmospheric conditions. Here we use the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber at CERN and find that dimethylamine above three parts per trillion by volume can enhance particle formation rates more than 1,000-fold compared with ammonia, sufficient to account for the particle formation rates observed in the atmosphere. Molecular analysis of the clusters reveals that the faster nucleation is explained by a base-stabilization mechanism involving acid-amine pairs, which strongly decrease evaporation. The ion-induced contribution is generally small, reflecting the high stability of sulphuric acid-dimethylamine clusters and indicating that galactic cosmic rays exert only a small influence on their formation, except at low overall formation rates. Our experimental measurements are well reproduced by a dynamical model based on quantum chemical calculations of binding energies of molecular clusters, without any fitted parameters. These results show that, in regions of the atmosphere near amine sources, both amines and sulphur dioxide should be considered when assessing the impact of anthropogenic activities on particle formation.
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| 2. |
- Donahue, Neil M., et al.
(författare)
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How do organic vapors contribute to new-particle formation?
- 2013
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Ingår i: Faraday discussions. - : Royal Society of Chemistry. - 1359-6640 .- 1364-5498. ; 165, s. 91-104
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Tidskriftsartikel (refereegranskat)abstract
- Highly oxidised organic vapors can effectively stabilize sulphuric acid in heteronuclear clusters and drive new-particle formation. We present quantum chemical calculations of cluster stability, showing that multifunctional species can stabilize sulphuric acid and also present additional polar functional groups for subsequent cluster growth. We also model the multi-generation oxidation of vapors associated with secondary organic aerosol formation using a two-dimensional volatility basis set. The steady-state saturation ratios and absolute concentrations of extremely low volatility products are sufficient to drive new-particle formation with sulphuric acid at atmospherically relevant rates.
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| 3. |
- Kulmala, Markku, et al.
(författare)
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Direct Observations of Atmospheric Aerosol Nucleation
- 2013
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Ingår i: Science. - : American Association for the Advancement of Science (AAAS). - 0036-8075 .- 1095-9203. ; 339:6122, s. 943-946
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Tidskriftsartikel (refereegranskat)abstract
- Atmospheric nucleation is the dominant source of aerosol particles in the global atmosphere and an important player in aerosol climatic effects. The key steps of this process occur in the sub-2-nanometer (nm) size range, in which direct size-segregated observations have not been possible until very recently. Here, we present detailed observations of atmospheric nanoparticles and clusters down to 1-nm mobility diameter. We identified three separate size regimes below 2-nm diameter that build up a physically, chemically, and dynamically consistent framework on atmospheric nucleation-more specifically, aerosol formation via neutral pathways. Our findings emphasize the important role of organic compounds in atmospheric aerosol formation, subsequent aerosol growth, radiative forcing and associated feedbacks between biogenic emissions, clouds, and climate.
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| 4. |
- Lehtipalo, Katrianne, et al.
(författare)
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How Do Amines Affect the Growth of Recently Formed Aerosol Particles
- 2013
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Ingår i: NUCLEATION AND ATMOSPHERIC AEROSOLS. - : American Institute of Physics (AIP). - 9780735411524 ; , s. 295-297
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Konferensbidrag (refereegranskat)abstract
- Growth rates of recently born nanometer-scale particles were measured during the CLOUD experiments at CERN. Combining the data from several recently developed measurement techniques allowed us to follow the growth of the particles starting from molecules to molecular clusters and finally to climatically relevant particles. We studied the binary system with sulphuric acid and water, and the ternary systems with ammonia or dimethylamine added to the chamber, both in purely neutral situation, and with ionization from cosmic rays or the CERN particle beam.
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| 5. |
- Schobesberger, Siegfried, et al.
(författare)
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Airborne measurements over the boreal forest of southern Finland during new particle formation events in 2009 and 2010
- 2013
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Ingår i: Boreal environment research. - 1239-6095 .- 1797-2469. ; 18:2, s. 145-163
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Tidskriftsartikel (refereegranskat)abstract
- Schobesberger, S., Vaananen, R., Leino, K., Virkkula, A., Backman, J., Pohja, T., Siivola, E., Franchin, A., Mikkila, J., Paramonov, M., Aalto, P.P., Krejci, R., Petaja, T. & Kulmala, M. 2013: Airborne measurements over the boreal forest of southern Finland during new particle formation events in 2009 and 2010. Boreal Env. Res. 18: 145-163. We conducted airborne observations of aerosol physical properties over the southern Finland boreal forest environment. The aim was to investigate the lower tropospheric aerosol (up to 4-km altitude) over an area of 250 by 200 km, in particular during new particle formation (NPF) events, and to address the spatial variability of aerosol number concentration and number size distribution. The regional NPF events, detected both airborne and at the ground, with air masses originating from the Arctic or northern Atlantic Ocean were studied throughout the boundary layer and throughout the area covered. Three suitable case studies are presented in more detail. In two of these studies, the concentrations of nucleation mode particles (3-10 nm in diameter) were found considerably higher (up to a factor of 30) in the upper parts of the planetary boundary layer compared to ground-based measurements during the nucleation events. The observed vertical variation can be connected to boundary layer dynamics and interactions between the boundary layer and the lower free troposphere, likely yielding high concentrations of newly formed aerosol particles. Our results suggest that nucleation does not necessarily occur close to the surface. In one presented case we found evidence of NPF occurring in a limited area above cloud, in the complete absence of a regional NPF event.
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