Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere. Almeida, J., Schobesberger, S., Kurten, A., Ortega, I., K., Kupiainen-Maatta, O., Praplan, A., P., Adamov, A., Amorim, A., Bianchi, F., Breitenlechner, M., David, A., Dommen, J., Donahue, N., M., Downard, A., Dunne, E., Duplissy, J., Ehrhart, S., Flagan, R., C., Franchin, A., Guida, R., Hakala, J., Hansel, A., Heinritzi, M., Henschel, H., Jokinen, T., Junninen, H., Kajos, M., Kangasluoma, J., Keskinen, H., Kupc, A., Kurten, T., Kvashin, A., N., Laaksonen, A., Lehtipalo, K., Leiminger, M., Leppa, J., Loukonen, V., Makhmutov, V., Mathot, S., McGrath, M., J., Nieminen, T., Olenius, T., Onnela, A., Petaja, T., Riccobono, F., Riipinen, I., Rissanen, M., Rondo, L., Ruuskanen, T., Santos, F., D., Sarnela, N., Schallhart, S., Schnitzhofer, R., Seinfeld, J., H., Simon, M., Sipila, M., Stozhkov, Y., Stratmann, F., Tome, A., Trostl, J., Tsagkogeorgas, G., Vaattovaara, P., Viisanen, Y., Virtanen, A., Vrtala, A., Wagner, P., E., Weingartner, E., Wex, H., Williamson, C., Wimmer, D., Ye, P., L., Yli-Juuti, T., Carslaw, K., S., Kulmala, M., Curtius, J., Baltensperger, U., Worsnop, D., R., Vehkamaki, H., & Kirkby, J. Nature, 502:359-+, 2013.
Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere [link]Website  abstract   bibtex   
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.
@article{
 title = {Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere},
 type = {article},
 year = {2013},
 identifiers = {[object Object]},
 pages = {359-+},
 volume = {502},
 websites = {<Go to ISI>://WOS:000325706300050},
 id = {6f1165b0-d702-304c-9ebe-5708147cc346},
 created = {2014-10-08T16:26:04.000Z},
 file_attached = {false},
 profile_id = {363623ef-1990-38f1-b354-f5cdaa6548b2},
 group_id = {02267cec-5558-3876-9cfc-78d056bad5b9},
 last_modified = {2017-03-14T17:32:24.802Z},
 read = {false},
 starred = {false},
 authored = {false},
 confirmed = {true},
 hidden = {false},
 citation_key = {Almeida2013},
 source_type = {JOUR},
 notes = {Almeida, Joao Schobesberger, Siegfried Kuerten, Andreas Ortega, Ismael K. Kupiainen-Maatta, Oona Praplan, Arnaud P. Adamov, Alexey Amorim, Antonio Bianchi, Federico Breitenlechner, Martin David, Andre Dommen, Josef Donahue, Neil M. Downard, Andrew Dunne, Eimear Duplissy, Jonathan Ehrhart, Sebastian Flagan, Richard C. Franchin, Alessandro Guida, Roberto Hakala, Jani Hansel, Armin Heinritzi, Martin Henschel, Henning Jokinen, Tuija Junninen, Heikki Kajos, Maija Kangasluoma, Juha Keskinen, Helmi Kupc, Agnieszka Kurten, Theo Kvashin, Alexander N. Laaksonen, Ari Lehtipalo, Katrianne Leiminger, Markus Leppa, Johannes Loukonen, Ville Makhmutov, Vladimir Mathot, Serge McGrath, Matthew J. Nieminen, Tuomo Olenius, Tinja Onnela, Antti Petaja, Tuukka Riccobono, Francesco Riipinen, Ilona Rissanen, Matti Rondo, Linda Ruuskanen, Taina Santos, Filipe D. Sarnela, Nina Schallhart, Simon Schnitzhofer, Ralf Seinfeld, John H. Simon, Mario Sipila, Mikko Stozhkov, Yuri Stratmann, Frank Tome, Antonio Troestl, Jasmin Tsagkogeorgas, Georgios Vaattovaara, Petri Viisanen, Yrjo Virtanen, Annele Vrtala, Aron Wagner, Paul E. Weingartner, Ernest Wex, Heike Williamson, Christina Wimmer, Daniela Ye, Penglin Yli-Juuti, Taina Carslaw, Kenneth S. Kulmala, Markku Curtius, Joachim Baltensperger, Urs Worsnop, Douglas R. Vehkamaki, Hanna Kirkby, Jasper<m:linebreak></m:linebreak>Vehkamaki, Hanna/A-8262-2008; Santos, Filipe/M-7709-2013; Virtanen, Annele/E-7699-2010; Worsnop, Douglas/D-2817-2009; Donahue, Neil/A-2329-2008; Kirkby, Jasper/A-4973-2012; Bianchi, Federico/G-8428-2012; Junninen, Heikki/C-2157-2014; Henschel, Henning/A-5060-2012; Sipila, Mikko/G-3024-2010; Kurten, Theo/G-2120-2012; Carslaw, Ken/C-8514-2009; Petaja, Tuukka/A-8009-2008; Tome, Antonio/A-5681-2013; Riipinen, Ilona/I-9379-2012; Dunne, Eimear/H-1567-2014; Weingartner, Ernest/B-6793-2009; Duplissy, Jonathan/A-1723-2010<m:linebreak></m:linebreak>Vehkamaki, Hanna/0000-0002-5018-1255; Santos, Filipe/0000-0001-7316-1479; Virtanen, Annele/0000-0002-2917-5344; Worsnop, Douglas/0000-0002-8928-8017; Donahue, Neil/0000-0003-3054-2364; Kirkby, Jasper/0000-0003-2341-9069; Junninen, Heikki/0000-0001-7178-9430; Henschel, Henning/0000-0001-7196-661X; Petaja, Tuukka/0000-0002-1881-9044; Dunne, Eimear/0000-0001-7085-8473;},
 private_publication = {false},
 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.},
 bibtype = {article},
 author = {Almeida, J and Schobesberger, S and Kurten, A and Ortega, I K and Kupiainen-Maatta, O and Praplan, A P and Adamov, A and Amorim, A and Bianchi, F and Breitenlechner, M and David, A and Dommen, J and Donahue, N M and Downard, A and Dunne, E and Duplissy, J and Ehrhart, S and Flagan, R C and Franchin, A and Guida, R and Hakala, J and Hansel, A and Heinritzi, M and Henschel, H and Jokinen, T and Junninen, H and Kajos, M and Kangasluoma, J and Keskinen, H and Kupc, A and Kurten, T and Kvashin, A N and Laaksonen, A and Lehtipalo, K and Leiminger, M and Leppa, J and Loukonen, V and Makhmutov, V and Mathot, S and McGrath, M J and Nieminen, T and Olenius, T and Onnela, A and Petaja, T and Riccobono, F and Riipinen, I and Rissanen, M and Rondo, L and Ruuskanen, T and Santos, F D and Sarnela, N and Schallhart, S and Schnitzhofer, R and Seinfeld, J H and Simon, M and Sipila, M and Stozhkov, Y and Stratmann, F and Tome, A and Trostl, J and Tsagkogeorgas, G and Vaattovaara, P and Viisanen, Y and Virtanen, A and Vrtala, A and Wagner, P E and Weingartner, E and Wex, H and Williamson, C and Wimmer, D and Ye, P L and Yli-Juuti, T and Carslaw, K S and Kulmala, M and Curtius, J and Baltensperger, U and Worsnop, D R and Vehkamaki, H and Kirkby, J},
 journal = {Nature}
}

Downloads: 0