Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation
Autor(a) principal: | |
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Data de Publicação: | 2011 |
Outros Autores: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
Tipo de documento: | Artigo |
Idioma: | eng |
Título da fonte: | Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
Texto Completo: | http://hdl.handle.net/10400.6/5755 |
Resumo: | Atmospheric aerosols exert an important influence on climate through their effects on stratiform cloud albedo and lifetime and the invigoration of convective storms. Model calculations suggest that almost half of the global cloud condensation nuclei in the atmospheric boundary layer may originate from the nucleation of aerosols from trace condensable vapours, although the sensitivity of the number of cloud condensation nuclei to changes of nucleation rate may be small. Despite extensive research, fundamental questions remain about the nucleation rate of sulphuric acid particles and the mechanisms responsible, including the roles of galactic cosmic rays and other chemical species such as ammonia. Here we present the first results from the CLOUD experiment at CERN. We find that atmospherically relevant ammonia mixing ratios of 100 parts per trillion by volume, or less, increase the nucleation rate of sulphuric acid particles more than 100-1,000-fold. Time-resolved molecular measurements reveal that nucleation proceeds by a base-stabilization mechanism involving the stepwise accretion of ammonia molecules. Ions increase the nucleation rate by an additional factor of between two and more than ten at ground-level galactic-cosmic-ray intensities, provided that the nucleation rate lies below the limiting ion-pair production rate. We find that ion-induced binary nucleation of H(2)SO(4)-H(2)O can occur in the mid-troposphere but is negligible in the boundary layer. However, even with the large enhancements in rate due to ammonia and ions, atmospheric concentrations of ammonia and sulphuric acid are insufficient to account for observed boundary-layer nucleation. |
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Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleationAerosolsNucleationCosmic raysAtmospheric aerosols exert an important influence on climate through their effects on stratiform cloud albedo and lifetime and the invigoration of convective storms. Model calculations suggest that almost half of the global cloud condensation nuclei in the atmospheric boundary layer may originate from the nucleation of aerosols from trace condensable vapours, although the sensitivity of the number of cloud condensation nuclei to changes of nucleation rate may be small. Despite extensive research, fundamental questions remain about the nucleation rate of sulphuric acid particles and the mechanisms responsible, including the roles of galactic cosmic rays and other chemical species such as ammonia. Here we present the first results from the CLOUD experiment at CERN. We find that atmospherically relevant ammonia mixing ratios of 100 parts per trillion by volume, or less, increase the nucleation rate of sulphuric acid particles more than 100-1,000-fold. Time-resolved molecular measurements reveal that nucleation proceeds by a base-stabilization mechanism involving the stepwise accretion of ammonia molecules. Ions increase the nucleation rate by an additional factor of between two and more than ten at ground-level galactic-cosmic-ray intensities, provided that the nucleation rate lies below the limiting ion-pair production rate. We find that ion-induced binary nucleation of H(2)SO(4)-H(2)O can occur in the mid-troposphere but is negligible in the boundary layer. However, even with the large enhancements in rate due to ammonia and ions, atmospheric concentrations of ammonia and sulphuric acid are insufficient to account for observed boundary-layer nucleation.uBibliorumKirkby, JasperCurtius, JoachimAlmeida, JoãoDunne, EimearDuplissy, JonathanEhrhart, SebastianFranchin, AlessandroGagné, StéphanieIckes, LuisaKürten, AndreasKupc, AgnieszkaMetzger, AxelRiccobono, FrancescoRondo, LindaSchobesberger, SiegfriedTsagkogeorgas, GeorgiosWimmer, DanielaAmorim, AntónioBianchi, FedericoBreitenlechner, MartinDavid, AndréDommen, JosefDownard, AndrewEhn, MikaelFlagan, RichardHaider, StefanHansel, ArminHauser, DanielJud, WernerJunninen, HeikkiKreissl, FabianKvashin, AlexanderLaaksonen, AriLehtipalo, KatrianneLima, JorgeLovejoy, Edward R.Makhmutov, VladimirMathot, SergeMikkilä, JyriMinginette, PierreMogo, SandraNieminen, TuomoOnnela, AnttiPereira, PauloPetäjä, TuukkaSchnitzhofer, RalfSeinfeld, JohnSipilä, MikkoStozhkov, YuriStratmann, FrankTomé, AntónioVanhanen, JoonasViisanen, YrjoVrtala, AronWagner, PaulWalther, HansueliWeingartner, ErnestWex, HeikeWinkler, PaulCarslaw, Kenneth S.Worsnop, DouglasBaltensperger, UrsKulmala, Markku2018-08-27T15:39:12Z20112011-01-01T00:00:00Zinfo:eu-repo/semantics/publishedVersioninfo:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10400.6/5755eng10.1038/nature10343metadata only accessinfo:eu-repo/semantics/openAccessreponame:Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos)instname:Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãoinstacron:RCAAP2024-02-21T03:38:56Zoai:ubibliorum.ubi.pt:10400.6/5755Portal AgregadorONGhttps://www.rcaap.pt/oai/openaireopendoar:71602024-03-20T00:46:32.892096Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informaçãofalse |
dc.title.none.fl_str_mv |
Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation |
title |
Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation |
spellingShingle |
Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation Kirkby, Jasper Aerosols Nucleation Cosmic rays |
title_short |
Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation |
title_full |
Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation |
title_fullStr |
Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation |
title_full_unstemmed |
Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation |
title_sort |
Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation |
author |
Kirkby, Jasper |
author_facet |
Kirkby, Jasper Curtius, Joachim Almeida, João Dunne, Eimear Duplissy, Jonathan Ehrhart, Sebastian Franchin, Alessandro Gagné, Stéphanie Ickes, Luisa Kürten, Andreas Kupc, Agnieszka Metzger, Axel Riccobono, Francesco Rondo, Linda Schobesberger, Siegfried Tsagkogeorgas, Georgios Wimmer, Daniela Amorim, António Bianchi, Federico Breitenlechner, Martin David, André Dommen, Josef Downard, Andrew Ehn, Mikael Flagan, Richard Haider, Stefan Hansel, Armin Hauser, Daniel Jud, Werner Junninen, Heikki Kreissl, Fabian Kvashin, Alexander Laaksonen, Ari Lehtipalo, Katrianne Lima, Jorge Lovejoy, Edward R. Makhmutov, Vladimir Mathot, Serge Mikkilä, Jyri Minginette, Pierre Mogo, Sandra Nieminen, Tuomo Onnela, Antti Pereira, Paulo Petäjä, Tuukka Schnitzhofer, Ralf Seinfeld, John Sipilä, Mikko Stozhkov, Yuri Stratmann, Frank Tomé, António Vanhanen, Joonas Viisanen, Yrjo Vrtala, Aron Wagner, Paul Walther, Hansueli Weingartner, Ernest Wex, Heike Winkler, Paul Carslaw, Kenneth S. Worsnop, Douglas Baltensperger, Urs Kulmala, Markku |
author_role |
author |
author2 |
Curtius, Joachim Almeida, João Dunne, Eimear Duplissy, Jonathan Ehrhart, Sebastian Franchin, Alessandro Gagné, Stéphanie Ickes, Luisa Kürten, Andreas Kupc, Agnieszka Metzger, Axel Riccobono, Francesco Rondo, Linda Schobesberger, Siegfried Tsagkogeorgas, Georgios Wimmer, Daniela Amorim, António Bianchi, Federico Breitenlechner, Martin David, André Dommen, Josef Downard, Andrew Ehn, Mikael Flagan, Richard Haider, Stefan Hansel, Armin Hauser, Daniel Jud, Werner Junninen, Heikki Kreissl, Fabian Kvashin, Alexander Laaksonen, Ari Lehtipalo, Katrianne Lima, Jorge Lovejoy, Edward R. Makhmutov, Vladimir Mathot, Serge Mikkilä, Jyri Minginette, Pierre Mogo, Sandra Nieminen, Tuomo Onnela, Antti Pereira, Paulo Petäjä, Tuukka Schnitzhofer, Ralf Seinfeld, John Sipilä, Mikko Stozhkov, Yuri Stratmann, Frank Tomé, António Vanhanen, Joonas Viisanen, Yrjo Vrtala, Aron Wagner, Paul Walther, Hansueli Weingartner, Ernest Wex, Heike Winkler, Paul Carslaw, Kenneth S. Worsnop, Douglas Baltensperger, Urs Kulmala, Markku |
author2_role |
author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author author |
dc.contributor.none.fl_str_mv |
uBibliorum |
dc.contributor.author.fl_str_mv |
Kirkby, Jasper Curtius, Joachim Almeida, João Dunne, Eimear Duplissy, Jonathan Ehrhart, Sebastian Franchin, Alessandro Gagné, Stéphanie Ickes, Luisa Kürten, Andreas Kupc, Agnieszka Metzger, Axel Riccobono, Francesco Rondo, Linda Schobesberger, Siegfried Tsagkogeorgas, Georgios Wimmer, Daniela Amorim, António Bianchi, Federico Breitenlechner, Martin David, André Dommen, Josef Downard, Andrew Ehn, Mikael Flagan, Richard Haider, Stefan Hansel, Armin Hauser, Daniel Jud, Werner Junninen, Heikki Kreissl, Fabian Kvashin, Alexander Laaksonen, Ari Lehtipalo, Katrianne Lima, Jorge Lovejoy, Edward R. Makhmutov, Vladimir Mathot, Serge Mikkilä, Jyri Minginette, Pierre Mogo, Sandra Nieminen, Tuomo Onnela, Antti Pereira, Paulo Petäjä, Tuukka Schnitzhofer, Ralf Seinfeld, John Sipilä, Mikko Stozhkov, Yuri Stratmann, Frank Tomé, António Vanhanen, Joonas Viisanen, Yrjo Vrtala, Aron Wagner, Paul Walther, Hansueli Weingartner, Ernest Wex, Heike Winkler, Paul Carslaw, Kenneth S. Worsnop, Douglas Baltensperger, Urs Kulmala, Markku |
dc.subject.por.fl_str_mv |
Aerosols Nucleation Cosmic rays |
topic |
Aerosols Nucleation Cosmic rays |
description |
Atmospheric aerosols exert an important influence on climate through their effects on stratiform cloud albedo and lifetime and the invigoration of convective storms. Model calculations suggest that almost half of the global cloud condensation nuclei in the atmospheric boundary layer may originate from the nucleation of aerosols from trace condensable vapours, although the sensitivity of the number of cloud condensation nuclei to changes of nucleation rate may be small. Despite extensive research, fundamental questions remain about the nucleation rate of sulphuric acid particles and the mechanisms responsible, including the roles of galactic cosmic rays and other chemical species such as ammonia. Here we present the first results from the CLOUD experiment at CERN. We find that atmospherically relevant ammonia mixing ratios of 100 parts per trillion by volume, or less, increase the nucleation rate of sulphuric acid particles more than 100-1,000-fold. Time-resolved molecular measurements reveal that nucleation proceeds by a base-stabilization mechanism involving the stepwise accretion of ammonia molecules. Ions increase the nucleation rate by an additional factor of between two and more than ten at ground-level galactic-cosmic-ray intensities, provided that the nucleation rate lies below the limiting ion-pair production rate. We find that ion-induced binary nucleation of H(2)SO(4)-H(2)O can occur in the mid-troposphere but is negligible in the boundary layer. However, even with the large enhancements in rate due to ammonia and ions, atmospheric concentrations of ammonia and sulphuric acid are insufficient to account for observed boundary-layer nucleation. |
publishDate |
2011 |
dc.date.none.fl_str_mv |
2011 2011-01-01T00:00:00Z 2018-08-27T15:39:12Z |
dc.type.status.fl_str_mv |
info:eu-repo/semantics/publishedVersion |
dc.type.driver.fl_str_mv |
info:eu-repo/semantics/article |
format |
article |
status_str |
publishedVersion |
dc.identifier.uri.fl_str_mv |
http://hdl.handle.net/10400.6/5755 |
url |
http://hdl.handle.net/10400.6/5755 |
dc.language.iso.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
10.1038/nature10343 |
dc.rights.driver.fl_str_mv |
metadata only access info:eu-repo/semantics/openAccess |
rights_invalid_str_mv |
metadata only access |
eu_rights_str_mv |
openAccess |
dc.format.none.fl_str_mv |
application/pdf |
dc.source.none.fl_str_mv |
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instacron_str |
RCAAP |
institution |
RCAAP |
reponame_str |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
collection |
Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) |
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Repositório Científico de Acesso Aberto de Portugal (Repositórios Cientìficos) - Agência para a Sociedade do Conhecimento (UMIC) - FCT - Sociedade da Informação |
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