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Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation

2011Journal article Restricted access
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dc.contributor.authorKirkby, Jasper
dc.contributor.authorCurtius, Joachim
dc.contributor.authorAlmeida, João
dc.contributor.authorDunne, Eimear
dc.contributor.authorDuplissy, Jonathan
dc.contributor.authorEhrhart, Sebastian
dc.contributor.authorFranchin, Alessandro
dc.contributor.authorGagné, Stéphanie
dc.contributor.authorIckes, Luisa
dc.contributor.authorKürten, Andreas
dc.contributor.authorKupc, Agnieszka
dc.contributor.authorMetzger, Axel
dc.contributor.authorRiccobono, Francesco
dc.contributor.authorRondo, Linda
dc.contributor.authorSchobesberger, Siegfried
dc.contributor.authorTsagkogeorgas, Georgios
dc.contributor.authorWimmer, Daniela
dc.contributor.authorAmorim, António
dc.contributor.authorBianchi, Federico
dc.contributor.authorBreitenlechner, Martin
dc.contributor.authorDavid, André
dc.contributor.authorDommen, Josef
dc.contributor.authorDownard, Andrew
dc.contributor.authorEhn, Mikael
dc.contributor.authorFlagan, Richard
dc.contributor.authorHaider, Stefan
dc.contributor.authorHansel, Armin
dc.contributor.authorHauser, Daniel
dc.contributor.authorJud, Werner
dc.contributor.authorJunninen, Heikki
dc.contributor.authorKreissl, Fabian
dc.contributor.authorKvashin, Alexander
dc.contributor.authorLaaksonen, Ari
dc.contributor.authorLehtipalo, Katrianne
dc.contributor.authorLima, Jorge
dc.contributor.authorLovejoy, Edward R.
dc.contributor.authorMakhmutov, Vladimir
dc.contributor.authorMathot, Serge
dc.contributor.authorMikkilä, Jyri
dc.contributor.authorMinginette, Pierre
dc.contributor.authorMogo, Sandra
dc.contributor.authorNieminen, Tuomo
dc.contributor.authorOnnela, Antti
dc.contributor.authorPereira, Paulo
dc.contributor.authorPetäjä, Tuukka
dc.contributor.authorSchnitzhofer, Ralf
dc.contributor.authorSeinfeld, John
dc.contributor.authorSipilä, Mikko
dc.contributor.authorStozhkov, Yuri
dc.contributor.authorStratmann, Frank
dc.contributor.authorTomé, António
dc.contributor.authorVanhanen, Joonas
dc.contributor.authorViisanen, Yrjo
dc.contributor.authorVrtala, Aron
dc.contributor.authorWagner, Paul
dc.contributor.authorWalther, Hansueli
dc.contributor.authorWeingartner, Ernest
dc.contributor.authorWex, Heike
dc.contributor.authorWinkler, Paul
dc.contributor.authorCarslaw, Kenneth S.
dc.contributor.authorWorsnop, Douglas
dc.contributor.authorBaltensperger, Urs
dc.contributor.authorKulmala, Markku
dc.date.accessioned2018-08-27T15:39:12Z
dc.date.available2018-08-27T15:39:12Z
dc.date.issued2011
dc.description.abstractAtmospheric 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.pt_PT
dc.description.versioninfo:eu-repo/semantics/publishedVersionpt_PT
dc.identifier.doi10.1038/nature10343pt_PT
dc.identifier.urihttp://hdl.handle.net/10400.6/5755
dc.language.isoengpt_PT
dc.peerreviewedyespt_PT
dc.subjectAerosolspt_PT
dc.subjectNucleationpt_PT
dc.subjectCosmic rayspt_PT
dc.titleRole of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleationpt_PT
dc.typejournal article
dspace.entity.typePublication
oaire.citation.endPage433pt_PT
oaire.citation.issue7361pt_PT
oaire.citation.startPage429pt_PT
oaire.citation.titleNaturept_PT
oaire.citation.volume476pt_PT
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rcaap.embargofctCopyright cedido à editora no momento da publicação.pt_PT
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