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Molecular understanding of atmospheric particle formation from sulfuric acid and large oxidized organic molecules

Schobesberger, Siegfried and Downard, Andrew J. and Flagan, Richard C. and Junninen, Heikki and Bianchi, Federico and Lönn, Gustaf (2013) Molecular understanding of atmospheric particle formation from sulfuric acid and large oxidized organic molecules. Proceedings of the National Academy of Sciences of the United States of America, 110 (43). pp. 17223-17228. ISSN 0027-8424. PMCID PMC3808659. doi:10.1073/pnas.1306973110. https://resolver.caltech.edu/CaltechAUTHORS:20131125-131044563

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Abstract

Atmospheric aerosols formed by nucleation of vapors affect radiative forcing and therefore climate. However, the underlying mechanisms of nucleation remain unclear, particularly the involvement of organic compounds. Here, we present high-resolution mass spectra of ion clusters observed during new particle formation experiments performed at the Cosmics Leaving Outdoor Droplets chamber at the European Organization for Nuclear Research. The experiments involved sulfuric acid vapor and different stabilizing species, including ammonia and dimethylamine, as well as oxidation products of pinanediol, a surrogate for organic vapors formed from monoterpenes. A striking resemblance is revealed between the mass spectra from the chamber experiments with oxidized organics and ambient data obtained during new particle formation events at the Hyytiälä boreal forest research station. We observe that large oxidized organic compounds, arising from the oxidation of monoterpenes, cluster directly with single sulfuric acid molecules and then form growing clusters of one to three sulfuric acid molecules plus one to four oxidized organics. Most of these organic compounds retain 10 carbon atoms, and some of them are remarkably highly oxidized (oxygen-to-carbon ratios up to 1.2). The average degree of oxygenation of the organic compounds decreases while the clusters are growing. Our measurements therefore connect oxidized organics directly, and in detail, with the very first steps of new particle formation and their growth between 1 and 2 nm in a controlled environment. Thus, they confirm that oxidized organics are involved in both the formation and growth of particles under ambient conditions.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1073/pnas.1306973110DOIarticle
http://www.pnas.org/content/110/43/17223.abstractPublisherarticle
http://www.pnas.org/content/suppl/2013/10/03/1306973110.DCSupplementalPublisherSupplemental Material
http://www.ncbi.nlm.nih.gov/pubmed/?term=PMC3808659PubMed Centralabstract
ORCID:
AuthorORCID
Flagan, Richard C.0000-0001-5690-770X
Bianchi, Federico0000-0003-2996-3604
Additional Information:© 2013 National Academy of Sciences. Approved September 5, 2013 (received for review April 12, 2013). Published online before print October 7, 2013. The European Organization for Nuclear Research (CERN)’s support of CLOUD with important technical and financial resources and provision of a particle beam from the Proton Synchrotron is gratefully acknowledged. This research was funded by the European Commission 7th Framework Programme (Marie Curie Initial Training Network “CLOUD-ITN,” Grant 215072), the European Research Council (ERC) Advanced Grant Atmospheric nucleation: from molecular to global scale (ATMNUCLE) (Grant 227463), the ERC Starting Grant “Role of Molecular Clusters in Atmospheric Particle Formation (MOCAPAF)” (Grant 257360), the Academy of Finland via the Centre of Excellence Programme (Project 1118615) and Grant 1133872, the German Federal Ministry of Education and Research (Project 01LK0902A), the Swiss National Science Foundation (Projects 206621_125025 and 206620_130527), the Austrian Science Fund (Projects P19546 and L593), the Portuguese Foundation for Science and Technology (Project CERN/FP/116387/2010), the Russian Foundation for Basic Research (Grant N08-02-91006-CERN), the Davidow Foundation, the Royal Society Wolfson Research Award, and the US National Science Foundation (Grants AGS1136479 and CHE1012293).
Funders:
Funding AgencyGrant Number
Marie Curie Fellowship215072
European Research Council (ERC)227463
European Research Council (ERC)257360
Academy of Finland1118615
Academy of Finland1133872
Deutsche Forschungsgemeinschaft (DFG)01LK0902A
Swiss National Science Foundation (SNSF)206621_125025
Swiss National Science Foundation (SNSF)206620_130527
FWF Der WissenschaftsfondsP19546
FWF Der WissenschaftsfondsL593
Fundação para a Ciência e a Tecnologia (FCT)CERN/FP/116387/2010
Russian Foundation for Basic ResearchN08-02-91006-CERN
Davidow FoundationUNSPECIFIED
Royal SocietyUNSPECIFIED
NSFAGS-1136479
NSFCHE-1012293
Subject Keywords:aerosol particles ; atmospheric nucleation ; atmospheric chemistry ;mass spectrometry
Issue or Number:43
PubMed Central ID:PMC3808659
DOI:10.1073/pnas.1306973110
Record Number:CaltechAUTHORS:20131125-131044563
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20131125-131044563
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:42686
Collection:CaltechAUTHORS
Deposited By: Juan Valdivia
Deposited On:26 Nov 2013 18:23
Last Modified:10 Nov 2021 16:26

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