Molecular understanding of atmospheric particle formation from sulfuric acid and large oxidized organic molecules
Siegfried Schobesberger,Heikki Junninen,F. Bianchi,Gustaf Lönn,Mikael Ehn,Katrianne Lehtipalo,Josef Dommen,Sebastian Ehrhart,Ismael K. Ortega,Alessandro Franchin,Tuomo Nieminen,Francesco Riccobono,Manuel Hutterli,Jonathan Duplissy,Joao Almeida,António Amorim,Martin Breitenlechner,Andrew J. Downard,Eimear M. Dunne,Eimear M. Dunne,Richard C. Flagan,Maija Kajos,Helmi Keskinen,Jasper Kirkby,Agnieszka Kupc,Andreas Kürten,Theo Kurtén,Ari Laaksonen,Ari Laaksonen,Serge Mathot,Antti Onnela,Arnaud P. Praplan,Linda Rondo,Filipe Duarte Santos,Simon Schallhart,R. Schnitzhofer,Mikko Sipilä,António Tomé,Georgios Tsagkogeorgas,Hanna Vehkamäki,Daniela Wimmer,Daniela Wimmer,Urs Baltensperger,Kenneth S. Carslaw,Joachim Curtius,Armin Hansel,Tuukka Petäjä,Markku Kulmala,Neil M. Donahue,Douglas R. Worsnop +49 more
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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 confirm that oxidized organics are involved in both the formation and growth of particles under ambient conditions.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 Hyytiala 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.read more
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Journal ArticleDOI
The role of low-volatility organic compounds in initial particle growth in the atmosphere
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TL;DR: It is shown that organic vapours alone can drive nucleation, and a particle growth model is presented that quantitatively reproduces the measurements and implements a parameterization of the first steps of growth in a global aerosol model that can change substantially in response to concentrations of atmospheric cloud concentration nuclei.
Journal ArticleDOI
Ion-induced nucleation of pure biogenic particles
Jasper Kirkby,Jasper Kirkby,Jonathan Duplissy,Jonathan Duplissy,Kamalika Sengupta,Carla Frege,Hamish Gordon,Christina Williamson,Christina Williamson,Martin Heinritzi,Martin Heinritzi,Mario Simon,Chao Yan,Joao Almeida,Joao Almeida,Jasmin Tröstl,Tuomo Nieminen,Tuomo Nieminen,Ismael K. Ortega,Robert Wagner,Alexey Adamov,António Amorim,Anne-Kathrin Bernhammer,F. Bianchi,F. Bianchi,Martin Breitenlechner,Sophia Brilke,Xuemeng Chen,J. S. Craven,Antonio Dias,Sebastian Ehrhart,Sebastian Ehrhart,Richard C. Flagan,Alessandro Franchin,Claudia Fuchs,Roberto Guida,Jani Hakala,Christopher R. Hoyle,Tuija Jokinen,Heikki Junninen,Juha Kangasluoma,Jaeseok Kim,Jaeseok Kim,Manuel Krapf,Andreas Kürten,Ari Laaksonen,Ari Laaksonen,Katrianne Lehtipalo,Katrianne Lehtipalo,Vladimir Makhmutov,Serge Mathot,Ugo Molteni,Antti Onnela,Otso Peräkylä,Felix Piel,Tuukka Petäjä,Arnaud P. Praplan,Kirsty J. Pringle,Alexandru Rap,N. A. D. Richards,Ilona Riipinen,Matti P. Rissanen,Linda Rondo,Nina Sarnela,Siegfried Schobesberger,Siegfried Schobesberger,Catherine E. Scott,John H. Seinfeld,Mikko Sipilä,Mikko Sipilä,Gerhard Steiner,Gerhard Steiner,Gerhard Steiner,Yuri Stozhkov,Frank Stratmann,António Tomé,Annele Virtanen,Alexander L. Vogel,Andrea Christine Wagner,Paul E. Wagner,Ernest Weingartner,Daniela Wimmer,Daniela Wimmer,Paul M. Winkler,Penglin Ye,Xuan Zhang,Armin Hansel,Josef Dommen,Neil M. Donahue,Douglas R. Worsnop,Douglas R. Worsnop,Urs Baltensperger,Markku Kulmala,Markku Kulmala,Kenneth S. Carslaw,Joachim Curtius +95 more
TL;DR: Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.
Journal ArticleDOI
Multiphase chemistry at the atmosphere-biosphere interface influencing climate and public health in the anthropocene.
Ulrich Pöschl,Manabu Shiraiwa +1 more
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Journal ArticleDOI
Oxidation products of biogenic emissions contribute to nucleation of atmospheric particles.
Francesco Riccobono,Siegfried Schobesberger,Catherine E. Scott,Josef Dommen,Ismael K. Ortega,Linda Rondo,Joao Almeida,António Amorim,F. Bianchi,Martin Breitenlechner,A. David,Andrew J. Downard,Eimear M. Dunne,Jonathan Duplissy,Jonathan Duplissy,Sebastian Ehrhart,Richard C. Flagan,Alessandro Franchin,Armin Hansel,Heikki Junninen,Maija Kajos,Helmi Keskinen,Agnieszka Kupc,Andreas Kürten,Alexander N. Kvashin,Ari Laaksonen,Katrianne Lehtipalo,Vladimir Makhmutov,Serge Mathot,Tuomo Nieminen,Tuomo Nieminen,Antti Onnela,Tuukka Petäjä,Arnaud P. Praplan,Filipe Duarte Santos,Simon Schallhart,John H. Seinfeld,Mikko Sipilä,Mikko Sipilä,Dominick V. Spracklen,Yuri Stozhkov,Frank Stratmann,António Tomé,Georgios Tsagkogeorgas,Petri Vaattovaara,Yrjö Viisanen,Aron Vrtala,Paul E. Wagner,Ernest Weingartner,Heike Wex,Daniela Wimmer,Kenneth S. Carslaw,Joachim Curtius,Neil M. Donahue,Jasper Kirkby,Jasper Kirkby,Markku Kulmala,Markku Kulmala,Douglas R. Worsnop,Urs Baltensperger +59 more
TL;DR: It is shown, in experiments performed with the CLOUD (Cosmics Leaving Outdoor Droplets) chamber at CERN, that sulfuric acid and oxidized organic vapors at atmospheric concentrations reproduce particle nucleation rates observed in the lower atmosphere.
Journal ArticleDOI
Highly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key Contributor to Atmospheric Aerosol
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TL;DR: This Review defines HOM and describes the currently available techniques for their identification/quantification, followed by a summary of the current knowledge on their formation mechanisms and physicochemical properties.
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Shih Chen Wang,Richard C. Flagan +1 more
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