From quantum chemical formation free energies to evaporation rates
Ismael K. Ortega,Oona Kupiainen,Theo Kurtén,Tinja Olenius,Olli Wilkman,Matthew J. McGrath,Ville Loukonen,Hanna Vehkamäki +7 more
TLDR
In this paper, the authors used formation free energies calculated by quantum chemical methods to estimate the evaporation rates of species from sulfuric acid clusters containing ammonia or dimethylamine.Abstract:
. Atmospheric new particle formation is an important source of atmospheric aerosols. Large efforts have been made during the past few years to identify which molecules are behind this phenomenon, but the actual birth mechanism of the particles is not yet well known. Quantum chemical calculations have proven to be a powerful tool to gain new insights into the very first steps of particle formation. In the present study we use formation free energies calculated by quantum chemical methods to estimate the evaporation rates of species from sulfuric acid clusters containing ammonia or dimethylamine. We have found that dimethylamine forms much more stable clusters with sulphuric acid than ammonia does. On the other hand, the existence of a very deep local minimum for clusters with two sulfuric acid molecules and two dimethylamine molecules hinders their growth to larger clusters. These results indicate that other compounds may be needed to make clusters grow to larger sizes (containing more than three sulfuric acid molecules).read more
Citations
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Journal ArticleDOI
Direct observations of atmospheric aerosol nucleation.
Markku Kulmala,Jenni Kontkanen,Heikki Junninen,Katrianne Lehtipalo,Hanna E. Manninen,Tuomo Nieminen,Tuomo Nieminen,Tuukka Petäjä,Mikko Sipilä,Siegfried Schobesberger,Pekka Rantala,Alessandro Franchin,Tuija Jokinen,Emma Järvinen,Mikko Äijälä,Juha Kangasluoma,Jani Hakala,P. P. Aalto,Pauli Paasonen,Jyri Mikkilä,Joonas Vanhanen,Juho Aalto,Hannele Hakola,Ulla Makkonen,Taina Ruuskanen,Roy L. Mauldin,Roy L. Mauldin,Jonathan Duplissy,Hanna Vehkamäki,Jaana Bäck,Aki Kortelainen,Ilona Riipinen,Theo Kurtén,Murray V. Johnston,James N. Smith,James N. Smith,Mikael Ehn,Mikael Ehn,Thomas F. Mentel,Kari E. J. Lehtinen,Kari E. J. Lehtinen,Ari Laaksonen,Ari Laaksonen,Veli-Matti Kerminen,Douglas R. Worsnop +44 more
TL;DR: Three separate size regimes below 2-nm diameter are identified that build up a physically, chemically, and dynamically consistent framework on atmospheric nucleation—more specifically, aerosol formation via neutral pathways.
Journal ArticleDOI
Molecular understanding of sulphuric acid-amine particle nucleation in the atmosphere
Joao Almeida,Joao Almeida,Siegfried Schobesberger,Andreas Kürten,Ismael K. Ortega,Oona Kupiainen-Määttä,Arnaud P. Praplan,Alexey Adamov,António Amorim,F. Bianchi,Martin Breitenlechner,A. David,Josef Dommen,Neil M. Donahue,Andrew J. Downard,Eimear M. Dunne,Jonathan Duplissy,Sebastian Ehrhart,Richard C. Flagan,Alessandro Franchin,Roberto Guida,Jani Hakala,Armin Hansel,Martin Heinritzi,Henning Henschel,Tuija Jokinen,Heikki Junninen,Maija Kajos,Juha Kangasluoma,Helmi Keskinen,Agnieszka Kupc,Theo Kurtén,Alexander N. Kvashin,Ari Laaksonen,Ari Laaksonen,Katrianne Lehtipalo,Markus Leiminger,Johannes Leppä,Ville Loukonen,Vladimir Makhmutov,Serge Mathot,Matthew J. McGrath,Tuomo Nieminen,Tuomo Nieminen,Tinja Olenius,Antti Onnela,Tuukka Petäjä,Francesco Riccobono,Ilona Riipinen,Matti P. Rissanen,Linda Rondo,Taina Ruuskanen,Filipe Duarte Santos,Nina Sarnela,Simon Schallhart,R. Schnitzhofer,John H. Seinfeld,Mario Simon,Mikko Sipilä,Mikko Sipilä,Yuri Stozhkov,Frank Stratmann,António Tomé,Jasmin Tröstl,Georgios Tsagkogeorgas,Petri Vaattovaara,Yrjö Viisanen,Annele Virtanen,Aron Vrtala,Paul E. Wagner,Ernest Weingartner,Heike Wex,Christina Williamson,Daniela Wimmer,Daniela Wimmer,Penglin Ye,Taina Yli-Juuti,Kenneth S. Carslaw,Markku Kulmala,Markku Kulmala,Joachim Curtius,Urs Baltensperger,Douglas R. Worsnop,Hanna Vehkamäki,Jasper Kirkby,Jasper Kirkby +85 more
TL;DR: The 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.
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
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
Modelling of fuel droplet heating and evaporation: Recent results and unsolved problems
TL;DR: The most recent developments in the modelling of heating and evaporation of fuel droplets, the results of which were published in 2014-2017, are reviewed, and the most important unsolved problems are identified.
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