Ion-induced nucleation of pure biogenic particles

Jasper Kirkby; Jonathan Duplissy; Kamalika Sengupta; Carla Frege; Hamish Gordon; Christina Williamson; Martin Heinritzi; Mario Simon; Chao Yan; Joao Almeida; Jasmin Troestl; Tuomo Nieminen; Ismael K. Ortega; Robert Wagner; Alexey Adamov; Antonio Amorim; Anne-Kathrin Bernhammer; Federico Bianchi; Martin Breitenlechner; Sophia Brilke; Xuemeng Chen; Jill Craven; Antonio Dias; Sebastian Ehrhart; Richard C. Flagan; Alessandro Franchin; Claudia Fuchs; Roberto Guida; Jani Hakala; Christopher R. Hoyle; Tuija Jokinen; Heikki Junninen; Juha Kangasluoma; Jaeseok Kim; Manuel Krapf; Andreas Kuerten; Ari Laaksonen; Katrianne Lehtipalo; Vladimir Makhmutov; Serge Mathot; Ugo Molteni; Antti Onnela; Otso Peraekylae; Felix Piel; Tuukka Petaejae; Arnaud P. Praplan; Kirsty Pringle; Alexandru Rap; Nigel A. D. Richards; Ilona Riipinen; Matti P. Rissanen; Linda Rondo; Nina Sarnela; Siegfried Schobesberger; Catherine E. Scott; John H. Seinfeld; Mikko Sipilae; Gerhard Steiner; Yuri Stozhkov; Frank Stratmann; Antonio Tome; Annele Virtanen; Alexander L. Vogel; Andrea C. Wagner; Paul E. Wagner; Ernest Weingartner; Daniela Wimmer; Paul M. Winkler; Penglin Ye; Xuan Zhang; Armin Hansel; Josef Dommen; Neil M. Donahue; Douglas R. Worsnop; Urs Baltensperger; Markku Kulmala; Kenneth S. Carslaw; Joachim Curtius

doi:10.1038/nature17953

Ion-induced nucleation of pure biogenic particles

Jasper Kirkby (Corresponding author)
, Jonathan Duplissy
, Kamalika Sengupta
, Carla Frege
, Hamish Gordon
, Christina Williamson
, Martin Heinritzi
, Mario Simon
, Chao Yan
, Joao Almeida
, Jasmin Troestl
, Tuomo Nieminen
, Ismael K. Ortega
, Robert Wagner
, Alexey Adamov
, Antonio Amorim
, Anne-Kathrin Bernhammer
, Federico Bianchi
, Martin Breitenlechner
, Sophia Brilke

Xuemeng Chen, Jill Craven, Antonio Dias, Sebastian Ehrhart, Richard C. Flagan, Alessandro Franchin, Claudia Fuchs, Roberto Guida, Jani Hakala, Christopher R. Hoyle, Tuija Jokinen, Heikki Junninen, Juha Kangasluoma, Jaeseok Kim, Manuel Krapf, Andreas Kuerten, Ari Laaksonen, Katrianne Lehtipalo, Vladimir Makhmutov, Serge Mathot, Ugo Molteni, Antti Onnela, Otso Peraekylae, Felix Piel, Tuukka Petaejae, Arnaud P. Praplan, Kirsty Pringle, Alexandru Rap, Nigel A. D. Richards, Ilona Riipinen, Matti P. Rissanen, Linda Rondo, Nina Sarnela, Siegfried Schobesberger, Catherine E. Scott, John H. Seinfeld, Mikko Sipilae, Gerhard Steiner, Yuri Stozhkov, Frank Stratmann, Antonio Tome, Annele Virtanen, Alexander L. Vogel, Andrea C. Wagner, Paul E. Wagner, Ernest Weingartner, Daniela Wimmer, Paul M. Winkler, Penglin Ye, Xuan Zhang, Armin Hansel, Josef Dommen, Neil M. Donahue, Douglas R. Worsnop, Urs Baltensperger, Markku Kulmala, Kenneth S. Carslaw, Joachim Curtius

Aerosol Physics and Environmental Physics

Publications: Contribution to journal › Article › Peer Reviewed

Abstract

Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere, and that ions have a relatively minor role. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.

Original language	English
Pages (from-to)	521-526
Number of pages	6
Journal	Nature
Volume	533
Issue number	7604
DOIs	https://doi.org/10.1038/nature17953
Publication status	Published - 26 May 2016

Funding

We thank CERN for supporting CLOUD with important technical and financial resources, and for providing a particle beam from the CERN Proton Synchrotron. We also thank P. Carrie, L.-P. De Menezes, J. Dumollard, F. Josa, I. Krasin, R. Kristic, A. Laassiri, O. S. Maksumov, B. Marichy, H. Martinati, S. V. Mizin, R. Sitals, A. Wasem and M. Wilhelmsson for their contributions to the experiment. We thank the CSC Centre for Scientific Computing in Espoo, Finland for computer time. This research has received funding from the EC Seventh Framework Programme (Marie Curie Initial Training Network MC-ITN CLOUD-TRAIN no. 316662, EU Horizon 2020 Marie Curie grant no. 656994, ERC-Consolidator grant NANODYNAMITE no. 616075 and ERC-Advanced grant ATMNUCLE no. 227463), the German Federal Ministry of Education and Research (project no. 01LK1222A), the Swiss National Science Foundation (project nos 200020_135307, 200021_140663, 206021_144947/1 and 20FI20_149002/1), the Academy of Finland (Center of Excellence project no. 1118615), the Academy of Finland (135054, 133872, 251427, 139656, 139995, 137749, 141217, 141451), the Finnish Funding Agency for Technology and Innovation, the Vaisala Foundation, the Nessling Foundation, the Austrian Science Fund (FWF; project no. L593), the Portuguese Foundation for Science and Technology (project no. CERN/FP/116387/2010), the Swedish Research Council, Vetenskapsradet (grant 2011-5120), the Presidium of the Russian Academy of Sciences and Russian Foundation for Basic Research (grant 12-02-91522-CERN), the UK Natural Environment Research Council (grant NE/K015966/1), the Royal Society (Wolfson Merit Award), the US National Science Foundation (grants AGS1136479, AGS1447056 and CHE1012293), Caltech ESE Grant (Davidow Foundation), Dreyfus Award EP-11-117, the French National Research Agency (ANR), the Nord-Pas de Calais, and the European Funds for Regional Economic Development (FEDER, Labex-Cappa, ANR-11-LABX-0005-01).

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 13 Climate Action

Austrian Fields of Science 2012

103039 Aerosol physics
105206 Meteorology

Keywords

SECONDARY ORGANIC AEROSOL
ATMOSPHERIC SULFURIC-ACID
GASEOUS NITROUS-ACID
ALPHA-PINENE
OZONOLYSIS PRODUCTS
MASS-SPECTROMETER
MOLECULAR-WEIGHT
SIZE MAGNIFIER
COSMIC-RAYS
GROWTH

Access to Document

10.1038/nature17953

Cite this

Kirkby, J., Duplissy, J., Sengupta, K., Frege, C., Gordon, H., Williamson, C., Heinritzi, M., Simon, M., Yan, C., Almeida, J., Troestl, J., Nieminen, T., Ortega, I. K., Wagner, R., Adamov, A., Amorim, A., Bernhammer, A.-K., Bianchi, F., Breitenlechner, M., ... Curtius, J. (2016). Ion-induced nucleation of pure biogenic particles. Nature, 533(7604), 521-526. https://doi.org/10.1038/nature17953

@article{bb1d299d6feb415597dbcdf11a1e642c,

title = "Ion-induced nucleation of pure biogenic particles",

abstract = "Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere, and that ions have a relatively minor role. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.",

keywords = "SECONDARY ORGANIC AEROSOL, ATMOSPHERIC SULFURIC-ACID, GASEOUS NITROUS-ACID, ALPHA-PINENE, OZONOLYSIS PRODUCTS, MASS-SPECTROMETER, MOLECULAR-WEIGHT, SIZE MAGNIFIER, COSMIC-RAYS, GROWTH",

author = "Jasper Kirkby and Jonathan Duplissy and Kamalika Sengupta and Carla Frege and Hamish Gordon and Christina Williamson and Martin Heinritzi and Mario Simon and Chao Yan and Joao Almeida and Jasmin Troestl and Tuomo Nieminen and Ortega, \{Ismael K.\} and Robert Wagner and Alexey Adamov and Antonio Amorim and Anne-Kathrin Bernhammer and Federico Bianchi and Martin Breitenlechner and Sophia Brilke and Xuemeng Chen and Jill Craven and Antonio Dias and Sebastian Ehrhart and Flagan, \{Richard C.\} and Alessandro Franchin and Claudia Fuchs and Roberto Guida and Jani Hakala and Hoyle, \{Christopher R.\} and Tuija Jokinen and Heikki Junninen and Juha Kangasluoma and Jaeseok Kim and Manuel Krapf and Andreas Kuerten and Ari Laaksonen and Katrianne Lehtipalo and Vladimir Makhmutov and Serge Mathot and Ugo Molteni and Antti Onnela and Otso Peraekylae and Felix Piel and Tuukka Petaejae and Praplan, \{Arnaud P.\} and Kirsty Pringle and Alexandru Rap and Richards, \{Nigel A. D.\} and Ilona Riipinen and Rissanen, \{Matti P.\} and Linda Rondo and Nina Sarnela and Siegfried Schobesberger and Scott, \{Catherine E.\} and Seinfeld, \{John H.\} and Mikko Sipilae and Gerhard Steiner and Yuri Stozhkov and Frank Stratmann and Antonio Tome and Annele Virtanen and Vogel, \{Alexander L.\} and Wagner, \{Andrea C.\} and Wagner, \{Paul E.\} and Ernest Weingartner and Daniela Wimmer and Winkler, \{Paul M.\} and Penglin Ye and Xuan Zhang and Armin Hansel and Josef Dommen and Donahue, \{Neil M.\} and Worsnop, \{Douglas R.\} and Urs Baltensperger and Markku Kulmala and Carslaw, \{Kenneth S.\} and Joachim Curtius",

year = "2016",

month = may,

day = "26",

doi = "10.1038/nature17953",

language = "English",

volume = "533",

pages = "521--526",

journal = "Nature",

issn = "0028-0836",

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Kirkby, J, Duplissy, J, Sengupta, K, Frege, C, Gordon, H, Williamson, C, Heinritzi, M, Simon, M, Yan, C, Almeida, J, Troestl, J, Nieminen, T, Ortega, IK, Wagner, R, Adamov, A, Amorim, A, Bernhammer, A-K, Bianchi, F, Breitenlechner, M, Brilke, S, Chen, X, Craven, J, Dias, A, Ehrhart, S, Flagan, RC, Franchin, A, Fuchs, C, Guida, R, Hakala, J, Hoyle, CR, Jokinen, T, Junninen, H, Kangasluoma, J, Kim, J, Krapf, M, Kuerten, A, Laaksonen, A, Lehtipalo, K, Makhmutov, V, Mathot, S, Molteni, U, Onnela, A, Peraekylae, O, Piel, F, Petaejae, T, Praplan, AP, Pringle, K, Rap, A, Richards, NAD, Riipinen, I, Rissanen, MP, Rondo, L, Sarnela, N, Schobesberger, S, Scott, CE, Seinfeld, JH, Sipilae, M, Steiner, G, Stozhkov, Y, Stratmann, F, Tome, A, Virtanen, A, Vogel, AL, Wagner, AC, Wagner, PE, Weingartner, E, Wimmer, D, Winkler, PM, Ye, P, Zhang, X, Hansel, A, Dommen, J, Donahue, NM, Worsnop, DR, Baltensperger, U, Kulmala, M, Carslaw, KS & Curtius, J 2016, 'Ion-induced nucleation of pure biogenic particles', Nature, vol. 533, no. 7604, pp. 521-526. https://doi.org/10.1038/nature17953

TY - JOUR

T1 - Ion-induced nucleation of pure biogenic particles

AU - Kirkby, Jasper

AU - Duplissy, Jonathan

AU - Sengupta, Kamalika

AU - Frege, Carla

AU - Gordon, Hamish

AU - Williamson, Christina

AU - Heinritzi, Martin

AU - Simon, Mario

AU - Yan, Chao

AU - Almeida, Joao

AU - Troestl, Jasmin

AU - Nieminen, Tuomo

AU - Ortega, Ismael K.

AU - Wagner, Robert

AU - Adamov, Alexey

AU - Amorim, Antonio

AU - Bernhammer, Anne-Kathrin

AU - Bianchi, Federico

AU - Breitenlechner, Martin

AU - Brilke, Sophia

AU - Chen, Xuemeng

AU - Craven, Jill

AU - Dias, Antonio

AU - Ehrhart, Sebastian

AU - Flagan, Richard C.

AU - Franchin, Alessandro

AU - Fuchs, Claudia

AU - Guida, Roberto

AU - Hakala, Jani

AU - Hoyle, Christopher R.

AU - Jokinen, Tuija

AU - Junninen, Heikki

AU - Kangasluoma, Juha

AU - Kim, Jaeseok

AU - Krapf, Manuel

AU - Kuerten, Andreas

AU - Laaksonen, Ari

AU - Lehtipalo, Katrianne

AU - Makhmutov, Vladimir

AU - Mathot, Serge

AU - Molteni, Ugo

AU - Onnela, Antti

AU - Peraekylae, Otso

AU - Piel, Felix

AU - Petaejae, Tuukka

AU - Praplan, Arnaud P.

AU - Pringle, Kirsty

AU - Rap, Alexandru

AU - Richards, Nigel A. D.

AU - Riipinen, Ilona

AU - Rissanen, Matti P.

AU - Rondo, Linda

AU - Sarnela, Nina

AU - Schobesberger, Siegfried

AU - Scott, Catherine E.

AU - Seinfeld, John H.

AU - Sipilae, Mikko

AU - Steiner, Gerhard

AU - Stozhkov, Yuri

AU - Stratmann, Frank

AU - Tome, Antonio

AU - Virtanen, Annele

AU - Vogel, Alexander L.

AU - Wagner, Andrea C.

AU - Wagner, Paul E.

AU - Weingartner, Ernest

AU - Wimmer, Daniela

AU - Winkler, Paul M.

AU - Ye, Penglin

AU - Zhang, Xuan

AU - Hansel, Armin

AU - Dommen, Josef

AU - Donahue, Neil M.

AU - Worsnop, Douglas R.

AU - Baltensperger, Urs

AU - Kulmala, Markku

AU - Carslaw, Kenneth S.

AU - Curtius, Joachim

PY - 2016/5/26

Y1 - 2016/5/26

N2 - Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere, and that ions have a relatively minor role. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.

AB - Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere, and that ions have a relatively minor role. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.

KW - SECONDARY ORGANIC AEROSOL

KW - ATMOSPHERIC SULFURIC-ACID

KW - GASEOUS NITROUS-ACID

KW - ALPHA-PINENE

KW - OZONOLYSIS PRODUCTS

KW - MASS-SPECTROMETER

KW - MOLECULAR-WEIGHT

KW - SIZE MAGNIFIER

KW - COSMIC-RAYS

KW - GROWTH

UR - https://www.scopus.com/pages/publications/84971327870

U2 - 10.1038/nature17953

DO - 10.1038/nature17953

M3 - Article

SN - 0028-0836

VL - 533

SP - 521

EP - 526

JO - Nature

JF - Nature

IS - 7604

ER -

Ion-induced nucleation of pure biogenic particles

Abstract

Funding

UN SDGs

Austrian Fields of Science 2012

Keywords

Access to Document

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NANODYNAMITE: Quantifying Aerosol Nanoparticle Dynamics by High Time Resolution Experiments

Cite this

Ion-induced nucleation of pure biogenic particles

Abstract

Funding

UN SDGs

Austrian Fields of Science 2012

Keywords

Access to Document

Other files and links

Fingerprint

Projects

NANODYNAMITE: Quantifying Aerosol Nanoparticle Dynamics by High Time Resolution Experiments

Cite this