Elemental composition and clustering behaviour of α-pinene oxidation products for different oxidation conditions

A. P. Praplan; S. Schobesberger; F. Bianchi; M. P. Rissanen; M. Ehn; T. Jokinen; H. Junninen; A. Adamov; A. Amorim; J. Dommen; J. Duplissy; J. Hakala; A. Hansel; M. Heinritzi; J. Kangasluoma; J. Kirkby; M. Krapf; A. Kürten; K. Lehtipalo; F. Riccobono; L. Rondo; N. Sarnela; M. Simon; A. Tome; J. Troestl; P. M. Winkler; C. Williamson; P. Ye; J. Curtius; U. Baltensperger; N. M. Donahue; M. Kulmala; D. R. Worsnop

doi:10.5194/acp-15-4145-2015

Elemental composition and clustering behaviour of α-pinene oxidation products for different oxidation conditions

A. P. Praplan (Corresponding author)
, S. Schobesberger
, F. Bianchi
, M. P. Rissanen
, M. Ehn
, T. Jokinen
, H. Junninen
, A. Adamov
, A. Amorim
, J. Dommen
, J. Duplissy
, J. Hakala
, A. Hansel
, M. Heinritzi
, J. Kangasluoma
, J. Kirkby
, M. Krapf
, A. Kürten
, K. Lehtipalo
, F. Riccobono

L. Rondo, N. Sarnela, M. Simon, A. Tome, J. Troestl, P. M. Winkler, C. Williamson, P. Ye, J. Curtius, U. Baltensperger, N. M. Donahue, M. Kulmala, D. R. Worsnop

Aerosol Physics and Environmental Physics

Publications: Contribution to journal › Article › Peer Reviewed

Abstract

This study presents the difference between oxidised organic compounds formed by alpha-pinene oxidation under various conditions in the CLOUD environmental chamber: (1) pure ozonolysis (in the presence of hydrogen as hydroxyl radical (OH) scavenger) and (2) OH oxidation (initiated by nitrous acid (HONO) photolysis by ultraviolet light) in the absence of ozone.
We discuss results from three Atmospheric Pressure interface Time-of-Flight (APi-TOF) mass spectrometers measuring simultaneously the composition of naturally charged as well as neutral species (via chemical ionisation with nitrate). Natural chemical ionisation takes place in the CLOUD chamber and organic oxidised compounds form clusters with nitrate, bisulfate, bisulfate/sulfuric acid clusters, ammonium, and dimethylaminium, or get protonated. The results from this study show that this process is selective for various oxidised organic compounds with low molar mass and ions, so that in order to obtain a comprehensive picture of the elemental composition of oxidation products and their clustering behaviour, several instruments must be used. We compare oxidation products containing 10 and 20 carbon atoms and show that highly oxidised organic compounds are formed in the early stages of the oxidation.

Original language	English
Pages (from-to)	4145-4159
Number of pages	15
Journal	Atmospheric Chemistry and Physics
Volume	15
Issue number	8
DOIs	https://doi.org/10.5194/acp-15-4145-2015
Publication status	Published - 22 Apr 2015

Funding

We would like to 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, K. Ivanova, 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 important contributions to the experiment. This research has received funding from the EC Seventh Framework Programme (Marie Curie Initial Training Network "CLOUD-ITN" no. 215072, MC-ITN "CLOUD-TRAIN" no. 316662, ERC-Starting "MOCAPAF" grant no. 57360 and ERC-Advanced "ATMNUCLE" grant no. 227463), PEGASOS project funded by the European Commission under the Framework Programme 7 (FP7-ENV-2010-265148), the German Federal Ministry of Education and Research (project nos. 01LK0902A and 01LK1222A), the Swiss National Science Foundation (project nos. 200020_135307 and 206620_141278), 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. J3198-N21), 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 (grants 08-02-91006-CERN and 12-02-91522-CERN), the U.S. National Science Foundation (grants AGS1136479 and CHE1012293), and the Davidow Foundation. We thank the tofTools team for providing tools for mass spectrometry analysis.

Austrian Fields of Science 2012

103037 Environmental physics
103039 Aerosol physics

Keywords

SECONDARY ORGANIC AEROSOL
CONTROLLED CHEMICAL CONDITIONS
HIGH-NOX ENVIRONMENTS
SULFURIC-ACID
PARTICLE FORMATION
MASS-SPECTROMETRY
ATMOSPHERIC CONDITIONS
BOREAL FOREST
NUCLEATION
PHOTOOXIDATION

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http://phaidra.univie.ac.at/o:446492Licence: CC BY 3.0

Cite this

Praplan, A. P., Schobesberger, S., Bianchi, F., Rissanen, M. P., Ehn, M., Jokinen, T., Junninen, H., Adamov, A., Amorim, A., Dommen, J., Duplissy, J., Hakala, J., Hansel, A., Heinritzi, M., Kangasluoma, J., Kirkby, J., Krapf, M., Kürten, A., Lehtipalo, K., ... Worsnop, D. R. (2015). Elemental composition and clustering behaviour of α-pinene oxidation products for different oxidation conditions. Atmospheric Chemistry and Physics, 15(8), 4145-4159. https://doi.org/10.5194/acp-15-4145-2015

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abstract = "This study presents the difference between oxidised organic compounds formed by alpha-pinene oxidation under various conditions in the CLOUD environmental chamber: (1) pure ozonolysis (in the presence of hydrogen as hydroxyl radical (OH) scavenger) and (2) OH oxidation (initiated by nitrous acid (HONO) photolysis by ultraviolet light) in the absence of ozone. We discuss results from three Atmospheric Pressure interface Time-of-Flight (APi-TOF) mass spectrometers measuring simultaneously the composition of naturally charged as well as neutral species (via chemical ionisation with nitrate). Natural chemical ionisation takes place in the CLOUD chamber and organic oxidised compounds form clusters with nitrate, bisulfate, bisulfate/sulfuric acid clusters, ammonium, and dimethylaminium, or get protonated. The results from this study show that this process is selective for various oxidised organic compounds with low molar mass and ions, so that in order to obtain a comprehensive picture of the elemental composition of oxidation products and their clustering behaviour, several instruments must be used. We compare oxidation products containing 10 and 20 carbon atoms and show that highly oxidised organic compounds are formed in the early stages of the oxidation. ",

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author = "Praplan, \{A. P.\} and S. Schobesberger and F. Bianchi and Rissanen, \{M. P.\} and M. Ehn and T. Jokinen and H. Junninen and A. Adamov and A. Amorim and J. Dommen and J. Duplissy and J. Hakala and A. Hansel and M. Heinritzi and J. Kangasluoma and J. Kirkby and M. Krapf and A. K{\"u}rten and K. Lehtipalo and F. Riccobono and L. Rondo and N. Sarnela and M. Simon and A. Tome and J. Troestl and Winkler, \{P. M.\} and C. Williamson and P. Ye and J. Curtius and U. Baltensperger and Donahue, \{N. M.\} and M. Kulmala and Worsnop, \{D. R.\}",

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doi = "10.5194/acp-15-4145-2015",

language = "English",

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Praplan, AP, Schobesberger, S, Bianchi, F, Rissanen, MP, Ehn, M, Jokinen, T, Junninen, H, Adamov, A, Amorim, A, Dommen, J, Duplissy, J, Hakala, J, Hansel, A, Heinritzi, M, Kangasluoma, J, Kirkby, J, Krapf, M, Kürten, A, Lehtipalo, K, Riccobono, F, Rondo, L, Sarnela, N, Simon, M, Tome, A, Troestl, J, Winkler, PM, Williamson, C, Ye, P, Curtius, J, Baltensperger, U, Donahue, NM, Kulmala, M & Worsnop, DR 2015, 'Elemental composition and clustering behaviour of α-pinene oxidation products for different oxidation conditions', Atmospheric Chemistry and Physics, vol. 15, no. 8, pp. 4145-4159. https://doi.org/10.5194/acp-15-4145-2015

TY - JOUR

T1 - Elemental composition and clustering behaviour of α-pinene oxidation products for different oxidation conditions

AU - Praplan, A. P.

AU - Schobesberger, S.

AU - Bianchi, F.

AU - Rissanen, M. P.

AU - Ehn, M.

AU - Jokinen, T.

AU - Junninen, H.

AU - Adamov, A.

AU - Amorim, A.

AU - Dommen, J.

AU - Duplissy, J.

AU - Hakala, J.

AU - Hansel, A.

AU - Heinritzi, M.

AU - Kangasluoma, J.

AU - Kirkby, J.

AU - Krapf, M.

AU - Kürten, A.

AU - Lehtipalo, K.

AU - Riccobono, F.

AU - Rondo, L.

AU - Sarnela, N.

AU - Simon, M.

AU - Tome, A.

AU - Troestl, J.

AU - Winkler, P. M.

AU - Williamson, C.

AU - Ye, P.

AU - Curtius, J.

AU - Baltensperger, U.

AU - Donahue, N. M.

AU - Kulmala, M.

AU - Worsnop, D. R.

PY - 2015/4/22

Y1 - 2015/4/22

N2 - This study presents the difference between oxidised organic compounds formed by alpha-pinene oxidation under various conditions in the CLOUD environmental chamber: (1) pure ozonolysis (in the presence of hydrogen as hydroxyl radical (OH) scavenger) and (2) OH oxidation (initiated by nitrous acid (HONO) photolysis by ultraviolet light) in the absence of ozone. We discuss results from three Atmospheric Pressure interface Time-of-Flight (APi-TOF) mass spectrometers measuring simultaneously the composition of naturally charged as well as neutral species (via chemical ionisation with nitrate). Natural chemical ionisation takes place in the CLOUD chamber and organic oxidised compounds form clusters with nitrate, bisulfate, bisulfate/sulfuric acid clusters, ammonium, and dimethylaminium, or get protonated. The results from this study show that this process is selective for various oxidised organic compounds with low molar mass and ions, so that in order to obtain a comprehensive picture of the elemental composition of oxidation products and their clustering behaviour, several instruments must be used. We compare oxidation products containing 10 and 20 carbon atoms and show that highly oxidised organic compounds are formed in the early stages of the oxidation.

AB - This study presents the difference between oxidised organic compounds formed by alpha-pinene oxidation under various conditions in the CLOUD environmental chamber: (1) pure ozonolysis (in the presence of hydrogen as hydroxyl radical (OH) scavenger) and (2) OH oxidation (initiated by nitrous acid (HONO) photolysis by ultraviolet light) in the absence of ozone. We discuss results from three Atmospheric Pressure interface Time-of-Flight (APi-TOF) mass spectrometers measuring simultaneously the composition of naturally charged as well as neutral species (via chemical ionisation with nitrate). Natural chemical ionisation takes place in the CLOUD chamber and organic oxidised compounds form clusters with nitrate, bisulfate, bisulfate/sulfuric acid clusters, ammonium, and dimethylaminium, or get protonated. The results from this study show that this process is selective for various oxidised organic compounds with low molar mass and ions, so that in order to obtain a comprehensive picture of the elemental composition of oxidation products and their clustering behaviour, several instruments must be used. We compare oxidation products containing 10 and 20 carbon atoms and show that highly oxidised organic compounds are formed in the early stages of the oxidation.

KW - SECONDARY ORGANIC AEROSOL

KW - CONTROLLED CHEMICAL CONDITIONS

KW - HIGH-NOX ENVIRONMENTS

KW - SULFURIC-ACID

KW - PARTICLE FORMATION

KW - MASS-SPECTROMETRY

KW - ATMOSPHERIC CONDITIONS

KW - BOREAL FOREST

KW - NUCLEATION

KW - PHOTOOXIDATION

UR - https://www.scopus.com/pages/publications/84928804045

U2 - 10.5194/acp-15-4145-2015

DO - 10.5194/acp-15-4145-2015

M3 - Article

SN - 1680-7316

VL - 15

SP - 4145

EP - 4159

JO - Atmospheric Chemistry and Physics

JF - Atmospheric Chemistry and Physics

IS - 8

ER -

Elemental composition and clustering behaviour of α-pinene oxidation products for different oxidation conditions

Abstract

Funding

Austrian Fields of Science 2012

Keywords

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