Modelling the contribution of biogenic volatile organic compounds to new particle formation in the Julich plant atmosphere chamber
We used the Aerosol Dynamics gas- and particle-phase chemistry model for laboratory CHAMber studies (ADCHAM) to simulate the contribution of BVOC plant emissions to the observed new particle formation during photooxidation experiments performed in the Julich Plant-Atmosphere Chamber and to evaluate...
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Format: | Article in Journal/Newspaper |
Language: | English |
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COPERNICUS GESELLSCHAFT MBH
2016
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Online Access: | http://hdl.handle.net/10138/161734 |
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ftunivhelsihelda:oai:helda.helsinki.fi:10138/161734 |
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record_format |
openpolar |
institution |
Open Polar |
collection |
HELDA – University of Helsinki Open Repository |
op_collection_id |
ftunivhelsihelda |
language |
English |
topic |
SULFURIC-ACID CONCENTRATION AEROSOL WALL LOSSES TROPOSPHERIC DEGRADATION ACTIVITY-COEFFICIENTS THERMODYNAMIC MODEL OXIDATION-PRODUCTS NUCLEATION EMISSIONS GAS GROWTH 114 Physical sciences |
spellingShingle |
SULFURIC-ACID CONCENTRATION AEROSOL WALL LOSSES TROPOSPHERIC DEGRADATION ACTIVITY-COEFFICIENTS THERMODYNAMIC MODEL OXIDATION-PRODUCTS NUCLEATION EMISSIONS GAS GROWTH 114 Physical sciences Roldin, P. Liao, L. Mogensen, D. Dal Maso, M. Rusanen, A. Kerminen, V. -M. Mentel, T. F. Wildt, J. Kleist, E. Kiendler-Scharr, A. Tillmann, R. Ehn, M. Kulmala, Markku Boy, M. Modelling the contribution of biogenic volatile organic compounds to new particle formation in the Julich plant atmosphere chamber |
topic_facet |
SULFURIC-ACID CONCENTRATION AEROSOL WALL LOSSES TROPOSPHERIC DEGRADATION ACTIVITY-COEFFICIENTS THERMODYNAMIC MODEL OXIDATION-PRODUCTS NUCLEATION EMISSIONS GAS GROWTH 114 Physical sciences |
description |
We used the Aerosol Dynamics gas- and particle-phase chemistry model for laboratory CHAMber studies (ADCHAM) to simulate the contribution of BVOC plant emissions to the observed new particle formation during photooxidation experiments performed in the Julich Plant-Atmosphere Chamber and to evaluate how well smog chamber experiments can mimic the atmospheric conditions during new particle formation events. ADCHAM couples the detailed gas-phase chemistry from Master Chemical Mechanism with a novel aerosol dynamics and particle phase chemistry module. Our model simulations reveal that the observed particle growth may have either been controlled by the formation rate of semi- and low-volatility organic compounds in the gas phase or by acid catalysed heterogeneous reactions between semi-volatility organic compounds in the particle surface layer (e.g. peroxyhemiacetal dimer formation). The contribution of extremely low-volatility organic gas-phase compounds to the particle formation and growth was suppressed because of their rapid and irreversible wall losses, which decreased their contribution to the nano-CN formation and growth compared to the atmospheric situation. The best agreement between the modelled and measured total particle number concentration (R-2 > 0.95) was achieved if the nano-CN was formed by kinetic nucleation involving both sulphuric acid and organic compounds formed from OH oxidation of BVOCs. Peer reviewed |
author2 |
Department of Physics Ecosystem processes (INAR Forest Sciences) Aerosol-Cloud-Climate -Interactions (ACCI) |
format |
Article in Journal/Newspaper |
author |
Roldin, P. Liao, L. Mogensen, D. Dal Maso, M. Rusanen, A. Kerminen, V. -M. Mentel, T. F. Wildt, J. Kleist, E. Kiendler-Scharr, A. Tillmann, R. Ehn, M. Kulmala, Markku Boy, M. |
author_facet |
Roldin, P. Liao, L. Mogensen, D. Dal Maso, M. Rusanen, A. Kerminen, V. -M. Mentel, T. F. Wildt, J. Kleist, E. Kiendler-Scharr, A. Tillmann, R. Ehn, M. Kulmala, Markku Boy, M. |
author_sort |
Roldin, P. |
title |
Modelling the contribution of biogenic volatile organic compounds to new particle formation in the Julich plant atmosphere chamber |
title_short |
Modelling the contribution of biogenic volatile organic compounds to new particle formation in the Julich plant atmosphere chamber |
title_full |
Modelling the contribution of biogenic volatile organic compounds to new particle formation in the Julich plant atmosphere chamber |
title_fullStr |
Modelling the contribution of biogenic volatile organic compounds to new particle formation in the Julich plant atmosphere chamber |
title_full_unstemmed |
Modelling the contribution of biogenic volatile organic compounds to new particle formation in the Julich plant atmosphere chamber |
title_sort |
modelling the contribution of biogenic volatile organic compounds to new particle formation in the julich plant atmosphere chamber |
publisher |
COPERNICUS GESELLSCHAFT MBH |
publishDate |
2016 |
url |
http://hdl.handle.net/10138/161734 |
genre |
Arctic The Cryosphere |
genre_facet |
Arctic The Cryosphere |
op_relation |
10.5194/acp-15-10777-2015 P. Roldin would like to thank the Cryosphere-Atmosphere Interactions in a Changing Arctic Climate (CRAICC) and the Swedish Research Council for Environment, Agricultural Sciences and Spatial Planning FORMAS (Project no. 214-2014-1445) for financial support. L. Liao wishes to thank the Maj and Tor Nessling foundation for financial support (grant no. 2009362), as well as the Academy of Finland (project no. 128731). D. Mogensen would like to thank the doctoral program in Atmospheric Sciences (ATM-DP) at the University of Helsinki for financial support. We would like to acknowledge HENVI (Helsinki University Centre for Environment), The FCoE (The Centre of Excellence in Atmospheric Science From Molecular and Biological processes to the Global Climate (ATM)), the strategic research area MERGE (Modelling the Regional and Global Earth system) and the PEGASOS (Pan-European Gas-Aerosolsclimate interaction Study, project no. FP7-ENV-2010-265148) project. We would also like to thank Gordon McFiggans' research group at the University of Manchester, and especially David Topping, for helpful discussions and for providing the Python script (now a publicly available function called Comp-SysProp: http://ratty.cas.manchester.ac.uk/informatics/) to calculate Nannoolal-based sub-cooled liquid equilibrium saturation vapour pressures for all organic compounds included in this paper. Roldin , P , Liao , L , Mogensen , D , Dal Maso , M , Rusanen , A , Kerminen , V -M , Mentel , T F , Wildt , J , Kleist , E , Kiendler-Scharr , A , Tillmann , R , Ehn , M , Kulmala , M & Boy , M 2015 , ' Modelling the contribution of biogenic volatile organic compounds to new particle formation in the Julich plant atmosphere chamber ' , Atmospheric Chemistry and Physics , vol. 15 , no. 18 , pp. 10777-10798 . https://doi.org/10.5194/acp-15-10777-2015 ORCID: /0000-0002-2023-2461/work/29330861 ORCID: /0000-0002-4523-9889/work/68615139 84942636611 578c1a3e-cfbf-4e17-a774-9bb73a20aba0 http://hdl.handle.net/10138/161734 000362457400028 |
op_rights |
cc_by openAccess info:eu-repo/semantics/openAccess |
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1787421588798308352 |
spelling |
ftunivhelsihelda:oai:helda.helsinki.fi:10138/161734 2024-01-07T09:40:48+01:00 Modelling the contribution of biogenic volatile organic compounds to new particle formation in the Julich plant atmosphere chamber Roldin, P. Liao, L. Mogensen, D. Dal Maso, M. Rusanen, A. Kerminen, V. -M. Mentel, T. F. Wildt, J. Kleist, E. Kiendler-Scharr, A. Tillmann, R. Ehn, M. Kulmala, Markku Boy, M. Department of Physics Ecosystem processes (INAR Forest Sciences) Aerosol-Cloud-Climate -Interactions (ACCI) 2016-05-11T08:05:01Z 22 application/pdf http://hdl.handle.net/10138/161734 eng eng COPERNICUS GESELLSCHAFT MBH 10.5194/acp-15-10777-2015 P. Roldin would like to thank the Cryosphere-Atmosphere Interactions in a Changing Arctic Climate (CRAICC) and the Swedish Research Council for Environment, Agricultural Sciences and Spatial Planning FORMAS (Project no. 214-2014-1445) for financial support. L. Liao wishes to thank the Maj and Tor Nessling foundation for financial support (grant no. 2009362), as well as the Academy of Finland (project no. 128731). D. Mogensen would like to thank the doctoral program in Atmospheric Sciences (ATM-DP) at the University of Helsinki for financial support. We would like to acknowledge HENVI (Helsinki University Centre for Environment), The FCoE (The Centre of Excellence in Atmospheric Science From Molecular and Biological processes to the Global Climate (ATM)), the strategic research area MERGE (Modelling the Regional and Global Earth system) and the PEGASOS (Pan-European Gas-Aerosolsclimate interaction Study, project no. FP7-ENV-2010-265148) project. We would also like to thank Gordon McFiggans' research group at the University of Manchester, and especially David Topping, for helpful discussions and for providing the Python script (now a publicly available function called Comp-SysProp: http://ratty.cas.manchester.ac.uk/informatics/) to calculate Nannoolal-based sub-cooled liquid equilibrium saturation vapour pressures for all organic compounds included in this paper. Roldin , P , Liao , L , Mogensen , D , Dal Maso , M , Rusanen , A , Kerminen , V -M , Mentel , T F , Wildt , J , Kleist , E , Kiendler-Scharr , A , Tillmann , R , Ehn , M , Kulmala , M & Boy , M 2015 , ' Modelling the contribution of biogenic volatile organic compounds to new particle formation in the Julich plant atmosphere chamber ' , Atmospheric Chemistry and Physics , vol. 15 , no. 18 , pp. 10777-10798 . https://doi.org/10.5194/acp-15-10777-2015 ORCID: /0000-0002-2023-2461/work/29330861 ORCID: /0000-0002-4523-9889/work/68615139 84942636611 578c1a3e-cfbf-4e17-a774-9bb73a20aba0 http://hdl.handle.net/10138/161734 000362457400028 cc_by openAccess info:eu-repo/semantics/openAccess SULFURIC-ACID CONCENTRATION AEROSOL WALL LOSSES TROPOSPHERIC DEGRADATION ACTIVITY-COEFFICIENTS THERMODYNAMIC MODEL OXIDATION-PRODUCTS NUCLEATION EMISSIONS GAS GROWTH 114 Physical sciences Article publishedVersion 2016 ftunivhelsihelda 2023-12-14T00:15:40Z We used the Aerosol Dynamics gas- and particle-phase chemistry model for laboratory CHAMber studies (ADCHAM) to simulate the contribution of BVOC plant emissions to the observed new particle formation during photooxidation experiments performed in the Julich Plant-Atmosphere Chamber and to evaluate how well smog chamber experiments can mimic the atmospheric conditions during new particle formation events. ADCHAM couples the detailed gas-phase chemistry from Master Chemical Mechanism with a novel aerosol dynamics and particle phase chemistry module. Our model simulations reveal that the observed particle growth may have either been controlled by the formation rate of semi- and low-volatility organic compounds in the gas phase or by acid catalysed heterogeneous reactions between semi-volatility organic compounds in the particle surface layer (e.g. peroxyhemiacetal dimer formation). The contribution of extremely low-volatility organic gas-phase compounds to the particle formation and growth was suppressed because of their rapid and irreversible wall losses, which decreased their contribution to the nano-CN formation and growth compared to the atmospheric situation. The best agreement between the modelled and measured total particle number concentration (R-2 > 0.95) was achieved if the nano-CN was formed by kinetic nucleation involving both sulphuric acid and organic compounds formed from OH oxidation of BVOCs. Peer reviewed Article in Journal/Newspaper Arctic The Cryosphere HELDA – University of Helsinki Open Repository |