Comparison of the SAWNUC model with CLOUD measurements of sulphuric acid-water nucleation

Sebastian Ehrhart; Luisa Ickes; Joao Almeida; Antonio Amorim; Peter Barmet; Federico Bianchi; Josef Dommen; Eimear M. Dunne; Jonathan Duplissy; Alessandro Franchin; Juha Kangasluoma; Jasper Kirkby; Andreas Kürten; Agnieszka Kupc; Katrianne Lehtipalo; Tuomo Nieminen; Francesco Riccobono; Linda Rondo; Siegfried Schobesberger; Gerhard Steiner; Antonio Tome; Daniela Wimmer; Urs Baltensperger; Paul E. Wagner; Joachim Curtius

doi:10.1002/2015JD023723

Comparison of the SAWNUC model with CLOUD measurements of sulphuric acid-water nucleation

Sebastian Ehrhart (Corresponding author)
, Luisa Ickes
, Joao Almeida
, Antonio Amorim
, Peter Barmet
, Federico Bianchi
, Josef Dommen
, Eimear M. Dunne
, Jonathan Duplissy
, Alessandro Franchin
, Juha Kangasluoma
, Jasper Kirkby
, Andreas Kürten
, Agnieszka Kupc
, Katrianne Lehtipalo
, Tuomo Nieminen
, Francesco Riccobono
, Linda Rondo
, Siegfried Schobesberger
, Gerhard Steiner

Antonio Tome, Daniela Wimmer, Urs Baltensperger, Paul E. Wagner, Joachim Curtius

Aerosol Physics and Environmental Physics

Publications: Contribution to journal › Article › Peer Reviewed

Abstract

Binary nucleation of sulphuric acid-water particles is expected to be an important process in the free troposphere at low temperatures. SAWNUC (Sulphuric Acid Water Nucleation) is a model of binary nucleation that is based on laboratory measurements of the binding energies of sulphuric acid and water in charged and neutral clusters. Predictions of SAWNUC are compared for the first time comprehensively with experimental binary nucleation data from the CLOUD chamber at European Organization for Nuclear Research. The experimental measurements span a temperature range of 208-292 K, sulphuric acid concentrations from 1.106 to 1.109 cm ^-3, and distinguish between ion-induced and neutral nucleation. Good agreement, within a factor of 5, is found between the experimental and modeled formation rates for ion-induced nucleation at 278 K and below and for neutral nucleation at 208 and 223 K. Differences at warm temperatures are attributed to ammonia contamination which was indicated by the presence of ammonia-sulphuric acid clusters, detected by an Atmospheric Pressure Interface Time of Flight (APi-TOF) mass spectrometer. APi-TOF measurements of the sulphuric acid ion cluster distributions ((H ₂SO ₄)i. HSO- ₄ with i = 0, 1, …, 10) show qualitative agreement with the SAWNUC ion cluster distributions. Remaining differences between the measured and modeled distributions are most likely due to fragmentation in the APi-TOF. The CLOUD results are in good agreement with previously measured cluster binding energies and show the SAWNUC model to be a good representation of ion-induced and neutral binary nucleation of sulphuric acid-water clusters in the middle and upper troposphere.

Original language	English
Pages (from-to)	12,401-12,414
Number of pages	14
Journal	Journal of Geophysical Research: Atmospheres
Volume	121
Issue number	20
DOIs	https://doi.org/10.1002/2015JD023723
Publication status	Published - 27 Oct 2016

Funding

We thank Edward R. Lovejoy, Karl D. Froyd, and Jan Kazil for providing the SAWNUC model code. 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. This research has received funding from the EC Seventh Framework Programme (Marie Curie Initial Training Network "CLOUD-ITN" grant 215072 and "CLOUD-TRAIN" grant 316662, and ERC-Advanced "ATMNUCLE" grant 227463), the European Union's Horizon 2020 research and innovation programme (Marie Sklodowska-Curie grant 656994), the German Federal Ministry of Education and Research (project 01LK0902A and 01LK1222A), the Swiss National Science Foundation (project 206621_125025 and 206620_130527), the Academy of Finland Center of Excellence program (project 1118615), the Austrian Science Fund (FWF; project P19546 and L593), University of Innsbruck research fund for young scientists, the Portuguese Foundation for Science and Technology (project CERN/FP/116387/2010), and the Russian Foundation for Basic Research (grant N08-02-91006-CERN). The data are in the figures, tables, references, and in Kurten et al. [2016].

Austrian Fields of Science 2012

103037 Environmental physics
103039 Aerosol physics

Keywords

ion-induced nucleation
binary nucleation
AEROSOL-PARTICLE FORMATION
ION-INDUCED NUCLEATION
ATMOSPHERIC CONDITIONS
SPHERICAL-PARTICLES
ELECTRICAL MOBILITY
MASS-SPECTROMETER
1 NM
SIZE
IONIZATION
SYSTEM

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Ehrhart, S., Ickes, L., Almeida, J., Amorim, A., Barmet, P., Bianchi, F., Dommen, J., Dunne, E. M., Duplissy, J., Franchin, A., Kangasluoma, J., Kirkby, J., Kürten, A., Kupc, A., Lehtipalo, K., Nieminen, T., Riccobono, F., Rondo, L., Schobesberger, S., ... Curtius, J. (2016). Comparison of the SAWNUC model with CLOUD measurements of sulphuric acid-water nucleation. Journal of Geophysical Research: Atmospheres, 121(20), 12,401-12,414. https://doi.org/10.1002/2015JD023723

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title = "Comparison of the SAWNUC model with CLOUD measurements of sulphuric acid-water nucleation",

abstract = "Binary nucleation of sulphuric acid-water particles is expected to be an important process in the free troposphere at low temperatures. SAWNUC (Sulphuric Acid Water Nucleation) is a model of binary nucleation that is based on laboratory measurements of the binding energies of sulphuric acid and water in charged and neutral clusters. Predictions of SAWNUC are compared for the first time comprehensively with experimental binary nucleation data from the CLOUD chamber at European Organization for Nuclear Research. The experimental measurements span a temperature range of 208-292 K, sulphuric acid concentrations from 1.106 to 1.109 cm -3, and distinguish between ion-induced and neutral nucleation. Good agreement, within a factor of 5, is found between the experimental and modeled formation rates for ion-induced nucleation at 278 K and below and for neutral nucleation at 208 and 223 K. Differences at warm temperatures are attributed to ammonia contamination which was indicated by the presence of ammonia-sulphuric acid clusters, detected by an Atmospheric Pressure Interface Time of Flight (APi-TOF) mass spectrometer. APi-TOF measurements of the sulphuric acid ion cluster distributions ((H 2SO 4)i. HSO- 4 with i = 0, 1, …, 10) show qualitative agreement with the SAWNUC ion cluster distributions. Remaining differences between the measured and modeled distributions are most likely due to fragmentation in the APi-TOF. The CLOUD results are in good agreement with previously measured cluster binding energies and show the SAWNUC model to be a good representation of ion-induced and neutral binary nucleation of sulphuric acid-water clusters in the middle and upper troposphere. ",

keywords = "ion-induced nucleation, binary nucleation, AEROSOL-PARTICLE FORMATION, ION-INDUCED NUCLEATION, ATMOSPHERIC CONDITIONS, SPHERICAL-PARTICLES, ELECTRICAL MOBILITY, MASS-SPECTROMETER, 1 NM, SIZE, IONIZATION, SYSTEM",

author = "Sebastian Ehrhart and Luisa Ickes and Joao Almeida and Antonio Amorim and Peter Barmet and Federico Bianchi and Josef Dommen and Dunne, \{Eimear M.\} and Jonathan Duplissy and Alessandro Franchin and Juha Kangasluoma and Jasper Kirkby and Andreas K{\"u}rten and Agnieszka Kupc and Katrianne Lehtipalo and Tuomo Nieminen and Francesco Riccobono and Linda Rondo and Siegfried Schobesberger and Gerhard Steiner and Antonio Tome and Daniela Wimmer and Urs Baltensperger and Wagner, \{Paul E.\} and Joachim Curtius",

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doi = "10.1002/2015JD023723",

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journal = "Journal of Geophysical Research: Atmospheres",

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Ehrhart, S, Ickes, L, Almeida, J, Amorim, A, Barmet, P, Bianchi, F, Dommen, J, Dunne, EM, Duplissy, J, Franchin, A, Kangasluoma, J, Kirkby, J, Kürten, A, Kupc, A, Lehtipalo, K, Nieminen, T, Riccobono, F, Rondo, L, Schobesberger, S, Steiner, G, Tome, A, Wimmer, D, Baltensperger, U, Wagner, PE & Curtius, J 2016, 'Comparison of the SAWNUC model with CLOUD measurements of sulphuric acid-water nucleation', Journal of Geophysical Research: Atmospheres, vol. 121, no. 20, pp. 12,401-12,414. https://doi.org/10.1002/2015JD023723

TY - JOUR

T1 - Comparison of the SAWNUC model with CLOUD measurements of sulphuric acid-water nucleation

AU - Ehrhart, Sebastian

AU - Ickes, Luisa

AU - Almeida, Joao

AU - Amorim, Antonio

AU - Barmet, Peter

AU - Bianchi, Federico

AU - Dommen, Josef

AU - Dunne, Eimear M.

AU - Duplissy, Jonathan

AU - Franchin, Alessandro

AU - Kangasluoma, Juha

AU - Kirkby, Jasper

AU - Kürten, Andreas

AU - Kupc, Agnieszka

AU - Lehtipalo, Katrianne

AU - Nieminen, Tuomo

AU - Riccobono, Francesco

AU - Rondo, Linda

AU - Schobesberger, Siegfried

AU - Steiner, Gerhard

AU - Tome, Antonio

AU - Wimmer, Daniela

AU - Baltensperger, Urs

AU - Wagner, Paul E.

AU - Curtius, Joachim

PY - 2016/10/27

Y1 - 2016/10/27

N2 - Binary nucleation of sulphuric acid-water particles is expected to be an important process in the free troposphere at low temperatures. SAWNUC (Sulphuric Acid Water Nucleation) is a model of binary nucleation that is based on laboratory measurements of the binding energies of sulphuric acid and water in charged and neutral clusters. Predictions of SAWNUC are compared for the first time comprehensively with experimental binary nucleation data from the CLOUD chamber at European Organization for Nuclear Research. The experimental measurements span a temperature range of 208-292 K, sulphuric acid concentrations from 1.106 to 1.109 cm -3, and distinguish between ion-induced and neutral nucleation. Good agreement, within a factor of 5, is found between the experimental and modeled formation rates for ion-induced nucleation at 278 K and below and for neutral nucleation at 208 and 223 K. Differences at warm temperatures are attributed to ammonia contamination which was indicated by the presence of ammonia-sulphuric acid clusters, detected by an Atmospheric Pressure Interface Time of Flight (APi-TOF) mass spectrometer. APi-TOF measurements of the sulphuric acid ion cluster distributions ((H 2SO 4)i. HSO- 4 with i = 0, 1, …, 10) show qualitative agreement with the SAWNUC ion cluster distributions. Remaining differences between the measured and modeled distributions are most likely due to fragmentation in the APi-TOF. The CLOUD results are in good agreement with previously measured cluster binding energies and show the SAWNUC model to be a good representation of ion-induced and neutral binary nucleation of sulphuric acid-water clusters in the middle and upper troposphere.

AB - Binary nucleation of sulphuric acid-water particles is expected to be an important process in the free troposphere at low temperatures. SAWNUC (Sulphuric Acid Water Nucleation) is a model of binary nucleation that is based on laboratory measurements of the binding energies of sulphuric acid and water in charged and neutral clusters. Predictions of SAWNUC are compared for the first time comprehensively with experimental binary nucleation data from the CLOUD chamber at European Organization for Nuclear Research. The experimental measurements span a temperature range of 208-292 K, sulphuric acid concentrations from 1.106 to 1.109 cm -3, and distinguish between ion-induced and neutral nucleation. Good agreement, within a factor of 5, is found between the experimental and modeled formation rates for ion-induced nucleation at 278 K and below and for neutral nucleation at 208 and 223 K. Differences at warm temperatures are attributed to ammonia contamination which was indicated by the presence of ammonia-sulphuric acid clusters, detected by an Atmospheric Pressure Interface Time of Flight (APi-TOF) mass spectrometer. APi-TOF measurements of the sulphuric acid ion cluster distributions ((H 2SO 4)i. HSO- 4 with i = 0, 1, …, 10) show qualitative agreement with the SAWNUC ion cluster distributions. Remaining differences between the measured and modeled distributions are most likely due to fragmentation in the APi-TOF. The CLOUD results are in good agreement with previously measured cluster binding energies and show the SAWNUC model to be a good representation of ion-induced and neutral binary nucleation of sulphuric acid-water clusters in the middle and upper troposphere.

KW - ion-induced nucleation

KW - binary nucleation

KW - AEROSOL-PARTICLE FORMATION

KW - ION-INDUCED NUCLEATION

KW - ATMOSPHERIC CONDITIONS

KW - SPHERICAL-PARTICLES

KW - ELECTRICAL MOBILITY

KW - MASS-SPECTROMETER

KW - 1 NM

KW - SIZE

KW - IONIZATION

KW - SYSTEM

UR - https://www.scopus.com/pages/publications/84995694801

U2 - 10.1002/2015JD023723

DO - 10.1002/2015JD023723

M3 - Article

SN - 2169-897X

VL - 121

SP - 12,401-12,414

JO - Journal of Geophysical Research: Atmospheres

JF - Journal of Geophysical Research: Atmospheres

IS - 20

ER -

Comparison of the SAWNUC model with CLOUD measurements of sulphuric acid-water nucleation

Abstract

Funding

Austrian Fields of Science 2012

Keywords

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