Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates and temperatures
Andreas Kürten
(1)
,
Federico Bianchi
(2, 3, 4)
,
Joao Almeida
(1, 5)
,
Oona Kupiainen-Maata
(4)
,
Eimear Dunne
(6, 7)
,
Jonathan Duplissy
(4, 5)
,
Christina Williamson
(1, 8)
,
Peter Barmet
(2)
,
Martin Breitenlechner
(9, 10)
,
Josef Dommen
(2)
,
Neil M. Donahue
(11)
,
Rchard C. Flagan
(12)
,
Alessandro Franchin
(4)
,
Hamish Gordon
(5)
,
Jani Hakala
(4)
,
Armin Hansel
(9, 10)
,
Martin Heinritzi
(1)
,
Luisa Ickes
(1, 3)
,
Tuija Jokinen
(4)
,
Juha Kangasluoma
(4)
,
Jaeseok Kim
(13)
,
Jasper Kirkby
(1, 5)
,
Agnieszka Kupc
(8, 14)
,
Katrianne Lehtipalo
(2, 4)
,
Markus Leiminger
(1)
,
Vladimir Makhmutov
(15)
,
Antti Onnela
(9, 10)
,
Ismael K. Ortega Colomer
(16)
,
Tuukka Petäjä
(4)
,
Arnaud P. Praplan
(2, 17)
,
Francesco Riccobono
(2)
,
Matti P. Rissanen
(4)
,
Linda Rondo
(1)
,
Ralf Schnitzhofer
(9, 10)
,
Siegfried Schobesberger
(4, 18)
,
James N. Smith
(13, 19)
,
Gérard Steiner
(4, 9, 14)
,
Yuri Stozhkov
(15)
,
Antonio Tomé
(20)
,
Jasmin Tröstl
(2)
,
Georgios Tsagkogeorgas
(21)
,
Paul E. Wagner
(14)
,
Daniela Wimmer
(1, 4)
,
Penglin Ye
(11)
,
Urs Baltensperger
(2)
,
Ken Carslaw
(6)
,
Markku Kulmala
(4)
,
Joachim Curtius
(1)
1
IAU -
Institute for Atmospheric and Environmental Sciences [Frankfurt/Main]
2 LAC - Laboratory of Atmospheric Chemistry [Paul Scherrer Institute]
3 IAC - Institute for Atmospheric and Climate Science [Zürich]
4 Helsingin yliopisto = Helsingfors universitet = University of Helsinki
5 CERN - European Organization for Nuclear Research
6 University of Leeds
7 FMI - Finnish Meteorological Institute
8 CIRES - Cooperative Institute for Research in Environmental Sciences
9 Institut für Ionenphysik und Angewandte Physik - Institute for Ion Physics and Applied Physics [Innsbruck]
10 Ionicon Analytik GmbH
11 CAPS - Center for Atmospheric Particle Studies [Pittsburgh]
12 CALTECH - California Institute of Technology
13 University of Eastern Finland
14 Universität Wien = University of Vienna
15 Solar and Cosmic Ray Research Laboratory [Moscow]
16 ONERA - The French Aerospace Lab [Palaiseau]
17 Atmospheric Research Centre of Eastern Finland
18 Department of Atmospheric Sciences [Seattle]
19 Department of Chemistry [Irvine]
20 UBI - University of Beira Interior [Portugal]
21 TROPOS - Leibniz Institute for Tropospheric Research
2 LAC - Laboratory of Atmospheric Chemistry [Paul Scherrer Institute]
3 IAC - Institute for Atmospheric and Climate Science [Zürich]
4 Helsingin yliopisto = Helsingfors universitet = University of Helsinki
5 CERN - European Organization for Nuclear Research
6 University of Leeds
7 FMI - Finnish Meteorological Institute
8 CIRES - Cooperative Institute for Research in Environmental Sciences
9 Institut für Ionenphysik und Angewandte Physik - Institute for Ion Physics and Applied Physics [Innsbruck]
10 Ionicon Analytik GmbH
11 CAPS - Center for Atmospheric Particle Studies [Pittsburgh]
12 CALTECH - California Institute of Technology
13 University of Eastern Finland
14 Universität Wien = University of Vienna
15 Solar and Cosmic Ray Research Laboratory [Moscow]
16 ONERA - The French Aerospace Lab [Palaiseau]
17 Atmospheric Research Centre of Eastern Finland
18 Department of Atmospheric Sciences [Seattle]
19 Department of Chemistry [Irvine]
20 UBI - University of Beira Interior [Portugal]
21 TROPOS - Leibniz Institute for Tropospheric Research
Jonathan Duplissy
- Fonction : Auteur
- PersonId : 973654
Josef Dommen
- Fonction : Auteur
- PersonId : 852366
Tuija Jokinen
- Fonction : Auteur
- PersonId : 779621
- ORCID : 0000-0002-1280-1396
Ismael K. Ortega Colomer
- Fonction : Auteur
- PersonId : 850863
Tuukka Petäjä
- Fonction : Auteur
- PersonId : 779400
- ORCID : 0000-0002-1881-9044
Markku Kulmala
- Fonction : Auteur
- PersonId : 763836
- ORCID : 0000-0003-3464-7825
- IdRef : 15928953X
Joachim Curtius
- Fonction : Auteur
- PersonId : 775517
- ORCID : 0000-0003-3153-4630
Résumé
Binary nucleation of sulfuric acid and water as well as ternary nucleation involving ammonia are thought to be the dominant processes responsible for new particle formation (NPF) in the cold temperatures of the middle and upper troposphere. Ions are also thought to be important for particle nucleation in these regions. However, global models presently lack experimentally measured NPF rates under controlled laboratory conditions and so at present must rely on theoretical or empirical parameterizations. Here with data obtained in the European Organization for Nuclear Research CLOUD (Cosmics Leaving OUtdoor Droplets) chamber, we present the first experimental survey of NPF rates spanning free tropospheric conditions. The conditions during nucleation cover a temperature range from 208 to 298 K, sulfuric acid concentrations between 5 × 10^5 and 1 × 10^9 cm^-3 , and ammonia mixing ratios from zero added ammonia, i.e., nominally pure binary, to a maximum of ~1400 parts per trillion by volume (pptv). We performed nucleation studies under pure neutral conditions with zero ions being present in the chamber and at ionization rates of up to 75 ion pairs cm 3 s 1 to study neutral and ion-induced nucleation. We found that the contribution from ion-induced nucleation is small at temperatures between 208 and 248 K when ammonia is present at several pptv or higher. However, the presence of charges significantly enhances the nucleation rates, especially at 248 K with zero added ammonia, and for higher temperatures independent of NH3 levels. We compare these experimental data with calculated cluster formation rates from the Atmospheric Cluster Dynamics Code with cluster evaporation rates obtained from quantum chemistry.