The role of ions in new particle formation in the CLOUD chamber

Wagner, Robert; Yan, Chao; Lehtipalo, Katrianne; Duplissy, Jonathan; Nieminen, Tuomo; Kangasluoma, Juha; Ahonen, Lauri R.; Dada, Lubna; Kontkanen, Jenni; Manninen, Hanna E.; Dias, Antonio; Amorim, Antonio; Bauer, Paulus S.; Bergen, Anton; Bernhammer, Anne-Kathrin; Bianchi, Federico; Brilke, Sophia; Mazon, Stephany Buenrostro; Chen, Xuemeng; Draper, Danielle C.; Fischer, Lukas; Frege, Carla; Fuchs, Claudia; Garmash, Olga; Gordon, Hamish; Hakala, Jani; Heikkinen, Liine; Heinritzi, Martin; Hofbauer, Victoria; Hoyle, Christopher R.; Kirkby, Jasper; Kürten, Andreas; Kvashnin, Alexander N.; Laurila, Tiia; Lawler, Michael J.; Mai, Huajun; Makhmutov, Vladimir; Mauldin III, Roy L.; Molteni, Ugo; Nichman, Leonid; Nie, Wei; Ojdanic, Andrea; Onnela, Antti; Piel, Felix; Quéléver, Lauriane L. J.; Rissanen, Matti P.; Sarnela, Nina; Schallhart, Simon; Sengupta, Kamalika; Simon, Mario; Stolzenburg, Dominik; Stozhkov, Yuri; Tröstl, Jasmin; Viisanen, Yrjö; Vogel, Alexander L.; Wagner, Andrea C.; Xiao, Mao; Ye, Penglin; Baltensperger, Urs; Curtius, Joachim; Donahue, Neil M.; Flagan, Richard C.; Gallagher, Martin; Hansel, Armin; Smith, James N.; Tomé, António; Winkler, Paul M.; Worsnop, Douglas; Ehn, Mikael; Sipilä, Mikko; Kerminen, Veli-Matti; Petäjä, Tuukka; Kulmala, Markku

doi:10.5194/acp-17-15181-2017

The role of ions in new particle formation in the CLOUD chamber

Journal Article · Thu Dec 21 00:00:00 EST 2017 · Atmospheric Chemistry and Physics (Online)

DOI:https://doi.org/10.5194/acp-17-15181-2017· OSTI ID:1460017

Wagner, Robert; ; ; Duplissy, Jonathan; ; Kangasluoma, Juha; ; ; ; Manninen, Hanna E.; Dias, Antonio; Amorim, Antonio; Bauer, Paulus S.; Bergen, Anton; ; ; Brilke, Sophia; ; Chen, Xuemeng; Draper, Danielle C. more »

The formation of secondary particles in the atmosphere accounts for more than half of global cloud condensation nuclei. Experiments at the CERN CLOUD (Cosmics Leaving OUtdoor Droplets) chamber have underlined the importance of ions for new particle formation, but quantifying their effect in the atmosphere remains challenging. By using a novel instrument setup consisting of two nanoparticle counters, one of them equipped with an ion filter, we were able to further investigate the ion-related mechanisms of new particle formation. In autumn 2015, we carried out experiments at CLOUD on four systems of different chemical compositions involving monoterpenes, sulfuric acid, nitrogen oxides, and ammonia. We measured the influence of ions on the nucleation rates under precisely controlled and atmospherically relevant conditions. Our results indicate that ions enhance the nucleation process when the charge is necessary to stabilize newly formed clusters, i.e., in conditions in which neutral clusters are unstable. For charged clusters that were formed by ion-induced nucleation, we were able to measure, for the first time, their progressive neutralization due to recombination with oppositely charged ions. A large fraction of the clusters carried a charge at 1.5nm diameter. However, depending on particle growth rates and ion concentrations, charged clusters were largely neutralized by ion–ion recombination before they grew to 2.5nm. At this size, more than 90% of particles were neutral. In other words, particles may originate from ion-induced nucleation, although they are neutral upon detection at diameters larger than 2.5nm. Observations at Hyytiälä, Finland, showed lower ion concentrations and a lower contribution of ion-induced nucleation than measured at CLOUD under similar conditions. Although this can be partly explained by the observation that ion-induced fractions decrease towards lower ion concentrations, further investigations are needed to resolve the origin of the discrepancy.

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Research Organization:: University of California, Irvine, CA 92697, United States

Sponsoring Organization:: USDOE

Grant/Contract Number:: SC0014469

OSTI ID:: 1460017

Alternate ID(s):: OSTI ID: 1502074

Journal Information:: Atmospheric Chemistry and Physics (Online), Journal Name: Atmospheric Chemistry and Physics (Online) Journal Issue: 24 Vol. 17; ISSN 1680-7324

Publisher:: Copernicus Publications, EGUCopyright Statement

Country of Publication:: Germany

Language:: English

References (54)

Effect of ions on sulfuric acid-water binary particle formation: 2. Experimental data and comparison with QC-normalized classical nucleation theory: BINARY PARTICLE FORMATION EXPERIMENTS Duplissy, J.; Merikanto, J.; Franchin, A. Journal of Geophysical Research: Atmospheres, Vol. 121, Issue 4 https://doi.org/10.1002/2015JD023539	journal	February 2016
Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures Kürten, Andreas; Bianchi, Federico; Almeida, Joao Journal of Geophysical Research: Atmospheres, Vol. 121, Issue 20 https://doi.org/10.1002/2015JD023908	journal	October 2016
Atmospheric Ion-induced Aerosol Nucleation Curtius, J.; Lovejoy, E. R.; Froyd, K. D. Space Science Reviews, Vol. 125, Issue 1-4 https://doi.org/10.1007/s11214-006-9054-5	journal	December 2006
Turbulent deposition and gravitational sedimentation of an aerosol in a vessel of arbitrary shape Crump, James G.; Seinfeld, John H. Journal of Aerosol Science, Vol. 12, Issue 5 https://doi.org/10.1016/0021-8502(81)90036-7	journal	January 1981
Formation and growth rates of ultrafine atmospheric particles: a review of observations Kulmala, M.; Vehkamäki, H.; Petäjä, T. Journal of Aerosol Science, Vol. 35, Issue 2 https://doi.org/10.1016/j.jaerosci.2003.10.003	journal	March 2004
Sizing of neutral sub 3nm tungsten oxide clusters using Airmodus Particle Size Magnifier Kangasluoma, J.; Attoui, M.; Junninen, H. Journal of Aerosol Science, Vol. 87 https://doi.org/10.1016/j.jaerosci.2015.05.007	journal	September 2015
PTR3: An Instrument for Studying the Lifecycle of Reactive Organic Carbon in the Atmosphere Breitenlechner, Martin; Fischer, Lukas; Hainer, Markus Analytical Chemistry, Vol. 89, Issue 11 https://doi.org/10.1021/acs.analchem.6b05110	journal	May 2017
Heterogeneous Nucleation onto Ions and Neutralized Ions: Insights into Sign-Preference Kangasluoma, Juha; Samodurov, Alexander; Attoui, Michel The Journal of Physical Chemistry C, Vol. 120, Issue 13 https://doi.org/10.1021/acs.jpcc.6b01779	journal	March 2016
Diffusion of H ₂ SO ₄ in Humidified Nitrogen: Hydrated H ₂ SO ₄ Hanson, D. R.; Eisele, F. The Journal of Physical Chemistry A, Vol. 104, Issue 8 https://doi.org/10.1021/jp993622j	journal	March 2000
From molecular clusters to nanoparticles: Role of ambient ionization in tropospheric aerosol formation Yu, Fangqun; Turco, Richard P. Journal of Geophysical Research: Atmospheres, Vol. 106, Issue D5 https://doi.org/10.1029/2000JD900539	journal	March 2001
How significantly does coagulational scavenging limit atmospheric particle production? Kerminen, Veli-Matti; Pirjola, Liisa; Kulmala, Markku Journal of Geophysical Research: Atmospheres, Vol. 106, Issue D20 https://doi.org/10.1029/2001JD000322	journal	October 2001
Atmospheric ion-induced nucleation of sulfuric acid and water Lovejoy, E. R. Journal of Geophysical Research, Vol. 109, Issue D8 https://doi.org/10.1029/2003JD004460	journal	January 2004
Charging state of the atmospheric nucleation mode: Implications for separating neutral and ion-induced nucleation Kerminen, Veli-Matti; Anttila, Tatu; Petäjä, Tuukka Journal of Geophysical Research, Vol. 112, Issue D21 https://doi.org/10.1029/2007JD008649	journal	January 2007
Spatial distributions of particle number concentrations in the global troposphere: Simulations, observations, and implications for nucleation mechanisms Yu, Fangqun; Luo, Gan; Bates, Timothy S. Journal of Geophysical Research, Vol. 115, Issue D17 https://doi.org/10.1029/2009JD013473	journal	January 2010
Measurement of the gas phase concentration of H ₂ SO ₄ and methane sulfonic acid and estimates of H ₂ SO ₄ production and loss in the atmosphere Eisele, F. L.; Tanner, D. J. Journal of Geophysical Research: Atmospheres, Vol. 98, Issue D5 https://doi.org/10.1029/93JD00031	journal	May 1993
Natural and anthropogenic negative ions in the troposphere Eisele, F. L. Journal of Geophysical Research, Vol. 94, Issue D2 https://doi.org/10.1029/JD094iD02p02183	journal	January 1989
Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation Kirkby, Jasper; Curtius, Joachim; Almeida, João Nature, Vol. 476, Issue 7361 https://doi.org/10.1038/nature10343	journal	August 2011
Molecular understanding of sulphuric acid–amine particle nucleation in the atmosphere Almeida, João; Schobesberger, Siegfried; Kürten, Andreas Nature, Vol. 502, Issue 7471 https://doi.org/10.1038/nature12663	journal	October 2013
A large source of low-volatility secondary organic aerosol Ehn, Mikael; Thornton, Joel A.; Kleist, Einhard Nature, Vol. 506, Issue 7489 https://doi.org/10.1038/nature13032	journal	February 2014
Ion-induced nucleation of pure biogenic particles Kirkby, Jasper; Duplissy, Jonathan; Sengupta, Kamalika Nature, Vol. 533, Issue 7604 https://doi.org/10.1038/nature17953	journal	May 2016
Neutral molecular cluster formation of sulfuric acid–dimethylamine observed in real time under atmospheric conditions Kürten, Andreas; Jokinen, Tuija; Simon, Mario Proceedings of the National Academy of Sciences, Vol. 111, Issue 42 https://doi.org/10.1073/pnas.1404853111	journal	October 2014
The History of Condensation Nucleus Counters McMurry, Peter Aerosol Science and Technology, Vol. 33, Issue 4, p. 297-322 https://doi.org/10.1080/02786820050121512	journal	October 2000
Particle Size Magnifier for Nano-CN Detection Vanhanen, J.; Mikkilä, J.; Lehtipalo, K. Aerosol Science and Technology, Vol. 45, Issue 4 https://doi.org/10.1080/02786826.2010.547889	journal	March 2011
An Instrumental Comparison of Mobility and Mass Measurements of Atmospheric Small Ions Ehn, Mikael; Junninen, Heikki; Schobesberger, Siegfried Aerosol Science and Technology, Vol. 45, Issue 4 https://doi.org/10.1080/02786826.2010.547890	journal	March 2011
Scanning Electrical Mobility Spectrometer Wang, Shih Chen; Flagan, Richard C. Aerosol Science and Technology, Vol. 13, Issue 2 https://doi.org/10.1080/02786829008959441	journal	January 1990
Analysis of one year of Ion-DMPS data from the SMEAR II station, Finland Gagné, Stéphanie; Laakso, Lauri; Petäajä, Tuukka Tellus B: Chemical and Physical Meteorology, Vol. 60, Issue 3 https://doi.org/10.1111/j.1600-0889.2008.00347.x	journal	January 2008
Heterogeneous Nucleation Experiments Bridging the Scale from Molecular Ion Clusters to Nanoparticles Winkler, P. M.; Steiner, G.; Vrtala, A. Science, Vol. 319, Issue 5868 https://doi.org/10.1126/science.1149034	journal	March 2008
Direct Observations of Atmospheric Aerosol Nucleation Kulmala, M.; Kontkanen, J.; Junninen, H. Science, Vol. 339, Issue 6122 https://doi.org/10.1126/science.1227385	journal	February 2013
Aerosols, Cloud Microphysics, and Fractional Cloudiness Albrecht, B. A. Science, Vol. 245, Issue 4923 https://doi.org/10.1126/science.245.4923.1227	journal	September 1989
New particle formation in the free troposphere: A question of chemistry and timing Bianchi, F.; Trostl, J.; Junninen, H. Science, Vol. 352, Issue 6289 https://doi.org/10.1126/science.aad5456	journal	May 2016
Chemistry of Atmospheric Nucleation: On the Recent Advances on Precursor Characterization and Atmospheric Cluster Composition in Connection with Atmospheric New Particle Formation Kulmala, M.; Petäjä, T.; Ehn, M. Annual Review of Physical Chemistry, Vol. 65, Issue 1 https://doi.org/10.1146/annurev-physchem-040412-110014	journal	April 2014
Aerosol nucleation and its role for clouds and Earth's radiative forcing in the aerosol-climate model ECHAM5-HAM Kazil, J.; Stier, P.; Zhang, K. Atmospheric Chemistry and Physics, Vol. 10, Issue 22 https://doi.org/10.5194/acp-10-10733-2010	journal	January 2010
Atmospheric data over a solar cycle: no connection between galactic cosmic rays and new particle formation Kulmala, M.; Riipinen, I.; Nieminen, T. Atmospheric Chemistry and Physics, Vol. 10, Issue 4 https://doi.org/10.5194/acp-10-1885-2010	journal	January 2010
Hygroscopicity and chemical composition of Antarctic sub-micrometre aerosol particles and observations of new particle formation Asmi, E.; Frey, A.; Virkkula, A. Atmospheric Chemistry and Physics, Vol. 10, Issue 9 https://doi.org/10.5194/acp-10-4253-2010	journal	January 2010
EUCAARI ion spectrometer measurements at 12 European sites – analysis of new particle formation events Manninen, H. E.; Nieminen, T.; Asmi, E. Atmospheric Chemistry and Physics, Vol. 10, Issue 16 https://doi.org/10.5194/acp-10-7907-2010	journal	January 2010
New particle formation and ultrafine charged aerosol climatology at a high altitude site in the Alps (Jungfraujoch, 3580 m a.s.l., Switzerland) Boulon, J.; Sellegri, K.; Venzac, H. Atmospheric Chemistry and Physics, Vol. 10, Issue 19 https://doi.org/10.5194/acp-10-9333-2010	journal	January 2010
Radon activity in the lower troposphere and its impact on ionization rate: a global estimate using different radon emissions Zhang, K.; Feichter, J.; Kazil, J. Atmospheric Chemistry and Physics, Vol. 11, Issue 15 https://doi.org/10.5194/acp-11-7817-2011	journal	January 2011
The size-dependent charge fraction of sub-3-nm particles as a key diagnostic of competitive nucleation mechanisms under atmospheric conditions Yu, F.; Turco, R. P. Atmospheric Chemistry and Physics, Vol. 11, Issue 18 https://doi.org/10.5194/acp-11-9451-2011	journal	January 2011
Atmospheric sulphuric acid and neutral cluster measurements using CI-APi-TOF Jokinen, T.; Sipilä, M.; Junninen, H. Atmospheric Chemistry and Physics, Vol. 12, Issue 9 https://doi.org/10.5194/acp-12-4117-2012	journal	January 2012
Estimating the contribution of ion–ion recombination to sub-2 nm cluster concentrations from atmospheric measurements Kontkanen, J.; Lehtinen, K. E. J.; Nieminen, T. Atmospheric Chemistry and Physics, Vol. 13, Issue 22 https://doi.org/10.5194/acp-13-11391-2013	journal	January 2013
Suppression of new particle formation from monoterpene oxidation by NO _x Wildt, J.; Mentel, T. F.; Kiendler-Scharr, A. Atmospheric Chemistry and Physics, Vol. 14, Issue 6 https://doi.org/10.5194/acp-14-2789-2014	journal	January 2014
Major contribution of neutral clusters to new particle formation at the interface between the boundary layer and the free troposphere Rose, C.; Sellegri, K.; Asmi, E. Atmospheric Chemistry and Physics, Vol. 15, Issue 6 https://doi.org/10.5194/acp-15-3413-2015	journal	January 2015
Experimental investigation of ion–ion recombination under atmospheric conditions Franchin, A.; Ehrhart, S.; Leppä, J. Atmospheric Chemistry and Physics, Vol. 15, Issue 13 https://doi.org/10.5194/acp-15-7203-2015	journal	January 2015
How do air ions reflect variations in ionising radiation in the lower atmosphere in a boreal forest? Chen, Xuemeng; Kerminen, Veli-Matti; Paatero, Jussi Atmospheric Chemistry and Physics, Vol. 16, Issue 22 https://doi.org/10.5194/acp-16-14297-2016	journal	January 2016
Influence of temperature on the molecular composition of ions and charged clusters during pure biogenic nucleation Frege, Carla; Ortega, Ismael K.; Rissanen, Matti P. Atmospheric Chemistry and Physics, Vol. 18, Issue 1 https://doi.org/10.5194/acp-18-65-2018	journal	January 2018
Factors of air ion balance in a coniferous forest according to measurements in Hyytiälä, Finland Tammet, H.; Hõrrak, U.; Laakso, L. Atmospheric Chemistry and Physics, Vol. 6, Issue 11 https://doi.org/10.5194/acp-6-3377-2006	journal	January 2006
Charged and total particle formation and growth rates during EUCAARI 2007 campaign in Hyytiälä Manninen, H. E.; Nieminen, T.; Riipinen, I. Atmospheric Chemistry and Physics, Vol. 9, Issue 12 https://doi.org/10.5194/acp-9-4077-2009	journal	January 2009
Analysis of atmospheric neutral and charged molecular clusters in boreal forest using pulse-height CPC Lehtipalo, K.; Sipilä, M.; Riipinen, I. Atmospheric Chemistry and Physics, Vol. 9, Issue 12 https://doi.org/10.5194/acp-9-4177-2009	journal	January 2009
A high-resolution mass spectrometer to measure atmospheric ion composition Junninen, H.; Ehn, M.; Petäjä, T. Atmospheric Measurement Techniques, Vol. 3, Issue 4 https://doi.org/10.5194/amt-3-1039-2010	journal	January 2010
Performance of a corona ion source for measurement of sulfuric acid by chemical ionization mass spectrometry Kürten, A.; Rondo, L.; Ehrhart, S. Atmospheric Measurement Techniques, Vol. 4, Issue 3 https://doi.org/10.5194/amt-4-437-2011	journal	January 2011
The mathematical principles and design of the NAIS – a spectrometer for the measurement of cluster ion and nanometer aerosol size distributions Mirme, S.; Mirme, A. Atmospheric Measurement Techniques, Vol. 6, Issue 4 https://doi.org/10.5194/amt-6-1061-2013	journal	January 2013
Sub-3 nm particle size and composition dependent response of a nano-CPC battery Kangasluoma, J.; Kuang, C.; Wimmer, D. Atmospheric Measurement Techniques, Vol. 7, Issue 3 https://doi.org/10.5194/amt-7-689-2014	journal	January 2014
Operation of the Airmodus A11 nano Condensation Nucleus Counter at various inlet pressures and various operation temperatures, and design of a new inlet system Kangasluoma, Juha; Franchin, Alessandro; Duplissy, Jonahtan Atmospheric Measurement Techniques, Vol. 9, Issue 7 https://doi.org/10.5194/amt-9-2977-2016	journal	January 2016
How to reliably detect molecular clusters and nucleation mode particles with Neutral cluster and Air Ion Spectrometer (NAIS) Manninen, Hanna E.; Mirme, Sander; Mirme, Aadu Atmospheric Measurement Techniques, Vol. 9, Issue 8 https://doi.org/10.5194/amt-9-3577-2016	journal	January 2016

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