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

Abstract

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 bymore » 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.« less

Authors:
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Publication Date:
Research Org.:
University of California, Irvine, CA 92697, United States
Sponsoring Org.:
USDOE
OSTI Identifier:
1460017
Alternate Identifier(s):
OSTI ID: 1502074
Grant/Contract Number:  
SC0014469
Resource Type:
Journal Article: Published Article
Journal Name:
Atmospheric Chemistry and Physics (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics (Online) Journal Volume: 17 Journal Issue: 24; Journal ID: ISSN 1680-7324
Publisher:
Copernicus Publications, EGU
Country of Publication:
Germany
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

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, and Kulmala, Markku. The role of ions in new particle formation in the CLOUD chamber. Germany: N. p., 2017. Web. doi:10.5194/acp-17-15181-2017.
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. The role of ions in new particle formation in the CLOUD chamber. Germany. https://doi.org/10.5194/acp-17-15181-2017
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, and Kulmala, Markku. 2017. "The role of ions in new particle formation in the CLOUD chamber". Germany. https://doi.org/10.5194/acp-17-15181-2017.
@article{osti_1460017,
title = {The role of ions in new particle formation in the CLOUD chamber},
author = {Wagner, Robert and Yan, Chao and Lehtipalo, Katrianne and Duplissy, Jonathan and Nieminen, Tuomo and Kangasluoma, Juha and Ahonen, Lauri R. and Dada, Lubna and Kontkanen, Jenni and Manninen, Hanna E. and Dias, Antonio and Amorim, Antonio and Bauer, Paulus S. and Bergen, Anton and Bernhammer, Anne-Kathrin and Bianchi, Federico and Brilke, Sophia and Mazon, Stephany Buenrostro and Chen, Xuemeng and Draper, Danielle C. and Fischer, Lukas and Frege, Carla and Fuchs, Claudia and Garmash, Olga and Gordon, Hamish and Hakala, Jani and Heikkinen, Liine and Heinritzi, Martin and Hofbauer, Victoria and Hoyle, Christopher R. and Kirkby, Jasper and Kürten, Andreas and Kvashnin, Alexander N. and Laurila, Tiia and Lawler, Michael J. and Mai, Huajun and Makhmutov, Vladimir and Mauldin III, Roy L. and Molteni, Ugo and Nichman, Leonid and Nie, Wei and Ojdanic, Andrea and Onnela, Antti and Piel, Felix and Quéléver, Lauriane L. J. and Rissanen, Matti P. and Sarnela, Nina and Schallhart, Simon and Sengupta, Kamalika and Simon, Mario and Stolzenburg, Dominik and Stozhkov, Yuri and Tröstl, Jasmin and Viisanen, Yrjö and Vogel, Alexander L. and Wagner, Andrea C. and Xiao, Mao and Ye, Penglin and Baltensperger, Urs and Curtius, Joachim and Donahue, Neil M. and Flagan, Richard C. and Gallagher, Martin and Hansel, Armin and Smith, James N. and Tomé, António and Winkler, Paul M. and Worsnop, Douglas and Ehn, Mikael and Sipilä, Mikko and Kerminen, Veli-Matti and Petäjä, Tuukka and Kulmala, Markku},
abstractNote = {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.},
doi = {10.5194/acp-17-15181-2017},
url = {https://www.osti.gov/biblio/1460017}, journal = {Atmospheric Chemistry and Physics (Online)},
issn = {1680-7324},
number = 24,
volume = 17,
place = {Germany},
year = {Thu Dec 21 00:00:00 EST 2017},
month = {Thu Dec 21 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at https://doi.org/10.5194/acp-17-15181-2017

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Cited by: 42 works
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Works referenced in this record:

The History of Condensation Nucleus Counters
journal, October 2000


Radon activity in the lower troposphere and its impact on ionization rate: a global estimate using different radon emissions
journal, January 2011


An Instrumental Comparison of Mobility and Mass Measurements of Atmospheric Small Ions
journal, March 2011


Experimental investigation of ion–ion recombination under atmospheric conditions
journal, January 2015


Aerosol nucleation and its role for clouds and Earth's radiative forcing in the aerosol-climate model ECHAM5-HAM
journal, January 2010


Turbulent deposition and gravitational sedimentation of an aerosol in a vessel of arbitrary shape
journal, January 1981


Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures
journal, October 2016


Natural and anthropogenic negative ions in the troposphere
journal, January 1989


Charging state of the atmospheric nucleation mode: Implications for separating neutral and ion-induced nucleation
journal, January 2007


New particle formation in the free troposphere: A question of chemistry and timing
journal, May 2016


Heterogeneous Nucleation onto Ions and Neutralized Ions: Insights into Sign-Preference
journal, March 2016


PTR3: An Instrument for Studying the Lifecycle of Reactive Organic Carbon in the Atmosphere
journal, May 2017


Particle Size Magnifier for Nano-CN Detection
journal, March 2011


Sub-3 nm particle size and composition dependent response of a nano-CPC battery
journal, January 2014


Aerosols, Cloud Microphysics, and Fractional Cloudiness
journal, September 1989


Neutral molecular cluster formation of sulfuric acid–dimethylamine observed in real time under atmospheric conditions
journal, October 2014


Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation
journal, August 2011


Estimating the contribution of ion–ion recombination to sub-2 nm cluster concentrations from atmospheric measurements
journal, January 2013


How to reliably detect molecular clusters and nucleation mode particles with Neutral cluster and Air Ion Spectrometer (NAIS)
journal, January 2016


Direct Observations of Atmospheric Aerosol Nucleation
journal, February 2013


Analysis of one year of Ion-DMPS data from the SMEAR II station, Finland
journal, January 2008


Charged and total particle formation and growth rates during EUCAARI 2007 campaign in Hyytiälä
journal, January 2009


Formation and growth rates of ultrafine atmospheric particles: a review of observations
journal, March 2004


EUCAARI ion spectrometer measurements at 12 European sites – analysis of new particle formation events
journal, January 2010


Atmospheric ion-induced nucleation of sulfuric acid and water
journal, January 2004


A high-resolution mass spectrometer to measure atmospheric ion composition
journal, January 2010


Performance of a corona ion source for measurement of sulfuric acid by chemical ionization mass spectrometry
journal, January 2011


Factors of air ion balance in a coniferous forest according to measurements in Hyytiälä, Finland
journal, January 2006


A large source of low-volatility secondary organic aerosol
journal, February 2014


From molecular clusters to nanoparticles: Role of ambient ionization in tropospheric aerosol formation
journal, March 2001


Heterogeneous Nucleation Experiments Bridging the Scale from Molecular Ion Clusters to Nanoparticles
journal, March 2008


How do air ions reflect variations in ionising radiation in the lower atmosphere in a boreal forest?
journal, January 2016


Operation of the Airmodus A11 nano Condensation Nucleus Counter at various inlet pressures and various operation temperatures, and design of a new inlet system
journal, January 2016


Atmospheric data over a solar cycle: no connection between galactic cosmic rays and new particle formation
journal, January 2010


Molecular understanding of sulphuric acid–amine particle nucleation in the atmosphere
journal, October 2013


Ion-induced nucleation of pure biogenic particles
journal, May 2016


How significantly does coagulational scavenging limit atmospheric particle production?
journal, October 2001


Analysis of atmospheric neutral and charged molecular clusters in boreal forest using pulse-height CPC
journal, January 2009


Atmospheric Ion-induced Aerosol Nucleation
journal, December 2006


Sizing of neutral sub 3nm tungsten oxide clusters using Airmodus Particle Size Magnifier
journal, September 2015


Scanning Electrical Mobility Spectrometer
journal, January 1990


Suppression of new particle formation from monoterpene oxidation by NO x
journal, January 2014


Diffusion of H 2 SO 4 in Humidified Nitrogen:  Hydrated H 2 SO 4
journal, March 2000


Atmospheric sulphuric acid and neutral cluster measurements using CI-APi-TOF
journal, January 2012