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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 neutralizedmore » 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.« less
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Publication Date:
Grant/Contract Number:
SC0014469
Type:
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 GmbH
Sponsoring Org:
USDOE
Country of Publication:
Germany
Language:
English
OSTI Identifier:
1460017

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., 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. 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, and Kulmala, Markku. 2017. "The role of ions in new particle formation in the CLOUD chamber". Germany. doi: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 = {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 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},
journal = {Atmospheric Chemistry and Physics (Online)},
number = 24,
volume = 17,
place = {Germany},
year = {2017},
month = {12}
}