Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures. Kuerten, A., Bianchi, F., Almeida, J., Kupiainen-Maatta, O., Dunne, E., M., Duplissy, J., Williamson, C., Barmet, P., Breitenlechner, M., Dommen, J., Donahue, N., M., Flagan, R., C., Franchin, A., Gordon, H., Hakala, J., Hansel, A., Heinritzi, M., Ickes, L., Jokinen, T., Kangasluoma, J., Kim, J., Kirkby, J., Kupc, A., Lehtipalo, K., Leiminger, M., Makhmutov, V., Onnela, A., Ortega, I., K., Petaja, T., Praplan, A., P., Riccobono, F., Rissanen, M., P., Rondo, L., Schnitzhofer, R., Schobesberger, S., Smith, J., N., Steiner, G., Stozhkov, Y., Tome, A., Trostl, J., Tsagkogeorgas, G., Wagner, P., E., Wimmer, D., Ye, P., Baltensperger, U., Carslaw, K., Kulmala, M., Curtius, J., Kürten, A., Bianchi, F., Almeida, J., Kupiainen-Määttä, O., Dunne, E., M., Duplissy, J., Williamson, C., Barmet, P., Breitenlechner, M., Dommen, J., Donahue, N., M., Flagan, R., C., Franchin, A., Gordon, H., Hakala, J., Hansel, A., Heinritzi, M., Ickes, L., Jokinen, T., Kangasluoma, J., Kim, J., Kirkby, J., Kupc, A., Lehtipalo, K., Leiminger, M., Makhmutov, V., Onnela, A., Ortega, I., K., Petäjä, T., Praplan, A., P., Riccobono, F., Rissanen, M., P., Rondo, L., Schnitzhofer, R., Schobesberger, S., Smith, J., N., Steiner, G., Stozhkov, Y., Tomé, A., Tröstl, J., Tsagkogeorgas, G., Wagner, P., E., Wimmer, D., Ye, P., Baltensperger, U., Carslaw, K., Kulmala, M., & Curtius, J. Journal of Geophysical Research, 121(20):12,377-12,400, 2016.
Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures [link]Website  doi  abstract   bibtex   
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 × 105 and 1 × 109cm-3, and ammonia mixing ratios from zero added ammonia, i.e., nominally pure binary, to a maximumof ~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.
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 title = {Experimental particle formation rates spanning tropospheric sulfuric acid and ammonia abundances, ion production rates, and temperatures},
 type = {article},
 year = {2016},
 pages = {12,377-12,400},
 volume = {121},
 websites = {http://onlinelibrary.wiley.com/doi/10.1002/2015JD023908/full},
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 abstract = {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 × 105 and 1 × 109cm-3, and ammonia mixing ratios from zero added ammonia, i.e., nominally pure binary, to a maximumof ~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.},
 bibtype = {article},
 author = {Kuerten, Andreas and Bianchi, Federico and Almeida, Joao and Kupiainen-Maatta, Oona and Dunne, Eimear M. and Duplissy, Jonathan and Williamson, Christina and Barmet, Peter and Breitenlechner, Martin and Dommen, Josef and Donahue, Neil M. and Flagan, Richard C. and Franchin, Alessandro and Gordon, Hamish and Hakala, Jani and Hansel, Armin and Heinritzi, Martin and Ickes, Luisa and Jokinen, Tuija and Kangasluoma, Juha and Kim, Jaeseok and Kirkby, Jasper and Kupc, Agnieszka and Lehtipalo, Katrianne and Leiminger, Markus and Makhmutov, Vladimir and Onnela, Antti and Ortega, Ismael K. and Petaja, Tuukka and Praplan, Arnaud P. and Riccobono, Francesco and Rissanen, Matti P. and Rondo, Linda and Schnitzhofer, Ralf and Schobesberger, Siegfried and Smith, James N. and Steiner, Gerhard and Stozhkov, Yuri and Tome, Antonio and Trostl, Jasmin and Tsagkogeorgas, Georgios and Wagner, Paul E. and Wimmer, Daniela and Ye, Penglin and Baltensperger, Urs and Carslaw, Ken and Kulmala, Markku and Curtius, Joachim and Kürten, Andreas and Bianchi, Federico and Almeida, Joao and Kupiainen-Määttä, Oona and Dunne, Eimear M. and Duplissy, Jonathan and Williamson, Christina and Barmet, Peter and Breitenlechner, Martin and Dommen, Josef and Donahue, Neil M. and Flagan, Richard C. and Franchin, Alessandro and Gordon, Hamish and Hakala, Jani and Hansel, Armin and Heinritzi, Martin and Ickes, Luisa and Jokinen, Tuija and Kangasluoma, Juha and Kim, Jaeseok and Kirkby, Jasper and Kupc, Agnieszka and Lehtipalo, Katrianne and Leiminger, Markus and Makhmutov, Vladimir and Onnela, Antti and Ortega, Ismael K. and Petäjä, Tuukka and Praplan, Arnaud P. and Riccobono, Francesco and Rissanen, Matti P. and Rondo, Linda and Schnitzhofer, Ralf and Schobesberger, Siegfried and Smith, James N. and Steiner, Gerhard and Stozhkov, Yuri and Tomé, António and Tröstl, Jasmin and Tsagkogeorgas, Georgios and Wagner, Paul E. and Wimmer, Daniela and Ye, Penglin and Baltensperger, Urs and Carslaw, Ken and Kulmala, Markku and Curtius, Joachim},
 doi = {10.1002/2015JD023908},
 journal = {Journal of Geophysical Research},
 number = {20}
}

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