Effect of ions on sulfuric acid-water binary particle formation II: Experimental data and comparison with QC-normalized classical nucleation theory

Autor: Duplissy, Jonathan, Merikanto, J., Franchin, A., Tsagkogeorgas, G., Kangasluoma, J., Wimmer, D., Vuollekoski, H., Schobesberger, S., Lehtipalo, K., Flagan, R.C., Brus, D., Donahue, N.M., Vehkämäki, H., Almeida, J., Amorim, A., Barmet, P., Bianchi, F., Breitenlechner, M., Dunne, E.M., Guida, R., Henschel, H., Junninen, H., Kirkby, J., Kürten, A., Kupc, A., Määttänen, Anni, Makhmutov, V., Mathot, S., Nieminen, T., Onnela, A., Praplan, A.P., Riccobono, F., Rondo, L., Steiner, G., Tome, A., Walther, H., Baltensperger, U., Carslaw, K.S., Dommen, J., Hansel, A., Petäjä, T., Sipilä, M., Stratmann, F., Vrtala, A., Wagner, P.E., Worsnop, D.R., Curtius, J., Kulmala, M.
Přispěvatelé: Helsinki Institute of Physics (HIP), University of Helsinki, Department of Physics [Helsinki], Falculty of Science [Helsinki], University of Helsinki-University of Helsinki, Finnish Meteorological Institute (FMI), Leibniz Institute for Tropospheric Research (TROPOS), Institute for Atmospheric and Environmental Sciences [Frankfurt/Main] (IAU), Goethe-University Frankfurt am Main, Department of Atmospheric Sciences [Seattle], University of Washington [Seattle], Departments of Environmental Science and Engineering and Chemical Engineering, California Institute of Technology (CALTECH), Center for Atmospheric Particle Studies [Pittsburgh] (CAPS), Carnegie Mellon University [Pittsburgh] (CMU), CERN Theoretical Physics Department, CERN [Genève], CENTRA-SIM, IDL-Faculdade de Ciencias da Universidade de Lisboa, Laboratory of Atmospheric Chemistry [Paul Scherrer Institute] (LAC), Paul Scherrer Institute (PSI), Department Construction, Traffic and Environment, Canton of Aargau, Institute for Atmospheric and Climate Science [Zürich] (IAC), Eidgenössische Technische Hochschule - Swiss Federal Institute of Technology [Zürich] (ETH Zürich), Institut für Ionenphysik und Angewandte Physik - Institute for Ion Physics and Applied Physics [Innsbruck], Leopold Franzens Universität Innsbruck - University of Innsbruck, School of Earth and Environment [Leeds] (SEE), University of Leeds, Aerosol Physics and Environmental Physics [Vienna], University of Vienna [Vienna], PLANETO - LATMOS, Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS), Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Université Pierre et Marie Curie - Paris 6 (UPMC)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS), Solar and Cosmic Ray Research Laboratory [Moscow], P. N. Lebedev Physical Institute of the Russian Academy of Sciences [Moscow] (LPI RAS), Russian Academy of Sciences [Moscow] (RAS)-Russian Academy of Sciences [Moscow] (RAS), Helsingin yliopisto = Helsingfors universitet = University of Helsinki, Helsingin yliopisto = Helsingfors universitet = University of Helsinki-Helsingin yliopisto = Helsingfors universitet = University of Helsinki
Jazyk: angličtina
Rok vydání: 2016
Předmět:
Zdroj: Journal of Geophysical Research: Atmospheres
Journal of Geophysical Research: Atmospheres, American Geophysical Union, 2016, 121 (4), pp.1752-1775. ⟨10.1002/2015JD023539⟩
Journal of Geophysical Research: Atmospheres, 2016, 121 (4), pp.1752-1775. ⟨10.1002/2015JD023539⟩
ISSN: 2169-897X
2169-8996
DOI: 10.1002/2015JD023539⟩
Popis: International audience; We report comprehensive, demonstrably contaminant-free measurements of binary particle formation rates by sulfuric acid and water for neutral and ion-induced pathways conducted in the European Organization for Nuclear Research Cosmics Leaving Outdoor Droplets chamber. The recently developed Atmospheric Pressure interface-time of flight-mass spectrometer was used to detect contaminants in charged clusters and to identify runs free of any contaminants. Four parameters were varied to cover ambient conditions: sulfuric acid concentration (105 to 109 mol cm−3), relative humidity (11% to 58%), temperature (207 K to 299 K), and total ion concentration (0 to 6800 ions cm−3). Formation rates were directly measured with novel instruments at sizes close to the critical cluster size (mobility size of 1.3 nm to 3.2 nm). We compare our results with predictions from Classical Nucleation Theory normalized by Quantum Chemical calculation (QC-normalized CNT), which is described in a companion paper. The formation rates predicted by the QC-normalized CNT were extended from critical cluster sizes to measured sizes using the UHMA2 sectional particle microphysics model. Our results show, for the first time, good agreement between predicted and measured particle formation rates for the binary (neutral and ion-induced) sulfuric acid-water system. Formation rates increase with RH, sulfuric acid, and ion concentrations and decrease with temperature at fixed RH and sulfuric acid concentration. Under atmospheric conditions, neutral particle formation dominates at low temperatures, while ion-induced particle formation dominates at higher temperatures. The good agreement between the theory and our comprehensive data set gives confidence in using the QC-normalized CNT as a powerful tool to study neutral and ion-induced binary particle formation in atmospheric modeling.
Databáze: OpenAIRE
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