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Role of Sulphuric Acid, Ammonia and Galactic Cosmic Rays in Atmospheric Aerosol Nucleation

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Role of Sulphuric Acid, Ammonia and Galactic Cosmic Rays in Atmospheric Aerosol Nucleation LETTER doi:10.1038/nature10343 Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation Jasper Kirkby1, Joachim Curtius2, Joa˜o Almeida2,3, Eimear Dunne4, Jonathan Duplissy1,5,6, Sebastian Ehrhart2, Alessandro Franchin5, Ste´phanie Gagne´5,6, Luisa Ickes2, Andreas Ku¨rten2, Agnieszka Kupc7, Axel Metzger8, Francesco Riccobono9, Linda Rondo2, Siegfried Schobesberger5, Georgios Tsagkogeorgas10, Daniela Wimmer2, Antonio Amorim3, Federico Bianchi9,11, Martin Breitenlechner8, Andre´ David1, Josef Dommen9, Andrew Downard12, Mikael Ehn5, Richard C. Flagan12, Stefan Haider1, Armin Hansel8, Daniel Hauser8, Werner Jud8, Heikki Junninen5, Fabian Kreissl2, Alexander Kvashin13, Ari Laaksonen14, Katrianne Lehtipalo5, Jorge Lima3, Edward R. Lovejoy15, Vladimir Makhmutov13, Serge Mathot1, Jyri Mikkila¨5, Pierre Minginette1, Sandra Mogo3, Tuomo Nieminen5, Antti Onnela1, Paulo Pereira3, Tuukka Peta¨ja¨5, Ralf Schnitzhofer8, John H. Seinfeld12, Mikko Sipila¨5,6, Yuri Stozhkov13, Frank Stratmann10, Antonio Tome´3, Joonas Vanhanen5, Yrjo Viisanen16, Aron Vrtala7, Paul E. Wagner7, Hansueli Walther9, Ernest Weingartner9, Heike Wex10, Paul M. Winkler7, Kenneth S. Carslaw4, Douglas R. Worsnop5,17, Urs Baltensperger9 & Markku Kulmala5 Atmospheric aerosols exert an important influence on climate1 in the atmosphere25,26. Because the primary source of ions in the global through their effects on stratiform cloud albedo and lifetime2 and troposphere is galactic cosmic rays (GCRs), their role in atmospheric the invigoration of convective storms3. Model calculations suggest nucleation is of considerable interest as a possible physical mechanism that almost half of the global cloud condensation nuclei in the for climate variability caused by the Sun27,28. atmospheric boundary layer may originate from the nucleation of Here we address three issues that currently limit our understanding of aerosols from trace condensable vapours4, although the sensitivity of atmospheric nucleation and its influence on climate7. First, quantitative the number of cloud condensation nuclei to changes of nucleation measurements of the roles of ions and ternary vapours are lacking. rate may be small5,6. Despite extensive research, fundamental Second, the nucleation mechanism and the molecular composition of questions remain about the nucleation rate of sulphuric acid the critical nucleus have not been directly measured. Third, it remains an particles and the mechanisms responsible, including the roles of open question whether laboratory measurements are able to reproduce galactic cosmic rays and other chemical species such as ammonia7. atmospheric observations: recent experiments have concluded that atmo- Here we present the first results from the CLOUD experiment at spheric concentrations of H2SO4 and H2O without ternary vapours are CERN. We find that atmospherically relevant ammonia mixing sufficient29 or insufficient19 to explain boundary-layer nucleation rates. ratios of 100 parts per trillion by volume, or less, increase the nuc- We present here the first results from the CLOUD experiment at leation rate of sulphuric acid particles more than 100–1,000-fold. CERN (see Methods, Supplementary Information and Supplementary Time-resolved molecular measurements reveal that nucleation pro- Fig. 1 for experimental details). The measurements, obtained at the ceeds by a base-stabilization mechanism involving the stepwise CERN Proton Synchrotron, represent the most rigorous laboratory accretion of ammonia molecules. Ions increase the nucleation rate evaluation yet accomplished of binary, ternary and ion-induced nuc- by an additional factor of between two and more than ten at ground- leation of sulphuric acid particles under atmospheric conditions. 23 21 level galactic-cosmic-ray intensities, provided that the nucleation The nucleation rates (J,cm s ) are measured under neutral (Jn), rate lies below the limiting ion-pair production rate. We find that GCR (Jgcr) and charged pion beam (Jch) conditions, corresponding to 23 ion-induced binary nucleation of H2SO4–H2O can occur in the mid- ion-pair concentrations of about 0, 400 and 3,000 cm , respectively. troposphere but is negligible in the boundary layer. However, even A typical sequence of Jn, Jgcr and Jch measurements is shown in Sup- with the large enhancements in rate due to ammonia and ions, plementary Fig. 2 and is described in the Supplementary Information. atmospheric concentrations of ammonia and sulphuric acid are Both Jgcr and Jch comprise the sum of ion-induced and neutral nuc- insufficient to account for observed boundary-layer nucleation. leation rates, whereas Jn measures the neutral rate alone. The nuc- The primary vapour responsible for atmospheric nucleation is leation rates are shown in Fig. 1 as a function of [H2SO4] at 248, 278 thought to be sulphuric acid. However, theory suggests that peak con- and 292 K. As the temperature is reduced, lower H2SO4 concentrations centrations in the boundary layer (106–107 cm23; ref. 8) are usually too are sufficient to maintain the same nucleation rates, as a result of the low for the binary nucleation of H2SO4–H2O to proceed. Furthermore, decrease in the H2SO4 saturation vapour pressure. Apart from con- after nucleation there is generally insufficient H2SO4 to grow the clusters taminants (see below), the only condensable vapours present in the to cloud condensation nucleus sizes (more than 50 nm), so organic chamber for these data are H2SO4 and H2O. The experimental results species are primarily responsible for particle growth9,10.Nucleationof are slightly higher than model calculations30 based on thermochemical 23 sulphuric acid particles is known to be enhanced by the presence of data for charged H2SO4–H2O clusters under Jch ionization condi- ternary species such as ammonia11–13 or organic compounds14 such as tions, but they show similar curvature and slope. 15–17 18,19 amines or oxidized organic compounds . Ions are also expected to The presence of ions from ground-level GCR ionization (Jgcr curves) enhance nucleation20–24, and ion-induced nucleation has been observed enhances the neutral nucleation rate roughly twofold at 292 K and 1CERN, CH-1211 Geneva, Switzerland. 2Goethe-University of Frankfurt, Institute for Atmospheric and Environmental Sciences, 60438 Frankfurt am Main, Germany. 3SIM, University of Lisbon and University of Beira Interior, 1749-016 Lisbon, Portugal. 4University of Leeds, School of Earth and Environment, LS2-9JT Leeds, United Kingdom. 5University of Helsinki, Department of Physics, FI-00014 Helsinki, Finland. 6Helsinki Institute of Physics, University of Helsinki, FI-00014 Helsinki, Finland. 7University of Vienna, Faculty of Physics, 1090 Vienna, Austria. 8Ionicon Analytik GmbH and University of Innsbruck, Institute for Ion and Applied Physics, 6020 Innsbruck, Austria. 9Paul Scherrer Institut, Laboratory of Atmospheric Chemistry, CH-5232 Villigen, Switzerland. 10Leibniz Institute for Tropospheric Research, 04318 Leipzig, Germany. 11University of Milan, Department of Inorganic, Metallorganic, and Analytical Chemistry, 20133 Milan, Italy. 12California Institute of Technology, Division of Chemistry and Chemical Engineering, Pasadena, California 91125, USA, 13Lebedev Physical Institute, Solar and Cosmic Ray Research Laboratory, 119991 Moscow, Russia. 14University of Eastern Finland, FI-70211 Kuopio, Finland. 15NOAA Earth System Research Laboratory, Boulder, Colorado 80305, USA. 16Finnish Meteorological Institute, FI-00101 Helsinki, Finland. 17Aerodyne Research Inc., Billerica, Massachusetts 01821, USA. 25 AUGUST 2011 | VOL 476 | NATURE | 429 ©2011 Macmillan Publishers Limited. All rights reserved RESEARCH LETTER 6 100 a 5 10 ) –1 s 1 –3 4 (cm 1.7 J 0.1 3 ) –1 s –3 0.01 2 (cm Nucleation rate, 1.7 J 0.001 1 100 b 0 10 Nucleation rate, 0 1,000 2,000 3,000 4,000 5,000 Negative ion concentration (cm–3) 1 Figure 2 | Plots of nucleation rate against negative ion concentration. Nucleation rates as a function of negative ion concentration at 292 K and 8 23 0.1 [H2SO4] 5 4.5 3 10 cm (purple line), and at 278 K and 8 23 [H2SO4] 5 1.5 3 10 cm (green line). Triangles, Jch; filled circles, Jgcr; open circles, Jn. All measurements were made at 38% relative humidity and 35 p.p.t.v. 0.01 NH3. Neutral nucleation rates, Jn, were effectively measured at zero ion pair concentration (ion or charged-cluster lifetime ,1 s). The curves are fits of the 2 p form J 5 j0 1 k[ion ] , where j0, k and p are free parameters. The error bars 0.001 indicate only the point-to-point 1s errors; the nucleation rates and ion 5 6 7 8 107 2 3 4 5 6 78 108 2 3 4 5 6 7 8 109 concentrations each have estimated overall scale uncertainties of 630%. –3 Sulphuric acid concentration, [H2SO4] (cm ) The chemical composition of nucleating clusters containing up to 2 Figure 1 | Plots of nucleation rate against H2SO4 concentration. Neutral, n 5 20 sulphuric acid molecules, including the HSO4 ion, is shown GCR and charged (pion beam) nucleation rates are shown at 1.7 nm diameter, in Fig. 3. At 292 K the clusters above n 5 4 are found always to be J1.7, as a function of sulphuric acid concentration at 38% relative humidity. accompanied by additional nitrogen-containing molecules, comprising a, Rates at 292 K; b, rates at 248 K (blue) and 278 K (green). The NH3 mixing NH , amines (mainly dimethylamine and ethylamine) and urea ratios correspond to the contaminant level (,35 p.p.t.v. at 278 and 292 K; 3 (Fig.3c, d). Althoughtheseternary vapours werenotintentionallyadded ,50 p.p.t.v. at 248 K). Triangles, Jch; filled circles, Jgcr; open circles, Jn.The 30 to the chamber—at least initially—they are crucial to the nucleation. The predictions of the PARNUC model for binary H2SO4–H2O charged nucleation, Jch, are indicated by the coloured bands. The fitted curves are drawn measured contaminant mixing ratios of ammonia and total amines were to guide the eye. The error bars indicate the estimated total statistical and less than 35 parts per trillion by volume (p.p.t.v.) and less than 50 p.p.t.v., systematic 1s measurement uncertainties, although the overall factor 2 respectively. It is notable that the nucleating H2SO4 clusters included systematic scale uncertainty on [H2SO4] is not shown.
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