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Lawler, Michael Joseph ; Winkler, Paul M. ; Kim, Jaeseok ; Ahlm, Lars ; Tröstl, Jasmin ; Praplan, Arnaud Patrick ; Schobesberger, Siegfried ; Kürten, Christoph Andreas ; Kirkby, Jasper ; Bianchi, Federico ; Duplissy, Jonathan ; Hansel, Armin ; Jokinen, Tuija ; Keskinen, Helmi ; Lehtipalo, Katrianne ; Leiminger, Markus ; Petäjä, Tuukka ; Rissanen, Matti P. ; Rondo, Linda ; Simon, Mario ; Sipilä, Mikko ; Williamson, Christina ; Wimmer, Daniela ; Riipinen, Ilona ; Virtanen, Annele ; Smith, James N.
New particle formation driven by acid–base chemistry was initiated in the CLOUD chamber at CERN by introducing atmospherically relevant levels of gas-phase sulfuric acid and dimethylamine (DMA). Ammonia was also present in the chamber as a gas-phase contaminant from earlier experiments. The composition of particles with volume median diameters (VMDs) as small as 10 nm was measured by the Thermal Desorption Chemical Ionization Mass Spectrometer (TDCIMS). Particulate ammonium-to-dimethylaminium ratios were higher than the gas-phase ammonia-to-DMA ratios, suggesting preferential uptake of ammonia over DMA for the collected 10–30 nm VMD particles. This behavior is not consistent with present nanoparticle physicochemical models, which predict a higher dimethylaminium fraction when NH3 and DMA are present at similar gas-phase concentrations. Despite the presence in the gas phase of at least 100 times higher base concentrations than sulfuric acid, the recently formed particles always had measured base : acid ratios lower than 1 : 1. The lowest base fractions were found in particles below 15 nm VMD, with a strong size-dependent composition gradient. The reasons for the very acidic composition remain uncertain, but a plausible explanation is that the particles did not reach thermodynamic equilibrium with respect to the bases due to rapid heterogeneous conversion of SO2 to sulfate. These results indicate that sulfuric acid does not require stabilization by ammonium or dimethylaminium as acid–base pairs in particles as small as 10 nm.
Tröstl, Jasmin ; Chuang, Wayne K. ; Gordon, Hamish ; Heinritzi, Martin ; Yan, Chao ; Molteni, Ugo ; Ahlm, Lars ; Frege, Carla ; Bianchi, Federico ; Wagner, Robert ; Simon, Mario ; Lehtipalo, Katrianne ; Williamson, Christina ; Craven, Jill ; Duplissy, Jonathan ; Adamov, Alexey ; Almeida, Joao ; Bernhammer, Anne-Kathrin ; Breitenlechner, Martin ; Brilke, Sophia ; Dias, Antonio ; Ehrhart, Sebastian ; Flagan, Richard C. ; Franchin, Alessandro ; Fuchs, Claudia ; Guida, Roberto ; Gysel, Martin ; Hansel, Armin ; Hoyle, Christopher Robert ; Jokinen, Tuija ; Junninen, Heikki ; Kangasluoma, Juha ; Keskinen, Helmi ; Kim, Jaeseok ; Krapf, Manuel ; Kürten, Christoph Andreas ; Laaksonen, Ari ; Lawler, Michael Joseph ; Leiminger, Markus ; Mathot, Serge ; Möhler, Ottmar ; Nieminen, Tuomo ; Onnela, Antti ; Petäjä, Tuukka ; Piel, Felix ; Miettinen, Pasi ; Rissanen, Matti P. ; Rondo, Linda ; Sarnela, Nina ; Schobesberger, Siegfried ; Sengupta, Kamalika ; Sipilä, Mikko ; Smith, James N. ; Steiner, Gerhard ; Tomé, Antonio ; Virtanen, Annele ; Wagner, Andrea Christine ; Weingartner, Ernest ; Wimmer, Daniela ; Winkler, Paul M. ; Ye, Penglin ; Carslaw, Kenneth S. ; Curtius, Joachim ; Dommen, Josef ; Kirkby, Jasper ; Kulmala, Markku ; Riipinen, Ilona ; Worsnop, Douglas R. ; Donahue, Neil McPherson ; Baltensperger, Urs
About half of present-day cloud condensation nuclei originate from atmospheric nucleation, frequently appearing as a burst of new particles near midday1. Atmospheric observations show that the growth rate of new particles often accelerates when the diameter of the particles is between one and ten nanometres2,3. In this critical size range, new particles are most likely to be lost by coagulation with pre-existing particles4, thereby failing to form new cloud condensation nuclei that are typically 50 to 100 nanometres across. Sulfuric acid vapour is often involved in nucleation but is too scarce to explain most subsequent growth5,6, leaving organic vapours as the most plausible alternative, at least in the planetary boundary layer7,8,9,10. Although recent studies11,12,13 predict that low-volatility organic vapours contribute during initial growth, direct evidence has been lacking. The accelerating growth may result from increased photolytic production of condensable organic species in the afternoon2, and the presence of a possible Kelvin (curvature) effect, which inhibits organic vapour condensation on the smallest particles (the nano-Köhler theory)2,14, has so far remained ambiguous. Here we present experiments performed in a large chamber under atmospheric conditions that investigate the role of organic vapours in the initial growth of nucleated organic particles in the absence of inorganic acids and bases such as sulfuric acid or ammonia and amines, respectively. Using data from the same set of experiments, it has been shown15 that organic vapours alone can drive nucleation. We focus on the growth of nucleated particles and find that the organic vapours that drive initial growth have extremely low volatilities (saturation concentration less than 10−4.5 micrograms per cubic metre). As the particles increase in size and the Kelvin barrier falls, subsequent growth is primarily due to more abundant organic vapours of slightly higher volatility (saturation concentrations of 10−4.5 to 10−0.5 micrograms per cubic metre). We present a particle growth model that quantitatively reproduces our measurements. Furthermore, we implement a parameterization of the first steps of growth in a global aerosol model and find that concentrations of atmospheric cloud concentration nuclei can change substantially in response, that is, by up to 50 per cent in comparison with previously assumed growth rate parameterizations.
Hoyle, Christopher Robert ; Fuchs, Claudia ; Järvinen, Emma ; Saathoff, Harald ; Dias, Antonio ; El Haddad, Imad ; Gysel, Martin ; Coburn, Sean C. ; Tröstl, Jasmin ; Bernhammer, Anne-Kathrin ; Bianchi, Federico ; Breitenlechner, Martin ; Corbin, Joel C. ; Craven, Jill ; Donahue, Neil McPherson ; Duplissy, Jonathan ; Ehrhart, Sebastian ; Frege, Carla ; Gordon, Hamish ; Höppel, Niko Florian ; Heinritzi, Martin ; Kristensen, Thomas Bjerring ; Molteni, Ugo ; Nichman, Leonid ; Pinterich, Tamara ; Prévôt, André Stephan Henry ; Simon, Mario ; Slowik, Jay G. ; Steiner, Gerhard ; Tomé, Antonio ; Vogel, Alexander L. ; Volkamer, Rainer ; Wagner, Andrea Christine ; Wagner, Robert ; Wexler, Anthony S. ; Williamson, Christina ; Winkler, Paul M. ; Yan, Chao ; Amorim, Antonio ; Dommen, Josef ; Curtius, Joachim ; Gallagher, Martin William ; Flagan, Richard C. ; Hansel, Armin ; Kirkby, Jasper ; Kulmala, Markku ; Möhler, Ottmar ; Stratmann, Frank ; Worsnop, Douglas R. ; Baltensperger, Urs
The growth of aerosol due to the aqueous phase oxidation of sulfur dioxide by ozone was measured in laboratory-generated clouds created in the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN). Experiments were performed at 10 and −10 °C, on acidic (sulfuric acid) and on partially to fully neutralised (ammonium sulfate) seed aerosol. Clouds were generated by performing an adiabatic expansion – pressurising the chamber to 220 hPa above atmospheric pressure, and then rapidly releasing the excess pressure, resulting in a cooling, condensation of water on the aerosol and a cloud lifetime of approximately 6 min. A model was developed to compare the observed aerosol growth with that predicted using oxidation rate constants previously measured in bulk solutions. The model captured the measured aerosol growth very well for experiments performed at 10 and −10 °C, indicating that, in contrast to some previous studies, the oxidation rates of SO2 in a dispersed aqueous system can be well represented by using accepted rate constants, based on bulk measurements. To the best of our knowledge, these are the first laboratory-based measurements of aqueous phase oxidation in a dispersed, super-cooled population of droplets. The measurements are therefore important in confirming that the extrapolation of currently accepted reaction rate constants to temperatures below 0 °C is correct.
Hoyle, Christopher Robert ; Fuchs, Claudia ; Järvinen, Emma ; Saathoff, Harald ; Dias, Antonio ; El Haddad, Imad ; Gysel, Martin ; Coburn, Sean C. ; Tröstl, Jasmin ; Bernhammer, Anne-Kathrin ; Bianchi, Federico ; Breitenlechner, Martin ; Corbin, Joel C. ; Craven, Jill ; Donahue, Neil McPherson ; Duplissy, Jonathan ; Ehrhart, Sebastian ; Frege, Carla ; Gordon, Hamish ; Höppel, Niko Florian ; Heinritzi, Martin ; Kristensen, Thomas Bjerring ; Molteni, Ugo ; Nichman, Leonid ; Pinterich, Tamara ; Prévôt, André Stephan Henry ; Simon, Mario ; Slowik, Jay G. ; Steiner, Gerhard ; Tomé, Antonio ; Vogel, Alexander L. ; Volkamer, Rainer ; Wagner, Andrea Christine ; Wagner, Robert ; Wexler, Anthony S. ; Williamson, Christina ; Winkler, Paul M. ; Yan, Chao ; Amorim, Antonio ; Dommen, Josef ; Curtius, Joachim ; Gallagher, Martin William ; Flagan, Richard C. ; Hansel, Armin ; Kirkby, Jasper ; Kulmala, Markku ; Möhler, Ottmar ; Stratmann, Frank ; Worsnop, Douglas R. ; Baltensperger, Urs
The growth of aerosol due to the aqueous phase oxidation of sulfur dioxide by ozone was measured in laboratory-generated clouds created in the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at the European Organization for Nuclear Research (CERN). Experiments were performed at 10 and −10 °C, on acidic (sulfuric acid) and on partially to fully neutralised (ammonium sulfate) seed aerosol. Clouds were generated by performing an adiabatic expansion – pressurising the chamber to 220 hPa above atmospheric pressure, and then rapidly releasing the excess pressure, resulting in a cooling, condensation of water on the aerosol and a cloud lifetime of approximately 6 min. A model was developed to compare the observed aerosol growth with that predicted using oxidation rate constants previously measured in bulk solutions. The model captured the measured aerosol growth very well for experiments performed at 10 and −10 °C, indicating that, in contrast to some previous studies, the oxidation rates of SO2 in a dispersed aqueous system can be well represented by using accepted rate constants, based on bulk measurements. To the best of our knowledge, these are the first laboratory-based measurements of aqueous phase oxidation in a dispersed, super-cooled population of droplets. The measurements are therefore important in confirming that the extrapolation of currently accepted reaction rate constants to temperatures below 0 °C is correct.
Wagner, Robert ; Yan, Chao ; Lehtipalo, Katrianne ; Duplissy, Jonathan ; Nieminen, Tuomo ; Kangasluoma, Juha ; Ahonen, Lauri R. ; Dada, Lubna ; Kontkanen, Jenni ; Manninen, Hanna Elina ; Dias, Antonio ; Amorim, Antonio ; Bauer, Paulus Salomon ; Bergen, Anton ; Bernhammer, Anne-Kathrin ; Bianchi, Federico ; Brilke, Sophia ; Buenrostro Mazon, Stephany ; 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 Robert ; Kirkby, Jasper ; Kürten, Christoph Andreas ; Kvashnin, Alexander N. ; Laurila, Tiia ; Lawler, Michael Joseph ; Mai, Huajun ; Makhmutov, Vladimir ; Mauldin, Roy Lee ; 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 Christine ; Xiao, Mao ; Ye, Penglin ; Baltensperger, Urs ; Curtius, Joachim ; Donahue, Neil McPherson ; Flagan, Richard C. ; Gallagher, Martin William ; Hansel, Armin ; Smith, James N. ; Tomé, Antonio ; Winkler, Paul M. ; Worsnop, Douglas R. ; Ehn, Mikael ; Sipilä, Mikko ; Kerminen, Veli-Matti ; Petäjä, Tuukka ; Kulmala, Markku
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 nano-particle 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 where 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 1.2 nm diameter. However, depending on particle growth rates and ion concentrations, charged clusters were largely neutralized by ion–ion recombination before they grew to 2.2 nm. 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 2.2 nm. 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.