Auflistung nach Autor:in "Stratmann, Frank"

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Evolution of nanoparticle composition in CLOUD in presence of sulphuric acid, ammonia and organics
(AIP Publishing, 24.06.2013) Keskinen, Helmi; Virtanen, Annele; Joutsensaari, Jorma; Tsagkogeorgas, Georgios; Duplissy, Jonathan; Schobesberger, Siegfried; Gysel, Martin; Riccobono, Francesco; Slowik, Jay Gates; Bianchi, Federico; Yli-Juuti, Taina; Lehtipalo, Katrianne; Rondo, Linda; Breitenlechner, Martin; Kupc, Agnieszka; Almeida, João; Amorim, Antonio; Dunne, Eimear M.; Downard, Andrew J.; Ehrhart, Sebastian; Franchin, Alessandro; Kajos, Maija K.; Kirkby, Jasper; Kürten, Andreas; Nieminen, Tuomo; Makhmutov, Vladimir; Mathot, Serge; Miettinen, Pasi; Onnela, Antti; Petäjä, Tuukka; Praplan, Arnaud; Santos, Filipe D.; Schallhart, Simon; Sipilä, Mikko; Stozhkov, Yuri; Tomé, Antonio; Vaattovaara, Petri; Wimmer, Daniela; Prévôt, André S.H.; Dommen, Josef; Donahue, Neil M.; Flagan, Richard C.; Viisanen, Yrjö; Weingartner, Ernest; Riipinen, Ilona; Hansel, Armin; Curtius, Joachim; Kulmala, Markku; Worsnop, Douglas R.; Baltensperger, Urs; Wex, Heike; Stratmann, Frank; Laaksonen, Ari; DeMott, Paul J.; O'Dowd, Colin D.
04B - Beitrag Konferenzschrift
Evolution of particle composition in CLOUD nucleation experiments
(Copernicus, 2013) Keskinen, Helmi; Virtanen, Annele; Joutsensaari, Jorma; Tsagkogeorgas, Georgios; Duplissy, Jonathan; Schobesberger, Siegfried; Gysel, Martin; Riccobono, Francesco; Slowik, Jay Gates; Bianchi, Federico; Yli-Juuti, Taina; Lehtipalo, Katrianne; Rondo, Linda; Breitenlechner, Martin; Kupc, Agnieszka; Almeida, João; Amorim, Antonio; Dunne, Eimear M.; Downard, Andrew J.; Ehrhart, Sebastian; Franchin, Alessandro; Kajos, Maija K.; Kirkby, Jasper; Kürten, Andreas; Nieminen, Tuomo; Makhmutov, Vladimir; Mathot, Serge; Miettinen, Pasi; Onnela, Antti; Petäjä, Tuukka; Praplan, Arnaud; Santos, Felipe D.; Schallhart, Simon; Sipilä, Mikko; Stozhkov, Yuri; Tomé, Antonio; Vaattovaara, Petri; Wimmer, Daniela; Prévôt, André; Dommen, Josef; Donahue, Neil M.; Flagan, Richard C.; Weingartner, Ernest; Viisanen, Yrjö; Riipinen, Ilona; Hansel, Armin; Curtius, Joachim; Kulmala, Markku; Worsnop, Douglas R.; Baltensperger, Urs; Wex, Heike; Stratmann, Frank; Laaksonen, Ari
Sulphuric acid, ammonia, amines, and oxidised organics play a crucial role in nanoparticle formation in the atmosphere. In this study, we investigate the composition of nucleated nanoparticles formed from these compounds in the CLOUD (Cosmics Leaving Outdoor Droplets) chamber experiments at CERN (Centre européen pour la recherche nucléaire). The investigation was carried out via analysis of the particle hygroscopicity, ethanol affinity, oxidation state, and ion composition. Hygroscopicity was studied by a hygroscopic tandem differential mobility analyser and a cloud condensation nuclei counter, ethanol affinity by an organic differential mobility analyser and particle oxidation level by a high-resolution time-of-flight aerosol mass spectrometer. The ion composition was studied by an atmospheric pressure interface time-of-flight mass spectrometer. The volume fraction of the organics in the particles during their growth from sizes of a few nanometers to tens of nanometers was derived from measured hygroscopicity assuming the Zdanovskii–Stokes–Robinson relationship, and compared to values gained from the spectrometers. The ZSR-relationship was also applied to obtain the measured ethanol affinities during the particle growth, which were used to derive the volume fractions of sulphuric acid and the other inorganics (e.g. ammonium salts). In the presence of sulphuric acid and ammonia, particles with a mobility diameter of 150 nm were chemically neutralised to ammonium sulphate. In the presence of oxidation products of pinanediol, the organic volume fraction of freshly nucleated particles increased from 0.4 to ~0.9, with an increase in diameter from 2 to 63 nm. Conversely, the sulphuric acid volume fraction decreased from 0.6 to 0.1 when the particle diameter increased from 2 to 50 nm. The results provide information on the composition of nucleated aerosol particles during their growth in the presence of various combinations of sulphuric acid, ammonia, dimethylamine and organic oxidation products.
01A - Beitrag in wissenschaftlicher Zeitschrift
Influence of gas-to-particle partitioning on the hygroscopic and droplet activation behaviour of α-pinene secondary organic aerosol
(Royal Society of Chemistry, 05.08.2009) Jurányi, Zsófia; Gysel, Martin; Duplissy, Jonathan; Weingartner, Ernest; Tritscher, Torsten; Dommen, Josef; Henning, Silvia; Ziese, Markus; Kiselev, Alexej; Stratmann, Frank; George, Ingrid; Baltensperger, Urs
Hygroscopic properties of secondary organic aerosol (SOA) formed by photooxidation of different concentrations (10–27 or 220–270 ppb) of α-pinene precursor were investigated at different relative humidities (RH) using a hygroscopicity tandem differential mobility analyzer (HTDMA, RH = 95–97%) and using the mobile version of the Leipzig Aerosol Cloud Interaction Simulator (LACIS-mobile, RH = 98–99.3%). In addition, the cloud condensation nuclei (CCN) activity was measured applying two CCN counters (CCNC). An apparent single-hygroscopicity parameter, κ, of ∼0.09, ∼0.07–0.13, and ∼0.02–0.04 was derived from CCNC, HTDMA and LACIS data, respectively, assuming the surface tension of pure water. Closure between HTDMA and CCNC data was achieved within experimental uncertainty, whereas closure between LACIS and CCNC was only achieved by assuming a concentration-dependent surface tension reduction, consequently resulting in lower CCNC-derived κ values. Comparing different experimental techniques at varying precursor concentrations in more detail reveals further open questions. Varying precursor concentration influences hygroscopic growth factors at subsaturated RH, while it has no effect on the CCN activation. This difference in behaviour might be caused by precursor concentration-dependent surface tension depression or changing droplet solution concentration dependence of the water activity coefficient with varying SOA composition. Furthermore, evidence was found that the SOA might need several seconds to reach the equilibrium growth factor at high RH.
01A - Beitrag in wissenschaftlicher Zeitschrift
Ion-induced nucleation of pure biogenic particles
(Springer, 26.05.2016) Kirby, Jasper; Duplissy, Jonathan; Sengupta, Kamalika; Frege, Carla; Gordon, Hamish; Williamson, Christina; Heinritzi, Martin; Simon, Mario; Yan, Chao; Almeida, João; Tröstl, Jasmin; Nieminen, Tuomo; Ortega, Ismael K.; Wagner, Robert; Adamov, Alexey; Amorim, Antonio; Bernhammer, Anne-Kathrin; Bianchi, Federico; Breitenlechner, Martin; Brilke, Sophia; Chen, Xuemeng; Craven, Jill; Dias, Antonio; Ehrhart, Sebastian; Flagan, Richard C.; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Hakala, Jani; Hoyle, Christopher R.; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kim, Jaeseok; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Molteni, Ugo; Onnela, Antti; Peräkylä, Otso; Piel, Felix; Petäjä, Tuukka; Praplan, Arnaud P.; Pringle, Kirsty; Rap, Alexandru; Richards, Nigel A.D.; Riipinen, Ilona; Rissanen, Matti P.; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Scott, Catherine E.; Seinfeld, John H.; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Virtanen, Annele; Vogel, Alexander L.; Wagner, Andrea C.; Wagner, Paul E.; Weingartner, Ernest; Wimmer, Daniela; Winkler, Paul M.; Ye, Penglin; Zhang, Xuan; Hansel, Armin; Dommen, Josef; Donahue, Neil M.; Worsnop, Douglas R.; Baltensperger, Urs; Kulmala, Markku; Carslaw, Kenneth S.; Curtius, Joachim
Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere, and that ions have a relatively minor role. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.
01A - Beitrag in wissenschaftlicher Zeitschrift
Molecular understanding of sulphuric acid–amine particle nucleation in the atmosphere
(Springer, 2013) Almeida, João; Schobesberger, Siegfried; Kürten, Andreas; Ortega, Ismael K.; Kupiainen-Määttä, Oona; Praplan, Arnaud P.; Adamov, Alexey; Amorim, Antonio; Bianchi, Federico; Breitenlechner, Martin; David, André; Dommen, Josef; Donahue, Neil M.; Downard, Andrew; Dunne, Eimear; Duplissy, Jonathan; Ehrhart, Sebastian; Flagan, Richard C.; Franchin, Alessandro; Guida, Roberto; Hakala, Jani; Hansel, Armin; Heinritzi, Martin; Henschel, Henning; Jokinen, Tuija; Junninen, Heikki; Kajos, Maija; Kangasluoma, Juha; Keskinen, Helmi; Kupc, Agnieszka; Kurtén, Theo; Kvashin, Alexander N.; Laaksonen, Ari; Lehtipalo, Katrianne; Leiminger, Markus; Leppä, Johannes; Loukonen, Ville; Makhmutov, Vladimir; Mathot, Serge; McGrath, Matthew J.; Nieminen, Tuomo; Olenius, Tinja; Onnela, Antti; Petäjä, Tuukka; Riccobono, Francesco; Riipinen, Ilona; Rissanen, Matti; Rondo, Linda; Ruuskanen, Taina; Santos, Filipe D.; Sarnela, Nina; Schallhart, Simon; Schnitzhofer, Ralf; Seinfeld, John H.; Simon, Mario; Sipilä, Mikko; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Tröstl, Jasmin; Tsagkogeorgas, Georgios; Vaattovaara, Petri; Viisanen, Yrjo; Virtanen, Annele; Vrtala, Aron; Wagner, Paul E.; Weingartner, Ernest; Wex, Heike; Williamson, Christina; Wimmer, Daniela; Ye, Penglin; Yli-Juuti, Taina; Carslaw, Kenneth S.; Kulmala, Markku; Curtius, Joachim; Baltensperger, Urs; Worsnop, Douglas R.; Vehkamäki, Hanna; Kirkby, Jasper
01A - Beitrag in wissenschaftlicher Zeitschrift
Oxidation products of biogenic emissions contribute to nucleation of atmospheric particles
(American Association for the Advancement of Science, 2014) Riccobono, Francesco; Schobesberger, Siegfried; Scott, Catherine E.; Dommen, Josef; Ortega, Ismael K.; Rondo, Linda; Almeida, João; Amorim, Antonio; Bianchi, Federico; Breitenlechner, Martin; David, André; Downard, Andrew; Dunne, Eimear M.; Duplissy, Jonathan; Ehrhart, Sebastian; Flagan, Richard C.; Franchin, Alessandro; Hansel, Armin; Junninen, Heikki; Kajos, Maija; Keskinen, Helmi; Kupc, Agnieszka; Kürten, Andreas; Kvashin, Alexander N.; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Nieminen, Tuomo; Onnela, Antti; Petäjä, Tuukka; Praplan, Arnaud P.; Santos, Filipe D.; Schallhart, Simon; Seinfeld, John H.; Sipilä, Mikko; Spracklen, Dominick V.; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Tsagkogeorgas, Georgios; Vaattovaara, Petri; Viisanen, Yrjö; Vrtala, Aron; Wagner, Paul E.; Weingartner, Ernest; Wex, Heike; Wimmer, Daniela; Carslaw, Kenneth S.; Curtius, Joachim; Donahue, Neil M.; Kirkby, Jasper; Kulmala, Markku; Worsnop, Douglas R.; Baltensperger, Urs
Out of the Air New-particle formation from gaseous precursors in the atmosphere is a complex and poorly understood process with importance in atmospheric chemistry and climate. Laboratory studies have had trouble reproducing the particle formation rates that must occur in the natural world. Riccobono et al. used the CLOUD (Cosmics Leaving Outdoor Droplets) chamber at CERN to recreate a realistic atmospheric environment. Sulfuric acid and oxidized organic vapors in typical natural concentrations caused particle nucleation at similar rates to those observed in the lower atmosphere.
01A - Beitrag in wissenschaftlicher Zeitschrift
Reduced anthropogenic aerosol radiative forcing caused by biogenic new particle formation
(National Academy of Sciences, 2016) Gordon, Hamish; Sengupta, Kamalika; Rap, Alexandru; Duplissy, Jonathan; Frege, Carla; Williamson, Christina; Heinritzi, Martin; Simon, Mario; Yan, Chao; Almeida, João; Tröstl, Jasmin; Nieminen, Tuomo; Ortega, Ismael K.; Wagner, Robert; Dunne, Eimear M.; Adamov, Alexey; Amorim, Antonio; Bernhammer, Anne-Kathrin; Bianchi, Federico; Breitenlechner, Martin; Brilke, Sophia; Chen, Xuemeng; Craven, Jill S.; Dias, Antonio; Ehrhart, Sebastian; Fischer, Lukas; Flagan, Richard C.; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Hakala, Jani; Hoyle, Christopher R.; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kim, Jaeseok; Kirkby, Jasper; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Molteni, Ugo; Monks, Sarah A.; Onnela, Antti; Peräkylä, Otso; Piel, Felix; Petäjä, Tuukka; Praplan, Arnaud P.; Pringle, Kirsty J.; Richards, Nigel A. D.; Rissanen, Matti P.; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Scott, Catherine E.; Seinfeld, John H.; Sharma, Sangeeta; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Virtanen, Annele; Vogel, Alexander Lucas; Wagner, Andrea C.; Wagner, Paul E.; Weingartner, Ernest; Wimmer, Daniela; Winkler, Paul M.; Ye, Penglin; Zhang, Xuan; Hansel, Armin; Dommen, Josef; Donahue, Neil M.; Worsnop, Douglas R.; Baltensperger, Urs; Kulmala, Markku; Curtius, Joachim; Carslaw, Kenneth S.
A mechanism for the formation of atmospheric aerosols via the gas to particle conversion of highly oxidized organic molecules is found to be the dominant aerosol formation process in the preindustrial boundary layer over land. The inclusion of this process in a global aerosol model raises baseline preindustrial aerosol concentrations and could lead to a reduction of 27% in estimates of anthropogenic aerosol radiative forcing.
01A - Beitrag in wissenschaftlicher Zeitschrift
Results from the CERN pilot CLOUD experiment
(Copernicus, 15.02.2010) Duplissy, Jonathan; Enghoff, Martin Bødker; Aplin, Karen L.; Arnold, Frank; Aufmhoff, Heinfried; Avngaard, Michael; Baltensperger, Urs; Bondo, Torsten; Bingham, Robert; Carslaw, Ken S.; Curtius, Joachim; David, A.; Fastrup, Bent; Gagné, Stéphanie; Hahn, F.; Harrison, Richerd Giles; Kellett, Barry; Kirkby, Jasper; Kulmala, Markku; Laakso, Lauri; Laaksonen, Ari; Lillestøl, Egil; Lockwood, Mike; Mäkelä, Jyrki Mikael; Makhmutov, Vladimir; Marsh, N. D.; Nieminen, Tuomo; Onnela, Antti; Pedersen, E.; Pedersen, Jens Olaf Pepke; Polny, Josef; Reichl, Udo; Seinfeld, John H.; Sipilä, Mikko; Stozhkov, Yuri; Stratmann, Frank; Svensmark, Henrik; Svensmark, Jacob; Veenhof, Rob; Verheggen, B.; Viisanen, Yrjö; Wagner, Paul E.; Wehrle, Günther; Weingartner, Ernest; Wex, Heike; Wilhelmsson, Mats; Winkler, Paul M.
During a 4-week run in October–November 2006, a pilot experiment was performed at the CERN Proton Synchrotron in preparation for the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment, whose aim is to study the possible influence of cosmic rays on clouds. The purpose of the pilot experiment was firstly to carry out exploratory measurements of the effect of ionising particle radiation on aerosol formation from trace H2SO4 vapour and secondly to provide technical input for the CLOUD design. A total of 44 nucleation bursts were produced and recorded, with formation rates of particles above the 3 nm detection threshold of between 0.1 and 100 cm−3s−1, and growth rates between 2 and 37 nm h−1. The corresponding H2O concentrations were typically around 106 cm−3 or less. The experimentally measured formation rates and H2SO4 concentrations are comparable to those found in the atmosphere, supporting the idea that sulphuric acid is involved in the nucleation of atmospheric aerosols. However, sulphuric acid alone is not able to explain the observed rapid growth rates, which suggests the presence of additional trace vapours in the aerosol chamber, whose identity is unknown. By analysing the charged fraction, a few of the aerosol bursts appear to have a contribution from ion-induced nucleation and ion-ion recombination to form neutral clusters. Some indications were also found for the accelerator beam timing and intensity to influence the aerosol particle formation rate at the highest experimental SO2 concentrations of 6 ppb, although none was found at lower concentrations. Overall, the exploratory measurements provide suggestive evidence for ion-induced nucleation or ion-ion recombination as sources of aerosol particles. However, in order to quantify the conditions under which ion processes become significant, improvements are needed in controlling the experimental variables and in the reproducibility of the experiments. Finally, concerning technical aspects, the most important lessons for the CLOUD design include the stringent requirement of internal cleanliness of the aerosol chamber, as well as maintenance of extremely stable temperatures (variations below 0.1 °C).
01A - Beitrag in wissenschaftlicher Zeitschrift
Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation
(Springer, 24.08.2011) Kirkby, Jasper; Curtius, Joachim; Almeida, João; Dunne, Eimear; Duplissy, Jonathan; Ehrhart, Sebastian; Franchin, Alessandro; Gagné, Stéphanie; Ickes, Luisa; Kürten, Andreas; Kupc, Agnieszka; Metzger, Axel; Riccobono, Francesco; Rondo, Linda; Schobesberger, Siegfried; Tsagkogeorgas, Georgios; Wimmer, Daniela; Amorim, Antonio; Bianchi, Federico; Breitenlechner, Martin; David, André; Dommen, Josef; Downard, Andrew; Ehn, Mikael; Flagan, Richard C.; Haider, Stefan; Hansel, Armin; Hauser, Daniel; Jud, Werner; Junninen, Heikki; Kreissl, Fabian; Kvashin, Alexander; Laaksonen, Ari; Lehtipalo, Katrianne; Lima, Jorge; Lovejoy, Edward R.; Makhmutov, Vladimir; Mathot, Serge; Mikkilä, Jyri; Minginette, Pierre; Mogo, Sandra; Nieminen, Tuomo; Onnela, Antti; Pereira, Paulo; Petäjä, Tuukka; Schnitzhofer, Ralf; Seinfeld, John H.; Sipilä, Mikko; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Vanhanen, Joonas; Viisanen, Yrjo; Vrtala, Aron; Wagner, Paul E.; Walther, Hansueli; Weingartner, Ernest; Wex, Heike; Winkler, Paul M.; Carslaw, Kenneth S.; Worsnop, Douglas R.; Baltensperger, Urs; Kulmala, Markku
Atmospheric aerosols exert an important influence on climate through their effects on stratiform cloud albedo and lifetime and the invigoration of convective storms. Model calculations suggest that almost half of the global cloud condensation nuclei in the atmospheric boundary layer may originate from the nucleation of aerosols from trace condensable vapours, although the sensitivity of the number of cloud condensation nuclei to changes of nucleation rate may be small. Despite extensive research, fundamental questions remain about the nucleation rate of sulphuric acid particles and the mechanisms responsible, including the roles of galactic cosmic rays and other chemical species such as ammonia. Here we present the first results from the CLOUD experiment at CERN. We find that atmospherically relevant ammonia mixing ratios of 100 parts per trillion by volume, or less, increase the nucleation rate of sulphuric acid particles more than 100–1,000-fold. Time-resolved molecular measurements reveal that nucleation proceeds by a base-stabilization mechanism involving the stepwise accretion of ammonia molecules. Ions increase the nucleation rate by an additional factor of between two and more than ten at ground-level galactic-cosmic-ray intensities, provided that the nucleation rate lies below the limiting ion-pair production rate. We find that ion-induced binary nucleation of H2SO4–H2O can occur in the mid-troposphere but is negligible in the boundary layer. However, even with the large enhancements in rate due to ammonia and ions, atmospheric concentrations of ammonia and sulphuric acid are insufficient to account for observed boundary-layer nucleation.
01A - Beitrag in wissenschaftlicher Zeitschrift