Auflistung nach Autor:in "Kirkby, Jasper"
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- PublikationAerosol nucleation and growth in a mixture of sulfuric acid/alpha-pinene oxidation products at the CERN CLOUD chamber(AIP Publishing, 2013) Tröstl, Jasmin; Bianchi, Federico; Kürten, Andreas; Rondo, Linda; Simon, Mario; Sarnela, Nina; Jokinen, Tuija; Heinritzi, Martin; Dommen, Josef; Kirkby, Jasper; Weingartner, Ernest; Baltensperger, Urs; DeMott, Paul J.; O'Dowd, Colin D. [in: Nucleation and Atmospheric Aerosols. 19th International Conference]The role of α-pinene in aerosol nucleation and growth was investigated using the CERN CLOUD chamber, a nano scanning mobility particle sizer (nanoSMPS) and several condensation particle counters (CPCs) with different diameter cut-offs. Different oxidation conditions for α-pinene - OH⋅ vs. ozone oxidation - were considered to investigate their contributions to particle nucleation and growth. Results from the latest CERN experiment from fall 2012 (CLOUD 7) are presented.04B - Beitrag Konferenzschrift
- PublikationEvolution 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. [in: Nucleation and atmospheric aerosols]04B - Beitrag Konferenzschrift
- PublikationEvolution 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 [in: Atmospheric Chemistry and Physics]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
- PublikationMolecular 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 [in: Nature]01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationOxidation 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 [in: Science]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
- PublikationReduced 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. [in: Proceedings of the National Academy of Sciences]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
- PublikationResults 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. [in: Atmospheric Chemistry and Physics]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
- PublikationRole of organics in particle nucleation. From the lab to global model(AIP Publishing, 2013) Dommen, Josef; Riccobono, Francesco; Schobesberger, Siegfried; Bianchi, Federico; Scott, Catherine; Ortega, Ismael K.; Rondo, Linda; Breitenlechner, Martin; Junninen, Heikki; Donahue, Neil M.; Kürten, Andreas; Praplan, Arnaud; Weingartner, Ernest; Hansel, Armin; Curtius, Joachim; Kirkby, Jasper; Kulmala, Markku; Carslaw, Kenneth S.; Worsnop, Douglas R.; Baltensperger, Urs; DeMott, Paul J.; O'Dowd Colin D. [in: Nucleation and atmospheric aerosols]04B - Beitrag Konferenzschrift
- PublikationRole 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 [in: Nature]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
- PublikationThe role of low-volatility organic compounds in initial particle growth in the atmosphere(Springer, 2016) 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 S.; Duplissy, Jonathan; Adamov, Alexey; Almeida, Joao; Bernhammer, Anne-Kathrin; Breitenlechner, Martin; Brilke, Sophia; Dias, Antònio; Ehrhart, Sebastian; Flagan, Richard C.; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Gysel, Martin; Hansel, Armin; Hoyle, Christopher R.; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Keskinen, Helmi; Kim, Jaeseok; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lawler, Michael; Leiminger, Markus; Mathot, Serge; Möhler, Ottmar; Nieminen, Tuomo; Onnela, Antti; Petäjä, Tuukka; Piel, Felix M.; Miettinen, Pasi; Rissanen, Matti P.; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Sengupta, Kamalika; Sipilä, Mikko; Smith, James N.; Steiner, Gerhard; Tomè, Antònio; Virtanen, Annele; Wagner, Andrea C.; 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 M.; Baltensperger, Urs [in: Nature]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.01A - Beitrag in wissenschaftlicher Zeitschrift