Browsing by Author "Winkler, Paul M."
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- ItemCauses and importance of new particle formation in the present-day and preindustrial atmospheres(Hoboken, NJ : Wiley, 2017) Gordon, Hamish; Kirkby, Jasper; Baltensperger, Urs; Bianchi, Federico; Breitenlechner, Martin; Curtius, Joachim; Dias, Antonio; Dommen, Josef; Donahue, Neil M.; Dunne, Eimear M.; Duplissy, Jonathan; Ehrhart, Sebastian; Flagan, Richard C.; Frege, Carla; Fuchs, Claudia; Hansel, Armin; Hoyle, Christopher R.; Kulmala, Markku; Kürten, Andreas; Lehtipalo, Katrianne; Makhmutov, Vladimir; Molteni, Ugo; Rissanen, Matti P.; Stozkhov, Yuri; Tröstl, Jasmin; Tsagkogeorgas, Georgios; Wagner, Robert; Williamson, Christina; Wimmer, Daniela; Winkler, Paul M.; Yan, Chao; Carslaw, Ken S.New particle formation has been estimated to produce around half of cloud-forming particles in the present-day atmosphere, via gas-to-particle conversion. Here we assess the importance of new particle formation (NPF) for both the present-day and the preindustrial atmospheres. We use a global aerosol model with parametrizations of NPF from previously published CLOUD chamber experiments involving sulfuric acid, ammonia, organic molecules, and ions. We find that NPF produces around 67% of cloud condensation nuclei at 0.2% supersaturation (CCN0.2%) at the level of low clouds in the preindustrial atmosphere (estimated uncertainty range 45–84%) and 54% in the present day (estimated uncertainty range 38–66%). Concerning causes, we find that the importance of biogenic volatile organic compounds (BVOCs) in NPF and CCN formation is greater than previously thought. Removing BVOCs and hence all secondary organic aerosol from our model reduces low-cloud-level CCN concentrations at 0.2% supersaturation by 26% in the present-day atmosphere and 41% in the preindustrial. Around three quarters of this reduction is due to the tiny fraction of the oxidation products of BVOCs that have sufficiently low volatility to be involved in NPF and early growth. Furthermore, we estimate that 40% of preindustrial CCN0.2% are formed via ion-induced NPF, compared with 27% in the present day, although we caution that the ion-induced fraction of NPF involving BVOCs is poorly measured at present. Our model suggests that the effect of changes in cosmic ray intensity on CCN is small and unlikely to be comparable to the effect of large variations in natural primary aerosol emissions.
- ItemThe effect of acid-base clustering and ions on the growth of atmospheric nano-particles(London : Nature Publishing Group, 2016) Lehtipalo, Katrianne; Rondo, Linda; Kontkanen, Jenni; Schobesberger, Siegfried; Jokinen, Tuija; Sarnela, Nina; Kürten, Andreas; Ehrhart, Sebastian; Franchin, Alessandro; Nieminen, Tuomo; Kulmala, Markku; Riccobono, Francesco; Sipila, Mikko; Yli-Juuti, Taina; Duplissy, Jonathan; Adamov, Alexey; Ahlm, Lars; Almeida, Joa˜o; Amorim, Antonio; Bianchi, Federico; Breitenlechner, Martin; Dommen, Josef; Downard, Andrew J.; Dunne, Eimear M.; Flagan, Richard C.; Guida, Roberto; Hakala, Jani; Hansel, Armin; Jud, Werner; Kangasluoma, Juha; Kerminen, Veli-Matti; Keskinen, Helmi; Kim, Jaeseok; Kirkby, Jasper; Kupc, Agnieszka; Kupiainen-Määttä, Oona; Laaksonen, Ari; Lawler, Michael J.; Leiminger, Markus; Mathot, Serge; Olenius, Tinja; Ortega, Ismael K.; Onnela, Antti; Petäjä, Tuukka; Praplan, Arnaud; Rissanen, Matti P.; Ruuskanen, Taina; Santos, Filipe D.; Schallhart, Simon; Schnitzhofer, Ralf; Simon, Mario; Smith, James N.; Tröstl, Jasmin; Tsagkogeorgas, Georgios; Tomé, António; Vaattovaara, Petri; Vehkamäki, Hanna; Vrtala, Aron E.; Wagner, Paul E.; Williamson, Christina; Wimmer, Daniela; Winkler, Paul M.; Virtanen, Annele; Donahue, Neil M.; Carslaw, Kenneth S.; Baltensperger, Urs; Riipinen, Ilona; Curtius, Joachim; Worsnop, Douglas R.; Kulmala, MarkkuThe growth of freshly formed aerosol particles can be the bottleneck in their survival to cloud condensation nuclei. It is therefore crucial to understand how particles grow in the atmosphere. Insufficient experimental data has impeded a profound understanding of nano-particle growth under atmospheric conditions. Here we study nano-particle growth in the CLOUD (Cosmics Leaving OUtdoors Droplets) chamber, starting from the formation of molecular clusters. We present measured growth rates at sub-3 nm sizes with different atmospherically relevant concentrations of sulphuric acid, water, ammonia and dimethylamine. We find that atmospheric ions and small acid-base clusters, which are not generally accounted for in the measurement of sulphuric acid vapour, can participate in the growth process, leading to enhanced growth rates. The availability of compounds capable of stabilizing sulphuric acid clusters governs the magnitude of these effects and thus the exact growth mechanism. We bring these observations into a coherent framework and discuss their significance in the atmosphere.
- ItemIon-induced nucleation of pure biogenic particles(London : Nature Publishing Group, 2016) Kirkby, Jasper; Duplissy, Jonathan; Sengupta, Kamalika; 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, JoachimAtmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood1. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours2. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere3,4, and that ions have a relatively minor role5. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded6,7. 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.
- ItemNew particle formation and sub-10nm size distribution measurements during the A-LIFE field experiment in Paphos, Cyprus(Katlenburg-Lindau : EGU, 2020) Brilke, Sophia; Fölker, Nikolaus; Kandler, Konrad; Müller, Thomas; Gong, Xianda; Peischl, Jeff; Weinzierl, Bernadett; Winkler, Paul M.Atmospheric particle size distributions were measured in Paphos, Cyprus, during the A-LIFE (absorbing aerosol layers in a changing climate: ageing, lifetime and dynamics) field experiment from 3 to 30 April 2017. The newly developed differential mobility analyser train (DMAtrain) was deployed for the first time in an atmospheric environment for the direct measurement of the nucleation mode size range between 1.8 and 10 nm diameter. The DMA-train set-up consists of seven size channels, of which five are set to fixed particle mobility diameters and two additional diameters are obtained by alternating voltage settings in one DMA every 10 s. In combination with a conventional mobility particle size spectrometer (MPSS) and an aerodynamic particle sizer (APS) the complete atmospheric aerosol size distribution from 1.8 nm to 10 μ m was covered. The focus of the A-LIFE study was to characterize new particle formation (NPF) in the eastern Mediterranean region at a measurement site with strong local pollution sources. The nearby Paphos airport was found to be a large emission source for nucleation mode particles, and we analysed the size distribution of the airport emission plumes at approximately 500 m from the main runway. The analysis yielded nine NPF events in 27 measurement days from the combined analysis of the DMAtrain, MPSS and trace gas monitors. Growth rate calculations were performed, and a size dependency of the initial growth rate (< 10 nm) was observed for one event case. Fast changes of the sub-10 nm size distribution on a timescale of a few minutes were captured by the DMA-train measurement during early particle growth and are discussed in a second event case. In two cases, particle formation and growth were detected in the nucleation mode size range which did not exceed the 10 nm threshold. This finding implies that NPF likely occurs more frequently than estimated from studies where the lower nanometre size regime is not covered by the size distribution measurements. © 2020 Author(s).
- ItemObservation of viscosity transition in α-pinene secondary organic aerosol(München : European Geopyhsical Union, 2016) Järvinen, Emma; Ignatius, Karoliina; Nichman, Leonid; Kristensen, Thomas B.; Fuchs, Claudia; Hoyle, Christopher R.; Höppel, Niko; Corbin, Joel C.; Craven, Jill; Duplissy, Jonathan; Ehrhart, Sebastian; El Haddad, Imad; Frege, Carla; Gordon, Hamish; Jokinen, Tuija; Kallinger, Peter; Kirkby, Jasper; Kiselev, Alexei; Naumann, Karl-Heinz; Petäjä, Tuukka; Pinterich, Tamara; Prevot, Andre S.H.; Saathoff, Harald; Schiebel, Thea; Sengupta, Kamalika; Simon, Mario; Slowik, Jay G.; Tröstl, Jasmin; Virtanen, Annele; Vochezer, Paul; Vogt, Steffen; Wagner, Andrea C.; Wagner, Robert; Williamson, Christina; Winkler, Paul M.; Yan, Chao; Baltensperger, Urs; Donahue, Neil M.; Flagan, Rick C.; Gallagher, Martin; Hansel, Armin; Kulmala, Markku; Stratmann, Frank; Worsnop, Douglas R.; Möhler, Ottmar; Leisner, Thomas; Schnaiter, MartinUnder certain conditions, secondary organic aerosol (SOA) particles can exist in the atmosphere in an amorphous solid or semi-solid state. To determine their relevance to processes such as ice nucleation or chemistry occurring within particles requires knowledge of the temperature and relative humidity (RH) range for SOA to exist in these states. In the Cosmics Leaving Outdoor Droplets (CLOUD) experiment at The European Organisation for Nuclear Research (CERN), we deployed a new in situ optical method to detect the viscous state of α-pinene SOA particles and measured their transition from the amorphous highly viscous state to states of lower viscosity. The method is based on the depolarising properties of laboratory-produced non-spherical SOA particles and their transformation to non-depolarising spherical particles at relative humidities near the deliquescence point. We found that particles formed and grown in the chamber developed an asymmetric shape through coagulation. A transition to a spherical shape was observed as the RH was increased to between 35 % at −10 °C and 80 % at −38 °C, confirming previous calculations of the viscosity-transition conditions. Consequently, α-pinene SOA particles exist in a viscous state over a wide range of ambient conditions, including the cirrus region of the free troposphere. This has implications for the physical, chemical, and ice-nucleation properties of SOA and SOA-coated particles in the atmosphere.