Auflistung nach Autor:in "Good, Nicholas"

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A synthesis of cloud condensation nuclei counter (CCNC) measurements within the EUCAARI network
(Copernicus, 2015) Paramonov, Mikhail; Kerminen, Veli-Matti; Gysel, Martin; Aalto, Pasi Pekka; Andreae, Meinrat O.; Asmi, Eija; Baltensperger, Urs; Bougiatioti, Aikaterini; Brus, David; Frank, Göran; Good, Nicholas; Gunthe, Sachin S.; Hao, Liqing; Irwin, Martin; Jaatinen, Antti; Jurányi, Zsófia; King, S. M.; Kortelainen, Aki; Kristensson, Adam; Lihavainen, Heikki; Kulmala, Markku; Lohmann, Ulrike; Martin, Scot T.; McFiggans, Gordon; Mihalopoulos, Nikolaos; Nenes, Athanasios; O'Dowd, Colin D.; Ovadnevaite, Jurgita; Petäjä, Tuukka; Pöschl, Ulrich; Roberts, Greg; Rose, Diana; Svenningsson, Birgitta; Swietlicki, Erik; Weingartner, Ernest; Whitehead, James; Wiedensohler, Alfred; Wittbom, Cerina; Sierau, Berko
Cloud condensation nuclei counter (CCNC) measurements performed at 14 locations around the world within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) framework have been analysed and discussed with respect to the cloud condensation nuclei (CCN) activation and hygroscopic properties of the atmospheric aerosol. The annual mean ratio of activated cloud condensation nuclei (NCCN) to the total number concentration of particles (NCN), known as the activated fraction A, shows a similar functional dependence on supersaturation S at many locations – exceptions to this being certain marine locations, a free troposphere site and background sites in south-west Germany and northern Finland. The use of total number concentration of particles above 50 and 100 nm diameter when calculating the activated fractions (A50 and A100, respectively) renders a much more stable dependence of A on S; A50 and A100 also reveal the effect of the size distribution on CCN activation. With respect to chemical composition, it was found that the hygroscopicity of aerosol particles as a function of size differs among locations. The hygroscopicity parameter κ decreased with an increasing size at a continental site in south-west Germany and fluctuated without any particular size dependence across the observed size range in the remote tropical North Atlantic and rural central Hungary. At all other locations κ increased with size. In fact, in Hyytiälä, Vavihill, Jungfraujoch and Pallas the difference in hygroscopicity between Aitken and accumulation mode aerosol was statistically significant at the 5 % significance level. In a boreal environment the assumption of a size-independent κ can lead to a potentially substantial overestimation of NCCN at S levels above 0.6 %. The same is true for other locations where κ was found to increase with size. While detailed information about aerosol hygroscopicity can significantly improve the prediction of NCCN, total aerosol number concentration and aerosol size distribution remain more important parameters. The seasonal and diurnal patterns of CCN activation and hygroscopic properties vary among three long-term locations, highlighting the spatial and temporal variability of potential aerosol–cloud interactions in various environments.
01A - Beitrag in wissenschaftlicher Zeitschrift
Analysis of the hygroscopic and volatile properties of ammonium sulphate seeded and unseeded SOA particles
(Copernicus, 28.01.2009) Meyer, Nic K.; Duplissy, Jonathan; Gysel, Martin; Metzger, Axel; Dommen, Josef; Weingartner, Ernest; Alfarra, Rami; Prévôt, André S.H.; Fletcher, C; Good, Nicholas; McFiggans, Gordan; Jonsson, Åsa M.; Hallquist, Mattias; Baltensperger, Urs; Ristovski, Zoran D.
The volatile and hygroscopic properties of ammonium sulphate seeded and unseeded secondary organic aerosol (SOA) derived from the photo-oxidation of atmospherically relevant concentrations of α-pinene were studied. The seed particles were electrospray generated ammonium sulphate ((NH4)2SO4) having diameters of approximately 33 nm with a quasi-mono-disperse size distribution (geometric standard deviation σg=1.3). The volatile and hygroscopic properties of both seeded and unseeded SOA were simultaneously measured with a VH-TDMA (volatility – hygroscopicity tandem differential mobility analyzer). VH-TDMA measurements of unseeded SOA show a decrease in the hygroscopic growth (HGF) factor for increased volatilisation temperatures such that the more volatile compounds appear to be more hygroscopic. This is opposite to the expected preferential evaporation of more volatile but less hygroscopic material, but could also be due to enhanced oligomerisation occurring at the higher temperature in the thermodenuder. In addition, HGF measurements of seeded SOA were measured as a function of time at two relative humidities, below (RH 75%) and above (RH 85%) the deliquescence relative humidity (DRH) of the pure ammonium sulphate seeds. As these measurements were conducted during the onset phase of photo-oxidation, during particle growth, they enabled us to find the dependence of the HGF as a function of the volume fraction of the SOA coating. HGF's measured at RH of 85% showed a continuous decrease as the SOA coating thickness increased. The measured growth factors show good agreements with ZSR predictions indicating that, at these RH values, there are only minor solute-solute interactions. At 75% RH, as the SOA fraction increased, a rapid increase in the HGF was observed indicating that an increasing fraction of the (NH4)2SO4 is subject to a phase transition, going into solution, with an increasing volume fraction of SOA. To our knowledge this is the first time that SOA derived from photo-oxidised α-pinene has been shown to affect the equilibrium water content of inorganic aerosols below their DRH. For SOA volume fractions above ~0.3 the measured growth factor followed roughly parallel to the ZSR prediction based on fully dissolved (NH4)2SO4 although with a small difference that was just larger than the error estimate. Both incomplete dissolution and negative solute-solute interactions could be responsible for the lower HGF observed compared to the ZSR predictions.
01A - Beitrag in wissenschaftlicher Zeitschrift
Cloud forming potential of secondary organic aerosol under near atmospheric conditions
(Wiley, 2008) Duplissy, Jonathan; Gysel, Martin; Alfarra, M. Rami; Dommen, Josef; Metzger, Axel; Prévôt, André S.H.; Weingartner, Ernest; Laaksonen, Ari; Raatikainen, Tomi; Good, Nicholas; Turner, S. Fiona; McFiggans, Gordon; Baltensperger, Urs
Cloud droplets form by nucleation on atmospheric aerosol particles. Populations of such particles invariably contain organic material, a major source of which is thought to be condensation of photo‐oxidation products of biogenic volatile organic compounds (VOCs). We demonstrate that smog chamber studies of the formation of such biogenic secondary organic aerosol (SOA) formed during photo‐oxidation must be conducted at near atmospheric concentrations to yield atmospherically representative particle composition, hygroscopicity and cloud‐forming potential. Under these conditions, the hygroscopicity measured at 95% relative humidity can be used reliably to predict the CCN activity of the SOA particles by assuming droplet surface tension of pure water. We also show that the supersaturation required to activate a given size of particle decreases with age.
01A - Beitrag in wissenschaftlicher Zeitschrift
Intercomparison study of six HTDMAs. results and recommendations
(Copernicus, 24.07.2009) Duplissy, Jonathan; Gysel, Martin; Sjogren, S.; Meyer, Nickolas; Good, Nicholas; Kammermann, Lukas; Michaud, Vincent; Weigel, Ralf; Martins dos Santos, Sebastiao; Gruening, Carsten; Villani, P.; Laj, Paolo; Sellegri, Karine; Metzger, Axel; McFiggans, Gordon B.; Wehrle, Günther; Richter, René; Dommen, Josef; Ristovski, Zoran; Baltensperger, Urs; Weingartner, Ernest
We report on an intercomparison of six different hygroscopicity tandem differential mobility analysers HTDMAs). These HTDMAs are used worldwide in laboratory experiments and field campaigns to measure the water uptake of aerosol particles and have never been intercompared. After an investigation of the different design of the instruments with their advantages and inconveniencies, the methods for calibration, validation and data analysis are presented. Measurements of nebulised ammonium sulphate as well as of secondary organic aerosol generated from a smog chamber were performed. Agreement and discrepancies between the instruments and to the theory are discussed, and final recommendations for a standard instrument are given, as a benchmark for laboratory or field experiments to ensure a high quality of HTDMA data.
01A - Beitrag in wissenschaftlicher Zeitschrift
Widening the gap between measurement and modelling of secondary organic aerosol properties?
(Copernicus, 2010) Good, Nicholas; Topping, D. O.; Duplissy, Jonathan; Gysel, Martin; Meyer, Nic K.; Metzger, Axel; Turner, S. F.; Baltensperger, Urs; Ristovski, Zoran; Weingartner, Ernest; Coe, Hugh; McFiggans, Gordan
The link between measured sub-saturated hygroscopicity and cloud activation potential of secondary organic aerosol particles produced by the chamber photo-oxidation of α-pinene in the presence or absence of ammonium sulphate seed aerosol was investigated using two models of varying complexity. A simple single hygroscopicity parameter model and a more complex model (incorporating surface effects) were used to assess the detail required to predict the cloud condensation nucleus (CCN) activity from the sub-saturated water uptake. Sub-saturated water uptake measured by three hygroscopicity tandem differential mobility analyser (HTDMA) instruments was used to determine the water activity for use in the models. The predicted CCN activity was compared to the measured CCN activation potential using a continuous flow CCN counter. Reconciliation using the more complex model formulation with measured cloud activation could be achieved widely different assumed surface tension behavior of the growing droplet; this was entirely determined by the instrument used as the source of water activity data. This unreliable derivation of the water activity as a function of solute concentration from sub-saturated hygroscopicity data indicates a limitation in the use of such data in predicting cloud condensation nucleus behavior of particles with a significant organic fraction. Similarly, the ability of the simpler single parameter model to predict cloud activation behaviour was dependent on the instrument used to measure sub-saturated hygroscopicity and the relative humidity used to provide the model input. However, agreement was observed for inorganic salt solution particles, which were measured by all instruments in agreement with theory. The difference in HTDMA data from validated and extensively used instruments means that it cannot be stated with certainty the detail required to predict the CCN activity from sub-saturated hygroscopicity. In order to narrow the gap between measurements of hygroscopic growth and CCN activity the processes involved must be understood and the instrumentation extensively quality assured. It is impossible to say from the results presented here due to the differences in HTDMA data whether: i) Surface tension suppression occurs ii) Bulk to surface partitioning is important iii) The water activity coefficient changes significantly as a function of the solute concentration.
01A - Beitrag in wissenschaftlicher Zeitschrift