lnstitut für Sensorik und Elektronik
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Publikation Fine and ultrafine particles in the Zürich (Switzerland) area measured with a mobile laboratory: an assessment of the seasonal and regional variation throughout a year(Copernicus, 24.09.2003) Bukowiecki, Nicolas; Dommen, Josef; Prévôt, André S.H.; Weingartner, Ernest; Baltensperger, UrsOn occasion of the project YOGAM (year of gas phase and aerosol measurements), the spatial and temporal variation of selected aerosol and gas phase parameters was assessed for the Zürich (Switzerland) area with a new mobile pollutant measurement laboratory. This assessment based on on-road measurements along a specified route on selected days during different seasons in 2001/2002, covering urban, suburban and rural regions. Special focus was put on the investigation and characterization of particles in the fine (particle diameter D<2.5 mm) and ultrafine (D<100 nm) size ranges. Analysis of Variance (ANOVA) showed that the variance of all considered fine and ultrafine aerosol parameters (i.e. particle background and total number concentration for particles larger than 3 nm, number concentrations in the size ranges 7-30 nm and 80-140 nm, as well as the active surface area concentration) was significantly larger for day-to-day than for spatial variation. However, Principal Component Analysis (PCA) found a similar regional pollution pattern within every single measuring day. Lowest particle background levels (D>3 nm) were found in rural areas at higher elevation (15 000 cmˉ³), while corresponding mean background values for urban and freeway-influenced areas were typically 35 000 cmˉ³ and >80 000 cmˉ³, respectively. Meteorology, i.e. prevailing weather conditions not only governed the day-to-day concentration variations in the selected area, but also influenced the formation of primary (directly traffic-related) and in few cases secondary (biogenic or anthropogenic) ultrafine particles. Overall, low temperatures regularly enhanced primary ultrafine particle formation in urban areas. There was a possible indication for relatively low number concentrations of secondary ultrafine particles during a few warm and sunny spring days. Mobile measurements as they were performed in this study have been shown to be suitable for pollutant assessments to obtain good information on spatial and day-to-day variability. For experimental studies concerning spatial resolution on a relatively short time scale (<1 day), a mobile measurement design may even be more appropriate than a network of stationary measuring sites.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Seasonal and diurnal characteristics of water soluble inorganic compounds in the gas and aerosol phase in the Zurich area(Copernicus, 2006) Fisseha, Rebeka; Dommen, Josef; Gutzwiller, Lukas; Weingartner, Ernest; Gysel, Martin; Emmenegger, C.; Kalberer, Markus; Baltensperger, UrsGas and aerosol samples were taken using a wet effluent diffusion denuder/aerosol collector (WEDD/AC) coupled to ion chromatography (IC) in the city of Zurich, Switzerland from August to September 2002 and in March 2003. Major water soluble inorganic ions; nitrate, sulfate, and nitrite were analyzed online with a time resolution of two hours for the gas and aerosol phase. The fraction of water soluble inorganic anions in PM10 varied from 15% in August to about 38% in March. Seasonal and diurnal variations of nitrate in the gas and aerosol phase were observed with more than 50% of the total nitrate in the gas phase during August and more than 80% of nitrate in the aerosol phase during March exceeding the concentration of sulfate by a factor of 2. Aerosol sulfate, on the other hand, did not show significant variability with season. However, in the gas phase, the SO2 concentration was 6.5 times higher in winter than in summer. Nitrous acid (HONO) also showed a diurnal variation in both the gas and aerosol phase with the lowest concentration (0.2–0.6 µg/m³) in the afternoon. The primary pollutants, NO, CO and SO2 mixing ratios were often at their highest between 04:00–10:00 local time due to the build up of fresh vehicle emission under a nocturnal inversion.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation 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, JoachimAtmospheric 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 ZeitschriftPublikation Impact of aftertreatment devices on primary emissions and secondary organic aerosol formation potential from in-use diesel vehicles: results from smog chamber experiments(Copernicus, 06.12.2010) Chirico, Roberto; DeCarlo, Peter F.; Heringa, Maarten F.; Tritscher, Torsten; Richter, René; Prévôt, André S. H.; Dommen, Josef; Weingartner, Ernest; Wehrle, Günther; Gysel, Martin; Laborde, Marie; Baltensperger, UrsDiesel particulate matter (DPM) is a significant source of aerosol in urban areas and has been linked to adverse health effects. Although newer European directives have introduced increasingly stringent standards for primary PM emissions, gaseous organics emitted from diesel cars can still lead to large amounts of secondary organic aerosol (SOA) in the atmosphere. Here we present results from smog chamber investigations characterizing the primary organic aerosol (POA) and the corresponding SOA formation at atmospherically relevant concentrations for three in-use diesel vehicles with different exhaust aftertreatment systems. One vehicle lacked exhaust aftertreatment devices, one vehicle was equipped with a diesel oxidation catalyst (DOC) and the third vehicle used both a DOC and diesel particulate filter (DPF). The experiments presented here were obtained from the vehicles at conditions representative of idle mode, and for one car in addition at a speed of 60 km/h. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was used to measure the organic aerosol (OA) concentration and to obtain information on the chemical composition. For the conditions explored in this paper, primary aerosols from vehicles without a particulate filter consisted mainly of black carbon (BC) with a low fraction of organic matter (OM, OM/BC < 0.5), while the subsequent aging by photooxidation resulted in a consistent production of SOA only for the vehicles without a DOC and with a deactivated DOC. After 5 h of aging ~80% of the total organic aerosol was on average secondary and the estimated "emission factor" for SOA was 0.23–0.56 g/kg fuel burned. In presence of both a DOC and a DPF, only 0.01 g SOA per kg fuel burned was produced within 5 h after lights on. The mass spectra indicate that POA was mostly a non-oxidized OA with an oxygen to carbon atomic ratio (O/C) ranging from 0.10 to 0.19. Five hours of oxidation led to a more oxidized OA with an O/C range of 0.21 to 0.37.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Investigations of primary and secondary particulate matter of different wood combustion appliances with a high-resolution time-of-flight aerosol mass spectrometer(Copernicus, 23.06.2011) Heringa, Maarten F.; DeCarlo, Peter F.; Chirico, Roberto; Tritscher, Torsten; Dommen, Josef; Weingartner, Ernest; Richter, René; Wehrle, Günther; Prévôt, André S.H.; Baltensperger, UrsA series of photo-oxidation smog chamber experiments were performed to investigate the primary emissions and secondary aerosol formation from two different log wood burners and a residential pellet burner under different burning conditions: starting and flaming phase. Emissions were sampled from the chimney and injected into the smog chamber leading to primary organic aerosol (POA) concentrations comparable to ambient levels. The composition of the aerosol was measured by an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and black carbon (BC) instrumentation. The primary emissions were then exposed to xenon light to initiate photo-chemistry and subsequent secondary organic aerosol (SOA) production. After correcting for wall losses, the average increase in organic matter (OM) concentrations by SOA formation for the starting and flaming phase experiments with the two log wood burners was found to be a factor of 4.1±1.4 after five hours of aging. No SOA formation was observed for the stable burning phase of the pellet burner. The startup emissions of the pellet burner showed an increase in OM concentration by a factor of 3.3. Including the measured SOA formation potential, average emission factors of BC+POA+SOA, calculated from CO2 emission, were found to be in the range of 0.04 to 3.9 g/kg wood for the stable burning pellet burner and an old log wood burner during startup respectively. SOA contributed significantly to the ion C2H4O2+ at mass to charge ratio m/z 60, a commonly used marker for primary emissions of wood burning. This contribution at m/z 60 can overcompensate for the degradation of levoglucosan leading to an overestimation of the contribution of wood burning or biomass burning to the total OM. The primary organic emissions from the three different burners showed a wide range in O:C atomic ratio (0.19−0.60) for the starting and flaming conditions, which also increased during aging. Primary wood burning emissions have a rather low relative contribution at m/z 43 (f 43) to the total organic mass spectrum. The non-oxidized fragment C3H7+ has a considerable contribution at m/z 43 for the fresh OA with an increasing contribution of the oxygenated ion C2H3O+ during aging. After five hours of aging, the OA has a rather low C2H3O+ signal for a given CO2+ fraction, possibly indicating a higher ratio of acid to non-acid oxygenated compounds in wood burning OA compared to other oxygenated organic aerosol (OOA).01A - Beitrag in wissenschaftlicher ZeitschriftPublikation 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, ErnestWe 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 ZeitschriftPublikation Volatility and hygroscopicity of aging secondary organic aerosol in a smog chamber(Copernicus, 18.11.2011) Tritscher, Torsten; Dommen, Josef; DeCarlo, Peter F.; Gysel, Martin; Barmet, Peter B.; Praplan, Arnaud P.; Weingartner, Ernest; Prévôt, Andre S.H.; Riipinen, Ilona; Donahue, Neil M.; Baltensperger, UrsThe evolution of secondary organic aerosols (SOA) during (photo-)chemical aging processes was investigated in a smog chamber. Fresh SOA from ozonolysis of 10 to 40 ppb α-pinene was formed followed by aging with OH radicals. The particles' volatility and hygroscopicity (expressed as volume fraction remaining (VFR) and hygroscopicity parameter κ) were measured in parallel with a volatility and hygroscopicity tandem differential mobility analyzer (V/H-TDMA). An aerosol mass spectrometer (AMS) was used for the chemical characterization of the aerosol. These measurements were used as sensitive parameters to reveal the mechanisms possibly responsible for the changes in the SOA composition during aging. A change of VFR and/or κ during processing of atmospheric aerosols may occur either by addition of SOA mass (by condensation) or by a change of SOA composition leading to different aerosol properties. The latter may occur either by heterogeneous reactions on the surface of the SOA particles, by condensed phase reactions like oligomerization or by an evaporation – gas-phase oxidation – recondensation cycle. The condensation mechanism showed to be dominant when there is a substantial change in the aerosol mass by addition of new molecules to the aerosol phase with time. Experiments could be divided into four periods based on the temporal evolution (qualitative changes) of VFR, κ and organic mass: O3 induced condensation, ripening, and OH induced chemical aging first with substantial mass gain and then without significant mass gain. During the O3 induced condensation the particles' volatility decreased (increasing VFR) while the hygroscopicity increased. Thereafter, in the course of ripening volatility continued to decrease, but hygroscopicity stayed roughly constant. After exposing the SOA to OH radicals an OH induced chemical aging with substantial mass gain started resulting in the production of at least 50 % more SOA mass. This new SOA mass was highly volatile and oxidized. This period was then followed by further OH induced chemical aging without significant mass gain leading to a decrease of volatility while hygroscopicity and SOA mass stayed roughly constant.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation 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 ZeitschriftPublikation Relating hygroscopicity and composition of organic aerosol particulate matter(Copernicus, 10.02.2011) Duplissy, Jonathan; DeCarlo, Peter F.; Dommen, Josef; Alfarra, M. Rami; Metzger, Axel; Barmpadimos, Iakovos; Prevot, Andre S.H.; Weingartner, Ernest; Tritscher, Torsten; Gysel, Martin; Aiken, Allison C.; Jimenez, Jose L; Canagaratna, Manjula R.; Worsnop, Douglas R.; Collins, Don R.; Tomlinson, Jason; Baltensperger, UrsA hygroscopicity tandem differential mobility analyzer (HTDMA) was used to measure the water uptake (hygroscopicity) of secondary organic aerosol (SOA) formed during the chemical and photochemical oxidation of several organic precursors in a smog chamber. Electron ionization mass spectra of the non-refractory submicron aerosol were simultaneously determined with an aerosol mass spectrometer (AMS), and correlations between the two different signals were investigated. SOA hygroscopicity was found to strongly correlate with the relative abundance of the ion signal m/z 44 expressed as a fraction of total organic signal (f44). m/z 44 is due mostly to the ion fragment CO2+ for all types of SOA systems studied, and has been previously shown to strongly correlate with organic O/C for ambient and chamber OA. The analysis was also performed on ambient OA from two field experiments at the remote site Jungfraujoch, and the megacity Mexico City, where similar results were found. A simple empirical linear relation between the hygroscopicity of OA at subsaturated RH, as given by the hygroscopic growth factor (GF) or "ϰorg" parameter, and f44 was determined and is given by ϰorg = 2.2 × f44 − 0.13. This approximation can be further verified and refined as the database for AMS and HTDMA measurements is constantly being expanded around the world. The use of this approximation could introduce an important simplification in the parameterization of hygroscopicity of OA in atmospheric models, since f44 is correlated with the photochemical age of an air mass.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Aging induced changes on NEXAFS fingerprints in individual combustion particles(Copernicus, 24.11.2011) Zelenay, Veronika; Mooser, René; Tritscher, Torsten; Křepelová, Adela; Heringa, Maarten F.; Chirico, Roberto; Prévôt, André SH.; Weingartner, Ernest; Baltensperger, Urs; Dommen, Josef; Watts, B.; Raabe, Jörg; Huthwelker, Thomas; Ammann, MarkusAbstract. Soot particles can significantly influence the Earth's climate by absorbing and scattering solar radiation as well as by acting as cloud condensation nuclei. However, despite their environmental (as well as economic and political) importance, the way these properties are affected by atmospheric processing of the combustion exhaust gases is still a subject of discussion. In this work, individual soot particles emitted from two different vehicles, a EURO 2 transporter, a EURO 3 passenger car, and a wood stove were investigated on a single-particle basis. The emitted exhaust, including the particulate and the gas phase, was processed in a smog chamber with artificial solar radiation. Single particle specimens of both unprocessed and aged soot were characterized using near edge X-ray absorption fine structure spectroscopy (NEXAFS) and scanning electron microscopy. Comparison of NEXAFS spectra from the unprocessed particles and those resulting from exhaust photooxidation in the chamber revealed changes in the carbon functional group content. For the wood stove emissions, these changes were minor, related to the relatively mild oxidation conditions. For the EURO 2 transporter emissions, the most apparent change was that of carboxylic carbon from oxidized organic compounds condensing on the primary soot particles. For the EURO 3 car emissions oxidation of primary soot particles upon photochemical aging has likely contributed as well. Overall, the changes in the NEXAFS fingerprints were in qualitative agreement with data from an aerosol mass spectrometer. Furthermore, by taking full advantage of our in situ microreactor concept, we show that the soot particles from all three combustion sources changed their ability to take up water under humid conditions upon photochemical aging of the exhaust. Due to the selectivity and sensitivity of the NEXAFS technique for the water mass, also small amounts of water taken up into the internal voids of agglomerated particles could be detected. Because such small amounts of water uptake do not lead to measurable changes in particle diameter, it may remain beyond the limits of volume growth measurements, especially for larger agglomerated particles.01A - Beitrag in wissenschaftlicher Zeitschrift