lnstitut für Sensorik und Elektronik
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Publikation Coating of soot and (NH4)2SO4 particles by ozonolysis products of α-pinene(Elsevier, 10/2003) Saathoff, Harald; Naumann, Karl-Heinz; Schnaiter, Martin; Schöck, Werner; Möhler, Ottmar; Schurath, Ulrich; Weingartner, Ernest; Gysel, Martin; Baltensperger, UrsThe ozonolysis of α-pinene in a large aerosol chamber was used to generate secondary organic aerosol (SOA) mass by homogeneous nucleation, or by heterogeneous nucleation, either on soot, or on (NH4)2SO4 seed aerosols. The rate of the α-pinene + ozone reaction and the aerosol yield of ∼19% are in good agreement with literature data. The organic coating of soot particles leads to a compaction of the fractal agglomerates expressed by an increase in fractal dimension from 1.9 to 2.1 for Diesel soot, and from 2.0 to 2.3 for spark generated “Palas” soot. The dielectric coating of the soot particles with SOA layers between 2 to 11 nm gives rise to a substantial enhancement of their single scattering albedo, from about 0.2 to 0.5, and increases the effective absorption coefficients of both soot types by ca. 30%. The coating of both soot types increases the hygroscopic growth factors (HGF) to values close below the HGF measured for pure SOA material d/d0∼1:12 at 90% RH.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Properties of jet engine combustion particles during the PartEmis experiment: Hygroscopicity at subsaturated conditions(Wiley, 06.06.2003) Gysel, Martin; Nyeki, Stephan; Weingartner, Ernest; Baltensperger, Urs; Giebl, Heinrich; Hitzenberger, Regina; Petzold, Andreas; Wilson, C. W.Hygroscopic properties of combustion particles were measured online with a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) during PartEmis jet engine combustor experiments. The combustor was operated at old and modern cruise conditions with fuel sulfur contents (FSC) of 50, 410 and 1270 μg/g, and hygroscopic growth factors (HGF) of particles with different dry diameters were investigated at relative humidities RH ≤ 95%. HGFs increased strongly with increasing FSC (HGF[95% RH, 50 nm, modern cruise] = 1.01 and 1.16 for low and high FSC, respectively), and decreased with increasing particle size at fixed FSC, whereas no significant difference was detected between old and modern cruise. HGFs agreed well with a two-parameter theoretical model which provided an estimate of the sulfuric acid content of dry particles, indicating a nearly linear dependence on FSC.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Properties of jet engine combustion particles during the PartEmis experiment. Hygroscopic growth at supersaturated conditions(Wiley, 31.07.2003) Hitzenberger, Regina; Giebl, Heinrich; Petzold, Andreas; Gysel, Martin; Nyeki, Stephan; Weingartner, Ernest; Baltensperger, Urs; Wilson, C. W.During the EU Project PartEmis, the microphysical properties of aircraft combustion aerosol were investigated. This study is focused on the ability of exhaust aerosols to act as cloud condensation nuclei (CCN). The combustor was operated at two different conditions representing old and modern aircraft engine technology. CCN concentrations were measured with the University of Vienna CCN counter [Giebl et al., 2002] at supersaturations around 0.7%. The activation ratio (fraction of CCN in total aerosol) depended on the fuel sulphur content (FSC) and also on the operation conditions. CCN/CN ratios increased from 0.93 through 1.43 to 5.15*10ˉ³ (old cruise conditions) and 0.67 through 3.04 to 7.94*10ˉ³ (modern cruise conditions) when FSC increased from 50 through 410 to1270 μg/g. The activation behaviour was modelled using classical theories and with a semi-empirical model [Gysel et al., 2003] based on measured hygroscopicity of the aerosol under subsaturated conditions, which gave the best agreement.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Properties of jet engine combustion particles during the PartEmis experiment. Microphysics and Chemistry(Wiley, 15.07.2003) Petzold, Andreas; Stein, Claudia; Nyeki, Stephan; Gysel, Martin; Weingartner, Ernest; Baltensperger, Urs; Giebl, Heinrich; Hitzenberger, Regina; Döpelheuer, Andreas; Vrchoticky, Susi; Puxbaum, Hans; Johnson, M.; Hurley, Chris D.; Marsh, Richard; Wilson, Chris W.The particles emitted from an aircraft engine combustor were investigated in the European project PartEmis. Measured aerosol properties were mass and number concentration, size distribution, mixing state, thermal stability of internally mixed particles, hygroscopicity, and cloud condensation nuclei (CCN) activation potential. The combustor operation conditions corresponded to modern and older engine gas path temperatures at cruise altitude, with fuel sulphur contents (FSC) of 50, 410, and 1270 μg/g. Operation conditions and FSC showed only a weak influence on the microphysical aerosol properties, except for hygroscopic and CCN properties. Particles of size D ≥ 30 nm were almost entirely internally mixed. Particles of sizes D < 20 nm showed a considerable volume fraction of compounds that volatilise at 390 K (10–15%) and 573 K (4–10%), while respective fractions decreased to <5% for particles of size D ≥ 50 nm.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Hygroscopicity of aerosol particles at low temperatures. 1. New low-temperature H-TDMA instrument. setup and first applications(American Chemical Society, 22.11.2001) Weingartner, Ernest; Gysel, Martin; Baltensperger, UrsA hygroscopicity tandem differential mobility analyzer (H-TDMA) is described that allows a fast and accurate determination of the water uptake by submicrometer aerosol particles at temperatures below 0 °C. To avoid volatilization of semivolatile particles, the humidification works without heating the gas stream, and the gas-phase composition is not changed during the analysis. The applied scanning mobility analysis allows a fast and accurate measurement of the humidogram, but care has to be taken with too high scanning velocities leading to artifacts in the particle size measurement. During a field campaign at a high-alpine site (Jungfraujoch, 3580 m above sea level), humidograms of free tropospheric particles were measured at T = −10 °C. The hygroscopic growth of these particles was characterized by monomodal growth distributions, which means that in the observed size range (dry particle diameters (Do) = 50−250 nm) the free tropospheric aerosol was to a large extent internally mixed. No distinct deliquescence was observed, indicating that the multicomponent aerosol particles are present in a liquid state even at a low relative humidity (RH) <10%. At RH 85%, average hygroscopic growth factors of 1.44, 1.49, and 1.53 were measured for Do = 50, 100, and 250 nm. The estimated soluble volume fraction of the particles in the observed size range was found to be 0.79, 0.86, and 0.91, respectively.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Hygroscopicity of aerosol particles at low temperatures. 2. Theoretical and experimental hygroscopic properties of laboratory generated aerosols(American Chemical Society, 21.11.2001) Gysel, Martin; Weingartner, Ernest; Baltensperger, UrsA Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) system has been used to measure hygroscopic growth curves and deliquescence relative humidities (DRH) of laboratory generated (NH4)2SO4, NaCl, and NaNO3 particles at temperatures T = 20 °C and −10 °C. Good agreement (better than 3.5%) between measured growth curves and Köhler theory was found using empirical temperature and concentration dependent values for water activity, solution density, and surface tension. The measured growth curves only experience a small temperature dependence in the observed temperature range. Therefore, to a first approximation, it is possible to neglect the temperature dependence of the water activity for theoretical calculations in the temperature range −10 °C < T < 25 °C. The small differences between experiment and theory, which were predominantly observed for NaCl particles, are probably caused by a small amount of water adsorbed on the “dry” crystals. It was also observed that these particles experience a significant restructuring at relative humidity RH < DRH, which was also taken into account for a comparison with theoretical curves. If salt particles are used for instrument calibration, precautions regarding the dry particle diameter have to be taken.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Hygroscopic growth and water uptake kinetics of two-phase aerosol particles consisting of ammonium sulfate, adipic and humic acid mixtures(Elsevier, 02/2007) Sjögren, Staffan; Gysel, Martin; Weingartner, Ernest; Baltensperger, Urs; Cubison, Michael J.; Coe, Hugh; Zardini, Alessandro A.; Marcolli, Claudia; Krieger, Ulrich K.; Peter, ThomasThe hygroscopic growth of solid aerosol particles consisting of mixtures of ammonium sulfate and either adipic acid or Aldrich humic acid sodium salt was characterized with a hygroscopicity tandem differential mobility analyzer and an electrodynamic balance. In particular, the time required for the aerosol particle phase and the surrounding water vapor to reach equilibrium at high relative humidity (RH) was investigated. Depending on the chemical composition of the particles, residence times of > 40 s were required to reach equilibrium at 85% RH, yielding up to a 7% reduction in the measured hygroscopic growth factors from measurements at 4 s residence time compared to measurements at equilibrium. We suggest that the solid organic compound, when present as the dominant component, encloses the water-soluble inorganic salt in veins and cavities, resulting in the observed slow water uptake. Comparison with predictions from the Zdanovskii-Stokes-Robinson relation shows enhanced water uptake of the mixed particles. This is explained with the presence of the salt solution in veins resulting in a negative curvature of the solution meniscus at the opening of the vein. In conclusion, it is important for studies of mixtures of water soluble compounds with insoluble material to allow for sufficient residence time at the specified humidity to reach equilibrium before the hygroscopicity measurements.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation 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, UrsCloud 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 ZeitschriftPublikation Secondary organic aerosols from anthropogenic and biogenic precursors(Royal Society of Chemistry, 2005) Baltensperger, Urs; Kalberer, Markus; Dommen, Josef; Paulsen, Dwane; Alfarra, M. Rami; Coe, Hugh; Fisseha, Rebeka; Gascho, Astrid; Gysel, Martin; Nyeki, Stephan; Sax, Mirjam; Steinbacher, Martin; Prévôt, André S.H.; Sjögren, Staffan; Weingartner, Ernest; Zenobi, RenatoSecondary organic aerosol (SOA) formation from the photooxidation of an anthropogenic (1,3,5-trimethylbenzene) and a biogenic (α-pinene) precursor was investigated at the new PSI smog chamber. The chemistry of the gas phase was followed by proton transfer reaction mass spectrometry, while the aerosol chemistry was investigated with aerosol mass spectrometry, ion chromatography, laser desorption ionization mass spectrometry, and infrared spectroscopy, along with volatility and hygroscopicity studies. Evidence for oligomer formation for SOA from both precursors was given by an increasing abundance of compounds with a high molecular weight (up to 1000 Da) and by an increasing thermal stability with increasing aging time. The results were compared to data obtained from ambient aerosol samples, revealing a number of similar features.01A - Beitrag in wissenschaftlicher ZeitschriftPublikation Properties of jet engine combustion particles during the PartEmis experiment. Particle size spectra (d > 15 nm) and volatility(Wiley, 18.09.2004) Nyeki, Staphan; Gysel, Martin; Weingartner, Ernest; Baltensperger, Urs; Hitzenberger, Regina; Petzold, Andreas; Wilson, Chris W.Size distributions (d > 15 nm) and volatile properties of combustion particles were measured during test-rig experiments on a jet engine, consisting of a combustor and three simulated turbine stages (HES). The combustor was operated to simulate legacy (inlet temperature 300°C) and contemporary (500°C) cruise conditions, using kerosene with three different fuel sulfur contents (FSC; 50, 400 and 1300 μg gˉ¹). Measurements found that contemporary cruise conditions resulted in lower number emission indices (EI N15) and higher geometric mean particle diameter (dG) than for legacy conditions. Increasing FSC resulted in an overall increase in EIN15 and decrease in dG. The HES stages or fuel additive (APA101) had little influence on EI N15 or dG, however, this is uncertain due to the measurement variability. EI N15 for non-volatile particles was largely independent of all examined conditions.01A - Beitrag in wissenschaftlicher Zeitschrift
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