Browsing by Author "Bukowiecki, Nicolas"
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Publication A 17 month climatology of the cloud condensation nuclei number concentration at the high alpine site Jungfraujoch(Wiley, 24.05.2011) Jurányi, Zsófia; Gysel, Martin; Weingartner, Ernest; Bukowiecki, Nicolas; Kammermann, Lorenz; Baltensperger, UrsBetween May 2008 and September 2009 the cloud condensation nuclei (CCN) number concentration, NCCN, was measured at the high alpine site Jungfraujoch, which is located in the free troposphere most of the time. Measurements at 10 different supersaturations (0.12%–1.18%) were made using a CCN counter (CCNC). The monthly median NCCN values show a distinct seasonal variability with ∼5–12 times higher values in summer than in winter. The major part of this variation can be explained by the seasonal amplitude of total aerosol number concentration (∼4.5 times higher values in summer), but it is further amplified (factor of ∼1.1–2.6) by a shift of the particle number size distribution toward slightly larger sizes in summer. In contrast to the extensive properties, the monthly median of the critical dry diameter, above which the aerosols activate as CCN, does not show a seasonal cycle (relative standard deviations of the monthly median critical dry diameters at the different supersaturations are 4–9%) or substantial variability (relative standard deviations of individual data points at the different supersaturations are less than 18–37%). The mean CCN-derived hygroscopicity of the aerosol corresponds to a value of the hygroscopicity parameter κ of 0.20 (assuming a surface tension of pure water) with moderate supersaturation dependence. NCCN can be reliably predicted throughout the measurement period with knowledge of the above-mentioned averaged κ value and highly time-resolved (∼5 min) particle number size distribution data. The predicted NCCN was within 0.74 to 1.29 times the measured value during 80% of the time (94,499 data points in total at 10 different supersaturations).01A - Beitrag in wissenschaftlicher ZeitschriftPublication A European aerosol phenomenology - 6. Scattering properties of atmospheric aerosol particles from 28 ACTRIS sites(Copernicus, 2018) Pandolfi, Marco; Alados-Arboledas, Lucas; Alastuey, Andrés; Andrade, Marcos; Angelov, Christo; Artiñano, Begoña; Backman, John; Baltensperger, Urs; Bonasoni, Paolo; Bukowiecki, Nicolas; Collaud Coen, Martine; Conil, Sébastien; Coz, Esther; Crenn, Vincent; Dudoitis, Vadimas; Ealo, Marina; Eleftheriadis, Kostas; Favez, Olivier; Fetfatzis, Prodromos; Fiebig, Markus; Flentje, Harald; Ginot, Patrick; Gysel, Martin; Henzing, Bas; Hoffer, Andras; Holubova Smejkalova, Adela; Kalapov, Ivo; Kalivitis, Nikos; Kouvarakis, Giorgos; Kristensson, Adam; Kulmala, Markku; Lihavainen, Heikki; Lunder, Chris; Luoma, Krista; Lyamani, Hassan; Marinoni, Angela; Mihalopoulos, Nikolaos; Moerman, Marcel; Nicolas, José; O'Dowd, Colin D.; Petäjä, Tuukka; Petit, Jean-Eudes; Pichon, Jean Marc; Prokopciuk, Nina; Putaud, Jean-Philippe; Rodríguez, Sergio; Sciare, Jean; Sellegri, Karine; Swietlicki, Erik; Titos, Gloria; Tuch, Thomas; Tunved, Peter; Ulevicius, Vidmantas; Vaishya, Aditya; Vana, Milan; Virkkula, Aki; Vratolis, Stergios; Weingartner, Ernest; Wiedensohler, Alfred; Laj, PaoloThis paper presents the light-scattering properties of atmospheric aerosol particles measured over the past decade at 28 ACTRIS observatories, which are located mainly in Europe. The data include particle light scattering (σsp) and hemispheric backscattering (σbsp) coefficients, scattering Ångström exponent (SAE), backscatter fraction (BF) and asymmetry parameter (g). An increasing gradient of σsp is observed when moving from remote environments (arctic/mountain) to regional and to urban environments. At a regional level in Europe, σsp also increases when moving from Nordic and Baltic countries and from western Europe to central/eastern Europe, whereas no clear spatial gradient is observed for other station environments. The SAE does not show a clear gradient as a function of the placement of the station. However, a west-to-east-increasing gradient is observed for both regional and mountain placements, suggesting a lower fraction of fine-mode particle in western/south-western Europe compared to central and eastern Europe, where the fine-mode particles dominate the scattering. The g does not show any clear gradient by station placement or geographical location reflecting the complex relationship of this parameter with the physical properties of the aerosol particles. Both the station placement and the geographical location are important factors affecting the intra-annual variability. At mountain sites, higher σsp and SAE values are measured in the summer due to the enhanced boundary layer influence and/or new particle-formation episodes. Conversely, the lower horizontal and vertical dispersion during winter leads to higher σsp values at all low-altitude sites in central and eastern Europe compared to summer. These sites also show SAE maxima in the summer (with corresponding g minima). At all sites, both SAE and g show a strong variation with aerosol particle loading. The lowest values of g are always observed together with low σsp values, indicating a larger contribution from particles in the smaller accumulation mode. During periods of high σsp values, the variation of g is less pronounced, whereas the SAE increases or decreases, suggesting changes mostly in the coarse aerosol particle mode rather than in the fine mode. Statistically significant decreasing trends of σsp are observed at 5 out of the 13 stations included in the trend analyses. The total reductions of σsp are consistent with those reported for PM2.5 and PM10 mass concentrations over similar periods across Europe.01A - Beitrag in wissenschaftlicher ZeitschriftPublication A European aerosol phenomenology-5. Climatology of black carbon optical properties at 9 regional background sites across Europe(Elsevier, 2016) Zanatta, Marco; Gysel, Martin; Bukowiecki, Nicolas; Müller, Thomas; Weingartner, Ernest; Areskoug, Hans; Fiebig, Markus; Yttri, Karl Espen; Mihalopoulos, Nikolaos; Kouvarakis, Giorgos; Beddows, David; Harrison, Roy; Cavalli, Fabrizia; Putaud, Jean; Spindler, Gerald; Wiedensohler, Alfred; Alastuey, Andrés; Pandolfi, Marco; Sellegri, Karine; Swietlicki, Erik; Jaffrezo, Jean-Luc; Baltensperger, Urs; Laj, Paolo01A - Beitrag in wissenschaftlicher ZeitschriftPublication A mobile pollutant measurement laboratory - measuring gas phase and aerosol ambient concentrations with high spatial and temporal resolution(Elsevier, 12/2002) Bukowiecki, Nicolas; Dommen, Josef; Prévôt, André S.H.; Richter, Rene; Weingartner, Ernest; Baltensperger, UrsA mobile pollutant measurement laboratory was designed and built at the Paul Scherrer Institute (Switzerland) for the measurement of on-road ambient concentrations of a large set of trace gases and aerosol parameters with high time resolution (<15 s for most instruments), along with geographical and meteorological information. This approach allowed for pollutant level measurements both near traffic (e.g. in urban areas or on freeways/main roads) and at rural locations far away from traffic, within short periods of time and at different times of day and year. Such measurements were performed on a regular base during the project year of gas phase and aerosol measurements (YOGAM). This paper presents data measured in the Zürich (Switzerland) area on a late autumn day (6 November) in 2001. The local urban particle background easily reached 50 000 cmˉ³, with additional peak particle number concentrations of up to 400 000 cmˉ³. The regional background of the total particle number concentration was not found to significantly correlate with the distance to traffic and anthropogenic emissions of carbon monoxide and nitrogen oxides. On the other hand, this correlation was significant for the number concentration of particles in the size range 50–150 nm, indicating that the particle number concentration in this size range is a better traffic indicator than the total number concentration. Particle number size distribution measurements showed that daytime urban ambient air is dominated by high number concentrations of ultrafine particles (nanoparticles) with diameters < 50 nm, which are immediately formed by traffic exhaust and thus belong to the primary emissions. However, significant variation of the nanoparticle mode was also observed in number size distributions measured in rural areas both at daytime and nighttime, suggesting that nanoparticles are not exclusively formed by primary traffic emissions. While urban daytime total number concentrations were increased by a factor of 10 compared to the nighttime background, corresponding factors for total surface area and total volume concentrations were 2 and 1.5, respectively.01A - Beitrag in wissenschaftlicher ZeitschriftPublication A review of more than 20 years of aerosol observation at the high altitude research station Jungfraujoch, Switzerland (3580 m asl)(Taiwan Association for Aerosol Research, 2016) Bukowiecki, Nicolas; Weingartner, Ernest; Gysel, Martin; Coen, Martine Collaud; Zieger, Paul; Herrmann, Erik; Steinbacher, Martin; Gäggeler, Heinz W.; Baltensperger, Urs01A - Beitrag in wissenschaftlicher ZeitschriftPublication Aerosol decadal trends – Part 1. In-situ optical measurements at GAW and IMPROVE stations(Copernicus, 2013) Collaud Coen, Martine; Andrews, Elisabeth; Asmi, Ari; Baltensperger, Urs; Bukowiecki, Nicolas; Day, Derek; Fiebig, Markus; Fjaeraa, Ann Mari; Flentje, Harald; Hyvärinen, Antti-Pekka; Jefferson, Anne; Jennings, Stephen G.; Kouvarakis, Giorgos; Lihavainen, Heikki; Lund Myhre, Cathrine; Malm, William; Mihalopoulos, Nikolaos; Molenar, John; O'Dowd, Colin; Ogren, John A.; Schichtel, Bret; Sheridan, Patrick; Virkkula, Aki; Weingartner, Ernest; Weller, Rolf; Laj, PaoloCurrently many ground-based atmospheric stations include in-situ measurements of aerosol physical and optical properties, resulting in more than 20 long-term (> 10 yr) aerosol measurement sites in the Northern Hemisphere and Antarctica. Most of these sites are located at remote locations and monitor the aerosol particle number concentration, wavelength-dependent light scattering, backscattering, and absorption coefficients. The existence of these multi-year datasets enables the analysis of long-term trends of these aerosol parameters, and of the derived light scattering Ångström exponent and backscatter fraction. Since the aerosol variables are not normally distributed, three different methods (the seasonal Mann-Kendall test associated with the Sen's slope, the generalized least squares fit associated with an autoregressive bootstrap algorithm for confidence intervals, and the least-mean square fit applied to logarithms of the data) were applied to detect the long-term trends and their magnitudes. To allow a comparison among measurement sites, trends on the most recent 10 and 15 yr periods were calculated. No significant trends were found for the three continental European sites. Statistically significant trends were found for the two European marine sites but the signs of the trends varied with aerosol property and location. Statistically significant decreasing trends for both scattering and absorption coefficients (mean slope of −2.0% yr−1) were found for most North American stations, although positive trends were found for a few desert and high-altitude sites. The difference in the timing of emission reduction policy for the Europe and US continents is a likely explanation for the decreasing trends in aerosol optical parameters found for most American sites compared to the lack of trends observed in Europe. No significant trends in scattering coefficient were found for the Arctic or Antarctic stations, whereas the Arctic station had a negative trend in absorption coefficient. The high altitude Pacific island station of Mauna Loa presents positive trends for both scattering and absorption coefficients.01A - Beitrag in wissenschaftlicher ZeitschriftPublication Aerosol decadal trends – Part 2. In-situ aerosol particle number concentrations at GAW and ACTRIS stations(Copernicus, 2013) Asmi, Ari; Collaud Coen, Martine; Ogren, John A.; Andrews, Elisabeth; Sheridan, Patrick; Jefferson, Anne; Weingartner, Ernest; Baltensperger, Urs; Bukowiecki, Nicolas ; Lihavainen, Heikki; Kivekäs, Niku; Asmi, Eija; Aalto, Pasi Pekka; Kulmala, Markku; Wiedensohler, Alfred; Birmili, Wolfram; Hamed, Amar; O'Dowd, Colin; Jennings, Stephen G.; Weller, Rolf; Flentje, Harald; Fjaeraa, Ann Mari; Fiebig, Markus; Myhre, Cathrine Lund; Hallar, Anna Gannet; Swietlicki, Erik; Kristensson, Adam; Laj, PaoloWe have analysed the trends of total aerosol particle number concentrations (N) measured at long-term measurement stations involved either in the Global Atmosphere Watch (GAW) and/or EU infrastructure project ACTRIS. The sites are located in Europe, North America, Antarctica, and on Pacific Ocean islands. The majority of the sites showed clear decreasing trends both in the full-length time series, and in the intra-site comparison period of 2001–2010, especially during the winter months. Several potential driving processes for the observed trends were studied, and even though there are some similarities between N trends and air temperature changes, the most likely cause of many northern hemisphere trends was found to be decreases in the anthropogenic emissions of primary particles, SO2 or some co-emitted species. We could not find a consistent agreement between the trends of N and particle optical properties in the few stations with long time series of all of these properties. The trends of N and the proxies for cloud condensation nuclei (CCN) were generally consistent in the few European stations where the measurements were available. This work provides a useful comparison analysis for modelling studies of trends in aerosol number concentrations.01A - Beitrag in wissenschaftlicher ZeitschriftPublication Analysis of long‐term aerosol size distribution data from Jungfraujoch with emphasis on free tropospheric conditions, cloud influence, and air mass transport(Wiley, 2015) Herrmann, Erik; Weingartner, Ernest; Henne, Stephan; Vuilleumier, Laurent; Bukowiecki, Nicolas; Steinbacher, Martin; Conen, Franz; Collaud Coen, Martine; Hammer, Emanuel; Jurányi, Zsófia; Baltensperger, Urs; Gysel, MartinSix years of aerosol size distribution measurements between 20 and 600 nm diameters and total aerosol concentration above 10 nm from March 2008 to February 2014 at the high‐alpine site Jungfraujoch are presented. The size distribution was found to be typically bimodal with mode diameters and widths relatively stable throughout the year and the observation period. New particle formation was observed on 14.5% of all days without a seasonal preference. Particles typically grew only into the Aitken mode and did not reach cloud condensation nucleus (CCN) sizes on the time scale of several days. Growth of preexisting particles in the Aitken mode, on average, contributed very few CCN. We concluded that the dominant fraction of CCN at Jungfraujoch originated in the boundary layer. A number of approaches were used to distinguish free tropospheric (FT) conditions and episodes with planetary boundary layer (PBL) influence. In the absence of PBL injections, the concentration of particles larger than 90 nm (N90, roughly corresponding to the CCN concentration) reached a value ~40 cm−3 while PBL influence caused N90 concentrations of several hundred or even 1000 cm−3. Comparing three criteria for free tropospheric conditions, we found FT prevalence for 39% of the time with over 60% during winter and below 20% during summer. It is noteworthy that a simple criterion based on standard trace gas measurements appeared to outperform alternative approaches.01A - Beitrag in wissenschaftlicher ZeitschriftPublication Chemical and physical influences on aerosol activation in liquid clouds. A study based on observations from the Jungfraujoch, Switzerland(Copernicus, 2016) Hoyle, Christopher R.; Webster, Clare S.; Rieder, Harald E.; Nenes, Athanasios; Hammer, Emanuel; Herrmann, Erik; Gysel, Martin; Bukowiecki, Nicolas; Weingartner, Ernest; Steinbacher, Martin; Baltensperger, UrsA simple statistical model to predict the number of aerosols which activate to form cloud droplets in warm clouds has been established, based on regression analysis of data from four summertime Cloud and Aerosol Characterisation Experiments (CLACE) at the high-altitude site Jungfraujoch (JFJ). It is shown that 79 % of the observed variance in droplet numbers can be represented by a model accounting only for the number of potential cloud condensation nuclei (defined as number of particles larger than 80 nm in diameter), while the mean errors in the model representation may be reduced by the addition of further explanatory variables, such as the mixing ratios of O3, CO, and the height of the measurements above cloud base. The statistical model has a similar ability to represent the observed droplet numbers in each of the individual years, as well as for the two predominant local wind directions at the JFJ (northwest and southeast). Given the central European location of the JFJ, with air masses in summer being representative of the free troposphere with regular boundary layer in-mixing via convection, we expect that this statistical model is generally applicable to warm clouds under conditions where droplet formation is aerosol limited (i.e. at relatively high updraught velocities and/or relatively low aerosol number concentrations). A comparison between the statistical model and an established microphysical parametrization shows good agreement between the two and supports the conclusion that cloud droplet formation at the JFJ is predominantly controlled by the number concentration of aerosol particles.01A - Beitrag in wissenschaftlicher ZeitschriftPublication Contribution of new particle formation to the total aerosol concentration at the high‐altitude site Jungfraujoch (3580 m asl, Switzerland)(Wiley, 2016) Tröstl, Jasmin; Herrmann, Erik; Frege, Carla; Bianchi, Federico; Molteni, Ugo; Bukowiecki, Nicolas; Hoyle, Christopher R.; Steinbacher, Martin; Weingartner, Ernest; Dommen, Josef; Gysel, Martin; Baltensperger, UrsPrevious modeling studies hypothesized that a large fraction of cloud condensation nuclei (CCN) is attributed to new particle formation (NPF) in the free troposphere. Despite the potential importance of this process, only few long‐term observations have been performed to date. Here we present the results of a 12 month campaign of NPF observations at the high‐altitude site Jungfraujoch (JFJ, 3580 m above sea level (asl)). Our results show that NPF significantly adds to the total aerosol concentration at the JFJ and only occurs via previous precursor entrainment from the planetary boundary layer (PBL). Freshly nucleated particles do not directly grow to CCN size (90 nm) within observable time scales (maximum 48 h). The contribution of NPF to the CCN concentration is low within this time frame compared to other sources, such as PBL entrainment of larger particles. A multistep growth mechanism is proposed which allows previously formed Aitken mode particles to add to the CCN concentration. A parametrization is derived to explain formation rates at the JFJ, showing that precursor concentration, PBL influence, and global radiation are the key factors controlling new particle formation at the site.01A - Beitrag in wissenschaftlicher ZeitschriftPublication Contribution of railway traffic to local PM10 concentrations in Switzerland(Elsevier, 02/2007) Gehrig, Robert; Hill, Matz; Lienemann, Peter; Zwicky, Christoph N.; Bukowiecki, Nicolas; Weingartner, Ernest; Baltensperger, Urs; Buchmann, BrigitteField measurement campaigns of PM10 and its elemental composition (daily sampling on filters) covering different seasons were performed at two sites near the busiest railway station of Switzerland in Zurich (at a distance of 10 m from the tracks) and at a site near a very busy railway line with more than 700 trains per day. At this latter site parallel samples were taken at 10, 36 and 120 m distances from the tracks with the aim to study the distance dependence of the railway induced PM10 concentrations. To distinguish the relatively small railway emissions from the regional background (typically 20–25 μg m−3), simultaneous samples were also taken at an urban background site in Zurich. The differences in PM10 and elemental concentrations between the railway exposed sites and the background site were allocated to the railway contribution. Small, however, measurable PM10 concentration differences were found at all sites. The elemental composition of these differences revealed iron as the only quantitatively important constituent. As a long-term average it amounted to approximately 1 μg m−3 Fe at a distance of 10 m from the tracks at all three sites. Assuming that iron was at least partly oxidised (e.g. in the form of Fe2O3) the contribution can amount up to 1.5 μg m−3. Emissions of copper, manganese and chromium from trains were also clearly identified. However, compared to iron these, elements were emitted in very low quantities. No significant contribution from rock material (calcium, aluminium, magnesium, sodium) was observed as might have been expected from erosion, abrasion and resuspension from the gravel below the tracks. Particle emissions from diesel exhaust were not considered as trains in Switzerland are operated nearly exclusively by electric locomotives. The railway, induced contribution to ambient PM10 decreased rapidly with increasing distance from the tracks. At a distance of 120 m this contribution dropped to only 25% of the contribution observed at 10 m distance.01A - Beitrag in wissenschaftlicher ZeitschriftPublication Deposition uniformity and particle size distribution of ambient aerosol collected with a rotating drum impactor(Taylor & Francis, 30.06.2009) Bukowiecki, Nicolas; Richard, Agnes; Furger, Markus; Weingartner, Ernest; Aguirre, Myriam; Huthwelker, Thomas; Lienemann, Peter; Gehrig, Robert; Baltensperger, UrsRotating drum impactors (RDI) are cascade type impactors used for size and time resolved aerosol sampling, mostly followed by spectrometric analysis of the deposited material. They are characterized by one rectangular nozzle per stage and are equipped with an automated stepping mechanism for the impaction wheels. An existing three-stage rotating drum impactor was modified, to obtain new midpoint cutoff diameters at 2.5 μm, 1 μm, and 0.1 μm, respectively. For RDI samples collected under ambient air conditions, information on the size-segregation and the spatial uniformity of the deposited particles are key factors for a reliable spectrometric analysis of the RDI deposits. Two aerodynamic particle sizers (APS) were used for the determination of the RDI size fractionation characteristics, using polydisperse laboratory room air as quasi-stable proxy for urban ambient air. This experimental approach was suitable for the scope of this study, but was subject to numerous boundary conditions that limit a general use. Aerodynamic stage penetration midpoint diameters were estimated to be 2.4 and 1.0 μm for the first two RDI stages. Additionally, the spatial uniformity and geometrical size distribution of the deposited aerosol were investigated using micro-focus synchrotron radiation X-ray fluorescence spectrometry (micro-SR-XRF) and transmission electron microscopy (TEM), respectively. The size distribution of the particles found on the TEM samples agreed well with the results from the APS experiments. The RDI deposits showed sufficient uniformity for subsequent spectrometric analysis, but in the 2.5–10 μm size range the particle area density was very low. All of the applied methods confirmed the theoretical cutoff values of the modified RDI and showed that compared to other cascade impactors, the determined stage penetration sharpness was rather broad for the individual impactor stages.01A - Beitrag in wissenschaftlicher ZeitschriftPublication EUCAARI ion spectrometer measurements at 12 European sites – analysis of new particle formation events(Copernicus, 25.08.2010) Manninen, Hanna E.; Nieminen, Tuomo; Asmi, Eija; Gagné, Stéphanie; Häkkinen, Silja; Lehtipalo, Katrianne; Aalto, Pasi Pekka; Vana, Marko; Mirme, Aadu; Mirme, Sander; Hõrrak, Urmas; Plass-Dülmer, Christian; Stange, Gert; Kiss, Gyula; Hoffer, András; Törő, N.; Moerman, Marcel; Henzing, Bas; de Leeuw, Gerrit; Brinkenberg, Marcel; Kouvarakis, Giorgos N.; Bougiatioti, Aikaterini; Mihalopoulos, Nikolaos; O'Dowd, Colin D.; Ceburnis, Darius; Arneth, Almut; Svenningsson, Brigitta; Swietlicki, Erik; Tarozzi, Leone; Decesari, Stefano; Facchini, Maria Cristina; Birmili, Wolfram; Sonntag, André; Wiedensohler, Alfred; Boulon, Julien; Sellegri, Karine; Laj, Paolo; Gysel, Martin; Bukowiecki, Nicolas; Weingartner, Ernest; Wehrle, Günther; Laaksonen, Ari; Hamed, Amar; Joutsensaari, Jorma; Petäjä, Tuukka; Kerminen, Veli-Matti; Kulmala, MarkkuWe present comprehensive results on continuous atmospheric cluster and particle measurements in the size range ~1–42 nm within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) project. We focused on characterizing the spatial and temporal variation of new particle formation events and relevant particle formation parameters across Europe. Different types of air ion and cluster mobility spectrometers were deployed at 12 field sites across Europe from March 2008 to May 2009. The measurements were conducted in a wide variety of environments, including coastal and continental locations as well as sites at different altitudes (both in the boundary layer and the free troposphere). New particle formation events were detected at all of the 12 field sites during the year-long measurement period. From the data, nucleation and growth rates of newly formed particles were determined for each environment. In a case of parallel ion and neutral cluster measurements, we could also estimate the relative contribution of ion-induced and neutral nucleation to the total particle formation. The formation rates of charged particles at 2 nm accounted for 1–30% of the corresponding total particle formation rates. As a significant new result, we found out that the total particle formation rate varied much more between the different sites than the formation rate of charged particles. This work presents, so far, the most comprehensive effort to experimentally characterize nucleation and growth of atmospheric molecular clusters and nanoparticles at ground-based observation sites on a continental scale.01A - Beitrag in wissenschaftlicher ZeitschriftPublication Evaluating the capabilities and uncertainties of droplet measurements for the fog droplet spectrometer (FM-100)(Copernicus, 2012) Spiegel, Johanna K.; Zieger, Paul; Bukowiecki, Nicolas; Hammer, Emanuel; Weingartner, Ernest; Eugster, WernerAbstract. Droplet size spectra measurements are crucial to obtain a quantitative microphysical description of clouds and fog. However, cloud droplet size measurements are subject to various uncertainties. This work focuses on the error analysis of two key measurement uncertainties arising during cloud droplet size measurements with a conventional droplet size spectrometer (FM-100): first, we addressed the precision with which droplets can be sized with the FM-100 on the basis of the Mie theory. We deduced error assumptions and proposed a new method on how to correct measured size distributions for these errors by redistributing the measured droplet size distribution using a stochastic approach. Second, based on a literature study, we summarized corrections for particle losses during sampling with the FM-100. We applied both corrections to cloud droplet size spectra measured at the high alpine site Jungfraujoch for a temperature range from 0 °C to 11 °C. We showed that Mie scattering led to spikes in the droplet size distributions using the default sizing procedure, while the new stochastic approach reproduced the ambient size distribution adequately. A detailed analysis of the FM-100 sampling efficiency revealed that particle losses were typically below 10% for droplet diameters up to 10 μm. For larger droplets, particle losses can increase up to 90% for the largest droplets of 50 μm at ambient wind speeds below 4.4 m s−1 and even to >90% for larger angles between the instrument orientation and the wind vector (sampling angle) at higher wind speeds. Comparisons of the FM-100 to other reference instruments revealed that the total liquid water content (LWC) measured by the FM-100 was more sensitive to particle losses than to re-sizing based on Mie scattering, while the total number concentration was only marginally influenced by particle losses. Consequently, for further LWC measurements with the FM-100 we strongly recommend to consider (1) the error arising due to Mie scattering, and (2) the particle losses, especially for larger droplets depending on the set-up and wind conditions.01A - Beitrag in wissenschaftlicher ZeitschriftPublication 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 ZeitschriftPublication Ground-based and airborne in-situ measurements of the Eyjafjallajökull volcanic aerosol plume in Switzerland in spring 2010(Copernicus, 04.10.2011) Bukowiecki, Nicolas; Zieger, Paul; Weingartner, Ernest; Jurányi, Zsófia; Gysel, Martin; Neininger, Bruno; Schneider, Boris; Hueglin, Christoph; Ulrich, Andrea; Wichser, Adrian; Henne, Stephan; Brunner, Dominik; Kaegi, Ralf; Schwikowski, Margit; Tobler, Leonhard; Wienhold, Frank G.; Engel, Ilana; Buchmann, Brigitte; Peter, Thomas; Baltensperger, UrsThe volcanic aerosol plume resulting from the Eyjafjallajökull eruption in Iceland in April and May 2010 was detected in clear layers above Switzerland during two periods (17–19 April 2010 and 16–19 May 2010). In-situ measurements of the airborne volcanic plume were performed both within ground-based monitoring networks and with a research aircraft up to an altitude of 6000 m a.s.l. The wide range of aerosol and gas phase parameters studied at the high altitude research station Jungfraujoch (3580 m a.s.l.) allowed for an in-depth characterization of the detected volcanic aerosol. Both the data from the Jungfraujoch and the aircraft vertical profiles showed a consistent volcanic ash mode in the aerosol volume size distribution with a mean optical diameter around 3 ± 0.3 μm. These particles were found to have an average chemical composition very similar to the trachyandesite-like composition of rock samples collected near the volcano. Furthermore, chemical processing of volcanic sulfur dioxide into sulfate clearly contributed to the accumulation mode of the aerosol at the Jungfraujoch. The combination of these in-situ data and plume dispersion modeling results showed that a significant portion of the first volcanic aerosol plume reaching Switzerland on 17 April 2010 did not reach the Jungfraujoch directly, but was first dispersed and diluted in the planetary boundary layer. The maximum PM10 mass concentrations at the Jungfraujoch reached 30 μgm−3 and 70 μgm−3 (for 10-min mean values) duri ng the April and May episode, respectively. Even low-altitude monitoring stations registered up to 45 μgm−3 of volcanic ash related PM10 (Basel, Northwestern Switzerland, 18/19 April 2010). The flights with the research aircraft on 17 April 2010 showed one order of magnitude higher number concentrations over the northern Swiss plateau compared to the Jungfraujoch, and a mass concentration of 320 (200–520) μgm−3 on 18 May 2010 over the northwestern Swiss plateau. The presented data significantly contributed to the time-critical assessment of the local ash layer properties during the initial eruption phase. Furthermore, dispersion models benefited from the detailed information on the volcanic aerosol size distribution and its chemical composition.01A - Beitrag in wissenschaftlicher ZeitschriftPublication Investigation of the effective peak supersaturation for liquid-phase clouds at the high-alpine site Jungfraujoch, Switzerland (3580 m a.s.l.)(Copernicus, 2014) Hammer, Emanuel; Bukowiecki, Nicolas; Gysel, Martin; Jurányi, Zsófia; Hoyle, Christopher R.; Vogt, Roland; Baltensperger, Urs; Weingartner, ErnestAerosols influence the Earth's radiation budget directly through absorption and scattering of solar radiation in the atmosphere but also indirectly by modifying the properties of clouds. However, climate models still suffer from large uncertainties as a result of insufficient understanding of aerosol-cloud interactions. At the high altitude research station Jungfraujoch (JFJ; 3580 m a.s.l., Switzerland) cloud condensation nuclei (CCN) number concentrations at eight different supersaturations (SS) from 0.24% to 1.18% were measured using a CCN counter during Summer 2011. Simultaneously, in-situ aerosol activation properties of the prevailing ambient clouds were investigated by measuring the total and interstitial (non-activated) dry particle number size distributions behind two different inlet systems. Combining all experimental data, a new method was developed to retrieve the so-called effective peak supersaturation SSpeak, as a measure of the SS at which ambient clouds are formed. A 17-month CCN climatology was then used to retrieve the SSpeak values also for four earlier summer campaigns (2000, 2002, 2004 and 2010) where no direct CCN data were available. The SSpeak values varied between 0.01% and 2.0% during all campaigns. An overall median SSpeak of 0.35% and dry activation diameter of 87 nm was observed. It was found that the difference in topography between northwest and southeast plays an important role for the effective peak supersaturation in clouds formed in the vicinity of the JFJ, while differences in the number concentration of potential CCN only play a minor role. Results show that air masses coming from the southeast (with the slowly rising terrain of the Aletsch Glacier) generally experience lower SSpeak values than air masses coming from the northwest (steep slope). The observed overall median values were 0.41% and 0.22% for northwest and southeast wind conditions, respectively, corresponding to literature values for cumulus clouds and shallow-layer clouds. These cloud types are consistent with weather observations routinely performed at the JFJ.01A - Beitrag in wissenschaftlicher ZeitschriftPublication Investigation of the planetary boundary layer in the Swiss Alps using remote sensing and in situ measurements(Springer, 2014) Ketterer, Christine; Zieger, Paul; Bukowiecki, Nicolas; Collaud Coen, Martine; Maier, Olaf; Ruffieux, Dominique; Weingartner, Ernest01A - Beitrag in wissenschaftlicher ZeitschriftPublication Iron, manganese and copper emitted by cargo and passenger trains in Zürich (Switzerland). Size-segregated mass concentrations in ambient air(Elsevier, 02/2007) Bukowiecki, Nicolas; Gehrig, Robert; Hill, Matthias; Lienemann, Peter; Zwicky, Christoph N.; Buchmann, Brigitte; Weingartner, Ernest; Baltensperger, UrsParticle emissions caused by railway traffic have hardly been investigated in the past, due to their obviously minor influence on air quality compared to automotive traffic. In this study, emissions related to particle abrasion from wheels and tracks were investigated next to a busy railway line in Zürich (Switzerland), where trains run nearly exclusively with electrical locomotives. Hourly size-segregated aerosol samples (0.1–1, 1–2.5 and 2.5–10 μm) were collected with a rotating drum impactor (RDI) and subsequently analyzed by synchrotron radiation X-ray fluorescence spectrometry (SR-XRF). In this way, hourly elemental mass concentrations were obtained for chromium, manganese, iron and copper, which are the elements most relevant for railway abrasion. Additionally, daily aerosol filters were collected at the same site as well as at a background site for subsequent analysis by gravimetry and wavelength dispersive XRF (WD-XRF). Railway related ambient air concentrations of iron and manganese were calculated for the coarse (2.5–10 μm) and fine (<2.5 μm) particle fraction by means of a Mn/Fe ratio investigation. The comparison to train type and frequency data showed that 75% and 60% of the iron and manganese mass concentrations related to cargo and passenger trains, respectively, were found in the coarse mode. The railway related iron mass concentration normalized by the train frequency ranges between 10 and 100 ng mˉ³ h iron in 10 m distance to the tracks, depending on train type. It is estimated that the personal exposure next to a busy railway line above ground is more than a magnitude lower than inside a subway station.01A - Beitrag in wissenschaftlicher ZeitschriftPublication New particle formation in the free troposphere. A question of chemistry and timing(American Association for the Advancement of Science, 2016) Bianchi, Federico; Tröstl, Jasmin; Junninen, Heikki; Frege, Carla; Henne, Stephan; Hoyle, Christopher R.; Molteni, Ugo; Herrmann, Erik; Adamov, Alexey; Bukowiecki, Nicolas; Chen, Xuemeng; Duplissy, Jonathan; Gysel, Martin; Hutterli, Manuel; Kangasluoma, Juha; Kontkanen, Jenni; Kürten, Andreas; Manninen, Hanna E.; Münch, Steffen; Peräkylä, Otso; Petäjä, Tuukka; Rondo, Linda; Williamson, Christina; Weingartner, Ernest; Curtius, Joachim; Worsnop, Douglas R.; Kulmala, Markku; Dommen, Josef; Baltensperger, UrsFrom neutral to new Many of the particles in the troposphere are formed in situ, but what fraction of all tropospheric particles do they constitute and how exactly are they made? Bianchi et al report results from a high-altitude research station. Roughly half of the particles were newly formed by the condensation of highly oxygenated multifunctional compounds. A combination of laboratory results, field measurements, and model calculations revealed that neutral nucleation is more than 10 times faster than ion-induced nucleation, that particle growth rates are size-dependent, and that new particle formation occurs during a limited time window.01A - Beitrag in wissenschaftlicher Zeitschrift