Gysel, Martin

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Martin Gysel

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2009 - 200912010 - 201514
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Autor:in: Jurányi, Zsófia × Anfangsdatum: 2004 ×

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  • Vorschaubild nicht verfügbar
    Publikation
    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, Martin [in: Journal of Geophysical Research: Atmospheres]
    Six 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 Zeitschrift
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    Publikation
    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 [in: Atmospheric Chemistry and Physics]
    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
  • Vorschaubild
    Publikation
    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, Ernest [in: Atmospheric Chemistry and Physics]
    Aerosols 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 Zeitschrift
  • Vorschaubild nicht verfügbar
    Publikation
    Predicting hygroscopic growth using single particle chemical composition estimates
    (Wiley, 2014) Healy, Robert M.; Evans, Greg J.; Murphy, Michael; Jurányi, Zsófia; Tritscher, Torsten; Laborde, Marie; Weingartner, Ernest; Gysel, Martin; Poulain, Laurent; Kamilli, Katharina A.; Wiedensohler, Alfred; O'Connor, Ian P.; McGillicuddy, Eoin; Sodeau, John R.; Wenger, John C. [in: Journal of Geophysical Research: Atmospheres]
    Single particle mass spectral data, collected in Paris, France, have been used to predict hygroscopic growth at the single particle level. The mass fractions of black carbon, organic aerosol, ammonium, nitrate, and sulphate present in each particle were estimated using a combination of single particle mass spectrometer and bulk aerosol chemical composition measurements. The Zdanovskii‐Stokes‐Robinson (ZSR) approach was then applied to predict hygroscopic growth factors based on these mass fraction estimates. Smaller particles with high black carbon mass fractions and low inorganic ion mass fractions exhibited the lowest predicted growth factors, while larger particles with high inorganic ion mass fractions exhibited the highest growth factors. Growth factors were calculated for subsaturated relative humidity (90%) to enable comparison with hygroscopic tandem differential mobility analyzer measurements. Mean predicted and measured hygroscopic growth factors for 110, 165, and 265 nm particles were found to agree within 6%. Single particle‐based ZSR hygroscopicity estimates offer an advantage over bulk aerosol composition‐based hygroscopicity estimates by providing additional chemical mixing state information. External mixing can be determined for particles of a given diameter through examination of the predicted hygroscopic growth factor distributions. Using this approach, 110 nm and 265 nm particles were found to be predominantly internally mixed; however, external mixing of 165 nm particles was observed periodically when thinly coated and thickly coated black carbon particles were simultaneously detected. Single particle‐resolved chemical information will be useful for modeling efforts aimed at constraining cloud condensation nuclei activity and hygroscopic growth.
    01A - Beitrag in wissenschaftlicher Zeitschrift
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    Publikation
    CCN activity and volatility of β-caryophyllene secondary organic aerosol
    (Copernicus, 2013) Frosch, Mia; Bilde, Merete; Nenes, Athanasios; Praplan, Arnaud P.; Jurányi, Zsófia; Dommen, Josef; Gysel, Martin; Weingartner, Ernest; Baltensperger, Urs [in: Atmospheric Chemistry and Physics]
    In a series of smog chamber experiments, the cloud condensation nuclei (CCN) activity of secondary organic aerosol (SOA) generated from ozonolysis of β-caryophyllene was characterized by determining the CCN derived hygroscopicity parameter, κCCN, from experimental data. Two types of CCN counters, operating at different temperatures, were used. The effect of semi-volatile organic compounds on the CCN activity of SOA was studied using a thermodenuder. Overall, SOA was only slightly CCN active (with κCCN in the range 0.001–0.16), and in dark experiments with no OH scavenger present, κCCN decreased when particles were sent through the thermodenuder (with a temperature up to 50 °C). SOA was generated under different experimental conditions: In some experiments, an OH scavenger (2-butanol) was added. SOA from these experiments was less CCN active than SOA produced in experiments without an OH scavenger (i.e. where OH was produced during ozonolysis). In other experiments, lights were turned on, either without or with the addition of HONO (OH source). This led to the formation of more CCN active SOA. SOA was aged up to 30 h through exposure to ozone and (in experiments with no OH scavenger present) to OH. In all experiments, the derived κCCN consistently increased with time after initial injection of β-caryophyllene, showing that chemical ageing increases the CCN activity of β-caryophyllene SOA. κCCN was also observed to depend on supersaturation, which was explained either as an evaporation artifact from semi-volatile SOA (only observed in experiments lacking light exposure) or, alternatively, by effects related to chemical composition depending on dry particle size. Using the method of Threshold Droplet Growth Analysis it was also concluded that the activation kinetics of the SOA do not differ significantly from calibration ammonium sulphate aerosol for particles aged for several hours.
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Vorschaubild
    Publikation
    Black carbon physical properties and mixing state in the European megacity Paris
    (Copernicus, 2013) Laborde, Marie; Crippa, Monica; Tritscher, Torsten; Jurányi, Zsófia; Decarlo, Peter; Temime-Roussel, Brice; Marchand, Nicolas; Eckhardt, Sabine; Stohl, Andreas; Baltensperger, Urs; Prévôt, André S.H.; Weingartner, Ernest; Gysel, Martin [in: Atmospheric Chemistry and Physics]
    Aerosol hygroscopicity and refractory black carbon (rBC) properties were characterised during wintertime at a suburban site in Paris, one of the biggest European cities. Hygroscopic growth factor (GF) frequency distributions, characterised by distinct modes of more-hygroscopic background aerosol and non- or slightly hygroscopic aerosol of local (or regional) origin, revealed an increase of the relative contribution of the local sources compared to the background aerosol with decreasing particle size. BC-containing particles in Paris were mainly originating from fresh traffic emissions, whereas biomass burning only gave a minor contribution. The mass size distribution of the rBC cores peaked on average at an rBC core mass equivalent diameter of DMEV ~ 150 nm. The BC-containing particles were moderately coated (coating thickness Δcoat ~ 33 nm on average for rBC cores with DMEV = 180–280 nm) and an average mass absorption coefficient (MAC) of ~ 8.6 m2 g−1 at the wavelength λ = 880 nm was observed. Different time periods were selected to investigate the properties of BC-containing particles as a function of source and air mass type. The traffic emissions were found to be non-hygroscopic (GF ≈ 1.0), and essentially all particles with a dry mobility diameter (D0) larger than D0 = 110 nm contained an rBC core. rBC from traffic emissions was further observed to be uncoated within experimental uncertainty (Δcoat ~ 2 nm ± 10 nm), to have the smallest BC core sizes (maximum of the rBC core mass size distribution at DMEV ~ 100 nm) and to have the smallest MAC (~ 7.3 m2g−1 at λ = 880 nm). The biomass burning aerosol was slightly more hygroscopic than the traffic emissions (with a distinct slightly-hygroscopic mode peaking at GF ≈ 1.1–1.2). Furthermore, only a minor fraction (≤ 10%) of the slightly-hygroscopic particles with 1.1 ≤ GF ≤ 1.2 (and D0 = 265 nm) contained a detectable rBC core. The BC-containing particles from biomass burning were found to have a medium coating thickness as well as slightly larger mean rBC core sizes and MAC values compared to traffic emissions. The aerosol observed under the influence of aged air masses and air masses from Eastern Continental Europe was dominated by a~more-hygroscopic mode peaking at GF ≈ 1.6. Most particles (95%), in the more-hygroscopic mode at D0 = 265 nm, did not contain a detectable rBC core. A significant fraction of the BC-containing particles had a substantial coating with non-refractory aerosol components. MAC values of ~ 8.8 m2g−1 and ~ 8.3 m2g−1 at λ = 880 nm and mass mean rBC core diameters of 150 nm and 200 nm were observed for the aged and continental air mass types, respectively. The reason for the larger rBC core sizes compared to the fresh emissions – transport effects or a different rBC source – remains unclear. The dominant fraction of the BC-containing particles was found to have no or very little coating with non-refractory matter. The lack of coatings is consistent with the observation that the BC-containing particles are non- or slightly-hygroscopic, which makes them poor cloud condensation nuclei. It can therefore be expected that wet removal through nucleation scavenging is inefficient for fresh BC-containing particles in urban plumes. The mixing-state-specific cloud droplet activation behaviour of BC-containing particles including the effects of atmospheric aging processes should be considered in global simulations of atmospheric BC, as the wet removal efficiency remains a major source of uncertainty in its life-cycle.
    01A - Beitrag in wissenschaftlicher Zeitschrift
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    Publikation
    Hygroscopic mixing state of urban aerosol derived from size-resolved cloud condensation nuclei measurements during the MEGAPOLI campaign in Paris
    (Copernicus, 2013) Jurányi, Zsófia; Tritscher, Torsten; Gysel, Martin; Laborde, Marie; Gomes, L.; Roberts, G.; Baltensperger, Urs; Weingartner, Ernest [in: Atmospheric Chemistry and Physics]
    Abstract. Ambient aerosols are a complex mixture of particles with different physical and chemical properties and consequently distinct hygroscopic behaviour. The hygroscopicity of a particle determines its water uptake at subsaturated relative humidity (RH) and its ability to form a cloud droplet at supersaturated RH. These processes influence Earth's climate and the atmospheric lifetime of the particles. Cloud condensation nuclei (CCN) number size distributions (i.e. CCN number concentrations as a function of dry particle diameter) were measured close to Paris during the MEGAPOLI campaign in January–February 2010, covering 10 different supersaturations (SS = 0.1–1.0%). The time-resolved hygroscopic mixing state with respect to CCN activation was also derived from these measurements. Simultaneously, a hygroscopicity tandem differential mobility analyser (HTDMA) was used to measure the hygroscopic growth factor (ratio of wet to dry mobility diameter) distributions at RH = 90%. The aerosol was highly externally mixed and its mixing state showed significant temporal variability. The average particle hygroscopicity was relatively low at subsaturation (RH = 90%; mean hygroscopicity parameter κ = 0.12–0.27) and increased with increasing dry diameter in the range 35–265 nm. The mean κ value, derived from the CCN measurements at supersaturation, ranged from 0.08 to 0.24 at SS = 1.0–0.1%. Two types of mixing-state resolved hygroscopicity closure studies were performed, comparing the water uptake ability measured below and above saturation. In the first type the CCN counter was connected in series with the HTDMA and and closure was achieved over the whole range of probed dry diameters, growth factors and supersaturations using the κ-parametrization for the water activity and assuming surface tension of pure water in the Köhler theory. In the second closure type we compared hygroscopicity distributions derived from parallel monodisperse CCN measurements and HTDMA measurements. Very good agreement was found at all supersaturations, which shows that monodisperse CCN measurements are a reliable alternative to determine the hygroscopic mixing state of ambient aerosols.
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Vorschaubild nicht verfügbar
    Publikation
    Hygroscopic properties of fresh and aged wood burning particles
    (Elsevier, 2013) Martin, Maria; Tritscher, Torsten; Jurányi, Zsófia; Heringa, Maarten F.; Sierau, Berko; Weingartner, Ernest; Chirico, Roberto; Gysel, Martin; Prévôt, André S.H.; Baltensperger, Urs; Lohmann, Ulrike [in: Journal of Aerosol Science]
    01A - Beitrag in wissenschaftlicher Zeitschrift
  • Vorschaubild nicht verfügbar
    Publikation
    Relating cloud condensation nuclei activity and oxidation level of α-pinene secondary organic aerosols
    (Wiley, 30.11.2011) Frosch, Mia; Bilde, Merete; DeCarlo, Peter F.; Jurányi, Zsófia; Tritscher, Torsten; Dommen, Josef; Donahue, Neil M.; Gysel, Martin; Weingartner, Ernest; Baltensperger, Urs [in: Journal of Geophysical Research: Atmospheres]
    During a series of smog chamber experiments, the effects of chemical and photochemical aging on the ability of organic aerosols generated from ozonolysis of α-pinene to act as cloud condensation nuclei (CCN) were investigated. In particular, the study focused on the relation between oxygenation and the CCN-derived single hygroscopicity parameter κ for different experimental conditions: varying precursor concentrations (10–40 ppb), different OH sources (photolysis of HONO either with or without the addition of NO or ozonolysis of tetramethylethylene), and exposure to light. Oxygenation was described by the contribution of the aerosol mass spectrometer (AMS) mass fragment m/z 44 to the total organic signal (f44) and the oxygen to carbon molar ratio (O/C), likewise determined with AMS. CCN activity, described by the hygroscopicity parameter κ, was determined with a CCN counter. It was found that f44 increases with decreasing precursor concentration and with chemical aging, whereas neither of these affects CCN activity. Overall, κ is largely independent of O/C in the range 0.3 < O/C < 0.6 (0.07 < f44 < 0.12), although an empirical unweighted least squares fit was determined: κ = (0.071 ± 0.02) · (O/C) + (0.0785 ± 0.009) for particles with diameter in the range 59–200 nm. Growth kinetics of activating secondary organic aerosols were found to be comparable to those of ammonium sulfate and were not influenced by chemical aging.
    01A - Beitrag in wissenschaftlicher Zeitschrift
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    Publikation
    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, Urs [in: Atmospheric Chemistry and Physics]
    The 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 Zeitschrift