Hochschule für Technik und Umwelt FHNW

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13-month climatology of the aerosol hygroscopicity at the free tropospheric site Jungfraujoch (3580 m a.s.l.)
(Copernicus, 16.11.2010) Kammermann, Lukas; Gysel, Martin; Weingartner, Ernest; Baltensperger, Urs
A hygroscopicity tandem differential mobility analyzer (HTDMA) was operated at the high-alpine site Jungfraujoch in order to characterize the hygroscopic diameter growth factors of the free tropospheric Aitken and accumulation mode aerosol. More than ~5000 h of valid data were collected for the dry diameters D0 = 35, 50, 75, 110, 165, and 265 nm during the 13-month measurement period from 1 May 2008 through 31 May 2009. No distinct seasonal variability of the hygroscopic properties was observed. Annual mean hygroscopic diameter growth factors (D/D0) at 90% relative humidity were found to be 1.34, 1.43, and 1.46 for D0 = 50, 110, and 265 nm, respectively. This size dependence can largely be attributed to the Kelvin effect because corresponding values of the hygroscopicity parameter κ are nearly independent of size. The mean hygroscopicity of the Aitken and accumulation mode aerosol at the free tropospheric site Jungfraujoch was found to be κ≈0.24 with little variability throughout the year. The impact of Saharan dust events, a frequent phenomenon at the Jungfraujoch, on aerosol hygroscopicity was shown to be negligible for D0<265 nm. Thermally driven injections of planetary boundary layer (PBL) air, particularly observed in the early afternoon of summer days with convective anticyclonic weather conditions, lead to a decrease of aerosol hygroscopicity. However, the effect of PBL influence is not seen in the annual mean hygroscopicity data because the effect is small and those conditions (weather class, season and time of day) with PBL influence are relatively rare. Aerosol hygroscopicity was found to be virtually independent of synoptic wind direction during advective weather situations, i.e. when horizontal motion of the atmosphere dominates over thermally driven convection. This indicates that the hygroscopic behavior of the aerosol observed at the Jungfraujoch can be considered representative of the lower free troposphere on at least a regional if not continental scale.
01A - Beitrag in wissenschaftlicher Zeitschrift
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, Urs
Between 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 Zeitschrift
A combined particle trap/HTDMA hygroscopicity study of mixed inorganic/organic aerosol particles
(Copernicus, 19.09.2008) Zardini, Alessandro A.; Sjogren, S.; Marcolli, Claudia; Krieger, Ulrich K.; Gysel, Martin; Weingartner, Ernest; Baltensperger, Urs; Peter, Thomas
Atmospheric aerosols are often mixtures of inorganic and organic material. Organics can represent a large fraction of the total aerosol mass and are comprised of water-soluble and insoluble compounds. Increasing attention was paid in the last decade to the capability of mixed inorganic/organic aerosol particles to take up water (hygroscopicity). We performed hygroscopicity measurements of internally mixed particles containing ammonium sulfate and carboxylic acids (citric, glutaric, adipic acid) in parallel with an electrodynamic balance (EDB) and a hygroscopicity tandem differential mobility analyzer (HTDMA). The organic compounds were chosen to represent three distinct physical states. During hygroscopicity cycles covering hydration and dehydration measured by the EDB and the HTDMA, pure citric acid remained always liquid, adipic acid remained always solid, while glutaric acid could be either. We show that the hygroscopicity of mixtures of the above compounds is well described by the Zdanovskii-Stokes-Robinson (ZSR) relationship as long as the two-component particle is completely liquid in the ammonium sulfate/glutaric acid system; deviations up to 10% in mass growth factor (corresponding to deviations up to 3.5% in size growth factor) are observed for the ammonium sulfate/citric acid 1:1 mixture at 80% RH. We observe even more significant discrepancies compared to what is expected from bulk thermodynamics when a solid component is present. We explain this in terms of a complex morphology resulting from the crystallization process leading to veins, pores, and grain boundaries which allow for water sorption in excess of bulk thermodynamic predictions caused by the inverse Kelvin effect on concave surfaces.
01A - Beitrag in wissenschaftlicher Zeitschrift
A compact and portable deposition chamber to study nanoparticles in air-exposed tissue
(Mary Ann Liebert, 2013) Mertes, Peter; Praplan, Arnaud P.; Künzi, Lisa; Dommen, Josef; Baltensperger, Urs; Geiser, Marianne; Weingartner, Ernest; Ricka, Jaroslav; Fierz, Martin; Kalberer, Markus
01A - Beitrag in wissenschaftlicher Zeitschrift
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, Paolo
01A - Beitrag in wissenschaftlicher Zeitschrift
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, Urs
A 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 Zeitschrift
A new method to discriminate secondary organic aerosols from different sources using high-resolution aerosol mass spectra
(Copernicus, 2012) Heringa, Maarten F.; DeCarlo, Peter F.; Chirico, Roberto; Tritscher, Torsten; Clairotte, Michael; Mohr, Christine; Crippa, Monica; Slowik, Jay Gates; Pfaffenberger, Lisa; Dommen, Josef; Weingartner, Ernest; Prévôt, André S.H.; Baltensperger, Urs
Abstract. Organic aerosol (OA) represents a significant and often major fraction of the non-refractory PM1 (particulate matter with an aerodynamic diameter da < 1 μm) mass. Secondary organic aerosol (SOA) is an important contributor to the OA and can be formed from biogenic and anthropogenic precursors. Here we present results from the characterization of SOA produced from the emissions of three different anthropogenic sources. SOA from a log wood burner, a Euro 2 diesel car and a two-stroke Euro 2 scooter were characterized with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and compared to SOA from α-pinene. The emissions were sampled from the chimney/tailpipe by a heated inlet system and filtered before injection into a smog chamber. The gas phase emissions were irradiated by xenon arc lamps to initiate photo-chemistry which led to nucleation and subsequent particle growth by SOA production. Duplicate experiments were performed for each SOA type, with the averaged organic mass spectra showing Pearson's r values >0.94 for the correlations between the four different SOA types after five hours of aging. High-resolution mass spectra (HR-MS) showed that the dominant peaks in the MS, m/z 43 and 44, are dominated by the oxygenated ions C2H3O+ and CO2+, respectively, similarly to the relatively fresh semi-volatile oxygenated OA (SV-OOA) observed in the ambient aerosol. The atomic O:C ratios were found to be in the range of 0.25–0.55 with no major increase during the first five hours of aging. On average, the diesel SOA showed the lowest O:C ratio followed by SOA from wood burning, α-pinene and the scooter emissions. Grouping the fragment ions revealed that the SOA source with the highest O:C ratio had the largest fraction of small ions. The HR data of the four sources could be clustered and separated using principal component analysis (PCA). The model showed a significant separation of the four SOA types and clustering of the duplicate experiments on the first two principal components (PCs), which explained 79% of the total variance. Projection of ambient SV-OOA spectra resolved by positive matrix factorization (PMF) showed that this approach could be useful to identify large contributions of the tested SOA sources to SV-OOA. The first results from this study indicate that the SV-OOA in Barcelona is strongly influenced by diesel emissions in winter while in summer at SIRTA at the southwestern edge of Paris SV-OOA is more similar to alpha-pinene SOA. However, contributions to the ambient SV-OOA from SOA sources that are not covered by the model can cause major interference and therefore future expansions of the PCA model with additional SOA sources is recommended.
01A - Beitrag in wissenschaftlicher Zeitschrift
A study of wood burning and traffic aerosols in an Alpine valley using a multi-wavelength aethalometer
(Elsevier, 20.09.2008) Sandradewi, Jisca; Prévôt, André S.H.; Weingartner, Ernest; Schmidhauser, Ralph; Gysel, Martin; Baltensperger, Urs
We present a study of aerosol light absorption using a multi-wavelength Aethalometer (l ¼ 370–950 nm) in an Alpine valley where the major local emissions of aerosols in winter are from domestic wood burning and traffic. The measurements were done in winter and summer periods in 2004 and 2005. Much stronger diurnal trends in CO, NOx and aerosol light absorption parameters were observed in winter than in summer. The average (71 S.D.) PM10 concentrations measured at this site were 31.5721.7 mg m 3 in winter and 15.8710.0 mg m 3 in summer. The highest PM10 concentrations were observed between 18:00 and 22:00 h CET in both campaigns, with 45.4721.0 mg m 3 for winter and 21.079.5 mg m 3 for summer. The average (71 S.D.) power law exponents of the absorption coefficients (also called absorption exponent) with l ¼ 370–950 nm, a370–950 nm were 1.670.25 in winter and 1.170.05 in summer. The calculation of a separately for lower and higher wavelengths (i.e., a370–520 nm and a660–950 nm) provided a better description of the wavelength dependence from the UV- to the near-IR region. The highest mean values of a370–520 nm and a660–950 nm were observed between 22:00 and 02:00 h CET in winter with 2.770.4 and 1.370.1, respectively. Comparison of a370–520 nm with CO and NOx data indicated that the relative contribution of wood burning versus traffic was responsible for the seasonal and diurnal variability of a. The seasonal and diurnal trends of a were not attributed to changes in the particle size since the aerosol volume size distributions (dV/d log D) were found to be similar in both campaigns.
01A - Beitrag in wissenschaftlicher Zeitschrift
Absorption of light by soot particles: determination of the absorption coefficient by means of aethalometers
(Elsevier, 10/2003) Weingartner, Ernest; Saathoff, Harald; Schnaiter, Martin; Streit, Niklaus; Bitnar, B.; Baltensperger, Urs
01A - Beitrag in wissenschaftlicher Zeitschrift
Adaptation of dry nephelometer measurements to ambient conditions at the Jungfraujoch
(American Chemical Society, 2005) Nessler, Remo; Weingartner, Ernest; Baltensperger, Urs
01A - Beitrag in wissenschaftlicher Zeitschrift
Aerosol climatology and planetary boundary influence at the Jungfraujoch analyzed by synoptic weather types
(Copernicus, 23.06.2011) Collaud Coen, Martine; Weingartner, Ernest; Furger, Markus; Nyeki, Stephan; Prévôt, André S. H.; Steinbacher, Matjaz; Baltensperger, Urs
Fourteen years of meteorological parameters, aerosol variables (absorption and scattering coef-ficients, aerosol number concentration) and trace gases (CO, NOx, SO2) measured at the Jungfraujoch (JFJ, 3580 m a.s.l.) have been analyzed as a function of different synoptic weather types. The Schüepp synoptic weather type of the Alps (SYNALP) classification from the Alpine Weather Statistics (AWS) was used to define the synoptic meteorology over the whole Swiss region. The seasonal contribution of each synoptic weather type to the aerosol concentration was deduced from the aerosol annual cycles while the planetary boundary layer (PBL) influence was estimated by means of the diurnal cycles. Since aerosols are scavenged by precipitation, the diurnal cycle of the CO concentration was also used to identify polluted air masses. SO2 and NOx concentrations were used as precursor tracers for new particle formation and growth, respectively. The aerosol optical parameters and number concentration show elevated loadings during advective weather types during the December–March period and for the convective anti-cyclonic and convective indifferent weather types during the April–September period. This study confirms the consensus view that the JFJ is mainly influenced by the free troposphere during winter and by injection of air parcels from the PBL during summer. A more detailed picture is, however, drawn where the JFJ is completely influenced by free tropospheric air masses in win-ter during advective weather types and largely influenced by the PBL also during the night in summer during the subsidence weather type. Between these two extreme situations, the PBL influence at the JFJ depends on both the time of year and the synoptic weather type. The frac-tion of PBL air transported to the JFJ was estimated by the relative increase of the specific hu-midity and CO.
01A - Beitrag in wissenschaftlicher Zeitschrift
Aerosol climatology at the high‐alpine site Jungfraujoch, Switzerland
(Wiley, 01.08.1997) Baltensperger, Urs; Gäggeler, Heinz W.; Jost, Dieter T.; Lugauer, Matthias; Schwikowski, Margit; Weingartner, Ernest; Seibert, Petra
Continuous aerosol measurements have been performed at the high-alpine site Jungfraujoch (3450 m above sea level) since 1988 by means of an epiphaniometer. The instrument, which determines the Fuchs surface area of the aerosol particles, was operated with a time resolution of 30 min. High correlation coefficients (r>0.8) were found between the epiphaniometer signal and other aerosol parameters, which could be attributed to a rather constant size distribution of the Jungfraujoch aerosol in the accumulation range (0.1
01A - Beitrag in wissenschaftlicher Zeitschrift
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, Paolo
Currently 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 Zeitschrift
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, Paolo
We 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 Zeitschrift
Aerosol nucleation and growth in a mixture of sulfuric acid/alpha-pinene oxidation products at the CERN CLOUD chamber
(AIP Publishing, 2013) Tröstl, Jasmin; Bianchi, Federico; Kürten, Andreas; Rondo, Linda; Simon, Mario; Sarnela, Nina; Jokinen, Tuija; Heinritzi, Martin; Dommen, Josef; Kirkby, Jasper; Weingartner, Ernest; Baltensperger, Urs; DeMott, Paul J.; O'Dowd, Colin D.
The role of α-pinene in aerosol nucleation and growth was investigated using the CERN CLOUD chamber, a nano scanning mobility particle sizer (nanoSMPS) and several condensation particle counters (CPCs) with different diameter cut-offs. Different oxidation conditions for α-pinene - OH⋅ vs. ozone oxidation - were considered to investigate their contributions to particle nucleation and growth. Results from the latest CERN experiment from fall 2012 (CLOUD 7) are presented.
04B - Beitrag Konferenzschrift
Aerosol partitioning between the interstitial and the condensed phase in mixed‐phase clouds
(Wiley, 13.12.2007) Verheggen, Bart; Cozic, Julie; Weingartner, Ernest; Bower, Keith; Mertes, Stephan; Connolly, Paul; Gallagher, Martin; Flynn, Michael; Choularton, Tom; Baltensperger, Urs
The partitioning of aerosol particles between the cloud and the interstitial phase (i.e., unactivated aerosol) has been investigated during several Cloud and Aerosol Characterization Experiments (CLACE‐3, CLACE‐3½ and CLACE‐4) conducted in winter and summer 2004 and winter 2005 at the high alpine research station Jungfraujoch (3580 m altitude, Switzerland). Ambient air was sampled using different inlets in order to determine the activated fraction of aerosol particles, FN, defined as the fraction of the total aerosol number concentration (with particle diameter dp > 100 nm) that has been incorporated into cloud particles. The liquid and ice water content of mixed‐phase clouds were characterized by analyzing multiple cloud probes. The dependence of the activated fraction on several environmental factors is discussed on the basis of more than 900 h of in‐cloud observations and parameterizations for key variables are given. FN is found to increase with increasing liquid water content and to decrease with increasing particle number concentration in liquid clouds. FN also decreases with increasing cloud ice mass fraction and with decreasing temperature from 0 to −25°C. The Wegener‐Bergeron‐Findeisen process probably contributed to this trend, since the presence of ice crystals causes liquid droplets to evaporate, thus releasing the formerly activated particles back into the interstitial phase. Ice nucleation could also have prevented additional cloud condensation nuclei from activating. The observed activation behavior has significant implications for our understanding of the indirect effect of aerosols on climate.
01A - Beitrag in wissenschaftlicher Zeitschrift
Aerosol partitioning in natural mixed‐phase clouds
(Wiley, 16.03.2004) Henning, Silvia; Bojinski, Stephan; Diehl, Karoline; Ghan, Steven; Nyeki, Stephan; Weingartner, Ernest; Wurzler, Sabine; Baltensperger, Urs
In situ aerosol and cloud drop microphysical measurements at a high-alpine site are used to investigate aerosol partitioning between cloud and interstitial phases in natural, mid-latitude, mixed-phase clouds. Measurements indicate a decrease in the activated aerosol fraction (FN) for particle diameters dP > 100 nm with cloud temperature from FN ~ 0.54 in summer liquid-phase clouds to FN ~ 0.08 in winter mixed-phase clouds. The latter may be attributed to the Bergeron-Findeisen mechanism whereby ice crystals grow at the expense of liquid water drops, releasing formerly activated aerosols back into the interstitial phase. This provides a means to distinguish the indirect effects of aerosols on drops and ice crystals.
01A - Beitrag in wissenschaftlicher Zeitschrift
Aerosol processing in mixed‐phase clouds in ECHAM5‐HAM. Model description and comparison to observations
(Wiley, 15.04.2008) Hoose, Corinna; Lohmann, Ulrike; Stier, Philip; Verheggen, Bart; Weingartner, Ernest
The global aerosol‐climate model ECHAM5‐HAM has been extended by an explicit treatment of cloud‐borne particles. Two additional modes for in‐droplet and in‐crystal particles are introduced, which are coupled to the number of cloud droplet and ice crystal concentrations simulated by the ECHAM5 double‐moment cloud microphysics scheme. Transfer, production, and removal of cloud‐borne aerosol number and mass by cloud droplet activation, collision scavenging, aqueous‐phase sulfate production, freezing, melting, evaporation, sublimation, and precipitation formation are taken into account. The model performance is demonstrated and validated with observations of the evolution of total and interstitial aerosol concentrations and size distributions during three different mixed‐phase cloud events at the alpine high‐altitude research station Jungfraujoch (Switzerland). Although the single‐column simulations cannot be compared one‐to‐one with the observations, the governing processes in the evolution of the cloud and aerosol parameters are captured qualitatively well. High scavenged fractions are found during the presence of liquid water, while the release of particles during the Bergeron‐Findeisen process results in low scavenged fractions after cloud glaciation. The observed coexistence of liquid and ice, which might be related to cloud heterogeneity at subgrid scales, can only be simulated in the model when assuming nonequilibrium conditions.
01A - Beitrag in wissenschaftlicher Zeitschrift
Aerosol single particle composition at the Jungfraujoch
(Elsevier, 01/2005) Hinz, Klaus-Peter; Trimborn, Achim; Weingartner, Ernest; Henning, Silvia; Baltensperger, Urs; Spengler, Bernhard
01A - Beitrag in wissenschaftlicher Zeitschrift
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, Markus
Abstract. 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