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- ItemMeasurements of aerosol and CCN properties in the Mackenzie River delta (Canadian Arctic) during spring-summer transition in May 2014(Katlenburg-Lindau : EGU, 2018) Herenz, Paul; Wex, Heike; Henning, Silvia; Kristensen, Thomas Bjerring; Rubach, Florian; Roth, Anja; Borrmann, Stephan; Bozem, Heiko; Schulz, Hannes; Stratmann, FrankWithin the framework of the RACEPAC (Radiation-Aerosol-Cloud Experiment in the Arctic Circle) project, the Arctic aerosol, arriving at a ground-based station in Tuktoyaktuk (Mackenzie River delta area, Canada), was characterized during a period of 3 weeks in May 2014. Basic meteorological parameters and particle number size distributions (PNSDs) were observed and two distinct types of air masses were found. One type were typical Arctic haze air masses, termed accumulation-type air masses, characterized by a monomodal PNSD with a pronounced accumulation mode at sizes above 100 nm. These air masses were observed during a period when back trajectories indicate an air mass origin in the north-east of Canada. The other air mass type is characterized by a bimodal PNSD with a clear minimum around 90ĝ€†nm and with an Aitken mode consisting of freshly formed aerosol particles. Back trajectories indicate that these air masses, termed Aitken-type air masses, originated from the North Pacific. In addition, the application of the PSCF receptor model shows that air masses with their origin in active fire areas in central Canada and Siberia, in areas of industrial anthropogenic pollution (Norilsk and Prudhoe Bay Oil Field) and the north-west Pacific have enhanced total particle number concentrations (N CN). Generally, N CN ranged from 20 to 500 cmg'3, while cloud condensation nuclei (CCN) number concentrations were found to cover a range from less than 10 up to 250 cmg'3 for a supersaturation (SS) between 0.1 and 0.7 %. The hygroscopicity parameter of the CCN was determined to be 0.23 on average and variations in were largely attributed to measurement uncertainties.
Furthermore, simultaneous PNSD measurements at the ground station and on the Polar 6 research aircraft were performed. We found a good agreement of ground-based PNSDs with those measured between 200 and 1200 m. During two of the four overflights, particle number concentrations at 3000 m were found to be up to 20 times higher than those measured below 2000 m; for one of these two flights, PNSDs measured above 2000 m showed a different shape than those measured at lower altitudes. This is indicative of long-range transport from lower latitudes into the Arctic that can advect aerosol from different regions in different heights. - ItemNumber size distributions and seasonality of submicron particles in Europe 2008–2009(München : European Geopyhsical Union, 2011) Asmi, A.; Wiedensohler, A.; Laj, P.; Fjaeraa, A.-M.; Sellegri, K.; Birmili, W.; Weingartner, E.; Baltensperger, U.; Zdimal, V.; Zikova, N.; Putaud, J.-P.; Marinoni, A.; Tunved, P.; Hansson, H.-C.; Fiebig, M.; Kivekäs, N.; Lihavainen, H.; Asmi, E.; Ulevicius, V.; Aalto, P.P.; Swietlicki, E.; Kristensson, A.; Mihalopoulos, N.; Kalivitis, N.; Kalapov, I.; Kiss, G.; de Leeuw, G.; Henzing, B.; Harrison, R.M.; Beddows, D.; O'Dowd, C.; Jennings, S.G.; Flentje, H.; Weinhold, K.; Meinhardt, F.; Ries, L.; Kulmala, M.Two years of harmonized aerosol number size distribution data from 24 European field monitoring sites have been analysed. The results give a comprehensive overview of the European near surface aerosol particle number concentrations and number size distributions between 30 and 500 nm of dry particle diameter. Spatial and temporal distribution of aerosols in the particle sizes most important for climate applications are presented. We also analyse the annual, weekly and diurnal cycles of the aerosol number concentrations, provide log-normal fitting parameters for median number size distributions, and give guidance notes for data users. Emphasis is placed on the usability of results within the aerosol modelling community. We also show that the aerosol number concentrations of Aitken and accumulation mode particles (with 100 nm dry diameter as a cut-off between modes) are related, although there is significant variation in the ratios of the modal number concentrations. Different aerosol and station types are distinguished from this data and this methodology has potential for further categorization of stations aerosol number size distribution types. The European submicron aerosol was divided into characteristic types: Central European aerosol, characterized by single mode median size distributions, unimodal number concentration histograms and low variability in CCN-sized aerosol number concentrations; Nordic aerosol with low number concentrations, although showing pronounced seasonal variation of especially Aitken mode particles; Mountain sites (altitude over 1000 m a.s.l.) with a strong seasonal cycle in aerosol number concentrations, high variability, and very low median number concentrations. Southern and Western European regions had fewer stations, which decreases the regional coverage of these results. Aerosol number concentrations over the Britain and Ireland had very high variance and there are indications of mixed air masses from several source regions; the Mediterranean aerosol exhibit high seasonality, and a strong accumulation mode in the summer. The greatest concentrations were observed at the Ispra station in Northern Italy with high accumulation mode number concentrations in the winter. The aerosol number concentrations at the Arctic station Zeppelin in Ny-\AA lesund in Svalbard have also a strong seasonal cycle, with greater concentrations of accumulation mode particles in winter, and dominating summer Aitken mode indicating more recently formed particles. Observed particles did not show any statistically significant regional work-week or weekday related variation in number concentrations studied. Analysis products are made for open-access to the research community, available in a freely accessible internet site. The results give to the modelling community a reliable, easy-to-use and freely available comparison dataset of aerosol size distributions.
- ItemOn the sub-micron aerosol size distribution in a coastal-rural site at El Arenosillo Station (SW – Spain)(München : European Geopyhsical Union, 2011) Sorribas, M.; de la Morena, B.A.; Wehner, B.; López, J.F.; Prats, N.; Mogo, S.; Wiedensohler, A.; Cachorro, V.E.This study focuses on the analysis of the sub-micron aerosol characteristics at El Arenosillo Station, a rural and coastal environment in South-western Spain between 1 August 2004 and 31 July 2006 (594 days). The mean total concentration (NT) was 8660 cm−3 and the mean concentrations in the nucleation (NNUC), Aitken (NAIT) and accumulation (NACC) particle size ranges were 2830 cm−3, 4110 cm−3 and 1720 cm−3, respectively. Median size distribution was characterised by a single-modal fit, with a geometric diameter, median number concentration and geometric standard deviation of 60 nm, 5390 cm−3 and 2.31, respectively. Characterisation of primary emissions, secondary particle formation, changes to meteorology and long-term transport has been necessary to understand the seasonal and annual variability of the total and modal particle concentration. Number concentrations exhibited a diurnal pattern with maximum concentrations around noon. This was governed by the concentrations of the nucleation and Aitken modes during the warm seasons and only by the nucleation mode during the cold seasons. Similar monthly mean total concentrations were observed throughout the year due to a clear inverse variation between the monthly mean NNUC and NACC. It was related to the impact of desert dust and continental air masses on the monthly mean particle levels. These air masses were associated with high values of NACC which suppressed the new particle formation (decreasing NNUC). Each day was classified according to a land breeze flow or a synoptic pattern influence. The median size distribution for desert dust and continental aerosol was dominated by the Aitken and accumulation modes, and marine air masses were dominated by the nucleation and Aitken modes. Particles moved offshore due to the land breeze and had an impact on the particle burden at noon, especially when the wind was blowing from the NW sector in the morning during summer time. This increased NNUC and NAIT by factors of 3.1 and 2.4, respectively. Nucleation events with the typical "banana" shape were characterised by a mean particle nucleation rate of 0.74 cm−3 s−1, a mean growth rate of 1.96 nm h−1 and a mean total duration of 9.25 h (starting at 10:55 GMT and ending at 20:10 GMT). They were observed for 48 days. Other nucleation events were identified as those produced by the emissions from the industrial areas located at a distance of 35 km. They were observed for 42 days. Both nucleation events were strongly linked to the marine air mass origin.
- ItemOne year of Raman lidar observations of free-tropospheric aerosol layers over South Africa(München : European Geopyhsical Union, 2015) Giannakaki, E.; Pfüller, A.; Korhonen, K.; Mielonen, T.; Laakso, L.; Vakkari, V.; Baars, H.; Engelmann, R.; Beukes, J.P.; Van Zyl, P.G.; Josipovic, M.; Tiitta, P.; Chiloane, K.; Piketh, S.; Lihavainen, H.; Lehtinen, K.E.J.; Komppula, M.Raman lidar data obtained over a 1 year period has been analysed in relation to aerosol layers in the free troposphere over the Highveld in South Africa. In total, 375 layers were observed above the boundary layer during the period 30 January 2010 to 31 January 2011. The seasonal behaviour of aerosol layer geometrical characteristics, as well as intensive and extensive optical properties were studied. The highest centre heights of free-tropospheric layers were observed during the South African spring (2520 ± 970 m a.g.l., also elsewhere). The geometrical layer depth was found to be maximum during spring, while it did not show any significant difference for the rest of the seasons. The variability of the analysed intensive and extensive optical properties was high during all seasons. Layers were observed at a mean centre height of 2100 ± 1000 m with an average lidar ratio of 67 ± 25 sr (mean value with 1 standard deviation) at 355 nm and a mean extinction-related Ångström exponent of 1.9 ± 0.8 between 355 and 532 nm during the period under study. Except for the intensive biomass burning period from August to October, the lidar ratios and Ångström exponents are within the range of previous observations for urban/industrial aerosols. During Southern Hemispheric spring, the biomass burning activity is clearly reflected in the optical properties of the observed free-tropospheric layers. Specifically, lidar ratios at 355 nm were 89 ± 21, 57 ± 20, 59 ± 22 and 65 ± 23 sr during spring (September–November), summer (December–February), autumn (March–May) and winter (June–August), respectively. The extinction-related Ångström exponents between 355 and 532 nm measured during spring, summer, autumn and winter were 1.8 ± 0.6, 2.4 ± 0.9, 1.8 ± 0.9 and 1.8 ± 0.6, respectively. The mean columnar aerosol optical depth (AOD) obtained from lidar measurements was found to be 0.46 ± 0.35 at 355 nm and 0.25 ± 0.2 at 532 nm. The contribution of free-tropospheric aerosols on the AOD had a wide range of values with a mean contribution of 46%.
- ItemTechnical Note: One year of Raman-lidar measurements in Gual Pahari EUCAARI site close to New Delhi in India – Seasonal characteristics of the aerosol vertical structure(München : European Geopyhsical Union, 2012) Komppula, M.; Mielonen, T.; Arola, A.; Korhonen, K.; Lihavainen, H.; Hyvärinen, A.-P.; Baars, H.; Engelmann, R.; Althausen, D.; Ansmann, A.; Müller, D.; Panwar, T.S.; Hooda, R.K.; Sharma, V.P.; Kerminen, V.-M.; Lehtinen, K.E.J.; Viisanen, Y.One year of multi-wavelength (3 backscatter + 2 extinction + 1 depolarization) Raman lidar measurements at Gual Pahari, close to New Delhi, were analysed. The data was split into four seasons: spring (March–May), summer (June–August), autumn (September–November) and winter (December–February). The vertical profiles of backscatter, extinction, and lidar ratio and their variability during each season are presented. The measurements revealed that, on average, the aerosol layer was at its highest in spring (5.5 km). In summer, the vertically averaged (between 1–3 km) backscatter and extinction coefficients had the highest averages (3.3 Mm−1 sr−1 and 142 Mm−1 at 532 nm, respectively). Aerosol concentrations were slightly higher in summer compared to other seasons, and particles were larger in size. The autumn showed the highest lidar ratio and high extinction-related Ångström exponents (AEext), indicating the presence of smaller probably absorbing particles. The winter had the lowest backscatter and extinction coefficients, but AEext was the highest, suggesting still a large amount of small particles.
- ItemAerosol particle number size distributions and particulate light absorption at the ZOTTO tall tower (Siberia), 2006–2009(München : European Geopyhsical Union, 2011) Heintzenberg, J.; Birmili, W.; Otto, R.; Andreae, M.O.; Mayer, J.-C.; Chi, X.; Panov, A.This paper analyses aerosol particle number size distributions, particulate absorption at 570 nm wavelength and carbon monoxide (CO) measured between September 2006 and January 2010 at heights of 50 and 300 m at the Zotino Tall Tower Facility (ZOTTO) in Siberia (60.8° N; 89.35° E). Average number, surface and volume concentrations are broadly comparable to former studies covering shorter observation periods. Fits of multiple lognormal distributions yielded three maxima in probability distribution of geometric mean diameters in the Aitken and accumulation size range and a possible secondary maximum in the nucleation size range below 25 nm. The seasonal cycle of particulate absorption shows maximum concentrations in high winter (December) and minimum concentrations in mid-summer (July). The 90th percentile, however, indicates a secondary maximum in July/August that is likely related to forest fires. The strongly combustion derived CO shows a single winter maximum and a late summer minimum, albeit with a considerably smaller seasonal swing than the particle data due to its longer atmospheric lifetime. Total volume and even more so total number show a more complex seasonal variation with maxima in winter, spring, and summer. A cluster analysis of back trajectories and vertical profiles of the pseudo-potential temperature yielded ten clusters with three levels of particle number concentration: Low concentrations in Arctic air masses (400–500 cm−3), mid-level concentrations for zonally advected air masses from westerly directions between 55° and 65° N (600–800 cm−3), and high concentrations for air masses advected from the belt of industrial and population centers in Siberia and Kazakhstan (1200 cm−3). The observational data is representative for large parts of the troposphere over Siberia and might be particularly useful for the validation of global aerosol transport models.
- ItemVariability in the mass absorption cross section of black carbon (BC) aerosols is driven by BC internal mixing state at a central European background site (Melpitz, Germany) in winter(Katlenburg-Lindau : European Geosciences Union, 2021) Yuan, Jinfeng; Modini, Robin Lewis; Zanatta, Marco; Herber, Andreas B.; Müller, Thomas; Wehner, Birgit; Poulain, Laurent; Tuch, Thomas; Baltensperger, Urs; Gysel-Beer, MartinProperties of atmospheric black carbon (BC) particles were characterized during a field experiment at a rural background site (Melpitz, Germany) in February 2017. BC absorption at a wavelength of 870 nm was measured by a photoacoustic extinctiometer, and BC physical properties (BC mass concentration, core size distribution and coating thickness) were measured by a single-particle soot photometer (SP2). Additionally, a catalytic stripper was used to intermittently remove BC coatings by alternating between ambient and thermo-denuded conditions. From these data the mass absorption cross section of BC (MACBC) and its enhancement factor (EMAC) were inferred for essentially waterfree aerosol as present after drying to low relative humidity (RH). Two methods were applied independently to investigate the coating effect on EMAC: A correlation method (MACBC; ambient vs. BC coating thickness) and a denuding method (MACBC; ambient vs. MACBC; denuded). Observed EMAC values varied from 1.0 to 1.6 (lower limit from denuding method) or 1:2 to 1.9 (higher limit from correlation method), with the mean coating volume fraction ranging from 54% to 78% in the dominating mass equivalent BC core diameter range of 200?220 nm.MACBC and EMAC were strongly correlated with coating thickness of BC. By contrast, other potential drivers of EMAC variability, such as different BC sources (air mass origin and absorption Angström exponent), coating composition (ratio of inorganics to organics) and BC core size distribution, had only minor effects. These results for ambient BC measured at Melpitz during winter show that the lensing effect caused by coatings on BC is the main driver of the variations in MACBC and EMAC, while changes in other BC particle properties such as source, BC core size or coating composition play only minor roles at this rural background site with a large fraction of aged particles. Indirect evidence suggests that potential dampening of the lensing effect due to unfavorable morphology was most likely small or even negligible.
- ItemAerosol dynamics and dispersion of radioactive particles(Katlenburg-Lindau : European Geosciences Union, 2021) Schoenberg, Pontus von; Tunved, Peter; Grahn, Håkan; Wiedensohler, Alfred; Krejci, Radovan; Brännström, NiklasIn the event of a failure of a nuclear power plant with release of radioactive material into the atmosphere, dispersion modelling is used to understand how the released radioactivity is spread. For the dispersion of particles, Lagrangian particle dispersion models (LPDMs) are commonly used, in which model particles, representing the released material, are transported through the atmosphere. These model particles are usually inert and undergo only first-order processes such as dry deposition and simplified wet deposition along the path through the atmosphere. Aerosol dynamic processes including coagulation, condensational growth, chemical interactions, formation of new particles and interaction with new aerosol sources are usually neglected in such models. The objective of this study is to analyse the impact of these advanced aerosol dynamic processes if they were to be included in LPDM simulations for use in radioactive preparedness. In this investigation, a fictitious failure of a nuclear power plant is studied for three geographically and atmospherically different sites. The incident was simulated with a Lagrangian single-trajectory box model with a new simulation for each hour throughout a year to capture seasonal variability of meteorology and variation in the ambient aerosol. (a) We conclude that modelling of wet deposition by incorporating an advanced cloud parameterization is advisable, since it significantly influence simulated levels of airborne and deposited activity including radioactive hotspots, and (b) we show that inclusion of detailed ambient-aerosol dynamics can play a large role in the model result in simulations that adopt a more detailed representation of aerosol–cloud interactions. The results highlight a potential necessity for implementation of more detailed representation of general aerosol dynamic processes into LPDMs in order to cover the full range of possible environmental characteristics that can apply during a release of radionuclides into the atmosphere.
- ItemThe Smithsonian solar constant data revisited: No evidence for a strong effect of solar activity in ground-based insolation data(Göttingen : Copernicus GmbH, 2011) Feulner, G.Apparent evidence for a strong signature of solar activity in ground-based insolation data was recently reported. In particular, a strong increase of the irradiance of the direct solar beam with sunspot number as well as a decline of the brightness of the solar aureole and the measured precipitable water content of the atmosphere with solar activity were presented. The latter effect was interpreted as evidence for cosmic-ray-induced aerosol formation. Here I show that these spurious results are due to a failure to correct for seasonal variations and the effects of volcanic eruptions and local pollution in the data. After correcting for these biases, neither the atmospheric water content nor the brightness of the solar aureole show any significant change with solar activity, and the variations of the solar-beam irradiance with sunspot number are in agreement with previous estimates. Hence there is no evidence for the influence of solar activity on the climate being stronger than currently thought.
- ItemOrganic aerosol source apportionment by offline-AMS over a full year in Marseille(Katlenburg-Lindau : EGU, 2017) Bozzetti, Carlo; El Haddad, Imad; Salameh, Dalia; Daellenbach, Kaspar Rudolf; Fermo, Paola; Gonzalez, Raquel; Minguillón, María Cruz; Iinuma, Yoshiteru; Poulain, Laurent; Elser, Miriam; Müller, Emanuel; Slowik, Jay Gates; Jaffrezo, Jean-Luc; Baltensperger, Urs; Marchand, Nicolas; Prévôt, André Stephan HenryWe investigated the seasonal trends of OA sources affecting the air quality of Marseille (France), which is the largest harbor of the Mediterranean Sea. This was achieved by measurements of nebulized filter extracts using an aerosol mass spectrometer (offline-AMS). In total 216 PM2.5 (particulate matter with an aerodynamic diameter < 2.5 μm) filter samples were collected over 1 year from August 2011 to July 2012. These filters were used to create 54 composite samples which were analyzed by offline-AMS. The same samples were also analyzed for major water-soluble ions, metals, elemental and organic carbon (EC/OC), and organic markers, including n-alkanes, hopanes, polycyclic aromatic hydrocarbons (PAHs), lignin and cellulose pyrolysis products, and nitrocatechols. The application of positive matrix factorization (PMF) to the water-soluble AMS spectra enabled the extraction of five factors, related to hydrocarbon-like OA (HOA), cooking OA (COA), biomass burning OA (BBOA), oxygenated OA (OOA), and an industry-related OA (INDOA). Seasonal trends and relative contributions of OA sources were compared with the source apportionment of OA spectra collected from the AMS field deployment at the same station but in different years and for shorter monitoring periods (February 2011 and July 2008). Online- and offline-AMS source apportionment revealed comparable seasonal contribution of the different OA sources. Results revealed that BBOA was the dominant source during winter, representing on average 48 % of the OA, while during summer the main OA component was OOA (63 % of OA mass on average). HOA related to traffic emissions contributed on a yearly average 17 % to the OA mass, while COA was a minor source contributing 4 %. The contribution of INDOA was enhanced during winter (17 % during winter and 11 % during summer), consistent with an increased contribution from light alkanes, light PAHs (fluoranthene, pyrene, phenanthrene), and selenium, which is commonly considered as a unique coal combustion and coke production marker. Online- and offline-AMS source apportionments revealed evolving levoglucosan : BBOA ratios, which were higher during late autumn and March. A similar seasonality was observed in the ratios of cellulose combustion markers to lignin combustion markers, highlighting the contribution from cellulose-rich biomass combustion, possibly related to agricultural activities.