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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. - ItemNew particle formation in the Svalbard region 2006-2015(Katlenburg-Lindau : EGU, 2017) Heintzenberg, Jost; Tunved, Peter; Galí, Martí; Leck, CarolineEvents of new particle formation (NPF) were analyzed in a 10-year data set of hourly particle size distributions recorded on Mt. Zeppelin, Spitsbergen, Svalbard. Three different types of NPF events were identified through objective search algorithms. The first and simplest algorithm utilizes short-term increases in particle concentrations below 25 nm (PCT (percentiles) events). The second one builds on the growth of the sub-50 nm diameter median (DGR (diameter growth) events) and is most closely related to the classical "banana type" of event. The third and most complex, multiple-size approach to identifying NPF events builds on a hypothesis suggesting the concurrent production of polymer gel particles at several sizes below ca. 60 nm (MEV (multisize growth) events). As a first and general conclusion, we can state that NPF events are a summer phenomenon and not related to Arctic haze, which is a late winter to early spring feature. The occurrence of NPF events appears to be somewhat sensitive to the available data on precipitation. The seasonal distribution of solar flux suggests some photochemical control that may affect marine biological processes generating particle precursors and/or atmospheric photochemical processes that generate condensable vapors from precursor gases. Notably, the seasonal distribution of the biogenic methanesulfonate (MSA) follows that of the solar flux although it peaks before the maxima in NPF occurrence. A host of ancillary data and findings point to varying and rather complex marine biological source processes. The potential source regions for all types of new particle formation appear to be restricted to the marginal-ice and open-water areas between northeastern Greenland and eastern Svalbard. Depending on conditions, yet to be clarified new particle formation may become visible as short bursts of particles around 20 nm (PCT events), longer events involving condensation growth (DGR events), or extended events with elevated concentrations of particles at several sizes below 100 nm (MEV events). The seasonal distribution of NPF events peaks later than that of MSA and DGR, and in particular than that of MEV events, which reach into late summer and early fall with open, warm, and biologically active waters around Svalbard. Consequently, a simple model to describe the seasonal distribution of the total number of NPF events can be based on solar flux and sea surface temperature, representing environmental conditions for marine biological activity and condensation sink, controlling the balance between new particle nucleation and their condensational growth. Based on the sparse knowledge about the seasonal cycle of gel-forming marine microorganisms and their controlling factors, we hypothesize that the seasonal distribution of DGR and, more so, MEV events reflect the seasonal cycle of the gel-forming phytoplankton.
- ItemMercury distribution in the upper troposphere and lowermost stratosphere according to measurements by the IAGOS-CARIBIC observatory: 2014-2016(Katlenburg-Lindau : EGU, 2018) Slemr, Franz; Weigelt, Andreas; Ebinghaus, Ralf; Bieser, Johannes; Brenninkmeijer, Carl A. M.; Rauthe-Schöch, Armin; Hermann, Markus; Martinsson, Bengt G.; van Velthoven, Peter; Bönisch, Harald; Neumaier, Marco; Zahn, Andreas; Ziereis, HelmutMercury was measured onboard the IAGOS-CARIBIC passenger aircraft from May 2005 until February 2016 during near monthly sequences of mostly four intercontinental flights from Germany to destinations in North and South America, Africa and South and East Asia. Most of these mercury data were obtained using an internal default signal integration procedure of the Tekran instrument but since April 2014 more precise and accurate data were obtained using post-flight manual integration of the instrument raw signal. In this paper we use the latter data. Increased upper tropospheric total mercury (TM) concentrations due to large scale biomass burning were observed in the upper troposphere (UT) at the equator and southern latitudes during the flights to Latin America and South Africa in boreal autumn (SON) and boreal winter (DJF). TM concentrations in the lowermost stratosphere (LMS) decrease with altitude above the thermal tropopause but the gradient is less steep than reported before. Seasonal variation of the vertical TM distribution in the UT and LMS is similar to that of other trace gases with surface sources and stratospheric sinks. Speciation experiments suggest comparable TM and gaseous elementary mercury (GEM) concentrations at and below the tropopause leaving little space for Hg2+ (TM-thinsp;GEM) being the dominating component of TM here. In the stratosphere significant GEM concentrations were found to exist up to 4 km altitude above the thermal tropopause. Correlations with N2O as a reference tracer suggest stratospheric lifetimes of 72±37 and 74±27 years for TM and GEM, respectively, comparable to the stratospheric lifetime of COS. This coincidence, combined with pieces of evidence from us and other researchers, corroborates the hypothesis that Hg2+ formed by oxidation in the stratosphere attaches to sulfate particles formed mainly by oxidation of COS and is removed with them from the stratosphere by air mass exchange, gravitational sedimentation and cloud scavenging processes.
- ItemSpatial, temporal and source contribution assessments of black carbon over the northern interior of South Africa(Katlenburg-Lindau : EGU, 2017) Chiloane, Kgaugelo Euphinia; Beukes, Johan Paul; van Zyl, Pieter Gideon; Maritz, Petra; Vakkari, Ville; Josipovic, Miroslav; Venter, Andrew Derick; Jaars, Kerneels; Tiitta, Petri; Kulmala, Markku; Wiedensohler, Alfred; Liousse, Catherine; Mkhatshwa, Gabisile Vuyisile; Ramandh, Avishkar; Laakso, LauriAfter carbon dioxide (CO2), aerosol black carbon (BC) is considered to be the second most important contributor to global warming. This paper presents equivalent black carbon (eBC) (derived from an optical absorption method) data collected from three sites in the interior of South Africa where continuous measurements were conducted, i.e. Elandsfontein, Welgegund and Marikana, as well elemental carbon (EC) (determined by evolved carbon method) data at five sites where samples were collected once a month on a filter and analysed offline, i.e. Louis Trichardt, Skukuza, Vaal Triangle, Amersfoort and Botsalano. Analyses of eBC and EC spatial mass concentration patterns across the eight sites indicate that the mass concentrations in the South African interior are in general higher than what has been reported for the developed world and that different sources are likely to influence different sites. The mean eBC or EC mass concentrations for the background sites (Welgegund, Louis Trichardt, Skukuza, Botsalano) and sites influenced by industrial activities and/or nearby settlements (Elandsfontein, Marikana, Vaal Triangle and Amersfoort) ranged between 0.7 and 1.1, and 1.3 and 1.4 μg m-3, respectively. Similar seasonal patterns were observed at all three sites where continuous measurement data were collected (Elandsfontein, Marikana and Welgegund), with the highest eBC mass concentrations measured from June to October, indicating contributions from household combustion in the cold winter months (June-August), as well as savannah and grassland fires during the dry season (May to mid-October). Diurnal patterns of eBC at Elandsfontein, Marikana and Welgegund indicated maximum concentrations in the early mornings and late evenings, and minima during daytime. From the patterns it could be deduced that for Marikana and Welgegund, household combustion, as well as savannah and grassland fires, were the most significant sources, respectively. Possible contributing sources were explored in greater detail for Elandsfontein, with five main sources being identified as coal-fired power stations, pyrometallurgical smelters, traffic, household combustion, as well as savannah and grassland fires. Industries on the Mpumalanga Highveld are often blamed for all forms of pollution, due to the NO2 hotspot over this area that is attributed to NOx emissions from industries and vehicle emissions from the Johannesburg. Pretoria megacity. However, a comparison of source strengths indicated that household combustion as well as savannah and grassland fires were the most significant sources of eBC, particularly during winter and spring months, while coal-fired power stations, pyrometallurgical smelters and traffic contribute to eBC mass concentration levels year round.
- ItemAerosol activation characteristics and prediction at the central European ACTRIS research station of Melpitz, Germany(Katlenburg-Lindau : EGU, 2022) Wang, Yuan; Henning, Silvia; Poulain, Laurent; Lu, Chunsong; Stratmann, Frank; Wang, Yuying; Niu, Shengjie; Pöhlker, Mira L.; Herrmann, Hartmut; Wiedensohler, AlfredUnderstanding aerosol particle activation is essential for evaluating aerosol indirect effects (AIEs) on climate. Long-term measurements of aerosol particle activation help to understand the AIEs and narrow down the uncertainties of AIEs simulation. However, they are still scarce. In this study, more than 4 years of comprehensive aerosol measurements were utilized at the central European research station of Melpitz, Germany, to gain insight into the aerosol particle activation and provide recommendations on improving the prediction of number concentration of cloud condensation nuclei (CCN, NCCN). (1) The overall CCN activation characteristics at Melpitz are provided. As supersaturation (SS) increases from 0.1% to 0.7%, the median NCCN increases from 399 to 2144cm-3, which represents 10% to 48% of the total particle number concentration with a diameter range of 10-800nm, while the median hygroscopicity factor (κ) and critical diameter (Dc) decrease from 0.27 to 0.19 and from 176 to 54nm, respectively. (2) Aerosol particle activation is highly variable across seasons, especially at low-SS conditions. At SSCombining double low line0.1%, the median NCCN and activation ratio (AR) in winter are 1.6 and 2.3 times higher than the summer values, respectively. (3) Both κ and the mixing state are size-dependent. As the particle diameter (Dp) increases, κ increases at Dp of 1/440 to 100nm and almost stays constant at Dp of 100 to 200nm, whereas the degree of the external mixture keeps decreasing at Dp of 1/440 to 200nm. The relationships of κ vs. Dp and degree of mixing vs. Dp were both fitted well by a power-law function. (4) Size-resolved κ improves the NCCN prediction. We recommend applying the κ-Dp power-law fit for NCCN prediction at Melpitz, which performs better than using the constant κ of 0.3 and the κ derived from particle chemical compositions and much better than using the NCCN (AR) vs. SS relationships. The κ-Dp power-law fit measured at Melpitz could be applied to predict NCCN for other rural regions. For the purpose of improving the prediction of NCCN, long-term monodisperse CCN measurements are still needed to obtain the κ-Dp relationships for different regions and their seasonal variations.
- ItemA European aerosol phenomenology - 6: Scattering properties of atmospheric aerosol particles from 28 ACTRIS sites(Katlenburg-Lindau : EGU, 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, Nikos; Moerman, Marcel; Nicolas, José; O'Dowd, Colin; 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 intraannual 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.
- ItemThe EMEP Intensive Measurement Period campaign, 2008-2009: Characterizing carbonaceous aerosol at nine rural sites in Europe(Katlenburg-Lindau : EGU, 2019) Yttri, Karl Espen; Simpson, David; Bergström, Robert; Kiss, Gyula; Szidat, Sönke; Ceburnis, Darius; Eckhardt, Sabine; Hueglin, Christoph; Nøjgaard, Jacob Klenø; Perrino, Cinzia; Pisso, Ignazio; Prevot, Andre Stephan Henry; Putaud, Jean-Philippe; Spindler, Gerald; Vana, Milan; Zhang, Yan-Lin; Aas, WencheCarbonaceous aerosol (total carbon, TCp) was source apportioned at nine European rural background sites, as part of the European Measurement and Evaluation Programme (EMEP) Intensive Measurement Periods in fall 2008 and winter/spring 2009. Five predefined fractions were apportioned based on ambient measurements: elemental and organic carbon, from combustion of biomass (ECbb and OCbb) and from fossil-fuel (ECff and OCff) sources, and remaining non-fossil organic carbon (OCrnf), dominated by natural sources.OCrnf made a larger contribution to TCp than anthropogenic sources (ECbb, OCbb, ECff, and OCff) at four out of nine sites in fall, reflecting the vegetative season, whereas anthropogenic sources dominated at all but one site in winter/spring. Biomass burning (OCbb + ECbb) was the major anthropogenic source at the central European sites in fall, whereas fossil-fuel (OCff + ECff) sources dominated at the southernmost and the two northernmost sites. Residential wood burning emissions explained 30 %-50 % of TCp at most sites in the first week of sampling in fall, showing that this source can be the dominant one, even outside the heating season. In winter/spring, biomass burning was the major anthropogenic source at all but two sites, reflecting increased residential wood burning emissions in the heating season. Fossil-fuel sources dominated EC at all sites in fall, whereas there was a shift towards biomass burning for the southernmost sites in winter/spring.Model calculations based on base-case emissions (mainly officially reported national emissions) strongly underpredicted observational derived levels of OCbb and ECbb outside Scandinavia. Emissions based on a consistent bottom-up inventory for residential wood burning (and including intermediate volatility compounds, IVOCs) improved model results compared to the base-case emissions, but modeled levels were still substantially underestimated compared to observational derived OCbb and ECbb levels at the southernmost sites.Our study shows that natural sources are a major contributor to carbonaceous aerosol in Europe, even in fall and in winter/spring, and that residential wood burning emissions are equally as large as or larger than that of fossil-fuel sources, depending on season and region. The poorly constrained residential wood burning emissions for large parts of Europe show the obvious need to improve emission inventories, with harmonization of emission factors between countries likely being the most important step to improve model calculations for biomass burning emissions, and European PM2.5 concentrations in general. © Author(s) 2019.
- ItemHeterogeneous N2O5 uptake coefficient and production yield of ClNO2 in polluted northern China: Roles of aerosol water content and chemical composition(Katlenburg-Lindau : EGU, 2018) Tham, Yee Jun; Wang, Zhe; Li, Qinyi; Wang, Weihao; Wang, Xinfeng; Lu, Keding; Ma, Nan; Yan, Chao; Kecorius, Simonas; Wiedensohler, Alfred; Zhang, Yuanhang; Wang, TaoHeterogeneous uptake of dinitrogen pentoxide (N2O5) and production of nitryl chloride (ClNO2) are important nocturnal atmospheric processes that have significant implications for the production of secondary pollutants. However, the understanding of N2O5 uptake processes and ClNO2 production remains limited, especially in China. This study presents a field investigation of the N2O5 heterogeneous uptake coefficient (γ(N2O5)) and ClNO2 production yield (ϕ) in a polluted area of northern China during the summer of 2014. The N2O5 uptake coefficient and ClNO2 yield were estimated by using the simultaneously measured ClNO2 and total nitrate in 10 selected cases, which have concurrent increases in the ClNO2 and nitrate concentrations and relatively stable environmental conditions. The determined γ(N2O5) and ϕ values varied greatly, with an average of 0.022 for γ(N2O5) (±0.012, standard deviation) and 0.34 for ϕ (±0.28, standard deviation). The variations in γ(N2O5) could not be fully explained by the previously derived parameterizations of N2O5 uptake that consider nitrate, chloride, and the organic coating. Heterogeneous uptake of N2O5 was found to have a strong positive dependence on the relative humidity and aerosol water content. This result suggests that the heterogeneous uptake of N2O5 in Wangdu is governed mainly by the amount of water in the aerosol, and is strongly water limited, which is different from most of the field observations in the US and Europe. The ClNO2 yield estimated from the parameterization was also overestimated comparing to that derived from the observation. The observation-derived ϕ showed a decreasing trend with an increasing ratio of acetonitrile to carbon monoxide, an indicator of biomass burning emissions, which suggests a possible suppressive effect on the production yield of ClNO2 in the plumes influenced by biomass burning in this region. The findings of this study illustrate the need to improve our understanding and to parameterize the key factors for γ(N2O5) and ϕ to accurately assess photochemical and haze pollution.