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- ItemVariability of sub-micrometer particle number size distributions and concentrations in the Western Mediterranean regional background(Milton Park : Taylor & Francis, 2013) Cusack, Michael; Pérez, NoemÍ; Pey, Jorge; Wiedensohler, Alfred; Alastuey, AndrésThis study focuses on the daily and seasonal variability of particle number size distributions and concentrations, performed at the Montseny (MSY) regional background station in the western Mediterranean from October 2010 to June 2011. Particle number concentrations at MSY were shown to be within range of various other sites across Europe reported in literature, but the seasonality of the particle number size distributions revealed significant differences. The Aitken mode is the dominant particle mode at MSY, with arithmetic mean concentrations of 1698 cm3, followed by the accumulation mode (877 cm3) and the nucleation mode (246 cm3). Concentrations showed a strong seasonal variability with large increases in particle number concentrations observed from the colder to warmer months. The modality of median size distributions was typically bimodal, except under polluted conditions when the size distribution was unimodal. During the colder months, the daily variation of particle number size distributions are strongly influenced by a diurnal breeze system, whereby the Aitken and accumulation modes vary similarly to PM1 and BC mass concentrations, with nocturnal minima and sharp day-time increases owing to the development of a diurnal mountain breeze. Under clean air conditions, high levels of nucleation and lower Aitken mode concentrations were measured, highlighting the importance of new particle formation as a source of particles in the absence of a significant condensation sink. During the warmer months, nucleation mode concentrations were observed to be relatively elevated both under polluted and clean conditions due to increased photochemical reactions, with enhanced subsequent growth owing to elevated concentrations of condensable organic vapours produced from biogenic volatile organic compounds, indicating that nucleation at MSY does not exclusively occur under clean air conditions. Finally, mixing of air masses between polluted and non-polluted boundary layer air, and brief changes in the air mass being sampled gave rise to unusual particle number size distributions, with specific cases of such behaviour discussed at length.
- ItemIn situ measurements of optical properties at Tinfou (Morocco) during the Saharan Mineral Dust Experiment SAMUM 2006(Milton Park : Taylor & Francis, 2017) Schladitz, A.; Müller, T.; Kaaden, N.; Massling, A.; Kandler, K.; Ebert, M.; Weinbruch, S.; Deutscher, C.; Wiedensohler, A.In situ measurements of optical and physical properties of mineral dust were performed at the outskirts of the Saharan Desert in the framework of the Saharan Mineral Dust Experiment part 1 (SAMUM-1). Goals of the field study were to achieve information on the extent and composition of the dust particle size distribution and the optical properties of dust at the ground. For the particle number size distribution, measured with a DMPS/APS, a size dependent dynamic shape factor was considered. The mean refractive index of the particles in this field study is 1.53–4.1 × 10-3i at 537 nm wavelength and 1.53–3.1 × 10-3i at 637 nm wavelength derived from measurements of scattering and absorption coefficients, as well as the particle size distribution. Whereas the real part of the refractive index is rather constant, the imaginary part varies depending on the mineral dust concentrations. For high dust concentration the single scattering albedo is primarily influenced by iron oxide and is 0.96 ± 0.02 and 0.98 ± 0.01 at 537 nm and 637 nm wavelength, respectively. During low dust concentration the single scattering albedo is more influenced by a soot-type absorber and is 0.89 ± 0.02 and 0.93 ± 0.01 for the same wavelengths.
- ItemOccurrence of an ultrafine particle mode less than 20 nm in diameter in the marine boundary layer during Arctic summer and autumn(Milton Park : Taylor & Francis, 2017) Wiedensohler, Alfred; Covert, David S.; Swietlicki, Erik; Aalto, Pasi; Heintzenberg, Jost; Leck, CarolineThe International Arctic Ocean Expedition 1991 (IAOE-91) provided a platform to study the occurrence and size distributions of ultrafine particles in the marine boundary layer (MBL) during Arctic summer and autumn. Measurements of both aerosol physics, and gas/particulate chemistry were taken aboard the Swedish icebreaker Oden. Three separate submicron aerosol modes were found: an ultrafine mode (Dp < 20 nm), the Aitken mode (20 < Dp < 100 nm), and the accumulation mode (Dp > 100 nm). We evaluated correlations between ultrafine particle number concentrations and mean diameter with the entire measured physical, chemical, and meteorological data set. Multivariate statistical methods were then used to make these comparisons. A principal component (PC) analysis indicated that the observed variation in the data could be explained by the influence from several types of air masses. These were characterised by contributions from the open sea or sources from the surrounding continents and islands. A partial least square (PLS) regression of the ultrafine particle concentration was also used. These results implied that the ultrafine particles were produced above or in upper layers of the MBL and mixed downwards. There were also indications that the open sea acted as a source of the precursors for ultrafine particle production. No anti-correlation was found between the ultrafine and accumulation particle number concentrations, thus indicating that the sources were in separate air masses.
- ItemOverview of the atmospheric research program during the International Arctic Ocean Expedition of 1991 (IAOE-91) and its scientific results(Milton Park : Taylor & Francis, 2017) Leck, C.; Bigg, E.K.; Covert, D.S.; Heintzenberg, J.; Maenhaut, W.; Nilsson, E.D.; Wiedensohler, A.The broad aim of the Atmospheric program of the International Arctic Ocean Expedition (IAOE-91) was to test the hypothesis that marine biogenically produced dimethyl sulfide (DMS) gas can exert a significant global climatic control. The hypothesis states that DMS is transferred to the atmosphere and is oxidised to form airborne particles. Some of these grow large enough to act as cloud condensation nuclei (CCN) which help determine cloud droplet concentration. The latter has a strong influence on cloud albedo and hence on the radiation balance of the area affected. In summer, the central Arctic is a specially favourable region for studying the natural sulfur cycle in that the open waters surrounding the pack ice are the only significant sources of DMS and there are almost no anthropogenic particle sources. Concentrations of seawater and atmospheric DMS decreased at about the same rate during the period of measurements, (1 August to 6 October, latitudes 75°N to 90°N) spanning about three orders of magnitude. Methane sulfonate and nonsea salt sulfate in the submicrometer particles, which may be derived from atmospheric DMS, also decreased similarly, suggesting that the first part of the hypothesis under test was true. Influences on cloud droplet concentration and radiation balance could not be measured. Size-resolved aerosol chemistry showed a much lower proportion of methane sulfonate to be associated with supermicrometer particles than has been found elsewhere. Its molar ratio to nonsea salt sulfate suggested that the processes controlling the particulate chemistry do not exhibit a net temperature dependence. Elemental analysis of the aerosol also revealed the interesting possibility that debris from Siberian rivers transported on the moving ice represent a fairly widespread source of supermicrometer crustal material within the pack ice. Highly resolved measurements of aerosol number size distributions were made in the diameter range 3 nm to 500 nm. 3 distinct modal sizes were usually present, the “ultrafine”, “Aitken” and “accumulation” modes centred on 14, 45 and 170 nm diameter, respectively. The presence of ultrafine particles, implying recent production, was more frequent than has been found in lower latitude remote marine areas. Evidence suggests that they were mixed to the surface from higher levels. Sudden and often drastic changes in aerosol concentration and size distribution were surprisingly frequent in view of the relatively slowly changing meteorology of the central Arctic during the study period and the absence of strong pollution sources. They were most common in particles likely to have taken part in cloud formation (> 80 nm diameter). 2 factors appear to have been involved in these sudden changes. The 1st was the formation of vertical gradients in aerosol concentration due to interactions between particles and clouds or favoured regions for new particle production during periods of stability. The 2nd was sporadic localised breakdowns of the stability, bringing changed particle concentrations to the measurement level. Probable reasons for these sporadic mixing events were indicated by the structure of the Marine Boundary Layer (MBL) investigated with high resolution rawinsondes. Low level jets were present about 60% of the time, producing conditions conductive to turbulence and shear-induced waves. It is concluded that an even more detailed study of meteorological processes in the MBL in conjunction with more highly time-resolved measurements of gas-aerosol physics and chemistry appears to be essential in any future research aimed at studying the indirect, cloud mediated, effect of aerosol particles.
- ItemGlobal-scale atmosphere monitoring by in-service aircraft – current achievements and future prospects of the European Research Infrastructure IAGOS(Milton Park : Taylor & Francis, 2015) Petzold, Andreas; Thouret, Valerie; Gerbig, Christoph; Zahn, Andreas; Brenninkmeijer, Carl A.M.; Gallagher, Martin; Hermann, Markus; Pontaud, Marc; Ziereis, Helmut; Boulanger, Damien; Marshall, Julia; Nédélec, Philippe; Smit, Herman G.J.; Friess, Udo; Flaud, Jean-Marie; Wahner, Andreas; Cammas, Jean-Pierre; Volz-Thomas, AndreasThe European Research Infrastructure IAGOS (In-service Aircraft for a Global Observing System) operates a global-scale monitoring system for atmospheric trace gases, aerosols and clouds utilising the existing global civil aircraft. This new monitoring infrastructure builds on the heritage of the former research projects MOZAIC (Measurement of Ozone and Water Vapour on Airbus In-service Aircraft) and CARIBIC (Civil Aircraft for the Regular Investigation of the Atmosphere Based on an Instrument Container). CARIBIC continues within IAGOS and acts as an important airborne measurement reference standard within the wider IAGOS fleet. IAGOS is a major contributor to the in-situ component of the Copernicus Atmosphere Monitoring Service (CAMS), the successor to the Global Monitoring for the Environment and Security – Atmospheric Service, and is providing data for users in science, weather services and atmospherically relevant policy. IAGOS is unique in collecting regular in-situ observations of reactive gases, greenhouse gases and aerosol concentrations in the upper troposphere and lowermost stratosphere (UTLS) at high spatial resolution. It also provides routine vertical profiles of these species in the troposphere over continental sites or regions, many of which are undersampled by other networks or sampling studies, particularly in Africa, Southeast Asia and South America. In combination with MOZAIC and CARIBIC, IAGOS has provided long-term observations of atmospheric chemical composition in the UTLS since 1994. The longest time series are 20 yr of temperature, H2O and O3, and 9–15 yr of aerosols, CO, NO y , CO2, CH4, N2O, SF6, Hg, acetone, ~30 HFCs and ~20 non-methane hydrocarbons. Among the scientific highlights which have emerged from these data sets are observations of extreme concentrations of O3 and CO over the Pacific basin that have never or rarely been recorded over the Atlantic region for the past 12 yr; detailed information on the temporal and regional distributions of O3, CO, H2O, NO y and aerosol particles in the UTLS, including the impacts of cross-tropopause transport, deep convection and lightning on the distribution of these species; characterisation of ice-supersaturated regions in the UTLS; and finally, improved understanding of the spatial distribution of upper tropospheric humidity including the finding that the UTLS is much more humid than previously assumed.
- ItemElectron microscopy of particles collected at Praia, Cape Verde, during the Saharan Mineral Dust Experiment: Particle chemistry, shape, mixing state and complex refractive index(Milton Park : Taylor & Francis, 2017) Kandler, K.; Lieke, K.; Benker, N.; Emmel, C.; Küpper, M.; Müller-Ebert, D.; Ebert, M.; Scheuvens, D.; Schladitz, A.; Schütz, L.; Weinbruch, S.A large field experiment of the Saharan Mineral Dust Experiment (SAMUM) was performed in Praia, Cape Verde, in January and February 2008. The aerosol at Praia is a superposition of mineral dust, sea-salt, sulphates and soot. Particles smaller than 500 nm are mainly mineral dust, mineral dust–sulphate mixtures, sulphates and soot–sulphate mixtures. Particles larger then 2.5μm consist of mineral dust, sea-salt and few mineral dust–sulphate mixtures. A transition range exists in between. The major internal mixtures are mineral dust–sulphate and soot–sulphate. Mineral dust–sea-salt mixtures occur occasionally, mineral dust–soot mixtures were not observed. The aspect ratio was 1.3–1.4 for dry particles smaller than 500 nm and 1.6–1.7 for larger ones. Parameterizations are given for dry and humid state. Although the real part of the refractive index showed low variation (1.55–1.58 at 532 nm), a multi-modal imaginary part was detected as function of particle size, reflecting the complex composition. Soot mainly influences the absorption for wavelengths longer than the haematite absorption edge, whereas for shorter wavelengths dust is dominating. The refractive index of the aerosol depends on the source region of the mineral dust and on the presence/absence of a marine component.
- ItemMicrophysical and optical properties of dust and tropical biomass burning aerosol layers in the Cape Verde region - an overview of the airborne in situ and lidar measurements during SAMUM-2(Milton Park : Taylor & Francis, 2017) Weinzierl, Bernadett; Sauer, Daniel; Esselborn, Michael; Petzold, Andreas; Veira, Andreas; Rose, Maximilian; Mund, Susanne; Wirth, Martin; Ansmann, Albert; Tesche, Matthias; Gross, Silke; Freudenthaler, VolkerIn the framework of the Saharan Mineral Dust Experiment (SAMUM) airborne High Spectral Resolution Lidar and in situ measurements of the particle size, aerosol mixing state and absorption coefficient were conducted. Here, the properties of mineral dust and tropical biomass burning layers in the Cape Verde region in January/February 2008 are investigated and compared with the properties of fresh dust observed in May/June 2006 close the Sahara. In the Cape Verde area, we found a complex stratification with dust layers covering the altitude range below 2 km and biomass burning layers aloft. The aerosol type of the individual layers was classified based on depolarization and lidar ratios and, in addition, on in situ measured Ångström exponents of absorption åap. The dust layers had a depth of 1.3 ± 0.4 km and showed a median åap of 3.95. The median effective diameter Deff was 2.5 μm and the dust layers over Cape Verde yielded clear signals of aging: large particles were depleted due to gravitational settling and the accumulation mode diameter was shifted towards larger sizes as a result of coagulation. The tropical biomass layers had a depth of 2.0 ± 1.1 km and were characterized by a median åap of 1.34. They always contained a certain amount of large dust particles and showed a median Deff of 1.1 μm and a fine mode Deff,fine of 0.33. The dust and biomass burning layers had a median aerosol optical depth (AOD) of 0.23 and 0.09, respectively. The median contributions to the AOD of the total atmospheric column below 10 km were 75 and 37%, respectively.
- ItemTrends in the composition of wet deposition: Effects of the atmospheric rehabilitation in East-Germany(Milton Park : Taylor & Francis, 2017) Marquardt, Wolfgang; Brüggemann, Erika; Ihle, PeterThe chemical components in precipitation largely depend on type and quantity of emissions on the course of the air masses at the sampling site. Beginning in 1982, the concentrations of major ions in precipitation at initially 3 sites are described in total as well as arrival sectors. For regions with specific geographical or emission features, 5 to 7 sectors for every sampling site are established, e.g., Scandinavia, or the centres of brown coal combustion in the former GDR. Particulary from the sectors of the former GDR, the precipitation was over-averaged contaminated anthropogenically in the years before the political change. Some components were significantly raised in comparison to other sectors. However, acidity remained on the level of the other sectors in the 80 s. In the early 90s, anthropogenic emissions were systematically reduced partly by substitution of brown coal of inferior quality, better flue gas cleaning and partly by closing down industries. The effect of such steps on the wet deposition is being studied in a national German SANA research project (SANA: scientific program of rehabilitation of the atmosphere). In this project, the sampling sites were extended to 7 while maintaining the sampling procedure and the recording of relevant meteorological input-data. As a result, there now exists a homogeneous long-term data base allowing us to study the effects of emissions on wet deposition by the rehabilitation of the atmosphere in the former GDR. The paper focusses on changes in sulphate, nitrate, calcium, acidity, chloride and potassium concentrations in precipitation at the 3 so-called long-term sites. There are conspicuous decreases of some ions on one hand, but there is also an increase of nitrate and acidity, especially in recent years.
- ItemSources of increase in lowermost stratospheric sulphurous and carbonaceous aerosol background concentrations during 1999–2008 derived from CARIBIC flights(Milton Park : Taylor & Francis, 2014) Friberg, Johan; Martinsson, Bengt G.; Andersson, Sandra M.; Brenninkmeijer, Carl A.M.; Hermann, Markus; Van Velthoven, Peter F.J.; Zahn, AndreasThis study focuses on sulphurous and carbonaceous aerosol, the major constituents of particulate matter in the lowermost stratosphere (LMS), based on in situ measurements from 1999 to 2008. Aerosol particles in the size range of 0.082 mm were collected monthly during intercontinental flights with the CARIBIC passenger aircraft, presenting the first long-term study on carbonaceous aerosol in the LMS. Elemental concentrations were derived via subsequent laboratory-based ion beam analysis. The stoichiometry indicates that the sulphurous fraction is sulphate, while an O/C ratio of 0.2 indicates that the carbonaceous aerosol is organic. The concentration of the carbonaceous component corresponded on average to approximately 25% of that of the sulphurous, and could not be explained by forest fires or biomass burning, since the average mass ratio of Fe to K was 16 times higher than typical ratios in effluents from biomass burning. The data reveal increasing concentrations of particulate sulphur and carbon with a doubling of particulate sulphur from 1999 to 2008 in the northern hemisphere LMS. Periods of elevated concentrations of particulate sulphur in the LMS are linked to downward transport of aerosol from higher altitudes, using ozone as a tracer for stratospheric air. Tropical volcanic eruptions penetrating the tropical tropopause are identified as the likely cause of the particulate sulphur and carbon increase in the LMS, where entrainment of lower tropospheric air into volcanic jets and plumes could be the cause of the carbon increase.
- ItemSize distribution, mass concentration, chemical and mineralogical composition and derived optical parameters of the boundary layer aerosol at Tinfou, Morocco, during SAMUM 2006(Milton Park : Taylor & Francis, 2017) Kandler, K.; Schütz, L.; Deutscher, C.; Ebert, M.; Hofmann, H.; Jäckel, S.; Jaenicke, R.; Knippertz, P.; Lieke, K.; Massling, A.; Petzold, A.; Schladitz, A.; Weinzierl, B.; Wiedensohler, A.; Zorn, S.; Weinbruch, S.During the SAMUM 2006 field campaign in southern Morocco, physical and chemical properties of desert aerosols were measured. Mass concentrations ranging from 30μgm−3 for PM2.5 under desert background conditions up to 300 000μgm−3 for total suspended particles (TSP) during moderate dust storms were measured. TSP dust concentrations are correlated with the local wind speed, whereasPM10 andPM2.5 concentrations are determined by advection from distant sources. Size distributions were measured for particles with diameter between 20 nm and 500μm (parametrizations are given). Two major regimes of the size spectrum can be distinguished. For particles smaller than 500 nm diameter, the distributions show maxima around 80 nm, widely unaffected of varying meteorological and dust emission conditions. For particles larger than 500 nm, the range of variation may be up to one order of magnitude and up to three orders of magnitude for particles larger than 10μm. The mineralogical composition of aerosol bulk samples was measured by X-ray powder diffraction. Major constituents of the aerosol are quartz, potassium feldspar, plagioclase, calcite, hematite and the clay minerals illite, kaolinite and chlorite. A small temporal variability of the bulk mineralogical composition was encountered. The chemical composition of approximately 74 000 particles was determined by electron microscopic single particle analysis. Three size regimes are identified: for smaller than 500 nm in diameter, the aerosol consists of sulphates and mineral dust. For larger than 500 nm up to 50μm, mineral dust dominates, consisting mainly of silicates, and—to a lesser extent—carbonates and quartz. For diameters larger than 50μm, approximately half of the particles consist of quartz. Time series of the elemental composition show a moderate temporal variability of the major compounds. Calcium-dominated particles are enhanced during advection from a prominent dust source in Northern Africa (Chott El Djerid and surroundings). The particle aspect ratio was measured for all analysed particles. Its size dependence reflects that of the chemical composition. For larger than 500 nm particle diameter, a median aspect ratio of 1.6 is measured. Towards smaller particles, it decreases to about 1.3 (parametrizations are given). From the chemical/mineralogical composition, the aerosol complex refractive index was determined for several wavelengths from ultraviolet to near-infrared. Both real and imaginary parts show lower values for particles smaller than 500 nm in diameter (1.55–2.8 × 10−3i at 530 nm) and slightly higher values for larger particles (1.57–3.7 × 10−3i at 530 nm).