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- ItemComplex refractive indices of Saharan dust samples at visible and near UV wavelengths: A laboratory study(München : European Geopyhsical Union, 2012) Wagner, R.; Ajtai, T.; Kandler, K.; Lieke, K.; Linke, C.; Müller, T.; Schnaiter, M.; Vragel, M.We have retrieved the wavelength-dependent imaginary parts of the complex refractive index for five different Saharan dust aerosol particles of variable mineralogical composition at wavelengths between 305 and 955 nm. The dust particles were generated by dispersing soil samples into a laboratory aerosol chamber, typically yielding particle sizes with mean diameters ranging from 0.3 to 0.4 μm and maximum diameters from 2 to 4 μm. The extinction and absorption coefficients as well as the number size distribution of the dust particles were simultaneously measured by various established techniques. An inversion scheme based on a spheroidal dust model was employed to deduce the refractive indices. The retrieved imaginary parts of the complex refractive index were in the range from 0.003 to 0.005, 0.005 to 0.011, and 0.016 to 0.050 at the wavelengths 955, 505, and 305 nm. The hematite content of the dust particles was determined by electron-microscopical single particle analysis. Hematite volume fractions in the range from 1.1 to 2.7% were found for the different dusts, a range typical for atmospheric mineral dust. We have performed a sensitivity study to assess how accurately the retrieved imaginary refractive indices could be reproduced by calculations with mixing rule approximations using the experimentally determined hematite contents as input.
- ItemMass deposition fluxes of Saharan mineral dust to the tropical northeast Atlantic Ocean: An intercomparison of methods(München : European Geopyhsical Union, 2014) Niedermeier, N.; Held, A.; Müller, T.; Heinold, B.; Schepanski, K.; Tegen, I.; Kandler, K.; Ebert, M.; Weinbruch, S.; Read, K.; Lee, J.; Fomba, K.W.; Müller, K.; Herrmann, H.; Wiedensohler, A.Mass deposition fluxes of mineral dust to the tropical northeast Atlantic Ocean were determined within this study. In the framework of SOPRAN (Surface Ocean Processes in the Anthropocene), the interaction between the atmosphere and the ocean in terms of material exchange were investigated at the Cape Verde atmospheric observatory (CVAO) on the island Sao Vicente for January 2009. Five different methods were applied to estimate the deposition flux, using different meteorological and physical measurements, remote sensing, and regional dust transport simulations. The set of observations comprises micrometeorological measurements with an ultra-sonic anemometer and profile measurements using 2-D anemometers at two different heights, and microphysical measurements of the size-resolved mass concentrations of mineral dust. In addition, the total mass concentration of mineral dust was derived from absorption photometer observations and passive sampling. The regional dust model COSMO-MUSCAT was used for simulations of dust emission and transport, including dry and wet deposition processes. This model was used as it describes the AOD's and mass concentrations realistic compared to the measurements and because it was run for the time period of the measurements. The four observation-based methods yield a monthly average deposition flux of mineral dust of 12–29 ng m−2 s−1. The simulation results come close to the upper range of the measurements with an average value of 47 ng m−2 s−1. It is shown that the mass deposition flux of mineral dust obtained by the combination of micrometeorological (ultra-sonic anemometer) and microphysical measurements (particle mass size distribution of mineral dust) is difficult to compare to modeled mass deposition fluxes when the mineral dust is inhomogeneously distributed over the investigated area.
- ItemAirborne observations of the Eyjafjalla volcano ash cloud over Europe during air space closure in April and May 2010(München : European Geopyhsical Union, 2011) Schumann, U.; Weinzierl, B.; Reitebuch, O.; Schlager, H.; Minikin, A.; Forster, C.; Baumann, R.; Sailer, T.; Graf, K.; Mannstein, H.; Voigt, C.; Rahm, S.; Simmet, R.; Scheibe, M.; Lichtenstern, M.; Stock, P.; Rüba, H.; Schäuble, D.; Tafferner, A.; Rautenhaus, M.; Gerz, T.; Ziereis, H.; Krautstrunk, M.; Mallaun, C.; Gayet, J.-F.; Lieke, K.; Kandler, K.; Ebert, M.; Weinbruch, S.; Stohl, A.; Gasteiger, J.; Groß, S.; Freudenthaler, V.; Wiegner, M.; Ansmann, A.; Tesche, M.; Olafsson, H.; Sturm, K.Airborne lidar and in-situ measurements of aerosols and trace gases were performed in volcanic ash plumes over Europe between Southern Germany and Iceland with the Falcon aircraft during the eruption period of the Eyjafjalla volcano between 19 April and 18 May 2010. Flight planning and measurement analyses were supported by a refined Meteosat ash product and trajectory model analysis. The volcanic ash plume was observed with lidar directly over the volcano and up to a distance of 2700 km downwind, and up to 120 h plume ages. Aged ash layers were between a few 100 m to 3 km deep, occurred between 1 and 7 km altitude, and were typically 100 to 300 km wide. Particles collected by impactors had diameters up to 20 μm diameter, with size and age dependent composition. Ash mass concentrations were derived from optical particle spectrometers for a particle density of 2.6 g cm−3 and various values of the refractive index (RI, real part: 1.59; 3 values for the imaginary part: 0, 0.004 and 0.008). The mass concentrations, effective diameters and related optical properties were compared with ground-based lidar observations. Theoretical considerations of particle sedimentation constrain the particle diameters to those obtained for the lower RI values. The ash mass concentration results have an uncertainty of a factor of two. The maximum ash mass concentration encountered during the 17 flights with 34 ash plume penetrations was below 1 mg m−3. The Falcon flew in ash clouds up to about 0.8 mg m−3 for a few minutes and in an ash cloud with approximately 0.2 mg m−3 mean-concentration for about one hour without engine damage. The ash plumes were rather dry and correlated with considerable CO and SO2 increases and O3 decreases. To first order, ash concentration and SO2 mixing ratio in the plumes decreased by a factor of two within less than a day. In fresh plumes, the SO2 and CO concentration increases were correlated with the ash mass concentration. The ash plumes were often visible slantwise as faint dark layers, even for concentrations below 0.1 mg m−3. The large abundance of volatile Aitken mode particles suggests previous nucleation of sulfuric acid droplets. The effective diameters range between 0.2 and 3 μm with considerable surface and volume contributions from the Aitken and coarse mode aerosol, respectively. The distal ash mass flux on 2 May was of the order of 500 (240–1600) kg s−1. The volcano induced about 10 (2.5–50) Tg of distal ash mass and about 3 (0.6–23) Tg of SO2 during the whole eruption period. The results of the Falcon flights were used to support the responsible agencies in their decisions concerning air traffic in the presence of volcanic ash.
- ItemSingle-particle characterization of ice-nucleating particles and ice particle residuals sampled by three different techniques(München : European Geopyhsical Union, 2015) Worringen, A.; Kandler, K.; Benker, N.; Dirsch, T.; Mertes, S.; Schenk, L.; Kästner, U.; Frank, F.; Nillius, B.; Bundke, U.; Rose, D.; Curtius, J.; Kupiszewski, P.; Weingartner, E.; Vochezer, P.; Schneider, J.; Schmidt, S.; Weinbruch, S.; Ebert, M.In the present work, three different techniques to separate ice-nucleating particles (INPs) as well as ice particle residuals (IPRs) from non-ice-active particles are compared. The Ice Selective Inlet (ISI) and the Ice Counterflow Virtual Impactor (Ice-CVI) sample ice particles from mixed-phase clouds and allow after evaporation in the instrument for the analysis of the residuals. The Fast Ice Nucleus Chamber (FINCH) coupled with the Ice Nuclei Pumped Counterflow Virtual Impactor (IN-PCVI) provides ice-activating conditions to aerosol particles and extracts the activated particles for analysis. The instruments were run during a joint field campaign which took place in January and February 2013 at the High Alpine Research Station Jungfraujoch (Switzerland). INPs and IPRs were analyzed offline by scanning electron microscopy and energy-dispersive X-ray microanalysis to determine their size, chemical composition and mixing state. Online analysis of the size and chemical composition of INP activated in FINCH was performed by laser ablation mass spectrometry. With all three INP/IPR separation techniques high abundances (median 20–70%) of instrumental contamination artifacts were observed (ISI: Si-O spheres, probably calibration aerosol; Ice-CVI: Al-O particles; FINCH + IN-PCVI: steel particles). After removal of the instrumental contamination particles, silicates, Ca-rich particles, carbonaceous material and metal oxides were the major INP/IPR particle types obtained by all three techniques. In addition, considerable amounts (median abundance mostly a few percent) of soluble material (e.g., sea salt, sulfates) were observed. As these soluble particles are often not expected to act as INP/IPR, we consider them as potential measurement artifacts. Minor types of INP/IPR include soot and Pb-bearing particles. The Pb-bearing particles are mainly present as an internal mixture with other particle types. Most samples showed a maximum of the INP/IPR size distribution at 200–400 nm in geometric diameter. In a few cases, a second supermicron maximum was identified. Soot/carbonaceous material and metal oxides were present mainly in the sub-micrometer range. Silicates and Ca-rich particles were mainly found with diameters above 1 μm (using ISI and FINCH), in contrast to the Ice-CVI which also sampled many submicron particles of both groups. Due to changing meteorological conditions, the INP/IPR composition was highly variable if different samples were compared. Thus, the observed discrepancies between the different separation techniques may partly result from the non-parallel sampling. The differences of the particle group relative number abundance as well as the mixing state of INP/IPR clearly demonstrate the need of further studies to better understand the influence of the separation techniques on the INP/IPR chemical composition. Also, it must be concluded that the abundance of contamination artifacts in the separated INP and IPR is generally large and should be corrected for, emphasizing the need for the accompanying chemical measurements. Thus, further work is needed to allow for routine operation of the three separation techniques investigated.
- ItemA comprehensive laboratory study on the immersion freezing behavior of illite NX particles: A comparison of 17 ice nucleation measurement techniques(München : European Geopyhsical Union, 2015) Hiranuma, N.; Augustin-Bauditz, S.; Bingemer, H.; Budke, C.; Curtius, J.; Danielczok, A.; Diehl, K.; Dreischmeier, K.; Ebert, M.; Frank, F.; Hoffmann, N.; Kandler, K.; Kiselev, A.; Koop, T.; Leisner, T.; Möhler, O.; Nillius, B.; Peckhaus, A.; Rose, D.; Weinbruch, S.; Wex, H.; Boose, Y.; DeMott, P.J.; Hader, J.D.; Hill, T.C.J.; Kanji, Z.A.; Kulkarn, G.; Levin, E.J.T.; McCluskey, C.S.; Murakami, M.; Murray, B.J.; Niedermeier, D.; Petters, M.D.; O'Sullivan, D.; Saito, A.; Schill, G.P.; Tajiri, T.; Tolbert, M.A.; Welti, A.; Whale, T.F.; Wright, T.P.; Yamashita, K.Immersion freezing is the most relevant heterogeneous ice nucleation mechanism through which ice crystals are formed in mixed-phase clouds. In recent years, an increasing number of laboratory experiments utilizing a variety of instruments have examined immersion freezing activity of atmospherically relevant ice-nucleating particles. However, an intercomparison of these laboratory results is a difficult task because investigators have used different ice nucleation (IN) measurement methods to produce these results. A remaining challenge is to explore the sensitivity and accuracy of these techniques and to understand how the IN results are potentially influenced or biased by experimental parameters associated with these techniques. Within the framework of INUIT (Ice Nuclei Research Unit), we distributed an illite-rich sample (illite NX) as a representative surrogate for atmospheric mineral dust particles to investigators to perform immersion freezing experiments using different IN measurement methods and to obtain IN data as a function of particle concentration, temperature (T), cooling rate and nucleation time. A total of 17 measurement methods were involved in the data intercomparison. Experiments with seven instruments started with the test sample pre-suspended in water before cooling, while 10 other instruments employed water vapor condensation onto dry-dispersed particles followed by immersion freezing. The resulting comprehensive immersion freezing data set was evaluated using the ice nucleation active surface-site density, ns, to develop a representative ns(T) spectrum that spans a wide temperature range (−37 °C < T < −11 °C) and covers 9 orders of magnitude in ns. In general, the 17 immersion freezing measurement techniques deviate, within a range of about 8 °C in terms of temperature, by 3 orders of magnitude with respect to ns. In addition, we show evidence that the immersion freezing efficiency expressed in ns of illite NX particles is relatively independent of droplet size, particle mass in suspension, particle size and cooling rate during freezing. A strong temperature dependence and weak time and size dependence of the immersion freezing efficiency of illite-rich clay mineral particles enabled the ns parameterization solely as a function of temperature. We also characterized the ns(T) spectra and identified a section with a steep slope between −20 and −27 °C, where a large fraction of active sites of our test dust may trigger immersion freezing. This slope was followed by a region with a gentler slope at temperatures below −27 °C. While the agreement between different instruments was reasonable below ~ −27 °C, there seemed to be a different trend in the temperature-dependent ice nucleation activity from the suspension and dry-dispersed particle measurements for this mineral dust, in particular at higher temperatures. For instance, the ice nucleation activity expressed in ns was smaller for the average of the wet suspended samples and higher for the average of the dry-dispersed aerosol samples between about −27 and −18 °C. Only instruments making measurements with wet suspended samples were able to measure ice nucleation above −18 °C. A possible explanation for the deviation between −27 and −18 °C is discussed. Multiple exponential distribution fits in both linear and log space for both specific surface area-based ns(T) and geometric surface area-based ns(T) are provided. These new fits, constrained by using identical reference samples, will help to compare IN measurement methods that are not included in the present study and IN data from future IN instruments.
- ItemCharacterization of aerosol properties at Cyprus, focusing on cloud condensation nuclei and ice-nucleating particles(Göttingen : Copernicus GmbH, 2019) Gong, X.; Wex, H.; Müller, T.; Wiedensohler, A.; Höhler, K.; Kandler, K.; Ma, N.; Dietel, B.; Schiebel, T.; Möhler, O.; Stratmann, F.As part of the A-LIFE (Absorbing aerosol layers in a changing climate: aging, LIFEtime and dynamics) campaign, ground-based measurements were carried out in Paphos, Cyprus, to characterize the abundance, properties, and sources of aerosol particles in general and cloud condensation nuclei (CCN) and ice-nucleating particles (INP) in particular. New particle formation (NPF) events with subsequent growth of the particles into the CCN size range were observed. Aitken mode particles featured k values of 0.21 to 0.29, indicating the presence of organic materials. Accumulation mode particles featured a higher hygroscopicity parameter, with a median k value of 0.57, suggesting the presence of sulfate and maybe sea salt particles mixed with organic carbon. A clear downward trend of k with increasing supersaturation and decreasing dcrit was found. Super-micron particles originated mainly from sea-spray aerosol (SSA) and partly from mineral dust. INP concentrations (NINP) were measured in the temperature range from-6:5 to-26:5 °C, using two freezing array-type instruments. NINP at a particular temperature span around 1 order of magnitude below-20 °C and about 2 orders of magnitude at warmer temperatures (T >-18 °C). Few samples showed elevated concentrations at temperatures >-15 °C, which suggests a significant contribution of biological particles to the INP population, which possibly could originate from Cyprus. Both measured temperature spectra and NINP probability density functions (PDFs) indicate that the observed INP (ice active in the temperature range between-15 and-20 °C) mainly originate from long-range transport. There was no correlation between NINP and particle number concentration in the size range> 500 nm (N>500 nm). Parameterizations based on N>500 nm were found to overestimate NINP by about 1 to 2 orders of magnitude. There was also no correlation between NINP and particle surface area concentration. The ice active surface site density (ns) for the polluted aerosol encountered in the eastern Mediterranean in this study is about 1 to 3 orders of magnitude lower than the ns found for dust aerosol particles in previous studies. This suggests that observed NINP PDFs such as those derived here could be a better choice for modeling NINP if the aerosol particle composition is unknown or uncertain.
- 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.
- 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).
- ItemNumerical simulations of optical properties of Saharan dust aerosols with emphasis on lidar applications(Milton Park : Taylor & Francis, 2017) Wiegner, M.; Gasteiger, J.; Kandler, K.; Weinzierl, B.; Rasp, K.; Esselborn, M.; Freudenthaler, V.; Heese, B.; Toledano, C.; Tesche, M.; Althausen, D.In the framework of the Saharan Mineral Dust Experiment (SAMUM) for the first time the spectral dependence of particle linear depolarization ratios was measured by combining four lidar systems. In this paper these measurements are compared with results from scattering theory based on the T-matrix method. For this purpose, in situ measurements—size distribution, shape distribution and refractive index—were used as input parameters; particle shape was approximated by spheroids. A sensitivity study showed that lidar-related parameters—lidar ratio Sp and linear depolarization ratio δp—are very sensitive to changes of all parameters. The simulated values of the δp are in the range of 20% and 31% and thus in the range of the measurements. The spectral dependence is weak, so that it could not be resolved by the measurements. Calculated lidar ratios based on the measured microphysics and considering equivalent radii up to 7.5μm show a range of possible values between 29 and 50 sr at λ = 532 nm. Larger Sp might be possible if the real part of the refractive index is small and the imaginary part is large. A strict validation was however not possible as too many microphysical parameters influence Sp and δp that could not be measured with the required accuracy.
- 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.