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- ItemFour-dimensional distribution of the 2010 Eyjafjallajökull volcanic cloud over Europe observed by EARLINET(München : European Geopyhsical Union, 2013) Pappalardo, G.; Mona, L.; D'Amico, G.; Wandinger, U.; Adam, M.; Amodeo, A.; Ansmann, A.; Apituley, A.; Alados Arboledas, L.; Balis, D.; Boselli, A.; Bravo-Aranda, J.A.; Chaikovsky, A.; Comeron, A.; Cuesta, J.; De Tomasi, F.; Freudenthaler, V.; Gausa, M.; Giannakaki, E.; Giehl, H.; Giunta, A.; Grigorov, I.; Groß, S.; Haeffelin, M.; Hiebsch, A.; Iarlori, M.; Lange, D.; Linné, H.; Madonna, F.; Mattis, I.; Mamouri, R.-E.; McAuliffe, M.A.P.; Mitev, V.; Molero, F.; Navas-Guzman, F.; Nicolae, D.; Papayannis, A.; Perrone, M.R.; Pietras, C.; Pietruczuk, A.; Pisani, G.; Preißler, J.; Pujadas, M.; Rizi, V.; Ruth, A.A.; Schmidt, J.; Schnell, F.; Seifert, P.; Serikov, I.; Sicard, M.; Simeonov, V.; Spinelli, N.; Stebel, K.; Tesche, M.; Trickl, T.; Wang, X.; Wagner, F.; Wiegner, M.; Wilson, K.M.The eruption of the Icelandic volcano Eyjafjallajökull in April–May 2010 represents a "natural experiment" to study the impact of volcanic emissions on a continental scale. For the first time, quantitative data about the presence, altitude, and layering of the volcanic cloud, in conjunction with optical information, are available for most parts of Europe derived from the observations by the European Aerosol Research Lidar NETwork (EARLINET). Based on multi-wavelength Raman lidar systems, EARLINET is the only instrument worldwide that is able to provide dense time series of high-quality optical data to be used for aerosol typing and for the retrieval of particle microphysical properties as a function of altitude. In this work we show the four-dimensional (4-D) distribution of the Eyjafjallajökull volcanic cloud in the troposphere over Europe as observed by EARLINET during the entire volcanic event (15 April–26 May 2010). All optical properties directly measured (backscatter, extinction, and particle linear depolarization ratio) are stored in the EARLINET database available at http://www.earlinet.org. A specific relational database providing the volcanic mask over Europe, realized ad hoc for this specific event, has been developed and is available on request at http://www.earlinet.org. During the first days after the eruption, volcanic particles were detected over Central Europe within a wide range of altitudes, from the upper troposphere down to the local planetary boundary layer (PBL). After 19 April 2010, volcanic particles were detected over southern and south-eastern Europe. During the first half of May (5–15 May), material emitted by the Eyjafjallajökull volcano was detected over Spain and Portugal and then over the Mediterranean and the Balkans. The last observations of the event were recorded until 25 May in Central Europe and in the Eastern Mediterranean area. The 4-D distribution of volcanic aerosol layering and optical properties on European scale reported here provides an unprecedented data set for evaluating satellite data and aerosol dispersion models for this kind of volcanic events.
- ItemThe Pagami Creek smoke plume after long-range transport to the upper troposphere over Europe – Aerosol properties and black carbon mixing state(München : European Geopyhsical Union, 2014) Dahlkötter, F.; Gysel, M.; Sauer, D.; Minikin, A.; Baumann, R.; Seifert, P.; Ansmann, A.; Fromm, M.; Voigt, C.; Weinzierl, B.During the CONCERT 2011 field experiment with the DLR research aircraft Falcon, an enhanced aerosol layer with particle linear depolarization ratios of 6–8% at 532 nm was observed at altitudes above 10 km over northeast Germany on 16 September 2011. Dispersion simulations with HYSPILT suggest that the elevated aerosol layer originated from the Pagami Creek forest fire in Minnesota, USA, which caused pyro-convective uplift of particles and gases. The 3–4 day-old smoke plume had high total refractory black carbon (rBC) mass concentrations of 0.03–0.35 μg m−3 at standard temperature and pressure (STP) with rBC mass equivalent diameter predominantly smaller than 130 nm. Assuming a core-shell particle structure, the BC cores exhibit very thick (median: 105–136 nm) BC-free coatings. A large fraction of the BC-containing particles disintegrated into a BC-free fragment and a BC fragment while passing through the laser beam of the Single Particle Soot Photometer (SP2). In this study, the disintegration is a result of very thick coatings around the BC cores. This is in contrast to a previous study in a forest-fire plume, where it was hypothesized to be a result of BC cores being attached to a BC-free particle. For the high-altitude forest-fire aerosol layer observed in this study, increased mass specific light-absorption cross sections of BC can be expected due to the very thick coatings around the BC cores, while this would not be the case for the attached-type morphology. We estimate the BC mass import from the Pagami Creek forest fire into the upper troposphere/lower stratosphere (UTLS) region (best estimate: 25 Mg rBC). A comparison to black carbon emission rates from aviation underlines the importance of pyro-convection on the BC load in the UTLS region. Our study provides detailed information on the microphysics and the mixing state of BC in the forest-fire aerosol layer in the upper troposphere that can be used to better understand and investigate the radiative impact of such upper tropospheric aerosol layers.
- ItemCeilometer lidar comparison: Backscatter coefficient retrieval and signal-to-noise ratio determination(München : European Geopyhsical Union, 2010) Heese, B.; Flentje, H.; Althausen, D.; Ansmann, A.; Frey, S.The potential of a new generation of ceilometer instruments for aerosol monitoring has been studied in the Ceilometer Lidar Comparison (CLIC) study. The used ceilometer was developed by Jenoptik, Germany, and is designed to find both thin cirrus clouds at tropopause level and aerosol layers at close ranges during day and night-time. The comparison study was performed to determine up to which altitude the ceilometers are capable to deliver particle backscatter coefficient profiles. For this, the derived ceilometer profiles are compared to simultaneously measured lidar profiles at the same wavelength. The lidar used for the comparison was the multi-wavelengths Raman lidar PollyXT. To demonstrate the capabilities and limits of ceilometers for the derivation of particle backscatter coefficient profiles from their measurements two examples of the comparison results are shown. Two cases, a daytime case with high background noise and a less noisy night-time case, are chosen. In both cases the ceilometer profiles compare well with the lidar profiles in atmospheric structures like aerosol layers or the boundary layer top height. However, the determination of the correct magnitude of the particle backscatter coefficient needs a calibration of the ceilometer data with an independent measurement of the aerosol optical depth by a sun photometer. To characterizes the ceilometers signal performance with increasing altitude a comprehensive signal-to-noise ratio study was performed. During daytime the signal-to-noise ratio is higher than 1 up to 4–5 km depending on the aerosol content. In our night-time case the SNR is higher than 1 even up to 8.5 km, so that also aerosol layers in the upper troposphere had been detected by the ceilometer.
- ItemThermodynamics of the formation of sulfuric acid dimers in the binary (H2SO4-H2O) and ternary (H2SO4-H2O-NH3) system(München : European Geopyhsical Union, 2015) Schmidt, J.; Ansmann, A.; Bühl, J.; Wandinger, U.Sulfuric acid is an important gas influencing atmospheric new particle formation (NPF). Both the binary (H2SO4–H2O) system and the ternary system involving ammonia (H2SO4–H2O–NH3) may be important in the free troposphere. An essential step in the nucleation of aerosol particles from gas-phase precursors is the formation of a dimer, so an understanding of the thermodynamics of dimer formation over a wide range of atmospheric conditions is essential to describe NPF. We have used the CLOUD chamber to conduct nucleation experiments for these systems at temperatures from 208 to 248 K. Neutral monomer and dimer concentrations of sulfuric acid were measured using a chemical ionization mass spectrometer (CIMS). From these measurements, dimer evaporation rates in the binary system were derived for temperatures of 208 and 223 K. We compare these results to literature data from a previous study that was conducted at higher temperatures but is in good agreement with the present study. For the ternary system the formation of H2SO4·NH3 is very likely an essential step in the formation of sulfuric acid dimers, which were measured at 210, 223, and 248 K. We estimate the thermodynamic properties (dH and dS) of the H2SO4·NH3 cluster using a simple heuristic model and the measured data. Furthermore, we report the first measurements of large neutral sulfuric acid clusters containing as many as 10 sulfuric acid molecules for the binary system using chemical ionization–atmospheric pressure interface time-of-flight (CI-APi-TOF) mass spectrometry.