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- ItemFirst long-term study of particle number size distributions and new particle formation events of regional aerosol in the North China Plain(München : European Geopyhsical Union, 2011) Shen, X.J.; Sun, J.Y.; Zhang, Y.M.; Wehner, B.; Nowak, A.; Tuch, T.; Zhang, X.C.; Wang, T.T.; Zhou, H.G.; Zhang, X.L.; Dong, F.; Birmili, W.; Wiedensohler, A.Atmospheric particle number size distributions (size range 0.003–10 μm) were measured between March 2008 and August 2009 at Shangdianzi (SDZ), a rural research station in the North China Plain. These measurements were made in an attempt to better characterize the tropospheric background aerosol in Northern China. The mean particle number concentrations of the total particle, as well as the nucleation, Aitken, accumulation and coarse mode were determined to be 1.2 ± 0.9 × 104, 3.6 ± 7.9 × 103, 4.4 ± 3.4 × 103, 3.5 ± 2.8 × 103 and 2 ± 3 cm−3, respectively. A general finding was that the particle number concentration was higher during spring compared to the other seasons. The air mass origin had an important effect on the particle number concentration and new particle formation events. Air masses from northwest (i.e. inner Asia) favored the new particle formation events, while air masses from southeast showed the highest particle mass concentration. Significant diurnal variations in particle number were observed, which could be linked to new particle formation events, i.e. gas-to-particle conversion. During particle formation events, the number concentration of the nucleation mode rose up to maximum value of 104 cm−3. New particle formation events were observed on 36% of the effective measurement days. The formation rate ranged from 0.7 to 72.7 cm−3 s−1, with a mean value of 8.0 cm−3 s−1. The value of the nucleation mode growth rate was in the range of 0.3–14.5 nm h−1, with a mean value of 4.3 nm h−1. It was an essential observation that on many occasions the nucleation mode was able to grow into the size of cloud condensation nuclei (CCN) within a matter of several hours. Furthermore, the new particle formation was regularly followed by a measurable increase in particle mass concentration and extinction coefficient, indicative of a high abundance of condensable vapors in the atmosphere under study.
- ItemAnalysis of number size distributions of tropical free tropospheric aerosol particles observed at Pico Espejo (4765 m a.s.l.), Venezuela(München : European Geopyhsical Union, 2011) Schmeissner, T.; Krejci, R.; Ström, J.; Birmili, W.; Wiedensohler, A.; Hochschild, G.; Gross, J.; Hoffmann, P.; Calderon, S.The first long-term measurements of aerosol number and size distributions in South-American tropical free troposphere (FT) were performed from March 2007 until March 2009. The measurements took place at the high altitude Atmospheric Research Station Alexander von Humboldt. The station is located on top of the Sierra Nevada mountain ridge at 4765 m a.s.l. nearby the city of Mérida, Venezuela. Aerosol size distribution and number concentration data was obtained with a custom-built Differential Mobility Particle Sizer (DMPS) system and a Condensational Particle Counter (CPC). The analysis of the annual and diurnal variability of the tropical FT aerosol focused mainly on possible links to the atmospheric general circulation in the tropics. Considerable annual and diurnal cycles of the particle number concentration were observed. Highest total particle number concentrations were measured during the dry season (January–March, 519 ± 613 cm−3), lowest during the wet season (July–September, 318 ± 194 cm−3). The more humid FT (relative humidity (RH) range 50–95 %) contained generally higher aerosol particle number concentrations (573 ± 768 cm−3 during dry season, 320 ± 195 cm−3 during wet season) than the dry FT (RH < 50 %, 454 ± 332 cm−3 during dry season, 275 ± 172 cm−3 during wet season), indicating the importance of convection for aerosol distributions in the tropical FT. The diurnal cycle in the variability of the particle number concentration was mainly driven by local orography.
- ItemAtmospheric dust modeling from meso to global scales with the online NMMB/BSC-Dust model – Part 2: Experimental campaigns in Northern Africa(München : European Geopyhsical Union, 2012) Haustein, K.; Pérez, C.; Baldasano, J.M.; Jorba, O.; Basart, S.; Miller, R.L.; Janjic, Z.; Black, T.; Nickovic, S.; Todd, M.C.; Washington, R.; Müller, D.; Tesche, M.; Weinzierl, B.; Esselborn, M.; Schladitz, A.The new NMMB/BSC-Dust model is intended to provide short to medium-range weather and dust forecasts from regional to global scales. It is an online model in which the dust aerosol dynamics and physics are solved at each model time step. The companion paper (Pérez et al., 2011) develops the dust model parameterizations and provides daily to annual evaluations of the model for its global and regional configurations. Modeled aerosol optical depth (AOD) was evaluated against AERONET Sun photometers over Northern Africa, Middle East and Europe with correlations around 0.6–0.7 on average without dust data assimilation. In this paper we analyze in detail the behavior of the model using data from the Saharan Mineral dUst experiment (SAMUM-1) in 2006 and the Bodélé Dust Experiment (BoDEx) in 2005. AOD from satellites and Sun photometers, vertically resolved extinction coefficients from lidars and particle size distributions at the ground and in the troposphere are used, complemented by wind profile data and surface meteorological measurements. All simulations were performed at the regional scale for the Northern African domain at the expected operational horizontal resolution of 25 km. Model results for SAMUM-1 generally show good agreement with satellite data over the most active Saharan dust sources. The model reproduces the AOD from Sun photometers close to sources and after long-range transport, and the dust size spectra at different height levels. At this resolution, the model is not able to reproduce a large haboob that occurred during the campaign. Some deficiencies are found concerning the vertical dust distribution related to the representation of the mixing height in the atmospheric part of the model. For the BoDEx episode, we found the diurnal temperature cycle to be strongly dependant on the soil moisture, which is underestimated in the NCEP analysis used for model initialization. The low level jet (LLJ) and the dust AOD over the Bodélé are well reproduced. The remaining negative AOD bias (due to underestimated surface wind speeds) can be substantially reduced by decreasing the threshold friction velocity in the model.
- ItemTotal OH reactivity measurements in Paris during the 2010 MEGAPOLI winter campaign(München : European Geopyhsical Union, 2012) Dolgorouky, C.; Gros, V.; Sarda-Esteve, R.; Sinha, V.; Williams, J.; Marchand, N.; Sauvage, S.; Poulain, L.; Sciare, J.; Bonsang, B.Hydroxyl radicals play a central role in the troposphere as they control the lifetime of many trace gases. Measurement of OH reactivity (OH loss rate) is important to better constrain the OH budget and also to evaluate the completeness of measured VOC budget. Total atmospheric OH reactivity was measured for the first time in an European Megacity: Paris and its surrounding areas with 12 million inhabitants, during the MEGAPOLI winter campaign 2010. The method deployed was the Comparative Reactivity Method (CRM). The measured dataset contains both measured and calculated OH reactivity from CO, NOx and VOCs measured via PTR-MS, GC-FID and GC-MS instruments. The reactivities observed in Paris covered a range from 10 s−1 to 130 s−1, indicating a large loading of chemical reactants. The present study showed that, when clean marine air masses influenced Paris, the purely local OH reactivity (20 s−1) is well explained by the measured species. Nevertheless, when there is a continental import of air masses, high levels of OH reactivity were obtained (120–130 s−1) and the missing OH reactivity measured in this case jumped to 75%. Using covariations of the missing OH reactivity to secondary inorganic species in fine aerosols, we suggest that the missing OH reactants were most likely highly oxidized compounds issued from photochemically processed air masses of anthropogenic origin.
- 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.
- ItemDiurnal variation of midlatitudinal NO3 column abundance over table mountain facility, California(Göttingen : Copernicus GmbH, 2011) Chen, C.M.; Cageao, R.P.; Lawrence, L.; Stutz, J.; Salawitch, R.J.; Jourdain, L.; Li, Q.; Sander, S.P.The column abundance of NO3 was measured over Table Mountain Facility, CA (34.4° 117.7° W) from May 2003 through September 2004, using lunar occultation near full moon with a grating spectrometer. The NO 3 column retrieval was performed with the differential optical absorption spectroscopy (DOAS) technique using both the 623 and 662 nm NO 3 absorption bands. Other spectral features such as Fraunhofer lines and absorption from water vapor and oxygen were removed using solar spectra obtained at different airmass factors. We observed a seasonal variation, with nocturnally averaged NO3 columns between 5-7 × 1013 molec cm-2 during October through March, and 5-22 × 10 13 molec cm-2 during April through September. A subset of the data, with diurnal variability vastly different from the temporal profile obtained from one-dimensional stratospheric model calculations, clearly has boundary layer contributions; this was confirmed by simultaneous long-path DOAS measurements. However, even the NO3 columns that did follow the modeled time evolution were often much larger than modeled stratospheric partial columns constrained by realistic temperatures and ozone concentrations. This discrepancy is attributed to substantial tropospheric NO3 in the free troposphere, which may have the same time dependence as stratospheric NO 3.
- ItemHygroscopic properties of atmospheric aerosol particles over the Eastern Mediterranean: Implications for regional direct radiative forcing under clean and polluted conditions(München : European Geopyhsical Union, 2011) Stock, M.; Cheng, Y.F.; Birmili, W.; Massling, A.; Wehner, B.; Müller, T.; Leinert, S.; Kalivitis, N.; Mihalopoulos, N.; Wiedensohler, A.This work examines the effect of direct radiative forcing of aerosols in the eastern Mediterranean troposphere as a function of air mass composition, particle size distribution and hygroscopicity, and relative humidity (RH). During intensive field measurements on the island of Crete, Greece, the hygroscopic properties of atmospheric particles were determined using a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) and a Hygroscopicity Differential Mobility Analyzer-Aerodynamic Particle Sizer (H-DMA-APS). Similar to former studies, the H-TDMA identified three hygroscopic sub-fractions of particles in the sub-μm range: a more hygroscopic group, a less hygroscopic group and a nearly hydrophobic particle group. The average hygroscopic particle growth factors at 90 % RH were a significant function of particle mobility diameter (Dp): 1.42 (± 0.05) at 30 nm compared to 1.63 (± 0.07) at 250 nm. The H-DMA-APS identified up to three hygroscopic sub-fractions at mobility diameters of 1.0 and 1.2 μm. The data recorded between 12 August and 20 October 2005 were classified into four distinct synoptic-scale air mass types distinguishing between different regions of origin (western Mediterranean vs. the Aegean Sea) as well as the degree of continental pollution (marine vs. continentally influenced). The hygroscopic properties of particles with diameter Dp≥150 nm showed the most pronounced dependency on air mass origin, with growth factors in marine air masses exceeding those in continentally influenced air masses. Particle size distributions and hygroscopic growth factors were used to calculate aerosol light scattering coefficients at ambient RH using a Mie model. A main result was the pronounced enhancement of particle scattering over the eastern Mediterranean due to hygroscopic growth, both in the marine and continentally influenced air masses. When RH reached its summer daytime values around 70–80 %, up to 50–70 % of the calculated visibility reduction was due to the hygroscopic growth of the particles by water compared to the effect of the dry particles alone. The estimated aerosol direct radiative forcings for both, marine and continentally influenced air masses were negative indicating a net cooling of the atmosphere due to the aerosol. The radiative forcing ΔFr was nevertheless governed by the total aerosol concentration most of the time: ΔFr was typically more negative for continentally influenced aerosols (ca. −4 W m−2) compared to rather clean marine aerosols (ca. −1.5 W m−2). When RH occasionally reached 90 % in marine air masses, ΔFr even reached values down to −7 W m−2. Our results emphasize, on the basis of explicit particle hygroscopicity measurements, the relevance of ambient RH for the radiative forcing of regional atmospheres.
- ItemLong-term in situ observations of biomass burning aerosol at a high altitude station in Venezuela – Sources, impacts and interannual variability(München : European Geopyhsical Union, 2013) Hamburger, T.; Matisāns, M.; Tunved, P.; Ström, J.; Calderon, S.; Hoffmann, P.; Hochschild, G.; Gross, J.; Schmeissner, T.; Wiedensohler, A.; Krejci, R.First long-term observations of South American biomass burning aerosol within the tropical lower free troposphere are presented. The observations were conducted between 2007 and 2009 at a high altitude station (4765 m a.s.l.) on the Pico Espejo, Venezuela. Sub-micron particle volume, number concentrations of primary particles and particle absorption were observed. Orographic lifting and shallow convection leads to a distinct diurnal cycle at the station. It enables measurements within the lower free troposphere during night-time and observations of boundary layer air masses during daytime and at their transitional regions. The seasonal cycle is defined by a wet rainy season and a dry biomass burning season. The particle load of biomass burning aerosol is dominated by fires in the Venezuelan savannah. Increases of aerosol concentrations could not be linked to long-range transport of biomass burning plumes from the Amazon basin or Africa due to effective wet scavenging of particles. Highest particle concentrations were observed within boundary layer air masses during the dry season. Ambient sub-micron particle volume reached 1.4±1.3 μm3 cm−3, refractory particle number concentrations (at 300 °C) 510±420 cm−3 and the absorption coefficient 0.91±1.2 Mm−1. The respective concentrations were lowest within the lower free troposphere during the wet season and averaged at 0.19±0.25 μm3 cm−3, 150±94 cm−3 and 0.15±0.26 Mm−1. A decrease of particle concentrations during the dry seasons from 2007–2009 could be connected to a decrease in fire activity in the wider region of Venezuela using MODIS satellite observations. The variability of biomass burning is most likely linked to the El Niño–Southern Oscillation (ENSO). Low biomass burning activity in the Venezuelan savannah was observed to follow La Niña conditions, high biomass burning activity followed El Niño conditions.
- ItemMulti-wavelength Raman lidar, sun photometric and aircraft measurements in combination with inversion models for the estimation of the aerosol optical and physico-chemical properties over Athens, Greece(München : European Geopyhsical Union, 2012) Mamouri, R.E.; Papayannis, A.; Amiridis, V.; Müller, D.; Kokkalis, P.; Rapsomanikis, S.; Karageorgos, E.T.; Tsaknakis, G.; Nenes, A.; Kazadzis, S.; Remoundaki, E.A novel procedure has been developed to retrieve, simultaneously, the optical, microphysical and chemical properties of tropospheric aerosols with a multi-wavelength Raman lidar system in the troposphere over an urban site (Athens, Greece: 37.9° N, 23.6° E, 200 m a.s.l.) using data obtained during the European Space Agency (ESA) THERMOPOLIS project, which took place between 15–31 July 2009 over the Greater Athens Area (GAA). We selected to apply our procedure for a case study of intense aerosol layers that occurred on 20–21 July 2009. The National Technical University of Athens (NTUA) EOLE 6-wavelength Raman lidar system has been used to provide the vertical profiles of the optical properties of aerosols (extinction and backscatter coefficients, lidar ratio) and the water vapor mixing ratio. An inversion algorithm was used to derive the mean aerosol microphysical properties (mean effective radius (reff), single-scattering albedo ω) and mean complex refractive index (m)) at selected heights in the 2–3 km height region. We found that reff was 0.14–0.4 (±0.14) μm, ω was 0.63–0.88 (±0.08) (at 532 nm) and m ranged from 1.44 (±0.10) + 0.01 (±0.01)i to 1.55 (±0.12) + 0.06 (±0.02)i, in good agreement (only for the reff values) with in situ aircraft measurements. The water vapor and temperature profiles were incorporated into the ISORROPIA II model to propose a possible in situ aerosol composition consistent with the retrieved m and ω values. The retrieved aerosol chemical composition in the 2–3 km height region gave a variable range of sulfate (0–60%) and organic carbon (OC) content (0–50%), although the OC content increased (up to 50%) and the sulfate content dropped (up to 30%) around 3 km height; the retrieved low ω value (0.63), indicates the presence of absorbing biomass burning smoke mixed with urban haze. Finally, the retrieved aerosol microphysical properties were compared with column-integrated sun photometer CIMEL data.
- 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.