DSpace :: Browsing by Author "Schneider, J."

Browsing by Author "Schneider, J."

Now showing 1 - 20 of 21

Aerosol particle measurements at three stationary sites in the megacity of Paris during summer 2009: Meteorology and air mass origin dominate aerosol particle composition and size distribution
(München : European Geopyhsical Union, 2013) Freutel, F.; Schneider, J.; Drewnick, F.; Weiden-Reinmüller, S.-L.; Crippa, M.; Prévôt, A.S.H.; Baltensperger, U.; Poulain, L.; Wiedensohler, R.A.; Sciare, J.; Sarda-Estève, R.; Burkhart, J.F.; Eckhardt, S.; Stohl, A.; Gros, V.; Colomb, A.; Michoud, V.; Doussin, J.F.; Borbon, A.; Haeffelin, M.; Morille, Y.; Beekmann, M.; Borrmann, S.
During July 2009, a one-month measurement campaign was performed in the megacity of Paris. Amongst other measurement platforms, three stationary sites distributed over an area of 40 km in diameter in the greater Paris region enabled a detailed characterization of the aerosol particle and gas phase. Simulation results from the FLEXPART dispersion model were used to distinguish between different types of air masses sampled. It was found that the origin of air masses had a large influence on measured mass concentrations of the secondary species particulate sulphate, nitrate, ammonium, and oxygenated organic aerosol measured with the Aerodyne aerosol mass spectrometer in the submicron particle size range: particularly high concentrations of these species (about 4 μg m−3, 2 μg m−3, 2 μg m−3, and 7 μg m−3, respectively) were measured when aged material was advected from continental Europe, while for air masses originating from the Atlantic, much lower mass concentrations of these species were observed (about 1 μg m−3, 0.2 μg m−3, 0.4 μg m−3, and 1–3 μg m−3, respectively). For the primary emission tracers hydrocarbon-like organic aerosol, black carbon, and NOx it was found that apart from diurnal source strength variations and proximity to emission sources, local meteorology had the largest influence on measured concentrations, with higher wind speeds leading to larger dilution and therefore smaller measured concentrations. Also the shape of particle size distributions was affected by wind speed and air mass origin. Quasi-Lagrangian measurements performed under connected flow conditions between the three stationary sites were used to estimate the influence of the Paris emission plume onto its surroundings, which was found to be rather small. Rough estimates for the impact of the Paris emission plume on the suburban areas can be inferred from these measurements: Volume mixing ratios of 1–14 ppb of NOx, and upper limits for mass concentrations of about 1.5 μg m−3 of black carbon and of about 3 μg m−3 of hydrocarbon-like organic aerosol can be deduced which originate from both, local emissions and the overall Paris emission plume. The secondary aerosol particle phase species were found to be not significantly influenced by the Paris megacity, indicating their regional origin. The submicron aerosol mass concentrations of particulate sulphate, nitrate, and ammonium measured during time periods when air masses were advected from eastern central Europe were found to be similar to what has been found from other measurement campaigns in Paris and south-central France for this type of air mass origin, indicating that the results presented here are also more generally valid.
Aerosol properties, source identification, and cloud processing in orographic clouds measured by single particle mass spectrometry on a central European mountain site during HCCT-2010
(München : European Geopyhsical Union, 2016) Roth, A.; Schneider, J.; Klimach, T.; Mertes, S.; van Pinxteren, D.; Herrmann, H.; Borrmann, S.
Cloud residues and out-of-cloud aerosol particles with diameters between 150 and 900 nm were analysed by online single particle aerosol mass spectrometry during the 6-week study Hill Cap Cloud Thuringia (HCCT)-2010 in September–October 2010. The measurement location was the mountain Schmücke (937 m a.s.l.) in central Germany. More than 160 000 bipolar mass spectra from out-of-cloud aerosol particles and more than 13 000 bipolar mass spectra from cloud residual particles were obtained and were classified using a fuzzy c-means clustering algorithm. Analysis of the uncertainty of the sorting algorithm was conducted on a subset of the data by comparing the clustering output with particle-by-particle inspection and classification by the operator. This analysis yielded a false classification probability between 13 and 48 %. Additionally, particle types were identified by specific marker ions. The results from the ambient aerosol analysis show that 63 % of the analysed particles belong to clusters having a diurnal variation, suggesting that local or regional sources dominate the aerosol, especially for particles containing soot and biomass burning particles. In the cloud residues, the relative percentage of large soot-containing particles and particles containing amines was found to be increased compared to the out-of-cloud aerosol, while, in general, organic particles were less abundant in the cloud residues. In the case of amines, this can be explained by the high solubility of the amines, while the large soot-containing particles were found to be internally mixed with inorganics, which explains their activation as cloud condensation nuclei. Furthermore, the results show that during cloud processing, both sulfate and nitrate are added to the residual particles, thereby changing the mixing state and increasing the fraction of particles with nitrate and/or sulfate. This is expected to lead to higher hygroscopicity after cloud evaporation, and therefore to an increase of the particles' ability to act as cloud condensation nuclei after their cloud passage.
Assessment of cloud supersaturation by size-resolved aerosol particle and cloud condensation nuclei (CCN) measurements
(München : European Geopyhsical Union, 2014) Krüger, M.L.; Mertes, S.; Klimach, T.; Cheng, Y.F.; Su, H.; Schneider, J.; Andreae, M.O.; Pöschl, U.; Rose, D.
In this study we show how size-resolved measurements of aerosol particles and cloud condensation nuclei (CCN) can be used to characterize the supersaturation of water vapor in a cloud. The method was developed and applied during the ACRIDICON-Zugspitze campaign (17 September to 4 October 2012) at the high-Alpine research station Schneefernerhaus (German Alps, 2650 m a.s.l.). Number size distributions of total and interstitial aerosol particles were measured with a scanning mobility particle sizer (SMPS), and size-resolved CCN efficiency spectra were recorded with a CCN counter system operated at different supersaturation levels. During the evolution of a cloud, aerosol particles are exposed to different supersaturation levels. We outline and compare different estimates for the lower and upper bounds (Slow, Shigh) and the average value (Savg) of peak supersaturation encountered by the particles in the cloud. A major advantage of the derivation of Slow and Savg from size-resolved CCN efficiency spectra is that it does not require the specific knowledge or assumptions about aerosol hygroscopicity that are needed to derive estimates of Slow, Shigh, and Savg from aerosol size distribution data. For the investigated cloud event, we derived Slow ≈ 0.07–0.25%, Shigh ≈ 0.86–1.31% and Savg ≈ 0.42–0.68%.
Chemical composition of cloud water in the puerto rican tropical trade wind cumuli
(Dordrecht : Springer, 2009) Gioda, A.; Mayol-Bracero, O.L.; Morales-García, F.; Collett, J.; Decesari, S.; Emblico, L.; Facchini, M.C.; Morales-De Jesús, R.J.; Mertes, S.; Borrmann, S.; Walter, S.; Schneider, J.
As part of the Rain In Cumulus over the Ocean Experiment (RICO) and the Puerto Rico Aerosol and Cloud Study (PRACS), cloud water was collected at East Peak (EP) in Puerto Rico. The main objective of this study was to determine the concentrations of water-soluble species (Cl-, NO3 -, SO4 2-, NH4 +, Ca 2+, H+, Mg2+, K+, and Na +) in water samples taken from clouds influenced by tropical trade winds. The most abundant inorganic species were Na+ (average 465 μeq l-1) and Cl- (434 μeq l-1), followed by Mg2+ (105 μeq l-1), SO4 2- (61 μeq l-1), and NO3 - (25 μeq l -1). High concentrations of nss-SO4 2 (28 μeq l-1), NO3 - (86 μeq l-1), and H+ (14.5 μeq l-1) were measured with a shift in air masses origin from the North Atlantic to North American continent, which reflected a strong anthropogenic influence on cloud chemistry at EP. Long-range transport of particles and acid gases seems to be the factor responsible for fluctuations in concentrations and pH of cloud water at East Peak. When under trade wind influences the liquid phase concentrations of all inorganic substances were similar to those found in clouds in other clean maritime environments. © 2008 Springer Science+Business Media B.V.
Clouds and aerosols in Puerto Rico – a new evaluation
(München : European Geopyhsical Union, 2008) Allan, J.D.; Baumgardner, D.; Raga, G.B.; Mayol-Bracero, O.L.; Morales-García, F.; García-García, F.; Montero-Martínez, G.; Borrmann, S.; Schneider, J.; Mertes, S.; Walter, S.; Gysel, M.; Dusek, U.; Frank, G.P.; Krämer, M.
The influence of aerosols, both natural and anthropogenic, remains a major area of uncertainty when predicting the properties and behaviour of clouds and their influence on climate. In an attempt to better understand warm cloud formation in a tropical marine environment, a period of intensive measurements took place in December 2004 in Puerto Rico, using some of the latest developments in online instrumentation such as aerosol mass spectrometers, cloud condensation nuclei counters and a hygroscopicity tandem differential mobility analyser. Simultaneous online measurements of aerosol size distributions, composition, hygroscopicity and optical properties were made near the lighthouse of Cape San Juan in the north-eastern corner of the island and at the top of East Peak mountain (1040 m a.s.l.), the two sites separated by 17 km. Additional measurements of the cloud droplet residual and interstitial aerosol properties were made at the mountain site, accompanied by measurements of cloud droplet size distributions, liquid water content and the chemical composition of cloud and rain water samples. Both aerosol composition and cloud properties were found to be sensitive to wind sector. Air from the east-northeast (ENE) was mostly free of anthropogenic influences, the submicron fraction being mainly composed of non-sea salt sulphate, while that from the east-southeast (ESE) was found to be moderately influenced by populated islands upwind, adding smaller (<100 nm), externally mixed, carbonaceous particles to the aerosol that increased the number concentrations by over a factor of 3. This change in composition was also accompanied with a reduction in the measured hygroscopicity and fractional cloud activation potential of the aerosol. At the mountain site, the average cloud droplet concentrations increased from 193 to 519 cm−3, median volume diameter decreased from 20 to 14 μm and the liquid water content increased from 0.24 to 0.31 g m−3 when the winds shifted from the ENE to ESE. Larger numbers of interstitial particles were recorded, most notably at sizes greater than 100 nm, which were absent during clean conditions. The average size of the residual particles and concentrations of cloudwater nitrate, sulphate and insoluble material increased during polluted conditions. Previous studies in Puerto Rico had reported the presence of a significant non-anthropogenic organic fraction in the aerosols measured and concluded that this was a factor controlling the in situ cloud properties. However, this was not observed in our case. In contrast to the 1.00±0.14 μg m−3 of organic carbon measured in 1992 and 1995, the organic matter measured in the current study of 0.17±0.35 μg m−3 is many times lower, most of which can be attributed to anthropogenic sources. During clean conditions, the submicron aerosol was observed to be almost entirely inorganic, an observation supported by the hygroscopicity measurements. This suggests that organic aerosols from marine sources may not be completely ubiquitous (either spatially or temporally) in this environment and requires further investigation to quantify their true extent and implications, with more extensive, longer-term sampling in conjunction with wind field analyses.
Coal fly ash: Linking immersion freezing behavior and physicochemical particle properties
(Göttingen : Copernicus GmbH, 2018) Grawe, S.; Augustin-Bauditz, S.; Clemen, H.-C.; Ebert, M.; Eriksen Hammer, S.; Lubitz, J.; Reicher, N.; Rudich, Y.; Schneider, J.; Staacke, R.; Stratmann, F.; Welti, A.; Wex, H.
To date, only a few studies have investigated the potential of coal fly ash particles to trigger heterogeneous ice nucleation in cloud droplets. The presented measurements aim at expanding the sparse dataset and improving process understanding of how physicochemical particle properties can influence the freezing behavior of coal fly ash particles immersed in water. Firstly, immersion freezing measurements were performed with two single particle techniques, i.e., the Leipzig Aerosol Cloud Interaction Simulator (LACIS) and the SPectrometer for Ice Nuclei (SPIN). The effect of suspension time on the efficiency of the coal fly ash particles when immersed in a cloud droplet is analyzed based on the different residence times of the two instruments and employing both dry and wet particle generation. Secondly, two cold-stage setups, one using microliter sized droplets (Leipzig Ice Nucleation Array) and one using nanoliter sized droplets (WeIzmann Supercooled Droplets Observation on Microarray setup) were applied. We found that coal fly ash particles are comparable to mineral dust in their immersion freezing behavior when being dry generated. However, a significant decrease in immersion freezing efficiency was observed during experiments with wet-generated particles in LACIS and SPIN. The efficiency of wet-generated particles is in agreement with the cold-stage measurements. In order to understand the reason behind the deactivation, a series of chemical composition, morphology, and crystallography analyses (single particle mass spectrometry, scanning electron microscopy coupled with energy dispersive X-ray microanalysis, X-ray diffraction analysis) were performed with dry- and wet-generated particles. From these investigations, we conclude that anhydrous CaSO4 and CaO - which, if investigated in pure form, show the same qualitative immersion freezing behavior as observed for dry-generated coal fly ash particles - contribute to triggering heterogeneous ice nucleation at the particle-water interface. The observed deactivation in contact with water is related to changes in the particle surface properties which are potentially caused by hydration of CaSO4 and CaO. The contribution of coal fly ash to the ambient population of ice-nucleating particles therefore depends on whether and for how long particles are immersed in cloud droplets.
Comprehensive assessment of meteorological conditions and airflow connectivity during HCCT-2010
(München : European Geopyhsical Union, 2014) Tilgner, A.; Schöne, L.; Bräuer, P.; van Pinxteren, D.; Hoffmann, E.; Spindler, G.; Styler, S.A.; Mertes, S.; Birmili, W.; Otto, R.; Merkel, M.; Weinhold, K.; Wiedensohler, A.; Deneke, H.; Schrödner, R.; Wolke, R.; Schneider, J.; Haunold, W.; Engel, A.; Wéber, A.; Herrmann, H.
This study presents a comprehensive assessment of the meteorological conditions and atmospheric flow during the Lagrangian-type "Hill Cap Cloud Thuringia 2010" experiment (HCCT-2010), which was performed in September and October 2010 at Mt. Schmücke in the Thuringian Forest, Germany and which used observations at three measurement sites (upwind, in-cloud, and downwind) to study physical and chemical aerosol–cloud interactions. A Lagrangian-type hill cap cloud experiment requires not only suitable cloud conditions but also connected airflow conditions (i.e. representative air masses at the different measurement sites). The primary goal of the present study was to identify time periods during the 6-week duration of the experiment in which these conditions were fulfilled and therefore which are suitable for use in further data examinations. The following topics were studied in detail: (i) the general synoptic weather situations, including the mesoscale flow conditions, (ii) local meteorological conditions and (iii) local flow conditions. The latter were investigated by means of statistical analyses using best-available quasi-inert tracers, SF6 tracer experiments in the experiment area, and regional modelling. This study represents the first application of comprehensive analyses using statistical measures such as the coefficient of divergence (COD) and the cross-correlation in the context of a Lagrangian-type hill cap cloud experiment. This comprehensive examination of local flow connectivity yielded a total of 14 full-cloud events (FCEs), which are defined as periods during which all connected flow and cloud criteria for a suitable Lagrangian-type experiment were fulfilled, and 15 non-cloud events (NCEs), which are defined as periods with connected flow but no cloud at the summit site, and which can be used as reference cases. The overall evaluation of the identified FCEs provides the basis for subsequent investigations of the measured chemical and physical data during HCCT-2010 (see https://www.atmos-chem-phys.net/special_issue287.html).
Experimental study of the role of physicochemical surface processing on the IN ability of mineral dust particles
(München : European Geopyhsical Union, 2011) Niedermeier, D.; Hartmann, S.; Clauss, T.; Wex, H.; Kiselev, A.; Sullivan, R.C.; DeMott, P.J.; Petters, M.D.; Reitz, P.; Schneider, J.; Mikhailov, E.; Sierau, B.; Stetzer, O.; Reimann, B.; Bundke, U.; Shaw, R.A.; Buchholz, A.; Mentel, T.F.; Stratmann, F.
During the measurement campaign FROST 2 (FReezing Of duST 2), the Leipzig Aerosol Cloud Interaction Simulator (LACIS) was used to investigate the influence of various surface modifications on the ice nucleating ability of Arizona Test Dust (ATD) particles in the immersion freezing mode. The dust particles were exposed to sulfuric acid vapor, to water vapor with and without the addition of ammonia gas, and heat using a thermodenuder operating at 250 °C. Size selected, quasi monodisperse particles with a mobility diameter of 300 nm were fed into LACIS and droplets grew on these particles such that each droplet contained a single particle. Temperature dependent frozen fractions of these droplets were determined in a temperature range between −40 °C ≤T≤−28 °C. The pure ATD particles nucleated ice over a broad temperature range with their freezing behavior being separated into two freezing branches characterized through different slopes in the frozen fraction vs. temperature curves. Coating the ATD particles with sulfuric acid resulted in the particles' IN potential significantly decreasing in the first freezing branch (T>−35 °C) and a slight increase in the second branch (T≤−35 °C). The addition of water vapor after the sulfuric acid coating caused the disappearance of the first freezing branch and a strong reduction of the IN ability in the second freezing branch. The presence of ammonia gas during water vapor exposure had a negligible effect on the particles' IN ability compared to the effect of water vapor. Heating in the thermodenuder led to a decreased IN ability of the sulfuric acid coated particles for both branches but the additional heat did not or only slightly change the IN ability of the pure ATD and the water vapor exposed sulfuric acid coated particles. In other words, the combination of both sulfuric acid and water vapor being present is a main cause for the ice active surface features of the ATD particles being destroyed. A possible explanation could be the chemical transformation of ice active metal silicates to metal sulfates. The strongly enhanced reaction between sulfuric acid and dust in the presence of water vapor and the resulting significant reductions in IN potential are of importance for atmospheric ice cloud formation. Our findings suggest that the IN concentration can decrease by up to one order of magnitude for the conditions investigated.
Formation of organic aerosol in the Paris region during the MEGAPOLI summer campaign: Evaluation of the volatility-basis-set approach within the CHIMERE model
(Göttingen : Copernicus, 2013) Zhang, Q.J.; Beekmann, M.; Drewnick, F.; Freutel, F.; Schneider, J.; Crippa, M.; Prevot, A.S.H.; Baltensperger, U.; Poulain, L.; Wiedensohler, A.; Sciare, J.; Gros, V.; Borbon, A.; Colomb, A.; Michoud, V.; Doussin, J.-F.; Denier Van Der Gon, H.A.C.; Haeffelin, M.; Dupont, J.-C.; Siour, G.; Petetin, H.; Bessagnet, B.; Pandis, S.N.; Hodzic, A.; Sanchez, O.; Honoré, C.; Perrussel, O.
Simulations with the chemistry transport model CHIMERE are compared to measurements performed during the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) summer campaign in the Greater Paris region in July 2009. The volatility-basis-set approach (VBS) is implemented into this model, taking into account the volatility of primary organic aerosol (POA) and the chemical aging of semi-volatile organic species. Organic aerosol is the main focus and is simulated with three different configurations with a modified treatment of POA volatility and modified secondary organic aerosol (SOA) formation schemes. In addition, two types of emission inventories are used as model input in order to test the uncertainty related to the emissions. Predictions of basic meteorological parameters and primary and secondary pollutant concentrations are evaluated, and four pollution regimes are defined according to the air mass origin. Primary pollutants are generally overestimated, while ozone is consistent with observations. Sulfate is generally overestimated, while ammonium and nitrate levels are well simulated with the refined emission data set. As expected, the simulation with non-volatile POA and a single-step SOA formation mechanism largely overestimates POA and underestimates SOA. Simulation of organic aerosol with the VBS approach taking into account the aging of semi-volatile organic compounds (SVOC) shows the best correlation with measurements. High-concentration events observed mostly after long-range transport are well reproduced by the model. Depending on the emission inventory used, simulated POA levels are either reasonable or underestimated, while SOA levels tend to be overestimated. Several uncertainties related to the VBS scheme (POA volatility, SOA yields, the aging parameterization), to emission input data, and to simulated OH levels can be responsible for this behavior. Despite these uncertainties, the implementation of the VBS scheme into the CHIMERE model allowed for much more realistic organic aerosol simulations for Paris during summertime. The advection of SOA from outside Paris is mostly responsible for the highest OA concentration levels. During advection of polluted air masses from northeast (Benelux and Central Europe), simulations indicate high levels of both anthropogenic and biogenic SOA fractions, while biogenic SOA dominates during periods with advection from Southern France and Spain.
Heterogeneous freezing of droplets with immersed mineral dust particles – measurements and parameterization
(München : European Geopyhsical Union, 2010) Niedermeier, D.; Hartmann, S.; Shaw, R.A.; Covert, D.; Mentel, T.F.; Schneider, J.; Mentel, T.F.; Poulain, L.; Reitz, P.; Spindler, C.; Clauss, T.; Kiselev, A.; Hallbauer, E.; Wex, H.; Mildenberger, K.; Stratmann, F.
During the measurement campaign FROST (FReezing Of duST), LACIS (Leipzig Aerosol Cloud Interaction Simulator) was used to investigate the immersion freezing behavior of size selected, coated and uncoated Arizona Test Dust (ATD) particles with a mobility diameter of 300 nm. Particles were coated with succinic acid (C4H6O4), sulfuric acid (H2SO4) and ammonium sulfate ((NH4)2SO4). Ice fractions at mixed-phase cloud temperatures ranging from 233.15 K to 239.15 K (±0.60 K) were determined for all types of particles. In this temperature range, pure ATD particles and those coated with C4H6O4 or small amounts of H2SO4 were found to be the most efficient ice nuclei (IN). ATD particles coated with (NH4)2SO4 were the most inefficient IN. Since the supercooled droplets were highly diluted before freezing occurred, a freezing point suppression due to the soluble material on the particles (and therefore in the droplets) cannot explain this observation. Therefore, it is reasonable to assume that the coatings lead to particle surface alterations which cause the differences in the IN abilities. Two different theoretical approaches based on the stochastic and the singular hypotheses were applied to clarify and parameterize the freezing behavior of the particles investigated. Both approaches describe the experimentally determined results, yielding parameters that can subsequently be used to compare our results to those from other studies. However, we cannot clarify at the current state which of the two approaches correctly describes the investigated immersion freezing process. But both approaches confirm the assumption that the coatings lead to particle surface modifications lowering the nucleation efficiency. The stochastic approach interprets the reduction in nucleation rate from coating as primarily due to an increase in the thermodynamic barrier for ice formation (i.e., changes in interfacial free energies). The singular approach interprets the reduction as resulting from a reduced surface density of active sites.
The impact of mineral dust on cloud formation during the Saharan dust event in April 2014 over Europe
(Göttingen : Copernicus GmbH, 2018) Weger, M.; Heinold, B.; Engler, C.; Schumann, U.; Seifert, A.; Fößig, R.; Voigt, C.; Baars, H.; Blahak, U.; Borrmann, S.; Hoose, C.; Kaufmann, S.; Krämer, M.; Seifert, P.; Senf, F.; Schneider, J.; Tegen, I.
A regional modeling study on the impact of desert dust on cloud formation is presented for a major Saharan dust outbreak over Europe from 2 to 5 April 2014. The dust event coincided with an extensive and dense cirrus cloud layer, suggesting an influence of dust on atmospheric ice nucleation. Using interactive simulation with the regional dust model COSMO-MUSCAT, we investigate cloud and precipitation representation in the model and test the sensitivity of cloud parameters to dust-cloud and dust-radiation interactions of the simulated dust plume. We evaluate model results with ground-based and spaceborne remote sensing measurements of aerosol and cloud properties, as well as the in situ measurements obtained during the ML-CIRRUS aircraft campaign. A run of the model with single-moment bulk microphysics without online dust feedback considerably underestimated cirrus cloud cover over Germany in the comparison with infrared satellite imagery. This was also reflected in simulated upper-Tropospheric ice water content (IWC), which accounted for only 20 % of the observed values. The interactive dust simulation with COSMO-MUSCAT, including a two-moment bulk microphysics scheme and dust-cloud as well as dust-radiation feedback, in contrast, led to significant improvements. The modeled cirrus cloud cover and IWC were by at least a factor of 2 higher in the relevant altitudes compared to the noninteractive model run. We attributed these improvements mainly to enhanced deposition freezing in response to the high mineral dust concentrations. This was corroborated further in a significant decrease in ice particle radii towards more realistic values, compared to in situ measurements from the ML-CIRRUS aircraft campaign. By testing different empirical ice nucleation parameterizations, we further demonstrate that remaining uncertainties in the ice-nucleating properties of mineral dust affect the model performance at least as significantly as including the online representation of the mineral dust distribution. Dust-radiation interactions played a secondary role for cirrus cloud formation, but contributed to a more realistic representation of precipitation by suppressing moist convection in southern Germany. In addition, a too-low specific humidity in the 7 to 10 km altitude range in the boundary conditions was identified as one of the main reasons for misrepresentation of cirrus clouds in this model study.
In situ, satellite measurement and model evidence on the dominant regional contribution to fine particulate matter levels in the Paris megacity
(Katlenburg-Lindau : EGU, 2015) Beekmann, M.; Prévôt, A.S.H.; Drewnick, F.; Sciare, J.; Pandis, S.N.; Denier van der Gon, H.A.C.; Crippa, M.; Freutel, F.; Poulain, L.; Ghersi, V.; Rodriguez, E.; Beirle, S.; Zotter, P.; von der Weiden-Reinmüller, S.-L.; Bressi, M.; Fountoukis, C.; Petetin, H.; Szidat, S.; Schneider, J.; Rosso, A.; El Haddad, I.; Megaritis, A.; Zhang, Q.J.; Michoud, V.; Slowik, J.G.; Moukhtar, S.; Kolmonen, P.; Stohl, A.; Eckhardt, S.; Borbon, A.; Gros, V.; Marchand, N.; Jaffrezo, J.L.; Schwarzenboeck, A.; Colomb, A.; Wiedensohler, A.; Borrmann, S.; Lawrence, M.; Baklanov, A.; Baltensperger, U.
A detailed characterization of air quality in the megacity of Paris (France) during two 1-month intensive campaigns and from additional 1-year observations revealed that about 70 % of the urban background fine particulate matter (PM) is transported on average into the megacity from upwind regions. This dominant influence of regional sources was confirmed by in situ measurements during short intensive and longer-term campaigns, aerosol optical depth (AOD) measurements from ENVISAT, and modeling results from PMCAMx and CHIMERE chemistry transport models. While advection of sulfate is well documented for other megacities, there was surprisingly high contribution from long-range transport for both nitrate and organic aerosol. The origin of organic PM was investigated by comprehensive analysis of aerosol mass spectrometer (AMS), radiocarbon and tracer measurements during two intensive campaigns. Primary fossil fuel combustion emissions constituted less than 20 % in winter and 40 % in summer of carbonaceous fine PM, unexpectedly small for a megacity. Cooking activities and, during winter, residential wood burning are the major primary organic PM sources. This analysis suggests that the major part of secondary organic aerosol is of modern origin, i.e., from biogenic precursors and from wood burning. Black carbon concentrations are on the lower end of values encountered in megacities worldwide, but still represent an issue for air quality. These comparatively low air pollution levels are due to a combination of low emissions per inhabitant, flat terrain, and a meteorology that is in general not conducive to local pollution build-up. This revised picture of a megacity only being partially responsible for its own average and peak PM levels has important implications for air pollution regulation policies.
In-cloud sulfate addition to single particles resolved with sulfur isotope analysis during HCCT-2010
(München : European Geopyhsical Union, 2014) Harris, E.; Sinha, B.; van Pinxteren, D.; Schneider, J.; Poulain, L.; Collett, J.; D'Anna, B.; Fahlbusch, B.; Foley, S.; Fomba, K.W.; George, C.; Gnauk, T.; Henning, S.; Lee, T.; Mertes, S.; Roth, A.; Stratmann, F.; Borrmann, S.; Hoppe, P.; Herrmann, H.
In-cloud production of sulfate modifies aerosol size distribution, with important implications for the magnitude of indirect and direct aerosol cooling and the impact of SO2 emissions on the environment. We investigate which sulfate sources dominate the in-cloud addition of sulfate to different particle classes as an air parcel passes through an orographic cloud. Sulfate aerosol, SO2 and H2SO4 were collected upwind, in-cloud and downwind of an orographic cloud for three cloud measurement events during the Hill Cap Cloud Thuringia campaign in autumn 2010 (HCCT-2010). Combined SEM and NanoSIMS analysis of single particles allowed the δ34S of particulate sulfate to be resolved for particle size and type. The most important in-cloud SO2 oxidation pathway at HCCT-2010 was aqueous oxidation catalysed by transition metal ions (TMI catalysis), which was shown with single particle isotope analyses to occur primarily in cloud droplets nucleated on coarse mineral dust. In contrast, direct uptake of H2SO4 (g) and ultrafine particulate were the most important sources modifying fine mineral dust, increasing its hygroscopicity and facilitating activation. Sulfate addition to "mixed" particles (secondary organic and inorganic aerosol) and coated soot was dominated by in-cloud aqueous SO2 oxidation by H2O2 and direct uptake of H2SO4 (g) and ultrafine particle sulfate, depending on particle size mode and time of day. These results provide new insight into in-cloud sulfate production mechanisms, and show the importance of single particle measurements and models to accurately assess the environmental effects of cloud processing.
Irreversible loss of ice nucleation active sites in mineral dust particles caused by sulphuric acid condensation
(München : European Geopyhsical Union, 2010) Sullivan, R.C.; Petters, M.D.; DeMott, P.J.; Kreidenweis, S.M.; Wex, H.; Niedermeier, D.; Hartmann, S.; Clauss, T.; Stratmann, F.; Reitz, P.; Schneider, J.; Sierau, B.
During the FROST-2 (FReezing Of duST) measurement campaign conducted at the Leipzig Aerosol Cloud Interaction Simulator (LACIS), we investigated changes in the ice nucleation properties of 300 nm Arizona Test Dust mineral particles following thermochemical processing by varying amounts and combinations of exposure to sulphuric acid vapour, ammonia gas, water vapour, and heat. The processed particles' heterogeneous ice nucleation properties were determined in both the water subsaturated and supersaturated humidity regimes at −30 °C and −25 °C using Colorado State University's continuous flow diffusion chamber. The amount of sulphuric acid coating material was estimated by an aerosol mass spectrometer and from CCN-derived hygroscopicity measurements. The condensation of sulphuric acid decreased the dust particles' ice nucleation ability in proportion to the amount of sulphuric acid added. Heating the coated particles in a thermodenuder at 250 °C – intended to evaporate the sulphuric acid coating – reduced their freezing ability even further. We attribute this behaviour to accelerated acid digestion of ice active surface sites by heat. Exposing sulphuric acid coated dust to ammonia gas produced particles with similarly poor freezing potential; however a portion of their ice nucleation ability could be restored after heating in the thermodenuder. In no case did any combination of thermochemical treatments increase the ice nucleation ability of the coated mineral dust particles compared to unprocessed dust. These first measurements of the effect of identical chemical processing of dust particles on their ice nucleation ability under both water subsaturated and mixed-phase supersaturated cloud conditions revealed that ice nucleation was more sensitive to all coating treatments in the water subsaturated regime. The results clearly indicate irreversible impairment of ice nucleation activity in both regimes after condensation of concentrated sulphuric acid. This implies that the sulphuric acid coating caused permanent chemical and/or physical modification of the ice active surface s
Mass-spectrometric identification of primary biological particle markers and application to pristine submicron aerosol measurements in Amazonia
(München : European Geopyhsical Union, 2011) Schneider, J.; Freutel, F.; Zorn, S.R.; Chen, Q.; Farmer, D.K.; Jimenez, J.L.; Martin, S.T.; Artaxo, P.; Wiedensohler, A.; Borrmann, S.
The detection of primary biological material in submicron aerosol by means of thermal desorption/electron impact ionization aerosol mass spectrometry was investigated. Mass spectra of amino acids, carbohydrates, small peptides, and proteins, all of which are key building blocks of biological particles, were recorded in laboratory experiments. Several characteristic marker fragments were identified. The intensity of the marker signals relative to the total organic mass spectrum allows for an estimation of the content of primary biological material in ambient organic aerosol. The developed method was applied to mass spectra recorded during AMAZE-08, a field campaign conducted in the pristine rainforest of the central Amazon Basin, Brazil, during the wet season of February and March 2008. The low abundance of identified marker fragments places upper limits of 7.5% for amino acids and 5.6% for carbohydrates on the contribution of primary biological aerosol particles (PBAP) to the submicron organic aerosol mass concentration during this time period. Upper limits for the absolute submicron concentrations for both compound classes range from 0.01 to 0.1 μg m−3. Carbohydrates and proteins (composed of amino acids) make up for about two thirds of the dry mass of a biological cell. Thus, our findings suggest an upper limit for the PBAP mass fraction of about 20% to the submicron organic aerosol measured in Amazonia during AMAZE-08.
An overview of the Amazonian Aerosol Characterization Experiment 2008 (AMAZE-08)
(München : European Geopyhsical Union, 2010) Martin, S.T.; Andreae, M.O.; Althausen, D.; Artaxo, P.; Baars, H.; Borrmann, S.; Chen, Q.; Farmer, D.K.; Guenther, A.; Gunthe, S.S.; Jimenez, J.L.; Karl, T.; Longo, K.; Manzi, A.; Müller, T.; Pauliquevis, T.; Petters, M.D.; Prenni, A.J.; Pöschl, U.; Rizzo, L.V.; Schneider, J.; Smith, J.N.; Swietlicki, E.; Tota, J.; Wang, J.; Wiedensohler, A.; Zorn, S.R.
The Amazon Basin provides an excellent environment for studying the sources, transformations, and properties of natural aerosol particles and the resulting links between biological processes and climate. With this framework in mind, the Amazonian Aerosol Characterization Experiment (AMAZE-08), carried out from 7 February to 14 March 2008 during the wet season in the central Amazon Basin, sought to understand the formation, transformations, and cloud-forming properties of fine- and coarse-mode biogenic aerosol particles, especially as related to their effects on cloud activation and regional climate. Special foci included (1) the production mechanisms of secondary organic components at a pristine continental site, including the factors regulating their temporal variability, and (2) predicting and understanding the cloud-forming properties of biogenic particles at such a site. In this overview paper, the field site and the instrumentation employed during the campaign are introduced. Observations and findings are reported, including the large-scale context for the campaign, especially as provided by satellite observations. New findings presented include: (i) a particle number-diameter distribution from 10 nm to 10 μm that is representative of the pristine tropical rain forest and recommended for model use; (ii) the absence of substantial quantities of primary biological particles in the submicron mode as evidenced by mass spectral characterization; (iii) the large-scale production of secondary organic material; (iv) insights into the chemical and physical properties of the particles as revealed by thermodenuder-induced changes in the particle number-diameter distributions and mass spectra; and (v) comparisons of ground-based predictions and satellite-based observations of hydrometeor phase in clouds. A main finding of AMAZE-08 is the dominance of secondary organic material as particle components. The results presented here provide mechanistic insight and quantitative parameters that can serve to increase the accuracy of models of the formation, transformations, and cloud-forming properties of biogenic natural aerosol particles, especially as related to their effects on cloud activation and regional climate.
Planets, candidates, and binaries from the CoRoT/Exoplanet programme: The CoRoT transit catalogue
(Les Ulis : EDP Sciences, 2018) Deleuil, M.; Aigrain, S.; Moutou, C.; Cabrera, J.; Bouchy, F.; Deeg, H. J.; Almenara, J.-M.; Hébrard, G.; Santerne, A.; Alonso, R.; Bonomo, A.S.; Bordé, P.; Csizmadia, S.; Dìaz, R.F.; Erikson, A.; Fridlund, M.; Gandolfi, D.; Guenther, E.; Guillot, T.; Guterman, P.; Grziwa, S.; Hatzes, A.; Léger, A.; Mazeh, T.; Ofir, A.; Ollivier, M.; Pätzold, M.; Parviainen, H.; Rauer, H.; Rouan, D.; Schneider, J.; Titz-Weider, R.; Tingley, B.; Weingrill, J.
The CoRoT space mission observed 163 665 stars over 26 stellar fields in the faint star channel. The exoplanet teams detected a total of 4123 transit-like features in the 177 454 light curves. We present the complete re-analysis of all these detections carried out with the same softwares so that to ensure their homogeneous analysis. Although the vetting process involves some human evaluation, it also involves a simple binary flag system over basic tests: Detection significance, presence of a secondary, difference between odd and even depths, colour dependence, V-shape transit, and duration of the transit. We also gathered the information from the large accompanying ground-based programme carried out on the planet candidates and checked how useful the flag system could have been at the vetting stage of the candidates. From the initial list of transit-like features, we identified and separated 824 false alarms of various kind, 2269 eclipsing binaries among which 616 are contact binaries and 1653 are detached ones, 37 planets and brown dwarfs, and 557 planet candidates. We provide the catalogue of all these transit-like features, including false alarms. For the planet candidates, the catalogue gives not only their transit parameters but also the products of their light curve modelling: Reduced radius, reduced semi-major axis, and impact parameter, together with a summary of the outcome of follow-up observations when carried out and their current status. For the detached eclipsing binaries, the catalogue provides, in addition to their transit parameters, a simple visual classification. Among the planet candidates whose nature remains unresolved, we estimate that eight (within an error of three) planets are still to be identified. After correcting for geometric and sensitivity biases, we derived planet and brown dwarf occurrences and confirm disagreements with Kepler estimates, as previously reported by other authors from the analysis of the first runs: Small-size planets with orbital period less than ten days are underabundant by a factor of three in the CoRoT fields whereas giant planets are overabundant by a factor of two. These preliminary results would however deserve further investigations using the recently released CoRoT light curves that are corrected of the various instrumental effects and a homogeneous analysis of the stellar populations observed by the two missions.
Single-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.
Surface modification of mineral dust particles by sulphuric acid processing: Implications for ice nucleation abilities
(München : European Geopyhsical Union, 2011) Reitz, P.; Spindler, C.; Mentel, T.F.; Poulain, L.; Wex, H.; Mildenberger, K.; Niedermeier, D.; Hartmann, S.; Clauss, T.; Stratmann, F.; Sullivan, R.C.; DeMott, P.J.; Petters, M.D.; Sierau, B.; Schneider, J.
The ability of coated mineral dust particles to act as ice nuclei (IN) was investigated at LACIS (Leipzig Aerosol Cloud Interaction Simulator) during the FROST1- and FROST2-campaigns (Freezing of dust). Sulphuric acid was condensed on the particles which afterwards were optionally humidified, treated with ammonia vapour and/or heat. By means of aerosol mass spectrometry we found evidence that processing of mineral dust particles with sulphuric acid leads to surface modifications of the particles. These surface modifications are most likely responsible for the observed reduction of the IN activation of the particles. The observed particle mass spectra suggest that different treatments lead to different chemical reactions on the particle surface. Possible chemical reaction pathways and products are suggested and the implications on the IN efficiency of the treated dust particles are discussed.
Three years of routine Raman lidar measurements of tropospheric aerosols: Backscattering, extinction, and residual layer height
(Göttingen : Copernicus GmbH, 2002) Schneider, J.; Eixmann, R.
We have performed a three-year series of routine lidar measurements at preselected times. The measurements were performed between 1 December 1997, and 30 November 2000, at Kühlungsborn, Germany (54°07′N, 11°46′E). Using a Rayleigh/Mie/Raman lidar system, we measured the aerosol backscatter coefficients at three wavelengths and the extinction coefficient at one wavelength. The present data analysis focuses on after-sunset Raman measurements obtained on cloud-free days. Aerosol backscatter profiles are available for altitudes above 100 m, while the majority of the extinction measurements has been restricted to heights above the residual layer. The residual layer shows an annual cycle with its maximum height in summer (2000 m) and minimum height in winter (850 m). The backscatter coefficients in the residual layer were found to be about 10 times higher than above. The mean aerosol optical depth above the residual layer and below 5 km is 0.3(±1.0) × 10-2 in summer, and 1.5(±1.0) × 10-2 in winter, which almost is negligible compared to values measured in during daytime in the planetary boundary layer. A cluster analysis of the backward trajectories yielded two major directions of air mass origin above the residual layer and 4 major directions inside. A marked difference between the aerosol properties dependent on the air mass origin could be found for air masses originating from the west and travelling at high wind speeds. Comparing the measured spectral dependence of the backscatter coefficients with data from the Global Aerosol Data Set, we found a general agreement, but only a few conclusions with respect to the aerosol type could be drawn due to the high variability of the measured backscatter coefficients.

Browsing by Author "Schneider, J."

Results Per Page

Sort Options