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- ItemEvaluation of the shortwave cloud radiative effect over the ocean by use of ship and satellite observations(München : European Geopyhsical Union, 2012) Hanschmann, T.; Deneke, H.; Roebeling, R.; Macke, A.In this study the shortwave cloud radiative effect (SWCRE) over ocean calculated by the ECHAM 5 climate model is evaluated for the cloud property input derived from ship based measurements and satellite based estimates and compared to ship based radiation measurements. The ship observations yield cloud fraction, liquid water path from a microwave radiometer, cloud bottom height as well as temperature and humidity profiles from radiosonde ascents. Level-2 products of the Satellite Application Facility on Climate Monitoring (CM~SAF) from the Spinning Enhanced Visible and InfraRed Imager (SEVIRI) have been used to characterize clouds. Within a closure study six different experiments have been defined to find the optimal set of measurements to calculate downward shortwave radiation (DSR) and the SWCRE from the model, and their results have been evaluated under seven different synoptic situations. Four of these experiments are defined to investigate the advantage of including the satellite-based cloud droplet effective radius as additional cloud property. The modeled SWCRE based on satellite retrieved cloud properties has a comparable accuracy to the modeled SWCRE based on ship data. For several cases, an improvement through introducing the satellite-based estimate of effective radius as additional information to the ship based data was found. Due to their different measuring characteristics, however, each dataset shows best results for different atmospheric conditions.
- ItemTrace metal characterization of aerosol particles and cloud water during HCCT 2010(München : European Geopyhsical Union, 2015) Fomba, K.W.; van Pinxteren, D.; Müller, K.; Iinuma, Y.; Lee, T.; Collett Jr., J.L.; Herrmann, H.Trace metal characterization of bulk and size-resolved aerosol and cloud water samples were performed during the Hill Cap Cloud Thuringia (HCCT) campaign. Cloud water was collected at the top of Mt. Schmücke while aerosol samples were collected at two stations upwind and downwind of Mt. Schmücke. Fourteen trace metals including Ti, V, Fe, Mn, Co, Zn, Ni, Cu, As, Sr, Rb, Pb, Cr, and Se were investigated during four full cloud events (FCEs) that fulfilled the conditions of a continuous air mass flow through the three stations. Aerosol particle trace metal concentrations were found to be lower than those observed in the same region during previous field experiments but were within a similar range to those observed in other rural regions in Europe. Fe and Zn were the most abundant elements with concentration ranges of 0.2–111.6 and 1.1–32.1 ng m−3, respectively. Fe, Mn, and Ti were mainly found in coarse mode aerosols while Zn, Pb, and As were mostly found in the fine mode. Correlation and enrichment factor analysis of trace metals revealed that trace metals such as Ti and Rb were mostly of crustal origin while trace metals such as Zn, Pb, As, Cr, Ni, V, and Cu were of anthropogenic origin. Trace metals such as Fe and Mn were of mixed origins including crustal and combustion sources. Trace metal cloud water concentration decreased from Ti, Mn, Cr, to Co with average concentrations of 9.18, 5.59, 5.54, and 0.46 μg L−1, respectively. A non-uniform distribution of soluble Fe, Cu, and Mn was observed across the cloud drop sizes. Soluble Fe and Cu were found mainly in cloud droplets with diameters between 16 and 22 μm, while Mn was found mostly in larger drops greater than 22 μm. Fe(III) was the main form of soluble Fe especially in the small and larger drops with concentrations ranging from 2.2 to 37.1 μg L−1. In contrast to other studies, Fe(II) was observed mainly in the evening hours, implying its presence was not directly related to photochemical processes. Aerosol–cloud interaction did not lead to a marked increase in soluble trace metal concentrations; rather it led to differences in the chemical composition of the aerosol due to preferential loss of aerosol particles through physical processes including cloud drop deposition to vegetative surfaces.
- ItemResults from the CERN pilot CLOUD experiment(München : European Geopyhsical Union, 2010) Duplissy, J.; Enghoff, M.B.; Aplin, K.L.; Arnold, F.; Aufmhoff, H.; Avngaard, M.; Baltensperger, U.; Bondo, T.; Bingham, R.; Carslaw, K.; Curtius, J.; David, A.; Fastrup, B.; Gagné, S.; Hahn, F.; Harrison, R.G.; Kellett, B.; Kirkby, J.; Kulmala, M.; Laakso, L.; Laaksonen, A.; Lillestol, E.; Lockwood, M.; Mäkelä, J.; Makhmutov, V.; Marsh, N.D.; Nieminen, T.; Onnela, A.; Pedersen, E.; Pedersen, J.O.P.; Polny, J.; Reichl, U.; Seinfeld, J.H.; Sipilä, M.; Stozhkov, Y.; Stratmann, F.; Svensmark, H.; Svensmark, J.; Veenhof, R.; Verheggen, B.; Viisanen, Y.; Wagner, P.E.; Wehrle, G.; Weingartner, E.; Wex, H.; Wilhelmsson, M.; Winkler, P.M.During a 4-week run in October–November 2006, a pilot experiment was performed at the CERN Proton Synchrotron in preparation for the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment, whose aim is to study the possible influence of cosmic rays on clouds. The purpose of the pilot experiment was firstly to carry out exploratory measurements of the effect of ionising particle radiation on aerosol formation from trace H2SO4 vapour and secondly to provide technical input for the CLOUD design. A total of 44 nucleation bursts were produced and recorded, with formation rates of particles above the 3 nm detection threshold of between 0.1 and 100 cm−3s−1, and growth rates between 2 and 37 nm h−1. The corresponding H2O concentrations were typically around 106 cm−3 or less. The experimentally-measured formation rates and \htwosofour concentrations are comparable to those found in the atmosphere, supporting the idea that sulphuric acid is involved in the nucleation of atmospheric aerosols. However, sulphuric acid alone is not able to explain the observed rapid growth rates, which suggests the presence of additional trace vapours in the aerosol chamber, whose identity is unknown. By analysing the charged fraction, a few of the aerosol bursts appear to have a contribution from ion-induced nucleation and ion-ion recombination to form neutral clusters. Some indications were also found for the accelerator beam timing and intensity to influence the aerosol particle formation rate at the highest experimental SO2 concentrations of 6 ppb, although none was found at lower concentrations. Overall, the exploratory measurements provide suggestive evidence for ion-induced nucleation or ion-ion recombination as sources of aerosol particles. However in order to quantify the conditions under which ion processes become significant, improvements are needed in controlling the experimental variables and in the reproducibility of the experiments. Finally, concerning technical aspects, the most important lessons for the CLOUD design include the stringent requirement of internal cleanliness of the aerosol chamber, as well as maintenance of extremely stable temperatures (variations below 0.1 °C
- ItemTemporal evolution of stable water isotopologues in cloud droplets in a hill cap cloud in central Europe (HCCT-2010)(München : European Geopyhsical Union, 2012) Spiegel, J.K.; Aemisegger, F.; Scholl, M.; Wienhold, F.G.; Collett Jr., J.L.; Lee, T.; van Pinxteren, D.; Mertes, S.; Tilgner, A.; Herrmann, H.; Werner, R.A.; Buchmann, N.; Eugster, W.In this work, we present the first study resolving the temporal evolution of δ2H and δ18O values in cloud droplets during 13 different cloud events. The cloud events were probed on a 937 m high mountain chain in Germany in the framework of the Hill Cap Cloud Thuringia 2010 campaign (HCCT-2010) in September and October 2010. The δ values of cloud droplets ranged from −77‰ to −15‰ (δ2H) and from −12.1‰ to −3.9‰ (δ18O) over the whole campaign. The cloud water line of the measured δ values was δ2H=7.8×δ18O+13×10−3, which is of similar slope, but with higher deuterium excess than other Central European Meteoric Water Lines. Decreasing δ values in the course of the campaign agree with seasonal trends observed in rain in central Europe. The deuterium excess was higher in clouds developing after recent precipitation revealing episodes of regional moisture recycling. The variations in δ values during one cloud event could either result from changes in meteorological conditions during condensation or from variations in the δ values of the water vapor feeding the cloud. To test which of both aspects dominated during the investigated cloud events, we modeled the variation in δ values in cloud water using a closed box model. We could show that the variation in δ values of two cloud events was mainly due to changes in local temperature conditions. For the other eleven cloud events, the variation was most likely caused by changes in the isotopic composition of the advected and entrained vapor. Frontal passages during two of the latter cloud events led to the strongest temporal changes in both δ2H (≈ 6‰ per hour) and δ18O (≈ 0.6‰ per hour). Moreover, a detailed trajectory analysis for the two longest cloud events revealed that variations in the entrained vapor were most likely related to rain out or changes in relative humidity and temperature at the moisture source region or both. This study illustrates the sensitivity of stable isotope composition of cloud water to changes in large scale air mass properties and regional recycling of moisture.
- ItemKinetic measurements of the reactivity of hydrogen peroxide and ozone towards small atmospherically relevant aldehydes, ketones and organic acids in aqueous solutions(München : European Geopyhsical Union, 2014) Schöne, L.; Herrmann, H.Free radical reactions are an important degradation process for organic compounds within the aqueous atmospheric environment. Nevertheless, non-radical oxidants such as hydrogen peroxide and ozone also contribute to the degradation and conversion of these substances (Tilgner and Herrmann, 2010). In this work, kinetic investigations of non-radical reactions were conducted using UV / Vis spectroscopy (dual-beam spectrophotometer and stopped flow technique) and a capillary electrophoresis system applying pseudo-first order kinetics to reactions of glyoxal, methylglyoxal, glycolaldehyde, glyoxylic, pyruvic and glycolic acid as well as methacrolein (MACR) and methyl vinyl ketone (MVK) with H2O2 and ozone at 298 K. The measurements indicate rather small rate constants at room temperature of k2nd < 3 M−1 s−1 (except for the unsaturated compounds exposed to ozone). Compared to radical reaction rate constants the values are about 10 orders of magnitude smaller (kOH• ~109 M−1 s−1). However, when considering the much larger non-radical oxidant concentrations compared to radical concentrations in urban cloud droplets, calculated first-order conversion rate constants change the picture towards H2O2 reactions becoming more important, especially when compared to the nitrate radical. For some reactions mechanistic suggestions are also given.
- ItemInvestigation of the adiabatic assumption for estimating cloud micro- and macrophysical properties from satellite and ground observations(München : European Geopyhsical Union, 2016) Merk, D.; Deneke, H.; Pospichal, B.; Seifert, P.Cloud properties from both ground-based as well as from geostationary passive satellite observations have been used previously for diagnosing aerosol–cloud interactions. In this investigation, a 2-year data set together with four selected case studies are analyzed with the aim of evaluating the consistency and limitations of current ground-based and satellite-retrieved cloud property data sets. The typically applied adiabatic cloud profile is modified using a sub-adiabatic factor to account for entrainment within the cloud. Based on the adiabatic factor obtained from the combination of ground-based cloud radar, ceilometer and microwave radiometer, we demonstrate that neither the assumption of a completely adiabatic cloud nor the assumption of a constant sub-adiabatic factor is fulfilled (mean adiabatic factor 0.63 ± 0.22). As cloud adiabaticity is required to estimate the cloud droplet number concentration but is not available from passive satellite observations, an independent method to estimate the adiabatic factor, and thus the influence of mixing, would be highly desirable for global-scale analyses. Considering the radiative effect of a cloud described by the sub-adiabatic model, we focus on cloud optical depth and its sensitivities. Ground-based estimates are here compared vs. cloud optical depth retrieved from the Meteosat SEVIRI satellite instrument resulting in a bias of −4 and a root mean square difference of 16. While a synergistic approach based on the combination of ceilometer, cloud radar and microwave radiometer enables an estimate of the cloud droplet concentration, it is highly sensitive to radar calibration and to assumptions about the moments of the droplet size distribution. Similarly, satellite-based estimates of cloud droplet concentration are uncertain. We conclude that neither the ground-based nor satellite-based cloud retrievals applied here allow a robust estimate of cloud droplet concentration, which complicates its use for the study of aerosol–cloud interactions.
- ItemCloud water composition during HCCT-2010: Scavenging efficiencies, solute concentrations, and droplet size dependence of inorganic ions and dissolved organic carbon(München : European Geopyhsical Union, 2016) van Pinxteren, Dominik; Fomba, Khanneh Wadinga; Mertes, Stephan; Müller, Konrad; Spindler, Gerald; Schneider, Johannes; Lee, Taehyoung; Collett, Jeffrey L.; Herrmann, HartmutCloud water samples were taken in September/October 2010 at Mt. Schmücke in a rural, forested area in Germany during the Lagrange-type Hill Cap Cloud Thuringia 2010 (HCCT-2010) cloud experiment. Besides bulk collectors, a three-stage and a five-stage collector were applied and samples were analysed for inorganic ions (SO42−,NO3−, NH4+, Cl−, Na+, Mg2+, Ca2+, K+), H2O2 (aq), S(IV), and dissolved organic carbon (DOC). Campaign volume-weighted mean concentrations were 191, 142, and 39 µmol L−1 for ammonium, nitrate, and sulfate respectively, between 4 and 27 µmol L−1 for minor ions, 5.4 µmol L−1 for H2O2 (aq), 1.9 µmol L−1 for S(IV), and 3.9 mgC L−1 for DOC. The concentrations compare well to more recent European cloud water data from similar sites. On a mass basis, organic material (as DOC × 1.8) contributed 20–40 % (event means) to total solute concentrations and was found to have non-negligible impact on cloud water acidity. Relative standard deviations of major ions were 60–66 % for solute concentrations and 52–80 % for cloud water loadings (CWLs). The similar variability of solute concentrations and CWLs together with the results of back-trajectory analysis and principal component analysis, suggests that concentrations in incoming air masses (i.e. air mass history), rather than cloud liquid water content (LWC), were the main factor controlling bulk solute concentrations for the cloud studied. Droplet effective radius was found to be a somewhat better predictor for cloud water total ionic content (TIC) than LWC, even though no single explanatory variable can fully describe TIC (or solute concentration) variations in a simple functional relation due to the complex processes involved. Bulk concentrations typically agreed within a factor of 2 with co-located measurements of residual particle concentrations sampled by a counterflow virtual impactor (CVI) and analysed by an aerosol mass spectrometer (AMS), with the deviations being mainly caused by systematic differences and limitations of the approaches (such as outgassing of dissolved gases during residual particle sampling). Scavenging efficiencies (SEs) of aerosol constituents were 0.56–0.94, 0.79–0.99, 0.71–98, and 0.67–0.92 for SO42−, NO3−, NH4+, and DOC respectively when calculated as event means with in-cloud data only. SEs estimated using data from an upwind site were substantially different in many cases, revealing the impact of gas-phase uptake (for volatile constituents) and mass losses across Mt. Schmücke likely due to physical processes such as droplet scavenging by trees and/or entrainment. Drop size-resolved cloud water concentrations of major ions SO42−, NO3−, and NH4+ revealed two main profiles: decreasing concentrations with increasing droplet size and “U” shapes. In contrast, profiles of typical coarse particle mode minor ions were often increasing with increasing drop size, highlighting the importance of a species' particle concentration size distribution for the development of size-resolved solute concentration patterns. Concentration differences between droplet size classes were typically < 2 for major ions from the three-stage collector and somewhat more pronounced from the five-stage collector, while they were much larger for minor ions. Due to a better separation of droplet populations, the five-stage collector was capable of resolving some features of solute size dependencies not seen in the three-stage data, especially sharp concentration increases (up to a factor of 5–10) in the smallest droplets for many solutes.
- ItemComparing contact and immersion freezing from continuous flow diffusion chambers(München : European Geopyhsical Union, 2016) Nagare, Baban; Marcolli, Claudia; Welti, André; Stetzer, Olaf; Lohmann, UlrikeIce nucleating particles (INPs) in the atmosphere are responsible for glaciating cloud droplets between 237 and 273 K. Different mechanisms of heterogeneous ice nucleation can compete under mixed-phase cloud conditions. Contact freezing is considered relevant because higher ice nucleation temperatures than for immersion freezing for the same INPs were observed. It has limitations because its efficiency depends on the number of collisions between cloud droplets and INPs. To date, direct comparisons of contact and immersion freezing with the same INP, for similar residence times and concentrations, are lacking. This study compares immersion and contact freezing efficiencies of three different INPs. The contact freezing data were obtained with the ETH CoLlision Ice Nucleation CHamber (CLINCH) using 80 µm diameter droplets, which can interact with INPs for residence times of 2 and 4 s in the chamber. The contact freezing efficiency was calculated by estimating the number of collisions between droplets and particles. Theoretical formulations of collision efficiencies gave too high freezing efficiencies for all investigated INPs, namely AgI particles with 200 nm electrical mobility diameter, 400 and 800 nm diameter Arizona Test Dust (ATD) and kaolinite particles. Comparison of freezing efficiencies by contact and immersion freezing is therefore limited by the accuracy of collision efficiencies. The concentration of particles was 1000 cm−3 for ATD and kaolinite and 500, 1000, 2000 and 5000 cm−3 for AgI. For concentrations < 5000 cm−3, the droplets collect only one particle on average during their time in the chamber. For ATD and kaolinite particles, contact freezing efficiencies at 2 s residence time were smaller than at 4 s, which is in disagreement with a collisional contact freezing process but in accordance with immersion freezing or adhesion freezing. With “adhesion freezing”, we refer to a contact nucleation process that is enhanced compared to immersion freezing due to the position of the INP on the droplet, and we discriminate it from collisional contact freezing, which assumes an enhancement due to the collision of the particle with the droplet. For best comparison with contact freezing results, immersion freezing experiments of the same INPs were performed with the continuous flow diffusion chamber Immersion Mode Cooling chAmber–Zurich Ice Nucleation Chamber (IMCA–ZINC) for a 3 s residence time. In IMCA–ZINC, each INP is activated into a droplet in IMCA and provides its surface for ice nucleation in the ZINC chamber. The comparison of contact and immersion freezing results did not confirm a general enhancement of freezing efficiency for contact compared with immersion freezing experiments. For AgI particles the onset of heterogeneous freezing in CLINCH was even shifted to lower temperatures compared with IMCA–ZINC. For ATD, freezing efficiencies for contact and immersion freezing experiments were similar. For kaolinite particles, contact freezing became detectable at higher temperatures than immersion freezing. Using contact angle information between water and the INP, it is discussed how the position of the INP in or on the droplets may influence its ice nucleation activity.
- ItemIce nucleation by water-soluble macromolecules(München : European Geopyhsical Union, 2015) Pummer, B.G.; Budke, C.; Augustin-Bauditz, S.; Niedermeier, D.; Felgitsch, L.; Kampf, C.J.; Huber, R.G.; Liedl, K.R.; Loerting, T.; Moschen, T.; Schauperl, M.; Tollinger, M.; Morris, C.E.; Wex, H.; Grothe, H.; Pöschl, U.; Koop, T.; Fröhlich-Nowoisky, J.Cloud glaciation is critically important for the global radiation budget (albedo) and for initiation of precipitation. But the freezing of pure water droplets requires cooling to temperatures as low as 235 K. Freezing at higher temperatures requires the presence of an ice nucleator, which serves as a template for arranging water molecules in an ice-like manner. It is often assumed that these ice nucleators have to be insoluble particles. We point out that also free macromolecules which are dissolved in water can efficiently induce ice nucleation: the size of such ice nucleating macromolecules (INMs) is in the range of nanometers, corresponding to the size of the critical ice embryo. As the latter is temperature-dependent, we see a correlation between the size of INMs and the ice nucleation temperature as predicted by classical nucleation theory. Different types of INMs have been found in a wide range of biological species and comprise a variety of chemical structures including proteins, saccharides, and lipids. Our investigation of the fungal species Acremonium implicatum, Isaria farinosa, and Mortierella alpina shows that their ice nucleation activity is caused by proteinaceous water-soluble INMs. We combine these new results and literature data on INMs from fungi, bacteria, and pollen with theoretical calculations to develop a chemical interpretation of ice nucleation and water-soluble INMs. This has atmospheric implications since many of these INMs can be released by fragmentation of the carrier cell and subsequently may be distributed independently. Up to now, this process has not been accounted for in atmospheric models.
- ItemThe influence of clouds on radical concentrations: Observations and modelling studies of HOx during the Hill Cap Cloud Thuringia (HCCT) campaign in 2010(München : European Geopyhsical Union, 2015) Whalley, L.K.; Stone, D.; George, I.J.; Mertes, S.; van Pinxteren, D.; Tilgner, A.; Herrmann, H.; Evans, M.J.; Heard, D.E.The potential for chemistry occurring in cloud droplets to impact atmospheric composition has been known for some time. However, the lack of direct observations and uncertainty in the magnitude of these reactions led to this area being overlooked in most chemistry transport models. Here we present observations from Mt Schmücke, Germany, of the HO2 radical made alongside a suite of cloud measurements. HO2 concentrations were depleted in-cloud by up to 90% with the rate of heterogeneous loss of HO2 to clouds necessary to bring model and measurements into agreement, demonstrating a dependence on droplet surface area and pH. This provides the first observationally derived assessment for the uptake coefficient of HO2 to cloud droplets and was found to be in good agreement with theoretically derived parameterisations. Global model simulations, including this cloud uptake, showed impacts on the oxidising capacity of the troposphere that depended critically on whether the HO2 uptake leads to production of H2O2 or H2O.