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- ItemOptimizing the detection, ablation, and ion extraction efficiency of a single-particle laser ablation mass spectrometer for application in environments with low aerosol particle concentrations(Katlenburg-Lindau : Copernicus, 2020) Clemen, Hans-Christian; Schneider, Johannes; Klimach, Thomas; Helleis, Frank; Köllner, Franziska; Hünig, Andreas; Rubach, Florian; Mertes, Stephan; Wex, Heike; Stratmann, Frank; Welti, André; Kohl, Rebecca; Frank, Fabian; Borrmann, StephanThe aim of this study is to show how a newly developed aerodynamic lens system (ALS), a delayed ion extraction (DIE), and better electric shielding improve the efficiency of the Aircraft-based Laser ABlation Aerosol MAss spectrometer (ALABAMA). These improvements are applicable to single-particle laser ablation mass spectrometers in general. To characterize the modifications, extensive sizeresolved measurements with spherical polystyrene latex particles (PSL; 150-6000 nm) and cubic sodium chloride particles (NaCl; 400-1700 nm) were performed. Measurements at a fixed ALS position show an improved detectable particle size range of the new ALS compared to the previously used Liu-type ALS, especially for supermicron particles. At a lens pressure of 2.4 hPa, the new ALS achieves a PSL particle size range from 230 to 3240 nm with 50% detection efficiency and between 350 and 2000 nm with 95% detection efficiency. The particle beam divergence was determined by measuring the detection efficiency at variable ALS positions along the laser cross sections and found to be minimal for PSL at about 800 nm. Compared to measurements by singleparticle mass spectrometry (SPMS) instruments using Liutype ALSs, the minimum particle beam divergence is shifted towards larger particle sizes. However, there are no disadvantages compared to the Liu-type lenses for particle sizes down to 200 nm. Improvements achieved by using the DIE and an additional electric shielding could be evaluated by size-resolved measurements of the hit rate, which is the ratio of laser pulses yielding a detectable amount of ions to the total number of emitted laser pulses. In particular, the hit rate for multiply charged particles smaller than 500 nm is significantly improved by preventing an undesired deflection of these particles in the ion extraction field. Moreover, it was found that by using the DIE the ion yield of the ablation, ionization, and ion extraction process could be increased, resulting in up to 7 times higher signal intensities of the cation spectra. The enhanced ion yield results in a larger effective width of the ablation laser beam, which in turn leads to a hit rate of almost 100% for PSL particles in the size range from 350 to 2000 nm. Regarding cubic NaCl particles the modifications of the ALABAMA result in an up to 2 times increased detection efficiency and an up to 5 times increased hit rate. The need for such instrument modifications arises in particular for measurements of particles that are present in low number concentrations such as ice-nucleating particles (INPs) in general, but also aerosol particles at high altitudes or in pristine environments. Especially for these low particle number concentrations, improved efficiencies help to overcome the statistical limitations of single-particle mass spectrometer measurements. As an example, laboratory INP measurements carried out in this study show that the appli- cation of the DIE alone increases the number of INP mass spectra per time unit by a factor of 2 to 3 for the sampled substances. Overall, the combination of instrument modifications presented here resulted in an increased measurement efficiency of the ALABAMA for different particle types and particles shape as well as for highly charged particles. © 2020 Copernicus GmbH. All rights reserved.
- ItemIce residual properties in mixed-phase clouds at the high-alpine Jungfraujoch site(Hoboken, NJ : Wiley, 2016) Kupiszewski, Piotr; Zanatta, Marco; Mertes, Stephan; Vochezer, Paul; Lloyd, Gary; Schneider, Johannes; Schenk, Ludwig; Schnaiter, Martin; Baltensperger, Urs; Weingartner, Ernest; Gysel, MartinIce residual (IR) and total aerosol properties were measured in mixed-phase clouds (MPCs) at the high-alpine Jungfraujoch research station. Black carbon (BC) content and coating thickness of BC-containing particles were determined using single-particle soot photometers. The ice activated fraction (IAF), derived from a comparison of IR and total aerosol particle size distributions, showed an enrichment of large particles in the IR, with an increase in the IAF from values on the order of 10−4 to 10−3 for 100 nm (diameter) particles to 0.2 to 0.3 for 1 μm (diameter) particles. Nonetheless, due to the high number fraction of submicrometer particles with respect to total particle number, IR size distributions were still dominated by the submicrometer aerosol. A comparison of simultaneously measured number size distributions of BC-free and BC-containing IR and total aerosol particles showed depletion of BC by number in the IR, suggesting that BC does not play a significant role in ice nucleation in MPCs at the Jungfraujoch. The potential anthropogenic climate impact of BC via the glaciation effect in MPCs is therefore likely to be negligible at this site and in environments with similar meteorological conditions and a similar aerosol population. The IAF of the BC-containing particles also increased with total particle size, in a similar manner as for the BC-free particles, but on a level 1 order of magnitude lower. Furthermore, BC-containing IR were found to have a thicker coating than the BC-containing total aerosol, suggesting the importance of atmospheric aging for ice nucleation.
- ItemUptake of nitric acid, ammonia, and organics in orographic clouds: Mass spectrometric analyses of droplet residual and interstitial aerosol particles(München : European Geopyhsical Union, 2017) Schneider, Johannes; Mertes, Stephan; van Pinxteren, Dominik; Herrmann, Hartmut; Borrmann, StephanConcurrent in situ analyses of interstitial aerosol and cloud droplet residues have been conducted at the Schmücke mountain site during the Hill Cap Cloud Thuringia campaign in central Germany in September and October 2010. Cloud droplets were sampled from warm clouds (temperatures between −3 and +16 °C) by a counterflow virtual impactor and the submicron-sized residues were analyzed by a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS), while the interstitial aerosol composition was measured by an high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). During cloud-free periods, the submicron out-of-cloud aerosol was analyzed using both instruments, allowing for intercomparison between the two instruments. Further instrumentation included black carbon measurements and optical particle counters for the aerosol particles as well as optical sizing instrumentation for the cloud droplets. The results show that, under cloud conditions, on average 85 % of the submicron aerosol mass partitioned into the cloud liquid phase. Scavenging efficiencies of nitrate, ammonium, sulfate, and organics ranged between 60 and 100 %, with nitrate having, in general, the highest values. For black carbon, the scavenging efficiency was markedly lower (about 24 %). The nitrate and ammonium mass fractions were found to be markedly enhanced in cloud residues, indicating uptake of gaseous nitric acid and ammonia into the aqueous phase. This effect was found to be temperature dependent: at lower temperatures, the nitrate and ammonium mass fractions in the residues were higher. Also, the oxidation state of the organic matter in cloud residues was found to be temperature dependent: the O : C ratio was lower at higher temperatures. A possible explanation for this observation is a more effective uptake and/or higher concentrations of low-oxidized water-soluble volatile organic compounds, possibly of biogenic origin, at higher temperatures. Organic nitrates were observed in cloud residuals as well as in the out-of-cloud aerosol, but no indication of a preferred partitioning of organic nitrates into the aqueous phase or into the gas phase was detected. Assuming the uptake of nitric acid and ammonia in cloud droplets will be reversible, it will lead to a redistribution of nitrate and ammonium among the aerosol particles, leading to more uniform, internally mixed particles after several cloud passages.
- 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.
- ItemOnline single particle analysis of ice particle residuals from mountain-top mixed-phase clouds using laboratory derived particle type assignment(München : European Geopyhsical Union, 2017) Schmidt, Susan; Schneider, Johannes; Klimach, Thomas; Mertes, Stephan; Schenk, Ludwig Paul; Kupiszewski, Piotr; Curtius, Joachim; Borrmann, StephanIn situ single particle analysis of ice particle residuals (IPRs) and out-of-cloud aerosol particles was conducted by means of laser ablation mass spectrometry during the intensive INUIT-JFJ/CLACE campaign at the high alpine research station Jungfraujoch (3580 m a.s.l.) in January–February 2013. During the 4-week campaign more than 70 000 out-of-cloud aerosol particles and 595 IPRs were analyzed covering a particle size diameter range from 100 nm to 3 µm. The IPRs were sampled during 273 h while the station was covered by mixed-phase clouds at ambient temperatures between −27 and −6 °C. The identification of particle types is based on laboratory studies of different types of biological, mineral and anthropogenic aerosol particles. The outcome of these laboratory studies was characteristic marker peaks for each investigated particle type. These marker peaks were applied to the field data. In the sampled IPRs we identified a larger number fraction of primary aerosol particles, like soil dust (13 ± 5 %) and minerals (11 ± 5 %), in comparison to out-of-cloud aerosol particles (2.4 ± 0.4 and 0.4 ± 0.1 %, respectively). Additionally, anthropogenic aerosol particles, such as particles from industrial emissions and lead-containing particles, were found to be more abundant in the IPRs than in the out-of-cloud aerosol. In the out-of-cloud aerosol we identified a large fraction of aged particles (31 ± 5 %), including organic material and secondary inorganics, whereas this particle type was much less abundant (2.7 ± 1.3 %) in the IPRs. In a selected subset of the data where a direct comparison between out-of-cloud aerosol particles and IPRs in air masses with similar origin was possible, a pronounced enhancement of biological particles was found in the IPRs.
- ItemA comprehensive in situ and remote sensing data set from the Arctic CLoud Observations Using airborne measurements during polar Day (ACLOUD) campaign(Katlenburg-Lindau : Copernics Publications, 2019) Ehrlich, André; Wendisch, Manfred; Lüpkes, Christof; Buschmann, Matthias; Bozem, Heiko; Chechin, Dmitri; Clemen, Hans-Christian; Dupuy, Régis; Eppers, Olliver; Hartmann, Jörg; Herber, Andreas; Jäkel, Evelyn; Järvinen, Emma; Jourdan, Olivier; Kästner, Udo; Kliesch, Leif-Leonard; Köllner, Franziska; Mech, Mario; Mertes, Stephan; Neuber, Roland; Ruiz-Donoso, Elena; Schnaiter, Martin; Schneide, Johannes; Stapf, Johannes; Zanatta, MarcoThe Arctic CLoud Observations Using airborne measurements during polar Day (ACLOUD) campaign was carried out north-west of Svalbard (Norway) between 23 May and 6 June 2017. The objective of ACLOUD was to study Arctic boundary layer and mid-level clouds and their role in Arctic amplification. Two research aircraft (Polar 5 and 6) jointly performed 22 research flights over the transition zone between open ocean and closed sea ice. Both aircraft were equipped with identical instrumentation for measurements of basic meteorological parameters, as well as for turbulent and radiative energy fluxes. In addition, on Polar 5 active and passive remote sensing instruments were installed, while Polar 6 operated in situ instruments to characterize cloud and aerosol particles as well as trace gases. A detailed overview of the specifications, data processing, and data quality is provided here. It is shown that the scientific analysis of the ACLOUD data benefits from the coordinated operation of both aircraft. By combining the cloud remote sensing techniques operated on Polar 5, the synergy of multi-instrument cloud retrieval is illustrated. The remote sensing methods were validated using truly collocated in situ and remote sensing observations. The data of identical instruments operated on both aircraft were merged to extend the spatial coverage of mean atmospheric quantities and turbulent and radiative flux measurement. Therefore, the data set of the ACLOUD campaign provides comprehensive in situ and remote sensing observations characterizing the cloudy Arctic atmosphere. All processed, calibrated, and validated data are published in the World Data Center PANGAEA as instrument-separated data subsets (Ehrlich et al., 2019b, https://doi.org/10.1594/PANGAEA.902603).
- ItemThe Arctic Cloud Puzzle: Using ACLOUD/PASCAL Multiplatform Observations to Unravel the Role of Clouds and Aerosol Particles in Arctic Amplification(Boston, Mass. : ASM, 2019) Wendisch, Manfred; Macke, Andreas; Ehrlich, André; Lüpkes, Christof; Mech, Mario; Chechin, Dmitry; Dethloff, Klaus; Velasco, Carola Barrientos; Bozem, Heiko; Brückner, Marlen; Clemen, Hans-Christian; Crewell, Susanne; Donth, Tobias; Dupuy, Regis; Ebell, Kerstin; Egerer, Ulrike; Engelmann, Ronny; Engler, Christa; Eppers, Oliver; Gehrmann, Martin; Gong, Xianda; Gottschalk, Matthias; Gourbeyre, Christophe; Griesche, Hannes; Hartmann, Jörg; Hartmann, Markus; Heinold, Bernd; Herber, Andreas; Herrmann, Hartmut; Heygster, Georg; Hoor, Peter; Jafariserajehlou, Soheila; Jäkel, Evelyn; Järvinen, Emma; Jourdan, Olivier; Kästner, Udo; Kecorius, Simonas; Knudsen, Erlend M.; Köllner, Franziska; Kretzschmar, Jan; Lelli, Luca; Leroy, Delphine; Maturilli, Marion; Mei, Linlu; Mertes, Stephan; Mioche, Guillaume; Neuber, Roland; Nicolaus, Marcel; Nomokonova, Tatiana; Notholt, Justus; Palm, Mathias; van Pinxteren, Manuela; Quaas, Johannes; Richter, Philipp; Ruiz-Donoso, Elena; Schäfer, Michael; Schmieder, Katja; Schnaiter, Martin; Schneider, Johannes; Schwarzenböck, Alfons; Seifert, Patric; Shupe, Matthew D.; Siebert, Holger; Spreen, Gunnar; Stapf, Johannes; Stratmann, Frank; Vogl, Teresa; Welti, André; Wex, Heike; Wiedensohler, Alfred; Zanatta, Marco; Zeppenfeld, SebastianClouds play an important role in Arctic amplification. This term represents the recently observed enhanced warming of the Arctic relative to the global increase of near-surface air temperature. However, there are still important knowledge gaps regarding the interplay between Arctic clouds and aerosol particles, and surface properties, as well as turbulent and radiative fluxes that inhibit accurate model simulations of clouds in the Arctic climate system. In an attempt to resolve this so-called Arctic cloud puzzle, two comprehensive and closely coordinated field studies were conducted: the Arctic Cloud Observations Using Airborne Measurements during Polar Day (ACLOUD) aircraft campaign and the Physical Feedbacks of Arctic Boundary Layer, Sea Ice, Cloud and Aerosol (PASCAL) ice breaker expedition. Both observational studies were performed in the framework of the German Arctic Amplification: Climate Relevant Atmospheric and Surface Processes, and Feedback Mechanisms (AC) project. They took place in the vicinity of Svalbard, Norway, in May and June 2017. ACLOUD and PASCAL explored four pieces of the Arctic cloud puzzle: cloud properties, aerosol impact on clouds, atmospheric radiation, and turbulent dynamical processes. The two instrumented Polar 5 and Polar 6 aircraft; the icebreaker Research Vessel (R/V) Polarstern; an ice floe camp including an instrumented tethered balloon; and the permanent ground-based measurement station at Ny-Ålesund, Svalbard, were employed to observe Arctic low- and mid-level mixed-phase clouds and to investigate related atmospheric and surface processes. The Polar 5 aircraft served as a remote sensing observatory examining the clouds from above by downward-looking sensors; the Polar 6 aircraft operated as a flying in situ measurement laboratory sampling inside and below the clouds. Most of the collocated Polar 5/6 flights were conducted either above the R/V Polarstern or over the Ny-Ålesund station, both of which monitored the clouds from below using similar but upward-looking remote sensing techniques as the Polar 5 aircraft. Several of the flights were carried out underneath collocated satellite tracks. The paper motivates the scientific objectives of the ACLOUD/PASCAL observations and describes the measured quantities, retrieved parameters, and the applied complementary instrumentation. Furthermore, it discusses selected measurement results and poses critical research questions to be answered in future papers analyzing the data from the two field campaigns.
- ItemA modelling study on the activation of small Aitken-mode aerosol particles during CIME 97(Milton Park : Taylor & Francis, 2016) Gérémy, Guiléne; Wobrock, Wolfram; Flossmann, Andrea I.; Schwarzenböck, Alfons; Mertes, StephanDuring February 1997, one of the 2 observational periods of CIME (cloud ice mountain experiment), a joint field experiment funded by the European Commission, took place on the summit of the Puy de Doˆme in the centre of France. During this experiment the droplet spectra were measured with an FSSP and the aerosol particles in the drops and in the interstitial particle phase were measured with a counterflow virtual impactor and a round jet impactor inside a windtunnel. Very low aerosol particle and drop concentrations were observed and particles as small as 25 nm in diameter were found to activate. Two datasets obtained on 15 February and 17 February were used to study the activation of the small Aitken-mode particles and the spectral form of the droplet spectrum and the scavenging fraction. Numerous sensitivity studies were performed investigating the roˆ le of the number density and chemical composition of the aerosol particles. The roˆ le of mixing inside the orographic cloud was studied by using a new technique. It considers the fact that the air arriving on the summit of the Puy de Doˆme is a mixture of air of different origins. Thus, it weighs the results of a spectral scavenging model (DESCAM or EXMIX) calculated along a number of individual trajectories. The weighing function is derived from tracer and trajectory studies with a 3-dimensional mesoscale model. The model was able to reproduce the activation of aerosol particles as small as 25 nm. It was caused by the low aerosol particle number concentrations. In general, we can conclude that the variability found in the sensitivity tests of the dynamical and chemical factors allows to reproduce the shape of the observed results. As too many free parameters exit at the moment we cannot quantify the contribution of each factor studied to the observed scavenging fraction, however, it seems that dynamics dominates.
- ItemFelduntersuchungen von Budgets und Konversionen organischer Partikelinhaltsstoffe in troposphärischen Wolkenprozessen (FEBUKO): Projektabschlussbericht ; Teilprojekte: IfT-1: Physiko-chemische Charakterisierung von Luft, Partikeln und Wolkenwasser in Wolkenexperimenten; IfT-2: Phasenaufteilung von biogenen und anthropogenen organischen Aerosolkomponenten und flüchtiger organischer Substanzen in Wolken; BTU: Anteil und Modifikation organischer und reaktiver Substanzen in der Aerosol- und Wolkenwasserphase während des Wolkendurchganges; ZUF: Aerosolpartikel und Wolkentropfen als Quelle von Peroxyradikalen und Wasserstoffperoxid - Photochemie im atmosphärischen Mehrphasensystem durch organische Chromophore; TUD: Bestimmung organischer Spezies (Aldehyde, Ketone, Carbonsäuren) in Einzeltropfen zur Bestimmung der zugehörigen Aerosolgrößen und des Wolkenscavengings(Hannover : Technische Informationsbibliothek, 2004) Herrmann, Hartmut; Wiedensohler, Alfred; Mertes, Stephan; Wieprecht, Wolfgang; Jaeschke, Wolfgang; Bächmann, Knut[no abstract available]
- ItemReservoiraufteilung von Ruß, organischen Bestandteilen, Gesamtkohlenstoff, löslichen Substanzen und Aerosolpartikeln (Anzahl und Masse) in der Tropfen- und Zwischenraumphase von Wolken : Abschlussbericht(Leipzig : Leibniz-Institut für Troposphärenforschung, 2002) Mertes, Stephan; Schwarzenböck, A.; Brüggemann, E.; Gnauk, T.; Dippel, B.[no abstract available]