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    Mehrwellenlängenlidar- und Flugzeugmessungen im Rahmen eines AerosäulenschlieĂŸungsexperiments : SchluĂŸbericht
    (Leipzig : Leibniz-Institut fĂ¼r Troposphärenforschung, 2000) Ansmann, Albert; Wandinger, Ulla; MĂ¼ller, Detlef; Althausen, Dietrich; Wendisch, Manfred; Keil, Andreas; MĂ¼ller, Dörthe
    [no abstract available]
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    Measurements of particle backscatter, extinction, and lidar ratio at 1064 nm with the rotational raman method in Polly-XT
    (Les Ulis : EDP Sciences, 2018) Engelmann, Ronny; Haarig, Moritz; Baars, Holger; Ansmann, Albert; Kottas, Michael; Marinou, Eleni; Nicolae, D.; Makoto, A.; Vassilis, A.; Balis, D.; Behrendt, A.; Comeron, A.; Gibert, F.; Landulfo, E.; McCormick, M.P.; Senff, C.; Veselovskii, I.; Wandinger, U.
    We replaced a 1064-nm interference filter of a Polly-XT lidar system by a 1058-nm filter to observe pure rotational Raman backscattering from atmospheric Nitrogen and Oxygen. Polly-XT is compact Raman lidar with a Nd:YAG laser (20 Hz, 200 mJ at 1064 nm) and a 30-cm telescope mirror which applies photomultipliers in photoncounting mode. We present the first measured signals at 1058 nm and the derived extinction profile from measurements aboard RV Polarstern and in Leipzig. In combination with another Polly-XT system we could also derive particle backscatter and lidar ratio profiles at 1064 nm.
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    Development of an online-coupled MARGA upgrade for the 2 h interval quantification of low-molecular-weight organic acids in the gas and particle phases
    (Göttingen : Copernicus GmbH, 2019) Stieger, B.; Spindler, G.; Van Pinxteren, D.; GrĂ¼ner, A.; Wallasch, M.; Herrmann, H.
    A method is presented to quantify the lowmolecular- weight organic acids such as formic, acetic, propionic, butyric, pyruvic, glycolic, oxalic, malonic, succinic, malic, glutaric, and methanesulfonic acid in the atmospheric gas and particle phases, based on a combination of the Monitor for AeRosols and Gases in ambient Air (MARGA) and an additional ion chromatography (Compact IC) instrument. Therefore, every second hourly integrated MARGA gas and particle samples were collected and analyzed by the Compact IC, resulting in 12 values per day for each phase. A proper separation of the organic target acids was initially tackled by a laboratory IC optimization study, testing different separation columns, eluent compositions and eluent flow rates for both isocratic and gradient elution. Satisfactory resolution of all compounds was achieved using a gradient system with two coupled anion-exchange separation columns. Online pre-concentration with an enrichment factor of approximately 400 was achieved by solid-phase extraction consisting of a methacrylate-polymer-based sorbent with quaternary ammonium groups. The limits of detection of the method range between 0.5 ngm3 for malonate and 17.4 ngm3 for glutarate. Precisions are below 1.0 %, except for glycolate (2.9 %) and succinate (1.0 %). Comparisons of inorganic anions measured at the TROPOS research site in Melpitz, Germany, by the original MARGA and the additional Compact IC are in agreement with each other (R2 D0.95-0.99). Organic acid concentrations from May 2017 as an example period are presented. Monocarboxylic acids were dominant in the gas phase with mean concentrations of 306 ngm3 for acetic acid, followed by formic (199 ngm3), propionic (83 ngm3), pyruvic (76 ngm3), butyric (34 ngm3) and glycolic acid (32 ngm3). Particulate glycolate, oxalate and methanesulfonate were quantified with mean concentrations of 26, 31 and 30 ngm3, respectively. Elevated concentrations of gas-phase formic acid and particulate oxalate in the late afternoon indicate photochemical formation as a source.
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    Mobility particle size spectrometers: Calibration procedures and measurement uncertainties
    (Philadelphia, Pa : Taylor & Francis, 2017) Wiedensohler, A.; Wiesner, A.; Weinhold, K.; Birmili, W.; Hermann, M.; Merkel, M.; MĂ¼ller, T.; Pfeifer, S.; Schmidt, A.; Tuch, T.; Velarde, F.; Quincey, P.; Seeger, S.; Nowak, A.
    Mobility particle size spectrometers (MPSS) belong to the essential instruments in aerosol science that determine the particle number size distribution (PNSD) in the submicrometer size range. Following calibration procedures and target uncertainties against standards and reference instruments are suggested for a complete MPSS quality assurance program: (a) calibration of the CPC counting efficiency curve (within 5% for the plateau counting efficiency; within 1 nm for the 50% detection efficiency diameter), (b) sizing calibration of the MPSS, using a certified polystyrene latex (PSL) particle size standard at 203 nm (within 3%), (c) intercomparison of the PNSD of the MPSS (within 10% and 20% of the dN/dlogDP concentration for the particle size range 20–200 and 200–800 nm, respectively), and (d) intercomparison of the integral PNC of the MPSS (within 10%). Furthermore, following measurement uncertainties have been investigated: (a) PSL particle size standards in the range from 100 to 500 nm match within 1% after sizing calibration at 203 nm. (b) Bipolar diffusion chargers based on the radioactive nuclides Kr85, Am241, and Ni63 and a new ionizer based on corona discharge follow the recommended bipolar charge distribution, while soft X-ray-based charges may alter faster than expected. (c) The use of a positive high voltage supply show a 10% better performance than a negative one. (d) The intercomparison of the integral PNC of an MPSS against the total number concentration is still within the target uncertainty at an ambient pressure of approximately 500 hPa. Copyright © 2018 Published with license by American Association for Aerosol Research.
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    Wildfires as a source of airborne mineral dust - Revisiting a conceptual model using large-eddy simulation (LES)
    (Göttingen : Copernicus GmbH, 2018) Wagner, R.; Jähn, M.; Schepanski, K.
    Airborne mineral dust is a key player in the Earth system and shows manifold impacts on atmospheric properties such as the radiation budget and cloud microphysics. Investigations of smoke plumes originating from wildfires found significant fractions of mineral dust within these plumes - most likely raised by strong, turbulent fire-related winds. This study presents and revisits a conceptual model describing the emission of mineral dust particles during wildfires. This is achieved by means of high-resolution large-eddy simulation (LES), conducted with the All Scale Atmospheric Model (ASAM). The impact of (a) different fire properties representing idealized grassland and shrubland fires, (b) different ambient wind conditions modulated by the fire's energy flux, and (c) the wind's capability to mobilize mineral dust particles was investigated. Results from this study illustrate that the energy release of the fire leads to a significant increase in near-surface wind speed, which consequently enhances the dust uplift potential. This is in particular the case within the fire area where vegetation can be assumed to be widely removed and uncovered soil is prone to wind erosion. The dust uplift potential is very sensitive to fire properties, such as fire size, shape, and intensity, but also depends on the ambient wind velocity. Although measurements already showed the importance of wildfires for dust emissions, pyro-convection is so far neglected as a dust emission process in atmosphere-aerosol models. The results presented in this study can be seen as the first step towards a systematic parameterization representing the connection between typical fire properties and related dust emissions.
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    Combining cloud radar and radar wind profiler for a value added estimate of vertical air motion and particle terminal velocity within clouds
    (Göttingen : Copernicus GmbH, 2018) Radenz, M.; BĂ¼hl, J.; Lehmann, V.; Görsdorf, U.; Leinweber, R.
    Vertical-stare observations from a 482MHz radar wind profiler and a 35GHz cloud radar are combined on the level of individual Doppler spectra to measure vertical air motions in clear air, clouds and precipitation. For this purpose, a separation algorithm is proposed to remove the influence of falling particles from the wind profiler Doppler spectra and to calculate the terminal fall velocity of hydrometeors. The remaining error of both vertical air motion and terminal fall velocity is estimated to be better than 0.1ms-1 using numerical simulations. This combination of instruments allows direct measurements of in-cloud vertical air velocity and particle terminal fall velocity by means of ground-based remote sensing. The possibility of providing a profile every 10s with a height resolution of < 100m allows further insight into the process scale of in-cloud dynamics. The results of the separation algorithm are illustrated by two case studies, the first covering a deep frontal cloud and the second featuring a shallow mixed-phase cloud.
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    Triple-wavelength lidar observations of the linear depolarization ratio of dried marine particles
    (Les Ulis : EDP Sciences, 2018) Haarig, Moritz; Ansmann, Albert; Baars, Holger; Engelmann, Ronny; Althausen, Dietrich; Bohlmann, Stephanie; Gasteiger, Josef; Farrell, David; Nicolae, D.; Makoto, A.; Vassilis, A.; Balis, D.; Behrendt, A.; Comeron, A.; Gibert, F.; Landulfo, E.; McCormick, M.P.; Senff, C.; Veselovskii, I.; Wandinger, U.
    For aerosol typing with lidar, sea salt particles are usually assumed to be spherical with a consequently low depolarization ratio. Evidence of dried marine particles at the top of the humid marine aerosol layer with a depolarization ratio up to 0.1 has been found at predominately maritime locations on Barbados and in the Southern Atlantic. The depolarization ratio for these probably cubic sea salt particles has been measured at three wavelengths (355, 532 and 1064 nm) simultaneously for the first time and compared to model simulations.
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    Study of mixed phase clouds over west Africa: Ice-crystal corner reflection effects observed with a two-wavelength polarization lidar
    (Les Ulis : EDP Sciences, 2018) Veselovskii, Igor; Goloub, Philippe; Podvin, Thierry; Tanre, Didier; Ansmann, Albert; Korenskiy, Michail; Borovoi, Anatoli; Hu, Qiaoyun; Bovchaliuk, Valentin; Whiteman, David N.; Nicolae, D.; Makoto, A.; Vassilis, A.; Balis, D.; Behrendt, A.; Comeron, A.; Gibert, F.; Landulfo, E.; McCormick, M.P.; Senff, C.; Veselovskii, I.; Wandinger, U.
    Lidar sounding is used for the analysis of possible contribution of the corner reflection (CR) effect to the total backscattering in case of ice crystals. Our study is based on observations of mixed phase clouds performed during the SHADOW campaign in Senegal. Mie-Raman lidar allows measurements at 355 nm and 532 nm at 43 dg. off-zenith angle, so the extinction and backscattering Ångström exponents can be evaluated. In some measurements we observed the positive values of backscattering Ångström exponent, which can be attributed to the corner reflection by horizontally oriented ice plates.
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    Tropospheric Aqueous-Phase Oxidation of Isoprene-Derived Dihydroxycarbonyl Compounds
    (Washington, DC : Soc., 2017) Otto, Tobias; Stieger, Bastian; Mettke, Peter; Herrmann, Hartmut
    The dihydroxycarbonyls 3,4-dihydroxy-2-butanone (DHBO) and 2,3-dihydroxy-2-methylpropanal (DHMP) formed from isoprene oxidation products in the atmospheric gas phase under low-NO conditions can be expected to form aqSOA in the tropospheric aqueous phase because of their solubility. In the present study, DHBO and DHMP were investigated concerning their radical-driven aqueous-phase oxidation reaction kinetics. For DHBO and DHMP the following rate constants at 298 K are reported: k(OH + DHBO) = (1.0 ± 0.1) × 109 L mol-1 s-1, k(NO3 + DHBO) = (2.6 ± 1.6) × 106 L mol-1 s-1, k(SO4-+ DHBO) = (2.3 ± 0.2) × 107 L mol-1 s-1, k(OH + DHMP) = (1.2 ± 0.1) × 109 L mol-1 s-1, k (NO3 + DHMP) = (7.9 ± 0.7) × 106 L mol-1 s-1, k(SO4- + DHMP) = (3.3 ± 0.2) × 107 L mol-1 s-1, together with their respective temperature dependences. The product studies of both DHBO and DHMP revealed hydroxydicarbonyls, short chain carbonyls, and carboxylic acids, such as hydroxyacetone, methylglyoxal, and lactic and pyruvic acid as oxidation products with single yields up to 25%. The achieved carbon balance was 75% for DHBO and 67% for DHMP. An aqueous-phase oxidation scheme for both DHBO and DHMP was developed on the basis of the experimental findings to show their potential to contribute to the aqSOA formation. It can be expected that the main contribution to aqSOA occurs via acid formation while other short-chain oxidation products are expected to back-partition into the gas phase to undergo further oxidation there.
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    Large-scale modeling of absorbing aerosols and their semi-direct effects
    (Basel : MDPI AG, 2018) Tegen, I.; Heinold, B.
    Radiative effects of absorbing black carbon and mineral dust aerosols are estimated from global aerosol climate model simulations with fixed sea surface temperatures as a boundary condition. Semi-direct effects are approximated as the residual between the total direct radiative effect and the instantaneous direct radiative effect of the simulated absorbing aerosol species. No distinction is made for aerosols from natural and anthropogenic sources. Results for global average are highly uncertain due to high model variability, but consistent with previous estimates. The global average results for black carbon aerosol semi-direct effects are small due to cancellation of regionally positive or negative effects, and may be positive or negative overall, depending on the model setup. The presence of mineral dust aerosol above dark surfaces and below a layer containing black carbon aerosol may enhance the reflectivity and act to enhance the positive radiative effect of black carbon aerosol. When mineral dust is absent the semi-direct effect at the top-of-atmosphere of black carbon aerosol from both anthropogenic and natural sources is -0.03 Wm-2, while averaging to +0.09 Wm-2 if dust is included.