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- ItemResults and recommendations from an intercomparison of six Hygroscopicity-TDMA systems(München : European Geopyhsical Union, 2011) Massling, A.; Niedermeier, N.; Hennig, T.; Fors, E.O.; Swietlicki, E.; Ehn, M.; Hämeri, K.; Villani, P.; Laj, P.; Good, N.; McFiggans, G.; Wiedensohler, A.The performance of six custom-built Hygrocopicity-Tandem Differential Mobility Analyser (H-TDMA) systems was investigated in the frame of an international calibration and intercomparison workshop held in Leipzig, February 2006. The goal of the workshop was to harmonise H-TDMA measurements and develop recommendations for atmospheric measurements and their data evaluation. The H-TDMA systems were compared in terms of the sizing of dry particles, relative humidity (RH) uncertainty, and consistency in determination of number fractions of different hygroscopic particle groups. The experiments were performed in an air-conditioned laboratory using ammonium sulphate particles or an external mixture of ammonium sulphate and soot particles. The sizing of dry particles of the six H-TDMA systems was within 0.2 to 4.2% of the selected particle diameter depending on investigated size and individual system. Measurements of ammonium sulphate aerosol found deviations equivalent to 4.5% RH from the set point of 90% RH compared to results from previous experiments in the literature. Evaluation of the number fraction of particles within the clearly separated growth factor modes of a laboratory generated externally mixed aerosol was done. The data from the H-TDMAs was analysed with a single fitting routine to investigate differences caused by the different data evaluation procedures used for each H-TDMA. The differences between the H-TDMAs were reduced from +12/−13% to +8/−6% when the same analysis routine was applied. We conclude that a common data evaluation procedure to determine number fractions of externally mixed aerosols will improve the comparability of H-TDMA measurements. It is recommended to ensure proper calibration of all flow, temperature and RH sensors in the systems. It is most important to thermally insulate the aerosol humidification unit and the second DMA and to monitor these temperatures to an accuracy of 0.2 °C. For the correct determination of external mixtures, it is necessary to take into account size-dependent losses due to diffusion in the plumbing between the DMAs and in the aerosol humidification unit.
- ItemIncreasing the spatial resolution of cloud property retrievals from Meteosat SEVIRI by use of its high-resolution visible channel: Evaluation of candidate approaches with MODIS observations(Katlenburg-Lindau : Copernicus, 2020) Werner, Frank; Deneke, HartwigThis study presents and evaluates several candidate approaches for downscaling observations from the Spinning Enhanced Visible and Infrared Imager (SEVIRI) in order to increase the horizontal resolution of subsequent cloud optical thickness (τ) and effective droplet radius (reff) retrievals from the native ≈ 3km×3km spatial resolution of the narrowband channels to ≈ 1km×1km. These methods make use of SEVIRI's coincident broadband high-resolution visible (HRV) channel. For four example cloud fields, the reliability of each downscaling algorithm is evaluated by means of collocated 1km×1km MODIS radiances, which are reprojected to the horizontal grid of the HRV channel and serve as reference for the evaluation. By using these radiances, smoothed with the modulation transfer function of the native SEVIRI channels, as retrieval input, the accuracy at the SEVIRI standard resolution can be evaluated and an objective comparison of the accuracy of the different downscaling algorithms can be made. For the example scenes considered in this study, it is shown that neglecting high-frequency variations below the SEVIRI standard resolution results in significant random absolute deviations of the retrieved τ and reff of up to ≈ 14 and ≈ 6μm, respectively, as well as biases. By error propagation, this also negatively impacts the reliability of the subsequent calculation of liquid water path (WL) and cloud droplet number concentration (ND), which exhibit deviations of up to ≈ 89gm-2 and ≈ 177cm-3, respectively. For τ , these deviations can be almost completely mitigated by the use of the HRV channel as a physical constraint and by applying most of the presented downscaling schemes. Uncertainties in retrieved reff at the native SEVIRI resolution are smaller, and the improvements from downscaling the observations are less obvious than for τ. Nonetheless, the right choice of downscaling scheme yields noticeable improvements in the retrieved reff. Furthermore, the improved reliability in retrieved cloud products results in significantly reduced uncertainties in derived WL and ND. In particular, one downscaling approach provides clear improvements for all cloud products compared to those obtained from SEVIRI's standard resolution and is recommended for future downscaling endeavors. This work advances efforts to mitigate impacts of scale mismatches among channels of multiresolution instruments on cloud retrievals. © Author(s) 2020.
- ItemVertical profiles of aerosol mass concentration derived by unmanned airborne in situ and remote sensing instruments during dust events(Katlenburg-Lindau : Copernicus, 2018) Mamali, Dimitra; Marinou, Eleni; Sciare, Jean; Pikridas, Michael; Kokkalis, Panagiotis; Kottas, Michael; Binietoglou, Ioannis; Tsekeri, Alexandra; Keleshis, Christos; Engelmann, Ronny; Baars, Holger; Ansmann, Albert; Amiridis, Vassilis; Russchenberg, Herman; Biskos, GeorgeIn situ measurements using unmanned aerial vehicles (UAVs) and remote sensing observations can independently provide dense vertically resolved measurements of atmospheric aerosols, information which is strongly required in climate models. In both cases, inverting the recorded signals to useful information requires assumptions and constraints, and this can make the comparison of the results difficult. Here we compare, for the first time, vertical profiles of the aerosol mass concentration derived from light detection and ranging (lidar) observations and in situ measurements using an optical particle counter on board a UAV during moderate and weak Saharan dust episodes. Agreement between the two measurement methods was within experimental uncertainty for the coarse mode (i.e. particles having radii > 0.5 μm), where the properties of dust particles can be assumed with good accuracy. This result proves that the two techniques can be used interchangeably for determining the vertical profiles of aerosol concentrations, bringing them a step closer towards their systematic exploitation in climate models.
- ItemIn-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.
- ItemIntercomparison of 15 aerodynamic particle size spectrometers (APS 3321): Uncertainties in particle sizing and number size distribution(München : European Geopyhsical Union, 2016) Pfeifer, Sascha; Müller, Thomas; Weinhold, Kay; Zikova, Nadezda; dos Santos, Sebastiao Martins; Marinoni, Angela; Bischof, Oliver F.; Kykal, Carsten; Ries, Ludwig; Meinhardt, Frank; Aalto, Pasi; Mihalopoulos, Nikolaos; Wiedensohler, AlfredAerodynamic particle size spectrometers are a well-established method to measure number size distributions of coarse mode particles in the atmosphere. Quality assurance is essential for atmospheric observational aerosol networks to obtain comparable results with known uncertainties. In a laboratory study within the framework of ACTRIS (Aerosols, Clouds, and Trace gases Research Infrastructure Network), 15 aerodynamic particle size spectrometers (APS model 3321, TSI Inc., St. Paul, MN, USA) were compared with a focus on flow rates, particle sizing, and the unit-to-unit variability of the particle number size distribution. Flow rate deviations were relatively small (within a few percent), while the sizing accuracy was found to be within 10 % compared to polystyrene latex (PSL) reference particles. The unit-to-unit variability in terms of the particle number size distribution during this study was within 10 % to 20 % for particles in the range of 0.9 up to 3 µm, which is acceptable for atmospheric measurements. For particles smaller than that, the variability increased up to 60 %, probably caused by differences in the counting efficiencies of individual units. Number size distribution data for particles smaller than 0.9 µm in aerodynamic diameter should only be used with caution. For particles larger than 3 µm, the unit-to-unit variability increased as well. A possible reason is an insufficient sizing accuracy in combination with a steeply sloping particle number size distribution and the increasing uncertainty due to decreasing counting. Particularly this uncertainty of the particle number size distribution must be considered if higher moments of the size distribution such as the particle volume or mass are calculated, which require the conversion of the aerodynamic diameter measured to a volume equivalent diameter. In order to perform a quantitative quality assurance, a traceable reference method for the particle number concentration in the size range 0.5–3 µm is needed.
- ItemInfluence of aerosol copper on HO2 uptake: A novel parameterized equation(Katlenburg-Lindau : EGU, 2020) Song, Huan; Chen, Xiaorui; Lu, Keding; Zou, Qi; Tan, Zhaofeng; Fuchs, Hendrik; Wiedensohler, Alfred; Moon, Daniel R.; Heard, Dwayne E.; Baeza-Romero, María-Teresa; Zheng, Mei; Wahner, Andreas; Kiendler-Scharr, Astrid; Zhang, YuanhangHeterogeneous uptake of hydroperoxyl radicals (HO2) onto aerosols has been proposed to be a significant sink of HOx , hence impacting the atmospheric oxidation capacity. Accurate calculation of the HO2 uptake coefficient HO2 is key to quantifying the potential impact of this atmospheric process. Laboratory studies show that HO2 can vary by orders of magnitude due to changes in aerosol properties, especially aerosol soluble copper (Cu) concentration and aerosol liquid water content (ALWC). In this study we present a state-of-the-art model called MARK to simulate both gas- and aerosol-phase chemistry for the uptake of HO2 onto Cu-doped aerosols. Moreover, a novel parameterization of HO2 uptake was developed that considers changes in relative humidity (RH) and condensed-phase Cu ion concentrations and which is based on a model optimization using previously published and new laboratory data included in this work. This new parameterization will be applicable to wet aerosols, and it will complement current IUPAC recommendations. The new parameterization is as follows (the explanations for symbols are in the Appendix): (Formula presented) All parameters used in the paper are summarized in Table A1. Using this new equation, field data from a field campaign were used to evaluate the impact of the HO2 uptake onto aerosols on the ROx (=OH+HO2 CRO2) budget. Highly variable values for HO2 uptake were obtained for the North China Plain (median value <0.1). © 2020 Copernicus GmbH. All rights reserved.
- ItemAerosol hygroscopicity parameter derived from the light scattering enhancement factor measurements in the North China Plain(Göttingen : Copernicus, 2014) Chen, J.; Zhao, C.S.; Ma, N.; Yan, P.The relative humidity (RH) dependence of aerosol light scattering is an essential parameter for accurate estimation of the direct radiative forcing induced by aerosol particles. Because of insufficient information on aerosol hygroscopicity in climate models, a more detailed parameterization of hygroscopic growth factors and resulting optical properties with respect to location, time, sources, aerosol chemistry and meteorology are urgently required. In this paper, a retrieval method to calculate the aerosol hygroscopicity parameter, κ, is proposed based on the in situ measured aerosol light scattering enhancement factor, namely f(RH), and particle number size distribution (PNSD) obtained from the HaChi (Haze in China) campaign. Measurements show that f(RH) increases sharply with increasing RH, and that the time variance of f(RH) is much greater at higher RH. A sensitivity analysis reveals that the f(RH) is more sensitive to the aerosol hygroscopicity than PNSD. f(RH) for polluted cases is distinctly higher than that for clean periods at a specific RH. The derived equivalent κ, combined with the PNSD measurements, is applied in the prediction of the cloud condensation nuclei (CCN) number concentration. The predicted CCN number concentration with the derived equivalent κ agrees well with the measured ones, especially at high supersaturations. The proposed calculation algorithm of κ with the f(RH) measurements is demonstrated to be reasonable and can be widely applied.
- ItemComparison of storm damage functions and their performance(Göttingen : Copernicus GmbH, 2015) Prahl, B.F.; Rybski, D.; Burghoff, O.; Kropp, J.P.
- ItemAn intercomparison study of analytical methods used for quantification of levoglucosan in ambient aerosol filter samples(München : European Geopyhsical Union, 2015) Yttri, K.E.; Schnelle-Kreis, J.; Maenhaut, W.; Abbaszade, G.; Alves, C.; Bjerke, A.; Bonnier, N.; Bossi, R.; Claeys, M.; Dye, C.; Evtyugina, M.; García-Gacio, D.; Hillamo, R.; Hoffer, A.; Hyder, M.; Iinuma, Y.; Jaffrezo, J.-L.; Kasper-Giebl, A.; Kiss, G.; López-Mahia, P.L.; Pio, C.; Piot, C.; Ramirez-Santa-Cruz, C.; Sciare, J.; Teinilä, K.; Vermeylen, R.; Vicente, A.; Zimmermann, R.The monosaccharide anhydrides (MAs) levoglucosan, galactosan and mannosan are products of incomplete combustion and pyrolysis of cellulose and hemicelluloses, and are found to be major constituents of biomass burning (BB) aerosol particles. Hence, ambient aerosol particle concentrations of levoglucosan are commonly used to study the influence of residential wood burning, agricultural waste burning and wildfire emissions on ambient air quality. A European-wide intercomparison on the analysis of the three monosaccharide anhydrides was conducted based on ambient aerosol quartz fiber filter samples collected at a Norwegian urban background site during winter. Thus, the samples' content of MAs is representative for BB particles originating from residential wood burning. The purpose of the intercomparison was to examine the comparability of the great diversity of analytical methods used for analysis of levoglucosan, mannosan and galactosan in ambient aerosol filter samples. Thirteen laboratories participated, of which three applied high-performance anion-exchange chromatography (HPAEC), four used high-performance liquid chromatography (HPLC) or ultra-performance liquid chromatography (UPLC) and six resorted to gas chromatography (GC). The analytical methods used were of such diversity that they should be considered as thirteen different analytical methods. All of the thirteen laboratories reported levels of levoglucosan, whereas nine reported data for mannosan and/or galactosan. Eight of the thirteen laboratories reported levels for all three isomers. The accuracy for levoglucosan, presented as the mean percentage error (PE) for each participating laboratory, varied from −63 to 20%; however, for 62% of the laboratories the mean PE was within ±10%, and for 85% the mean PE was within ±20%. For mannosan, the corresponding range was −60 to 69%, but as for levoglucosan, the range was substantially smaller for a subselection of the laboratories; i.e. for 33% of the laboratories the mean PE was within ±10%. For galactosan, the mean PE for the participating laboratories ranged from −84 to 593%, and as for mannosan 33% of the laboratories reported a mean PE within ±10%. The variability of the various analytical methods, as defined by their minimum and maximum PE value, was typically better for levoglucosan than for mannosan and galactosan, ranging from 3.2 to 41% for levoglucosan, from 10 to 67% for mannosan and from 6 to 364% for galactosan. For the levoglucosan to mannosan ratio, which may be used to assess the relative importance of softwood versus hardwood burning, the variability only ranged from 3.5 to 24 . To our knowledge, this is the first major intercomparison on analytical methods used to quantify monosaccharide anhydrides in ambient aerosol filter samples conducted and reported in the scientific literature. The results show that for levoglucosan the accuracy is only slightly lower than that reported for analysis of SO42- (sulfate) on filter samples, a constituent that has been analysed by numerous laboratories for several decades, typically by ion chromatography and which is considered a fairly easy constituent to measure. Hence, the results obtained for levoglucosan with respect to accuracy are encouraging and suggest that levels of levoglucosan, and to a lesser extent mannosan and galactosan, obtained by most of the analytical methods currently used to quantify monosaccharide anhydrides in ambient aerosol filter samples, are comparable. Finally, the various analytical methods used in the current study should be tested for other aerosol matrices and concentrations as well, the most obvious being summertime aerosol samples affected by wildfires and/or agricultural fires.
- Item1064nm rotational Raman lidar for particle extinction and lidar-ratio profiling: Cirrus case study(München : European Geopyhsical Union, 2016) Haarig, Moritz; Engelmann, Ronny; Ansmann, Albert; Veselovskii, Igor; Whiteman, David N.; Althausen, DietrichFor the first time, vertical profiles of the 1064 nm particle extinction coefficient obtained from Raman lidar observations at 1058 nm (nitrogen and oxygen rotational Raman backscatter) are presented. We applied the new technique in the framework of test measurements and performed several cirrus observations of particle backscatter and extinction coefficients, and corresponding extinction-to-backscatter ratios at the wavelengths of 355, 532, and 1064 nm. The cirrus backscatter coefficients were found to be equal for all three wavelengths keeping the retrieval uncertainties in mind. The multiple-scattering-corrected cirrus extinction coefficients at 355 nm were on average about 20–30 % lower than the ones for 532 and 1064 nm. The cirrus-mean extinction-to-backscatter ratio (lidar ratio) was 31 ± 5 sr (355 nm), 36 ± 5 sr (532 nm), and 38 ± 5 sr (1064 nm) in this single study. We further discussed the requirements needed to obtain aerosol extinction profiles in the lower troposphere at 1064 nm with good accuracy (20 % relative uncertainty) and appropriate temporal and vertical resolution.