10 results
Search Results
Now showing 1 - 10 of 10
- ItemNumerical simulations of optical properties of Saharan dust aerosols with emphasis on lidar applications(Milton Park : Taylor & Francis, 2017) Wiegner, M.; Gasteiger, J.; Kandler, K.; Weinzierl, B.; Rasp, K.; Esselborn, M.; Freudenthaler, V.; Heese, B.; Toledano, C.; Tesche, M.; Althausen, D.In the framework of the Saharan Mineral Dust Experiment (SAMUM) for the first time the spectral dependence of particle linear depolarization ratios was measured by combining four lidar systems. In this paper these measurements are compared with results from scattering theory based on the T-matrix method. For this purpose, in situ measurements—size distribution, shape distribution and refractive index—were used as input parameters; particle shape was approximated by spheroids. A sensitivity study showed that lidar-related parameters—lidar ratio Sp and linear depolarization ratio δp—are very sensitive to changes of all parameters. The simulated values of the δp are in the range of 20% and 31% and thus in the range of the measurements. The spectral dependence is weak, so that it could not be resolved by the measurements. Calculated lidar ratios based on the measured microphysics and considering equivalent radii up to 7.5μm show a range of possible values between 29 and 50 sr at λ = 532 nm. Larger Sp might be possible if the real part of the refractive index is small and the imaginary part is large. A strict validation was however not possible as too many microphysical parameters influence Sp and δp that could not be measured with the required accuracy.
- 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.
- 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.
- ItemCharacterization of the planetary boundary layer during SAMUM-2 by means of lidar measurements(Milton Park : Taylor & Francis, 2017) Groß, Silke; Gasteiger, Josef; Freudenthaler, Volker; Wiegner, Matthias; Geiß, Alexander; Schladitz, Alexander; Toledano, Carlos; Kandler, Konrad; Tesche, Matthias; Ansmann, Albert; Wiedensohler, AlfredMeasurements with two Raman-depolarization lidars of the Meteorological Institute of the Ludwig-Maximilians- Universit¨at, M¨unchen, Germany, performed during SAMUM-2, were used to characterize the planetary boundary layer (PBL) over Praia, Cape Verde. A novel approach was used to determine the volume fraction of dust υd in the PBL. This approach primarily relies on accurate measurements of the linear depolarization ratio. Comparisons with independent in situ measurements showed the reliability of this approach. Based on our retrievals, two different phases could be distinguished within the measurement period of almost one month. The first (22–31 January 2008) was characterized by high aerosol optical depth (AOD) in the PBL and large υd > 95%. During the second phase, the AOD in the PBL was considerably lower and υd less than ∼40%. These findings were in very good agreement with ground based in situ measurements, when ambient volume fractions are considered that were calculated from the actual measurements of the dry volume fraction. Only in cases when dust was not the dominating aerosol component (second phase), effects due to hygroscopic growth became important.
- ItemEvaluation of long-range transport and deposition of desert dust with the CTM MOCAGE(Milton Park : Taylor & Francis, 2017) Martet, M.; Peuch, V-H.; Laurent, B.; Marticorena, B.; Bergametti, G.Desert dust modelling and forecasting attract growing interest, due to the numerous impacts of dusts on climate, numerical weather prediction, health, ecosystems, transportation, as well as on many industrial activities. The validation of numerical tools is a very important activity in this context, and we present here an example of such an effort, combining in situ (horizontal visibility in SYNOP messages, IMPROVE database) and remote-sensing data (satellite imagery, AERONET aerosol optical thickness data). Interestingly, these measurements are available routinely, and not only in the context of dedicated measurements campaign; thus, they can be used in an operational context to monitor the performances of operational forecasting systems. MOCAGE is the chemistry-transport model of Météo-France, used operationally to forecast the three-dimensional transport of dusts and their deposition. Two very long-range transport episodes of dust have been studied: one case of Saharan dust transported to East America through Asia and Pacific observed in November 2004 and one case of Saharan dust transported from West Africa to Caribbean Islands in May 2007. Episodes of geographical extension had seldom been studied, and they provide a very selective reference to compare the modelled desert dusts with. The representation of dusts in MOCAGE appears to be realistic in these two very different cases. In turn, the model simulations are used to make the link between the complementary information provided by the different measurements tools, providing a fully consistent picture of the entire episodes. The evolution of the aerosol size distribution during the episodes has also been studied. With no surprise, our study underlines that deposition processes are very sensitive to the size of dust particles. If the atmospheric cycle, in terms of mass, is very much under the influence of larger particles (some micrometres and above), only the finer particles actually travel over thousands of kilometres. This illustrates the need for an accurate representation of size distributions for this aerosol component in numerical models and advocates for using a size-resolved (bin) approach as sinks, and particularly, deposition do not affect the emitted log-normal distributions symmetrically on both sides of the median diameter. Overall, the results presented in this study provide an evaluation of Météo-France operational dust forecasting system MOCAGE.
- 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.
- ItemComparing turbulent parameters obtained from LITOS and radiosonde measurements(München : European Geopyhsical Union, 2015) Schneider, A.; Gerding, M.; Lübken, F.-J.Stratospheric turbulence is important for the mixing of trace species and the energy balance, but direct measurements are sparse due to the required resolution and accuracy. Recently, turbulence parameters such as the energy dissipation rate ε were inferred from standard radiosonde data by means of a Thorpe analysis. To this end, layers with vertically decreasing potential temperature are analysed, which is expected to indicate turbulence. Such an application assumes a proportionality between the Thorpe length LT and the Ozmidov scale LO. While this relation is accepted for the ocean, experimental evidence for such proportionality in the stratosphere is sparse. We have developed a high-resolution (8 kHz) turbulence measurement system called LITOS (Leibniz Institute Turbulence Observations in the Stratosphere), which for the first time resolves the inner scale of turbulence in the stratosphere. Therewith the energy dissipation rate ε can be determined by spectral analysis. This independent value for ε enables us to check the relation LO ∝ LT. In our measurements no such proportionality can be seen, although the mean of the ratio LO/LT is close to what is assumed in radiosonde analyses. Dissipation rates for individual layers obtained from radiosondes deviate up to a factor of ~3000 from those obtained by spectral analysis. Some turbulent layers measured by LITOS are not observed by the radiosonde at all, and vice versa. However, statements about the statistical mean seem to be possible by Thorpe analysis.
- ItemModeling of wave-induced irradiance variability in the upper ocean mixed layer(München : European Geopyhsical Union, 2012) Hieronymi, M.; Macke, A.; Zielinski, O.A Monte Carlo based radiative transfer model has been developed for calculating the availability of solar radiation within the top 100 m of the ocean. The model is optimized for simulations of spatial high resolution downwelling irradiance Ed fluctuations that arise from the lensing effect of waves at the water surface. In a first step the accuracy of simulation results has been verified by measurements of the oceanic underwater light field and through intercomparison with an established radiative transfer model. Secondly the potential depth-impact of nonlinear shaped single waves, from capillary to swell waves, is assessed by considering the most favorable conditions for light focusing, i.e. monochromatic light at 490 nm, very clear oceanic water with a low chlorophyll a content of 0.1 mg m−3 and high sun elevation. Finally light fields below irregular wave profiles accounting for realistic sea states were simulated. Our simulation results suggest that under open ocean conditions light flashes with 50% irradiance enhancements can appear down to 35 m depth, and light variability in the range of ±10% compared to the mean Ed is still possible in 100 m depth.