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Start date: 2000 × End date: 2009 × WGL Institute: TROPOS ×

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Now showing 1 - 10 of 71
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    Towards closing the gap between hygroscopic growth and activation for secondary organic aerosol - Part 2: Theoretical approaches
    (München : European Geopyhsical Union, 2009) Wex, H.; Petters, M.D.; Carrico, C.M.; Hallbauer, E.; Massling, A.; McMeeking, G.R.; Poulain, L.; Wu, Z.; Kreidenweis, S.M.; Stratmann, F.
    We examine the hygroscopic properties of secondary organic aerosol particles generated through the reaction of α-pinene and ozone using a continuous flow reaction chamber. The water activity versus composition relationship is calculated from measurements of growth factors at relative humidities up to 99.6% and from measurements of cloud condensation nuclei activity. The observed relationships are complex, suggesting highly non-ideal behavior for aerosol water contents at relative humidities less than 98%. We present two models that may explain the observed water activity-composition relationship equally well. The first model assumes that the aerosol is a pseudo binary mixture of infinitely water soluble compounds and sparingly soluble compounds that gradually enter the solution as dilution increases. The second model is used to compute the Gibbs free energy of the aerosol-water mixture and shows that the aerosol behaves similarly to what can be expected for single compounds that contain a certain fraction of oxygenated and non-polar functional groups.
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    Mehrwellenlängenlidar- und Flugzeugmessungen im Rahmen eines Aerosäulenschließungsexperiments : Schlußbericht
    (Leipzig : Leibniz-Institut für Troposphärenforschung, 2000) Ansmann, Albert; Wandinger, Ulla; Müller, Detlef; Althausen, Dietrich; Wendisch, Manfred; Keil, Andreas; Müller, Dörthe
    [no abstract available]
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    Out of Africa: High aerosol concentrations in the upper troposphere over Africa
    (München : European Geopyhsical Union, 2003) Heintzenberg, J.; Hermann, M.; Theiss, D.
    In the year 2000, six flights (three southbound and three northbound) of the CARIBIC project were conducted between Germany and two destinations in the southern hemisphere (Windhoek, Namibia and Cape Town, South Africa). In the present report, results on particle number concentrations are discussed in three size ranges (>4 nm, >12 nm, and >18 nm particle diameter) during the unique transequatorial Africa flights. The flights covered a total of about 80 h in May, July, and December. Thus, no claim can be made for long-term representativeness of the aerosol data. Nevertheless, they are the first upper systematic tropospheric transequatorial aerosol profiles over Africa. The average aerosol results show a broad maximum, roughly symmetrical to the equator, which compares well in latitudinal extent to a maximum of CO concentrations measured on the same flights. This export of continental surface aerosol to the upper troposphere will be dispersed on a global scale both with the easterly flow near the equator and with the westerlies in the adjacent subtropical regions. There was strong evidence of recent new particle formation before aerosol arrival at flight level, in particular during the time periods between 9:00 and 13:00 local time over Africa. Direct and indirect climate effects of the respective particulate matter remain to be investigated by future flights with the ongoing extension of the CARIBIC payload towards size-resolved measurements above 100 nm particle diameter. At the same time global chemical transport models and aerosol dynamics models need to be extended to be able to reproduce the CARIBIC findings over Africa.
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    LACIS-measurements and parameterization of sea-salt particle hygroscopic growth and activation
    (München : European Geopyhsical Union, 2008) Niedermeier, D.; Wex, H.; Voigtländer, J.; Stratmann, F.; Brüggemann, E.; Kiselev, A.; Henk, H.; Heintzenberg, J.
    The Leipzig Aerosol Cloud Interaction Simulator (LACIS) was used to investigate the hygroscopic growth and activation of sea-salt particles which were generated from three different sea-water samples. The measurements showed that the sea-salt particles exhibit a slightly reduced hygroscopic growth compared to pure NaCl particles. Köhler theory was utilized to model the hygroscopic growth of these particles. Some parameters used in this model are unknown for sea-salt. These parameters are combined in an "ionic density" ρion. For each sea-salt sample an average ρion was determined by fitting the Köhler equation to the data from the hygroscopic growth measurements. LACIS was also used to measure the activation of the sea-salt particles at three different supersaturations: 0.11%, 0.17% and 0.32%. A CCN-closure was tested by calculating the critical diameters Dcrit for the sea-salt particles at these supersaturations, using the Köhler model and the corresponding ρion as derived from the hygroscopic growth data. These calculated critical diameters were compared to the measured ones. Measured and calculated values of Dcrit agree within the level of uncertainty. Based on this successful closure, a new parameterization to describe sea-salt-particle hygroscopic growth (at RH>95%) and activation has been developed.
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    Modelling the optical properties of fresh biomass burning aerosol produced in a smoke chamber: Results from the EFEU campaign
    (München : European Geopyhsical Union, 2008) Hungershoefer, K.; Zeromskiene, K.; Iinuma, Y.; Helas, G.; Trentmann, J.; Trautmann, T.; Parmar, R.S.; Wiedensohler, A.; Andreae, M.O.; Schmid, O.
    A better characterisation of the optical properties of biomass burning aerosol as a function of the burning conditions is required in order to quantify their effects on climate and atmospheric chemistry. Controlled laboratory combustion experiments with different fuel types were carried out at the combustion facility of the Max Planck Institute for Chemistry (Mainz, Germany) as part of the "Impact of Vegetation Fires on the Composition and Circulation of the Atmosphere" (EFEU) project. The combustion conditions were monitored with concomitant CO2 and CO measurements. The mass scattering efficiencies of 8.9±0.2 m2 g−1 and 9.3±0.3 m2 g−1 obtained for aerosol particles from the combustion of savanna grass and an African hardwood (musasa), respectively, are larger than typically reported mainly due to differences in particle size distribution. The photoacoustically measured mass absorption efficiencies of 0.51±0.02 m2 g−1 and 0.50±0.02 m2 g−1 were at the lower end of the literature values. Using the measured size distributions as well as the mass scattering and absorption efficiencies, Mie calculations provided effective refractive indices of 1.60−0.010i (savanna grass) and 1.56−0.010i (musasa) (λ=0.55 μm). The apparent discrepancy between the low imaginary part of the refractive index and the high apparent elemental carbon (ECa) fractions (8 to 15%) obtained from the thermographic analysis of impactor samples can be explained by a positive bias in the elemental carbon data due to the presence of high molecular weight organic substances. Potential artefacts in optical properties due to instrument bias, non-natural burning conditions and unrealistic dilution history of the laboratory smoke cannot be ruled out and are also discussed in this study.
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    Columnar modelling of nucleation burst evolution in the convective boundary layer - First results from a feasibility study, Part I: Modelling approach
    (München : European Geopyhsical Union, 2006) Hellmuth, O.
    A high-order modelling approach to interpret "continental-type" particle formation bursts in the anthropogenically influenced convective boundary layer (CBL) is proposed. The model considers third-order closure for planetary boundary layer turbulence, sulphur and ammonia chemistry as well as aerosol dynamics. In Paper I of four papers, previous observations of ultrafine particle evolution are reviewed, model equations are derived, the model setup for a conceptual study on binary and ternary homogeneous nucleation is defined and shortcomings of process parameterisation are discussed. In the subsequent Papers II, III and IV simulation results, obtained within the framework of a conceptual study on the CBL evolution and new particle formation (NPF), will be presented and compared with observational findings.
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    Dust events in Beijing, China (2004–2006): Comparison of ground-based measurements with columnar integrated observations
    (München : European Geopyhsical Union, 2009) Wu, Z.J.; Cheng, Y.F.; Hu, M.; Wehner, B.; Sugimoto, N.; Wiedensohler, A.
    Ambient particle number size distributions spanning three years were used to characterize the frequency and intensity of atmospheric dust events in the urban areas of Beijing, China in combination with AERONET sun/sky radiometer data. Dust events were classified into two types based on the differences in particle number and volume size distributions and local weather conditions. This categorization was confirmed by aerosol index images, columnar aerosol optical properties, and vertical potential temperature profiles. During the type-1 events, dust particles dominated the total particle volume concentration (<10 μm), with a relative share over 70%. Anthropogenic particles in the Aitken and accumulation mode played a subordinate role here because of high wind speeds (>4 m s−1). The type-2 events occurred in rather stagnant air masses and were characterized by a lower volume fraction of coarse mode particles (on average, 55%). Columnar optical properties showed that the superposition of dust and anthropogenic aerosols in type-2 events resulted in a much higher AOD (average: 1.51) than for the rather pure dust aerosols in type-1 events (average AOD: 0.36). A discrepancy was found between the ground-based and column integrated particle volume size distributions, especially for the coarse mode particles. This discrepancy likely originates from both the limited comparability of particle volume size distributions derived from Sun photometer and in situ number size distributions, and the inhomogeneous vertical distribution of particles during dust events.
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    Aerosol- and updraft-limited regimes of cloud droplet formation: Influence of particle number, size and hygroscopicity on the activation of cloud condensation nuclei (CCN)
    (München : European Geopyhsical Union, 2009) Reutter, P.; Su, H.; Trentmann, J.; Simmel, M.; Rose, D.; Gunthe, S.S.; Wernli, H.; Andreae, M.O.; Pöschl, U.
    We have investigated the formation of cloud droplets under pyro-convective conditions using a cloud parcel model with detailed spectral microphysics and with the κ-Köhler model approach for efficient and realistic description of the cloud condensation nucleus (CCN) activity of aerosol particles. Assuming a typical biomass burning aerosol size distribution (accumulation mode centred at 120 nm), we have calculated initial cloud droplet number concentrations (NCD) for a wide range of updraft velocities (w=0.25–20 m s−1) and aerosol particle number concentrations (NCN=200–105 cm−3) at the cloud base. Depending on the ratio between updraft velocity and particle number concentration (w/NCN), we found three distinctly different regimes of CCN activation and cloud droplet formation: (1) An aerosol-limited regime that is characterized by high w/NCN ratios (>≈10−3 m s−1 cm3), high maximum values of water vapour supersaturation (Smax>≈0.5%), and high activated fractions of aerosol particles (NCN/NCN>≈90%). In this regime NCD is directly proportional to NCN and practically independent of w. (2) An updraft-limited regime that is characterized by low w/NCN ratios (<≈10−4 m s−1 cm3), low maximum values of water vapour supersaturation (Smax<≈0.2%), and low activated fractions of aerosol particles (NCD/NCN<≈20%). In this regime NCD is directly proportional to w and practically independent of NCN. (3) An aerosol- and updraft-sensitive regime (transitional regime), which is characterized by parameter values in between the two other regimes and covers most of the conditions relevant for pyro-convection. In this regime NCD depends non-linearly on both NCN and w. In sensitivity studies we have tested the influence of aerosol particle size distribution and hygroscopicity on NCD. Within the range of effective hygroscopicity parameters that is characteristic for continental atmospheric aerosols (κ≈0.05–0.6), we found that NCD depends rather weakly on the actual value of κ. A compensation of changes in κ and Smax leads to an effective buffering of NCD. Only for aerosols with very low hygroscopicity (κ<0.05) and also in the updraft-limited regime for aerosols with higher than average hygroscopicity (κ>0.3) did the relative sensitivities ∂lnNCD/∂lnκ≈ (ΔNCD/NCD)/(Δκ/κ) exceed values of ~0.2, indicating that a 50% difference in κ would change NCD by more than 10%. The influence of changing size distribution parameters was stronger than that of particle hygroscopicity. Nevertheless, similar regimes of CCN activation were observed in simulations with varying types of size distributions (polluted and pristine continental and marine aerosols with different proportions of nucleation, Aitken, accumulation, and coarse mode particles). In general, the different regimes can be discriminated with regard to the relative sensitivities of NCD against w and NCN (∂lnNCD/∂lnw and ∂lnNCD/∂lnNCN). We propose to separate the different regimes by relative sensitivity ratios, (∂lnNCD/∂lnw)/(∂lnNCD/∂lnNCN) of 4:1 and 1:4, respectively. The results of this and related studies suggest that the variability of initial cloud droplet number concentration in convective clouds is mostly dominated by the variability of updraft velocity and aerosol particle number concentration in the accumulation and Aitken mode. Coarse mode particles and the variability of particle composition and hygroscopicity appear to play major roles only at low supersaturation in the updraft-limited regime of CCN activation (Smax<0.2%).
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    Around the world in 17 days - Hemispheric-scale transport of forest fire smoke from Russia in May 2003
    (München : European Geopyhsical Union, 2004) Damoah, R.; Spichtinger, N.; Forster, C.; James, P.; Mattis, I.; Wandinger, U.; Beirle, S.; Wagner, T.; Stohl, A.
    In May 2003, severe forest fires in southeast Russia resulted in smoke plumes extending widely across the Northern Hemisphere. This study combines satellite data from a variety of platforms (Moderate Resolution Imaging Spectroradiometer (MODIS), Sea-viewing Wide Field-of-view Sensor (SeaWiFS), Earth Probe Total Ozone Mapping Spectrometer (TOMS) and Global Ozone Monitoring Experiment (GOME)) and vertical aerosol profiles derived with Raman lidar measurements with results from a Lagrangian particle dispersion model to understand the transport processes that led to the large haze plumes observed over North America and Europe. The satellite images provided a unique opportunity for validating model simulations of tropospheric transport on a truly hemispheric scale. Transport of the smoke occurred in two directions: Smoke travelling northwestwards towards Scandinavia was lifted over the Urals and arrived over the Norwegian Sea. Smoke travelling eastwards to the Okhotsk Sea was also lifted, it then crossed the Bering Sea to Alaska from where it proceeded to Canada and was later even observed over Scandinavia and Eastern Europe on its way back to Russia. Not many events of this kind, if any, have been observed, documented and simulated with a transport model comprehensively. The total transport time was about 17 days. We compared transport model simulations using meteorological analysis data from both the European Centre for Medium-Range Weather Forecast (ECMWF) and the National Center for Environmental Prediction (NCEP) in order to find out how well this event could be simulated using these two datasets. Although differences between the two simulations are found on small scales, both agree remarkably well with each other and with the observations on large scales. On the basis of the available observations, it cannot be decided which simulation was more realistic.