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- ItemComparing contact and immersion freezing from continuous flow diffusion chambers(München : European Geopyhsical Union, 2016) Nagare, Baban; Marcolli, Claudia; Welti, André; Stetzer, Olaf; Lohmann, UlrikeIce nucleating particles (INPs) in the atmosphere are responsible for glaciating cloud droplets between 237 and 273 K. Different mechanisms of heterogeneous ice nucleation can compete under mixed-phase cloud conditions. Contact freezing is considered relevant because higher ice nucleation temperatures than for immersion freezing for the same INPs were observed. It has limitations because its efficiency depends on the number of collisions between cloud droplets and INPs. To date, direct comparisons of contact and immersion freezing with the same INP, for similar residence times and concentrations, are lacking. This study compares immersion and contact freezing efficiencies of three different INPs. The contact freezing data were obtained with the ETH CoLlision Ice Nucleation CHamber (CLINCH) using 80 µm diameter droplets, which can interact with INPs for residence times of 2 and 4 s in the chamber. The contact freezing efficiency was calculated by estimating the number of collisions between droplets and particles. Theoretical formulations of collision efficiencies gave too high freezing efficiencies for all investigated INPs, namely AgI particles with 200 nm electrical mobility diameter, 400 and 800 nm diameter Arizona Test Dust (ATD) and kaolinite particles. Comparison of freezing efficiencies by contact and immersion freezing is therefore limited by the accuracy of collision efficiencies. The concentration of particles was 1000 cm−3 for ATD and kaolinite and 500, 1000, 2000 and 5000 cm−3 for AgI. For concentrations < 5000 cm−3, the droplets collect only one particle on average during their time in the chamber. For ATD and kaolinite particles, contact freezing efficiencies at 2 s residence time were smaller than at 4 s, which is in disagreement with a collisional contact freezing process but in accordance with immersion freezing or adhesion freezing. With “adhesion freezing”, we refer to a contact nucleation process that is enhanced compared to immersion freezing due to the position of the INP on the droplet, and we discriminate it from collisional contact freezing, which assumes an enhancement due to the collision of the particle with the droplet. For best comparison with contact freezing results, immersion freezing experiments of the same INPs were performed with the continuous flow diffusion chamber Immersion Mode Cooling chAmber–Zurich Ice Nucleation Chamber (IMCA–ZINC) for a 3 s residence time. In IMCA–ZINC, each INP is activated into a droplet in IMCA and provides its surface for ice nucleation in the ZINC chamber. The comparison of contact and immersion freezing results did not confirm a general enhancement of freezing efficiency for contact compared with immersion freezing experiments. For AgI particles the onset of heterogeneous freezing in CLINCH was even shifted to lower temperatures compared with IMCA–ZINC. For ATD, freezing efficiencies for contact and immersion freezing experiments were similar. For kaolinite particles, contact freezing became detectable at higher temperatures than immersion freezing. Using contact angle information between water and the INP, it is discussed how the position of the INP in or on the droplets may influence its ice nucleation activity.
- ItemPotential of polarization/Raman lidar to separate fine dust, coarse dust, maritime, and anthropogenic aerosol profiles(München : European Geopyhsical Union, 2017) Mamouri, Rodanthi-Elisavet; Ansmann, AlbertWe applied the recently introduced polarization lidar–photometer networking (POLIPHON) technique for the first time to triple-wavelength polarization lidar measurements at 355, 532, and 1064 nm. The lidar observations were performed at Barbados during the Saharan Aerosol Long-Range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) in the summer of 2014. The POLIPHON method comprises the traditional lidar technique to separate mineral dust and non-dust backscatter contributions and the new, extended approach to separate even the fine and coarse dust backscatter fractions. We show that the traditional and the advanced method are compatible and lead to a consistent set of dust and non-dust profiles at simplified, less complex aerosol layering and mixing conditions as is the case over the remote tropical Atlantic. To derive dust mass concentration profiles from the lidar observations, trustworthy extinction-to-volume conversion factors for fine, coarse, and total dust are needed and obtained from an updated, extended Aerosol Robotic Network sun photometer data analysis of the correlation between the fine, coarse and total dust volume concentration and the respective fine, coarse, and total dust extinction coefficient for all three laser wavelengths. Conversion factors (total volume to extinction) for pure marine aerosol conditions and continental anthropogenic aerosol situations are presented in addition. As a new feature of the POLIPHON data analysis, the Raman lidar method for particle extinction profiling is used to identify the aerosol type (marine or anthropogenic) of the non-dust aerosol fraction. The full POLIPHON methodology was successfully applied to a SALTRACE case and the results are discussed. We conclude that the 532 nm polarization lidar technique has many advantages in comparison to 355 and 1064 nm polarization lidar approaches and leads to the most robust and accurate POLIPHON products.
- ItemSaharan dust contribution to the Caribbean summertime boundary layer - A lidar study during SALTRACE(München : European Geopyhsical Union, 2016) Groß, Silke; Gasteiger, Josef; Freudenthaler, Volker; Müller, Thomas; Sauer, Daniel; Toledano, Carlos; Ansmann, AlbertDual-wavelength lidar measurements with the small lidar system POLIS of the Ludwig-Maximilians-Universität München were performed during the SALTRACE experiment at Barbados in June and July 2013. Based on high-accuracy measurements of the linear depolarization ratio down to about 200 m above ground level, the dust volume fraction and the dust mass concentration within the convective marine boundary layer can be derived. Additional information from radiosonde launches at the ground-based measurement site provide independent information on the convective marine boundary layer height and the meteorological situation within the convective marine boundary layer. We investigate the lidar-derived optical properties, the lidar ratio and the particle linear depolarization ratio at 355 and 532 nm and find mean values of 0.04 (SD 0.03) and 0.05 (SD 0.04) at 355 and 532 nm, respectively, for the particle linear depolarization ratio, and (26 ± 5) sr for the lidar ratio at 355 and 532 nm. For the concentration of dust in the convective marine boundary layer we find that most values were between 20 and 50 µgm−3. On most days the dust contribution to total aerosol volume was about 30–40 %. Comparing the dust contribution to the column-integrated sun-photometer measurements we see a correlation between high dust contribution, high total aerosol optical depth and a low Angström exponent, and of low dust contribution with low total aerosol optical depth.
- ItemLaboratory-generated mixtures of mineral dust particles with biological substances: Characterization of the particle mixing state and immersion freezing behavior(München : European Geopyhsical Union, 2016) Augustin-Bauditz, Stefanie; Wex, Heike; Denjean, Cyrielle; Hartmann, Susan; Schneider, Johannes; Schmidt, Susann; Ebert, Martin; Stratmann, FrankBiological particles such as bacteria, fungal spores or pollen are known to be efficient ice nucleating particles. Their ability to nucleate ice is due to ice nucleation active macromolecules (INMs). It has been suggested that these INMs maintain their nucleating ability even when they are separated from their original carriers. This opens the possibility of an accumulation of such INMs in soils, resulting in an internal mixture of mineral dust and INMs. If particles from such soils which contain biological INMs are then dispersed into the atmosphere due to wind erosion or agricultural processes, they could induce ice nucleation at temperatures typical for biological substances, i.e., above −20 up to almost 0 °C, while they might be characterized as mineral dust particles due to a possibly low content of biological material. We conducted a study within the research unit INUIT (Ice Nucleation research UnIT), where we investigated the ice nucleation behavior of mineral dust particles internally mixed with INM. Specifically, we mixed a pure mineral dust sample (illite-NX) with ice active biological material (birch pollen washing water) and quantified the immersion freezing behavior of the resulting particles utilizing the Leipzig Aerosol Cloud Interaction Simulator (LACIS). A very important topic concerning the investigations presented here as well as for atmospheric application is the characterization of the mixing state of aerosol particles. In the present study we used different methods like single-particle aerosol mass spectrometry, Scanning Electron Microscopy (SEM), Energy Dispersive X-ray analysis (EDX), and a Volatility–Hygroscopicity Tandem Differential Mobility Analyser (VH-TDMA) to investigate the mixing state of our generated aerosol. Not all applied methods performed similarly well in detecting small amounts of biological material on the mineral dust particles. Measuring the hygroscopicity/volatility of the mixed particles with the VH-TDMA was the most sensitive method. We found that internally mixed particles, containing ice active biological material, follow the ice nucleation behavior observed for the pure biological particles. We verified this by modeling the freezing behavior of the mixed particles with the Soccerball model (SBM). It can be concluded that a single INM located on a mineral dust particle determines the freezing behavior of that particle with the result that freezing occurs at temperatures at which pure mineral dust particles are not yet ice active.
- ItemProfiling of aerosol microphysical properties at several EARLINET/AERONET sites during the July 2012 ChArMEx/EMEP campaign(München : European Geopyhsical Union, 2016) Granados-Muñoz, María José; Navas-Guzmán, Francisco; Guerrero-Rascado, Juan Luis; Bravo-Aranda, Juan Antonio; Pereira, Sergio Nepomuceno; Basart, Sara; Baldasano, José María; Belegante, Livio; Chaikovsky, Anatoli; Comerón, Adolfo; D'Amico, Giuseppe; Dubovik, Oleg; Ilic, Luka; Kokkalis, Panos; Muñoz-Porcar, Constantino; Nickovic, Slobodan; Nicolae, Doina; Facchini, Maria Cristina; Olmo, Francisco José; Papayannis, Alexander; Pappalardo, Gelsomina; Rodríguez, Alejandro; Schepanski, Kerstin; Sicard, Michaël; Vukovic, Ana; Wandinger, Ulla; Dulac, François; Alados-Arboledas, LucasThe simultaneous analysis of aerosol microphysical properties profiles at different European stations is made in the framework of the ChArMEx/EMEP 2012 field campaign (9–11 July 2012). During and in support of this campaign, five lidar ground-based stations (Athens, Barcelona, Bucharest, Évora, and Granada) performed 72 h of continuous lidar measurements and collocated and coincident sun-photometer measurements. Therefore it was possible to retrieve volume concentration profiles with the Lidar Radiometer Inversion Code (LIRIC). Results indicated the presence of a mineral dust plume affecting the western Mediterranean region (mainly the Granada station), whereas a different aerosol plume was observed over the Balkans area. LIRIC profiles showed a predominance of coarse spheroid particles above Granada, as expected for mineral dust, and an aerosol plume composed mainly of fine and coarse spherical particles above Athens and Bucharest. Due to the exceptional characteristics of the ChArMEx database, the analysis of the microphysical properties profiles' temporal evolution was also possible. An in-depth analysis was performed mainly at the Granada station because of the availability of continuous lidar measurements and frequent AERONET inversion retrievals. The analysis at Granada was of special interest since the station was affected by mineral dust during the complete analyzed period. LIRIC was found to be a very useful tool for performing continuous monitoring of mineral dust, allowing for the analysis of the dynamics of the dust event in the vertical and temporal coordinates. Results obtained here illustrate the importance of having collocated and simultaneous advanced lidar and sun-photometer measurements in order to characterize the aerosol microphysical properties in both the vertical and temporal coordinates at a regional scale. In addition, this study revealed that the use of the depolarization information as input in LIRIC in the stations of Bucharest, Évora, and Granada was crucial for the characterization of the aerosol types and their distribution in the vertical column, whereas in stations lacking depolarization lidar channels, ancillary information was needed. Results obtained were also used for the validation of different mineral dust models. In general, the models better forecast the vertical distribution of the mineral dust than the column-integrated mass concentration, which was underestimated in most of the cases.
- ItemSize distribution and optical properties of mineral dust aerosols transported in the western Mediterranean(München : European Geopyhsical Union, 2016) Denjean, C.; Cassola, F.; Mazzino, A.; Triquet, S.; Chevaillier, S.; Grand, N.; Bourrianne, T.; Momboisse, G.; Sellegri, K.; Schwarzenbock, A.; Freney, E.; Mallet, M.; Formenti, P.This study presents in situ aircraft measurements of Saharan mineral dust transported over the western Mediterranean basin in June–July 2013 during the ChArMEx/ADRIMED (the Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) airborne campaign. Dust events differing in terms of source region (Algeria, Tunisia and Morocco), time of transport (1–5 days) and height of transport were sampled. Mineral dust were transported above the marine boundary layer, which conversely was dominated by pollution and marine aerosols. The dust vertical structure was extremely variable and characterized by either a single layer or a more complex and stratified structure with layers originating from different source regions. Mixing of mineral dust with pollution particles was observed depending on the height of transport of the dust layers. Dust layers carried a higher concentration of pollution particles below 3 km above sea level (a.s.l.) than above 3 km a.s.l., resulting in a scattering Ångström exponent up to 2.2 below 3 km a.s.l. However, the optical properties of the dust plumes remained practically unchanged with respect to values previously measured over source regions, regardless of the altitude. Moderate absorption of light by the dust plumes was observed with values of aerosol single scattering albedo at 530 nm ranging from 0.90 to 1.00. Concurrent calculations from the aerosol chemical composition revealed a negligible contribution of pollution particles to the absorption properties of the dust plumes that was due to a low contribution of refractory black carbon in regards to the fraction of dust and sulfate particles. This suggests that, even in the presence of moderate pollution, likely a persistent feature in the Mediterranean, the optical properties of the dust plumes could be assumed similar to those of native dust in radiative transfer simulations, modelling studies and satellite retrievals over the Mediterranean. Measurements also showed that the coarse mode of mineral dust was conserved even after 5 days of transport in the Mediterranean, which contrasts with the gravitational depletion of large particles observed during the transport of dust plumes over the Atlantic. Simulations with the WRF mesoscale meteorological model highlighted a strong vertical turbulence within the dust layers that could prevent deposition of large particles during their atmospheric transport. This has important implications for the dust radiative effects due to surface dimming, atmospheric heating and cloud formation. The results presented here add to the observational data set necessary for evaluating the role of mineral dust on the regional climate and rainfall patterns in the western Mediterranean basin and understanding their atmospheric transport at global scale.
- ItemNew developments in the representation of Saharan dust sources in the aerosol-climate model ECHAM6-HAM2(München : European Geopyhsical Union, 2016) Heinold, Bernd; Tegen, Ina; Schepanski, Kerstin; Banks, Jamie R.In the aerosol-climate model ECHAM6-HAM2, dust source activation (DSA) observations from Meteosat Second Generation (MSG) satellite are proposed to replace the original source area parameterization over the Sahara Desert. The new setup is tested in nudged simulations for the period 2007 to 2008. The evaluation is based on comparisons to dust emission events inferred from MSG dust index imagery, Aerosol Robotic Network (AERONET) sun photometer observations, and satellite retrievals of aerosol optical thickness (AOT). The model results agree well with AERONET measurements especially in terms of seasonal variability, and a good spatial correlation was found between model results and MSG-SEVIRI (Spinning-Enhanced Visible and InfraRed Imager) dust AOT as well as Multi-angle Imaging SpectroRadiometer (MISR) AOT. ECHAM6-HAM2 computes a more realistic geographical distribution and up to 20 % higher annual Saharan dust emissions, using the MSG-based source map. The representation of dust AOT is partly improved in the southern Sahara and Sahel. In addition, the spatial variability is increased towards a better agreement with observations depending on the season. Thus, using the MSG DSA map can help to circumvent the issue of uncertain soil input parameters. An important issue remains the need to improve the model representation of moist convection and stable nighttime conditions. Compared to sub-daily DSA information from MSG-SEVIRI and results from a regional model, ECHAM6-HAM2 notably underestimates the important fraction of morning dust events by the breakdown of the nocturnal low-level jet, while a major contribution is from afternoon-to-evening emissions.