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    Atmospheric black carbon and warming effects influenced by the source and absorption enhancement in central Europe
    (München : European Geopyhsical Union, 2014) Nordmann, S.; Cheng, Y.F.; Carmichael, G.R.; Yu, M.; van der Gon, H.A.C.Denier; Zhang, Q.; Saide, P.E.; Pöschl, U.; Su, H.; Birmili, W.; Wiedensohler, A.
    Particles containing black carbon (BC), a strong absorbing substance, exert a rather uncertain direct and indirect radiative forcing in the atmosphere. To investigate the mass concentration and absorption properties of BC particles over central Europe, the model WRF-Chem was used at a resolution of 12 km in conjunction with a high-resolution BC emission inventory (EUCAARI 42-Pan-European Carbonaceous Aerosol Inventory; 1/8° × 1/16°). The model simulation was evaluated using measurements of equivalent soot carbon, absorption coefficients and particle number concentrations at seven sites within the German Ultrafine Aerosol Network, PM mass concentrations from the dense measurement network of the German Federal Environmental Agency at 392 monitoring stations, and aerosol optical depth from MODIS and AERONET. A distinct time period (25 March to 10 April 2009) was chosen, during which the clean marine air mass prevailed in the first week and afterwards the polluted continental air mass mainly from the southeast dominated with elevated daily average BC concentration of up to 4 μ g m−3. The simulated PM mass concentration, aerosol number concentration and optical depth were in good agreement with the observations, while the modelled BC mass concentrations were found to be a factor of 2 lower than the observations. Together with back trajectories, detailed model bias analyses suggested that the current BC emission in countries to the east and south of Germany might be underestimated by a factor of 5, at least for the simulation period. Running the model with upscaled BC emissions in these regions led to a smaller model bias and a better correlation between model and measurement. In contrast, the particle absorption coefficient was positively biased by about 20% even when the BC mass concentration was underestimated by around 50%. This indicates that the internal mixture treatment of BC in the WRF-Chem optical calculation is unrealistic in our case, which overamplifies the light absorption by BC-containing particles. By adjusting the modelled mass absorption cross-section towards the measured values, the simulation of particle light absorption of BC was improved as well. Finally, the positive direct radiative forcing of BC particles at the top of the atmosphere was estimated to be in the range of 0 to +4 W m−2 over Germany for the model run with improved BC mass concentration and adjusted BC light absorption cross-section. This adjustment lowered the positive forcing of BC by up to 70%, compared with the internal mixing treatment of BC in the model simulation.
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    Diurnal variations of aerosol optical properties in the North China Plain and their influences on the estimates of direct aerosol radiative effect
    (München : European Geopyhsical Union, 2015) Kuang, Y.; Zhao, C.S.; Tao, J.C.; Ma, N.
    In this paper, the diurnal variations of aerosol optical properties and their influences on the estimation of daily average direct aerosol radiative effect (DARE) in the North China Plain (NCP) are investigated based on in situ measurements from Haze in China campaign. For ambient aerosol, the diurnal patterns of single scattering albedo (SSA) and asymmetry factor (g) in the NCP are both highest at dawn and lowest in the late afternoon, and quite different from those of dry-state aerosol. The relative humidity (RH) is the dominant factor which determines the diurnal pattern of SSA and g for ambient aerosol. Basing on the calculated SSA and g, several cases are designed to investigate the impacts of the diurnal changes of aerosol optical properties on DARE. The results demonstrate that the diurnal changes of SSA and g in the NCP have significant influences on the estimation of DARE at the top of the atmosphere (TOA). If the full temporal coverage of aerosol optical depth (AOD), SSA and g are available, an accurate estimation of daily average DARE can be achieved by using the daily averages of AOD, SSA and g. However, due to the lack of full temporal coverage data sets of SSA and g, their daily averages are usually not available. Basing on the results of designed cases, if the RH plays a dominant role in the diurnal variations of SSA and g, we suggest that using both SSA and g averaged over early morning and late afternoon as inputs for radiative transfer model to improve the accurate estimation of DARE. If the temporal samplings of SSA or g are too few to adopt this method, either averaged over early morning or late afternoon of both SSA and g can be used to improve the estimation of DARE at the TOA.
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    Adaption of the MODIS aerosol retrieval algorithm using airborne spectral surface reflectance measurements over urban areas: A case study
    (München : European Geopyhsical Union, 2015) Jäkel, E.; Mey, B.; Levy, R.; Gu, X.; Yu, T.; Li, Z.; Althausen, D.; Heese, B.; Wendisch, M.
    MODIS (MOderate-resolution Imaging Spectroradiometer) retrievals of aerosol optical depth (AOD) are biased over urban areas, primarily because the reflectance characteristics of urban surfaces are different than that assumed by the retrieval algorithm. Specifically, the operational "dark-target" retrieval is tuned towards vegetated (dark) surfaces and assumes a spectral relationship to estimate the surface reflectance in blue and red wavelengths. From airborne measurements of surface reflectance over the city of Zhongshan, China, were collected that could replace the assumptions within the MODIS retrieval algorithm. The subsequent impact was tested upon two versions of the operational algorithm, Collections 5 and 6 (C5 and C6). AOD retrieval results of the operational and modified algorithms were compared for a specific case study over Zhongshan to show minor differences between them all. However, the Zhongshan-based spectral surface relationship was applied to a much larger urban sample, specifically to the MODIS data taken over Beijing between 2010 and 2014. These results were compared directly to ground-based AERONET (AErosol RObotic NETwork) measurements of AOD. A significant reduction of the differences between the AOD retrieved by the modified algorithms and AERONET was found, whereby the mean difference decreased from 0.27±0.14 for the operational C5 and 0.19±0.12 for the operational C6 to 0.10±0.15 and -0.02±0.17 by using the modified C5 and C6 retrievals. Since the modified algorithms assume a higher contribution by the surface to the total measured reflectance from MODIS, consequently the overestimation of AOD by the operational methods is reduced. Furthermore, the sensitivity of the MODIS AOD retrieval with respect to different surface types was investigated. Radiative transfer simulations were performed to model reflectances at top of atmosphere for predefined aerosol properties. The reflectance data were used as input for the retrieval methods. It was shown that the operational MODIS AOD retrieval over land reproduces the AOD reference input of 0.85 for dark surface types (retrieved AOD = 0.87 (C5)). An overestimation of AOD = 0.99 is found for urban surfaces, whereas the modified C5 algorithm shows a good performance with a retrieved value of AOD = 0.86.
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    Profiling of Saharan dust from the Caribbean to western Africa-Part 1: Layering structures and optical properties from shipborne polarization/Raman lidar observations
    (Katlenburg-Lindau : EGU, 2017) Rittmeister, Franziska; Ansmann, Albert; Engelmann, Ronny; Skupin, Annett; Baars, Holger; Kanitz, Thomas; Kinne, Stefan
    We present final and quality-assured results of multiwavelength polarization/Raman lidar observations of the Saharan air layer (SAL) over the tropical Atlantic. Observations were performed aboard the German research vessel R/V Meteor during the 1-month transatlantic cruise from Guadeloupe to Cabo Verde over 4500 km from 61.5 to 20 W at 14-15 N in April-May 2013. First results of the shipborne lidar measurements, conducted in the framework of SALTRACE (Saharan Aerosol Long-range Transport and Aerosol-Cloud Interaction Experiment), were reported by Kanitz et al. (2014). Here, we present four observational cases representing key stages of the SAL evolution between Africa and the Caribbean in detail in terms of layering structures and optical properties of the mixture of predominantly dust and aged smoke in the SAL. We discuss to what extent the lidar results confirm the validity of the SAL conceptual model which describes the dust long-range transport and removal processes over the tropical Atlantic. Our observations of a clean marine aerosol layer (MAL, layer from the surface to the SAL base) confirm the conceptual model and suggest that the removal of dust from the MAL, below the SAL, is very efficient. However, the removal of dust from the SAL assumed in the conceptual model to be caused by gravitational settling in combination with large-scale subsidence is weaker than expected. To explain the observed homogenous (heightindependent) dust optical properties from the SAL base to the SAL top, from the African coast to the Caribbean, we have to assume that the particle sedimentation strength is reduced and dust vertical mixing and upward transport mechanisms must be active in the SAL. Based on lidar observations on 20 nights at different longitudes in May 2013, we found, on average, MAL and SAL layer mean values (at 532 nm) of the extinction-to-backscatter ratio (lidar ratio) of 17-5 sr (MAL) and 43±8 sr (SAL), of the particle linear depolarization ratio of 0:025±0:015 (MAL) and 0:19±0:09 (SAL), and of the particle extinction coefficient of 67±45Mm..1 (MAL) and 68±37Mm..1 (SAL). The 532 nm optical depth of the lofted SAL was found to be, on average, 0:15±0:13 during the ship cruise. The comparably low values of the SAL mean lidar ratio and depolarization ratio (compared to typical pure dust values of 50-60 sr and 0.3, respectively) in combination with backward trajectories indicate a smoke contribution to light extinction of the order of 20% during May 2013, at the end of the burning season in central-western Africa. 1.
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    In situ, satellite measurement and model evidence on the dominant regional contribution to fine particulate matter levels in the Paris megacity
    (Katlenburg-Lindau : EGU, 2015) Beekmann, M.; Prévôt, A.S.H.; Drewnick, F.; Sciare, J.; Pandis, S.N.; Denier van der Gon, H.A.C.; Crippa, M.; Freutel, F.; Poulain, L.; Ghersi, V.; Rodriguez, E.; Beirle, S.; Zotter, P.; von der Weiden-Reinmüller, S.-L.; Bressi, M.; Fountoukis, C.; Petetin, H.; Szidat, S.; Schneider, J.; Rosso, A.; El Haddad, I.; Megaritis, A.; Zhang, Q.J.; Michoud, V.; Slowik, J.G.; Moukhtar, S.; Kolmonen, P.; Stohl, A.; Eckhardt, S.; Borbon, A.; Gros, V.; Marchand, N.; Jaffrezo, J.L.; Schwarzenboeck, A.; Colomb, A.; Wiedensohler, A.; Borrmann, S.; Lawrence, M.; Baklanov, A.; Baltensperger, U.
    A detailed characterization of air quality in the megacity of Paris (France) during two 1-month intensive campaigns and from additional 1-year observations revealed that about 70 % of the urban background fine particulate matter (PM) is transported on average into the megacity from upwind regions. This dominant influence of regional sources was confirmed by in situ measurements during short intensive and longer-term campaigns, aerosol optical depth (AOD) measurements from ENVISAT, and modeling results from PMCAMx and CHIMERE chemistry transport models. While advection of sulfate is well documented for other megacities, there was surprisingly high contribution from long-range transport for both nitrate and organic aerosol. The origin of organic PM was investigated by comprehensive analysis of aerosol mass spectrometer (AMS), radiocarbon and tracer measurements during two intensive campaigns. Primary fossil fuel combustion emissions constituted less than 20 % in winter and 40 % in summer of carbonaceous fine PM, unexpectedly small for a megacity. Cooking activities and, during winter, residential wood burning are the major primary organic PM sources. This analysis suggests that the major part of secondary organic aerosol is of modern origin, i.e., from biogenic precursors and from wood burning. Black carbon concentrations are on the lower end of values encountered in megacities worldwide, but still represent an issue for air quality. These comparatively low air pollution levels are due to a combination of low emissions per inhabitant, flat terrain, and a meteorology that is in general not conducive to local pollution build-up. This revised picture of a megacity only being partially responsible for its own average and peak PM levels has important implications for air pollution regulation policies.
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    Saharan dust transport and deposition towards the tropicalnorthern Atlantic
    (Göttingen : Copernicus, 2009) Schepanski, K.; Tegen, I.; MacKe, A.
    We present a study of Saharan dust export towards the tropical North Atlantic using the regional dust emission, transport and deposition model LM-MUSCAT. Horizontal and vertical distribution of dust optical thickness, concentration, and dry and wet deposition rates are used to describe seasonality of dust export and deposition towards the eastern Atlantic for three typical months in different seasons. Deposition rates strongly depend on the vertical dust distribution, which differs with seasons. Furthermore the contribution of dust originating from the Bod́eĺe Depression to Saharan dust over the Atlantic is investigated. A maximum contribution of Bod́eĺe dust transported towards the Cape Verde Islands is evident in winter when the Bod́eĺe source area is most active and dominant with regard to activation frequency and dust emission. Limitations of using satellite retrievals to estimate dust deposition are highlighted.
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    Sun photometer retrievals of Saharan dust properties over Barbados during SALTRACE
    (Katlenburg-Lindau : EGU, 2019) Toledano, Carlos; Torres, Benjamín; Velasco-Merino, Cristian; Althausen, Dietrich; Groß, Silke; Wiegner, Matthias; Weinzierl, Bernadett; Gasteiger, Josef; Ansmann, Albert; González, Ramiro; Mateos, David; Farrel, David; Müller, Thomas; Haarig, Moritz; Cachorro, Victoria E.
    The Saharan Aerosol Long-Range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) was devoted to the investigation of Saharan dust properties over the Caribbean. The campaign took place in June-July 2013. A wide set of ground-based and airborne aerosol instrumentation was deployed at the island of Barbados for a comprehensive experiment. Several sun photometers performed measurements during this campaign: two AERONET (Aerosol Robotic Network) Cimel sun photometers and the Sun and Sky Automatic Radiometer (SSARA). The sun photometers were co-located with the ground-based multi-wavelength lidars BERTHA (Backscatter Extinction lidar Ratio Temperature Humidity profiling Apparatus) and POLIS (Portable Lidar System). Aerosol properties derived from direct sun and sky radiance observations are analyzed, and a comparison with the co-located lidar and in situ data is provided. The time series of aerosol optical depth (AOD) allows identifying successive dust events with short periods in between in which the marine background conditions were observed. The moderate aerosol optical depth in the range of 0.3 to 0.6 was found during the dust periods. The sun photometer infrared channel at the 1640nm wavelength was used in the retrieval to investigate possible improvements to aerosol size retrievals, and it was expected to have a larger sensitivity to coarse particles. The comparison between column (aerosol optical depth) and surface (dust concentration) data demonstrates the connection between the Saharan Air Layer and the boundary layer in the Caribbean region, as is shown by the synchronized detection of the successive dust events in both datasets. However the differences of size distributions derived from sun photometer data and in situ observations reveal the difficulties in carrying out a column closure study. © 2019 All rights reserved.
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    CARIBIC aircraft measurements of Eyjafjallajökull volcanic clouds in April/May 2010
    (München : European Geopyhsical Union, 2012) Rauthe-Schöch, A.; Weigelt, A.; Hermann, M.; Martinsson, B.G.; Baker, A.K.; Heue, K.-P.; Brenninkmeijer, C.A.M.; Zahn, A.; Scharffe, D.; Eckhardt, S.; Stohl, A.; van Velthoven, P.F.J.
    The Civil Aircraft for the Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) project investigates physical and chemical processes in the Earth's atmosphere using a Lufthansa Airbus long-distance passenger aircraft. After the beginning of the explosive eruption of the Eyjafjallajökull volcano on Iceland on 14 April 2010, the first CARIBIC volcano-specific measurement flight was carried out over the Baltic Sea and Southern Sweden on 20 April. Two more flights followed: one over Ireland and the Irish Sea on 16 May and the other over the Norwegian Sea on 19 May 2010. During these three special mission flights the CARIBIC container proved its merits as a comprehensive flying laboratory. The elemental composition of particles collected over the Baltic Sea during the first flight (20 April) indicated the presence of volcanic ash. Over Northern Ireland and the Irish Sea (16 May), the DOAS system detected SO2 and BrO co-located with volcanic ash particles that increased the aerosol optical depth. Over the Norwegian Sea (19 May), the optical particle counter detected a strong increase of particles larger than 400 nm diameter in a region where ash clouds were predicted by aerosol dispersion models. Aerosol particle samples collected over the Irish Sea and the Norwegian Sea showed large relative enhancements of the elements silicon, iron, titanium and calcium. Non-methane hydrocarbon concentrations in whole air samples collected on 16 and 19 May 2010 showed a pattern of removal of several hydrocarbons that is typical for chlorine chemistry in the volcanic clouds. Comparisons of measured ash concentrations and simulations with the FLEXPART dispersion model demonstrate the difficulty of detailed volcanic ash dispersion modelling due to the large variability of the volcanic cloud sources, extent and patchiness as well as the thin ash layers formed in the volcanic clouds.
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    Algorithms and uncertainties for the determination of multispectral irradiance components and aerosol optical depth from a shipborne rotating shadowband radiometer
    (Katlenburg-Lindau : Copernicus, 2017) Witthuhn, Jonas; Deneke, Hartwig; Macke, Andreas; Bernhard, Germar
    The 19-channel rotating shadowband radiometer GUVis-3511 built by Biospherical Instruments provides automated shipborne measurements of the direct, diffuse and global spectral irradiance components without a requirement for platform stabilization. Several direct sun products, including spectral direct beam transmittance, aerosol optical depth, Ångström exponent and precipitable water, can be derived from these observations. The individual steps of the data analysis are described, and the different sources of uncertainty are discussed. The total uncertainty of the observed direct beam transmittances is estimated to be about 4% for most channels within a 95% confidence interval for shipborne operation. The calibration is identified as the dominating contribution to the total uncertainty. A comparison of direct beam transmittance with those obtained from a Cimel sunphotometer at a land site and a manually operated Microtops II sunphotometer on a ship is presented. Measurements deviate by less than 3 and 4% on land and on ship, respectively, for most channels and in agreement with our previous uncertainty estimate. These numbers demonstrate that the instrument is well suited for shipborne operation, and the applied methods for motion correction work accurately. Based on spectral direct beam transmittance, aerosol optical depth can be retrieved with an uncertainty of 0.02 for all channels within a 95% confidence interval. The different methods to account for Rayleigh scattering and gas absorption in our scheme and in the Aerosol Robotic Network processing for Cimel sunphotometers lead to minor deviations. Relying on the cross calibration of the 940 nm water vapor channel with the Cimel sunphotometer, the column amount of precipitable water can be estimated with an uncertainty of ±0.034 cm.
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    Optical and geometrical aerosol particle properties over the United Arab Emirates
    (Katlenburg-Lindau : EGU, 2020) Filioglou, Maria; Giannakaki, Elina; Backman, John; Kesti, Jutta; Hirsikko, Anne; Engelmann, Ronny; O’Connor, Ewan; Leskinen, Jari T.T.; Shang, Xiaoxia; Korhonen, Hannele; Lihavainen, Heikki; Romakkaniemi, Sami; Komppula, Mika
    One year of ground-based night-time Raman lidar observations has been analysed under the Optimization of Aerosol Seeding In rain enhancement Strategies (OASIS) project, in order to characterize the aerosol particle properties over a rural site in the United Arab Emirates. In total, 1130 aerosol particle layers were detected during the 1-year measurement campaign which took place between March 2018 and February 2019. Several subsequent aerosol layers could be observed simultaneously in the atmosphere up to 11 km. The observations indicate that the measurement site is a receptor of frequent dust events, but predominantly the dust is mixed with aerosols of anthropogenic and/or marine origin. The mean aerosol optical depth over the measurement site ranged at 0.37±0.12 and 0.21±0.11 for 355 and 532 nm, respectively. Moreover, mean lidar ratios of 43±11 sr at a wavelength of 355 nm and 39±10 sr at 532 nm were found. The average linear particle depolarization ratio measured over the course of the campaign was 15±6% and 19±7% at the 355 and 532 nm wavelengths, respectively. Since the region is both a source and a receptor of mineral dust, we have also explored the properties of Arabian mineral dust of the greater area of the United Arab of Emirates and the Arabian Peninsula. The observed Arabian dust particle properties were 45±5 (42±5) sr at 355 (532) nm for the lidar ratio, 25±2% (31±2 %) for the linear particle depolarization ratio at 355 (532) nm, and 0.3±0.2 (0.2±0.2) for the extinction-related Angstrom exponent (backscatterrelated Angstrom exponent) between 355 and 532 nm. This study is the first to report comprehensive optical properties of the Arabian dust particles based on 1-year long observations, using to their fullest the capabilities of a multi-wavelength Raman lidar instrument. The results suggest that the mineral dust properties over the Middle East and western Asia, including the observation site, are comparable to those of African mineral dust with regard to the particle depolarization ratios, but not for lidar ratios. The smaller lidar ratio values in this study compared to the reference studies are attributed to the difference in the geochemical characteristics of the soil originating in the study region compared to northern Africa. © 2020 Royal Society of Chemistry. All rights reserved.