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- ItemProfiling 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, StefanWe 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.
- ItemAlgorithms 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, GermarThe 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.
- ItemVertical profiling of aerosol hygroscopic properties in the planetary boundary layer during the PEGASOS campaigns(München : European Geopyhsical Union, 2016) Rosati, Bernadette; Gysel, Martin; Rubach, Florian; Mentel, Thomas F.; Goger, Brigitta; Poulain, Laurent; Schlag, Patrick; Miettinen, Pasi; Pajunoja, Aki; Virtanen, Annele; Baltink, Henk Klein; Henzing, J.S. Bas; Größ, Johannes; Gobbi, Gian Paolo; Wiedensohler, Alfred; Kiendler-Scharr, Astrid; Decesari, Stefano; Facchini, Maria Cristina; Weingartner, Ernest; Baltensperger, UrsVertical profiles of the aerosol particles hygroscopic properties, their mixing state as well as chemical composition were measured above northern Italy and the Netherlands. An aerosol mass spectrometer (AMS; for chemical composition) and a white-light humidified optical particle spectrometer (WHOPS; for hygroscopic growth) were deployed on a Zeppelin NT airship within the PEGASOS project. This allowed one to investigate the development of the different layers within the planetary boundary layer (PBL), providing a unique in situ data set for airborne aerosol particles properties in the first kilometre of the atmosphere. Profiles measured during the morning hours on 20 June 2012 in the Po Valley, Italy, showed an increased nitrate fraction at  ∼  100 m above ground level (a.g.l.) coupled with enhanced hygroscopic growth compared to  ∼  700 m a. g. l. This result was derived from both measurements of the aerosol composition and direct measurements of the hygroscopicity, yielding hygroscopicity parameters (κ) of 0.34  ±  0.12 and 0.19  ±  0.07 for 500 nm particles, at  ∼  100 and  ∼  700 m a. g. l., respectively. The difference is attributed to the structure of the PBL at this time of day which featured several independent sub-layers with different types of aerosols. Later in the day the vertical structures disappeared due to the mixing of the layers and similar aerosol particle properties were found at all probed altitudes (mean κ ≈ 0.18  ±  0.07). The aerosol properties observed at the lowest flight level (100 m a. g. l.) were consistent with parallel measurements at a ground site, both in the morning and afternoon. Overall, the aerosol particles were found to be externally mixed, with a prevailing hygroscopic fraction. The flights near Cabauw in the Netherlands in the fully mixed PBL did not feature altitude-dependent characteristics. Particles were also externally mixed and had an even larger hygroscopic fraction compared to the results in Italy. The mean κ from direct measurements was 0.28 ±  0.10, thus considerably higher than κ values measured in Italy in the fully mixed PBL.
- ItemProfiling of aerosol microphysical properties at several EARLINET/AERONET sites during the July 2012 ChArMEx/EMEP campaign(München : European Geopyhsical Union, 2016) Granados-Muñoz, MarÃa José; Navas-Guzmán, Francisco; Guerrero-Rascado, Juan Luis; Bravo-Aranda, Juan Antonio; Pereira, Sergio Nepomuceno; Basart, Sara; Baldasano, José MarÃa; 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; RodrÃguez, 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.
- ItemFour-year long-path monitoring of ambient aerosol extinction at a central European urban site: Dependence on relative humidity(München : European Geopyhsical Union, 2016) Skupin, A.; Ansmann, A.; Engelmann, R.; Seifert, P.; Müller, T.The ambient aerosol particle extinction coefficient is measured with the Spectral Aerosol Extinction Monitoring System (SÆMS) along a 2.84 km horizontal path at 30–50 m height above ground in the urban environment of Leipzig (51.3° N, 12.4° E), Germany, since 2009. The dependence of the particle extinction coefficient (wavelength range from 300 to 1000 nm) on relative humidity up to almost 100 % was investigated. The main results are presented. For the wavelength of 550 nm, the mean extinction enhancement factor was found to be 1.75 ± 0.4 for an increase of relative humidity from 40 to 80 %. The respective 4-year mean extinction enhancement factor is 2.8 ± 0.6 for a relative-humidity increase from 40 to 95 %. A parameterization of the dependency of the urban particle extinction coefficient on relative humidity is presented. A mean hygroscopic exponent of 0.46 for the 2009–2012 period was determined. Based on a backward trajectory cluster analysis, the dependence of several aerosol optical properties for eight air flow regimes was investigated. Large differences were not found, indicating that local pollution sources widely control the aerosol conditions over the urban site. The comparison of the SÆMS extinction coefficient statistics with respective statistics from ambient AERONET sun photometer observations yields good agreement. Also, time series of the particle extinction coefficient computed from in situ-measured dry particle size distributions and humidity-corrected SÆMS extinction values (for 40 % relative humidity) were found in good overall consistency, which verifies the applicability of the developed humidity parameterization scheme. The analysis of the spectral dependence of particle extinction (Ångström exponent) revealed an increase of the 390–881 nm Ångström exponent from, on average, 0.3 (at 30 % relative humidity) to 1.3 (at 95 % relative humidity) for the 4-year period.
- ItemAerosol optical properties in the southeastern United States in summer - Part 1: Hygroscopic growth(Katlenburg-Lindau : EGU, 2016) Brock, Charles A.; Wagner, Nicholas L.; Anderson, Bruce E.; Attwood, Alexis R.; Beyersdorf, Andreas; Campuzano-Jost, Pedro; Carlton, Annmarie G.; Day, Douglas A.; Diskin, Glenn S.; Gordon, Timothy D.; Jimenez, Jose L.; Lack, Daniel A.; Liao, Jin; Markovic, Milos Z.; Middlebrook, Ann M.; Ng, Nga L.; Perring, Anne E.; Richardson, Matthews S.; Schwarz, Joshua P.; Washenfelder, Rebecca A.; Welti, Andre; Xu, Lu; Ziemba, Luke D.; Murphy, Daniel M.Aircraft observations of meteorological, trace gas, and aerosol properties were made during May–September 2013 in the southeastern United States (US) under fair-weather, afternoon conditions with well-defined planetary boundary layer structure. Optical extinction at 532 nm was directly measured at relative humidities (RHs) of  ∼  15,  ∼  70, and  ∼  90 % and compared with extinction calculated from measurements of aerosol composition and size distribution using the κ-Köhler approximation for hygroscopic growth. The calculated enhancement in hydrated aerosol extinction with relative humidity, f(RH), calculated by this method agreed well with the observed f(RH) at  ∼  90 % RH. The dominance of organic aerosol, which comprised 65 ± 10 % of particulate matter with aerodynamic diameter  <  1 µm in the planetary boundary layer, resulted in relatively low f(RH) values of 1.43 ± 0.67 at 70 % RH and 2.28 ± 1.05 at 90 % RH. The subsaturated κ-Köhler hygroscopicity parameter κ for the organic fraction of the aerosol must have been  <  0.10 to be consistent with 75 % of the observations within uncertainties, with a best estimate of κ  =  0.05. This subsaturated κ value for the organic aerosol in the southeastern US is broadly consistent with field studies in rural environments. A new, physically based, single-parameter representation was developed that better described f(RH) than did the widely used gamma power-law approximation.
- 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.
- ItemOptical properties of aerosol mixtures derived from sun-sky radiometry during SAMUM-2(Milton Park : Taylor & Francis, 2017) Toledano, C.; Wiegner, M.; Groß, S.; Freudenthaler, V.; Gasteiger, J.; Müller, D.; Müller, T.; Schladitz, A.; Weinzierl, B.; Torres, B.; O’neill, N.T.The SAMUM-2 experiment took place in the Cape Verde is lands in January–February 2008. The colocated ground-based and airborne instruments allow the study of desert dust optical and microphysical properties in a closure experiment. The Meteorological Institute of the University of Munich deployed one sun-sky photometer and two tropospheric lidar systems. A travelling AERONET-Cimel sun-sky radiometer was also deployed. During the measurement period the aerosol scenario over Cape Verde mostly consisted of a dust layer below 2 km and a smoke-dust layer above 2–4 km a.s.l. The Saharan dust arrived at the site from the NE, whereas the smoke originated in the African equatorial region. This paper describes the main results of the Sun photometer observations, supported by lidar information. An analysis of the variations in the aerosol optical depth (AOD) in the range 340–1550 nm, the Ångström exponent, volume size distributions and single scattering albedo is presented. The aerosol mixtures are analysed by means of the fine mode fraction of the AOD provided by the sun-sky inversion data and the Spectral Deconvolution Algorithm. The mean AOD (500 nm) was 0.31, with associated low ångström exponent of 0.46. Several types of events were detected within the data set, with prevalence of dust or mixtures as characterized by the Ångstr¨om exponents of extinction and absorption and the fine mode fraction. Aerosol properties derived from sunphotometry were compared to in situ measurements of size distribution, effective radius and single scattering albedo.
- ItemModelling lidar-relevant optical properties of complex mineral dust aerosols(Milton Park : Taylor & Francis, 2017) Gasteiger, Josef; Wiegner, Matthias; Groß, Silke; Freudenthaler, Volker; Toledano, Carlos; Tesche, Matthias; Kandler, KonradWe model lidar-relevant optical properties of mineral dust aerosols and compare the modelling results with optical properties derived from lidar measurements during the SAMUM field campaigns. The Discrete Dipole Approximation is used for optical modelling of single particles. For modelling of ensemble properties, the desert aerosol type of the OPAC aerosol dataset is extended by mixtures of absorbing and non-absorbing irregularly shaped mineral dust particles. Absorbing and non-absorbing particles are mixed to mimic the natural mineralogical inhomogeneity of dust particles. A sensitivity study reveals that the mineralogical inhomogeneity is critical for the lidar ratio at short wavelengths; it has to be considered for agreement with the observed wavelength dependence of the lidar ratio. The amount of particles with low aspect ratios (about 1.4 and lower) affects the lidar ratio at any lidar wavelength; their amount has to be low for agreement with SAMUM observations. Irregularly shaped dust particles with typical refractive indices, in general, have higher linear depolarization ratios than corresponding spheroids, and improve the agreement with the observations.
- ItemCloud condensation nuclei spectra derived from size distributions and hygroscopic properties of the aerosol in coastal south-west Portugal during ACE-2(Milton Park : Taylor & Francis, 2016) Dusek, Ulrike; Covert, David S.; Wiedensohler, Alfred; Neusüss, Christian; Weise, Diana; Cantrell, WillIn this work we propose and test a method to calculate cloud condensation nuclei (CCN) spectra basedon aerosol number size distributions and hygroscopic growth factors. Sensitivity studies show thatthis method can be used in a wide variety of conditions except when the aerosol consist mainly oforganic compounds. One crucial step in the calculations, estimating soluble ions in an aerosol particlebased on hygroscopic growth factors, is tested in an internal hygroscopic consistency study. The resultsshow that during the second Aerosol Characterization Experiment (ACE-2) the number concentrationof inorganic ions analyzed in impactor samples could be reproduced from measured growth factorswithin the measurement uncertainties at the measurement site in Sagres, Portugal. CCN spectra were calculated based on data from the ACE-2 field experiment at the Sagres site.The calculations overestimate measured CCN spectra on average by approximately 30%, which iscomparable to the uncertainties in measurements and calculations at supersaturations below 0.5%. Thecalculated CCN spectra were averaged over time periods when Sagres received clean air masses and airmasses influenced by aged and recent pollution. Pollution outbreaks enhance the CCN concentrationsat supersaturations near 0.2% by a factor of 3 (aged pollution) to 5 (recent pollution) compared to theclean marine background concentrations. In polluted air masses, the shape of the CCN spectra changes.The clean spectra can be approximated by a power function, whereas the polluted spectra are betterapproximated by an error function.