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- ItemLIVAS: A 3-D multi-wavelength aerosol/cloud database based on CALIPSO and EARLINET(München : European Geopyhsical Union, 2015) Amiridis, V.; Marinou, E.; Tsekeri, A.; Wandinger, U.; Schwarz, A.; Giannakaki, E.; Mamouri, R.; Kokkalis, P.; Binietoglou, I.; Solomos, S.; Herekakis, T.; Kazadzis, S.; Gerasopoulos, E.; Proestakis, E.; Kottas, M.; Balis, D.; Papayannis, A.; Kontoes, C.; Kourtidis, K.; Papagiannopoulos, N.; Mona, L.; Pappalardo, G.; Le Rille, O.; Ansmann, A.We present LIVAS (LIdar climatology of Vertical Aerosol Structure for space-based lidar simulation studies), a 3-D multi-wavelength global aerosol and cloud optical database, optimized to be used for future space-based lidar end-to-end simulations of realistic atmospheric scenarios as well as retrieval algorithm testing activities. The LIVAS database provides averaged profiles of aerosol optical properties for the potential spaceborne laser operating wavelengths of 355, 532, 1064, 1570 and 2050 nm and of cloud optical properties at the wavelength of 532 nm. The global database is based on CALIPSO observations at 532 and 1064 nm and on aerosol-type-dependent backscatter- and extinction-related Ångström exponents, derived from EARLINET (European Aerosol Research Lidar Network) ground-based measurements for the UV and scattering calculations for the IR wavelengths, using a combination of input data from AERONET, suitable aerosol models and recent literature. The required spectral conversions are calculated for each of the CALIPSO aerosol types and are applied to CALIPSO backscatter and extinction data corresponding to the aerosol type retrieved by the CALIPSO aerosol classification scheme. A cloud optical database based on CALIPSO measurements at 532 nm is also provided, neglecting wavelength conversion due to approximately neutral scattering behavior of clouds along the spectral range of LIVAS. Averages of particle linear depolarization ratio profiles at 532 nm are provided as well. Finally, vertical distributions for a set of selected scenes of specific atmospheric phenomena (e.g., dust outbreaks, volcanic eruptions, wild fires, polar stratospheric clouds) are analyzed and spectrally converted so as to be used as case studies for spaceborne lidar performance assessments. The final global data set includes 4-year (1 January 2008–31 December 2011) time-averaged CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations) data on a uniform grid of 1° × 1° with the original high vertical resolution of CALIPSO in order to ensure realistic simulations of the atmospheric variability in lidar end-to-end simulations.
- ItemTropospheric aerosol scattering and absorption over central Europe: A closure study for the dry particle state(München : European Geopyhsical Union, 2014) Ma, N.; Birmili, W.; Müller, T.; Tuch, T.; Cheng, Y.F.; Xu, W.Y.; Zhao, C.S.; Wiedensohler, A.This work analyses optical properties of the dry tropospheric aerosol measured at the regional Global Atmosphere Watch (GAW) observation site Melpitz in East Germany. For a continuous observation period between 2007 and 2010, we provide representative values of the dry-state scattering coefficient, hemispheric backscattering coefficient, absorption coefficient, single scattering albedo, and scattering Ångström exponent. Besides the direct measurement, the aerosol scattering coefficient was alternatively computed from experimental particle number size distributions using a Mie model. Within pre-defined limits, a closure could be achieved with the direct measurement. The achievement of closure implies that such calculations can be used as a high-level quality control measure for data sets involving multiple instrumentation. All dry-state optical properties show pronounced annual and diurnal variations, which are attributed to the corresponding variations in the regional emission fluxes, the intensity of secondary particle formation, and the mixing layer height. Air mass classification shows that atmospheric stability is a major factor influencing the dry aerosol properties at the GAW station. In the cold season, temperature inversions limit the volume available for atmospheric mixing, so that the dry-state aerosol optical properties near the ground proved quite sensitive to the geographical origin of the air mass. In the warm season, when the atmosphere is usually well-mixed during daytime, considerably less variability was observed for the optical properties between different air masses. This work provides, on the basis of quality-checked in situ measurements, a first step towards a climatological assessment of direct aerosol radiative forcing in the region under study.
- ItemLong term measurements of aerosol optical properties at a primary forest site in Amazonia(München : European Geopyhsical Union, 2013) Rizzo, L.V.; Artaxo, P.; Müller, T.; Wiedensohler, A.; Paixão, M.; Cirino, G.G.; Arana, A.; Swietlicki, E.; Roldin, P.; Fors, E.O.; Wiedemann, K.T.; Leal, L.S.M.; Kulmala, M.A long term experiment was conducted in a primary forest area in Amazonia, with continuous in-situ measurements of aerosol optical properties between February 2008 and April 2011, comprising, to our knowledge, the longest database ever in the Amazon Basin. Two major classes of aerosol particles, with significantly different optical properties were identified: coarse mode predominant biogenic aerosols in the wet season (January–June), naturally released by the forest metabolism, and fine mode dominated biomass burning aerosols in the dry season (July–December), transported from regional fires. Dry particle median scattering coefficients at the wavelength of 550 nm increased from 6.3 Mm−1 to 22 Mm−1, whereas absorption at 637 nm increased from 0.5 Mm−1 to 2.8 Mm−1 from wet to dry season. Most of the scattering in the dry season was attributed to the predominance of fine mode (PM2) particles (40–80% of PM10 mass), while the enhanced absorption coefficients are attributed to the presence of light absorbing aerosols from biomass burning. As both scattering and absorption increased in the dry season, the single scattering albedo (SSA) did not show a significant seasonal variability, in average 0.86 ± 0.08 at 637 nm for dry aerosols. Measured particle optical properties were used to estimate the aerosol forcing efficiency at the top of the atmosphere. Results indicate that in this primary forest site the radiative balance was dominated by the cloud cover, particularly in the wet season. Due to the high cloud fractions, the aerosol forcing efficiency absolute values were below −3.5 W m−2 in 70% of the wet season days and in 46% of the dry season days. Besides the seasonal variation, the influence of out-of-Basin aerosol sources was observed occasionally. Periods of influence of the Manaus urban plume were detected, characterized by a consistent increase on particle scattering (factor 2.5) and absorption coefficients (factor 5). Episodes of biomass burning and mineral dust particles advected from Africa were observed between January and April, characterized by enhanced concentrations of crustal elements (Al, Si, Ti, Fe) and potassium in the fine mode. During these episodes, median particle absorption coefficients increased by a factor of 2, whereas median SSA values decreased by 7%, in comparison to wet season conditions.
- ItemThe Ice Selective Inlet: A novel technique for exclusive extraction of pristine ice crystals in mixed-phase clouds(München : European Geopyhsical Union, 2015) Kupiszewski, P.; Weingartner, E.; Vochezer, P.; Schnaiter, M.; Bigi, A.; Gysel, M.; Rosati, B.; Toprak, E.; Mertes, S.; Baltensperger, U.Climate predictions are affected by high uncertainties partially due to an insufficient knowledge of aerosol–cloud interactions. One of the poorly understood processes is formation of mixed-phase clouds (MPCs) via heterogeneous ice nucleation. Field measurements of the atmospheric ice phase in MPCs are challenging due to the presence of much more numerous liquid droplets. The Ice Selective Inlet (ISI), presented in this paper, is a novel inlet designed to selectively sample pristine ice crystals in mixed-phase clouds and extract the ice residual particles contained within the crystals for physical and chemical characterization. Using a modular setup composed of a cyclone impactor, droplet evaporation unit and pumped counterflow virtual impactor (PCVI), the ISI segregates particles based on their inertia and phase, exclusively extracting small ice particles between 5 and 20 μm in diameter. The setup also includes optical particle spectrometers for analysis of the number size distribution and shape of the sampled hydrometeors. The novelty of the ISI is a droplet evaporation unit, which separates liquid droplets and ice crystals in the airborne state, thus avoiding physical impaction of the hydrometeors and limiting potential artefacts. The design and validation of the droplet evaporation unit is based on modelling studies of droplet evaporation rates and computational fluid dynamics simulations of gas and particle flows through the unit. Prior to deployment in the field, an inter-comparison of the optical particle size spectrometers and a characterization of the transmission efficiency of the PCVI was conducted in the laboratory. The ISI was subsequently deployed during the Cloud and Aerosol Characterization Experiment (CLACE) 2013 and 2014 – two extensive international field campaigns encompassing comprehensive measurements of cloud microphysics, as well as bulk aerosol, ice residual and ice nuclei properties. The campaigns provided an important opportunity for a proof of concept of the inlet design. In this work we present the setup of the ISI, including the modelling and laboratory characterization of its components, as well as field measurements demonstrating the ISI performance and validating the working principle of the inlet. Finally, measurements of biological aerosol during a Saharan dust event (SDE) are presented, showing a first indication of enrichment of bio-material in sub-2 μm ice residuals.
- ItemSurface matters: Limitations of CALIPSO V3 aerosol typing in coastal regions(München : European Geopyhsical Union, 2014) Kanitz, T.; Ansmann, A.; Foth, A.; Seifert, P.; Wandinger, U.; Engelmann, R.; Baars, H.; Althausen, D.; Casiccia, C.; Zamorano, F.In the CALIPSO data analysis, surface type (land/ocean) is used to augment the aerosol characterization. However, this surface-dependent aerosol typing prohibits a correct classification of marine aerosol over land that is advected from ocean to land. This might result in a systematic overestimation of the particle extinction coefficient and of the aerosol optical thickness (AOT) of up to a factor of 3.5 over land in coastal areas. We present a long-term comparison of CALIPSO and ground-based lidar observations of the aerosol conditions in the coastal environment of southern South America (Punta Arenas, Chile, 53° S), performed in December 2009–April 2010. Punta Arenas is almost entirely influenced by marine particles throughout the year, indicated by a rather low AOT of 0.02–0.04. However, we found an unexpectedly high fraction of continental aerosol in the aerosol types inferred by means of CALIOP observations and, correspondingly, too high values of particle extinction. Similar features of the CALIOP data analysis are presented for four other coastal areas around the world. Since CALIOP data serve as important input for global climate models, the influence of this systematic error was estimated by means of simplified radiative-transfer calculations.
- ItemComparison between CARIBIC aerosol samples analysed by accelerator-based methods and optical particle counter measurements(München : European Geopyhsical Union, 2014) Martinsson, B.G.; Friberg, J.; Andersson, S.M.; Weigelt, A.; Hermann, M.; Assmann, D.; Voigtländer, J.; Brenninkmeijer, C.A.M.; van Velthoven, P.J.F.; Zahn, A.Inter-comparison of results from two kinds of aerosol systems in the CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on a Instrument Container) passenger aircraft based observatory, operating during intercontinental flights at 9–12 km altitude, is presented. Aerosol from the lowermost stratosphere (LMS), the extra-tropical upper troposphere (UT) and the tropical mid troposphere (MT) were investigated. Aerosol particle volume concentration measured with an optical particle counter (OPC) is compared with analytical results of the sum of masses of all major and several minor constituents from aerosol samples collected with an impactor. Analyses were undertaken with the following accelerator-based methods: particle-induced X-ray emission (PIXE) and particle elastic scattering analysis (PESA). Data from 48 flights during 1 year are used, leading to a total of 106 individual comparisons. The ratios of the particle volume from the OPC and the total mass from the analyses were in 84% within a relatively narrow interval. Data points outside this interval are connected with inlet-related effects in clouds, large variability in aerosol composition, particle size distribution effects and some cases of non-ideal sampling. Overall, the comparison of these two CARIBIC measurements based on vastly different methods show good agreement, implying that the chemical and size information can be combined in studies of the MT/UT/LMS aerosol.
- ItemFine and coarse dust separation with polarization lidar(München : European Geopyhsical Union, 2014) Mamouri, R.E.; Ansmann, A.The polarization-lidar photometer networking (POLIPHON) method for separating dust and non-dust aerosol backscatter and extinction, volume, and mass concentration is extended to allow for a height-resolved separation of fine-mode and coarse-mode dust properties in addition. The method is applied to a period with complex aerosol layering of fine-mode background dust from Turkey and Arabian desert dust from Syria. The observation was performed at the combined European Aerosol Research Lidar Network (EARLINET) and Aerosol Robotic Network (AERONET) site of Limassol (34.7° N, 33° E), Cyprus, in September 2011. The dust profiling methodology and case studies are presented. Consistency between the column-integrated optical properties obtained with sun/sky photometer and the respective results derived by means of the new lidar-based method corroborate the applicability of the extended POLIPHON version.
- ItemAn optical particle size spectrometer for aircraft-borne measurements in IAGOS-CARIBIC(München : European Geopyhsical Union, 2016) Hermann, Markus; Weigelt, Andreas; Assmann, Denise; Pfeifer, Sascha; Müller, Thomas; Conrath, Thomas; Voigtländer, Jens; Heintzenberg, Jost; Wiedensohler, Alfred; Martinsson, Bengt G.; Deshler, Terry; Brenninkmeijer, Carl A.M.; Zahn, AndreasThe particle number size distribution is an important parameter to characterize the atmospheric aerosol and its influence on the Earth's climate. Here we describe a new optical particle size spectrometer (OPSS) for measurements of the accumulation mode particle number size distribution in the tropopause region on board a passenger aircraft (IAGOS-CARIBIC observatory: In-service Aircraft for a Global Observing System – Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container). A modified KS93 particle sensor from RION Co., Ltd., together with a new airflow system and a dedicated data acquisition system, is the key component of the CARIBIC OPSS. The instrument records individual particle pulse signal curves in the particle size range 130–1110 nm diameter (for a particle refractive index of 1.47-i0.006) together with a time stamp and thus allows the post-flight choice of the time resolution and the size distribution bin width. The CARIBIC OPSS has a 50 % particle detection diameter of 152 nm and a maximum asymptotic counting efficiency of 98 %. The instrument's measurement performance shows no pressure dependency and no particle coincidence for free tropospheric conditions. The size response function of the CARIBIC OPSS was obtained by a polystyrene latex calibration in combination with model calculations. Particle number size distributions measured with the new OPSS in the lowermost stratosphere agreed within a factor of 2 in concentration with balloon-borne measurements over western North America. Since June 2010 the CARIBIC OPSS is deployed once per month in the IAGOS-CARIBIC observatory.
- 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.
- ItemAging of secondary organic aerosol generated from the ozonolysis of α-pinene: Effects of ozone, light and temperature(München : European Geopyhsical Union, 2015) Denjean, C.; Formenti, P.; Picquet-Varrault, B.; Camredon, M.; Pangui, E.; Zapf, P.; Katrib, Y.; Giorio, C.; Tapparo, A.; Temime-Roussel, B.; Monod, A.; Aumont, B.; Doussin, J.F.A series of experiments was conducted in the CESAM (French acronym for Experimental Multiphasic Atmospheric Simulation Chamber) simulation chamber to investigate the evolution of the physical and chemical properties of secondary organic aerosols (SOAs) during different forcings. The present experiments represent a first attempt to comprehensively investigate the influence of oxidative processing, photochemistry, and diurnal temperature cycling upon SOA properties. SOAs generated from the ozonolysis of α-pinene were exposed under dry conditions (< 1% relative humidity) to (1) elevated ozone concentrations, (2) light (under controlled temperature conditions) or (3) light and heat (6 °C light-induced temperature increase), and the resultant changes in SOA optical properties (i.e. absorption and scattering), hygroscopicity and chemical composition were measured using a suite of instrumentation interfaced to the CESAM chamber. The complex refractive index (CRI) was derived from integrated nephelometer measurements of 525 nm wavelength, using Mie scattering calculations and measured number size distributions. The particle size growth factor (GF) was measured with a hygroscopic tandem differential mobility analyzer (H-TDMA). An aerosol mass spectrometer (AMS) was used for the determination of the f44 / f43 and O : C ratio of the particles bulk. No change in SOA size or chemical composition was observed during O3 and light exposure at constant temperature; in addition, GF and CRI of the SOA remained constant with forcing. On the contrary, illumination of SOAs in the absence of temperature control led to an increase in the real part of the CRI from 1.35 (±0.03) to 1.49 (±0.03), an increase of the GF from 1.04 (±0.02) to 1.14 (±0.02) and an increase of the f44 / f43 ratio from 1.73 (±0.03) to 2.23 (±0.03). The simulation of the experiments using the master chemical mechanism (MCM) and the Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) shows that these changes resulted from the evaporation of semi-volatile and less oxidized SOA species induced by the relatively minor increases in temperature (~ 6 °C). These surprising results suggest that α-pinene–O3 SOA properties may be governed more by local temperature fluctuations than by oxidative processing and photochemistry.