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Profiling of fine and coarse particle mass: Case studies of Saharan dust and Eyjafjallajökull/Grimsvötn volcanic plumes

2012, Ansmann, A., Seifert, P., Tesche, M., Wandinger, U.

The polarization lidar photometer networking (POLIPHON) method introduced to separate coarse-mode and fine-mode particle properties of Eyjafjallajökull volcanic aerosols in 2010 is extended to cover Saharan dust events as well. Furthermore, new volcanic dust observations performed after the Grimsvötn volcanic eruptions in 2011 are presented. The retrieval of particle mass concentrations requires mass-specific extinction coefficients. Therefore, a review of recently published mass-specific extinction coefficients for Saharan dust and volcanic dust is given. Case studies of four different scenarios corroborate the applicability of the profiling technique: (a) Saharan dust outbreak to central Europe, (b) Saharan dust plume mixed with biomass-burning smoke over Cape Verde, and volcanic aerosol layers originating from (c) the Eyjafjallajökull eruptions in 2010 and (d) the Grimsvötn eruptions in 2011. Strong differences in the vertical aerosol layering, aerosol mixing, and optical properties are observed for the different volcanic events.

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Measuring the morphology and density of internally mixed black carbon with SP2 and VTDMA: New insight into the absorption enhancement of black carbon in the atmosphere

2016, Zhang, Yuxuan, Zhang, Qiang, Cheng, Yafang, Su, Hang, Kecorius, Simonas, Wang, Zhibin, Wu, Zhijun, Hu, Min, Zhu, Tong, Wiedensohler, Alfred, He, Kebin

The morphology and density of black carbon (BC) cores in internally mixed BC (In-BC) particles affect their mixing state and absorption enhancement. In this work, we developed a new method to measure the morphology and effective density of the BC cores of ambient In-BC particles using a single-particle soot photometer (SP2) and a volatility tandem differential mobility analyzer (VTDMA) during the CAREBeijing-2013 campaign from 8 to 27 July 2013 at Xianghe Observatory. This new measurement system can select size-resolved ambient In-BC particles and measure the mobility diameter and mass of the In-BC cores. The morphology and effective density of the ambient In-BC cores are then calculated. For the In-BC cores in the atmosphere, changes in their dynamic shape factor (χ) and effective density (ρeff) can be characterized as a function of the aging process (Dp∕Dc) measured by SP2 and VTDMA. During an intensive field study, the ambient In-BC cores had an average shape factor χ of  ∼ 1.2 and an average density of  ∼ 1.2 g cm−3, indicating that ambient In-BC cores have a near-spherical shape with an internal void of  ∼ 30 %. From the measured morphology and density, the average shell ∕ core ratio and absorption enhancement (Eab) of ambient BC were estimated to be 2.1–2.7 and 1.6–1.9, respectively, for In-BC particles with sizes of 200–350 nm. When the In-BC cores were assumed to have a void-free BC sphere with a density of 1.8 g cm−3, the shell ∕ core ratio and Eab were overestimated by  ∼ 13 and  ∼ 17 %, respectively. The new approach developed in this work improves the calculations of the mixing state and optical properties of ambient In-BC particles by quantifying the changes in the morphology and density of ambient In-BC cores during aging.

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A methodology for investigating dust model performance using synergistic EARLINET/AERONET dust concentration retrievals

2015, Binietoglou, I., Basart, S., Alados-Arboledas, L., Amiridis, V., Argyrouli, A., Baars, H., Baldasano, J.M., Balis, D., Belegante, L., Bravo-Aranda, J.A., Burlizzi, P., Carrasco, V., Chaikovsky, A., Comerón, A., D'Amico, G., Filioglou, M., Granados-Muñoz, M.J., Haefele, A., Hervo, M., Iarlori, M., Kokkalis, P., Lange, D., Mamouri, R.E., Mattis, I., Molero, F., Montoux, N., Muñoz, A., Muñoz Porcar, C., Navas-Guzmán, F., Nicolae, D., Nisantzi, A., Papagiannopoulos, N., Papayannis, A., Pereira, S., Preißler, J., Pujadas, M., Rizi, V., Rocadenbosch, F., Sellegri, K., Simeonov, V., Tsaknakis, G., Wagner, F., Pappalardo, G.

Systematic measurements of dust concentration profiles at a continental scale were recently made possible by the development of synergistic retrieval algorithms using combined lidar and sun photometer data and the establishment of robust remote-sensing networks in the framework of Aerosols, Clouds, and Trace gases Research InfraStructure Network (ACTRIS)/European Aerosol Research Lidar Network (EARLINET). We present a methodology for using these capabilities as a tool for examining the performance of dust transport models. The methodology includes considerations for the selection of a suitable data set and appropriate metrics for the exploration of the results. The approach is demonstrated for four regional dust transport models (BSC-DREAM8b v2, NMMB/BSC-DUST, DREAMABOL, DREAM8-NMME-MACC) using dust observations performed at 10 ACTRIS/EARLINET stations. The observations, which include coincident multi-wavelength lidar and sun photometer measurements, were processed with the Lidar-Radiometer Inversion Code (LIRIC) to retrieve aerosol concentration profiles. The methodology proposed here shows advantages when compared to traditional evaluation techniques that utilize separately the available measurements such as separating the contribution of dust from other aerosol types on the lidar profiles and avoiding model assumptions related to the conversion of concentration fields to aerosol extinction values. When compared to LIRIC retrievals, the simulated dust vertical structures were found to be in good agreement for all models with correlation values between 0.5 and 0.7 in the 1–6 km range, where most dust is typically observed. The absolute dust concentration was typically underestimated with mean bias values of -40 to -20 μg m−3 at 2 km, the altitude of maximum mean concentration. The reported differences among the models found in this comparison indicate the benefit of the systematic use of the proposed approach in future dust model evaluation studies.

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Potential of polarization/Raman lidar to separate fine dust, coarse dust, maritime, and anthropogenic aerosol profiles

2017, Mamouri, Rodanthi-Elisavet, Ansmann, Albert

We 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.

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Mass deposition fluxes of Saharan mineral dust to the tropical northeast Atlantic Ocean: An intercomparison of methods

2014, Niedermeier, N., Held, A., Müller, T., Heinold, B., Schepanski, K., Tegen, I., Kandler, K., Ebert, M., Weinbruch, S., Read, K., Lee, J., Fomba, K.W., Müller, K., Herrmann, H., Wiedensohler, A.

Mass deposition fluxes of mineral dust to the tropical northeast Atlantic Ocean were determined within this study. In the framework of SOPRAN (Surface Ocean Processes in the Anthropocene), the interaction between the atmosphere and the ocean in terms of material exchange were investigated at the Cape Verde atmospheric observatory (CVAO) on the island Sao Vicente for January 2009. Five different methods were applied to estimate the deposition flux, using different meteorological and physical measurements, remote sensing, and regional dust transport simulations. The set of observations comprises micrometeorological measurements with an ultra-sonic anemometer and profile measurements using 2-D anemometers at two different heights, and microphysical measurements of the size-resolved mass concentrations of mineral dust. In addition, the total mass concentration of mineral dust was derived from absorption photometer observations and passive sampling. The regional dust model COSMO-MUSCAT was used for simulations of dust emission and transport, including dry and wet deposition processes. This model was used as it describes the AOD's and mass concentrations realistic compared to the measurements and because it was run for the time period of the measurements. The four observation-based methods yield a monthly average deposition flux of mineral dust of 12–29 ng m−2 s−1. The simulation results come close to the upper range of the measurements with an average value of 47 ng m−2 s−1. It is shown that the mass deposition flux of mineral dust obtained by the combination of micrometeorological (ultra-sonic anemometer) and microphysical measurements (particle mass size distribution of mineral dust) is difficult to compare to modeled mass deposition fluxes when the mineral dust is inhomogeneously distributed over the investigated area.

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Maritime aerosol network as a component of AERONET - First results and comparison with global aerosol models and satellite retrievals

2011, Smirnov, A., Holben, B.N., Giles, D.M., Slutsker, I., O'Neill, N.T., Eck, T.F., Macke, A., Croot, P., Courcoux, Y., Sakerin, S.M., Smyth, T.J., Zielinski, T., Zibordi, G., Goes, J.I., Harvey, M.J., Quinn, P.K., Nelson, N.B., Radionov, V.F., Duarte, C.M., Losno, R., Sciare, J., Voss, K.J., Kinne, S., Nalli, N.R., Joseph, E., Krishna Moorthy, K., Covert, D.S., Gulev, S.K., Milinevsky, G., Larouche, P., Belanger, S., Horne, E., Chin, M., Remer, L.A., Kahn, R.A., Reid, J.S., Schulz, M., Heald, C.L., Zhang, J., Lapina, K., Kleidman, R.G., Griesfeller, J., Gaitley, B.J., Tan, Q., Diehl, T.L.

The Maritime Aerosol Network (MAN) has been collecting data over the oceans since November 2006. Over 80 cruises were completed through early 2010 with deployments continuing. Measurement areas included various parts of the Atlantic Ocean, the Northern and Southern Pacific Ocean, the South Indian Ocean, the Southern Ocean, the Arctic Ocean and inland seas. MAN deploys Microtops hand-held sunphotometers and utilizes a calibration procedure and data processing traceable to AERONET. Data collection included areas that previously had no aerosol optical depth (AOD) coverage at all, particularly vast areas of the Southern Ocean. The MAN data archive provides a valuable resource for aerosol studies in maritime environments. In the current paper we present results of AOD measurements over the oceans, and make a comparison with satellite AOD retrievals and model simulations.

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Continuous vertical aerosol profiling with a multi-wavelength Raman polarization lidar over the Pearl River Delta, China

2017, Heese, Birgit, Baars, Holger, Bohlmann, Stephanie, Althausen, Dietrich, Deng, Ruru

A dataset of particle optical properties of the highly polluted atmosphere over the Pearl River Delta (PRD), Guangzhou, China, is presented in this paper. The data were derived from the measurements of a multiwavelength Raman and depolarization lidar PollyXT and a co-located AERONET sun photometer. The measurement campaign was conducted from November 2011 to mid-June 2012. These are the first Raman lidar measurements in the PRD that lasted for several months. A mean value of aerosol optical depth (AOD) of 0.54±0.33 was observed by the sun photometer at 500 nm in the polluted atmosphere over this megacity for the whole measurement period. The lidar profiles frequently show lofted aerosol layers, which reach altitudes of up to 2 to 3 km and, especially during the spring season, up to 5 km. These layers contain between 12 and 56% of the total AOD, with the highest values in spring. The aerosol types in these lofted layers are classified by their optical properties. The observed lidar ratio values range from 30 to 80 sr with a mean value of 48.0±10.7 sr at 532 nm. The linear particle depolarization ratio at 532 nm lies mostly below 5 %, with a mean value of 3.6±3.7 %. The majority of the Ångström exponents lie between 0.5 and 1.5, indicating a mixture of fine- and coarsemode aerosols. These results reveal that mostly urban pollution particles mixed with particles produced from biomass and industrial burning are present in the atmosphere above the Pearl River Delta. Trajectory analyses show that these pollution mixtures arise mainly from local and regional sources.

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Evaluation of the Lidar/Radiometer Inversion Code (LIRIC) to determine microphysical properties of volcanic and desert dust

2013, Wagner, J., Ansmann, A., Wandinger, U., Seifert, P., Schwarz, A., Tesche, M., Chaikovsky, A., Dubovik, O.

The Lidar/Radiometer Inversion Code (LIRIC) combines the multiwavelength lidar technique with sun/sky photometry and allows us to retrieve vertical profiles of particle optical and microphysical properties separately for fine-mode and coarse-mode particles. After a brief presentation of the theoretical background, we evaluate the potential of LIRIC to retrieve the optical and microphysical properties of irregularly shaped dust particles. The method is applied to two very different aerosol scenarios: a strong Saharan dust outbreak towards central Europe and an Eyjafjallajökull volcanic dust event. LIRIC profiles of particle mass concentrations for the coarse-mode as well as for the non-spherical particle fraction are compared with results for the non-spherical particle fraction as obtained with the polarization-lidar-based POLIPHON method. Similar comparisons for fine-mode and spherical particle fractions are presented also. Acceptable agreement between the different dust mass concentration profiles is obtained. LIRIC profiles of optical properties such as particle backscatter coefficient, lidar ratio, Ångström exponent, and particle depolarization ratio are compared with direct Raman lidar observations. Systematic deviations between the LIRIC retrieval products and the Raman lidar measurements of the desert dust lidar ratio, depolarization ratio, and spectral dependencies of particle backscatter and lidar ratio point to the applied spheroidal-particle model as main source for these uncertainties in the LIRIC results.

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Multi-wavelength Raman lidar, sun photometric and aircraft measurements in combination with inversion models for the estimation of the aerosol optical and physico-chemical properties over Athens, Greece

2012, Mamouri, R.E., Papayannis, A., Amiridis, V., Müller, D., Kokkalis, P., Rapsomanikis, S., Karageorgos, E.T., Tsaknakis, G., Nenes, A., Kazadzis, S., Remoundaki, E.

A novel procedure has been developed to retrieve, simultaneously, the optical, microphysical and chemical properties of tropospheric aerosols with a multi-wavelength Raman lidar system in the troposphere over an urban site (Athens, Greece: 37.9° N, 23.6° E, 200 m a.s.l.) using data obtained during the European Space Agency (ESA) THERMOPOLIS project, which took place between 15–31 July 2009 over the Greater Athens Area (GAA). We selected to apply our procedure for a case study of intense aerosol layers that occurred on 20–21 July 2009. The National Technical University of Athens (NTUA) EOLE 6-wavelength Raman lidar system has been used to provide the vertical profiles of the optical properties of aerosols (extinction and backscatter coefficients, lidar ratio) and the water vapor mixing ratio. An inversion algorithm was used to derive the mean aerosol microphysical properties (mean effective radius (reff), single-scattering albedo ω) and mean complex refractive index (m)) at selected heights in the 2–3 km height region. We found that reff was 0.14–0.4 (±0.14) μm, ω was 0.63–0.88 (±0.08) (at 532 nm) and m ranged from 1.44 (±0.10) + 0.01 (±0.01)i to 1.55 (±0.12) + 0.06 (±0.02)i, in good agreement (only for the reff values) with in situ aircraft measurements. The water vapor and temperature profiles were incorporated into the ISORROPIA II model to propose a possible in situ aerosol composition consistent with the retrieved m and ω values. The retrieved aerosol chemical composition in the 2–3 km height region gave a variable range of sulfate (0–60%) and organic carbon (OC) content (0–50%), although the OC content increased (up to 50%) and the sulfate content dropped (up to 30%) around 3 km height; the retrieved low ω value (0.63), indicates the presence of absorbing biomass burning smoke mixed with urban haze. Finally, the retrieved aerosol microphysical properties were compared with column-integrated sun photometer CIMEL data.

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Characterization and intercomparison of aerosol absorption photometers: Result of two intercomparison workshops

2011, Müller, T., Henzing, J.S., de Leeuw, G., Wiedensohler, A., Alastuey, A., Angelov, H., Bizjak, M., Collaud Coen, M., Engström, J.E., Gruening, C., Hillamo, R., Hoffer, A., Imre, K., Ivanow, P., Jennings, G., Sun, J.Y., Kalivitis, N., Karlsson, H., Komppula, M., Laj, P., Li, S.-M., Lunder, C., Marinoni, A., Martins dos Santos, S., Moerman, M., Nowak, A., Ogren, J.A., Petzold, A., Pichon, J.M., Rodriquez, S., Sharma, S., Sheridan, P.J., Teinilä, K., Tuch, T., Viana, M., Virkkula, A., Weingartner, E., Wilhelm, R., Wang, Y.Q.

Absorption photometers for real time application have been available since the 1980s, but the use of filter-based instruments to derive information on aerosol properties (absorption coefficient and black carbon, BC) is still a matter of debate. Several workshops have been conducted to investigate the performance of individual instruments over the intervening years. Two workshops with large sets of aerosol absorption photometers were conducted in 2005 and 2007. The data from these instruments were corrected using existing methods before further analysis. The inter-comparison shows a large variation between the responses to absorbing aerosol particles for different types of instruments. The unit to unit variability between instruments can be up to 30% for Particle Soot Absorption Photometers (PSAPs) and Aethalometers. Multi Angle Absorption Photometers (MAAPs) showed a variability of less than 5%. Reasons for the high variability were identified to be variations in sample flow and spot size. It was observed that different flow rates influence system performance with respect to response to absorption and instrumental noise. Measurements with non absorbing particles showed that the current corrections of a cross sensitivity to particle scattering are not sufficient. Remaining cross sensitivities were found to be a function of the total particle load on the filter. The large variation between the response to absorbing aerosol particles for different types of instruments indicates that current correction functions for absorption photometers are not adequate.