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Long-term profiling of mineral dust and pollution aerosol with multiwavelength polarization Raman lidar at the Central Asian site of Dushanbe, Tajikistan: Case studies

2017, Hofer, Julian, Althausen, Dietrich, Abdullaev, Sabur F., Makhmudov, Abduvosit N., Nazarov, Bakhron I., Schettler, Georg, Engelmann, Ronny, Baars, Holger, Fomba, K.Wadinga, Müller, Konrad, Heinold, Bernd, Kandler, Konrad, Ansmann, Albert

For the first time, continuous vertically resolved aerosol measurements were performed by lidar in Tajikistan, Central Asia. Observations with the multiwavelength polarization Raman lidar PollyXT were conducted during CADEX (Central Asian Dust EXperiment) in Dushanbe, Tajikistan, from March 2015 to August 2016. Co-located with the lidar, a sun photometer was also operated. The goal of CADEX is to provide an unprecedented data set on vertically resolved aerosol optical properties in Central Asia, an area highly affected by climate change but largely missing vertically resolved aerosol measurements. During the 18-month measurement campaign, mineral dust was detected frequently from ground to the cirrus level height. In this study, an overview of the measurement period is given and four typical but different example measurement cases are discussed in detail. Three of them are dust cases and one is a contrasting pollution aerosol case. Vertical profiles of the measured optical properties and the calculated dust and non-dust mass concentrations are presented. Dust source regions were identified by means of backward trajectory analyses. A lofted layer of Middle Eastern dust with an aerosol optical thickness (AOT) of 0.4 and an extinction-related Ångström exponent of 0.41 was measured. In comparison, two near-ground dust cases have Central Asian sources. One is an extreme dust event with an AOT of 1.5 and Ångström exponent of 0.12 and the other one is a most extreme dust event with an AOT of above 4 (measured by sun photometer) and an Ångström exponent of −0.08. The observed lidar ratios (and particle linear depolarization ratios) in the presented dust cases range from 40.3 to 46.9sr (and 0.18–0.29) at 355nm and from 35.7 to 42.9sr (0.31–0.35) at 532nm wavelength. The particle linear depolarization ratios indicate almost unpolluted dust in the case of a lofted dust layer and pure dust in the near-ground dust cases. The lidar ratio values are lower than typical lidar ratio values for Saharan dust (50–60sr) and comparable to Middle Eastern or west-Asian dust lidar ratios (35–45sr). In contrast, the presented case of pollution aerosol of local origin has an Ångström exponent of 2.07 and a lidar ratio (particle linear depolarization ratio) of 55.8sr (0.03) at 355nm and 32.8sr (0.08) at 532nm wavelength.

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In situ aerosol characterization at Cape Verde, Part 1: Particle number size distributions, hygroscopic growth and state of mixing of the marine and Saharan dust aerosol

2017, Schladitz, Alexander, Müller, Thomas, Nowak, Andreas, Kandler, Konrad, Lieke, Kirsten, Massling, Andreas, Wiedensohler, Alfred

Particle number size distributions and hygroscopic properties of marine and Saharan dust aerosol were investigated during the SAMUM-2 field study at Cape Verde in winter 2008. Aitken and accumulation mode particles were mainly assigned to the marine aerosol, whereas coarse mode particles were composed of sea-salt and a variable fraction of Saharan mineral dust. A new methodical approach was used to derive hygroscopic growth and state of mixing for a particle size range (volume equivalent) from dpve = 26 nm to 10 μm. For hygroscopic particles with dpve < 100 nm, the median hygroscopicity parameter κ is 0.35. From 100 nm < dpve < 350 nm, κ increases to 0.65. For larger particles, κ at dpve = 350 nm was used. For nearly hydrophobic particles, κ is between 0 and 0.1 for dpve < 250 nm and decreases to 0 for dpve > 250 nm. The mixing state of Saharan dust in terms of the number fraction of nearly hydrophobic particles showed the highest variation and ranges from 0.3 to almost 1. This study was used to perform a successful mass closure at ambient conditions and demonstrates the important role of hygroscopic growth of large sea-salt particles.

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Saharan Mineral Dust Experiments SAMUM-1 and SAMUM-2: What have we learned?

2011, Ansmann, Albert, Petzold, Andreas, Kandler, Konrad, Tegen, Ina, Wendisch, Manfred, Müller, Detlef, Weinzierl, Bernadett, Müller, Thomas, Heintzenberg, Jost

Two comprehensive field campaigns were conducted in 2006 and 2008 in the framework of the Saharan Mineral Dust Experiment (SAMUM) project. The relationship between chemical composition, shape morphology, size distribution and optical effects of the dust particles was investigated. The impact of Saharan dust on radiative transfer and the feedback of radiative effects upon dust emission and aerosol transport were studied. Field observations (ground-based, airborne and remote sensing) and modelling results were compared within a variety of dust closure experiments with a strong focus on vertical profiling. For the first time, multiwavelength Raman/polarization lidars and an airborne high spectral resolution lidar were involved in major dust field campaigns and provided profiles of the volume extinction coefficient of the particles at ambient conditions (for the full dust size distribution), of particle-shape-sensitive optical properties at several wavelengths, and a clear separation of dust and smoke profiles allowing for an estimation of the single-scattering albedo of the biomass-burning aerosol. SAMUM–1 took place in southern Morocco close to the Saharan desert in the summer of 2006, whereas SAMUM–2 was conducted in Cape Verde in the outflow region of desert dust and biomass-burning smoke from western Africa in the winter of 2008. This paper gives an overview of the SAMUM concept, strategy and goals, provides snapshots (highlights) of SAMUM–2 observations and modelling efforts, summarizes main findings of SAMUM–1 and SAMUM–2 and finally presents a list of remaining problems and unsolved questions.

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Regional modelling of Saharan dust and biomass-burning smoke, Part I: Model description and evaluation

2017, Heinold, Bernd, Tegen, Ina, Schepanski, Kerstin, Tesche, Matthias, Esselborn, Michael, Freudenthaler, Volker, Gross, Silke, Kandler, Konrad, Knippertz, Peter, Müller, Detlef, Schladitz, Alexander, Toledano, Carlos, Weinzierl, Bernadett, Ansmann, Albert, Althausen, Dietrich, Müller, Thomas, Petzold, Andreas, Wiedensohler, Alfred

The spatio-temporal evolution of the Saharan dust and biomass-burning plume during the SAMUM-2 field campaign in January and February 2008 is simulated at 28 km horizontal resolution with the regional model-system COSMOMUSCAT. The model performance is thoroughly tested using routine ground-based and space-borne remote sensing and local field measurements. Good agreement with the observations is found in many cases regarding transport patterns, aerosol optical thicknesses and the ratio of dust to smoke aerosol. The model also captures major features of the complex aerosol layering. Nevertheless, discrepancies in the modelled aerosol distribution occur, which are analysed in detail. The dry synoptic dynamics controlling dust uplift and transport during the dry season are well described by the model, but surface wind peaks associated with the breakdown of nocturnal low-level jets are not always reproduced. Thus, a strong dust outbreak is underestimated. While dust emission modelling is a priori more challenging, since strength and placement of dust sources depend on on-line computed winds, considerable inaccuracies also arise in observation-based estimates of biomass-burning emissions. They are caused by cloud and spatial errors of satellite fire products and uncertainties in fire emission parameters, and can lead to unrealistic model results of smoke transport.

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Dry versus wet marine particle optical properties: RH dependence of depolarization ratio, backscatter, and extinction from multiwavelength lidar measurements during SALTRACE

2017, Haarig, Moritz, Ansmann, Albert, Gasteiger, Josef, Kandler, Konrad, Althausen, Dietrich, Baars, Holger, Radenz, Martin, Farrell, David A.

Triple-wavelength lidar observations of the depolarization ratio and the backscatter coefficient of marine aerosol as a function of relative humidity (RH) are presented with a 5min time resolution. The measurements were performed at Barbados (13°N, 59°W) during the Saharan Aerosol Long-range Transport and Aerosol-Cloud interaction Experiment (SALTRACE) winter campaign in February 2014. The phase transition from spherical sea salt particles to cubic-like sea salt crystals was observed with a polarization lidar. The radiosonde and water-vapor Raman lidar observations show a drop in RH below 50% in the marine aerosol layer simultaneously with a strong increase in particle linear depolarization ratio, which reaches values up to 0.12±0.08 (at 355nm), 0.15±0.03 (at 532nm), and 0.10±0.01 (at 1064nm). The lidar ratio (extinction-to-backscatter ratio) increased from 19 and 23sr for spherical sea salt particles to 27 and 25sr (at 355 and 532nm, respectively) for cubic-like particle ensembles. Furthermore the scattering enhancement due to hygroscopic growth of the marine aerosol particles under atmospheric conditions was measured. Extinction enhancement factors from 40 to 80% RH of 1.94±0.94 at 355nm, 3.70±1.14 at 532nm, and 5.37±1.66 at 1064nm were found. The enhanced depolarization ratios and lidar ratios were compared to modeling studies of cubic sea salt particles.

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Modelling lidar-relevant optical properties of complex mineral dust aerosols

2017, Gasteiger, Josef, Wiegner, Matthias, Groß, Silke, Freudenthaler, Volker, Toledano, Carlos, Tesche, Matthias, Kandler, Konrad

We 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.

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Dust mobilization and aerosol transport from West Africa to Cape Verde - a meteorological overview of SAMUM-2

2017, Knippertz, Peter, Tesche, Matthias, Heinold, Bernd, Kandler, Konrad, Toledano, Carlos, Esselborn, Michael

The second field campaign of the SAharan Mineral dUst experiMent (SAMUM-2) was performed between 15 January and 14 February 2008 at the airport of Praia, Cape Verde, and provided valuable information to study the westward transport of Saharan dust and the mixing with biomass-burning smoke and sea-salt aerosol. Here lidar, meteorological, and particle measurements at Praia, together with operational analyses, trajectories, and satellite and synoptic station data are used to give an overview of the meteorological conditions and to place other SAMUM-2 measurements into a large-scale context. It is demonstrated that wintertime dust conditions at Cape Verde are closely related to the movement and intensification of mid-latitude high-pressure systems and the associated pressure gradients at their southern flanks. These cause dust emission over Mauritania, Mali, and Niger, and subsequent westward transport to Cape Verde within about 1–5 d. Dust emissions often peak around midday, suggesting a relation to daytime mixing of momentum from nocturnal low-level jets to the surface. The dust layer over Cape Verde is usually restricted to the lowest 1.5 km of the atmosphere. During periods with near-surface wind speeds about 5.5 ms−1, a maritime aerosol layer develops which often mixes with dust from above. On most days, the middle levels up to about 5 km additionally contain smoke that can be traced back to sources in southernWest Africa. Above this layer, clean air masses are transported to Cape Verde with the westerly flow at the southern side of the subtropical jet. The penetration of extra-tropical disturbances to low latitudes can bring troposphere-deep westerly flow and unusually clean conditions to the region.

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Properties of cloud condensation nuclei (CCN) in the trade wind marine boundary layer of the western North Atlantic

2016, Kristensen, Thomas B., Müller, Thomas, Kandler, Konrad, Benker, Nathalie, Hartmann, Markus, Prospero, Joseph M., Wiedensohler, Alfred, Stratmann, Frank

Cloud optical properties in the trade winds over the eastern Caribbean Sea have been shown to be sensitive to cloud condensation nuclei (CCN) concentrations. The objective of the current study was to investigate the CCN properties in the marine boundary layer (MBL) in the tropical western North Atlantic, in order to assess the respective roles of inorganic sulfate, organic species, long-range transported mineral dust and sea-salt particles. Measurements were carried out in June–July 2013, on the east coast of Barbados, and included CCN number concentrations, particle number size distributions and offline analysis of sampled particulate matter (PM) and sampled accumulation mode particles for an investigation of composition and mixing state with transmission electron microscopy (TEM) in combination with energy-dispersive X-ray spectroscopy (EDX). During most of the campaign, significant mass concentrations of long-range transported mineral dust was present in the PM, and influence from local island sources can be ruled out. The CCN and particle number concentrations were similar to what can be expected in pristine marine environments. The hygroscopicity parameter κ was inferred, and values in the range 0.2–0.5 were found during most of the campaign, with similar values for the Aitken and the accumulation mode. The accumulation mode particles studied with TEM were dominated by non-refractory material, and concentrations of mineral dust, sea salt and soot were too small to influence the CCN properties. It is highly likely that the CCN were dominated by a mixture of sulfate species and organic compounds.

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Thermal IR radiative properties of mixed mineral dust and biomass aerosol during SAMUM-2

2011, Köhler, Claas H., Trautmann, Thomas, Lindermeir, Erwin, Vreeling, Willem, Lieke, Kirsten, Kandler, Konrad, Weinzierl, Bernadett, Groß, Silke, Tesche, Matthias, Wendisch, Manfred

Ground-based high spectral resolution measurements of downwelling radiances from 800 to 1200 cm−1 were conducted between 20 January and 6 February 2008 within the scope of the SAMUM-2 field experiment. We infer the spectral signature of mixed biomass burning/mineral dust aerosols at the surface from these measurements and at top of the atmosphere from IASI observations. In a case study for a day characterized by the presence of high loads of both dust and biomass we attempt a closure with radiative transfer simulations assuming spherical particles. A detailed sensitivity analysis is performed to investigate the effect of uncertainties in the measurements ingested into the simulation on the simulated radiances. Distinct deviations between modelled and observed radiances are limited to a spectral region characterized by resonance bands in the refractive index. A comparison with results obtained during recent laboratory studies and field experiments reveals, that the deviations could be caused by the aerosol particles’ non-sphericity, although an unequivocal discrimination from measurement uncertainties is not possible. Based on radiative transfer simulations we estimate the aerosol’s direct radiative effect in the atmospheric window region to be 8 W m−2 at the surface and 1 W m−2 at top of the atmosphere.

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Characterization of the planetary boundary layer during SAMUM-2 by means of lidar measurements

2017, Groß, Silke, Gasteiger, Josef, Freudenthaler, Volker, Wiegner, Matthias, Geiß, Alexander, Schladitz, Alexander, Toledano, Carlos, Kandler, Konrad, Tesche, Matthias, Ansmann, Albert, Wiedensohler, Alfred

Measurements with two Raman-depolarization lidars of the Meteorological Institute of the Ludwig-Maximilians- Universit¨at, M¨unchen, Germany, performed during SAMUM-2, were used to characterize the planetary boundary layer (PBL) over Praia, Cape Verde. A novel approach was used to determine the volume fraction of dust υd in the PBL. This approach primarily relies on accurate measurements of the linear depolarization ratio. Comparisons with independent in situ measurements showed the reliability of this approach. Based on our retrievals, two different phases could be distinguished within the measurement period of almost one month. The first (22–31 January 2008) was characterized by high aerosol optical depth (AOD) in the PBL and large υd > 95%. During the second phase, the AOD in the PBL was considerably lower and υd less than ∼40%. These findings were in very good agreement with ground based in situ measurements, when ambient volume fractions are considered that were calculated from the actual measurements of the dry volume fraction. Only in cases when dust was not the dominating aerosol component (second phase), effects due to hygroscopic growth became important.