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- ItemIn 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(Milton Park : Taylor & Francis, 2017) Schladitz, Alexander; Müller, Thomas; Nowak, Andreas; Kandler, Konrad; Lieke, Kirsten; Massling, Andreas; Wiedensohler, AlfredParticle 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.
- 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.
- ItemDoppler lidar studies of heat island effects on vertical mixing of aerosols during SAMUM-2(Milton Park : Taylor & Francis, 2017) Engelmann, Ronny; Ansmann, Albert; Horn, Stefan; Seifert, Patric; Althausen, Dietrich; Tesche, Matthias; Esselborn, Michael; Fruntke, Julia; Lieke, Kirsten; Freudenthaler, Volker; Gross, SilkeA wind Doppler lidar was deployed next to three aerosol lidars during the SAMUM–2 campaign on the main island of Cape Verde. The effects of the differential heating of the island and the surrounding ocean and the orographic impact of the capital island Santiago and the small island on its luv side, Maio, are investigated. Horizontal and vertical winds were measured in the disturbed maritime boundary layer and compared to local radiosoundings. Lidar measurements from the research aircraft Falcon and a 3-D Large Eddy Simulation (LES) model were used in addition to study the heating effects on the scale of the islands. Indications are found that these effects can widely control the downward mixing from greater heights to the surface of African aerosols, mainly Saharan dust and biomass-burning smoke, which were detected in a complex layering over the Cape Verde region.
- 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.
- ItemElectron microscopy of particles collected at Praia, Cape Verde, during the Saharan Mineral Dust Experiment: Particle chemistry, shape, mixing state and complex refractive index(Milton Park : Taylor & Francis, 2017) Kandler, K.; Lieke, K.; Benker, N.; Emmel, C.; Küpper, M.; Müller-Ebert, D.; Ebert, M.; Scheuvens, D.; Schladitz, A.; Schütz, L.; Weinbruch, S.A large field experiment of the Saharan Mineral Dust Experiment (SAMUM) was performed in Praia, Cape Verde, in January and February 2008. The aerosol at Praia is a superposition of mineral dust, sea-salt, sulphates and soot. Particles smaller than 500 nm are mainly mineral dust, mineral dust–sulphate mixtures, sulphates and soot–sulphate mixtures. Particles larger then 2.5μm consist of mineral dust, sea-salt and few mineral dust–sulphate mixtures. A transition range exists in between. The major internal mixtures are mineral dust–sulphate and soot–sulphate. Mineral dust–sea-salt mixtures occur occasionally, mineral dust–soot mixtures were not observed. The aspect ratio was 1.3–1.4 for dry particles smaller than 500 nm and 1.6–1.7 for larger ones. Parameterizations are given for dry and humid state. Although the real part of the refractive index showed low variation (1.55–1.58 at 532 nm), a multi-modal imaginary part was detected as function of particle size, reflecting the complex composition. Soot mainly influences the absorption for wavelengths longer than the haematite absorption edge, whereas for shorter wavelengths dust is dominating. The refractive index of the aerosol depends on the source region of the mineral dust and on the presence/absence of a marine component.
- ItemSources of increase in lowermost stratospheric sulphurous and carbonaceous aerosol background concentrations during 1999–2008 derived from CARIBIC flights(Milton Park : Taylor & Francis, 2014) Friberg, Johan; Martinsson, Bengt G.; Andersson, Sandra M.; Brenninkmeijer, Carl A.M.; Hermann, Markus; Van Velthoven, Peter F.J.; Zahn, AndreasThis study focuses on sulphurous and carbonaceous aerosol, the major constituents of particulate matter in the lowermost stratosphere (LMS), based on in situ measurements from 1999 to 2008. Aerosol particles in the size range of 0.082 mm were collected monthly during intercontinental flights with the CARIBIC passenger aircraft, presenting the first long-term study on carbonaceous aerosol in the LMS. Elemental concentrations were derived via subsequent laboratory-based ion beam analysis. The stoichiometry indicates that the sulphurous fraction is sulphate, while an O/C ratio of 0.2 indicates that the carbonaceous aerosol is organic. The concentration of the carbonaceous component corresponded on average to approximately 25% of that of the sulphurous, and could not be explained by forest fires or biomass burning, since the average mass ratio of Fe to K was 16 times higher than typical ratios in effluents from biomass burning. The data reveal increasing concentrations of particulate sulphur and carbon with a doubling of particulate sulphur from 1999 to 2008 in the northern hemisphere LMS. Periods of elevated concentrations of particulate sulphur in the LMS are linked to downward transport of aerosol from higher altitudes, using ozone as a tracer for stratospheric air. Tropical volcanic eruptions penetrating the tropical tropopause are identified as the likely cause of the particulate sulphur and carbon increase in the LMS, where entrainment of lower tropospheric air into volcanic jets and plumes could be the cause of the carbon increase.
- ItemNear-global aerosol mapping in the upper troposphere and lowermost stratosphere with data from the CARIBIC project(Milton Park : Taylor & Francis, 2017) Heintzenberg, Jost; Hermann, Markus; Weigelt, Andreas; Kapustin, Vladimir; Anderson, Bruce; Thornhill, Kenneth; Van Velthoven, Peter; Zahn, Andreas; Brenninkmeijer, CarlThis study extrapolates aerosol data of the CARIBIC project from 1997 until June 2008 in along trajectories to compose large-scale maps and vertical profiles of submicrometre particle concentrations in the upper troposphere and lowermost stratosphere (UT/LMS). The extrapolation was validated by comparing extrapolated values with CARIBIC data measured near the respective trajectory position and by comparing extrapolated CARIBIC data to measurements by other experiments near the respective trajectory positions. Best agreement between extrapolated and measured data is achieved with particle lifetimes longer than the maximum length of used trajectories. The derived maps reveal regions of strong and frequent new particle formation, namely the Tropical Central and Western Africa with the adjacent Atlantic, South America, the Caribbean and Southeast Asia. These regions of particle formation coincide with those of frequent deep convective clouds. Vertical particle concentration profiles for the troposphere and the stratosphere confirm statistically previous results indicating frequent new particle formation in the tropopause region. There was no statistically significant increase in Aitken mode particle concentration between the first period of CARIBIC operation, 1997–2002, and the second period, 2004–2009. However, a significant increase in concentration occurred within the latter period when considering it in isolation.
- 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.
- ItemA simple non-linear analytical relationship between aerosol accumulation number and sub-micron volume, explaining their observed ratio in the clean and polluted marine boundary layer(Milton Park : Taylor & Francis, 2016) Van Dingenen, Rita; Virkkula, Aki O.; Raes, Frank; Bates, Timothy S.; Wiedensohler, AlfredWe propose an analytical expression for the relation between aerosol accumulation number and sub-micron volume over the marine boundary layer (MBL), based on a simple balance equation. By providing appropriate source and sink terms which account for entrainment, coagulation, in-cloud scavenging and condensational growth, the model is able to reproduce the observed ratio between MBL particles larger than 80 nm diameter (as a proxy for accumulation mode number) and submicron aerosol volume, from freshly polluted to background conditions. Entrainment and coagulation are essential in predicting the observed ratio. Budget and lifetime calculations show that, due to relatively low source rates of oceanic non-sea-salt-sulfate and sea-salt, the anthropogenic signature in aerosol volume remains significant even after 8 days of MBL transport.
- ItemAerosol physical properties and processes in the lower marine boundary layer: A comparison of shipboard sub-micron data from ACE-1 and ACE-2(Milton Park : Taylor & Francis, 2016) Bates, Timothy S.; Quinn, Patricia K.; Covert, David S.; Coffman, Derek J.; Johnson, James E.; Wiedensohler, AlfredThe goals of the IGAC Aerosol Characterization Experiments (ACE) are to determine and understand the properties and controlling processes of the aerosol in a globally representative range of natural and anthropogenically perturbed environments. ACE-1 was conducted in the remote marine atmosphere south of Australia while ACE-2 was conducted in the anthropogenically modified atmosphere of the Eastern North Atlantic. In-situ shipboard measurements from the RV Discoverer(ACE-1) and the RV Professor Vodyanitskiy(ACE-2), combined with calculated back trajectories can be used to define the physical properties of the sub-micron aerosol in marine boundary layer (MBL) air masses from the remote Southern Ocean, Western Europe, the Iberian coast, the Mediterranean and the background Atlantic Ocean. The differences in these aerosol properties, combined with dimethylsulfide, sulfur dioxide and meteorological measurements provide a means to assess processes that affect the aerosol distribution. The background sub-micron aerosol measured over the Atlantic Ocean during ACE-2 was more abundant (number and volume) and appeared to be more aged than that measured over the Southern Ocean during ACE-1. Based on seawater DMS measurements and wind speed, the oceanic source of non-sea-salt sulfur and sea-salt to the background marine atmosphere during ACE-1 and ACE-2 was similar. However, the synoptic meteorological pattern was quite different during ACE-1 and ACE-2. The frequent frontal passages during ACE-1 resulted in the mixing of nucleation mode particles into the marine boundary layer from the free troposphere and relatively short aerosol residence times. In the more stable meteorological setting of ACE-2, a significant nucleation mode aerosol was observed in the MBL only for a half day period associated with a weak frontal system. As a result of the longer MBL aerosol residence times, the average background ACE-2 accumulation mode aerosol had a larger diameter and higher number concentration than during ACE-1. The sub-micron aerosol number size distributions in the air masses that passed over Western Europe, the Mediterranean, and coastal Portugal were distinctly different from each other and the background aerosol. The differences can be attributed to the age of the air mass and the degree of cloud processing.