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- ItemCharacterization of the planetary boundary layer during SAMUM-2 by means of lidar measurements(Milton Park : Taylor & Francis, 2017) Groß, Silke; Gasteiger, Josef; Freudenthaler, Volker; Wiegner, Matthias; Geiß, Alexander; Schladitz, Alexander; Toledano, Carlos; Kandler, Konrad; Tesche, Matthias; Ansmann, Albert; Wiedensohler, AlfredMeasurements 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.
- 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.
- 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.
- ItemHygroscopic properties of aerosol particles in the northeastern Atlantic during ACE-2(Milton Park : Taylor & Francis, 2016) Swietlicki, Erik; Zhou, Jingchuan; Covert, David S.; Hämeri, Kaarle; Busch, Bernhard; Väkeva, Minna; Dusek, Ulrike; Berg, Olle H.; Wiedensohler, Alfred; Aalto, Pasi; Mäkelä, Jyrki; Martinsson, Bengt G.; Papaspiropoulos, Giorgos; Mentes, Besim; Frank, Göran; Stratmann, FrankMeasurements of the hygroscopic properties of sub-micrometer atmospheric aerosol particles were performed with hygroscopic tandem differential mobility analysers (H-TDMA) at 5 sites in the subtropical north-eastern Atlantic during the second Aerosol Characterization Experiment (ACE-2) from 16 June to 25 July 1997. Four of the sites were in the marine boundary layer and one was, at least occasionally, in the lower free troposphere. The hygroscopic diameter growth factors of individual aerosol particles in the dry particle diameter range 10−440 nm were generally measured for changes in relative humidity (RH) from <10% to 90%. In the marine boundary layer, growth factors at 90% RH were dependent on location, air mass type and particle size. The data was dominated by a unimodal growth distribution of more-hygroscopic particles, although a bimodal growth distribution including less-hygroscopic particles was observed at times, most often in the more polluted air masses. In clean marine air masses the more-hygroscopic growth factors ranged from about 1.6 to 1.8 with a consistent increase in growth factor with increasing particle size. There was also a tendency toward higher growth factors as sodium to sulphate molar ratio increased with increasing sea-salt contribution at higher wind speeds. During outbreaks of European pollution in the ACE-2 region, the growth factors of the largest particles were reduced, but only slightly. Growth factors at all sizes in both clean and polluted air masses were markedly lower at the Sagres, Portugal site due to more proximate continental influences. The frequency of occurrence of less-hygroscopic particles with a growth factor of ca. 1.15 was greatest during polluted conditions at Sagres. The free tropospheric 50 nm particles were predominately less-hygroscopic, with an intermediate growth factor of 1.4, but more-hygroscopic particles with growth factors of about 1.6 were also frequent. While these particles probably originate from within the marine boundary layer, the less-hygroscopic particles are probably more characteristic of lower free tropospheric air masses. For those occasions when measurements were made at 90% and an intermediate 60% or 70% RH, the growth factor G(RH) of the more-hygroscopic particles could be modelled empirically by a power law expression. For the ubiquitous more-hygroscopic particles, the expressions G(RH)=(1-RH/100)-0.210 for 50 nm Aitken mode particles and G(RH)=(1-RH/100)-0.233 for 166 nm accumulation mode particles are recommended for clean marine air masses in the north-eastern Atlantic within the range 0
- ItemIn situ aerosol characterization at Cape Verde, Part 2: Parametrization of relative humidity- and wavelength-dependent aerosol optical properties(Milton Park : Taylor & Francis, 2017) Schladitz, Alexander; Müller, Thomas; Nordmann, Stephan; Tesche, Matthias; Silke Groß, Silke Groß; Freudenthaler, Volker; Gasteiger, Josef; Wiedensohler, AlfredAn observation-based numerical study of humidity-dependent aerosol optical properties of mixed marine and Saharan mineral dust aerosol is presented. An aerosol model was developed based on measured optical and microphysical properties to describe the marine and Saharan dust aerosol at Cape Verde. A wavelength-dependent optical equivalent imaginary part of the refractive index and a scattering non-sphericity factor for Saharan dustwere derived. Simulations of humidity effects on optical properties by the aerosol model were validated with relative measurements of the extinction coefficient at ambient conditions. Parametrizations were derived to describe the humidity dependence of the extinction, scattering, and absorption coefficients as well as the asymmetry parameter and single scattering albedo. For wavelengths (300–950 nm) and dry dust volume fractions (0–1), aerosol optical properties as a function of relative humidity (RH = 0–90%) can be calculated from tabulated parameters. For instance, at a wavelength of 550 nm, a volume fraction of 0.5 of dust on the total particle volume (dry conditions) and a RH of 90%, the enhancements for the scattering, extinction and absorption coefficients are 2.55, 2.46 and 1.04, respectively, while the enhancements for the asymmetry parameter and single scattering albedo are 1.11 and 1.04.
- ItemRegional modelling of Saharan dust and biomass-burning smoke, Part I: Model description and evaluation(Milton Park : Taylor & Francis, 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, AlfredThe 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.