2016, Bates, Timothy S., Quinn, Patricia K., Covert, David S., Coffman, Derek J., Johnson, James E., Wiedensohler, Alfred

The 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.

2017, Tesche, Matthias, Gross, Silke, Ansmann, Albert, Müller, Detlef, Althausen, Dietrich, Freudenthaler, Volker, Esselborn, Michael

Extensive lidar measurements of Saharan dust and biomass-burning smoke were performed with one airborne and three ground-based instruments in the framework of the second part of the SAharan Mineral dUst experiMent (SAMUM-2a) during January and February of 2008 at Cape Verde. Further lidar observations with one system only were conducted duringMay and June of 2008 (SAMUM-2b). The active measurements were supported by Sun photometer observations. During winter, layers of mineral dust from the Sahara and biomass-burning smoke from southern West Africa pass Cape Verde on their way to South America while pure dust layers cross the Atlantic on their way to the Caribbean during summer. The mean 500-nm aerosol optical thickness (AOT) observed during SAMUM-2a was 0.35 ± 0.18. SAMUM-2a observations showed transport of pure dust within the lowermost 1.5 km of the atmospheric column. In the height range from 1.5 to 5.0 km, mixed dust/smoke layers with mean lidar ratios of 67 ± 14 sr at 355 and 532 nm, respectively, prevailed. Within these layers, wavelength-independent linear particle depolarization ratios of 0.12–0.18 at 355, 532, and 710 nm indicate a large contribution (30–70%) of mineral dust to the measured optical properties. Ångstr¨om exponents for backscatter and extinction of around 0.7 support this finding. Mean extinction coefficients in the height range between 2 and 4 km were 66 ± 6 Mm−1 at 355 nm and 48 ± 5 Mm−1 at 532 nm. Comparisons with airborne high-spectral-resolution lidar observations show good agreement within the elevated layers. 3–5 km deep dust layers where observed during SAMUM-2b. These layers showed optical properties similar to the ones of SAMUM-1 in Morocco with a mean 500-nm AOT of 0.4 ± 0.2. Dust extinction coefficients were about 80 ± 6 Mm−1 at 355 and 532 nm. Dust lidar ratios were 53 ± 10 sr at 355 and 532 nm, respectively. Dust depolarization ratios showed an increase with wavelength from 0.31 ± 0.10 at 532 nm to 0.37 ± 0.07 at 710 nm.

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.

2014, Nordmann, S., Cheng, Y.F., Carmichael, G.R., Yu, M., van der Gon, H.A.C.Denier, Zhang, Q., Saide, P.E., Pöschl, U., Su, H., Birmili, W., Wiedensohler, A.

Particles containing black carbon (BC), a strong absorbing substance, exert a rather uncertain direct and indirect radiative forcing in the atmosphere. To investigate the mass concentration and absorption properties of BC particles over central Europe, the model WRF-Chem was used at a resolution of 12 km in conjunction with a high-resolution BC emission inventory (EUCAARI 42-Pan-European Carbonaceous Aerosol Inventory; 1/8° × 1/16°). The model simulation was evaluated using measurements of equivalent soot carbon, absorption coefficients and particle number concentrations at seven sites within the German Ultrafine Aerosol Network, PM mass concentrations from the dense measurement network of the German Federal Environmental Agency at 392 monitoring stations, and aerosol optical depth from MODIS and AERONET. A distinct time period (25 March to 10 April 2009) was chosen, during which the clean marine air mass prevailed in the first week and afterwards the polluted continental air mass mainly from the southeast dominated with elevated daily average BC concentration of up to 4 μ g m−3. The simulated PM mass concentration, aerosol number concentration and optical depth were in good agreement with the observations, while the modelled BC mass concentrations were found to be a factor of 2 lower than the observations. Together with back trajectories, detailed model bias analyses suggested that the current BC emission in countries to the east and south of Germany might be underestimated by a factor of 5, at least for the simulation period. Running the model with upscaled BC emissions in these regions led to a smaller model bias and a better correlation between model and measurement. In contrast, the particle absorption coefficient was positively biased by about 20% even when the BC mass concentration was underestimated by around 50%. This indicates that the internal mixture treatment of BC in the WRF-Chem optical calculation is unrealistic in our case, which overamplifies the light absorption by BC-containing particles. By adjusting the modelled mass absorption cross-section towards the measured values, the simulation of particle light absorption of BC was improved as well. Finally, the positive direct radiative forcing of BC particles at the top of the atmosphere was estimated to be in the range of 0 to +4 W m−2 over Germany for the model run with improved BC mass concentration and adjusted BC light absorption cross-section. This adjustment lowered the positive forcing of BC by up to 70%, compared with the internal mixing treatment of BC in the model simulation.

2016, Quinn, P.K., Bates, T.S., Coffman, D.J., Coffman, Derek J., Miller, T.L., Johnson, J.E., Covert, D.S., Putaud, J.- P., Neusüß, C., Novakov, T.

Shipboard measurements of aerosol chemical composition and optical properties were made during both ACE-1 and ACE-2. ACE-1 focused on remote marine aerosol minimally perturbed by continental sources. ACE-2 studied the outflow of European aerosol into the NE Atlantic atmosphere. A variety of air masses were sampled during ACE-2 including Atlantic, polar, Iberian Peninsula, Mediterranean, and Western European. Reported here are mass size distributions of non-sea salt (nss) sulfate, sea salt, and methanesulfonate and submicron and supermicron concentrations of black and organic carbon. Optical parameters include submicron and supermicron aerosol scattering and backscattering coefficients at 550 nm, the absorption coefficient at 550±20 nm, the Ångström exponent for the 550 and 700 nm wavelength pair, and single scattering albedo at 550 nm. All data are reported at the measurement relative humidity of 55%. Measured concentrations of nss sulfate aerosol indicate that, relative to ACE-1, ACE-2 aerosol during both marine and continental flow was impacted by continental sources. Thus, while sea salt controlled the aerosol chemical composition and optical properties of both the submicron and supermicron aerosol during ACE-1, it played a relatively smaller role in ACE-2. This is confirmed by the larger average Ångström exponent for ACE-2 continental aerosol of 1.2±0.26 compared to the ACE-1 average of -0.03±0.38. The depletion of chloride from sea salt aerosol in ACE-2 continental air masses averaged 55±25% over all particle sizes. This compares to the ACE-2 marine average of 4.8±18% and indicates the enhanced interaction of anthropogenic acids with sea salt as continental air masses are transported into the marine atmosphere. Single scattering albedos averaged 0.95±0.03 for ACE-2 continental air masses. Averages for ACE-2 and ACE-1 marine air masses were 0.98±0.01 and 0.99±0.01, respectively.

2017, Schladitz, Alexander, Müller, Thomas, Nordmann, Stephan, Tesche, Matthias, Silke Groß, Silke Groß, Freudenthaler, Volker, Gasteiger, Josef, Wiedensohler, Alfred

An 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.

2015, D'Amico, Giuseppe, Amodeo, A., Baars, H., Binietoglou, I., Freudenthaler, V., Mattis, I., Wandinger, U., Pappalardo, G.

In this paper we describe the EARLINET Single Calculus Chain (SCC), a tool for the automatic analysis of lidar measurements. The development of this tool started in the framework of EARLINET-ASOS (European Aerosol Research Lidar Network – Advanced Sustainable Observation System); it was extended within ACTRIS (Aerosol, Clouds and Trace gases Research InfraStructure Network), and it is continuing within ACTRIS-2. The main idea was to develop a data processing chain that allows all EARLINET stations to retrieve, in a fully automatic way, the aerosol backscatter and extinction profiles starting from the raw lidar data of the lidar systems they operate. The calculus subsystem of the SCC is composed of two modules: a pre-processor module which handles the raw lidar data and corrects them for instrumental effects and an optical processing module for the retrieval of aerosol optical products from the pre-processed data. All input parameters needed to perform the lidar analysis are stored in a database to keep track of all changes which may occur for any EARLINET lidar system over the time. The two calculus modules are coordinated and synchronized by an additional module (daemon) which makes the whole analysis process fully automatic. The end user can interact with the SCC via a user-friendly web interface. All SCC modules are developed using open-source and freely available software packages. The final products retrieved by the SCC fulfill all requirements of the EARLINET quality assurance programs on both instrumental and algorithm levels. Moreover, the manpower needed to provide aerosol optical products is greatly reduced and thus the near-real-time availability of lidar data is improved. The high-quality of the SCC products is proven by the good agreement between the SCC analysis, and the corresponding independent manual retrievals. Finally, the ability of the SCC to provide high-quality aerosol optical products is demonstrated for an EARLINET intense observation period.

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, Frank

Measurements 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

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.

2011, Deng, Z.Z., Zhao, C.S., Ma, N., Liu, P.F., Ran, L., Xu, W.Y., Chen, J., Liang, Z., Liang, S., Huang, M.Y., Ma, X.C., Zhang, Q., Quan, J.N., Yan, P., Henning, S., Mildenberger, K., Sommerhage, E., Schäfer, M., Stratmann, F., Wiedensohler, A.

Size-resolved and bulk activation properties of aerosols were measured at a regional/suburban site in the North China Plain (NCP), which is occasionally heavily polluted by anthropogenic aerosol particles and gases. A Cloud Condensation Nuclei (CCN) closure study is conducted with bulk CCN number concentration (NCCN) and calculated CCN number concentration based on the aerosol number size distribution and size-resolved activation properties. The observed CCN number concentration (NCCN-obs) are higher than those observed in other locations than China, with average NCCN-obs of roughly 2000, 3000, 6000, 10 000 and 13 000 cm−3 at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.70%, respectively. An inferred critical dry diameter (Dm) is calculated based on the NCCN-obs and aerosol number size distribution assuming homogeneous chemical composition. The inferred cut-off diameters are in the ranges of 190–280, 160–260, 95–180, 65–120 and 50–100 nm at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.7%, with their mean values 230.1, 198.4, 128.4, 86.4 and 69.2 nm, respectively. Size-resolved activation measurements show that most of the 300 nm particles are activated at the investigated supersaturations, while almost no particles of 30 nm are activated even at the highest supersaturation of 0.72%. The activation ratio increases with increasing supersaturation and particle size. The slopes of the activation curves for ambient aerosols are not as steep as those observed in calibrations with ammonium sulfate suggesting that the observed aerosols is an external mixture of more hygroscopic and hydrophobic particles. The calculated CCN number concentrations (NCCN-calc) based on the size-resolved activation ratio and aerosol number size distribution correlate well with the NCCN-obs, and show an average overestimation of 19%. Sensitivity studies of the CCN closure show that the NCCN at each supersaturation is well predicted with the campaign average of size-resolved activation curves. These results indicate that the aerosol number size distribution is critical in the prediction of possible CCN. The CCN number concentration can be reliably estimated using time-averaged, size-resolved activation efficiencies without accounting for the temporal variations.